期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 59, 期 23, 页码 8941-8946出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202002311
关键词
homolytic; heterolytic processes; hydrogen evolution; molecular catalysis; nickel porphyrins; steric effect
资金
- Deutsche Forschungsgemeinschaft [Emmy Noether grant AP242/2-1, under Germany's Excellence Strategy - EXC 2033 - 390677874 - RESOLV] Funding Source: Medline
- Fundamental Research Funds for the Central Universities Funding Source: Medline
- National Natural Science Foundation of China [21101170, 21573139, and 21773146] Funding Source: Medline
- Research Funds of Shaanxi Normal University Funding Source: Medline
- Recruitment Program of Global Experts Funding Source: Medline
- Fraunhofer Internal Programs [Attract 097-602175] Funding Source: Medline
- Fok Ying-Tong Education Foundation for Outstanding Young Teachers in University Funding Source: Medline
Several H-H bond forming pathways have been proposed for the hydrogen evolution reaction (HER). Revealing these HER mechanisms is of fundamental importance for the rational design of catalysts and is also extremely challenging. Now, an unparalleled example of switching between homolytic and heterolytic HER mechanisms is reported. Three nickel(II) porphyrins were designed and synthesized with distinct steric effects by introducing bulky amido moieties to ortho- or para-positions of the meso-phenyl groups. These porphyrins exhibited different catalytic HER behaviors. For these Ni porphyrins, although their 1e-reduced forms are active to reduce trifluoroacetic acid, the resulting Ni hydrides (depending on the steric effects of porphyrin rings) have different pathways to make H-2. Understanding HER processes, especially controllable switching between homolytic and heterolytic H-H bond formation pathways through molecular engineering, is unprecedented in electrocatalysis.
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