Disordered Au Nanoclusters for Efficient Ammonia Electrosynthesis
Xianyun Peng, Rui Zhang, Yuying Mi, Hsiao‐Tsu Wang, Yucheng Huang, Lili Han, Ashley R. Head, Chih‐Wen Pao, Xijun Liu, Chung‐Li Dong, Qian Liu, Shusheng Zhang, W. F. Pong, Jun Luo, Huolin L. Xin
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.