Atomic Defects Engineering Boosts Urea Synthesis toward Carbon Dioxide and Nitrate Coelectroreduction

作者：Zifan Xu, Zhengwu Yang, Huan Lu, Jiangchen Zhu, Junlin Li, Minghui Fan, Zhi Zhao, Xiangdong Kong, Ke Wang, Zhigang Geng · 发表于：Nano Letters · 年份：2024 · DOI：10.1021/acs.nanolett.4c03451 · 被引用次数：28 · 研究领域：Ammonia Synthesis and Nitrogen Reduction、Catalytic Processes in Materials Science、Advanced Photocatalysis Techniques

The atomic defect engineering could feasibly decorate the chemical behaviors of reaction intermediates to regulate catalytic performance. Herein, we created oxygen vacancies on the surface of In(OH) 3 nanobelts for efficient urea electrosynthesis. When the oxygen vacancies were constructed on the surface of the In(OH) 3 nanobelts, the faradaic efficiency for urea reached 80.1%, which is 2.9 times higher than that (20.7%) of the pristine In(OH) 3 nanobelts. At −0.8 V versus reversible hydrogen electrode, In(OH) 3 nanobelts with abundant oxygen vacancies exhibited partial current density for urea of −18.8 mA cm –2 . Such a value represents the highest activity for urea electrosynthesis among recent reports. Density functional theory calculations suggested that the unsaturated In sites adjacent to oxygen defects helped to optimize the adsorbed configurations of key intermediates, promoting both the C–N coupling and the activation of the adsorbed CO 2 NH 2 intermediate. In-situ spectroscopy measurements further validated the promotional effect of the oxygen vacancies on urea electrosynthesis.