Disordered Au Nanoclusters for Efficient Ammonia Electrosynthesis.

Autor: Peng X; State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences, Fujian, Fuzhou, 350002, P. R. China.; Institute of Zhejiang University - Quzhou, Zhejiang, Quzhou, 324000, P. R. China., Zhang R; Department of Physics and Astronomy, University of California, Irvine, CA, 92697, USA., Mi Y; Institute for New Energy Materials & Low-Carbon Technologies and Tianjin Key Lab of Photoelectric Materials & Devices, School of Materials Science and Engineering, Tianjin University of Technology, Tianjin, 300384, P. R. China., Wang HT; Bachelor's Program in Advanced Materials Science, Tamkang University, New Taipei City, 25137, Taiwan.; Department of Physics, Tamkang University, New Taipei City, 251301, Taiwan., Huang YC; Department of Physics, Tamkang University, New Taipei City, 251301, Taiwan., Han L; State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences, Fujian, Fuzhou, 350002, P. R. China.; Department of Physics and Astronomy, University of California, Irvine, CA, 92697, USA., Head AR; Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton, NY, 11973, USA., Pao CW; National Synchrotron Radiation Research Center, Hsinchu, 30076, Taiwan., Liu X; 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, Guangxi, Nanning, 530004, P. R. China., Dong CL; Department of Physics, Tamkang University, New Taipei City, 251301, Taiwan., Liu Q; Institute for Advanced Study, Chengdu University, Sichuan, Chengdu, 610106, P. R. China., Zhang S; College of Chemistry, Zhengzhou University, Henan, Zhengzhou, 450000, P. R. China., Pong WF; Department of Physics, Tamkang University, New Taipei City, 251301, Taiwan., Luo J; Institute for New Energy Materials & Low-Carbon Technologies and Tianjin Key Lab of Photoelectric Materials & Devices, School of Materials Science and Engineering, Tianjin University of Technology, Tianjin, 300384, P. R. China., Xin HL; Department of Physics and Astronomy, University of California, Irvine, CA, 92697, USA.
Jazyk: angličtina
Zdroj: ChemSusChem [ChemSusChem] 2023 Apr 06; Vol. 16 (7), pp. e202201385. Date of Electronic Publication: 2023 Feb 08.
DOI: 10.1002/cssc.202201385
Abstrakt: The electrochemical nitrogen (N 2 ) reduction reaction (N 2 RR) under mild conditions is a promising and environmentally friendly alternative to the traditional Haber-Bosch process with high energy consumption and greenhouse emission for the synthesis of ammonia (NH 3 ), but high-yielding production is rendered challenging by the strong nonpolar N≡N bond in N 2 molecules, which hinders their dissociation or activation. In this study, disordered Au nanoclusters anchored on two-dimensional ultrathin Ti 3 C 2 T x MXene nanosheets are explored as highly active and selective electrocatalysts for efficient N 2 -to-NH 3 conversion, exhibiting exceptional activity with an NH 3 yield rate of 88.3±1.7 μg h -1  mg cat. -1 and a faradaic efficiency of 9.3±0.4 %. A combination of in situ near-ambient pressure X-ray photoelectron spectroscopy and operando X-ray absorption fine structure spectroscopy is employed to unveil the uniqueness of this catalyst for N 2 RR. The disordered structure is found to serve as the active site for N 2 chemisorption and activation during the N 2 RR process.
(© 2023 Wiley-VCH GmbH.)
Databáze: MEDLINE
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