Статті в журналах: "Nitrogen reduction reaction (NRR)"

1

Basu, Jaydeep, and Sanjib Ganguly. "Electrocatalytic Nitrogen Reduction Reaction (NRR)." Resonance 28, no. 2 (February 16, 2023): 279–91. http://dx.doi.org/10.1007/s12045-023-1548-x.

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Wang, Weiping, Xiaomiao Wang, Yunpeng Sun, Ye Tian, Xiaoxu Liu, Ke Chu, and Junjie Li. "Ultrasmall iridium nanoparticles on graphene for efficient nitrogen reduction reaction." New Journal of Chemistry 46, no. 12 (2022): 5464–69. http://dx.doi.org/10.1039/d1nj05843f.

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Ultrasmall iridium nanoparticles on reduced graphene oxide (Ir/RGO) exhibited a high NRR activity, attributed to the RGO-induced upshifting of the d-band center for active Ir sites, leading to decreased NRR energy barriers.

3

Wu, Jie, ZhongXu Wang, Siwei Li, Siqi Niu, Yuanyuan Zhang, Jing Hu, Jingxiang Zhao, and Ping Xu. "FeMoO4 nanorods for efficient ambient electrochemical nitrogen reduction." Chemical Communications 56, no. 50 (2020): 6834–37. http://dx.doi.org/10.1039/d0cc02217a.

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4

Liu, Yongqin, Liang Huang, Xinyang Zhu, Youxing Fang, and Shaojun Dong. "Coupling Cu with Au for enhanced electrocatalytic activity of nitrogen reduction reaction." Nanoscale 12, no. 3 (2020): 1811–16. http://dx.doi.org/10.1039/c9nr08788e.

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The electrochemical nitrogen reduction reaction (NRR) under ambient conditions is currently attracting intense attention, but it still remains a great challenge to develop highly selective and active NRR electrocatalysts.

5

Liu, Yunliang, Peiji Deng, Ruqiang Wu, Xiaoli Zhang, Chenghua Sun, and Haitao Li. "Oxygen vacancies for promoting the electrochemical nitrogen reduction reaction." Journal of Materials Chemistry A 9, no. 11 (2021): 6694–709. http://dx.doi.org/10.1039/d0ta11522c.

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Recent advances on the detection, preparation and application of oxygen vacancies (OVs) for the electro-nitrogen fixation process with a focus on the generating strategies of OVs, evaluation method and their role in NRR.

6

Liu, Kang, Junwei Fu, Li Zhu, Xiaodong Zhang, Hongmei Li, Hui Liu, Junhua Hu, and Min Liu. "Single-atom transition metals supported on black phosphorene for electrochemical nitrogen reduction." Nanoscale 12, no. 8 (2020): 4903–8. http://dx.doi.org/10.1039/c9nr09117c.

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Electrochemical nitrogen reduction reaction (NRR) is a promising route to produce ammonia under mild conditions. Single-atom W supported on BP was screened as a promising electrocatalyst with high catalytic activity, stability, and selectively for NRR.

7

Chen, Jiangyue, Hui Cheng, Liang-Xin Ding, and Haihui Wang. "Competing hydrogen evolution reaction: a challenge in electrocatalytic nitrogen fixation." Materials Chemistry Frontiers 5, no. 16 (2021): 5954–69. http://dx.doi.org/10.1039/d1qm00546d.

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The electrocatalytic N₂ reduction reaction (NRR) under mild conditions is a promising candidate for NH₃ synthesis. Nevertheless, competition between the H₂ evolution reaction and the NRR results in a low NH₃ yield rate and poor faradaic efficiency.

8

Milazzo, Rachela Gabriella, Marco Leonardi, Giuseppe Tranchida, Silvia Scalese, Luca Pulvirenti, Guido Gugliemo Condorelli, Corrado Bongiorno, Salvatore Lombardo, and Stefania M. S. Privitera. "Iron Based Catalysts for Nitrogen Reduction Reaction." ECS Meeting Abstracts MA2022-02, no. 48 (October 9, 2022): 1809. http://dx.doi.org/10.1149/ma2022-02481809mtgabs.

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Ammonia (NH3) is a fundamental feedstock for the global population not only for its wide use as fertilizer and chemical, but also for its potential as energy storage medium. Its synthesis at the industrial scale is based on the well-known Haber Bosch process, operating at high temperature (400-500°C) and high pressure (150-300atm), thus making it highly pollutant. Considering the global climate emergency, it is mandatory to develop a green ammonia synthesis that relies on milder conditions and may adopt renewable energy sources. The electrochemical synthesis, of NH3 from N2 and H2O at ambient conditions and using renewable energy driven electricity could be a promising approach. An efficient electrochemical ammonia synthesis however, is currently still lacking. The main reasons are the absence of adequate catalysts capable of dissociating the N2 triple bond and the competition with the hydrogen evolution reaction (HER) at the cathode, since the required potential is close to that of nitrogen reduction reaction (NRR), required for the ammonia formation. There are some reaction models in the literature but it is commonly accepted that the dissociative adsorption of N2 is the rate limiting step and extensive research has been done on nitrogen interaction with metal surfaces. Ru, Co, Bi, Au, Fe, Mo, etc based materials have been extensively tested for the green ammonia synthesis, but results are still conflicting also because a complete evaluation of environmental contaminations is still lacking. In this work we adopted as NRR catalyst Fe based nanoparticles on carbon cloth substrate via a simple and fast electroless deposition technique. We prepared a FeCl3 solutions with different concentrations in the range 1-10mM and deposited a drop on (3x1.5) cm2 samples of carbon cloth, on a hot plate, at 80°C. After evaporation of the water, the as deposited substrates were dipped in NaBH4 solution while stirring. The catalyst morphology has been studied by Scanning Electron Microscopy (SEM), as a function of the concentration. Very small particles, with a size ranging from 10 to 70nm, were obtained with the most diluted solution. The cluster size increases with increasing FeCl3 concentration in the solution, giving rise to strong coalescence effects and to the formation of a thicker and continuous layer in the case of the most concentrated solution. Scanning Transmission electron Microscopy (STEM) and Electron Energy Loss Spectroscopy (EELS) have been adopted to determine the composition. EELS spectra showed that the iron L-edge is that typical of Fe3O4 materials. The electrochemical ability to reduce nitrogen, with the formation of ammonia, was evaluated in a standard two compartment cell, with a phosphate buffered solution (PBS 0.1M) adopting a Zirfon membrane as a gas separator. Ar or N2 gas (both with a purity of 99.9999%) flowed in the cathode chamber after going through an acidic trap and a water trap, to be further purified. A rigorous protocol has been adopted to evaluate the ammonia production, including a two steps measurement of the environmental ammonia at the open circuit potential. The ammonia was measured by spectrophotometric analysis using the indophenol blue method. The electrochemical production of ammonia was obtained by chronoamperometry under constant voltage. For the iron-based catalysts, a very efficient activation procedure has been developed, based on cyclic voltammetry under N2 flow. The activation process allows an improvement up to 10 times in the ammonia generation rate. Moreover, a strong correlation has been found between the particle size of the catalyst and its activity for NRR, with the best results achieved with the sample covered with nanoparticles, exhibiting also the highest electrochemical active area. Iron based nanoparticles showed excellent activity for NRR, with a faradaic efficiency of 15% at -0.35 V vs RHE and a maximum ammonia production rate of 85µg mg-1 cat h-1. Acknowledgements:This project has received funding from the European Union’s Horizon 2020 research and innovation programme under grant agreement No101006941.

9

Johnson, Denis, and Abdoulaye Djire. "Improving the Selectivity of Nitrogen Reduction Reaction through the Mars-Van Krevelen Mechanism." ECS Meeting Abstracts MA2022-02, no. 49 (October 9, 2022): 1921. http://dx.doi.org/10.1149/ma2022-02491921mtgabs.

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The electrochemical nitrogen reduction reaction (NRR) process is an attractive alternative to minimizing the energy and greenhouse gas footprint from current ammonia (NH3) production processes. Most NRR catalysts operate through utilizing an associative or dissociative mechanism, during which the NRR competes with the hydrogen evolution reaction (HER), resulting in low selectivity. In this presentation, we report on a new active catalyst for NRR that operates through the Mars-van Krevelen (MvK) mechanism to increase the selectivity of NRR towards NH3. This new catalyst, two-dimensional (2D) Ti2N nitride MXene, was synthesized via an oxygen-assisted molten salt fluoride etching technique. We confirmed its phase purity and stability in aqueous electrolytes using various characterization techniques, including Raman, X-ray diffraction, and UV-Vis. The Ti2N nitride MXene catalyst achieved a high Faradaic efficiency (FE) of 19.85% towards NH3 at an applied potential of –250 mV vs. RHE with a yield of 11.33 μg/cm2/hr in a 0.1 m hydrochloric acid (HCl) N2-saturated electrolyte. Electrocatalytic activity and selectivity obtained in an Ar-saturated electrolyte confirm that the new catalyst operates through an MvK mechanism. These results can be expanded to a broad class of systems enabling the MvK mechanism and constitute the foundation of NRR technology based on MXenes.

10

Johnson, Denis, and Abdoulaye Djire. "(Digital Presentation) Achieving High Selectivity for the Nitrogen Reduction Reaction through the Mars-Van Krevelen Mechanism." ECS Meeting Abstracts MA2022-01, no. 36 (July 7, 2022): 1548. http://dx.doi.org/10.1149/ma2022-01361548mtgabs.

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Electrochemical nitrogen reduction reaction (NRR) technology is a viable alternative to reducing the energy and greenhouse gas footprint from the current ammonia (NH3) production technology. Most NRR catalysts suffer from low selectivity towards NH3 because they operate by using an associative or dissociative mechanism, during which the NRR competes with the hydrogen evolution reaction (HER). In this presentation, we report on a new catalyst and untapped mechanism for NRR to increase the selectivity towards NH3. This untapped Mars-van Krevelen (MvK) mechanism reduces the competition between NRR and HER by eliminating the sluggish hydrogenation reactions of the dissolved N2 molecule. The new catalyst, two-dimensional (2D) Ti2N nitride MXene, was synthesized via an oxygen-assisted molten salt fluoride etching technique. We confirmed its phase purity and stability in aqueous electrolytes using various characterization techniques, including x-ray diffraction (XRD), Raman spectroscopy, scanning electron microscopy (SEM), and cyclic voltammetry (CV). Through an MvK mechanism, the Ti2N nitride MXene catalyst achieved a high Faradaic efficiency (FE) of 19.85% towards NH3 at an applied potential of –250 mV vs. RHE with a yield of 11.33 μg/cm2/hr in a 0.1M hydrochloric acid (HCl) N2-saturated electrolyte. These results constitute the foundation of NRR technology based on MXenes and can be expanded to a broad class of systems evoking the MvK mechanism.

11

Wang, Haiyan, Yuzhuo Chen, Ruxue Fan, Jiadong Chen, Zhe Wang, Shanjun Mao, and Yong Wang. "Selective Electrochemical Reduction of Nitrogen to Ammonia by Adjusting the Three-Phase Interface." Research 2019 (November 30, 2019): 1–12. http://dx.doi.org/10.34133/2019/1401209.

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The electrochemical nitrogen reduction reaction (NRR) provides a sustainable and alternative avenue to the Haber-Bosch process for ammonia (NH3) synthesis. Despite the great efforts made on catalysts and electrolytes, unfortunately, current NRR suffers from low selectivity due to the overwhelming competition with the hydrogen evolution reaction (HER). Here, we present an adjusted three-phase interface to enhance nitrogen (N2) coverage on a catalyst surface and achieve a record-high Faradic efficiency (FE) up to 97% in aqueous solution. The almost entirely suppressed HER process combined with the enhanced NRR activity, benefiting from the efficient three-interface contact line, is responsible for the excellent selectivity toward NH3, as evidenced by the theoretical and experimental results. Our strategy also demonstrates the applicability to other catalysts that feature strong H adsorption ability, to boost the FE for NH3 synthesis above 90% and to improve the NRR activity by engineering the catalysts.

12

Zhang, Bikun, Jian Zhou, Stephen R. Elliott, and Zhimei Sun. "Two-dimensional molybdenum carbides: active electrocatalysts for the nitrogen reduction reaction." Journal of Materials Chemistry A 8, no. 45 (2020): 23947–54. http://dx.doi.org/10.1039/d0ta07039d.

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13

Han, Bing, Haihong Meng, Fengyu Li, and Jingxiang Zhao. "Fe3 Cluster Anchored on the C2N Monolayer for Efficient Electrochemical Nitrogen Fixation." Catalysts 10, no. 9 (August 29, 2020): 974. http://dx.doi.org/10.3390/catal10090974.

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Under the current double challenge of energy and the environment, an effective nitrogen reduction reaction (NRR) has become a very urgent need. However, the largest production of ammonia gas today is carried out by the Haber–Bosch process, which has many disadvantages, among which energy consumption and air pollution are typical. As the best alternative procedure, electrochemistry has received extensive attention. In this paper, a catalyst loaded with Fe3 clusters on the two-dimensional material C2N (Fe3@C2N) is proposed to achieve effective electrochemical NRR, and our first-principles calculations reveal that the stable Fe3@C2N exhibits excellent catalytic performance for electrochemical nitrogen fixation with a limiting potential of 0.57 eV, while also suppressing the major competing hydrogen evolution reaction. Our findings will open a new door for the development of non-precious single-cluster catalysts for effective nitrogen reduction reactions.

14

Liu, Yiwen, Xianbin Meng, Zhiqiang Zhao, Kai Li, and Yuqing Lin. "Assembly of Hydrophobic ZIF-8 on CeO2 Nanorods as High-Efficiency Catalyst for Electrocatalytic Nitrogen Reduction Reaction." Nanomaterials 12, no. 17 (August 27, 2022): 2964. http://dx.doi.org/10.3390/nano12172964.

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The electrocatalytic nitrogen reduction reaction (NRR) can use renewable electricity to convert water and N2 into NH3 under normal temperature and pressure conditions. However, due to the competitiveness of the hydrogen evolution reaction (HER), the ammonia production rate (RNH3) and Faraday efficiency (FE) of NRR catalysts cannot meet the needs of large-scale industrialization. Herein, by assembling hydrophobic ZIF-8 on a cerium oxide (CeO2) nanorod, we designed an excellent electrocatalyst CeO2-ZIF-8 with intrinsic NRR activity. The hydrophobic ZIF-8 surface was conducive to the efficient three-phase contact point of N2 (gas), CeO2 (solid) and electrolyte (liquid). Therefore, N2 is concentrated and H+ is deconcentrated on the CeO2-ZIF-8 electrocatalyst surface, which improves NRR and suppresses HER and finally CeO2-ZIF-8 exhibits excellent NRR performance with an RNH3 of 2.12 μg h−1 cm−2 and FE of 8.41% at −0.50 V (vs. RHE). It is worth noting that CeO2-ZIF-8 showed excellent stability in the six-cycle test, and the RNH3 and FE variation were negligible. This study paves a route for inhibiting the competitive reaction to improve the NRR catalyst activity and may provide a new strategy for NRR catalyst design.

15

Zhang, Quan, Fang Luo, Ying Ling, Shenglin Xiao, Min Li, Konggang Qu, Yangang Wang, Jingxiang Xu, Weiwei Cai, and Zehui Yang. "Identification of functionality of heteroatoms in boron, nitrogen and fluorine ternary-doped carbon as a robust electrocatalyst for nitrogen reduction reaction powered by rechargeable zinc–air batteries." Journal of Materials Chemistry A 8, no. 17 (2020): 8430–39. http://dx.doi.org/10.1039/d0ta01572e.

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Li, Weixin, Wei Fang, Chen Wu, Khang Ngoc Dinh, Hao Ren, Lei Zhao, Chuntai Liu, and Qingyu Yan. "Bimetal–MOF nanosheets as efficient bifunctional electrocatalysts for oxygen evolution and nitrogen reduction reaction." Journal of Materials Chemistry A 8, no. 7 (2020): 3658–66. http://dx.doi.org/10.1039/c9ta13473e.

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Two dimensional (2D) bimetal–MOFs (CoxFe–MOF) nanosheets have been successfully synthesized, which can simultaneously meet the requirement of both OER and NRR, thus providing the potential for coupling both OER and NRR in a full-cell configuration.

17

Rostamikia, Gholamreza, Sharad Maheshwari, and Michael J. Janik. "Elementary kinetics of nitrogen electroreduction to ammonia on late transition metals." Catalysis Science & Technology 9, no. 1 (2019): 174–81. http://dx.doi.org/10.1039/c8cy01845f.

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Huo, Jinrong, Haocong Wei, Kai Zhang, Chenxu Zhao, and Chaozheng He. "Nitrogen Reduction Reaction Catalyzed by Diatomic Metals Supported by N-Doped Graphite." Catalysts 13, no. 1 (December 26, 2022): 49. http://dx.doi.org/10.3390/catal13010049.

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In this article, for the transition metal-nitrogen ligand Mn-M@N6-C (M = Ag, Bi, Cd, Co, Cr, Cu, Fe, Hf, Ir, Mo, Nb, Ni, Os, Pd, Pt, Re, Rh, Ru, Sc, Ta, Tc, V, Y, Zn, Zr, Ti, W), by comparing the amount of change in the length of the N-N triple-bond, and calculating the adsorption energy of N2 and the change of charge around N2, it is shown that the activation effect of Sc, Ti, Y, Nb-Mn@N6-C on the single-atomic layer of graphite substrate is relatively good. The calculation of structural stability shows that the Mn-M@N6-C (M = Sc, Ti, Y) load is relatively stable when it is on the single-atomic layer of the graphite substrate. Through calculations, a series of data such as the adsorption free energy and reaction path are obtained, and the final results show that the preferred reaction mechanism of NRR is the alternating path on Mn-Ti@N6-C, and the reaction limit potential is only 0.16 eV, Mn-Ti@N6-C and has good NRR activity. In addition, the vertical path on Mn-Y@N6-C has a reaction limit potential of 0.39 eV. Mn-Y@N6-C also has good NRR catalyzing activity.

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Xu, Fanfan, Linlin Zhang, Xin Ding, Meiyu Cong, Yu Jin, Lin Chen, and Yan Gao. "Selective electroreduction of dinitrogen to ammonia on a molecular iron phthalocyanine/O-MWCNT catalyst under ambient conditions." Chemical Communications 55, no. 94 (2019): 14111–14. http://dx.doi.org/10.1039/c9cc06574a.

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Li, Ruizhi, Jie Liang, Tingshuai Li, Luchao Yue, Qian Liu, Yonglan Luo, Mohamed S. Hamdy, Yibai Sun, and Xuping Sun. "Recent advances in MoS₂-based materials for electrocatalysis." Chemical Communications 58, no. 14 (2022): 2259–78. http://dx.doi.org/10.1039/d1cc04004a.

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Ma, Zuju, Chengwei Xiao, Zhitao Cui, Wei Du, Qiaohong Li, Rongjian Sa, and Chenghua Sun. "Defective Fe3GeTe2 monolayer as a promising electrocatalyst for spontaneous nitrogen reduction reaction." Journal of Materials Chemistry A 9, no. 11 (2021): 6945–54. http://dx.doi.org/10.1039/d0ta10494a.

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Ouyang, Wencheng, Qiuming Zhi, Lele Gong, Hao Sun, Minghui Liu, Jing Zhang, Xiao Han, Zhenhai Xia, and Lipeng Zhang. "Rational design of boron-containing co-doped graphene as highly efficient electro-catalysts for the nitrogen reduction reaction." Journal of Materials Chemistry A 9, no. 43 (2021): 24590–99. http://dx.doi.org/10.1039/d1ta04327g.

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The electrocatalytic nitrogen reduction reaction (NRR) under ambient conditions has been proposed as a sustainable alternative for nitrogen fixation and ammonia production in environmental and renewable energy fields.

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Younis, Muhammad Yawar, Somavia Ameen, Babar Iqbal, and Hamza Ijaz. "A Review on Advances in Electrocatalytic N2 Reduction to Ammonia." International Journal of Current Engineering and Technology 12, no. 02 (March 30, 2022): 114–21. http://dx.doi.org/10.14741/ijcet/v.12.2.3.

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Ammonia is one of the most important industrial chemicals which is prepared by the traditional Haber–Bosch process. Haber–Bosch process is an expensive process requiring higher temperature, pressure, and a lot of energy. Electrocatalytic nitrogen reduction reactions (NRR) have gained a lot of interest as the alternate method for the production of ammonia. For obtaining a higher yield, higher Faradic efficiency (PE), inhibition of side reactions e.g., hydrogen evolution reaction (HER), and reducing the production cost for ammonia by NRR, selection of appropriate catalysts, cell layout, and electrolyte selection are important controlling parameters for the NRR. Non-metallic catalysts are preferred over noble metallic catalysts due to their lower cost, more resources, and characteristic dorbital electron but have the issue of low selectivity due to the higher HER. The selectivity for the NRR can be improved by employing the catalysts with higher absorption of N2. PEM-type cells and the back-to-back cells are used to inhibit the HER. Apart from these factors, NRR is also dependent on other factors to obtain better experimental results e.g., no nitrides, removing the ammonia from contaminants sites, and controlling the experiment time.

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Zafari, Mohammad, Deepak Kumar, Muhammad Umer, and Kwang S. Kim. "Machine learning-based high throughput screening for nitrogen fixation on boron-doped single atom catalysts." Journal of Materials Chemistry A 8, no. 10 (2020): 5209–16. http://dx.doi.org/10.1039/c9ta12608b.

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Ling, Ying, Farhad M. D. Kazim, Shuangxiu Ma, Quan Zhang, Konggang Qu, Yangang Wang, Shenglin Xiao, Weiwei Cai, and Zehui Yang. "Strain induced rich planar defects in heterogeneous WS2/WO2 enable efficient nitrogen fixation at low overpotential." Journal of Materials Chemistry A 8, no. 26 (2020): 12996–3003. http://dx.doi.org/10.1039/c9ta13812a.

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Incorporation of WO₂ to WS₂ nanosheets can efficiently suppress the competitive hydrogen evolution reaction (HER) due to the reduction of edge defects and create new planar defects at heterointerfaces for nitrogen reduction reaction (NRR).

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Li, Tengfei, Xudong Yan, Lujun Huang, Jinghan Li, Lulu Yao, Qianying Zhu, Weiqiang Wang, et al. "Fluorine-free Ti3C2Tx (T = O, OH) nanosheets (∼50–100 nm) for nitrogen fixation under ambient conditions." Journal of Materials Chemistry A 7, no. 24 (2019): 14462–65. http://dx.doi.org/10.1039/c9ta03254a.

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Back, Seoin, and Yousung Jung. "On the mechanism of electrochemical ammonia synthesis on the Ru catalyst." Physical Chemistry Chemical Physics 18, no. 13 (2016): 9161–66. http://dx.doi.org/10.1039/c5cp07363d.

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The nitrogen reduction reaction (NRR) pathways involving various N–N dissociation steps are found to be comparable to the conventional associative mechanism. The competitive hydrogen adsorption and evolution is revealed to negatively affect the NRR for two reasons, an increase in NRR overpotentials as a function of partial H-coverages as well as a decreased number of active sites.

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Chen, Siru, Xuan Liu, Jiabin Xiong, Liwei Mi, Xue-Zhi Song, and Yanqiang Li. "Defect and interface engineering in metal sulfide catalysts for the electrocatalytic nitrogen reduction reaction: a review." Journal of Materials Chemistry A 10, no. 13 (2022): 6927–49. http://dx.doi.org/10.1039/d2ta00070a.

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Cao, Rong, Jie-Zhen Xia, and Qi Wu. "Computational Insight into Defective Boron Nitride Supported Double-Atom Catalysts for Electrochemical Nitrogen Reduction." Catalysts 12, no. 11 (November 10, 2022): 1404. http://dx.doi.org/10.3390/catal12111404.

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Designing highly selective and efficient double-atom electrocatalysts (DACs) is essential for achieving a superior nitrogen-reduction reaction (NRR) performance. Herein, we explored the defective boron nitride–supported cage-like double-atom catalysts to rummage the qualified NRR catalysts. Based on a systematic evaluation of the stability, N2 adsorption, NRR selectivity and activity of 10 DACs of TM1-TM2@VB-BN, we predicted Ru-Ti@VB-BN to be the NRR candidate with a limiting potential of −0.40 V. Compared to the corresponding single-atom catalysts, the introduction of Ti/Mo modulates the d-band center of the active metal atom, which improves the NRR performance. Moreover, the magnetic Ru-Ti dimer can facilitate the transfer of charge to molecular N2, ensuring a significant activation of the inert N≡N bond. This research not only opens up new avenues for designing boron nitride–supported DACs for NRR, but also deepens the understanding of DACs in N2 activation.

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Liu, Shiqiang, Zhiwen Cheng, Yawei Liu, Xiaoping Gao, Yujia Tan, Yuanyang Ren, and Zhemin Shen. "Boosting electrochemical nitrogen reduction reaction performance of two-dimensional Mo porphyrin monolayers via turning the coordination environment." Physical Chemistry Chemical Physics 23, no. 7 (2021): 4178–86. http://dx.doi.org/10.1039/d0cp06036d.

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Guo, Zhongyuan, Tianyi Wang, Haikun Liu, Siyao Qiu, Xiaoli Zhang, Yongjun Xu, Steven J. Langford, and Chenghua Sun. "Defective 2D silicon phosphide monolayers for the nitrogen reduction reaction: a DFT study." Nanoscale 14, no. 15 (2022): 5782–93. http://dx.doi.org/10.1039/d1nr08445c.

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Castellano-Varona, Blanca, Moussab Harb, Javier Araña, Luigi Cavallo, and Luis Miguel Azofra. "In silico design of novel NRR electrocatalysts: cobalt–molybdenum alloys." Chemical Communications 56, no. 87 (2020): 13343–46. http://dx.doi.org/10.1039/d0cc05921h.

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Leonardi, Marco, Giuseppe Tranchida, Roberto Corso, Rachela G. Milazzo, Salvatore A. Lombardo, and Stefania M. S. Privitera. "Role of the Membrane Transport Mechanism in Electrochemical Nitrogen Reduction Experiments." Membranes 12, no. 10 (October 2, 2022): 969. http://dx.doi.org/10.3390/membranes12100969.

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The electrochemical synthesis of ammonia through the nitrogen reduction reaction (NRR) is receiving much attention, since it is considered a promising alternative to the Haber–Bosch process. In NRR experiments, a Nafion membrane is generally adopted as a separator. However, its use is controversial since ammonia can be trapped in the membrane, to some extent, or even pass through it. We systematically investigate the interaction of a Nafion membrane with ammonia and with an electrolyte and compare it with Zirfon as a possible alternative separator. We show that Nafion containing ammonia can easily release it when immersed in a 0.1 M Na2SO4 ammonia-free electrolyte, due to the cation exchange mechanism (Na+-NH4+). Since Na2SO4 is a commonly adopted electrolyte for NRR experiments, this may cause serious measurement errors and non-reproducible results. The same experiments performed using the polysulfone Zirfon separator clearly show that it is immune to interactions with ammonia, because of its different ion conduction mechanism. The findings provide a deeper understanding of the choice of membrane and electrolyte to be adopted for NRR tests, and may allow one to obtain more accurate and reliable results.

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Yuan, Menglei, Yiling Bai, Jingxian Zhang, Tongkun Zhao, Shuwei Li, Hongyan He, Zhanjun Liu, Zhongde Wang, and Guangjin Zhang. "Work function regulation of nitrogen-doped carbon nanotubes triggered by metal nanoparticles for efficient electrocatalytic nitrogen fixation." Journal of Materials Chemistry A 8, no. 48 (2020): 26066–74. http://dx.doi.org/10.1039/d0ta08914a.

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The work function (W) is utilized as an effective descriptor to predict the electrochemical nitrogen reduction reaction (NRR) activity. The lower W value of M@NCNTs promotes the transfer of electrons from the catalyst surface to the adsorbed N₂.

35

Shu, Zheng, Hejin Yan, Hongfei Chen, and Yongqing Cai. "Mutual modulation via charge transfer and unpaired electrons of catalytic sites for the superior intrinsic activity of N₂ reduction: from high-throughput computation assisted with a machine learning perspective." Journal of Materials Chemistry A 10, no. 10 (2022): 5470–78. http://dx.doi.org/10.1039/d1ta10688k.

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36

Tan, Yao, Ying Xu, and Zhimin Ao. "Nitrogen fixation on a single Mo atom embedded stanene monolayer: a computational study." Physical Chemistry Chemical Physics 22, no. 25 (2020): 13981–88. http://dx.doi.org/10.1039/d0cp01963a.

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37

Zhao, Xue, Ziqiong Yang, Artem V. Kuklin, Glib V. Baryshnikov, Hans Ågren, Wenjing Wang, Xiaohai Zhou, and Haibo Zhang. "Potassium ions promote electrochemical nitrogen reduction on nano-Au catalysts triggered by bifunctional boron supramolecular assembly." Journal of Materials Chemistry A 8, no. 26 (2020): 13086–94. http://dx.doi.org/10.1039/d0ta04580b.

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Sustainable ambient electrochemical nitrogen reduction reaction has become a goal pursued by scientists, herein the potassium ion can effectively improve the E-NRR activity of Au anchored on the functional carrier.

38

Ferrara, Marcello, Michele Melchionna, Paolo Fornasiero, and Manuela Bevilacqua. "The Role of Structured Carbon in Downsized Transition Metal-Based Electrocatalysts toward a Green Nitrogen Fixation." Catalysts 11, no. 12 (December 15, 2021): 1529. http://dx.doi.org/10.3390/catal11121529.

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Electrocatalytic Nitrogen Reduction Reaction (NRR) to ammonia is one of the most recent trends of research in heterogeneous catalysis for sustainability. The stark challenges posed by the NRR arise from many factors, beyond the strongly unfavored thermodynamics. The design of efficient heterogeneous electrocatalysts must rely on a suitable interplay of different components, so that the majority of research is focusing on development of nanohybrids or nanocomposites that synergistically harness the NRR sequence. Nanostructured carbon is one of the most versatile and powerful conductive supports that can be combined with metal species in an opportune manner, so as to guide the correct proceeding of the reaction and boost the catalytic activity.

39

Wang, Zengyao, Jianfeng Shen, Wenzhi Fu, Jiangwen Liao, Juncai Dong, Peiyuan Zhuang, Ziyi Cao, Zhuolin Ye, Jiangyue Shi, and Mingxin Ye. "Controlled oxygen vacancy engineering on In2O3−x/CeO2−y nanotubes for highly selective and efficient electrocatalytic nitrogen reduction." Inorganic Chemistry Frontiers 7, no. 19 (2020): 3609–19. http://dx.doi.org/10.1039/d0qi00749h.

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Introducing and adjusting the oxygen vacancies (V_O) of transition metal oxides has been proposed as a significant and effective way to tackle the sluggish nitrogen reduction reaction (NRR) in the electrocatalysis process.

40

Fang, Bin, Junjie Yao, Xiaojun Zhang, Liang Ma, Yaqi Ye, Jiayi Tang, Guifu Zou, Junchang Zhang, Lin Jiang, and Yinghui Sun. "A large scaled-up monocrystalline 3R MoS2 electrocatalyst for efficient nitrogen reduction reactions." New Journal of Chemistry 45, no. 5 (2021): 2488–95. http://dx.doi.org/10.1039/d0nj05264g.

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Large-scale 3R MoS₂ was shown to be an efficient electrocatalyst for the NRR, and the NRR performance can be enhanced via improving the crystallinity of MoS₂ due to decreased resistance.

41

Liu, Xin, Chenyin Li, Fang Xu, Guohong Fan, and Hong Xu. "Density functional theory study of nitrogen-doped black phosphorene doped with monatomic transition metals as high performance electrocatalysts for N₂ reduction reaction." Nanotechnology 33, no. 24 (March 23, 2022): 245401. http://dx.doi.org/10.1088/1361-6528/ac5929.

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Abstract Ammonia (NH3) is an essential resource in human production and living activities, and its demand has been rising in recent years. The catalytic synthesis of NH3 from N2 under mild conditions, inspired by biological nitrogen fixation, has piqued the interest of researchers. In this paper, density functional theory (DFT) calculations were used to investigate the catalytic activity, mechanism, and selectivity of the TM embedded nitrogen-doped phosphorene as high-performance nitrogen reduction reaction (NRR) electrocatalysts in depth. The results show that Nb- and Mo-doped catalysts present excellent catalytic performance, with low limiting potentials of −0.41 and −0.18 V, respectively. The Mo–N3–BP catalyst, for example, not only has an extremely low overpotential (−0.02 V), but also presents superior selectivity to effectively inhibit the HER competition reaction. A deeper look into the catalytic mechanism reveals a volcano relationship between the d-band center and the catalytic activity (Mo and Nb are located near the peak of the volcano-type curve). The d-band center and charge of the metal center can be regarded as effective descriptors for NRR activity on TM embedded nitrogen-doped phosphorene electrocatalysts, which hope to serve as a guiding principle for the design of high performance NRR single-atom catalyst in the future.

42

Utomo, Wahyu Prasetyo, Hao Wu, and Yun Hau Ng. "Quantification Methodology of Ammonia Produced from Electrocatalytic and Photocatalytic Nitrogen/Nitrate Reduction." Energies 16, no. 1 (December 20, 2022): 27. http://dx.doi.org/10.3390/en16010027.

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Nitrogen reduction reaction (NRR) and nitrate reduction reaction (NO3−RR) provide a potential sustainable route by which to produce ammonia, a next-generation energy carrier. Many studies have been conducted over the years, mainly emphasizing material design and strategies to improve catalytic performance. Despite significant achievements in material design and corresponding fundamental knowledge, the produced ammonia is still very limited, which makes it prone to bias. The presence of interferants (e.g., cations and sacrificial reagents), the pH of the solution, and improper analytical procedure can lead to the over or underestimation of ammonia quantification. Therefore, the selection of the appropriate ammonia quantification method, which meets the sample solution condition, along with the proper analytical procedures, is of great importance. In this review, the state-of-the-art ammonia quantification method is summarized, emphasizing the advantages, limitations, and practicality for NRR and NO3−RR studies. Fundamental knowledge of the quantification method is introduced. Perspective on the considerations for selecting the suitable quantification method and for performing the quantification process is also provided. Although non exhaustive, this focused review can be useful as a guide to design the experimental setup and procedure for more reliable ammonia quantification results.

43

Chung, Sunki, Hyungkuk Ju, and Jaeyoung Lee. "Water-Assisted Electrochemical Ammonia Synthesis on Electrospun Cobalt-Molybdenum Carbide Composite." ECS Meeting Abstracts MA2022-01, no. 38 (July 7, 2022): 1703. http://dx.doi.org/10.1149/ma2022-01381703mtgabs.

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The electrochemical synthesis of ammonia under ambient condition has attracted significant attention as an alternative route for green ammonia production. However, competing hydrogen evolution reaction (HER) hinders selective ammonia synthesis through electrochemical nitrogen reduction reaction (NRR). For the broad adoption of such technology in industries, it is essential to overcome poor selectivity of NRR by developing effective electrocatalysts and controlling the reactant at the interface between electrode and electrolyte.[1,2] In this study, we prepared cobalt-molybdenum carbide-carbon nanofiber via electrospinning method as a selective NRR catalyst. Furthermore, we reveal the relationship between water adsorption ability and NRR selectivity on biphasic catalyst using isotopic-labeling and in-situ analyses. Reference [1] Journal of Electroanalytical Chemistry 2021, 896, 115157. [2] Journal of Energy Chemistry 2022, 67, 474–482.

44

Jiang, Qiuling, Yanan Meng, Kai Li, Ying Wang, and Zhijian Wu. "Screening Highly Efficient Hetero-Diatomic Doped PC6 Electrocatalysts for Selective Nitrogen Reduction to Ammonia." Journal of The Electrochemical Society 168, no. 11 (November 1, 2021): 116519. http://dx.doi.org/10.1149/1945-7111/ac3aba.

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Searching for highly efficient electrocatalysts toward nitrogen reduction reaction (NRR) is an important but challenging task for nitrogen utilization in industry. Here we have systematically designed a series of hetero-diatomic catalysts (DACs), in which transition metal atoms (Ti, V, Cr, Mn, Fe, Co, and Ni) are dispersed on PC6 monolayer to form AB@PC6 (A, B = Ti, V, Cr, Mn, Fe, Co, and Ni). Employing density functional theory (DFT) calculation, the V and Cr co-doped PC6 monolayer (VCr@PC6) among the 21 AB@PC6 catalysts is the most promising catalyst due to its low limiting potential of −0.41 V, relatively low energy barrier, and high ammonia selectivity toward hydrogen evolution reaction (HER). Insights on the high NRR activity of VCr@PC6 are also explored. The synergistic effect in DACs facilitates the electron transfer from metal pairs to PC6 monolayer, as well as suppresses the HER, leading to high selectivity and Faradaic efficiency. This work not only aims to seek the efficient DACs towards N2 reduction but also provides insights towards synergistic effects between hetero-atoms for the rational design of DACs.

45

Guo, Ruijie, Min Hu, Weiqing Zhang, and Jia He. "Boosting Electrochemical Nitrogen Reduction Performance over Binuclear Mo Atoms on N-Doped Nanoporous Graphene: A Theoretical Investigation." Molecules 24, no. 9 (May 8, 2019): 1777. http://dx.doi.org/10.3390/molecules24091777.

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Exploration of efficient catalysts is a priority for the electrochemical nitrogen reduction reaction (NRR) in order to receive a high product yield rate and faradaic efficiency of NH3, under ambient conditions. In the present contribution, the binding free energy of N2, NNH, and NH2 were used as descriptors to screen the potential NRR electrocatalyst among different single or binuclear transition metal atoms on N-doped nanoporous graphene. Results showed that the binuclear Mo catalyst might exhibit the highest catalytic activity. Further free energy profiles confirmed that binuclear Mo catalysts possess the lowest potential determining step (hydrogenation of NH2* to NH3). The improved activities could be ascribed to a down-shift of the density of states for Mo atoms. This investigation could contribute to the design of a highly active NRR electrocatalyst.

46

Li, Kai, Yan Li, Kun Jiang, Tao Li, Yun-Quan Liu, Shuirong Li, Duo Wang, and Yueyuan Ye. "The Importance of Molybdenum(IV) Active Sites in Promoting Electrochemical Reduction of N₂ to NH₃ with MoFe Bimetallic Catalysts." Journal of The Electrochemical Society 168, no. 12 (December 1, 2021): 126518. http://dx.doi.org/10.1149/1945-7111/ac3ff2.

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To overcome the low faradaic efficiency (FE) of single Mo or Fe based electrocatalysts in nitrogen reduction reactions (NRR) due to the competition from the hydrogen evolution reaction (HER), a series of bimetallic MoFe compound catalysts were prepared under an NH3 atmosphere through a facile precipitation-pyrolysis method. The formed tetravalent Mo was found to be capable of inducing better electronic interactions between the surface nitrogen species and the Fe metal groups, thus improving the FE. It was demonstrated that the prepared ternary MoFe-N catalyst exhibited a remarkable FE of 33.26 % and a high NH3 yield rate of 33.31 μg h−1 mg−1 cat. for NRR, which was believed to have been caused by an obvious change in the valence of Mo that resulted in a lower HER activity. X-ray photoelectron spectroscopy analysis further revealed that thermal processing under an NH3 atmosphere formed the Mo(IV) active sites in Mo–N bond, which led to a significant suppression in HER activity. Finally, through the study of the surface hydrogenation mechanism, it was concluded that the synergistic effect of the adsorbed H* and Mo active sites was the main reason for the improved performance of NRR.

47

Zhao, Wanghui, Lanlan Chen, Wenhua Zhang, and Jinlong Yang. "Single Mo1(W1, Re1) atoms anchored in pyrrolic-N3 doped graphene as efficient electrocatalysts for the nitrogen reduction reaction." Journal of Materials Chemistry A 9, no. 10 (2021): 6547–54. http://dx.doi.org/10.1039/d0ta11144a.

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Mo₁(W₁ and Re₁) supported by pyrrolic-N doped graphene (M₁/pyrrolic-N₃–G) are theoretically predicted as potential electrocatalysts for nitrogen reduction reaction (NRR) with high stability, activity and ammonia selectivity.

48

Mao, Yu-Jie, Lu Wei, Xin-Sheng Zhao, Yong-Sheng Wei, Jian-Wei Li, Tian Sheng, Fu-Chun Zhu, Na Tian, Zhi-You Zhou, and Shi-Gang Sun. "Excavated cubic platinum–iridium alloy nanocrystals with high-index facets as highly efficient electrocatalysts in N2 fixation to NH3." Chemical Communications 55, no. 63 (2019): 9335–38. http://dx.doi.org/10.1039/c9cc04034j.

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Excavated cubic Pt₉₃Ir₇ alloy nanocrystals enclosed by high-index {710} facets exhibit excellent electrocatalytic properties for the nitrogen reduction reaction (NRR) with high faradaic efficiency (40.8%) and NH₃ yield (28 μg h⁻¹ cm⁻²).

49

Yang, Sungbin, and Byungha Shin. "Enhancement of Li-Mediated Electrochemical Ammonia Synthesis By Modifying Main Element of Ylide Proton Shuttle." ECS Meeting Abstracts MA2022-02, no. 46 (October 9, 2022): 1721. http://dx.doi.org/10.1149/ma2022-02461721mtgabs.

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Ammonia is an essential chemical used various fields including agriculture and chemical engineering. It is also considered as one of the candidates for carbon-free hydrogen storage. Electrochemical nitrogen reduction reaction (ENRR) has been studied as an alternative to current energy-intensive and greenhouse gas emitting Habor-Bosch process. Lithium mediated nitrogen reduction reaction (Li-NRR), in which organic compounds replace water as the proton shuttle, is currently considered as the most promising route in terms of ammonia production rate. However, ethanol (EtOH), acommon proton shuttle in Li-NRR, has a limited electrochemical stability because it is prone to oxidation at the anode or can be consumed by forming byproducts at the cathode. Therefore, it is highly desirable to search for alternative proton shuttles. In this study, two different ylides—namely, tetrabutylphosphonium chloride (TBPCl) and tetrabutylammonium chloride (TBNCl)—were selected as the proton shuttle in place of EtOH. Both compounds showed spontaneous reaction with lithium nitride by forming ammonia. Both TBPCl and TBNCl showed a higher ammonia production rate and faradaic efficiency than EtOH. Interestingly, tetrabutylammonium chloride showed higher ammonia production rate than tetrabutylphosphonium chloride which may originate from the difference of the acidity. This work demonstrates the possibility of using ylides as an effective proton shuttle and points out the important role of the center atom of the ylides in Li-NRR.

50

Luo, Heng, Xiaoxu Wang, Chubin Wan, Lu Xie, Minhui Song, and Ping Qian. "A Theoretical Study of Fe Adsorbed on Pure and Nonmetal (N, F, P, S, Cl)-Doped Ti3C2O2 for Electrocatalytic Nitrogen Reduction." Nanomaterials 12, no. 7 (March 25, 2022): 1081. http://dx.doi.org/10.3390/nano12071081.

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The possibility of using transition metal (TM)/MXene as a catalyst for the nitrogen reduction reaction (NRR) was studied by density functional theory, in which TM is an Fe atom, and MXene is pure Ti3C2O2 or Ti3C2O2−x doped with N/F/P/S/Cl. The adsorption energy and Gibbs free energy were calculated to describe the limiting potentials of N2 activation and reduction, respectively. N2 activation was spontaneous, and the reduction potential-limiting step may be the hydrogenation of N2 to *NNH and the desorption of *NH3 to NH3. The charge transfer of the adsorbed Fe atoms to N2 molecules weakened the interaction of N≡N, which indicates that Fe/MXene is a potential catalytic material for the NRR. In particular, doping with nonmetals F and S reduced the limiting potential of the two potential-limiting steps in the reduction reaction, compared with the undoped pure structure. Thus, Fe/MXenes doped with these nonmetals are the best candidates among these structures.

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