催化作用
活动站点
电化学
镍
共价键
化学工程
化学
热解
材料科学
过渡金属
无机化学
作者
Changxia Li,Wen Ju,Sudarshan Vijay,Janis Timoshenko,Kaiwen Mou,David A Cullen,Jin Yang,Xingli Wang,Pradip Pachfule,Sven Brückner,Hyo Sang Jeon,Felix T Haase,Sze-Chun Tsang,Clara Rettenmaier,Karen Chan,Beatriz Roldan Cuenya,Arne Thomas,Peter Strasser
标识
DOI:10.1002/anie.202114707
摘要
Electrochemical CO2 reduction is a potential approach to convert CO2 into valuable chemicals using electricity as feedstock. Abundant and affordable catalyst materials are needed to upscale this process in a sustainable manner. Nickel-nitrogen-doped carbon (Ni-N-C) is an efficient catalyst for CO2 reduction to CO, and the single-site Ni-Nx motif is believed to be the active site. However, critical metrics for its catalytic activity, such as active site density and intrinsic turnover frequency, so far lack systematic discussion. In this work, we prepared a set of covalent organic framework (COF)-derived Ni-N-C catalysts, for which the Ni-Nx content could be adjusted by the pyrolysis temperature. The combination of high-angle annular dark-field scanning transmission electron microscopy and extended X-ray absorption fine structure evidenced the presence of Ni single-sites, and quantitative X-ray photoemission addressed the relation between active site density and turnover frequency.
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