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      Ionic Liquid‐Assisted Electrocatalytic NO Reduction to NH 3 by P‐Doped MoS 2

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          Abstract

          Ambient NH 3 electrosynthesis from NO reduction reaction (NORR) is attractive in replacing the industrial Haber‐Bosch route; however, the competitive hydrogen evolution reaction (HER) in aqueous electrolyte typically induces a limited selectivity and activity toward NH 3 production. Herein, hierarchical P‐doped MoS 2 nanospheres are developed as the NORR electrocatalyst in an ionic liquid (IL) electrolyte for catalyzing the reduction of NO to NH 3 with a maximal Faradaic efficiency of 69 % (−0.6 V vs RHE) and a peak yield rate of 388.3 μg h −1 mg cat. −1 (−0.7 V vs RHE), both of which are comparable to the best‐reported results. Moreover, the catalyst also shows stable NORR activity over 30 h and 6 cycles. Theoretical analyses further reveal that the P dopants in MoS 2 facilitate the activation and hydrogenation of NO. Besides, the employment of hydrophobic IL electrolyte also slows down the HER kinetics effectively.

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          Electronics and optoelectronics of two-dimensional transition metal dichalcogenides.

          Qing Hua Wang, Kourosh Kalantar-Zadeh, Andras Kis … (2012)
          The remarkable properties of graphene have renewed interest in inorganic, two-dimensional materials with unique electronic and optical attributes. Transition metal dichalcogenides (TMDCs) are layered materials with strong in-plane bonding and weak out-of-plane interactions enabling exfoliation into two-dimensional layers of single unit cell thickness. Although TMDCs have been studied for decades, recent advances in nanoscale materials characterization and device fabrication have opened up new opportunities for two-dimensional layers of thin TMDCs in nanoelectronics and optoelectronics. TMDCs such as MoS(2), MoSe(2), WS(2) and WSe(2) have sizable bandgaps that change from indirect to direct in single layers, allowing applications such as transistors, photodetectors and electroluminescent devices. We review the historical development of TMDCs, methods for preparing atomically thin layers, their electronic and optical properties, and prospects for future advances in electronics and optoelectronics.
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            Biomimetic hydrogen evolution: MoS2 nanoparticles as catalyst for hydrogen evolution.

            Berit Hinnemann, Poul Moses, Jacob Bonde … (2005)
            The electrochemical hydrogen evolution reaction is catalyzed most effectively by the Pt group metals. As H2 is considered as a future energy carrier, the need for these catalysts will increase and alternatives to the scarce and expensive Pt group catalysts will be needed. We analyze the ability of different metal surfaces and of the enzymes nitrogenase and hydrogenase to catalyze the hydrogen evolution reaction and find a necessary criterion for high catalytic activity. The necessary criterion is that the binding free energy of atomic hydrogen to the catalyst is close to zero. The criterion enables us to search for new catalysts, and inspired by the nitrogenase active site, we find that MoS2 nanoparticles supported on graphite are a promising catalyst. They catalyze electrochemical hydrogen evolution at a moderate overpotential of 0.1-0.2 V.
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              Rational design of electrocatalysts and photo(electro)catalysts for nitrogen reduction to ammonia (NH3) under ambient conditions

              Shi-Zhang Qiao, Chunxian Guo, Jingrun Ran … (2018)
              This perspective highlights the rational design of efficient electrocatalysts and photo(electro)catalysts for N 2 reduction to ammonia (NH 3 ) under ambient conditions. As one of the most important chemicals and carbon-free energy carriers, ammonia (NH 3 ) has a worldwide annual production of ∼150 million tons, and is mainly produced by the traditional high-temperature and high-pressure Haber–Bosch process which consumes massive amounts of energy. Very recently, electrocatalytic and photo(electro)catalytic reduction of N 2 to NH 3 , which can be performed at ambient conditions using renewable energy, have received tremendous attention. The overall performance of these electrocatalytic and photo(electro)catalytic systems is largely dictated by their core components, catalysts. This perspective for the first time highlights the rational design of electrocatalysts and photo(electro)catalysts for N 2 reduction to NH 3 under ambient conditions. Fundamental theory of catalytic reaction pathways for the N 2 reduction reaction and the corresponding material design principles are introduced first. Then, recently developed electrocatalysts and photo(electro)catalysts are summarized, with a special emphasis on the relationship between their physicochemical properties and NH 3 production performance. Finally, the opportunities in this emerging research field, in particular, the strategy of combining experimental and theoretical techniques to design efficient and stable catalysts for NH 3 production, are outlined.
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                Author and article information

                Contributors
                Journal
                Title: ChemCatChem
                Abbreviated Title: ChemCatChem
                Publisher: Wiley
                ISSN (Print): 1867-3880
                ISSN (Electronic): 1867-3899
                Publication date Created: February 08 2023
                Publication date (Electronic): January 04 2023
                Publication date (Print): February 08 2023
                Volume: 15
                Issue: 3
                Affiliations
                [1 ] Information Technology Research Institute Shenzhen Institute of Information Technology Shenzhen 518172 P. R. China
                [2 ] MOE Key Laboratory of New Processing Technology for Non-Ferrous Metals and Materials, and Guangxi Key Laboratory of Processing for Non-Ferrous Metals and Featured Materials School of Resource Environments and Materials Guangxi University Nanning 530004 P. R. China
                [3 ] School of Chemical Engineering and Materials Tianjin University of Science and Technology Tianjin 300457 P. R. China
                [4 ] College of Chemistry Zhengzhou University Zhengzhou 450000 P. R. China
                [5 ] Institute for Advanced Study Chengdu University Chengdu 610106 Sichuan P. R. China
                [6 ] ShenSi Lab Shenzhen Institute for Advanced Study University of Electronic Science and Technology of China Longhua Shenzhen 518110 P. R. China
                Article
                DOI: 10.1002/cctc.202201411
                SO-VID: 9f9c615a-a72a-48f4-a1d4-a4773db0bd9e
                Copyright © © 2023
                License:

                http://onlinelibrary.wiley.com/termsAndConditions#vor

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