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      NiFe layered double hydroxide nanosheet array for high-efficiency electrocatalytic reduction of nitric oxide to ammonia

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          Abstract

          A NiFe layered double hydroxide nanosheet array is designed as an efficient NORR catalyst for NH 3 electrosynthesis with a maximal FE of 82% and the highest yield rate of 1586.7 μg h −1 mg cat. −1, exceeding most recently reported results.

          Abstract

          Here, we demonstrate that under ambient conditions, a nickel-iron layered double hydroxide nanosheet array can exhibit a promising NORR performance, delivering a maximal faradaic efficiency of 82% and a corresponding yield rate of 112 μmol h −1 cm −2, along with high stability for over 30 h. This superior performance is further confirmed as a proof-of-concept for a Zn–NO battery, in which a peak power density of 1.8 mW cm −2 and a large NH 3 yield rate of 32 μmol h −1 cm −2 are observed. Theoretical analyses indicate that NiFe-LDH exhibits effective NO activation capacity and slow hydrogen evolution kinetics.

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          Most cited references40

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          Challenges in reduction of dinitrogen by proton and electron transfer.

          Ammonia is an important nutrient for the growth of plants. In industry, ammonia is produced by the energy expensive Haber-Bosch process where dihydrogen and dinitrogen form ammonia at a very high pressure and temperature. In principle one could also reduce dinitrogen upon addition of protons and electrons similar to the mechanism of ammonia production by nitrogenases. Recently, major breakthroughs have taken place in our understanding of biological fixation of dinitrogen, of molecular model systems that can reduce dinitrogen, and in the electrochemical reduction of dinitrogen at heterogeneous surfaces. Yet for efficient reduction of dinitrogen with protons and electrons major hurdles still have to be overcome. In this tutorial review we give an overview of the different catalytic systems, highlight the recent breakthroughs, pinpoint common grounds and discuss the bottlenecks and challenges in catalytic reduction of dinitrogen.
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            Nitrogen cycle electrocatalysis.

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              Au Sub-Nanoclusters on TiO2 toward Highly Efficient and Selective Electrocatalyst for N2 Conversion to NH3 at Ambient Conditions.

              As the NN bond in N2 is one of the strongest bonds in chemistry, the fixation of N2 to ammonia is a kinetically complex and energetically challenging reaction and, up to now, its synthesis is still heavily relying on energy and capital intensive Haber-Bosch process (150-350 atm, 350-550 °C), wherein the input of H2 and energy are largely derived from fossil fuels and thus result in large amount of CO2 emission. In this paper, it is demonstrated that by using Au sub-nanoclusters (≈0.5 nm ) embedded on TiO2 (Au loading is 1.542 wt%), the electrocatalytic N2 reduction reaction (NRR) is indeed possible at ambient condition. Unexpectedly, NRR with very high and stable production yield (NH3 : 21.4 µg h(-1) mg(-1)cat. , Faradaic efficiency: 8.11%) and good selectivity is achieved at -0.2 V versus RHE, which is much higher than that of the best results for N2 fixation under ambient conditions, and even comparable to the yield and activation energy under high temperatures and/or pressures. As isolated precious metal active centers dispersed onto oxide supports provide a well-defined system, the special structure of atomic Au cluster would promote other important reactions besides NRR for water splitting, fuel cells, and other electrochemical devices.
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                Author and article information

                Contributors
                Journal
                CHCOFS
                Chemical Communications
                Chem. Commun.
                Royal Society of Chemistry (RSC)
                1359-7345
                1364-548X
                July 19 2022
                2022
                : 58
                : 58
                : 8097-8100
                Affiliations
                [1 ]Key Laboratory of Carbon Materials of Zhejiang Province, College of Chemistry and Materials Engineering, Wenzhou University, Wenzhou, 325035, 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, China
                [3 ]College of Chemistry, Zhengzhou University, Zhengzhou, 450000, China
                [4 ]College of Materials Science and Engineering, Zhejiang University of Technology, Hangzhou, 310014, China
                [5 ]Institute for Advanced Study, Chengdu University, Chengdu, 610106, Sichuan, China
                [6 ]School of Chemical Engineering and Materials, Tianjin University of Science and Technology, Tianjin, 300457, China
                [7 ]Institute for New Energy Materials and Low-Carbon Technologies, School of Materials Science and Engineering, Tianjin University of Technology, Tianjin, 300384, China
                Article
                10.1039/D2CC02463B
                7d5b61f6-9938-48d9-b23f-0c707a7a610e
                © 2022

                http://rsc.li/journals-terms-of-use

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