材料科学
电解质
铜
Boosting(机器学习)
纳米技术
化学工程
电极
冶金
化学
物理化学
计算机科学
机器学习
工程类
作者
Mutian Ma,Likun Xiong,Yuan Dong,Qianqian Bai,Wei Hua,Zhangyi Zheng,Fenglei Lyu,Yuebin Lian,Zhihe Wei,Huihong Yuan,Zhenyang Jiao,Jian Cheng,Daqi Song,Min Wang,Zhiyuan Xing,Jun Zhong,Sheng Han,Zhao Deng,Yang Peng
标识
DOI:10.1002/adfm.202315667
摘要
Abstract Electrochemical carbon dioxide reduction (eCO 2 R) in neutral electrolytes represents a viable solution for alleviating energy and carbon losses associated with carbonate formation, but limited by suboptimal C 2+ selectivity and productivity owing to the higher C−C coupling kinetic barrier in such media. To address the issue, here Cu 2 O nanocubes are encapsulated within metalloporphyrin frameworks to create a benign microenvironment for C−C coupling, with the best catalyst of Cu 2 O@Cu−TCPP(Co) demonstrating a maximal C 2 H 4 and C 2+ FE of 54 ± 2% and 69 ± 4%, respectively, at 500 mA cm −2 in 1 M KCl. Comprehensive structural and spectrometric characterizations utilizing in situ attenuated total reflectance surface‐enhanced infrared absorption spectroscopy (ATR−SEIRAS), in situ X‐ray absorption spectroscopy (XAS), operando Raman, and high‐resolution transmission electron microscopy (HR−TEM) unveil that the high CO 2 adsorption endowed by the metal‐organic framework (MOF) overlayer, high CO concentration yield by metalloporphyrins, high local pH rendered by spatial confinement, as well as the highly dispersed Cu crystallites exposing (200) facets synergistically contribute to the asymmetric C−C coupling of *CO and *COH intermediates in favor of C 2+ production. Orchestrating the active moieties in a concerted fashion, this study offers a paradigm for the design of eCO 2 R catalysts in neutral electrolytes.
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