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Morell, Bonin Tyra. "Prestationsanalys av granulerataktivt kol (GAC) – en jämförelse mellan två etablerade GAC-typer." Thesis, Uppsala universitet, Institutionen för geovetenskaper, 2017. http://urn.kb.se/resolve?urn=urn:nbn:se:uu:diva-328611.
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Vattenverket Görväln i Järfälla planerar ett nytt vattenverk i framtiden, lokaliserat intill nuvarande vattenverk. Idag är den kemiska barriären, granulerat aktivt kol, ur funktion och utvärderas i det här projektet för att effektivisera processen. Den här studien fokuserar på att optimera den kemiska barriären genom att jämföra två sorter av granulerat aktivt kol (GAC). Jämförelsen sker genom analysering av löst organiskt kol (DOC), totalt organiskt kol (TOC), samt absorbans och fluorescens. Vattnet som använts i studien kommer direkt från det sandfiltrerade vattnet i Görvälnverkets reningsprocess. För att testa de olika GAC-sorterna konstruerades en kolonnuppsättning med överflödessystem. Syftet var att jämföra två olika GAC med kortare samt längre uppehållstid och deras absorberingsförmåga med avseende på DOC och TOC. Kolonner med längre kontakttid visade effektivare borttagning av DOC, TOC och fluorescerande ämnen oberoende av GAC-sort. Kolonner med FiltraSorb® 400 uppnår genombrott ungefär 30 % långsammare än Norit® 830 W för samma bäddvolymer. Skillnaden mellan längre kontakttid och kortare kontakttid var inte lika markant som skillnaden mellan GAC-sorterna. FiltraSorb® 400 presterade ungefär 30 % bättre vid borttagning av DOC och TOC jämfört mot Norit® 830 W. Adsorptionskapaciteten för Norit® 830 W försämrades betydligt snabbare än för FiltraSorb® 400. Det innebär att FiltraSorb® 400 behöver bakspolas mindre ofta och regenereras mer sällan än Norit® 830 W. FiltraSorb® 400 är därför den GAC-sort som rekommenderas för Görvälnverkets vatten med avseende på borttagning av DOC. Den här studien kommer att användas som underlag för pilotanläggningen som är stationerad intill kolonnuppställningen. Uppsättningen kommer också att användas för framtida kinetik och spårämnesförsök i vattenverket och på andra vattenverk.There are multiple steps to be done in the drinking water treatment process. The product must obtain high quality and to do so, it must reach certain requirements. One of the treatment steps in Görväln water treatment plant, Stockholm, is to use granular active carbon (GAC). The GAC function is to filter away taste and odor in addition to acting as a chemical barrier, although the latter does not work properly in the water treatment plant today.The project´s aim is comparing the performance of two types of GAC, Norit® 830 W and FiltraSorb® 400, together with the effect of longer (21 minutes) and shorter (7 minutes) contact time (EBCT). The contact time (EBCT) is the time, in minutes, that a body of water is in contact with the GAC-filter. A longer EBCT, means lower flow, which leads to longer time for the GAC to adsorb contaminants from the water.To evaluate the difference between the GAC-types a column-test was constructed. The test allows a direct comparison to full scale operations. The water used during this study was taken directly after the sand filtration process in Görväln. The water is clear and particles visible to the naked eye are eliminated during the sand filtration. However, the small dissolved organic components (carbon) are hard to remove, which makes the GAC-filter important.The performance of the GAC was evaluated by the removal efficiency of TOC, DOC and evaluation of fluorescence and absorbance capacity. The result indicated a better performance for both GAC using a longer contact time. Best effect of the long contact time was seen during the fluorescence measurement, where calculated indexes and removal of specific compounds were distinguished.The difference between longer, 21 minutes, and shorter, 7 minutes, contact time was not as significant as the difference between the two types of GAC. FiltraSorb® 400 had a significant higher adsorbance capacity for DOC and TOC, 30 % better than Norit® 830 W, at the same bed volume. Norit® 830 W reached breakthrough much faster (~80 %) than FiltraSorb® 400 (~50%) at around 4700 bed volumes.
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Zheng, Jing. "Application of GAC adsorption in pulp and paper mill effluent treatment." Thesis, National Library of Canada = Bibliothèque nationale du Canada, 2000. http://www.collectionscanada.ca/obj/s4/f2/dsk1/tape4/PQDD_0019/MQ58522.pdf.
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Al-Attas, Omar. "Competitive Adsorption of Iron and Natural Organic Matter in Groundwater Using Granular Activated Carbon." Thèse, Université d'Ottawa / University of Ottawa, 2012. http://hdl.handle.net/10393/23349.
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The treatment of potable water in Vars, ON is accomplished by filtering the colored, iron-laden groundwater through granular activated carbon (GAC) filters. When first installed, these filters unexpectedly experienced chromatographic displacements of iron into the produced water which resulted in orange-brown water at consumers’ taps. The treatment plant was later modified by adding potassium permanganate oxidation and a greensand filter prior to the GAC adsorption columns. Consequently, iron was almost completely removed and no longer caused operational problems. The main objective of this dissertation is to study the interactions between natural organic matter (NOM) and iron that caused the observed chromatographic effect. This study was divided into three main stages: a) characterization study on Vars groundwater and its treatment system; b) study of the competitive adsorption of iron with NOM in Vars groundwater; and c) evaluation of the rapid small-scale column test (RSSCT) for predicting the full-scale GAC column breakthroughs. The characterization of Vars groundwater showed that ferrous iron was found to be the dominant iron species, representing 90% of the total iron, and that 15 - 35% of the iron was complexed with NOM. It was hypothesized that the chromatographic displacement of iron from the GAC columns was caused by NOM-iron complexes; however, field mini-column experiments showed this was not the case. Thus, competitive adsorption between iron and NOM was seen as the more likely cause of the chromatographic effect. The adsorption capacity of ferrous iron in Vars raw water was less than that in organic-free water by a factor of 7 due to the competition with NOM over the GAC adsorbing sites. However, the NOM adsorption capacity was not reduced due to the presence of ferrous iron. It was hypothesized that ideal adsorption solution theory (IAST) models, which have been successful in describing competitive adsorption between target organic compounds and NOM, could model the competition between an inorganic compound such as ferrous iron and NOM. The hypothesis was proved to be correct, and the adsorption isotherm of iron in competition with NOM in Vars groundwater was simulated very well by several versions of the IAST model. However, none of the models were capable of simulating the competitive adsorption of NOM and ferrous iron simultaneously. Since the presence of iron did not significantly reduce the adsorption capacity of NOM, a simplified approach of using the single-solute NOM isotherm to represent the competitive NOM isotherm was recommended. The performance of the rapid small-scale column test (RSSCT) was evaluated in order to simulate the iron chromatographic effect observed at Vars’ full-scale GAC column. The RSSCT was not capable of predicting the iron phenomenon and the test proved to be problematic due to the oxidation and precipitation of iron within the small voids between the small-scale column’s GAC particles. The RSSCT, using constant and linear diffusivities, were applied to simulate the NOM adsorption after greensand treatment. Integrating both diffusivities, the tests predicted the onset and slope of the NOM breakthrough up to 10-L water treated/g GAC, which is equivalent to 250 days of operation time for the full-scale column. However, the NOM breakthroughs deviated beyond that point and the RSSCT using constant diffusivity underestimated the column performance greatly. On the other hand, the linear diffusivity RSSCT underestimated the performance to a lesser degree and its NOM breakthrough was quite parallel to the full-scale performance with lower NOM removals of 15%. The higher long-term NOM removal in the full-scale system may be explained by biodegradation, a phenomenon that was not considered by the short duration of RSSCT.
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Kelley, Thomas M. "Using Rapid Small Scale Column Testing to Evaluate Granular Activated Carbon Adsorption of Cyanotoxins from Drinking Water." University of Cincinnati / OhioLINK, 2017. http://rave.ohiolink.edu/etdc/view?acc_num=ucin150514901618082.
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Rosenzweig, Shirley Ferreira. "Adsorption of Copper (II) on Functionalized Carbon Nanotubes (CNT): A study of adsorption mechanisms and comparative analysis with Graphene Nanoplatelets (GNP) and Granular Activated Carbon (GAC) F-400." University of Cincinnati / OhioLINK, 2013. http://rave.ohiolink.edu/etdc/view?acc_num=ucin1368026548.
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Qiu, Yong. "STUDY ON TREATMENT TECHNOLOGIES FOR PERFLUOROCHEMICALS IN WASTEWATER." Doctoral thesis, 京都大学 (Kyoto University), 2007. http://hdl.handle.net/2433/44143.
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学位授与年月日: 2007-07-23 ; 学位の種類: 新制・課程博士 ; 学位記番号: 工博第2837号Perfluorochemicals (PFCs) were produced by industries and consumed “safely” as surfactants, repellents, additives, fire-fighting foams, polymer emulsifiers and insecticides for almost fifty years. However they are now considered as persistent, bioaccumulated and toxic (PBT) chemicals, and ubiquitously distributed in waster, air, human body and biota. Although some efforts were contributed to reduce PFCs in environment, such as development of alternatives and recycling processes, huge amount of persisted PFCs have already been discharged in environment and accumulated in biota including humans. In some industrialized areas, such as Yodo river basin in Japan, water environment and human blood were polluted by some PFCs, and thus reduction and control of PFCs were urgently required for the purpose of environmental safety and human health in these areas. Unfortunately, some studies implied that current water and wastewater treatment processes seemed ineffective to remove PFCs in trace levels. Therefore, this study will try to develop some proper technologies to treat trace level of PFCs in wastewater. In order to achieve this main objective, several works have been accomplished as follows. Current available literature has been reviewed to obtain a solid background for this study. Basic information of PFCs was summarized in physiochemical properties, PBT properties, productions and applications, regulations and etc.. Analytical methods for PFCs, especially of LC-ESI-MS/MS, were reviewed including pretreatment processes in diverse matrices, which derived objectives of chapter III. Distributions and behavior of PFCs were briefly discussed in water environments, biota sphere and human bloods. Available control strategies were shown in detail about alternatives, industrial recycling processes, and newly developed treatment processes. Current wastewater treatment processes showed inefficient removal for some PFCs, deriving objectives of chapter IV on the PFC behavior in treatment process. Newly developed treatment technologies seemed able to decompose PFCs completely but unsuitable for application in WWTP. Therefore, granular activated carbon (GAC) adsorption and ultra violet (UV) photolysis were developed in chapter V and VI as removal and degradation processes respectively. Fifteen kinds of PFCs were included in this study, consisting of twelve kinds of perfluorocarboxylic acids (PFCAs) with 4~18 carbons and three kinds of perfluoroalkyl sulfonates (PFASs) with 4~8 carbons. An integral procedure was developed in chapter III to pretreat wastewater samples. LC-ESI-MS/MS was applied to quantify all PFCs in trace level. Pretreatment methods were optimized between C18 and WAX-SPE processes for aqueous samples, and between IPE, AD-WAX and ASE-WAX processes for particulate samples. Standard spiking experiments were regularly conducted for each wastewater sample to calculate recovery rate and control analytical quality. As the result, WAX-SPE showed better performance on samples with very high organics concentrations, and C18-SPE performed better for long-chained PFCs. ASE-WAX was proposed as the optimum method to pretreat particulate samples because of the simple and time saving operations. 9H-PFNA was used as internal standard to estimate matrix effect in wastewater. Behavior of PFCs in a municipal WWTP has been studied in chapter IV by periodical surveys for six times in half a year. All PFCs used in this study were detected in WWTP influent and effluent. According to their carbon chain lengths, all PFCs can be classified into “Medium”, “Long” and “Short” patterns to simplify behavior analysis. PFCs in same pattern showed similar properties and behavior in wastewater treatment facilities. Very high concentrations of PFCs existed in WWTP influent, indicating some point sources of industrial discharge in this area. “Medium” PFCs, such as PFOA(8), PFNA(9) and PFOS(8), were primary contaminants in the WWTP and poorly removed by overall process. Performances of individual facilities were estimated for removal of each PFC. Primary clarification and secondary clarification were helpful to remove all PFCs in both aqueous phase and particulate phase. “Medium” PFCs in aqueous phase were increased after activated sludge process, but other PFCs can be effectively removed. Ozone seemed ineffective to decompose PFCs because of the strong stability of PFC molecules. Sand filtration and biological activated carbon (BAC) filtration in this WWTP can not remove PFCs effectively too, which required further studies. Performances of combined processes were estimated by integrating individual facilities along the wastewater flow. Activated sludge process coupled with clarifiers showed satisfied removal of most PFCs in the investigated WWTP except “Medium” PFCs. Adsorption characteristics of PFCs onto GAC have been studied by batch experiments in chapter V. Freundlich equation and homogenous surface diffusion model (HSDM) were applied to interpret experimental data. Isothermal and kinetics experiments implied that PFC adsorption on GAC was directly related with their carbon chain lengths. By ascendant carbon chain length, adsorption capacity for specific PFC was increased, and diffusion coefficient (Ds) was decreased. Ds of GAC adsorption was also decreased gradually in smaller GAC diameters. Coexisted natural organic matters (NOMs) reduced adsorption capacities by mechanism of competition and carbon fouling. Carbon fouling was found reducing adsorption capacity much more intensively than competition by organics. Acidic bulk solution was slightly helpful for adsorption of PFCs. However adsorption velocity or kinetics was not affected by NOM and pH significantly. GAC from Wako Company showed the best performance among four kinds of GACs, and Filtra 400 from Calgon Company was considered more suitable to removal all PFCs among the commercial GACs. Preliminary RSSCT and SBA results implied that background organics broke through fixed GAC bed much earlier than trace level of PFCs. Medium-chained PFCs can be effectively removed by fixed bed filtration without concerning biological processes. Direct photolysis process has been developed in chapter VI to decompose PFCAs in river water. Irradiation at UV254 nm and UV254+185 nm can both degrade PFCAs. Stepwise decomposition mechanism of PFCAs was confirmed by mass spectra analysis, and consecutive kinetics was proposed to simulate experimental data. PFASs can also be degraded by UV254+185 photolysis, although the products have not been identified yet. Coexisted NOMs reduced performance of UV photolysis for PFCAs by competition for UV photons. Sample volume or irradiation intensity showed significant influence on degradation of PFCAs. Local river water polluted by PFOA can be cleaned up by UV254+185 photolysis effectively. Ozone-related processes were also studied but ineffective to degrade PFC molecules. However, PFCs could be removed in aeration flow by another mechanism.
京都大学
0048
新制・課程博士
博士(工学)
甲第13340号
工博第2837号
新制||工||1417(附属図書館)
UT51-2007-M963
京都大学大学院工学研究科都市環境工学専攻
(主査)教授 田中 宏明, 教授 藤井 滋穂, 教授 伊藤 禎彦
学位規則第4条第1項該当
Doctor of Engineering
Kyoto University
DFAM
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Pereira, Claudia Mota Santos. "Comportamento de sistemas pós-filtros adsorvedores na remoção de compostos orgânicos precursores e subprodutos da desinfecção." Universidade de São Paulo, 2009. http://www.teses.usp.br/teses/disponiveis/3/3147/tde-14102009-104609/.
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O presente trabalho teve como objetivo avaliar a eficiência de pós-filtros adsorvedores constituídos de Carvão Ativado Granular (CAG) na remoção de compostos orgânicos precursores e na formação de subprodutos da desinfecção, em particular dos trialometanos (THM) na Estação de Tratamento de Água Alto da Boa Vista (ETA ABV), abastecida por reservatórios de água bruta com elevado grau de eutrofização. Os ensaios foram conduzidos em ETA Piloto composta por tanque de reservação de água filtrada, ozonizador, tanque de reservação de água ozonizada e 4 pós-filtros adsorvedores, sendo duas unidades dotadas de CAG de origem mineral e duas unidades dotadas de CAG de origem vegetal. Os filtros foram operados em paralelo, sendo que duas colunas foram alimentadas com água filtrada da ETA ABV (Filtro F3 CAG de origem mineral e Filtro F4 CAG de origem vegetal) e as outras duas alimentadas com água filtrada e ozonizada (Filtro F1 CAG de origem mineral e Filtro F2 CAG de origem vegetal). A avaliação da remoção de compostos orgânicos precursores e formação de subprodutos da desinfecção foi feita através de análises de carbono orgânico total (COT), UV-254 nm e formação de THM. A análise dos resultados gerados de julho de 2007 a dezembro de 2008 permitiu concluir que 93% do THM é formado nas primeiras 24 horas de contato da amostra com o cloro, simulando a pós cloração e pós alcalinização da ETA ABV. O processo de oxidação por ozônio não foi efetivo na remoção de THM instantâneo, visto que a média dos 38 valores de THM instantâneo para a água filtrada (17,8 ± 5,6 g/L) foi igual a média obtida para o THM instantâneo na água ozonizada. A remoção de THM pelos filtros de CAG foi mais significativa nos primeiros três meses de operação do sistema, apresentando remoção de 80% para os filtros com CAG de origem mineral e 70% para os filtros com CAG de origem vegetal, a partir do quarto mês de operação do sistema a remoção de THM caiu para um valor médio de 34%, o que mostra uma iminente saturação do leito adsorvedor. Os pós-filtros adsorvedores constituídos de CAG de origem mineral apresentaram melhor comportamento com respeito a remoção de THM e COT quando comparado com os pós-filtros dotados de CAG de origem vegetal.The main purpose of this work was to evaluate the performance of a Granular Activated Carbon (GAC) post-filter adsorbers in the removal of organic precursors and in the formation of disinfection byproducts, especially trihalomethanes (THM) in Alto da Boa Vista Water Treatment Plant (ABV WTP), which takes raw water from a highly eutrophized reservoirs. The tests was conducted on a Pilot WTP composed of filtered water tank, ozonator, ozonized water tank, and four post-filter adsorbers: two units with mineral GAC media and two units with vegetal GAC media. The filters were operated in parallel, with two columns fed with filtered water from ABV WTP (F3 Filter mineral GAC and F4 Filter vegetal GAC) and the other fed with ozonized water (F1 Filter mineral GAC and F2 Filter vegetal GAC). The evaluation of the removal of organic precursors and the formation of disinfection byproducts was made through analysis of Total Organic Carbon (TOC), UV-254 nm and THM formation. The results generated from July 2007 to December 2008 showed that 93% of THM is formed in the first 24 hours of contact with the chlorine in the sample, simulating the post chlorination and post alkalinization of ABV WTP in samples of filtered water, ozonized water, and post-filter adsorbers effluent. Ozone oxidation process was not effective in removing THM. Was found the same instantaneous THM values in the filtered water (17.8 g/L± 5.6 g/L) and in the ozonized water. During the first three months of post-filter adsorber operation, THM removal efficiencies were around 80% for F1 and F3 (mineral GAC media) and around 70% for F2 and F4 (vegetal GAC media). After four months of operation, THM removal efficiencies decreased to 34% average value, thus indicative of GAC saturation. Regarding THM and TOC removal efficacy, the mineral GAC performed better than the vegetal GAC.
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Skoglund, Oskar. "Evaluation of bark material and granulated active carbon for treatment of perfluoroalkyl substances (PFASs) in wastewater." Thesis, Uppsala universitet, Institutionen för geovetenskaper, 2017. http://urn.kb.se/resolve?urn=urn:nbn:se:uu:diva-317453.
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Per- and polyfluoroalkyl substances (PFASs) are a group of artificial chemicals which have been used in a wide area of applications such as surface protection agents in cloths and different industrial applications. It has been found that PFASs are potentially toxic and are frequently found in the environment due to their persistent and mobile properties. Effluents from wastewater treatment plants (WWTPs) have been identified as an important point source of PFASs. Bark, by-product from the paper and wood industry, is a low-cost adsorbent and has the potential to be used as a filter material for PFASs in WWTPs. In this study, the removal of PFASs in wastewater has been investigated using granulated active carbon (GAC) (n = 2) and bark (n = 2) in a pilot scale experiment at Kungsängsverket, Uppsala over a period of five weeks. The specific objects included: i) investigate the influence of flow-rate (10, 30 40 and 60 Ld-1 ) on the removal efficiency of PFASs in the GAC and bark filters, ii) investigate the influence of particle size of bark on the removal efficiency of PFASs and iii) establish what circumstances that potentially promotes removal of PFASs in GAC and bark filters. The results showed that GAC was the most effective method compared to bark, with a reduction of 73-93%, with increasing efficiency under low flow (10-30 L d-1 ) conditions. The removal efficiency of bark was 45% with a particle size of 2-5 mm and under low flow conditions (10-30 L d-1 ), while under high flow conditions (60 L d-1 ) with the same particle size the removal of PFASs was not efficient, instead the total PFAS concentration increased with 40%. In contrast, bark with a particle size of 5-7 mm proved to be not efficient in removing PFASs (removal efficiency = 0%). In general, the removal efficiency increased with smaller particle size of the adsorbent and lower flow rate. The results indicate that bark may be a low-cost alternative in reducing PFASs from wastewater, under certain conditions.Per- och polyfluroalkyla ämnen (PFAS) är en familj av artificiella fluorerade organiska föreningar som har använts sedan 1950-talet i en rad olika applikationer, såsom impregnering i kläder. Studier har visat att PFAS är potentiellt toxiska och att de förekommer globalt på grund av deras persistenta och mobila egenskaper. Spillvatten från avloppsreningsverk etablerats som en betydande källa för PFAS. Bark, vilket är en biprodukt från pappers- och träindustrin, är ett poröst material vilket möjligen kan användas som adsorbent av PFAS. Denna studie har jämfört effektiviteten hos granulerat aktivt kol (GAC) och bark för att minska PFAS i avloppsvatten. Experimentet var utformat som ett småskaligt kolonn-experiment vid Kungsängsängsverket, Uppsala, och pågick under en fem veckors period. Frågeställningen var att i) studera vilka effekter flödes-hastigheten (10, 30, 40 och 60 L d-1 ) har på reduktionen av PFAS hos GAC och barkfiltren, ii) studera vilka effekter partikelstorleken hos bark har på reduktion av PFAS och iii) redogöra vilka förhållanden som potentiellt gynnar reduktionen av PFAS i GAC och bark filtren. Resultaten visade att GAC var det mest effektiva av de två materialen, med en total reduktion på 73- 93% av PFAS, med ökande effektivitet under låga flödesförhållanden (10-30 L d-1 ). Bark minskade den totala mängden av PFAS med 45% då partikelstorleken var 2-5 mm och under låga flödesförhållanden (10-30 L d-1 ) medan bark med samma partikelstorlek under ökade flödesförhållanden (60 L d-1 ) visade en ökning på 40% av PFAS i det utgående vattnet. Bark med en partikelstorlek på 5-7 mm visade ingen reduktion av PFAS. Generellt visade resultaten att reduktionen av PFAS ökar under låga flödesförhållanden och minskad partikelstorlek. Resultaten visade att bark kan vara ett alternativt material för att minska PFAS i avloppsvatten förutsatt att gynnsamma förhållanden upprätthålls.
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Villars, Kathryn E. Villars. "Removal of Microcystin-LR from Drinking Water Using Granular Activated Carbon." The Ohio State University, 2018. http://rave.ohiolink.edu/etdc/view?acc_num=osu1532007603377473.
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Battrum, M. J. "Gas separation by adsorption." Thesis, University of Bath, 1987. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.376289.
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Becer, Metin Özkan Fehime S. "Gas adsorption in volumetric system/." [s.l.]: [s.n.], 2003. http://library.iyte.edu.tr/tezler/master/kimyamuh/T000256.rar.
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Chlendi, Mohamed. "Séparation de gaz par adsorption modulée en pression." Vandoeuvre-les-Nancy, INPL, 1993. http://www.theses.fr/1993INPL048N.
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L'objet de ce travail est la conception, l'étude et le dimensionnement d'opérations multicolonnes et multiadsorbants. Le travail présenté est surtout de nature méthodologique: il s'agit de développer et de tester des nouveaux outils et des nouvelles méthodes ayant un caractère assez géneral. Néanmoins, l'ensemble de cette étude s'appuiera sur une application proposée par le partenaire industriel de cette recherche: il s'agit de la production d'hydrogène pur par adsorption modulée en pression (PSA), à partir de gaz de cracking du gaz naturel. On a développé les modèles mathématiques utilisés pour simuler le procédé PSA ainsi que les méthodes de résolution adéquates. La description du logiciel de simulation PSASIM et ses différentes fonctionnalités sont illustrées par un exemple de procédé à 6 étapes et 2 colonnes. On a utilise PSASIM pour déterminer la longueur des couches d'adsorbant et la durée des étapes isobares. La caractérisation du fonctionnement global d'un procédé PSA est développée dans le dernier chapitre. On spécifie les différents critères de performance à étudier ainsi que les paramètres influents. On y développe deux démarches: plan d'expériences et réseau de neurones, qui conduisent à des polynômes ou des procédures simples donnant les performances en fonction des paramètres opératoires
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Heslop, Mark J. "Binary gas adsorption in molecular sieves." Thesis, Loughborough University, 1993. https://dspace.lboro.ac.uk/2134/6861.
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This thesis is concerned with the development of sorption-effect chromatography as a rapid method for the determination of binary gas-mixture adsorption isotherms.There are many alternative non-chromatographic methods but these have inherent disadvantages the direct experimental methods require excessive equilibration times and the predictive methods require the respective pure-component isotherms and an ideal adsorbed phase. A computer simulation has shown that for an alternative chromatographic method, good results will only be obtained if both binary isotherms are close to linear. Sorption-effect chromatography is characterised by the flowrate retention time (TN) which measures the change in column inventory when a perturbation is made to the system. Along with the standard composition retention time (Tx), this extra measurement allows the gradient of each binary isotherm to be evaluated. Subsequent integration will give the respective mixture isotherm. Three gas systems (nitrogen-argon, nitrogen-helium and argon-helium) have been investigated over zeolite 5A at different temperatures. The results confirm that the adsorbed phase amounts decrease, with increasing temperature and that there are degrees of component interaction. Experimentally, thermal fluctuations in the oven will cause noise on the flowrate record making TN determination difficult. Isolation of the column from direct air flow was seen to reduce the noise level. Also, using a computer simulation model, the heat of adsorption for the above zeolite 5A systems will be easily dissipated preventing any unwanted gas temperature rises; the comparatively small column diameter was found to be a significant factor. The employment of delay lines (empty tubes) in various locations has been investigated. To directly determine TN it is necessary to used delay lines downstream of the column. Also, the chromatographic method has been extended to determine mixture isotherms by considering the change in average column pressure rather than the motion of a composition front through the column. Delay lines situated upstream of the column are able to separate these two effects, and preliminary results are satisfactory. However, the use of delay lines anywhere in the system changes the measured retention times and the theory has to be adjusted to account for this.
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Wagner, Jeffrey A. "Gas adsorption on carbon nanohorn aggregates /." Available to subscribers only, 2008. http://proquest.umi.com/pqdweb?did=1594488041&sid=5&Fmt=2&clientId=1509&RQT=309&VName=PQD.
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Apolonatos, Georgia. "Gas adsorption with molecular sieve zeolites." Thesis, University of Ottawa (Canada), 1990. http://hdl.handle.net/10393/5907.
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Adsorption kinetics and equilibrium of CH$\sb4$, CO and N$\sb2$ gases were studied on various molecular sieve zeolites. Ethylyne was also tested, yet was found to be incompatible with the molecular sieves under consideration. The gas chromatographic technique was chosen as the method of studying the adsorption by which equilibrium and kinetic parameters are derived by matching the response peak to appropriate mathematical models. It was found that the synthetic zeolites (H-Mordenite, 4A zeolite, 5A zeolite) rather than naturally occurring Chabazite had a higher capacity for the adsorption of all three gases. Pure and binary gas isotherms of CH$\sb4$ and CO with molecular sieve 5A were also studied for the separation of these gases. These isotherms indicated that under the present conditions CO is preferentially adsorbed on the 5A zeolite and the adsorption capacity of the sieve increases with decreased temperature.
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Navaei, Milad. "Quartz crystal microbalance adsorption apparatus for high pressure gas adsorption measurements in nanomaterials." Thesis, Georgia Institute of Technology, 2011. http://hdl.handle.net/1853/41057.
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The primary objective of this study was to develop a sensitive and cost-effective sorption system to analyze adsorption and diffusion of different gases on micro porous materials and nanotubes. A high pressure Quartz Crystal Microbalance (QCM) based adsorption apparatus for single-component gas was developed. A QCM is an acoustic-wave resonator in which the acoustic wave propagates through the crystal. Therefore, it is highly responsive to addition or removal of small amounts of mass adsorbed or deposited on the surface of the crystal. This mass sensitivity makes the QCM an ideal tool for the study of gas adsorption. The QCM-based adsorption apparatus is advantageous over the commercialized none-gravimetric and gravimetric equipment in a way that it is low-cost, highly sensitive and accurate for mass sorption applications, satisfactorily stable in a controlled environment, and can be used for thin films.
The high pressure apparatus was calibrated using Matrimid 5218, whose thermodynamic properties and adsorption parameters are known. The Matrimid was spin-coated onto a 14 mm-diameter QCM, and sorption equilibrium data for were obtained for CO₂ gas at 25, 30, 48, and 52 ºC and partial pressure range between 0 to 4 bar. In order to compare the experimental data with available literature data, the experimental data was fitted into a dual-mode adsorption model. The model results from Henry's law and a Langmuir mechanism. Comparison of the experimental adsorption isotherm of Matrimide for CO₂ gas with literature data showed reasonable agreement between the experimental and literature data.
In this study, the adsorption parameters of aluminosilicate nanotubes are observed. Aluminosilicate nanotubes are ideal materials for chemical sensing, molecule separation, and gas storage; hence, there is a need for adsorption and diffusion data on this material.
The adsorption of CO₂, N₂, and CH₄ gases on aluminosilicate nanotubes samples has been studied in the temperature range of 20° to 120° Celsius and pressure range of 0 to 8 bar. The experimental results yield the CO₂ and N₂ heat of adsorptions of -32.9 and -28.1 kJ/mol respectively.
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Hart, J. "Separation of gases by adsorption." Thesis, University of Bath, 1987. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.234617.
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Wiersum, Andrew. "Developing a strategy to evaluate the potential of new porous materials for the separation of gases by adsorption." Thesis, Aix-Marseille, 2012. http://www.theses.fr/2012AIXM4817/document.
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Les Metal-Organic Framework (MOF) sont des adsorbants très prometteurs pour la séparation des gaz. Formés de centres métalliques reliés par des ligands organiques, ces matériaux présentent une structure organisée avec des pores de taille contrôlée ainsi que des surfaces et des volumes poreux très élevées. La possibilité de faire varier à la fois le centre métallique et le ligand organique donne aux MOFs une très grande diversité qu'on ne retrouve pas chez les zéolithes et les charbons actifs.L'objectif de cette étude a été d'évaluer le potentiel des MOFs en tant qu'adsorbants pour quatre procédés de séparation de gaz. En raison du grand nombre de MOFs disponibles, il a été nécessaire d'élaborer une stratégie pour identifier les matériaux les plus prometteurs dans chaque cas. Cette méthodologie comprend quatre étapes : une étape de criblage, une étape expérimentale, une étape de calcul et une étape d'évaluation.Pour l'étape de criblage, un nouvel appareil dit « à haut débit » a été développé pour mesurer des isothermes approximatives. Ensuite, un certain nombre de matériaux ont été retenus pour faire une étude plus approfondie de leurs propriétés d'adsorption. Des isothermes très précises ont été mesurées par gravimétrie tandis que les enthalpies d'adsorption ont été obtenues par microcalorimétrie. Dans l'étape de calcul, le modèle IAST a été utilisée pour prédire les sélectivités à partir des données en gaz pur. Enfin, les adsorbants ont été classés à l'aide d'un nouveau paramètre de sélection qui regroupe la sélectivité, la capacité efficace et l'enthalpie d'adsorption, où l'importance de chacun des paramètres peut être ajustée en fonction des besoins du procédéMetal-Organic Frameworks (MOFs) are seen to be one of the most promising classes of adsorbents for gas separations. Consisting of metal clusters connected by organic linkers to form a fully crystalline network, these materials have record breaking surface areas and pore volumes as well as a wide variety of pore structures and sizes. This, coupled with the possibility to use virtually any transition metal as well as functionalized linkers, gives MOFs the chemical and physical versatility often lacking in traditional adsorbents such as zeolites and activated carbons.The purpose of this study was to evaluate the potential of MOFs as adsorbents for four gas separations of interest to the petrochemical industry. Because of the diversity and number of MOFs available, a methodology was needed to help identify the most promising materials in each case. The proposed methodology comprises four stages: a screening step, an experimental step, a computational step and finally an evaluation step. For the first stage, a high-throughput setup was developed to measure rough adsorption isotherms. A number of materials were then selected for a more thorough investigation of their adsorption properties. Highly accurate isotherms were measured gravimetrically while precise adsorption enthalpies were obtained by microcalorimetry. Step three involved predicting the co-adsorption behaviour from the pure gas isotherms using the Ideal Adsorbed Solution Theory. Finally, the adsorbents were ranked based on a new selection parameter regrouping selectivity, working capacity and adsorption enthalpy where the importance of each term can be adjusted depending on the requirements of the process
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Tian, Jian Atwood J. L. "Molecular organic solids for gas adsorption and solid-gas interaction." Diss., Columbia, Mo. : University of Missouri--Columbia, 2009. http://hdl.handle.net/10355/6882.
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Title from PDF of title page (University of Missouri--Columbia, viewed on Feb 24, 2010). The entire thesis text is included in the research.pdf file; the official abstract appears in the short.pdf file; a non-technical public abstract appears in the public.pdf file. Dissertation advisor: Dr. Jerry L. Atwood. Vita. Includes bibliographical references.
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Newby, Ruth. "Gas adsorption studies in metal-organic frameworks." Thesis, University of Nottingham, 2016. http://eprints.nottingham.ac.uk/32287/.
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This thesis describes the synthesis of a novel highly stable metal-organic framework, NOTT-300(Cr), as well as the synthesis of three new mixed metal analogues of NOTT-300 using different compositions of aluminium and chromium. These new MOFs were used in gas sorption experiments to investigate potential selectivity and uses for gas stream separations with particular focus on CO2 and C2 hydrocarbons. The gas adsorption properties of NOTT-300(Al) for CO2 and C2 hydrocarbons are also investigated in detail. Chapter 1 – An introduction to MOFs, including their synthesis and various applications along with examples from the literature is discussed. The potential application of MOFs for difficult industrial separations is considered and a brief background on CO2 and climate change is discussed along with the current issues facing carbon capture technologies. The uses of C2 hydrocarbons and their difficult separation are also assessed. Chapter 2 – A novel Cr(III) containing analogue of NOTT-300 has been successfully synthesised (NOTT-300(Cr)) and the structure solved from the PXRD pattern. The gas adsorption properties, with specific focus on CO2 uptake and selectivity, are described and compared with those obtained for NOTT 300(Al). The CO2 adsorption in NOTT-300(Cr) was further probed using ¬in situ¬ gas loaded PXRD studies. Flow experiments were used along with IAST calculations to assess and compare the CO2/CH4 and CO2/N2 selectivity in NOTT-300(Cr) and compared with NOTT-300(Al). Although the CO2 adsorption capacity is higher for NOTT-300(Cr) than for NOTT 300(Al) (10.1 vs. 9.5 mmol g-1 at 273 K and 20 bar), the CO2 selectivity is lower due to an increased adsorption capacity for other gases such as CH4. Chapter 3 – A mixed metal NOTT-300 series containing varying amounts of Al and Cr, i.e. NOTT-300(AlCr2:1), NOTT-300(AlCr1:1) and NOTT 300(AlCr2:3), was synthesised in order to further probe the effect of the metal content on the CO2 adsorption and selectivity of this framework. Each of the materials show high CO2 adsorption capacity, however, there appears to be no specific trend in adsorption properties with respect to metal ratio. The CO2 adsorption and selectivity in NOTT 300(AlCr2:1) was further investigated using dual component adsorption isotherms and in situ gas loaded PXRD and IR studies. The three different OH groups present in the mixed metal materials form interactions of differing strength with the CO2 molecules, explaining the different adsorption properties across the series. The mixed metal series displays higher CO2 adsorption than NOTT-300(Al), but lower CO2 selectivity. When compared to NOTT 300(Cr) the CO2 adsorption of the heterometallic series is lower but the selectivities are comparable. Chapter 4 – The adsorption of C2 hydrocarbons and possible C2 separations and C2/C1 separations are investigated and compared in the NOTT-300 materials described in this thesis. All frameworks display considerably higher adsorption capacity for C2 hydrocarbons vs. CH4. However, the potential for C2 separations was more varied, with NOTT-300(AlCr1:1) showing moderate C2H4/C2H6 selectivity (2.7:1), while the calculated selectivity for NOTT 300(Cr) was negligible (1:1). NOTT-300(Al) was used in breakthrough experiments to assess the separation capability of two different hydrocarbon mixtures (C2H2/C2H4 and C2H4/C2H6).
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Xiong, Fengyang. "Desorption and Adsorption of Subsurface Shale Gas." The Ohio State University, 2020. http://rave.ohiolink.edu/etdc/view?acc_num=osu1591975402482308.
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Mohammad, Hasan Abid Urf Turabe Ali. "Ammonia gas adsorption on metal oxide nanoparticles." Thesis, Kansas State University, 2011. http://hdl.handle.net/2097/13094.
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Master of ScienceDepartment of Mechanical and Nuclear Engineering
Steven J. Eckels
NanoActiveTM metal oxide particles have the ability to destructively adsorb organophosphorus compounds and chlorocarbons. These nanomaterials with unique surface morphologies are subjected to separate, low concentrations of gaseous ammonia in air. NanoActiveTM materials based on magnesium oxide have large specific surface areas and defective sites that enhance surface reactivity and consequently improved adsorptivity. In gas contaminant removal by adsorption, presence of vast specific surface area is essential for effective gas-solid interaction to take place. This is also the case in many industrial and chemical applications such as purification of gases, separation and recovery of gases, catalysis etc,. Typically carbonaceous compounds are utilized and engineered in toxic gas control systems. The purpose of this study was to compare NanoActiveTM materials with carbon based compounds in the effectivity of toxic gas adsorption at low concentrations. A test facility was designed to investigate the adsorption properties of novel materials such as adorption capacity and adsorption rate. Adsorption capacity along with adsorption kinetics is a function of properties of the adsorbent and the adsorbate as well as experimental conditions. Nanomaterials were placed on a silica matrix and tested with increasing flow rates. Electrochemical sensing devices were placed at inlet and outlet of the facility to monitor real time continuous concentration profiles. Breakthrough curves were obtained from the packed bed column experiments and saturation limits of adsorbents were measured. Adsorption rates were obtained from the breakthrough curves using modified Wheeler-Jonas equation. The NanoActiveTM materials adsorbed ammonia though to a lesser extent than the Norit® compounds. This study also included measurement of pressure drop in packed beds. This information is useful in estimating energy losses in packed bed reactors. Brauner Emmet Teller tests were carried out for the calculation of surface area, pore volume and pore size of materials. These calculations suggest surface area alone had no notable influence on adsorption capacity and adsorption rates. This lead to the conclusion that adsorption was insignificant cause of absence of functional groups with affinity towards ammonia. In brief, adsorption of ammonia is possible on NanoActiveTM materials. However functional groups such as oxy-flouro compounds should be doped with novel materials to enhance the surface interactions.
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Ortiz, Cancino Olga. "Etude expérimentale de l'adsorption du méthane dans des gaz de schistes colombiens et de la séparation méthane/dioxyde de carbone." Thesis, Pau, 2018. http://www.theses.fr/2018PAUU3002/document.
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Dans cette thèse, nous avons développé 3 travaux principaux dans lesquels le phénomène d'adsorption joue un rôle prédominant.Selon le BP Statistical Review, le ratio réserves/production de la Colombie est proche de 12 et actuellement, toute la production de gaz naturel provient des réserves conventionnelles; para ailleurs, les réserves non conventionnelles de gaz techniquement récupérables sont 12 fois plus élevées que les conventionnelles. La plupart d’entre elles sont situées dans le Middle Magdalena Valley bassin (MMV). Dans ce contexte, nous avons mesuré la capacité d'adsorption du CH4 sur 5 échantillons obtenus de 3 forages exploratoires situés dans le MMV. Les mesures ont été réalisées à 50 et 75°C et pour pressures jusqu'à 3.5MPa. Les caractérisations géochimiques et structurales ont été réalisées à l'Université Autonome de Madrid. L'effet du carbone organique total (TOC), de la maturité thermique, de la teneur en argile et de la surface spécifique (SSA) sur la capacité d'adsorption du CH4 ont été étudiées. Les résultats montrent que la température a un effet négatif sur la capacité d'adsorption, et le TOC a un effet positif. Aucune corrélation n'a été observée entre la teneur en argile et la capacité d'adsorption normalisée en TOC par rapport au CH4, ce qui indique que les minéraux argileux ne contribuent pas significativement à l'adsorption du CH4 dans nos échantillons. De plus, il n'y a pas de tendance générale entre le TOC normalisé et la maturité thermique. Parmi les facteurs étudiés le TOC a la contribution majeure à la capacité d'adsorption. Une contribution similaire est trouvée pour la SSA, ce qui est cohérent, compte tenu de la corrélation positive entre le TOC et la SSA. Cet ensemble de données représente des informations significatives pour les estimations indirectes du gaz en place au cours des futures stratégies de récupération. Cette étude approfondit les projets en cours sur la compréhension de l'effet d'adsorption sur la production et l'évaluation du gaz de schiste de la Colombie. En plus, nous avons réalisé une étude sur l'adsorption sélective de CH4/CO2 sur un gaz de schiste, précédemment caractérisé. La capacité d'adsorption et l'enthalpie du CO2 et du CH4 à 50°C et pour pressions jusqu'à 3.2MPa ont été mesurées. De plus, les isothermes d'adsorption du mélange équimolaire CH4/CO2 ont été réalisées jusqu'à 2MPa à 50°C. Les résultats montrent que le CO2 est préférentiellement adsorbé par rapport au CH4, tant à l'état pur que dans le mélange équimolaire. La sélectivité estimée CO2/CH4 met en évidence une affinité significative du CO2 avec le kérogène de cet échantillon. Ces résultats sont d'un grand intérêt d'un point de vue industriel, car ils signifient que ce schiste pourrait être candidat à l'injection du CO2 comme méthode de récupération assistée et pour le stockage du CO2 quand il était épuisé.Enfin, sachant que les impacts environnementaux et sociétaux de la séparation et de la capture du CO2, nous avons exploré la séparation du CO2 d'un mélange équimolaire CH4/CO2 en utilisant des adsorbants de nanoparticules de silice (natives et fonctionnalisées avec des amines) développés à l'Université de Vigo. Nous avons mesurée la capacité d'adsorption et l'enthalpie du CO2 et du CH4 à 50°C et des pressions jusqu'à 3MPa et la capacité d'adsorption d'un mélange équimolaire CH4/CO2 à 50°C et jusqu'à 2MPa dans les deux séries de nanoparticules. Les résultats ont montré une adsorption préférentielle du CO2 sur le CH4, mais l'adsorption du CO2 est plus faible dans les particules natives que dans les particules fonctionnalisées. Cependant, les particules natives sont prometteuses pour la capture du CO2. La valeur de la sélectivité du CO2 par rapport au CH4 est presque identique pour les deux échantillons, cela signifie que le processus de fonctionnalisation n'a pas amélioré la performance des particules dans ce cas. Ces résultats obtenus sur la silice native ouvrent des perspectives et une ligne de travailIn this dissertation we developed three main works in which adsorption phenomenon play a predominant role.According to the BP Statistical Review, Colombia’s reserves/production ratio is close to 12 and currently all the natural gas production comes from conventional reserves; meanwhile its unconventional technically recoverable gas reserves are about twelve times greater than conventional ones. Most of them are located in the Middle Magdalena Valley Sedimentary Basin (MMV). In this context we measured the methane adsorption capacity on five shale core samples obtained during exploratory drilling from three boreholes located in the MMV. The experiments were carried out at 50 and 75°C and for pressure ranging up to 3.5 MPa under dry conditions. The geochemical and structural characterizations were carried out in the Department of Geology of the Universidad Autonoma de Madrid. The effect of total organic carbon (TOC), thermal maturity, clay content and specific surface area (SSA) on methane adsorption capacity was studied. The results shows that the temperature has a negative effect on the adsorption capacity, while TOC has a positive effect, even if no linear regression was found between TOC and methane adsorption capacity. No correlation was observed between the clay content and the TOC-normalized adsorption capacity to methane, which indicates that clay minerals do not significantly contribute to methane adsorption in the case of our samples. In addition, there is not a general trend between TOC normalized and thermal maturity. Among the factors investigated in the present study, TOC has the major contribution to the adsorption uptake. A similar contribution is found for the SSA, which is consistent, considering the positive correlation between TOC and SSA. This set of data represents meaningful information for indirect estimations of the gas in place during the future recovery strategies. And maybe the most important, this study furthers the ongoing projects on the understanding of the adsorption effect on shale gas production and assessment.In addition to this work, we made a study on selective CH4/CO2 adsorption on a shale gas, which was previously characterized. The adsorption capacity and enthalpy of CO2 and CH4 pure at 50°C and for pressures up to 3.2 MPa were measured. Additionally, the equimolar mixture methane/carbon dioxide adsorption isotherms was performed up to 2 MPa at the same temperature. The results show that CO2 is preferentially adsorbed than methane, both in pure state as in the mixture. The estimated selectivity CO2/CH4 highlights a significant affinity of CO2 with the kerogen of this sample. These results are of great interest from an industrial point of view, because they mean that this shale could be a candidate for CO2 injection as recovery method; and for CO2 storage when it was depleted. Finally, having into account that separation and capture of CO2 have environmental connotations, we explored the separation of CO2 from an equimolar CH4/CO2 mixture using adsorbents of silica nanoparticles (natives and functionalized with amines) developed in the University of Vigo. We measured the adsorption capacity and enthalpy of CO2 and CH4 at 50°C and pressures up to 3MPa and the equimolar CH4/CO2 adsorption capacity at the same temperature and up to 2 MPa in both set of nanoparticles. The results showed that there is a preferential adsorption to CO2 over CH4 (in pure state and in the mixture), but CO2 adsorption is lower in native particles than in functionalized ones. However native particles are promising for CO2 capture. The value of selectivity of CO2 over CH4 is almost the same for both samples, it means that the functionalization process did not improve the performance of the particles in this case. This kind of works has a lot of perspective for the future
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Zone, Ian Robert. "Dynamics and control of a pressure swing adsorption process." Thesis, University of Surrey, 1998. http://epubs.surrey.ac.uk/762/.
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Hommeril, François. "Etude théorique et expérimentale de la coadsorption sur surface homogène : cas du mélange (Kr, CH4) sur Graphite et MgO." Vandoeuvre-les-Nancy, INPL, 1991. http://docnum.univ-lorraine.fr/public/INPL_T_1991_HOMMERIL_F.pdf.
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Les données thermodynamiques du mouillage tridimensionnel, appliquées à l'adsorption, considéré comme un phénomène de mouillage bidimensionnel, permettent de schématiser simplement le comportement d'une couche mixte adsorbée. Il apparait que la condensation et le déplacements d'un gaz dans un alliage binaire adsorbé dépendent des potentiels chimiques des phases gazeuses à l'équilibre avec les constituants du mélange et des conditions de condensation des mêmes corps mais en phase pure. La résolution d'un modèle thermodynamique statistique s'appuyant sur l'approximation de Bregg-Williams et la simulation numérique de la coadsorption par la méthode de monte Carlo confirment et affinent ce phénomène. On montre notamment que plus l'affinité électrostatique entre les gaz est forte, plus la lacune de miscibilité est étendue. L'etude expérimentale, menée sur les systèmes Krypton-Méthane adsorbés sur graphite exfolié et MgO, a permis, en confirmant les différents résultats des modèles, de mettre en évidence quelques points remarquables. Ainsi, sur le graphite, l'augmentation de la pression partielle en méthane, induit-elle la démission d'une phase liquide dans un alliage solide constitue du melange krypton-methane. C'est la rétro-fusion bidimensionnelle. Sur le MgO, la nature des phases reste mal définie, mais il a été montré que la solution bidimensionnelle formée s'écarte notablement de l'idéalité
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Jordi, Robin Guy. "Batch frequency response techniques in gas phase adsorption applications /." [St. Lucia, Qld.], 2001. http://www.library.uq.edu.au/pdfserve.php?image=thesisabs/absthe16290.pdf.
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Rees, G. J. "Interfacial adsorption in a gas-liquid chromatographic system." Thesis, Swansea University, 1991. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.638636.
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Chromatographic retention due to adsorption at the liquid/gas and liquid/solid interfaces is possible in gas-liquid chromatographic (GLC) systems, especially with polar solutes from a non-polar stationary phase. The variation of retention volumes with sample size at 60oC on several series of columns, using different support materials, was studied for di iso-propyl ether (DIPE), a polar solute, on squalane, a non-polar stationary phase. Isolation of the total adsorption contributions to retention was then performed using a semi-empirical curve fitting procedure devised by Mathiasson and Jonsson. The adsorption retentions at infinite dilution on a fully wetted porous silica support (Porasil F) was extrapolated to zero loading where the gas/liquid interfacial area (Ax) approaches the value of the support surface area (As). As was measured using the BET nitrogen adsorption method, and the sum of the support/liquid and vapour/liquid adsorption coefficients was obtained. The solid/liquid interfacial adsorption coefficient, Ks, was estimated from adsorption liquid chromatographic parameters, and was found to be small in comparison with the gas/liquid interfacial adsorption coefficient, Kx. The variation with liquid loading of the adsorption contribution to retention on two silanised supports (Chromosorb P-AW DMCS and HMDS treated Porasil F) was studied. The gas liquid interfacial area at high loading was found to be small in comparison with that of untreated Porasil F, and comparable with values obtained by other workers. At squalane loadings where a wetting transition is postulated on the silanised support, the magnitude of Ax approaches that of the unsilanised support, and helps confirm the model for the wetting transition proposed by Conder and coworkers.
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Armstrong, Jayne. "Gas adsorption and separation properties of porous material." Thesis, University of Newcastle upon Tyne, 2013. http://hdl.handle.net/10443/2119.
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The development of new porous materials for use in applications such as gas storage and separation processes, catalysis, catalysts supports and the removal of environmentally unfriendly species has increased rapidly over the past decade. Research into the development of these new materials has been dominated by metal organic frameworks, covalent organic frameworks, nanoporous polymers and, most recently, porous organic cage molecules. This thesis describes adsorption studies of a metal organic framework, Zn (TBAPy) and a porous tetrahedral organic cage molecule of ~ 1 nm diameter formed by the condensation reaction of 1,3,5- triformylbenzene with 1,2-ethylenediamine. The development of metal organic frameworks has traditionally involved the formation of rigid network structures, analogous to that of zeolites. More recently the focus has shifted to those of dynamic, flexible framework materials, and the response of these materials to adsorption of gases and vapours. The metal organic framework Zn (TBAPy) is based on a zinc metal centre functionalised with benzoate fragments. The initial two-dimensional structure undergoes rearrangement of the paddlewheel units to form a 3D framework, Zn (TBAPy)' upon desolvation. The ability of this 3D network to separate p-xylene and m-xylene was investigated. It was found that these isomers produced different effects on the framework, with p-xylene producing a typical Type I isotherm, whereas m-xylene induced a structural change within the material, with a much slower rate of m-xylene adsorption at higher pressures. This could potentially lead to the equilibrium separation of these two isomers by the metal organic framework Zn (TBAPy)'. The 1 nm diameter tetrahedral cage molecules formed by the condensation reaction of 1,3,5-triformylbenzene with 1,2-ethylenediamine can exist in a number of stable polymorphs, Cage 1α, Cage 1β and Cage 1γ. These polymorphs can be interconverted by exposure to certain organic vapours/solvents. The conversion of Cage 1β to Cage 1α by adsorption of probe molecules ethyl acetate, 2-butanone, diethyl ether, pentane and methanol was studied. Adsorption of ethyl acetate, 2- butanone and diethyl ether produced unusual adsorption isotherms, which included desorption of adsorbed vapour with increasing pressure during the adsorption isotherms. This desorption is attributed to the structural change from Cage 1β to Cage 1α. The unusual desorption step is not observed for methanol or pentane adsorption. The adsorption of methyl acetate was studied over a wide temperature range in order to assess the thermodynamic and kinetic characteristics of the unusual desorption step. The adsorption of dichloromethane showed the reverse transformation of Cage 1α to Cage 1β, showing that the inter conversion produces stable polymorphs. The kinetics of the structural transformation followed an Avrami model and the mechanism is an activated process. Cage 1α has voids between the cages, which are connected by very narrow constrictions that allow the kinetic molecular sieving of oxygen, carbon dioxide and nitrogen. It was found that oxygen adsorbs approximately ten times faster than nitrogen on Cage 1α, with selectivity and rate constants similar to those observed for carbon molecular sieves. The thermodynamics and kinetic results are discussed in terms of structural characteristics and diffusion into molecular cage materials. The kinetic molecular sieving is not present in the polymorph Cage 1β, which has wider pores.
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Mutasim, Z. Z. "Separation of gas mixtures by pressure swing adsorption." Thesis, Swansea University, 1987. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.379811.
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Ma, Shengqian. "Gas Adsorption Applications of Porous Metal-Organic Frameworks." Miami University / OhioLINK, 2008. http://rave.ohiolink.edu/etdc/view?acc_num=miami1209411394.
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Kabir, Hocine. "Adsorption de mélanges de gaz en lit fixe, modulée en température et en pression : expérience, modélisation, simulations." Vandoeuvre-les-Nancy, INPL, 1993. http://www.theses.fr/1993INPL139N.
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Cette étude concerne les procédés d'adsorption de gaz pour lesquels la régénération de l'adsorbant est effectuée principalement par augmentation de la température. Les adsorbants sont des tamis moléculaires et les gaz utilisés expérimentalement sont essentiellement des alcanes et du dioxyde de carbone. En vue de modéliser de tels procédés, on effectue une description détaillée des différents phénomènes impliqués. Ainsi, on propose des modèles thermodynamiques pour décrire les équilibres multiconstituants gaz-solide à partir de mesures des isothermes des gaz purs ou de mesures de perturbations chromatographiques, ainsi que les méthodes expérimentales associées. On considère que le transfert de matière gaz-solide est représenté par une diffusion interne au grain uniquement. Le transfert de chaleur est étudié tant au niveau du grain d'adsorbant qu'au niveau de la colonne pour laquelle on envisage les trois cas : isotherme, adiabatique et intermédiaire. On étudie également le cas d'un mélange contenant un gaz condensable. La résolution numérique des équations conduit à un logiciel de simulation. Les simulations réalisées permettent d'explorer l'influence des paramètres opératoires sur l'histoire des concentrations en sortie de colonne, en saturation et en régénération, notamment l'influence du transfert de matière, du transfert de chaleur gaz-adsorbant, des pertes de chaleur a la paroi, de la température du gaz de régénération dans le cas d'une espèce condensable.
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Caja, Monique. "Adsorption du gaz naturel sur les charbons en conditions anhydres et saturées en eau : Etude des quantités adsorbées et du fractionnement isotopique." Aix-Marseille 2, 2000. http://www.theses.fr/2000AIX22019.
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Liow, Daniel Ann Keng. "The modelling of diffusion controlled Pressure Wing Adsorption." Thesis, University of Surrey, 1992. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.332279.
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Uner, Murat. "Adsorption Calorimetry In Supported Catalyst Characterization: Adsorption Structure Sensitivity On Pt/y-al2o3." Master's thesis, METU, 2004. http://etd.lib.metu.edu.tr/upload/2/12605511/index.pdf.
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In this study, the structure sensitivity of hydrogen, oxygen and carbon monoxide adsorption was investigated by changing the metal particle size of Pt/Al2O3 catalysts. 2 % Pt/Al2O3 catalysts were prepared by incipient wetness methodthe particle size of the catalysts was manipulated by calcining at different temperatures. The dispersion values for the catalysts calcined in air at 683K, 773K and 823K were measured as 0.62, 0.20 and 0.03 respectively. The differential heats of adsorption of hydrogen, carbon monoxide and oxygen were measured using a SETARAM C80 Tian-Calvet calorimeter. No structure dependency was observed for hydrogen, carbon monoxide or oxygen initial heats of adsorption. The adsorbate:metal stoichiometries at saturation systematically decreased with increasing particle size. Hydrogen chemisorption sites with low and intermediate heats were lost when the particle size increased. On the other hand, oxygen and carbon monoxide initial heats and adsorption site energy distributions did not change appreciably with the metal particle size.
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Huang, Liangliang. "Computational Study of Toxic Gas Removal by Reactive Adsorption." Thesis, North Carolina State University, 2013. http://pqdtopen.proquest.com/#viewpdf?dispub=3538542.
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Growing concerns about the environment and terrorist attacks prompt a search for effective adsorbents for removal of small molecule toxic gases, such as ammonia and hydrogen sulfide, under ambient conditions in the presence of moisture, where physical adsorption is not adequate. We use graphene oxide and CuBTC metal-organic framework as the adsorbents to explore toxic gas removal by reactive adsorption. Using ab initio density functional theory, atomistic reactive molecular dynamics and Monte Carlo simulation strategies, theoretical understanding of the underlying reaction and adsorption mechanisms of ammonia and hydrogen sulfide on graphene oxide and CuBTC metal-organic framework have been gained.
The ab initio calculation results show that ammonia and hydrogen sulfide decompose on carboxyl and epoxy functional groups and vacancy defects of graphene oxide. The existence of water molecules substantially reduces the adsorption/dissociation of ammonia or hydrogen sulfide on graphene oxide because the water molecules either form hydrogen bonds with the functional groups or adsorb more easily on the vacancy defects. Reactive molecular dynamics calculations by the ReaxFF method have been performed to propose realistic graphene oxide models for theoretical calculations. We also use reactive molecular dynamics simulation to study the thermal and hydrostatic stabilities of the CuBTC metal-organic framework and its application for ammonia removal. We predict the collapse temperature for CuBTC crystal structure and observe the partial collapse of CuBTC at lower temperatures upon ammonia adsorption. The results agree well with experiment data and provide insights on the reaction mechanism involved in such an ammonia removal process.
The research in this thesis can provide fundamental understanding, at the electronic and atomistic levels, of the roles of surface defects and functionalities for reactive adsorption of toxic gas molecules. In addition to developing experimental and theoretical algorithms to design effective adsorbents, the results are expected to find applications in air cleaning, energy storage, fuel cell technology and other scientific challenges where the separation of reactive molecules is involved.
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Chihara, Kazuyuki, Yosuke Kaneko, Takuya Terakado, and Hisashi Mizuochi. "Diffusion in multicomponent gas adsorption on MSC5A, chromatographic study." Universitätsbibliothek Leipzig, 2016. http://nbn-resolving.de/urn:nbn:de:bsz:15-qucosa-194787.
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Mangel, Astrid. "Gas adsorption and neutron scattering studies of chromatographic supports." Thesis, University of Exeter, 1994. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.239391.
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Chihara, Kazuyuki, Yosuke Kaneko, Takuya Terakado, and Hisashi Mizuochi. "Diffusion in multicomponent gas adsorption on MSC5A, chromatographic study." Diffusion fundamentals 3 (2015) 16, S. 1-4, 2005. https://ul.qucosa.de/id/qucosa%3A14304.
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Savage, Mathew. "Gas adsorption and binding properties of metal organic frameworks." Thesis, University of Nottingham, 2016. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.716474.
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This thesis describes the design, synthesis and extensive characterisation of adsorbate gas interactions of two porous Metal Organic Framework materials, constructed from the organic ligand molecule 3,3’,5,5’-biphenyl tetracarboxylic acid, and Bi111 and In111" ions respectively. Chapter 1 forms a general introduction to the global problems posed by the decrease of fossil fuel reserves, increase of pollution, and global warming, the structural and properties of MOFs, and the role they play within these fields. Particular attention is given to the determination of the nature of the binding interactions of gas molecules of interest within these materials, with the aim of designing future materials with improved properties. Chapter 2 presents the first highly porous MOF synthesised from the heavy Bi111 metal ion and investigates the density, porosity and gas adsorption properties of this material. Insight into the packing and binding of gas molecules within this material are gained by computational investigations. Chapter 3 discusses an In111 MOF, isostructural to NOTT-300 (Al), and the adsorption of the fuel gases H2 and CH4 within this material. The stepwise binding positions of these gases within this material are determined by Neutron Powder Diffraction experiments and the methane binding interactions with this material are studied computationally and by Inelastic Neutron Scattering. Chapter 4 investigates the flue gas sorption and separation properties of NOTT-300 (In) by studying the N2, CO2 and SO2 adsorption, selectivity and binding interactions of this material. The binding positions of CO2 and SO2 within NOTT-300 (In) are determined by single crystal and powder X-Ray diffraction respectively, and the framework interactions and separation properties studied by infrared spectroscopy. Interactions of N2, CO2 and SO2 with this material are further investigated by INS spectroscopy.
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Valente, Inês Alexandra Manata Antunes. "Adsorption equilibria of flue gas components on activated carbon." Master's thesis, Faculdade de Ciências e Tecnologia, 2014. http://hdl.handle.net/10362/12168.
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Marcus, Patrick. "Entwicklung und Validierung eines Labor-Schnelltests zur Beurteilung der Adsorbierbarkeit von organischen Einzelstoffen an Aktivkohle." Doctoral thesis, Saechsische Landesbibliothek- Staats- und Universitaetsbibliothek Dresden, 2005. http://nbn-resolving.de/urn:nbn:de:swb:14-1133172373836-74002.
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Zur Entfernung von anthropogenen organischen Spurenstoffen werden bei der Wasseraufbereitung sehr oft Aktivkohle-Festbettadsorber eingesetzt. Dabei konkurrieren die organischen Einzelstoffe während des Adsorptionsprozesses mit dem adsorbierbaren Anteil der natürlichen Wasserinhaltsstoffe um die aktiven Zentren der Aktivkohle. Durch dieses Konkurrenzverhalten ist es sehr schwierig, für einen zu untersuchenden organischen Einzelstoff seine Entfernbarkeit mittels Aktivkohle abzuschätzen. Gleichzeitig werden der Liste der aus dem Wasser zu entfernenden Substanzen ständig neue Stoffe hinzugefügt. Deshalb wäre es wünschenswert, eine schnelle, einfache und kostengünstige Methode zu haben, mit der unter wasserwerksnahen Bedingungen die Entfernbarkeit eines organischen Einzelstoffs bei der Aktivkohlefiltration in einem Großfilter bestimmt werden kann. Da die bisher entwickelten Methoden nicht in der Lage sind, all diese Vorgaben zu erfüllen, sollte im Rahmen dieser Arbeit eine neue Methode zur Beurteilung der Entfernbarkeit organischer Einzelstoffe mittels Aktivkohlefiltration entwickelt werden. Es wurde ein Aktivkohle-Kleinfiltertest konzipiert und aufgebaut, der eine Einstufung von organischen Substanzen, die auf den Rückhaltepotenzialen von Aktivkohlefiltern basiert, ermöglichen soll. Um die Einstufung nach Sontheimer in trinkwasserrelevante und nicht-trinkwasserrelevante Substanzen vornehmen zu können, wurde ein spezielles Bewertungskonzept entwickelt, das auf die Aktivkohle-Kleinfiltertest-Durchbruchskurven der verschiedenen organischen Einzelstoffe angewendet werden kann. Da der Kleinfiltertest einfach und kostengünstig durchzuführen sein sollte, wurde bei der Auslegung des gesamten Versuchaufbaus darauf geachtet, dass nur Zukaufteile oder Teile verwendet wurden, die sich aus Glas fertigen ließen. Die Versuchsparameter wurden so gewählt, dass die Versuchsvorbereitung und -durchführung nicht zu zeit- und arbeitsintensiv ist. Als Standard für die Versuchsdurchführung wurde eine handelsübliche und in der Wasseraufbereitung weitverbreitete Kohlesorte (F 300) und als Matrix Leitungswasser verwendet. Die Filterzulaufkonzentration des organischen Einzelstoffs wurde auf 500 µg/l festgelegt. Durch verschiedene Vorversuche konnte gezeigt werden, dass der Aktivkohle-Kleinfilter die kinetischen Vorgaben erfüllt und es zu keinen unerwünschten Effekten wie Kanalbildung oder Randeinflüssen kommt. Die Validierung der neu entwickelten Versuchsmethode ergab, dass die Kleinfilter-Durchbruchskurven von Substanzen, deren Entfernbarkeit in Aktivkohlefiltern von Wasserwerken bekannt ist (1,1,1-Trichlorethan, EDTA, Trichlorethen, Atrazin, Isoproturon), plausibel sind. Die Durchbruchsreihenfolge und der Durchbruchsbeginn der einzelnen Substanzen im Kleinfilter waren identisch mit denen in einem Großfilter. Zudem war die Trennschärfe des Kleinfilters für die schlecht (1,1,1-Trichlorethan und EDTA), mäßig (Trichlorethen) und gut (Atrazin und Isoproturon) zu entfernenden Substanzen ausreichend, so dass eine Einstufung in Entfernbarkeitsklassen ohne Probleme vorgenommen werden konnte. Um die organischen Einzelstoffe aufgrund der mit dem Kleinfiltertest aufgenommenen Durchbruchskurven einstufen zu können, musste ein Kriterium für die Trinkwasserrelevanz nach Sontheimer gefunden werden, das sich direkt aus den Durchbruchskurven ableiten lässt. Es bot sich an, eine bestimmte Ablaufkonzentration, die nach einer bestimmten Versuchslaufzeit erreicht wird, als Kriterium festzulegen. Durch die Durchbruchskurven der Stoffe, die bei der Validierung des Kleinfiltertests zum Einsatz kamen, wurde das Kriterium bei einem 10%igen Durchbruch nach 15000 BVT festgelegt. Mit Hilfe des Bewertungskonzepts wurden verschiedene organische Einzelstoffe, deren Entfernbarkeit in einem Wasserwerks-Aktivkohleadsorber nicht oder nur unzureichend bekannt war, anhand der jeweiligen Kleinfilter-Durchbruchskurven eingestuft (MTBE, ETBE, Amidotrizoesäure, Iopamidol).
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Mariano, Antonio Lorenzo. "Étude ab initio de matériaux avec spin crossover pour des applications dans l'adsorption de gaz." Thesis, Université Grenoble Alpes, 2021. http://www.theses.fr/2021GRALI035.
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Malgré de nombreux efforts en faveur de l'utilisation des énergies renouvelables, les combustibles fossiles continuent de dominer la production énergétique mondiale, ce qui entraîne des émissions importantes de gaz à effet de serre dans l'atmosphère.L'utilisation d'adsorbants solides très poreux et chimiquement accordables, tels que les cadres métallo-organiques (MOF), a suscité beaucoup d'intérêt au cours des 20 dernières années en raison de leur application potentielle dans les technologies de séparation des gaz et de capture du carbone. Dans ce travail, nous proposons de concevoir par calcul des MOFs dont la haute affinité pour les molécules invitées peut être modifiée par traitement thermique. Avec un choix approprié de ligands et de centres métalliques, les MOF présentant un croisement de spin induit thermiquement (SCO) et un changement concomitant des propriétés d'adsorption peuvent être développés pour éventuellement produire une capture et une libération de gaz plus efficaces sur le plan énergétique.D'un point de vue informatique, le défi de la simulation du phénomène de SCO en utilisant des méthodes de structure électronique ab initio est représenté par l'évaluation de la thermodynamique du SCO. Pour résoudre ce problème, nous développons un schéma basé sur la DFT+U pour obtenir une description précise des différences d'énergie à l'état de spin dans les complexes de Fe(II). Une évaluation critique de l'approche Hubbard U dans la description de l'énergie à l'état de spin est présentée et les résultats de cette analyse sont utilisés pour proposer une manière pratique et efficace de les surmonter. Cette approche, qui est testée et validée par rapport aux expériences et aux résultats de CASPT2/CC, est ensuite utilisée pour proposer la preuve de concept in silico du SCO-MOF induit par la température pour une libération efficace du gazThe use of highly porous, chemically tunable solid adsorbents such as metal-organic frameworks (MOFs) has attracted much interest in the past 20 years for their potential application in gas separation and carbon capture technologies. In this work, we propose to computationally design MOFs whose high affinity for guest molecules can be modified under temperature treatment. With a suitable choice of ligands and metal centers, MOFs exhibiting a thermally-induced spin crossover (SCO) and a concomitant change in the adsorption properties can be developed to possibly yield more energy-efficient gas capture-and-release.From a computational point of view, the challenge in simulating the SCO phenomenon using textit{ab initio} electronic structure methods is represented by the evaluation of the thermodynamics of SCO. To address this issue, we develop a DFT+U-based scheme to achieve an accurate description of spin-state energy differences in Fe(II) complexes. A critical assessment of the Hubbard U approach in the description of spin-state energetics is presented and insights from this analysis are used to propose a practical and efficient way to overcome them. This approach, which is tested and validated against experiments and coupled cluster-corrected CASPT2 results, is then used to propose the proof-of-concept in silico of temperature-induced SCO-MOF for efficient gas release
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Bestfather, Chris. "Upgrading landfill gas to natural gas quality: Bulk separation by pressure swing adsorption." Thesis, University of Ottawa (Canada), 2009. http://hdl.handle.net/10393/28403.
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Equilibrium adsorption properties are studied on zeolites for the application of upgrading biogas from landfills. Pure adsorption isotherms of carbon dioxide (CO2) and methane (CH4) measured with a constant volume apparatus. The Henry's Law constant and the heat of adsorption for NaLSX is also determined. The adiabatic working capacity and selectivity of four adsorbents is compared. NaLSX showed the highest capacity for CO2 at elevated temperatures.
The binary equilibrium of CO2/CH4 on NaLSX is measured in a modified gas chromatograph at total mixture pressures of 1 and 3.3 atmospheres. The adsorbed phase is dominated by CO2 with a selectivity of 20 to 100 for the separation of CO2 and CH4. The increase in total pressure resulted in an increase in adsorbent capacity and a decrease in selectivity. Finally, an economic analysis relates landfill size to PSA operational costs and returns.
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Chihara, Kazuyuki, Hidenori Nakamura, and Yosuke Kaneko. "Diffusion study of multi-component gas adsorption in MSC5A by chromatographic method: Diffusion study of multi-component gas adsorption in MSC5Aby chromatographic method." Diffusion fundamentals 6 (2007) 57, S. 1-2, 2007. https://ul.qucosa.de/id/qucosa%3A14236.
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Sangster, J. A. "Adsorption and electrosorption studies with activated charcoal cloth." Thesis, Liverpool John Moores University, 1988. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.233600.
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Karra, Jagadeswarareddy. "Development of porous metal-organic frameworks for gas adsorption applications." Diss., Georgia Institute of Technology, 2011. http://hdl.handle.net/1853/45751.
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Metal-organic frameworks are a new class of porous materials that have potential applications in gas storage, separations, catalysis, sensors, non-linear optics, displays and electroluminescent devices. They are synthesized in a "building-block" approach by self-assembly of metal or metal-oxide vertices interconnected by rigid linker molecules. The highly ordered nature of MOF materials and the ability to tailor the framework's chemical functionality by modifying the organic ligands give the materials great potential for high efficiency adsorbents. In particular, MOFs that selectively adsorb CO₂ over N₂, and CH₄ are very important because they have the potential to reduce carbon emissions from coal-fired power plants and substantially diminish the cost of natural gas production. Despite their importance, MOFs that show high selective gas adsorption behavior are not so common.
Development of MOFs for gas adsorption applications has been hindered by the lack of fundamental understanding of the interactions between the host-guest systems. Knowledge of how adsorbates bind to the material, and if so where and through which interaction, as well as how different species in adsorbed mixture compete and interact with the adsorption sites is a prerequisite for considering MOFs for adsorptive gas separation applications. In this work, we seek to understand the role of structural features (such as pore sizes, open metal site, functionalized ligands, pore volume, electrostatics) on the adsorptive separation of CO₂, CO and N₂ in prototype MOFs with the help of molecular modeling studies (GCMC simulations). Our simulation results suggest that the suitable MOFs for CO₂ adsorption and separation should have small size, open metal site, or large pore volume with functionalized groups.
Some of the experimental challenges in the MOF based adsorbents for CO₂ capture include designing MOFs with smaller pores with/without open metal sites. Constructing such type of porous MOFs can lead to greater CO₂ capacities and adsorption selectivities over mixtures of CH₄ or N₂. Therefore, in the second project, we focused on design and development of small pore MOFs with/without open metal sites for adsorptive separation of carbon dioxide from binary mixtures of methane and nitrogen. We have synthesized and characterized several new MOFs (single ligand and mixed ligand MOFs) using different characterization techniques like single-crystal X-ray diffraction, powder X-ray diffraction, TGA, BET, gravimetric adsorption and examined their applicability in CO₂/N₂ and CO₂/CH₄ mixture separations. Our findings from this study suggest that further, rational development of new MOF compounds for CO₂ capture applications should focus on enriching open metal sites, increasing the pore volume, and minimizing the size of large pores.
Flue gas streams and natural gas streams containing CO₂ are often saturated by water and its presence greatly reduces the CO₂ adsorption capacities and selectivities. So, in the third project, we investigated the structural stability of the developed MOFs by measuring water vapor adsorption isotherms on them at different humid conditions to understand which type of coordination environment in MOFs can resist humid environments. The results of this study suggest that MOFs connected through nitrogen-bearing ligands show greater water stability than materials constructed solely through carboxylic acid groups.
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Krause, Simon [Verfasser]. "Negative Gas Adsorption of Flexible Metal-Organic Frameworks / Simon Krause." München : Verlag Dr. Hut, 2019. http://d-nb.info/1219178330/34.
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Hunt, Joseph Ray. "Synthesis, characterization, and gas adsorption properties of covalent organic frameworks." Diss., Restricted to subscribing institutions, 2009. http://proquest.umi.com/pqdweb?did=1779835631&sid=1&Fmt=2&clientId=1564&RQT=309&VName=PQD.
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Chen, Linjiang. "Molecular simulations studies of gas adsorption in metal-organic frameworks." Thesis, University of Edinburgh, 2014. http://hdl.handle.net/1842/9366.
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Using computational tools ranging from molecular simulations – including both Monte Carlo and molecular dynamics methods – to quantum mechanical (QM) calculations (primarily at density functional theory (DFT) level), this work focuses on addressing some of the challenges faced in molecular simulations of gas adsorption in metal–organic frameworks (MOFs). This work consists of two themes: one concerns gas adsorption in MOFs with coordinatively unsaturated metal sites (cus’s), and the other one deals with predicting and understanding the breathing behaviour of the flexible MOF MIL-53(Sc). It has been shown experimentally that incorporation of cus’s – also known as “open” metal sites or unsaturated metal centres – into MOFs significantly enhances the uptake of certain gases such as CO2 and CH4. As a result of the considerably enhanced, localized guest-molecule interactions with the cus’s, it, however, remains a challenge to predict correctly adsorption isotherms and/or mechanisms in MOFs with cus’s using grand-canonical Monte Carlo (GCMC) simulations based on generic classical force fields. To address this problem, two multi-scale modelling approaches – which combine GCMC simulations with QM calculations – have been proposed in this work. The first approach is based on the direct implementation of a fluid–framework potential energy surface, calculated by a hybrid DFT/ab initio method, in the GCMC simulations. The second approach involves parameterization of ab initio force fields for GCMC simulations of gas adsorption in MOFs with cus’s. This approach focuses on the generation of accurate ab initio reference data, selection of semiempirical model potentials, and force-field fitting through a multi-objective genetic algorithm approach. The multi-scale simulation strategy not only yields adsorption isotherms in very good agreement with experimental data but also correctly captures adsorption mechanisms, including the adsorption on the cus’s, observed experimentally but absent from GCMC simulations based on generic force fields. The second challenge that this work aims to address concerns the “breathing” phenomenon of MOFs, in which the framework structure adapts its pore opening to accommodate guest molecules, for example. The breathing effect gives rise to some exceptional properties of these MOFs and hence promising applications. However, framework flexibility often poses a challenge for computational studies of such MOFs, because suitable flexible force fields for frameworks are lacking and the effort involved in developing a new one is no less a challenge. Here, an alternative to the force-field-based approach is adopted. Ab initio molecular dynamics (AIMD) simulations – which combine classical molecular dynamics simulations with electronic-structure calculations “on the fly” – have been deployed to study structural changes of the breathing MOF MIL-53(Sc) in response to changes in temperature over the range 100–623 K and adsorption of CO2 at 0–0.9 bar at 196 K. AIMD simulations employing dispersion-corrected DFT accurately simulated the experimentally observed closure of MIL-53(Sc) upon solvent removal and the transition of the empty MOF from the closed-pore phase to the very-narrow-pore phase with increasing temperature. AIMD simulations were also used to mimic the CO2 adsorption of MIL-53(Sc) in silico by allowing the MIL-53(Sc) framework to evolve freely in response to CO2 loadings corresponding to the two steps in the experimental adsorption isotherm. The resulting structures enabled the structure determination of the two CO2-containing intermediate and large-pore phases observed by experimental synchrotron X-ray diffraction studies with increasing CO2 pressure; this would not have been possible for the intermediate structure via conventional methods because of diffraction peak broadening. Furthermore, the strong and anisotropic peak broadening observed for the intermediate structure could be explained in terms of fluctuations of the framework predicted by the AIMD simulations. Fundamental insights from the molecular-level interactions further revealed the origin of the breathing of MIL-53(Sc) upon temperature variation and CO2 adsorption. Both the multi-scale simulation strategy for gas adsorption in MOFs with cus’s and the AIMD study of the stimuli-responsive breathing behaviour of MIL-53(Sc) illustrate the power and promise of combining molecular simulations with quantum mechanical calculations for the prediction and understanding of MOFs.
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Narayan, Shankar B. "Measurement of diffusion and adsorption in porous adsorbents." Thesis, McGill University, 1985. http://digitool.Library.McGill.CA:80/R/?func=dbin-jump-full&object_id=73968.
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