清华大学王定胜团队开发了高效电化学生产过氧化氢的铟单原子催化剂局部原子环境工程。相关研究成果发表在2022年1月18日出版的《德国应用化学》。

对p-嵌段金属单原子催化剂在2e氧还原反应（ORR）中的局部原子环境性质关系的深入研究尚未见报道。

该文中，在第一性原理计算的指导下，研究人员开发了一种杂原子修饰的In基金属有机骨架辅助方法，以精确合成最佳催化剂，其中单个In原子由空心碳棒（SAs/NSBC）支持的N，S-双第一配位和B-二配位组合锚定。In-SAs/NSBC在宽pH范围内表现出95%以上的高H₂O₂选择性。

此外，In-SAs/NSBC修饰的自然空气扩散电极在0.1 M KOH电解液中显示出前所未有的6.49过氧化氢GCatalys1 h1产率，在0.1 M PBS电解液中显示出前所未有的6.71 mol过氧化氢GCatalys1 h1产率。该策略为下一代高性能单原子材料的设计提供了可能，并为H₂O₂电合成提供了实用指导。

附：英文原文

Title: Engineering the Local Atomic Environments of Indium Single-Atom Catalysts for Efficient Electrochemical Production of Hydrogen Peroxide

Author: Erhuan Zhang, Lei Tao, Jingkun An, Jiangwei Zhang, Lingzhe Meng, Xiaobo Zheng, Yu Wang, Nan Li, Shixuan Du, Jiatao Zhang, Dingsheng Wang, Yadong Li

Issue&Volume: 2022-01-18

Abstract: The in-depth understanding of local atomic environments-property relationships on p-block metal single-atom catalyst toward 2e oxygen reduction reaction (ORR) is rarely reported. Here, guided by first-principles calculations, we develop a heteroatom-modified In-based metalorganic framework-assisted approach to accurately synthesize an optimal catalyst, in which single In atoms are anchored by combined N, S-dual first coordination and B second coordination supported by the hollow carbon rods (In SAs/NSBC). The In SAs/NSBC exhibits a high H2O2 selectivity of above 95% in a wide range of pH. Furthermore, the In SAs/NSBC-modified natural air diffusion electrode exhibits an unprecedented production rate of 6.49 peroxide gcatalyst1 h1 in 0.1 M KOH electrolyte and 6.71 mol peroxide gcatalyst1 h1 in 0.1 M PBS electrolyte, respectively. This strategy enables the design of next-generation high-performance single-atom materials, and provides a practical guidance for H2O2 electrosynthesis.

DOI: 10.1002/anie.202117347

Source: https://onlinelibrary.wiley.com/doi/10.1002/anie.202117347