Disordered Au Nanoclusters for Efficient Ammonia Electrosynthesis

• Published in: ChemSusChem Vol. 16; no. 7
• Main Authors: 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.
• Format: Journal Article
• Language: English
• Published: United States ChemPubSoc Europe 08.02.2023
• Subjects: ammonia; electrocatalysis; gold; INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; MXenes; nanoclusters
• ISSN: 1864-5631; 1864-564X

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.