化学
纳米片
选择性
共价键
电解质
吸附
催化作用
铜
共价有机骨架
化学工程
氧化还原
电流密度
离解(化学)
纳米技术
表面改性
无机化学
电极
有机化学
物理化学
物理
材料科学
量子力学
工程类
作者
Zhejiaji Zhu,Yuhao Zhu,Zhixin Ren,Di Liu,Fan Yue,Dafei Sheng,Pengpeng Shao,Xiaodan Huang,Xiao Feng,Anxiang Yin,Jing Xie,Bo Wang
摘要
CO2 electroreduction holds great promise for addressing global energy and sustainability challenges. Copper (Cu) shows great potential for effective conversion of CO2 toward specific value-added and/or high-energy-density products. However, its limitation lies in relatively low product selectivity. Herein, we present that the CO2 reduction reaction (CO2RR) pathway on commercially available Cu can be rationally steered by modulating the microenvironment in the vicinity of the Cu surface with two-dimensional sulfonated covalent organic framework nanosheet (COF-NS)-based ionomers. Specifically, the selectivity toward methane (CH4) can be enhanced to more than 60% with the total current density up to 500 mA cm-2 in flow cells in both acidic (pH = 2) and alkaline (pH = 14) electrolytes. The COF-NS, characterized by abundant apertures, can promote the accumulation of CO2 and K+ near the catalyst surface, alter the adsorption energy and surface coverage of *CO, facilitate the dissociation of H2O, and finally modulate the reaction pathway for the CO2RR. Our approach demonstrates the rational modulation of reaction interfaces for the CO2RR utilizing porous open framework ionomers, showcasing their potential practical applications.
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