Liu Yan, Wei Jie, Yang Zhengwu, Zheng Lirong, Zhao Jiankang, Song Zhimin, Zhou Yuhan, Cheng Jiajie, Meng Junyang, Geng Zhigang, Zeng Jie
Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, 230026, Anhui, PR China.
Institute of High Energy Physics, Chinese Academy of Sciences, 100049, Beijing, PR China.
Nat Commun. 2024 Apr 29;15(1):3619. doi: 10.1038/s41467-024-48035-4.
The nitrate (NO) electroreduction into ammonia (NH) represents a promising approach for sustainable NH synthesis. However, the variation of adsorption configurations renders great difficulties in the simultaneous optimization of binding energy for the intermediates. Though the extensively reported Cu-based electrocatalysts benefit NO adsorption, one of the key issues lies in the accumulation of nitrite (NO) due to its weak adsorption, resulting in the rapid deactivation of catalysts and sluggish kinetics of subsequent hydrogenation steps. Here we report a tandem electrocatalyst by combining Cu single atoms catalysts with adjacent CoO nanosheets to boost the electroreduction of NO to NH. The obtained tandem catalyst exhibits a yield rate for NH of 114.0 mg h cm, which exceeds the previous values for the reported Cu-based catalysts. Mechanism investigations unveil that the combination of CoO regulates the adsorption configuration of NO and strengthens the binding with NO, thus accelerating the electroreduction of NO to NH.
将硝酸盐（NO）电还原为氨（NH₃）是实现可持续NH₃合成的一种有前景的方法。然而，吸附构型的变化给同时优化中间体的结合能带来了巨大困难。尽管广泛报道的铜基电催化剂有利于NO的吸附，但关键问题之一在于亚硝酸盐（NO₂⁻）由于吸附较弱而积累，导致催化剂快速失活以及后续氢化步骤的动力学迟缓。在此，我们报道了一种通过将铜单原子催化剂与相邻的CoO纳米片相结合的串联电催化剂，以促进NO电还原为NH₃。所获得的串联催化剂的NH₃产率为114.0 mg h⁻¹ cm⁻²，超过了先前报道的铜基催化剂的值。机理研究表明，CoO的结合调节了NO的吸附构型并增强了与NO的结合，从而加速了NO电还原为NH₃的过程。
