Atomically Dispersed Manganese on Carbon Substrate for Aqueous and Aprotic CO2 Electrochemical Reduction

被引:46
作者
Wang, Meiling [1 ]
Yao, Ying [1 ,2 ]
Tian, Yuhui [3 ]
Yuan, Yifei [4 ]
Wang, Liguang [5 ]
Yang, Feiyang [1 ]
Ren, Jingjie [1 ]
Hu, Xinrong [1 ]
Wu, Feng [1 ,2 ]
Zhang, Shanqing [3 ]
Wu, Junxiu [5 ]
Lu, Jun [5 ]
机构
[1] Beijing Inst Technol, Sch Mat Sci & Engn, Beijing Key Lab Environm Sci & Engn, Beijing 100081, Peoples R China
[2] Beijing Inst Technol, Chongqing Innovat Ctr, Chongqing 401120, Peoples R China
[3] Griffith Univ, Ctr Clean Environm & Energy, Sch Environm & Sci, Gold Coast Campus, Gold Coast, Qld 4222, Australia
[4] Wenzhou Univ, Coll Chem & Mat Engn, Wenzhou 325035, Peoples R China
[5] Zhejiang Univ, Coll Chem & Biol Engn, Hangzhou 310027, Peoples R China
基金
中国国家自然科学基金;
关键词
electrochemical CO2 reduction; Li-CO2; batteries; manganese; mesoporous carbon; single-atom catalysts; second coordination spheres; POROUS CARBON; SURFACE-AREA; ION; NITROGEN; NANOSHEETS; GRAPHENE;
D O I
10.1002/adma.202210658
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
CO2 utilization and conversion are of great importance in alleviating the rising CO2 concentration in the atmosphere. Here, a single-atom catalyst (SAC) is reported for electrochemical CO2 utilization in both aqueous and aprotic electrolytes. Specifically, atomically dispersed Mn-N-4 sites are embedded in bowl-like mesoporous carbon particles with the functionalization of epoxy groups in the second coordination spheres. Theoretical calculations suggest that the epoxy groups near the Mn-N-4 site adjust the electronic structure of the catalyst with reduced reaction energy barriers for the electrocatalytic reduction of CO2 to CO. The resultant Mn-single-atom carbon with N and O doped catalyst (MCs-(N,O)) exhibits extraordinary electrocatalytic performance with a high CO faradaic efficiency of 94.5%, a high CO current density of 13.7 mA cm(-2), and a low overpotential of 0.44 V in the aqueous environment. Meanwhile, as a cathode catalyst for aprotic Li-CO2 batteries, the MCs-(N,O) with well-regulated active sites and unique mesoporous bowl-like morphology optimizes the nucleation behavior of discharge products. MCs-(N,O)-based batteries deliver a low overpotential and excellent cyclic stability of 1000 h. The findings in this work provide a new avenue to design and fabricate SACs for various electrochemical CO2 utilization systems.
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页数:11
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