Modulating the Nitrate Reduction Pathway on Unconventional Phase Ultrathin Nanoalloys for Selective Ammonia Electrosynthesis
Jingwen Zhou, Fu Liu, Zhihang Xu, Jian-An Yin, Liang Guo, Fengkun Hao, Yunhao Wang, Yuecheng Xiong, Xichen Zhou, Cheng Wang, Yangbo Ma, Xiang Meng, Pengyi Lu, Jinwen Yin, An Zhang, Jie Wang, Chenliang Ye, Qiang Li, Chongyi Ling, Hsiao‐Chien Chen, Hao Ming Chen, Ye Zhu, Jian Lü, Zhanxi Fan, Jian Lü, Zhanxi Fan
Abstract
High Resolution Image Download MS PowerPoint Slide Ammonia (NH 3 ) electrosynthesis from nitrate-polluted wastewater is a challenging but meaningful technique for the future green chemical and sewage disposal industries. The dominant difficulties lie in how to realize a highly selective, low-overpotential, and rapid electrocatalytic nitrate reduction reaction (NO 3 RR). Herein, we propose a catalyst crystal phase and electrode/electrolyte interface dual engineering strategy to enhance the neutral NO 3 RR performance of ultrathin alloy nanostructures. The obtained unconventional 2H-RhCu not only shows higher intrinsic NH 3 selectivity than its traditional face-centered cubic and amorphous/crystalline counterparts but also delivers superior Faradaic efficiency and yield rate toward NH 3 in K + -based electrolyte over those in Li + /Na + -based ones. In situ studies and theoretical calculations reveal that the faster generation/conversion kinetics of key intermediates, weaker N–N recombination, and unique *NO bri adsorption configuration at electrode/electrolyte interfaces account for this significant enhancement. In addition, rechargeable Zn-nitrate/methanol flow batteries with 2H-RhCu were constructed as a demonstration of potential applications.