文献详情
Homolytic versus Heterolytic Hydrogen Evolution Reaction Steered via Steric Effect
文献类型：期刊
期刊名称：Angewandte Chemie (International ed. in English)
年：2020
ISSN：1521-3773
关键词：heterolytic,homolytic,hydrogen evolution,nickel porphyrin,steric effect
所属部门：化学系
摘要：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. Herein we report an unparalleled example of switching between homolytic and heterolytic HER mechanisms.?We designed and synthesized three nickel(II) porphyrins with distinct steric effects by introducing bulky amido moieties to?ortho- or?para-positions of the?meso-phenyl ...More
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. Herein we report an unparalleled example of switching between homolytic and heterolytic HER mechanisms.?We designed and synthesized three nickel(II) porphyrins with distinct steric effects by introducing bulky amido moieties to?ortho- or?para-positions of the?meso-phenyl groups. We furthermore showed their different catalytic HER behaviors.?For these Ni porphyrins, although their 1e-reduced forms are active to reduce trifluoroacetic acid, the resulted Ni hydrides - depending on the steric effects of porphyrin rings - have different pathways to make H2. Understanding HER processes, especially controllable switching between homolytic and heterolytic H-H bond formation pathways through molecular engineering, is unprecedented in fundamentals of electrocatalysis.? 2020 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. ...Hide

DOI：10.1002/anie.202002311
百度学术：Homolytic versus Heterolytic Hydrogen Evolution Reaction Steered via Steric Effect
语言：外文
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