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Binyamin, Gary Neil. "Glucose electro-oxidizing biofuel cell anodes /." Digital version:, 2000. http://wwwlib.umi.com/cr/utexas/fullcit?p9992752.
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Satheesh, Srejith. "Fabrication and Validation of a Nano Engineered Glucose Powered Biofuel Cell." Thesis, KTH, Material- och nanofysik, 2014. http://urn.kb.se/resolve?urn=urn:nbn:se:kth:diva-162116.
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Fuel Cells are important forms of sustainable power generation and Biofuel Cells utilize the use of bio-compatible/biodegradable molecules as fuels. Glucose is an ideal candidate to serve this purpose. In this project, a Glucose Fuel Cell (GFC) has been fabricated using the nanomaterials developed in the lab. The skeletal system of this GFC is a three-layered structure; a Membrane Electrode Assembly (MEA) composed of carbon electrodes (anode and cathode) and a Poly Vinyl Alcohol/Poly Acrylic Acid (PVA/PAA) polymer electrolyte. Gold and Silver (Au and Ag) nanoparticles are utilized as catalyst on the anode and cathode respectively, which are prepared by the use of green chemistry practice. One of the GFC has been compacted under hot press and the other non-hot pressed. ,which led to different surface areas. For the validation of the GFC stacks, the glucose concentration was selected around biologically available levels, i.e at 400 mg/dL in both the cases. One trial on hot pressed membrane with 200 mg/dL of glucose is also studied. Short Circuit Current (SCC) and Open Circuit Voltage (OCV) were measured following which the voltages and currents were measured across load resistances. The Thermal Gravimetric Analysis (TGA) and Differential Scanning Calorimetry (DSC) studies were carried out on the membrane while the electrodes were characterized by Scanning Electron Microscopy (SEM). UV-Vis studies were carried out on the Au and Ag nanoparticle suspension before and after impregnation of carbon cloth electrodes. Inductively Coupled Plasma Optical Emission Spectrometer (ICP-OES) has been utilized to estimate the concentration and thus the number of nanoparticles adsorbed on the surface of the carbon cloth. The variations of output current with the thickness of the membranes were studied. The assembly containing the catalytic particles showed power levels ranging between 128.7 nW-332.2 nW in the glucose concentration of 400 mg/dL. Rigorous efforts are under process to scale down the power consumption of electronics to extremely low levels. GFCs could be used as power generators in such devices. The inexpensiveness of the fuel is a remarkable factor.
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Zhu, Ziwei [Verfasser]. "Making glucose oxidase fir for biofuel cell applications by directed protein evolution / Ziwei Zhu." Bremen : IRC-Library, Information Resource Center der Jacobs University Bremen, 2008. http://d-nb.info/1034891898/34.
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Campbell, Alan S. "Enzymatic Biosensor and Biofuel Cell Development Using Carbon Nanomaterials and Polymer-Based Protein Engineering." Research Showcase @ CMU, 2017. http://repository.cmu.edu/dissertations/859.
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The development of enzymatic biosensors and enzymatic biofuel cells (EBFCs) has been a significant area of research for decades. Enzymatic catalysis can provide for specific, reliable sensing of target analytes as well as the continuous generation of power from physiologically present fuels. However, the broad implementation of enzyme-based devices is still limited by low operational/storage stabilities and insufficient power densities. Approaches to improving upon these limitations have focused on the optimization of enzyme activity and electron transfer kinetics at enzyme-functionalized electrodes. Currently, such optimization can be performed through enzyme structural engineering, improvement of enzyme immobilization methodologies, and fabrication of advantageous electrode materials to enhance retained enzyme activity density at the electrode surface and electron transfer rates between enzymes and an electrode. In this work, varying electrode materials were studied to produce an increased understanding on the impacts of material properties on resulting biochemical, and electrochemical performances upon enzyme immobilization and an additional method of electroactive enzyme-based optimization was developed through the use of polymer-based protein engineering (PBPE). First, graphene/single-wall carbon nanotube cogels were studied as supports for membrane- and mediator-free EBFCs. The high available specific surface area and porosity of these materials allowed the rechargeable generation of a power density within one order of magnitude of the highest performing glucose-based EBFCs to date. Second, two additional carbon nanomaterial-based electrode materials were fabricated and examined as EBFC electrodes. Graphene-coated single-wall carbon nanotube gels and gold nanoparticle/multi-wall carbon nanotube-coated polyacrylonitrile fiber paddles were utilized as electroactive enzyme supports. The performance comparison of these three materials provided an increased understanding of the impact of material properties such as pore size, specific surface area and material surface curvature on enzyme biochemical and electrochemical characteristics upon immobilization. Third, PBPE techniques were applied to develop enzyme-redox polymer conjugates as a new platform for enzymatic biosensor and EBFC optimization. Poly(N-(3-dimethyl(ferrocenyl) methylammonium bromide)propyl acrylamide) (pFcAc) was grown directly from the surface of glucose oxidase (GOX) through atom-transfer radical polymerization. Utilization of the synthesized GOX-pFcAc conjugates led to a 24-fold increase in current generation efficiency and a 4-fold increase in EBFC power density compared to native GOX. GOX-pFcAc conjugates were further examined as working catalysts in carbon paper-based enzymatic biosensors, which provided reliable and selective glucose sensitivities and allowed a systematic analysis of sources of instability in enzyme-polymer conjugate-based biosensors and EBFCs. The knowledge gained through these studies and the in-depth characterization of an additional layer of optimization capacity using PBPE could potentially enhance the progress of enzymatic biosensor and EBFC development.
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Abreu, Caroline. "Conception et optimisation de piles enzymatiques glucose-O2 pour la gestion de puissance." Thesis, Lyon, 2017. http://www.theses.fr/2017LYSEC052/document.
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Ce mémoire est consacré à l’optimisation de la connexion enzymatique pour l’oxydation du glucose et la réduction du dioxygène dans une matrice de nanotubes de carbone (CNTs) sous forme de compression dans les biopiles à glucose, et à l’assemblage de biopiles dans un système à flux. Dans un premier temps, le transfert électronique indirect de la glucose oxydase (GOx) et de la glucose déshydrogénase FAD-dépendante (FADGDH) est optimisé dans une matrice nanostructurée de CNTs contenant différents médiateurs rédox. Ces bioanodes ont pu être combinées avec des biocathodes similaires à bases d’enzymes à cuivre, la laccase (Lac) et la bilirubine oxydase (BOD). La biopile GOx-NQ/Lac présente une puissance de l’ordre de 150 µW sous 150 mmol.L-1 de glucose et la biopile GOx-NQ/BOD orientée par la PP IX, quant à elle, possède une puissance de l’ordre de 0,5 mW sous 5 mmol.L-1 de glucose. Cette biopile présente une très bonne alternative à l’implantable ou à l’alimentation d’un appareil électronique à faible demande énergétique. La partie suivante concerne l’élaboration d’un design de biopile à flux optimisant la diffusion du substrat à l’intérieur de la bioélectrode. De ce fait, plusieurs systèmes de biopiles GOx-NQ/BOD à flux de substrat ont été étudiés. La configuration de flux traversant a permis d’obtenir une puissance de l’ordre de 1 mW sous 5 mmol.L-1 de glucose et oxygène dissous. La possibilité d’utiliser cette pile en décharge continue ou en cycle de charge/décharge a été étudiée. Ce système de biopile à flux de glucose a permis également d’associer plusieurs biopiles en série ou en parallèle. Ainsi, l’alimentation d’un minuteur et d’un test d’ovulation a pu être réalisée à l’aide de biopiles associées en série. D’autre part, l’utilisation d’un circuit de gestion de l’énergie a permis d’alimenter un capteur de température en stockant l’énergie produite par deux biopiles connectées en série. Cette partie se consacre également à une biopile basée sur l’association de la HRP à la cathode et la GOx-NQ à l’anode. Ce système est très intéressant puisque grâce à la maitrise du sens du flux de notre substrat, le peroxyde d’hydrogène formé par l’anode peut être alors consommé par la cathode. Cette pile s’est montrée parfaitement opérationnelle en condition physiologique et a abouti à l’obtention de puissances de l’ordre de 0,8 mWThis work is devoted to the optimization of the enzymatic connection for the oxidation of glucose and the reduction of dioxygen in a matrix of carbon nanotubes (CNTs) in the form of compression in glucose biofuel cells, and the assembly of biofuel cells in a flow system.First, mediated electron transfer of glucose oxidase (GOx) and FAD-dependent glucose dehydrogenase (FADGDH) is optimized in a nanostructured CNTs matrix containing different redox mediators. These bioanodes could be combined with similar biocathodes with copper enzyme bases, laccase (Lac) and bilirubin oxidase (BOD). The GOx-NQ/Lac biofuel cell has a power of the order of 150 μW under 150 mmol L-1 of glucose and the biofuel cell GOx-NQ/BOD oriented by the PP IX, order of 0.5 mW under 5 mmol L-1 of glucose. This biofuel cell presents a very good alternative to the implantable or to the supply of an electronic device with low energy demand.The next part concerns the development of a biofuel cell design with flux optimizing the diffusion of the substrate inside the bioelectrode. As a result, several GOx-NQ/BOD flow systems have been studied. The flow-through configuration made it possible to obtain a power of the order of 1 mW under 5 mmol L-1 of glucose and dissolved oxygen. The possibility of using this battery in continuous discharge or in charge/discharge cycle has been studied. This biofuel cell system with a glucose flow has also made it possible to associate several biofuel cells in series or in parallel. Thus, the power supply of a timer and an ovulation test could be realised using associated biofuel cells in series. The use of an energy management circuit made it possible to supply a temperature sensor by storing the energy produced by two biofuel cells connected in series.Moreover, this part is about another biofuel cell based on the association of HRP with the cathode and the GOx-NQ at the anode. This system is very interesting because, thanks to the control of the flow direction of our substrate, the hydrogen peroxide formed by the anode can then be consumed by the cathode. This stack was perfectly operational in physiological condition and led to the achievement of powers of the order of 0.8 mW
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Sales, Fernanda Cristina Pena Ferreira. "Desenvolvimento de bioeletrodos miniaturizados para a aplicação em biocélulas a combustível implantáveis." Universidade de São Paulo, 2017. http://www.teses.usp.br/teses/disponiveis/75/75134/tde-15012018-180634/.
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As biocélulas a combustível enzimáticas (BFCs) são dispositivos eletroquímicos que convertem energia química em energia elétrica, utilizando enzimas como biocatalisadores. Quando miniaturizada, uma BFC pode ser implantada em animais vertebrados e invertebrados, vislumbrando-se sua utilização na produção de energia elétrica para alimentar microdispositivos biomédicos e microssensores em pequenos insetos. No entanto, ainda é um desafio obter BFCs implantáveis e miniaturizadas, com uma potência suficiente (dezenas de microwatts) para alimentar microcircuitos eletrônicos de maneira estável e em longo prazo. Diante do exposto, esta tese de doutorado apresenta um estudo das propriedades eletroquímicas de eletrodos enzimáticos, visando a aplicação em BFCs de glicose/O2 miniaturizadas e implantáveis. Para isso, utilizaram-se fibras flexíveis de carbono (FCFs) modificadas com as enzimas bilirrubina oxidase (BOx) no cátodo e glicose desidrogenase (GDh) NAD-dependente no ânodo, a fim de se obter a redução de O2 e a oxidação de glicose, respectivamente. Os resultados obtidos mostram que FCFs previamente submetidas a um tratamento químico de oxidação com permanganato de potássio e com posterior eletrodepolimerização do mediador vermelho neutro produzem bioânodos estáveis e robustos. Estes eletrodos, combinados com biocátodos compostos por FCFs na ausência de mediadores redox, foram utilizados em BFCs miniaturizadas, que foram implantadas em formigas da espécie Atta sexdens rubrupilosa. A potência máxima da BFC operando in vivo foi 13,5 ± 3,8 µW cm-2 em 190 ± 58,9 mV, com corrente máxima de 143 ± 40,2 µA cm-2 e a voltagem de circuito aberto de 260 ± 99,6 mV. Acredita-se que estes valores ainda possam ser otimizados e este trabalho contribui para mostrar que a flexibilidade das FFC, a presença de um mediador de elétrons polimérico no ânodo, o uso do tratamento químico de oxidação com permanganato de potássio das fibras e a miniaturização dos eletrodos são elementos importantes, e que podem ser considerados no desenvolvimento de biocélulas a combustível implantáveis.Enzymatic biofuel cells (BFCs) are electrochemical devices that convert chemical energy into electrical energy using enzymes as biocatalysts. When miniaturized, BFCs can be implanted in vertebrate and invertebrate animals and, their use to produce electrical energy to feed biomedical microdevices and micro-sensors in small insects can be observed. However, it is still challenging to obtain implantable and miniaturized BFCs, with sufficient power (tens of microwatts) to power electronic microcircuits in a stable and long-term manner. In view of the above, this PhD thesis presents a study of the electrochemical properties of enzymatic electrodes, aiming to use them in miniaturized and implantable glucose/O2 BFCs. In order to obtain a reduction in O2 and oxidation of glucose, flexible carbon fibers (FCFs) modified with bilirubin oxidase (BOx) enzymes in the cathode and glucose dehydrogenase (GDh) at the anode, respectively, were used. The results show that FCFs previously submitted to a chemical treatment of oxidation with potassium permanganate and, subsequently, electropolymerization of the neutral red mediator produce stable and robust bioanodes. These electrodes, combined with biocathodes consisting of FCFs in the absence of redox mediators, were used in miniaturized BFCs, which were implanted in Atta sexdens rubrupilosa ant species. The BFC maximum power source, operating in vivo, was 13.5 ± 3.8 μW cm-2 at 190 ± 58.9 mV, with a maximum current of 143 ± 40.2 μA cm-2 and the open circuit voltage was 260 ± 99.6 mV. Although these values can be optimized, this research shows that the flexibility of the FCF, the presence of a polymer electron mediator on the anode, using the chemical treatment of oxidation with potassium permanganate of the fibers and electrode miniaturization are important elements, which can be considered in the development of implantable biofuels.
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Anschau, Andréia 1983. "Lipid production by Lipomyces starkeyi = strategy to obtain high cell density using xylose and glucose = Produção de lipídeos por Lipomyces starkeyi : estratégia para obtenção de alta densidade celular a partir de xilose a glicose." [s.n.], 2014. http://repositorio.unicamp.br/jspui/handle/REPOSIP/266100.
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Orientador: Telma Teixeira FrancoTese (doutorado) - Universidade Estadual de Campinas, Faculdade de Engenharia Química
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Resumo: Neste trabalho foram desenvolvidos estudos visando o estabelecimento de um processo de produção de lipídeos microbianos a partir de fontes renováveis, particularmente xilose, carboidrato derivado do processo de hidrólise de bagaço de cana-de-açúcar. Foi utilizada a levedura oleaginosa Lipomyces starkeyi DSM 70296, previamente selecionada no Laboratório de Engenharia Bioquímica, Biorefino e Produtos de Origem Renovável (LEBBPOR). A partir dos resultados preliminares em frascos agitados, partiu-se para estudos de batelada alimentada em biorreator (1,3 a 3L). Foram estudadas diferentes estratégias de alimentação, sendo que em batelada alimentada repetida, foram encontradas as maiores concentrações de células (85,4 g/L) e de lipídeos (41,8 g/L). Posteriormente foram estudados modos de operação em processos contínuos em meio sintético e meio contento o hidrolisado hemicelulósico (H-H). As maiores produtividades de células (0,443 g/g) e de lipídeos (0,236 g/g) foram encontradas em cultivo contínuo a 0,03h-1. Na vazão específica de alimentação de 0,06 h-1 foram obtidas as maiores produtividades de células (0,600 g/L.h) e de lipídeos (0.288 g/L.h). Análises de cromatografia em fase gasosa dos diferentes cultivos feitos revelaram que os principais constituintes deste complexo são os ácidos graxos de cadeia longa, como o ácido palmítico (C16:0), ácido esteárico (C18:0), ácido oleico (C18:1) e ácido linoleico. Foi estimado o número de cetano em torno de 61, muito próximo do biodiesel de palma. Também foram feitos estudos de balanço de massa e de energia em cultivo batelada alimentada utilizando somente xilose como fonte de carbono. O valor de calor de combustão (Qc) de 25,7 kJ/g obtido após 142 h de cultivo representa aproximadamente 56% do conteúdo energético do óleo diesel (45,4 kJ/g), indicando o potencial da L. starkeyi para biodiesel. Cultivos contínuos subsequentes foram feitos para a compreensão do processo de acúmulo de lipídeos, utilizando a ferramenta estatística de reconciliação de dados para melhorar os dados experimentais obtidos em quimiostato, reduzindo os erros experimentais para posterior cálculo de análise de fluxos metabólicos (MFA). Nesse sentido, os lipídeos produzidos por L. starkeyi apresentam relevante importância do ponto de vista acadêmico e industrial, podendo ser utilizados como matéria-prima para biodiesel e indústria oleoquímica
Abstract: Studies attempting the establishment of a microbial lipid production process from renewable resources, mainly xylose, were developed. This pentose, obtained from sugar cane bagasse hydrolysis. The oleaginous yeast Lipomyces starkeyi DSM 70296, previously selected at the Laboratory of Biochemical Engineering, Biorefining and Products from Renewable Sources (LEBBPOR), was used throughout this thesis. After preliminary studies in shake flasks, we started fed-batch studies in fermentor (1.3 to 3L). Among the strategies studied, the highest cell mass and lipid concentrations reached up to 85.4 and 41.8 g/L, respectively, when repeated fed?batch strategy was applied. Subsequently, continuous processes were studied in synthetic medium and media containing hemicellulosic hydrolysate (H-H). The highest overall cell mass (0.443 g/g) and lipid yields (0.236 g/g) were achieved at dilution rate of 0.03 h-1. At dilution rate of 0.06 h-1, were obtained the highest productivities of cell mass (0.600 g/L.h) and lipids (0.288 g/L.h). Gas chromatography of esterified lipids revealed that the major constituents of this complex are long-chain fatty acids, such as palmitic acid (C16:0), stearic acid (C18:0), oleic acid (C18:1), and linoleic acid (C18:2) with an estimated cetane (around 61) very close to the palm biodiesel. Also have been studies of mass and energy balances from fed-batch cultivation using xylose as sole carbon source. The combustion heat (Qc) value 25.7 (kJ/g) obtained after 142 h of fed-batch cultivation, represents approximately 56% of the energy content of diesel oil (45.4 kJ/g), indicating the potential of L. starkeyi for biodiesel. Continuous cultures were made subsequently to understanding the process of lipid accumulation using a statistical tool for data reconciliation was used to improve the experimental data obtained in chemostat culture reducing the experimental errors for subsequent calculation of metabolic flux analysis (MFA). In this sense, lipids produced by L. starkeyi have relevant importance of academic and industrial point of view, as feedstock for biodiesel and oleochemical industry applications
Doutorado
Processos em Tecnologia Química
Doutora em Engenharia Quimica
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Holade, Yaovi. "Transformation électrocatalytique de sucres couplée à la réduction enzymatique de l'oxygène moléculaire pour la production d'énergie." Thesis, Poitiers, 2015. http://www.theses.fr/2015POIT2262/document.
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Le développement de générateurs d'énergie pour alimenter des micro-appareils électroniques implantés est devenu une option inéluctable. L'objectif général qui a orienté ces recherches était l'élaboration et les études approfondies des propriétés nanomatériaux métalliques utilisables comme électrocatalyseurs afin de convertir l'énergie chimique en énergie électrique. Les nanomatériaux sont obtenus par la méthode de synthèse : Bromide Anion Exchange (BAE) qui a été scrupuleusement revisitée puis optimisée avec un agent réducteur faible (AA) et fort (NaBH4). Cette voie de synthèse a permis d'obtenir (rendement ≥ 90 %) des matériaux plurimétalliques composés d'or, de platine et de palladium. Un prétraitement des supports commerciaux des nanoparticules a permis d’augmenter leurs surfaces, spécifique et active respectivement de 48 et 120 %. Les études (électro)analytiques ont permis d'identifier les intermédiaires et produits de réaction du combustible. Le glucose s'oxyde sans rupture de la liaison C-C pour donner majoritairement du gluconate avec une sélectivité ≥ 88 %. Les tests réalisés en biopile hybride (cathode enzymatique) indiquent que les catalyseurs Au/C-AA et Au60Pt40/C-NaBH4 sont les meilleures anodes abiotiques (Pmax = 125 µW·cm-2 à 0,4 V). Par ailleurs, les piles sans membrane séparatrice et sans enzyme ont été réalisées avec succès pour activer un stimulateur cardiaque et un système de transmission d'information en mode "Wifi". Ces dispositifs, rapportés pour la première fois, ouvrent une ère nouvelle pour la conception de convertisseurs d'énergie pour alimenter les implants médicaux ou des appareils sans fil de détection et de surveillanceThe development of energy converters to power implanted micro-electronic devices has become a cornerstone item. The whole target which has governed this research was the design of advanced nanostructures metals used as electrocatalysts for converting chemical energy into electrical one. These nanomaterials were obtained by the synthesis method: Bromide Anion Exchange (BAE) that has been carefully revisited and optimized, using a weak reducing agent (AA) and strong one (NaBH4). It allowed to prepare efficiently various plurimetallic nanomaterials composed of gold, platinum and palladium (yield ≥ 90%). A thermal pretreatment of commercial carbon supports of nanoparticles has highly boosted their specific and active surface areas with a gain of 48 and 120%. Based on in situ and ex-situ (electro)analytical methods, the intermediates and final reaction products of the fuel oxidation were identified. Glucose electrooxidation occurs without C-C bond cleavage and gives predominantly gluconate with a selectivity ≥ 88 %. Results from the hybrid biofuel cell tests (with an enzyme as cathode catalyst) indicate that Au/C-AA and Au60Pt40/C-NaBH4 are the best abiotic anodes (Pmax = 125 µW cm-2 at 0.4 V cell voltage). A fuel cell without separating membrane and enzyme has been successfully constructed and used to activate a pacemaker and an information transmission system based on "wireless" mode. These last experiments, reported for the first time as using nanomaterials in membrane-less configuration, open a new approach in the design of advanced energy converters to power medical implants or remote systems for detection and electronic monitoring
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Kikuchi, Yoko. "Miniaturised glucose-oxygen biofuel cells." Thesis, Imperial College London, 2010. http://hdl.handle.net/10044/1/5868.
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Miniaturized glucose-oxygen biofuel cells are useful to power implantable medical devices such as biosensors. They are small, more biocompatible and run continuously on glucose and oxygen, providing cleaner energy at neutral environment. A typical glucose-oxygen biofuel cell consists of an anode with glucose oxidase (GOx) and a cathode with various oxygen reducing catalysts. This thesis describes experimental investigations of the major issues of such systems, viz.: complex electrode fabrication, enzyme instability and inefficient oxygen reduction. Electrodes were built using the simple and scaleable bulk modification method, where all the material was simply mixed and bound together into composites with epoxy resin. For the anodes, the composite made of 10% GOx with 7:7 TTF-TCNQ was found optimal. The GOx electrodes were modified with various enzyme stabilisers (PEI, DTT, PEG, GLC, FAD and mixture of PEI:DTT and PEI:FAD) and 2% of PEI-DTT (1:1 w/w) was most effective in the presence of O2. Its maximum output current density was 1.8 x 10-2 ± 9.9 x 10-3 A.m-2. It also showed the resistant against O2 electron deprivation and enzyme inhibition. Its KM.was 5 mM. For the cathodes, various oxygen reducing catalysts (metalised carbon, anthroquinone modified carbon, laccase and bilirubin oxidase) were incorporated into graphite composite and the electrodes were pretreated in different media in order to enhance their catalytic activity. None showed four-electron O2 reduction. NaOH-pretreated cobalt (II) salophen composite electrodes showed two-electron O2 reduction and were most catalytic. Its standard catalytic rate constant was 1.2 x 10-5 ± 1.2 x 10-6 m.s-1. Of the catalysts examined, metal complex composites gave the best results for oxygen-reducing cathodes and their pretreatment led to the synergetic effect because it increased the concentration of catalytic surface oxygen groups and enhanced oxygen reduction.
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Cadet, Marine. "Vers la conception d’une biopile enzymatique à glucose/oxygène efficace en milieu biologique." Thesis, Bordeaux, 2015. http://www.theses.fr/2015BORD0260/document.
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La première partie du travail présenté ici se concentre sur l’optimisation d’une cathode à oxygène. Tout d’abord, l’utilisation d’une nouvelle enzyme (la BOD de Magnaporthe oryzae) permet de multiplier le courant de réduction de l’oxygène en eau jusqu’à neuf fois. Ensuite la synthèse d’un polymère rédox adapté a permis d’améliorer le coefficient de diffusion des électrons dans l’hydrogel résultant en l’augmentation de la densité de courant générée. Enfin nous sommes passés d’uneélectrode de carbone en 2 dimensions à une fibre d’or poreuse tridimensionnelle. Après modification de cette fibre avec l’hydrogel rédox à base de BOD de M. oryzaenous avons évalué sa biocompatibilité : in vitro les tests ont montré l’absence totale de cytotoxicité et seule une très faible réponse inflammatoire ; in vivo aucune infection ne s’est déclarée pendant les 8 semaines d’implantation dans les souris etla formation d’une capsule fibrotique autour de l’électrode traduit sa bonne intégration dans les tissus de l’animal. La seconde partie concerne la biopile dans son intégralité, construite à partir de la cathode optimisée et d’une anode adaptée à base de GDH. Elle permet de générer jusqu’à 240 μW.cm-2 dans du tampon Pipes/CaCl2 à 5mM de glucose. La biopile a ensuite été testée dans du sang humain total. Un maximum de 129 μW.cm-2 a été obtenu dans un échantillon avec une glycémie de 8,2 mM sous air. De plus nous avons constaté que la densité de puissance délivrée augmente proportionnellement avec la glycémie des différents échantillons de sang testés, faisant de la biopile à la fois une source d’électricité et un biocapteur à glucose ce qui n’avait jamais été démontré auparavantThe first part of the work presented here focuses on the optimization of an oxygen cathode. First, the use of a new enzyme (BOD from Magnaporthe oryzae) permit to increase the current of reduction of oxygen into water by a factor nine. Then the synthesis of a suitable redox polymer greatly improved the diffusion coefficient of electrons in the hydrogel, resulting in an increase of the current density. Finally we switched from a two-dimensional carbon electrode to a three-dimensional porous gold fiber. After modification of the fiber with the redox hydrogel based on BOD from M. oryzae, we assessed its biocompatibility: in vitro the tests showed the total absence of cytotoxicity and only a very low inflammatory response; in vivo noinfection appeared during the 8 weeks of implantation in mice and the formation of afibrotic capsule around the device reflects its successful integration into the animal tissues.The second part concerns the full biofuel cell, elaborated from the optimized cathode and an adapted GDH-based anode. It could generate up to 240 μW.cm-2 at 5mMglucose in Pipes/CaCl2 buffer. The biofuel cell was then tested in whole human blood. A maximum of 129 μW.cm-2 was obtained in a sample with 8,2 mM glycaemiaunder air. In addition we observed that the delivered power density increased proportionally with the glycaemia of the different blood samples tested, making the biofuel cell both a power source and a glucose biosensor at the same time which had never been shown before
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Prévoteau, Antonin. "Électrodes enzymatiques à base d’hydrogels rédox en vue de l’oxydation du glucose : effet de la déglycosylation de la glucose oxydase et mise en évidence d’une réduction parasite de l’oxygène sur le médiateur rédox." Thesis, Bordeaux 1, 2010. http://www.theses.fr/2010BOR14102/document.
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La possibilité de convertir l’activité catalytique d’une oxydoréductase en un courant électrique a permis le développement d’une grande diversité d’électrodes enzymatiques. Les anodes catalysant l’oxydation du glucose font partie des plus étudiées pour leurs applications dans la mesure de la glycémie ou dans des biopiles glucose/O2. Parmi les nombreuses stratégies disponibles, l’utilisation d’hydrogels à base de complexes d’osmium en guise de médiateurs rédox fournit d’excellents résultats, qui restent cependant limités en terme de densité de courant ou de sélectivité. Durant cette thèse, la glucose oxydase (GOx) a été déglycosylée. Les électrodes préparées avec la nouvelle enzyme délivraient des courants catalytiques plus élevés, ce qui laissait supposer initialement une diminution de la distance de saut d’électron entre la GOx et le médiateur rédox suite au retrait des oligosaccharides. Une étude avec des électrodes de différentes compositions suggère au contraire que la déglycosylation n’améliore pas le transfert électronique intrinsèque mais la structure globale de l’hydrogel. De fait, une enzyme plus petite et plus négativement chargée doit induire un volume d’hydrogel plus faible pour une même composition molaire. En second lieu, une réduction parasite de l’oxygène affectant ces anodes, non envisagée jusqu’à aujourd’hui, a été mise en évidence et étudiée. En effet, l’interférence de l’O2 n’est usuellement attribuée qu’à sa réactivité avec la GOx. La présente étude prouve que l’O2 se réduit aussi sur les complexes d’osmium si leur potentiel standard E°’ est inférieur à + 0,07 V vs. Ag/AgCl. La cinétique de cette réaction croît exponentiellement quand le E°’ du complexe diminue. En plus d’abaisser le courant d’oxydation et donc les performances de l’anode, la génération de peroxyde d’hydrogène pourrait aussi altérer sa stabilité. Ces résultats suggèrent que le choix d’un médiateur de E°’ donné doit aussi dépendre de l’amplitude de cette réductionThe possibility of converting the catalytic activity of oxidoreductase enzymes into electric current has led to the development of a high diversity of enzyme electrodes. Anodes catalysing glucose oxidation have been amongst the most studied, especially for their application in monitoring blood glucose or glucose/O2 biofuel cells. Although one of the numerous strategies available, the use of osmium-based hydrogels as redox mediators, has given excellent results, some limitations still remain such as rather low current densities, stability or selectivity Initially, the study focused on the deglycosylation of glucose oxidase (GOx). When most of the oligosaccharides around this glycoenzyme were removed, the ensuing increase in the electrode catalytic current seemed a priori to support the hypothesis of a decrease in the electron hopping distance between the enzyme redox centres and the redox mediator. However, a systematic study of electrode response for different compositions leads us to conclude that deglycosylation does not improve the intrinsic electron transfer but the whole hydrogel structure. This seems due to the smaller size and higher surface charge of the deglycosylated GOx inducing smaller hydrogel volumes than in the native-based GOx. The study then proceeded to examine the oxygen side reduction of commonly used osmium-based redox polymers. The interference of O2 on glucose oxidation current has generally been attributed to O2 reactivity with GOx. The present study shows that O2 reduction also occurs on osmium-based polymers if their formal potential E°’ is below + 0.07 V vs. Ag/AgCl. The kinetics of this reaction appears to increase exponentially when E°’ decreases. As well as reducing the oxidation current and, consequently, lowering anode performances, the generation of hydrogen peroxide could also modify electrode stability. These results suggest that the choice of redox mediator for a given E°'must also take into account the extent of O2 reduction
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Katic, Janko. "Highly-Efficient Energy Harvesting Interfaces for Implantable Biosensors." Doctoral thesis, KTH, Integrerade komponenter och kretsar, 2017. http://urn.kb.se/resolve?urn=urn:nbn:se:kth:diva-206588.
Full textAbstract:
Energy harvesting is identified as an alternative solution for powering implantable biosensors. It can potentially enable the development of self-powered implants if the harvested energy is properly handled. This development implies that batteries, which impose many limitations, are replaced by miniature harvesting devices. Customized interface circuits are necessary to correct for differences in the voltage and power levels provided by harvesting devices from one side, and required by biosensor circuits from another. This thesis investigates the available harvesting sources within the human body, proposes various methods and techniques for designing power-efficient interfaces, and presents two CMOS implementations of such interfaces. Based on the investigation of suitable sources, this thesis focuses on glucose biofuel cells and thermoelectric harvesters, which provide appropriate performance in terms of power density and lifetime. In order to maximize the efficiency of the power transfer, this thesis undertakes the following steps. First, it performs a detailed analysis of all potential losses within the converter. Second, in relation to the performed analysis, it proposes a design methodology that aims to minimize the sum of losses and the power consumption of the control circuit. Finally, it presents multiple design techniques to further improve the overall efficiency. The combination of the proposed methods and techniques are validated by two highly efficient energy harvesting interfaces. The first implementation, a thermoelectric energy harvesting interface, is based on a single-inductor dual-output boost converter. The measurement results show that it achieves a peak efficiency of 86.6% at 30 μW. The second implementation combines the energy from two sources, glucose biofuel cell and thermoelectric harvester, to accomplish reliable multi-source harvesting. The measurements show that it achieves a peak efficiency of 89.5% when the combined input power is 66 μW.Energiskörd har identifierats som en alternativ lösning för att driva inplanterbara biosensorer. Det kan potentiellt möjliggöra utveckling av själv-drivna inplanterbara biosensorer. Denna utveckling innebär att batterier, som sätter många begränsningar, ersätts av miniatyriserade energiskördsenheter. Anpassade gränssnittskretsar är nödvändiga för att korrigera för de skillnader i spänning och effektnivå som produceras av de energialstrande enheterna, och de som krävs av biosensorkretsarna. Denna avhandling undersöker de tillgängliga källorna för energiskörd i den mänskliga kroppen, föreslår olika metoder och tekniker för att utforma effektsnåla gränssnitt och presenterar två CMOS-implementeringar av sådana gränssnitt. Baserat på undersökningen av lämpliga energiskördskällor, fokuserar denna avhandling på glukosbiobränsleceller och termoelektriska energiskördare, som har lämpliga prestanda i termer av effektdensitet och livstid. För att maximera effektiviteten hos effektöverföringen innehåller denna avhandling följande steg. Först görs en detaljerad analys av alla potentiella förluster inom boost-omvandlare. Sedan föreslår denna avhandling en designmetodik som syftar till att maximera den totala effektiviteten och effektförbrukningen. Slutligen presenterar den flera designtekniker för att ytterligare förbättra den totala effektiviteten. Kombinationen av de föreslagna metoderna och teknikerna är varierade genom två högeffektiva lågeffekts energigränssnittskretsar. Den första inplementeringen är ett termoelektriskt energiskördsgränssnitt baserat på en induktor, med dubbla utgångsomvandlare. Mätresultaten visar att omvandlaren uppnår en maximal effektivitet av 86.6% vid 30 μW. Det andra genomförandet kombinerar energin från två källor, en glukosbiobränslecell och en termoskördare, för att åstadkomma en tillförlitlig multi-källas energiskördslösning. Mätresultaten visar att omvandlaren uppnår en maximal effektivitet av 89.5% när den kombinerade ineffekten är 66 μW.
QC 20170508
Mi-SoC
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Reuillard, Bertrand. "Elaboration de bioélectrodes à base de nanotubes de carbone pour la réalisation de biopiles enzymatiques Glucose/02." Thesis, Grenoble, 2014. http://www.theses.fr/2014GRENI090/document.
Full textAbstract:
Ce mémoire est consacré à l'optimisation de la connexion enzymatique d'enzymes pour l'oxydation du glucose et la réduction de O2 sur matrices de nanotube de carbone (CNT) dans les biopiles à glucose.Premièrement, le transfert électronique indirect de la glucose oxydase (GOx) est optimisé dans une matrice nanostructurée de CNT contenant la 1,4-naphtoquinone comme médiateur rédox. Cette bioanode a ensuite été combinée avec des biocathodes similaires à bases d'enzymes à cuivre (laccase et tyrosinase). La biopile GOx-NQ/Lac a permis d'obtenir des puissances maximales de l'ordre de 1,5 mW.cm-2. Les utilisations de cette pile en décharge courte, longue et sa stabilité dans le temps ont également été étudiées. La seconde partie présente la préparation d'une autre anode basée sur la connexion indirecte d'une glucose déshydrogènase NAD+-dépendante (GDH-NAD+) comme alternative pour l'oxydation du glucose. La GDH-NAD+ a été combinée avec un catalyseur d'oxydation de NADH par différentes méthodes. Tout d'abord, elle a été encapsulée au sein du métallopolymère rédox, puis, la modification supramoléculaire a dans un second temps permis d'immobiliser le catalyseur moléculaire et l'enzyme à la surface des CNTs. Ces deux bioanodes ont permis respectivement l'obtention de courants catalytiques d'oxydation du glucose de 1,04 et 6 mA.cm-2. La seconde bioanode a été combinée avec une biocathode à base de BOD et a permis l'obtention de densités de courants maximales de l'ordre de 140 µW.cm-2 La dernière partie concerne l'élaboration d'une biocathode bienzymatique pour la réduction de O2. Le DET de la HRP sur CNTs a dans un premier temps été optimisé par modification de la surface par différents dérivés pyrène. Ensuite, la combinaison de la GOx et de la HRP sur la même électrode a permis de réduire efficacement O2 en 2 étapes. La biocathode est capable de délivrer une densité de courant maximale de l'ordre de 200 µA.cm-2. Cette dernière, combinée avec la bioanode GDH présentée précédemment a permis d'obtenir une biopile opérationnelle en conditions physiologiques et 10 mM de NAD+, en étant capable de débiter une densité de puissance maximale de l'ordre de 57 µW.cm-2This work focuses on the optimization of the electrical wiring of glucose oxidizing and dioxygen reducing enzymes on carbon nanotube (CNT) matrixes for glucose biofuel cells.In the first part, glucose oxidase (GOx) mediated electron transfer (MET) is optimized in nanostructured CNTs matrixes by mechanical compression of a CNTs/GOx composite containing 1,4-naphtoquinone as redox mediator. This bioanode was then combined with MCOs (laccase and tyrosinase) based biocathodes. The GOx-NQ/Lac biofuel cell was able to deliver a maximum power density of 1.5 mW.cm-2. The use of this biofuel cell in short/long time discharge and in storage has also been studied. The second part presents the preparation of another bioanode based on the indirect wiring of a NAD+-dependant glucose dehydrogenase (GDH-NAD+) as an alternative for glucose oxidation. The GDH-NAD+ has been combined with an NADH oxidation catalyst by two different techniques. The first one involves the encapsulation of the protein in the metallopolymer redox film, whereas the second one relies on the supramolecular modification of the CNTs by the molecular catalyst and the enzyme. Both bioanodes showed good catalytic properties toward glucose oxidation in presence of NAD+ with respectively 1.04 mA cm-2 and 6 mA cm-2. The latter has been combined with a BOD based biocathode to form a biofuel cell exhibiting maximum power densities of 140 µW cm-2. The last part of this work focuses on the design of a bienzymatic biocathode for O2 reduction. The DET of horseradish peroxidase (HRP) was first investigated and optimized by modification of the CNTs with pyrenes derivatives. The combination of the HRP with the GOx on the same electrode enables an efficient reduction of O2 in a 2-step process. The biocathode could exhibit maximum currents densities of 200 µA cm-2. This cathode along with the previous GDH bioanode formed a biofuel cell functional in physiological conditions and 10 mM NAD+ showing maximum power densities of 57 µW cm-2
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Roussarie, Elodie. "Identification et caractérisation de bilirubines oxydases pour l'élaboration de biopiles enzymatique à glucose/oxygène." Thesis, Bordeaux, 2018. http://www.theses.fr/2018BORD0161/document.
Full textAbstract:
La puissance de la biopile enzymatique à glucose/oxygène est limitée par sa partiecathodique. Afin de contourner cette limitation, nous avons étudié les enzymescathodiques : les Bilirubine oxydases (BODs). Dans le but de mieux appréhender ces BODs, lemécanisme réactionnel, la nature de l’étape limitante et l’effet des sels ont alors été étudiés.Deux mécanismes différents sont retrouvés en fonction du mode de transfert des protons etdes électrons (4 fois 1H+/1e- ou 2 fois 2H+/2e-). De plus, nous avons démontré que l’étapelimitante est l’oxydation du substrat pour les trois substrats testés et que les sels agissent auniveau du cuivre T1. Les principales limitations des BODs sont leur stabilité à 37 °C ainsi queleur inhibition par le NaCl. Deux techniques ont alors été utilisées pour identifier des BODsplus résistantes. La première méthode est l’extraction de nouvelles enzymes à partird’organismes extremophiles. Elle a permis d’isoler la BOD d’Anaerophaga thermohalophilaqui possède une bonne résistance au NaCl mais une densité de courant faible. Dans unsecond temps, afin de reconstruire des séquences ancestrales, la phylogénie de la familledes Bacillus Bacterium a été effectuée. Cette technique a permis l’identification de troisBODs possédant des caractéristiques très intéressantes : la BOD de Bacillus nakamurai etdeux BODs ancestrales (Noeud 10 et Noeud 13). Par exemple, après une heure à 37°C et 140mM de NaCl, le Noeud 10 possède une meilleure densité de courant que la BOD de Bacilluspumilus, qui est l’enzyme utilisée comme base de la phylogénie. La seconde technique estdonc une méthode de choix permettant la découverte de nouvelles enzymes à la fois plusstables et plus résistantes que les enzymes actuelles. Elle ouvre de grandes perspectivespour l’utilisation des BODs comme enzymes cathodiques ou pour d’autres applicationsbiotechnologiques. Enfin, nous avons montré que l’immobilisation de la BOD de B. pumilusdans le matériau Si-(HIPE) permet la décoloration cyclique de colorants chimiques surplusieurs moisPower of glucose/oxygen enzymatic biofuel cell is limited by the cathodic part. In order to prevent this limitation, we studied cathodic enzymes: Bilirubin oxidases (BODs). For this purpose, the kinetic mechanism, rate-limiting step and salts effect were determined. Two different mechanisms are observed depending on the electron/proton transfer (4 times1H+/1e- or 2 times 2H+/2e-). We also demonstrated that the rate-limiting step is the substrate oxidation for the three substrates tested and salts act around the T1 copper. Main BODs limitations are their stability at 37°C and their inhibition by NaCl. Two methods were used toidentify the most resistant BODs. The first one was the identification of new enzymes from extremophile organisms. It allows to isolate BOD from Anaerophaga thermohalophila whichhas good NaCl resistance but low current density. In addition, in order to reconstructancestral sequences, phylogeny of Bacillus Bacterium family was performed. This methodidentified three BODs with interesting features: BOD from Bacillus nakamurai and twoancestral BODs (Noeud 10 and Noeud 13). For example, after one hour at 37°C and 140 mMNaCl, Noeud 10 has a better current density than the BOD from Bacillus pumilus, which is theenzyme used as basis for the phylogeny. This second method allowed the discovery of newenzymes that were both more stable and more resistant than actual enzymes. Thistechnique opens up valuable prospects for the use of BODs as cathodic enzymes or for otherbiotechnological applications. In the end, we demonstrated that BOD from B. pumilusimmobilization in Si-(HIPE) materials allows cyclic discoloration of chemical dyes duringseveral months
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Ciniciato, Gustavo Pio Marchesi Krall. "Desenvolvimento de biocélulas a combustível de glicose/oxigênio em microfluídica." Universidade de São Paulo, 2013. http://www.teses.usp.br/teses/disponiveis/75/75134/tde-23042013-105430/.
Full textAbstract:
O objetivo principal desta tese foi o de se desenvolver uma biocélula a combustível enzimática em microfluídica, utilizando a glicose como combustível e o oxigênio como oxidante. Foram utilizadas as enzimas Glicose Oxidase ou Glicose Desidrogenase em um bioânodo, de forma a promover reações bioeletrocatalíticas de oxidação da glicose e as enzimas Lacase ou Bilirrubina Oxidase, de forma a promover reações bioeletrocatalíticas de redução do oxigênio molecular. O trabalho se procedeu por tentativas de imobilizar estas enzimas, de forma a promover o mecanismo de transferência eletrônica direta com um eletrodo. Nas situações as quais isso não foi possível, foram utilizados mediadores eletrônicos, de forma a promover o mecanismo de transferência eletrônica mediada. O melhor par de sistemas de bioeletrodos e mediadores foi escolhido para serem aplicados em uma biocélula a combustível. O trabalho se procedeu em adaptar este par de bioeletrodos desenvolvidos para um sistema de microfluídica em papel, sendo ambos biocátodo e bioânodo em papel. Como as condições de concentração de combustível e de cofatores foram otimizadas para o bioânodo, foi necessário trabalhar com os biocátodos, de forma a apresentar as características de um biocátodo respirador, para melhor utilizar o oxigênio presente no ar e a apresentar um desempenho tão bom quanto o dos bioânodos. A biocélula a combustível em papel possibilitou a geração de energia elétrica por até 18 dias, utilizando uma resistência de 1.7 kΩ, nas condições experimentais ideais. De forma a provar o conceito da tecnologia para aplicações reais, a biocélula a combustível em papel foi demonstrada a ter a capacidade de geração de energia elétrica suficiente para fazer um relógio funcionar por pelo menos 36 horas, utilizando a bebida isotônica Gatorade®, como combustível.The main objective of this thesis is to develop a microfluidic biofuel cell using glucose as the fuel and oxygen as the oxidant. The enzymes Glucose Oxidase or Glucose Dehydrogenase were used in a bioanode to promove the bioelectrocatalytic oxidation of glucose and the enzymes Laccase or Bilirubin Oxidase to promove the bioelectrocatalytic reduction of the molecular oxygen. The work was conducted by attempts to immobilize these enzymes in order to promote the mechanism of direct electron transfer with the electrode. For the situations where this was not observed, mediators were used in a way to promote the mechanism of mediated electron transfer. The best pair of bioelectrodes and mediatores was chosen to be applied in a biofuel cell. The work was carried out to adapt this par of developed bioelectrodes to a paper based microfluidic system, using both biocathode and bioanode in a paper-like design. As the conditions for concentration of fuel and cofactors were optimized for the bioanode, it was necessary to work on these biocathodes so as to have the characteristics of an air-breathing biocathode for a better use of the oxygen present in the air and to work with a performance as good as the bioanode. The paper based biofuel cell enabled the generation of electricity for up to 18 days using a resistance of 1.7 kΩ within the optimum experimental conditions. In order to prove the concept of this technology for real applications, the paper based biofuel cell was demonstrated to have the capacity for generation of enough electrical energy to power up a clock for at least 36 hours using the isotonic drink Gatored® as fuel.
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LIAO, KUAN-HUA, and 廖冠華. "Preparation, Characterization and Durability of Enzymatic Glucose/O2 Biofuel Cell." Thesis, 2019. http://ndltd.ncl.edu.tw/handle/5wcfhe.
Full textAbstract:
碩士國立勤益科技大學
化工與材料工程系
107
Glucose oxidase (GOx), bilirubin oxidase (BOD) and laccase (Lac) are used as bio-catalysts for the bioanode and biocathode, respectively, in this thesis. The properties and stability of bioanode and biocathode prepared by the immobilization of enzymes onto the anodizing mesoporous carbon (MC) named as MCP/Si-anodizing time by the casting (C) and enzyme absorption (EA) techniques are investigated. Finally, the characteristics of the membraneless glucose biofuel cell (GBFC) composed by the home-made bioanode and biocathode are also studied. The materials prepared in this thesis are characterized by FESEM, TEM, BET analyzer and contact angle analyzer, respectively. The electrochemical behaviors and stabilities of glucose oxidation reaction (GOR) on the bioanode and the oxygen reduction reaction (ORR) on the biocathode are analyzed by the polarization curve technique. The discharge properties and the stability of home-made GBFC are investigated by the constant current technique. When the GOx is immobilized by the casting method, the current collector Ausp is replaced by the Aued (electrodeposited by the hydrogen bubble dynamic template (HBDT) technique at 4.6 mA cm-2), MC0.5 support is anodized treatment for 5 s, the addition of 1 l 0.5% Triton X-100 interfacial agent between the MC0.5 and Aued, the good stability, reproducibility and the maximum current density of GOR on the chitosan/C-GOx/ TMPD (N,N,N’,N’-Tetramethyl-p-phenylenediamine)/MC0.5-5(MCP/Si - anodizing time)/T0.5/Aued (electrodeposited) /Ausp (sputtering)/Al2O3 (C-GOx/MC0.5-5) bioanode are obtained. The stable net GOR current density obtained at 7th polarization curve is 0.180 mA cm-2 at 0.2 V (vs. Ag/AgCl/3 M NaCl(aq)), which is 12 times for that obtained on chitosan/C-GOx/TMPD/MC0.5/T1/Ausp/Al2O3 bioanode. The detachment and deactivation fractions of GOx on C-GOx/MC0.5-5 bioanode are found to be 6.06 and 52.11%, respectively. When the GOx is immobilized onto MC0.5 by the adsorption method, the stable current density of GOR on EA-GOx/MC0.5-5-3 bioanode is 0.603 mA cm-2 at 8th polarization curve, and the detachment and deactivation fractions of GOx are found to be 5.00 and 19.58%, respectively. The results indicate that the stability of the bioanode is significantly improved by replacing the GOx immobilization technique from casting to adsorption method. When the BOD is immobilized by the casting method, the Aued current collector is prepared by HBDT technique at 3.2 mA cm-2, MC0.5 support is anodized treatment for 60 s, the addition of 1 l 0.5% Triton X-100 interfacial agent between the MC0.5 and Aued, the maximum current density of ORR on the chitosan/C-BOD/ABTS(2,2-azinobis(3-ethylbenzothiazoline-6-sulfonate))/MC0.5-60/T0.5/Aued/Ausp/Al2O3 (C-BOD/MC0.5-60) is obtained to be 0.218 mA cm-2 at 0.2 V, which is 1.4 times for that on chitosan/C-BOD/ABTS/MC0.5/T0.5/Ausp/Al2O3. The stable discharge curve and the maximum discharge power density of the membraneless GBFC composed by the EA-GOx/MC0.6-5-3 bioanode and C-BOD/MC0.5-60 biocathode is obtained to be 0.080 mW cm-2 (Ecell, discharge = 0.36 V) for 6th discharge cycle with open circuit voltage (OCV) of 0.56 V. By fixing the geometric area of biocathode as 0.250 cm2 and decreasing the anodic area to 0.050 cm2, the stable maximum power density of the GBFC with asymmetric electrode areas is obtained to be 0.125 mW cm-2 (Ecell, discharge = 0.17) for 6th discharge cycle with OCV of 0.45 V.
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Chen, Yen-Yu, and 陳彥宇. "Application of Glucose Dehydrogenase of Pseudomonas aeruginosa PAO1 on Biofuel cell." Thesis, 2006. http://ndltd.ncl.edu.tw/handle/63575550121234741373.
Full textAbstract:
碩士元智大學
生物科技暨生物資訊研究所
94
Biofuel cells are miniature power-generating systems that convert chemical energy to electrical energy by using biocatalysts to catalyze the oxidation of organic substances. Glucose dehydrogenase is an ideal anodic catalyst for biofuel cells because of its high catalytic efficiency, wide substrate specificity and insensitivity to oxygen. It is inherently limited to improve the efficiency of the biofuel cell system by enzyme modifications, immobilizations and electrodes modifications. To overcome these limitations, a powerful anode catalyst is essential. The glucose dehydrogenase in the membrane was washed by 1.5 % Triton X-100. Two types of glucose dehydrogenase in Pseudomonas aeruginosa PAO1 were co-purified by the DEAE sepharose chromatography, and existed in the form of complex. The activity of the glucose dehydrogenase was determined by dye-reduction method during the purification processes. By constant-potential method at 0.35 V and 25 ℃, using Ag/AgCl as a reference, one unit of GDHA and GDHB had a current density of 1814 ?嫀/cm2 and 2748 ?嫀/cm2, respectively. Compared with the current density of glucose oxidase of Aspergillus niger, the glucose dehydrogenase of P. aeruginosa PAO1 was a potential anodic catalyst in biofuel cell system.
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Chan, Chang Yeong, and 張永昌. "Preparation and properties of anode and full cell of enzymatic glucose/O2 biofuel cell." Thesis, 2012. http://ndltd.ncl.edu.tw/handle/32570166934156200620.
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碩士國立勤益科技大學
化工與材料工程系
100
Mesoporous carbon (MC) prepared by an one-step synthesis technique is used as the support of electrocatalysts. The properties of home-made MC are characterized by BET and TEM, respectively. Using the home-made MC as support, the factors affecting the anodic oxidation of glucose on the home-madeChitosan/GOx/MC/Au/Al2O3 are investigated. Finally, the properties of the home-made membraneless bio-fuel cell based on Chitosan/GOx/TMPD (N,N,N´,N´- Tetramethyl- p-phenylenediamine) /MC/Au/Al2O3 and Chitosan/BOD/ABTS (2,2’- azinobis(3-ethylbenzo-thiazoline-6-sulfonate))/MC/Au/Al2O3 as the anode and cathode, respectively, are also studied in this thesis. When the Chitosan/GOx/TMPD/MC/Au/Al2O3 is used as working electrode for anodic oxidation of glucose, the maximum enzyme utility is obtained for 100 μg (1.73U) GOx, the best electron transfer efficiency between the electrode and enzyme is obtained for immobilizing 2.5 μmol TMPD and the optimal pH and temperature are found to be 7.0 and 37 ˚C, respectively. Using Chitosan/GOx/TMPD/MC/Au/Al2O3 as the working electrode for anodic oxidation of glucose, the indirect electron transfer mechanism with TMPD as electron transfer mediator is found at -0.05 ~ 0.3 V, and the direct electron transfer pathway between GOx and the current collector is obtained for the potential greater than 0.3 V. Using Chitosan(0.18 µmol)/GOx(1.73U)/TMPD(2.5 µmol)/MC/Au/Al2O3 as the working electrode, the maximum current for anodic oxidation of glucose through the indirect electron transfer pathway is obtained to be 26.57±6.12μA (0.3 V) at 37℃in pH 7 buffer solution containing 30 mM glucose, and at the same time the limiting current is 41.34 ± 2.11 μA at 0.6 V (including the indirect and direct electronic transfer pathways). For the home-made membraneless glucose/O2 biofuel cell, the power density increases from 8.45±0.09 to a maximum value of 26.11±0.28 µW cm-2 by increasing pH from 5 to 7. Further increasing the pH to 8 the power density is decreased to 7.38±2.04 µW cm-2. Increasing the temperature from 20 to 25 oC the power density increases from 19.74±0.48 to a maximum value of 26.11±0.28 µW cm-2. The power density decreases to 7.20±0.99 µW cm-2 by further increasing temperature to 37 oC. The power density of the home-made biofuel cell increases from 19.24±2.74 to a maximum of 26.11±0.28 µW cm-2 by increasing the concentration of glucose from 20 to 30 mM, and the power density decreases to 18.49±0.45 µW cm-2 by further increasing the concentration of glucose to 60 mM. Therefore the maximum power density of home-made membraneless glucose/O2 biofuel cell is obtained to be 26.11±0.28 µW cm-2 at the optimal conditions of 37℃ and pH 7 buffer solution containing 30 mM glucose.
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Zhu, Ziwei. "Making glucose oxidase fir for biofuel cell applications by directed protein evolution /." 2006. http://www.jacobs-university.de/phd/files/1178727126.pdf.
Full textAbstract:
Thesis (Ph.D.)--International University Bremen, 2006.School of Engineering and Science. "Doctor of Philosophy in Biochemical Engineering." Includes bibliographical references (leaves 86-91). Also available online.
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Pai, Chieh An, and 白傑安. "Synthesis of binary PtRu nanoparticles/N-doped graphene composites for a glucose biofuel cell." Thesis, 2017. http://ndltd.ncl.edu.tw/handle/5f35gn.
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Lai, Wen-Ren, and 賴威任. "Enzymatic electrode based AC mode electrochemical technique for glucose detection and biofuel cell electrode development." Thesis, 2006. http://ndltd.ncl.edu.tw/handle/54137512076139794617.
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碩士國立臺灣大學
工程科學及海洋工程學研究所
94
Taking the research results on electrochemistry based detection methods developed in Nano-BioMEMS team of National Taiwan University, this dissertation proposed a fundamental theoretical model for the previously reported detection method and used this model to point out the potential advantages of using sine wave voltage as the primary power source. In order to prove the underlying advantage with respect to traditional electrochemical method, we developed a glucose enzymatic strip as the testing platform. The experimental data obtained indicated that higher linearity and lower than 5% coefficient of variation with respect to the glucose concentration rangking between 50 to 500 mg/dL can be obtained for 40% hematocrit whole blood test. Using different glucose concentrations standard solutions as the test samples, we compared the testing data obtained from our new voltage applied method and that of the traditional method. To determine right current sampling time, instant trigger voltage method was adopted, i.e., the response current created by dropping the glucose sample on strip was used to start the measurement process. By modulating the frequency and the amplitude of the applied sine wave voltage, a higher resolution and stronger response current can be obtained between measured voltage and the glucose concentration. Even at the high glucose concentration of 600 mg/dL, the new method achievees higher linearity when compared to traditional electrochemical method. To eliminate the non-Faraday current and to increase the signal-to-noise ratio this thesis proposed a new signal processing algorithm using the newly developed theoretical modeling. This approach recognized that non-Faraday current was induced by the double layer capacity effect created by applying the sine wave voltage and can thus be eliminated by proper signal processing algorithm. More specifically, it was identified that non-Faraday current can be integrated to zero if the integration time is set to be the integer times of the applied sine voltage period. The experimental data obtained clearly verified that this newly proposed integration signal processing algorithm and the newly proposed sine wave driving voltage method led to better singla to noise ratio and higher linearity when comparing the FFT spectrum of the signal at DC and at the applied driving voltage signal frequency. This research proves that the frequency of sine wave voltage can enhance the DC term of response current and this current is directly proportional to the sample glucose concentration and has higher sensitivity with respect to the glucose concentration. After several hundred measurements at the testing condition of 50Hz and 10mV amplitude sine wave voltage, it was found that this new approach can have better than 40% sensitivity when compared to the respone current obtained from the traditional method. This thesis also attempted to develop biofuel cells, which can use biocatalysts to convert chemical energy to electrical energy. As the long-term vision of this biofuel is to be used as the power source for embedded biosensors, glucose was applied as the substrate for the oxidation processes at the anode and oxygen was uesd as the substrates for the reduction processes at the cathode. Taking the enzymatic strip of glucose sensor as the starting point, we used glucose oxidase (EC 1.1.3.4) and bilirubim oxidase(EC 1.3.3.5) to catalyze the processes on the anode and the cathode. The enzyme and mediator were entrapped by the polypyrrole on the Au electrode through electropolymerization. The Cyclic Voltammetry was used to polymerize the pyrrole, which control the scan cycles and the scan rate to determine the deposit of polypyrrole. For final testing of this newly attempted biofuel cell, the GOx-polypyrrole electrode and the BOD- -polypyrrole electrode were integrated and it was identified that for glucose concentration 200mg/dL, 0.15V maximum voltage and 0.242μW/cm2 output power can be obtained when connecting to a 50kΩ load.
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Huang, Ping-Yi, and 黃秉毅. "Poly(aniline-co-o-phenylenediamine) for the immobilization of enzymes for the investigation of glucose/oxygen biofuel cell." Thesis, 2008. http://ndltd.ncl.edu.tw/handle/89777599608256485856.
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碩士國立成功大學
化學工程學系碩博士班
96
In our research, aniline and o-phenylenediamine (o-PD) was used as the monomer for electropolymerization of the immobilization material of glucose oxidase and laccase on carbon paper as the anode and cathode, respectively. Thus, the biofuel cell system was composed of the enzyme immobilized poly(aniline-co-o-PD). Addition of anodic redox mediator, HQS (8- hydroxyquinoline-5-sulfonic acid) and cathodic redox mediator ABTS (2,2’- azino-bis(3-ethylbenzothiazoline-6-sulfonic acid) will draw a significant effect on the power output of biofuel cell. Carbon nanotube was used in electropolymerization also increase the power density. Using SEM photos to observation the surface morphology of the enzyme electrode, we can discover the polymer films will increase by addition o-PD in electropolymerization. FT-IR spectrum will be able to prove that o-PD modified the longchain structure of polyanilne and become to side chain or network polymer structure. Additionally, using chronoamperometry method to find out the optimum pH for discharge of enzyme electrode Salt bridge was applied to connect the both side of cells as proton medium. The power density with respect to different operating voltages with glucose concentration of 10 mM. Increasing o-PD concentration in electropolymerization can achieve enormous enhancement of power density. The composited cell made by 0.4 M aniline and 0.2 M o-PD has a maximum power density of 13.76 �巰/cm2 at 0.26 V. Further investigation of the optimum concentration of CNTs, enzyme, cycles in electropolymerztion and the optimum operation condition to obtain the maximum power output. A Nafion proton exchange membrane was also inserted to separate both half cells. When system has a better convective flow environment for cell discharge, it has a maximum power density of 11.767 �巰/cm2 at 0.14 V. Finally, the power output of biofuel cell system in long-term operation will decreased, probably the activity of the enzyme decayed or damaged in cell operation or fell out of the enzymatic electrode. Therefore, further investigation is to maintain the maximum power density and enzyme activity in the long-term operation.
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Ting-YiHuang and 黃庭誼. "On the study of immobilization of enzyme by poly(3-methylthiophene-co-thiophene-3-acetic acid) on electrodes for glucose/oxygen biofuel cell." Thesis, 2012. http://ndltd.ncl.edu.tw/handle/14996562070943976121.
Full textAbstract:
碩士國立成功大學
化學工程學系碩博士班
100
Fuel cell is a device which transform chemical energy directly into electrical energy, and generates power and water continuously. The enzymatic biofuel cells become a promising technology because of its vast potential applications of in vivo and ex vivo aspects. Because glucose widely present in food and living organisms, it is used as the fuel in enzymatic biofuel cell. This project investigate the effects of the preparation conditions for enzyme-immobilized anode on the cell performance of biofuel cells. 3-methylthiophene/thiophene-3-acetic acid (3MT/T3A) copolymer were prepared on the gold electrode by electropolymerization, and enzymes were immobilized covalently by condensation reaction with the carboxyl groups in T3A. Glucose oxidase (GOx) and laccase were used as the anodic and cathodic enzymes, respectively. 8-hydroxyquinoline-5-sulfonic acid (HQS), N,N,N’,N’-tetramethyl-p-phenylenediamine (TMPD) were used as the anodic redox mediators and 2,2’-azino-bis(3-ethylbenzothiazoline-6-sulfonic acid) was used as the cathodic redox mediator. The effects of enzyme immobilization method, electropolymerizing charge, 3MT/T3A monomer ratio and concentration of mediator on the glucose oxidation current of half cell and the current of single cell were investigated. According to scanning electron microscope (SEM) images, the structure of 3MT/T3A was fluffy. when electropolymerizing charge increased, the structure of 3MT/T3A changed from granular to slender form. According to Fourier Transform Infrared Spectrometer (FTIR) spectra, 3MT/T3A copolymer had C=O band, and copolymer/GOx electrode had peptide band. From half cell experiments, the enzymatic electrode, prepared with enzyme-precipitated crosslinking (EPC) method at electropolymerizing potential of 1.77 (V vs Ag/Ag+) with charge of 1.6 C in an electrolyte containing 3MT:T3A monomer ratio 9:1 and 20 mM HQS had the highest oxidation current of glucose. Moreover, the electrode with TMPD as mediator gave more negative onset potential for glucose oxidation. In a single cell, the enzymatic electrode, prepared via EPC method at electropolymerizing potential of 1.77 (V vs Ag/Ag+) with charge of 1.6 C in an electrolyte containing 3MT:T3A monomer ratio 9:1 and 1 mM TMPD gave the larger maximum power density of 83.29 μW/cm2, which was about 11.7 times higher than that with HQS as mediator condition. In a single cell, the enzymatic electrode, prepared via EPC method at electropolymerizing potential of 1.77 (V vs Ag/Ag+) with charge of 1.6 C of anode and 2.0 C of cathode in an electrolyte containing 3MT:T3A monomer ratio 9:1, 1 mM TMPD and 10 mM ABTS gave the largest maximum power density of 186.90 μW/cm2.
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Cherdchim, Banyat. "Actions of lignocellulolytic enzymes on Abies grandis(grand fir) wood for application in biofuel production." Doctoral thesis, 2010. http://hdl.handle.net/11858/00-1735-0000-0006-B138-4.
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XU, JUN-XIANG, and 許俊翔. "3D Printing of Microfluidic Glucose Biofuel Cells." Thesis, 2018. http://ndltd.ncl.edu.tw/handle/wfa8p3.
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碩士國立高雄應用科技大學
機械工程系
106
Through this study novel photocurable 3D desktop printer (Formlabs, Form 2, USA) to make a biofuel cell body which had a flow passage of fuel conveyance. In this study, we utilized the enzyme as an electrode by inkjet printer (Dimatix, DMP 2800). The characteristics of the 3D printed flow channel are compared with the MEMS and the traditional process, which is convenient and rapid. The fabrication of parameters be control easily from designer. We used the printer to print the electrodes, and electrode patterns is created by CAD software whatever we need, and transfer the file to the printer, instead of the commonly screen printing method, to achieve digital design and manufacturing concept. This experiment successfully used 3D printing technology to make a biofuel cell body. The results can print a channel depth of 0.268 mm and put the paper and electrodes into assembly. The best results of printing silver electrode production. In printing the electrode of 5 layer, which is the best guide conductivity 198.39 Siemen / cm, and resistance is 0.07 Ω, the overall average of 161.73 Siemens / cm, a standard deviation of 23.34 Siemens /cm. Glucose biofuel cell performance is measured at cyclic voltammetry, showed a maximum oxidation peak at a glucose concentration of 10 mM at a pH of 5 and a current of 1.74 mA at a voltage of 1.62 V. However, it was observed at pH 7 and 10 mM glucose concentration of maximum oxidation peak voltage at 1.73 V, the peak value of 1.93 mA. This measured power in the cell environment of pH 5, 15 mM glucose concentration maximum power of 17.06 μWcm-2; environment at pH 7, 25 mM glucose concentration maximum power of 21.63 μWcm-2.
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Hsu, Chia-Hong, and 徐佳宏. "Glucose dehydrogenase from Thermus thermophilus applied to Biofuel Cells." Thesis, 2005. http://ndltd.ncl.edu.tw/handle/64917504353887197245.
Full textAbstract:
碩士元智大學
化學工程學系
93
Biofuel cells are miniature power-generating systems that convert chemical energy to electrical energy by using biocatalysts to catalyze the oxidation of organic substances. Because of its insensitivity to oxygen and high catalytic efficiency, glucose dehydrogenase is an ideal anodic catalyst for biofuel cells. However, the heat instability of this enzyme inherently limits its application in the bioanode. In this research, a thermostable glucose dehydrogenase was isolated from Thermus thermophilus. Utilizing the thermostable glucose dehydrogenase as the catalyst and potassium ferrocyanide as the mediator, we successfully produced a thermostable anodic system. The effects of glucose concentration, salt concentration and temperature on current density were evaluated. The glucose dehydrogenase in Thermus thermophilus was partially purified by the ammonium sulfate fractionation and phenyl-sepharose chromatography. The activity of the glucose dehydrogenase at every step was determined by dye-reduction method. In the study for anode of biofuel cell, the glucose dehydrogenase gave a current density of 52 μA cm-2 at 0.35 V with Ag/AgCl as a reference at 37oC. When the operating temperature was raised to 70oC , an anodic current density of 127 μA cm-2 at 0.35 V was obtained. The results show that the glucose dehydrogenase from Thermus thermophilus is a thermostable enzyme and has a wide reaction temperature. Its acitivity increased as the temperature was increased. The biofuel cell would get better efficiency by using the enzyme at higher operating temperatures.