甲烷
法拉第效率
铜
催化作用
质子化
材料科学
Atom(片上系统)
电化学
化学
离子
物理化学
电极
计算机科学
有机化学
嵌入式系统
冶金
作者
Yizhou Dai,Huan Li,Chuanhao Wang,Weiqing Xue,Menglu Zhang,Di Zhao,Jing Xue,Jiawei Li,Laihao Luo,Chunxiao Liu,Li Xu,Peixin Cui,Qiu Jiang,Tingting Zheng,Shuang‐Xi Gu,Yao Zhang,Jianping Xiao,Chuan Xia,Jie Zeng
标识
DOI:10.1038/s41467-023-39048-6
摘要
Electrochemical CO2 conversion to methane, powered by intermittent renewable electricity, provides an entrancing opportunity to both store renewable electric energy and utilize emitted CO2. Copper-based single atom catalysts are promising candidates to restrain C-C coupling, suggesting feasibility in further protonation of CO* to CHO* for methane production. In theoretical studies herein, we find that introducing boron atoms into the first coordination layer of Cu-N4 motif facilitates the binding of CO* and CHO* intermediates, which favors the generation of methane. Accordingly, we employ a co-doping strategy to fabricate B-doped Cu-Nx atomic configuration (Cu-NxBy), where Cu-N2B2 is resolved to be the dominant site. Compared with Cu-N4 motifs, as-synthesized B-doped Cu-Nx structure exhibits a superior performance towards methane production, showing a peak methane Faradaic efficiency of 73% at -1.46 V vs. RHE and a maximum methane partial current density of -462 mA cm-2 at -1.94 V vs. RHE. Extensional calculations utilizing two-dimensional reaction phase diagram analysis together with barrier calculation help to gain more insights into the reaction mechanism of Cu-N2B2 coordination structure.
科研通智能强力驱动
Strongly Powered by AbleSci AI