Disordered Au Nanoclusters for Efficient Ammonia Electrosynthesis
Abstract
Abstract 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.
- Authors:
-
[6];
[2]
- Chinese Academy of Sciences (CAS), Fuzhou (China). Fujian Institute of Research on the Structure of Matter; Zhejiang Univ., Quzhou (China)
- Univ. of California, Irvine, CA (United States)
- Tianjin Univ. of Technology, Tianjin (China)
- Tamkang Univ., Taipei (Taiwan)
- Chinese Academy of Sciences (CAS), Fuzhou (China). Fujian Institute of Research on the Structure of Matter; Univ. of California, Irvine, CA (United States)
- Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
- National Synchrotron Radiation Research Center, Hsinchu (Taiwan)
- Guangxi Univ., Nanning (China)
- Chengdu University (China)
- Zhengzhou University (China)
- Publication Date:
- Research Org.:
- Brookhaven National Laboratory (BNL), Upton, NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1963189
- Alternate Identifier(s):
- OSTI ID: 1923938
- Report Number(s):
- BNL-224155-2023-JAAM
Journal ID: ISSN 1864-5631
- Grant/Contract Number:
- SC0012704
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ChemSusChem
- Additional Journal Information:
- Journal Volume: 16; Journal Issue: 7; Journal ID: ISSN 1864-5631
- Publisher:
- ChemPubSoc Europe
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; ammonia; electrocatalysis; gold; MXenes; nanoclusters
Citation Formats
Peng, Xianyun, Zhang, Rui, Mi, Yuying, Wang, Hsiao‐Tsu, Huang, Yu‐Cheng, Han, Lili, Head, Ashley R., Pao, Chih‐Wen, Liu, Xijun, Dong, Chung‐Li, Liu, Qian, Zhang, Shusheng, Pong, Way‐Faung, Luo, Jun, and Xin, Huolin L. Disordered Au Nanoclusters for Efficient Ammonia Electrosynthesis. United States: N. p., 2023.
Web. doi:10.1002/cssc.202201385.
Peng, Xianyun, Zhang, Rui, Mi, Yuying, Wang, Hsiao‐Tsu, Huang, Yu‐Cheng, Han, Lili, Head, Ashley R., Pao, Chih‐Wen, Liu, Xijun, Dong, Chung‐Li, Liu, Qian, Zhang, Shusheng, Pong, Way‐Faung, Luo, Jun, & Xin, Huolin L. Disordered Au Nanoclusters for Efficient Ammonia Electrosynthesis. United States. https://doi.org/10.1002/cssc.202201385
Peng, Xianyun, Zhang, Rui, Mi, Yuying, Wang, Hsiao‐Tsu, Huang, Yu‐Cheng, Han, Lili, Head, Ashley R., Pao, Chih‐Wen, Liu, Xijun, Dong, Chung‐Li, Liu, Qian, Zhang, Shusheng, Pong, Way‐Faung, Luo, Jun, and Xin, Huolin L. Wed .
"Disordered Au Nanoclusters for Efficient Ammonia Electrosynthesis". United States. https://doi.org/10.1002/cssc.202201385. https://www.osti.gov/servlets/purl/1963189.
@article{osti_1963189,
title = {Disordered Au Nanoclusters for Efficient Ammonia Electrosynthesis},
author = {Peng, Xianyun and Zhang, Rui and Mi, Yuying and Wang, Hsiao‐Tsu and Huang, Yu‐Cheng and Han, Lili and Head, Ashley R. and Pao, Chih‐Wen and Liu, Xijun and Dong, Chung‐Li and Liu, Qian and Zhang, Shusheng and Pong, Way‐Faung and Luo, Jun and Xin, Huolin L.},
abstractNote = {Abstract 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.},
doi = {10.1002/cssc.202201385},
journal = {ChemSusChem},
number = 7,
volume = 16,
place = {United States},
year = {Wed Feb 08 00:00:00 EST 2023},
month = {Wed Feb 08 00:00:00 EST 2023}
}
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