期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 60, 期 14, 页码 7607-7611出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202016219
关键词
CO2 reduction; coordination environment; electrocatalysis; metal-organic frameworks; single-atom catalysts
资金
- NSFC [21725101, 21871244, 21521001, 22001242]
- China Postdoctoral Science Foundation [2019TQ0298, 2019M660151]
- International Partnership Program of CAS [211134KYSB20190109]
- Collaborative Innovation Program of Hefei Science Center, CAS [2020HSC-CIP005]
- Supercomputing Center of USTC
A single-atom Ni catalyst with different N coordination numbers was fabricated using a post-synthetic metal substitution strategy. The Ni-N-3-C catalyst showed significantly enhanced COOH* formation leading to accelerated CO2 reduction, achieving high CO Faradaic efficiency and excellent performance in Zn-CO2 battery. This work provides a new approach for modulation of coordination microenvironment in single-atom catalysts for CO2 utilization.
Single-atom catalysts (SACs) have attracted tremendous interests due to their ultrahigh activity and selectivity. However, the rational control over coordination microenvironment of SACs remains a grand challenge. Herein, a post-synthetic metal substitution (PSMS) strategy has been developed to fabricate single-atom Ni catalysts with different N coordination numbers (denoted Ni-N-x-C) on pre-designed N-doped carbon derived from metal-organic frameworks. When served for CO2 electroreduction, the obtained Ni-N-3-C catalyst achieves CO Faradaic efficiency (FE) up to 95.6 %, much superior to that of Ni-N-4-C. Theoretical calculations reveal that the lower Ni coordination number in Ni-N-3-C can significantly enhance COOH* formation, thereby accelerating CO2 reduction. In addition, Ni-N-3-C shows excellent performance in Zn-CO2 battery with ultrahigh CO FE and excellent stability. This work opens up a new and general avenue to coordination microenvironment modulation (MEM) of SACs for CO2 utilization.
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据