Disordered Au Nanoclusters for Efficient Ammonia Electrosynthesis

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.

doi:10.1002/cssc.202201385

Disordered Au Nanoclusters for Efficient Ammonia Electrosynthesis

Journal Article · Tue Feb 07 23:00:00 EST 2023 · ChemSusChem

DOI:https://doi.org/10.1002/cssc.202201385· OSTI ID:1963189

Peng, Xianyun ^[1]; Zhang, Rui ^[2]; Mi, Yuying ^[3]; Wang, Hsiao‐Tsu ^[4]; Huang, Yu‐Cheng ^[4]; Han, Lili ^[5]; ^[6]; Pao, Chih‐Wen ^[7]; Liu, Xijun ^[8]; Dong, Chung‐Li ^[4]; Liu, Qian ^[9]; Zhang, Shusheng ^[10]; Pong, Way‐Faung ^[4]; Luo, Jun ^[3]; ^[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)

The electrochemical nitrogen (N₂) reduction reaction (N₂RR) 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 (NH₃), but high-yielding production is rendered challenging by the strong nonpolar N≡N bond in N₂ molecules, which hinders their dissociation or activation. In this study, disordered Au nanoclusters anchored on two-dimensional ultrathin Ti₃C₂T_x MXene nanosheets are explored as highly active and selective electrocatalysts for efficient N₂-to-NH₃ conversion, exhibiting exceptional activity with an NH₃ yield rate of 88.3±1.7 μg h^–1 mg_cat.^–1 and a faradaic efficiency of 9.3±0.4 %. Further, 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 N₂RR. The disordered structure is found to serve as the active site for N₂ chemisorption and activation during the N₂RR process.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0012704

OSTI ID:: 1963189

Alternate ID(s):: OSTI ID: 1923938

Report Number(s):: BNL-224155-2023-JAAM

Journal Information:: ChemSusChem, Journal Name: ChemSusChem Journal Issue: 7 Vol. 16; ISSN 1864-5631

Publisher:: ChemPubSoc EuropeCopyright Statement

Country of Publication:: United States

Language:: English

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