电催化剂
金属有机骨架
催化作用
化学工程
材料科学
活动站点
太阳能燃料
膜
纳米技术
化学
电化学
电极
光催化
有机化学
物理化学
生物化学
工程类
吸附
作者
Subhabrata Mukhopadhyay,Ran Shimoni,Itamar Liberman,Raya Ifraemov,Illya Rozenberg,Idan Hod
标识
DOI:10.1002/anie.202102320
摘要
Abstract Electrochemically active Metal‐Organic Frameworks (MOFs) have been progressively recognized for their use in solar fuel production schemes. Typically, they are utilized as platforms for heterogeneous tethering of exceptionally large concentration of molecular electrocatalysts onto electrodes. Yet so far, the potential influence of their extraordinary chemical modularity on electrocatalysis has been overlooked. Herein, we demonstrate that, when assembled on a solid Ag CO 2 reduction electrocatalyst, a non‐catalytic UiO‐66 MOF acts as a porous membrane that systematically tunes the active site's immediate chemical environment, leading to a drastic enhancement of electrocatalytic activity and selectivity. Electrochemical analysis shows that the MOF membrane improves catalytic performance through physical and electrostatic regulation of reactants delivery towards the catalytic sites. The MOF also stabilizes catalytic intermediates via modulation of active site's secondary coordination sphere. This concept can be expanded to a wide range of proton‐coupled electrochemical reactions, providing new means for precise, molecular‐level manipulation of heterogeneous solar fuels systems.
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