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Atomically Dispersed Manganese on Carbon Substrate for Aqueous and Aprotic CO2 Electrochemical Reduction
被引:46
作者:

Wang, Meiling
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Beijing Inst Technol, Sch Mat Sci & Engn, Beijing Key Lab Environm Sci & Engn, Beijing 100081, Peoples R China Beijing Inst Technol, Sch Mat Sci & Engn, Beijing Key Lab Environm Sci & Engn, Beijing 100081, Peoples R China

Yao, Ying
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Beijing Inst Technol, Sch Mat Sci & Engn, Beijing Key Lab Environm Sci & Engn, Beijing 100081, Peoples R China
Beijing Inst Technol, Chongqing Innovat Ctr, Chongqing 401120, Peoples R China Beijing Inst Technol, Sch Mat Sci & Engn, Beijing Key Lab Environm Sci & Engn, Beijing 100081, Peoples R China

Tian, Yuhui
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h-index: 0
机构:
Griffith Univ, Ctr Clean Environm & Energy, Sch Environm & Sci, Gold Coast Campus, Gold Coast, Qld 4222, Australia Beijing Inst Technol, Sch Mat Sci & Engn, Beijing Key Lab Environm Sci & Engn, Beijing 100081, Peoples R China

Yuan, Yifei
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Wenzhou Univ, Coll Chem & Mat Engn, Wenzhou 325035, Peoples R China Beijing Inst Technol, Sch Mat Sci & Engn, Beijing Key Lab Environm Sci & Engn, Beijing 100081, Peoples R China

Wang, Liguang
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Zhejiang Univ, Coll Chem & Biol Engn, Hangzhou 310027, Peoples R China Beijing Inst Technol, Sch Mat Sci & Engn, Beijing Key Lab Environm Sci & Engn, Beijing 100081, Peoples R China

Yang, Feiyang
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Beijing Inst Technol, Sch Mat Sci & Engn, Beijing Key Lab Environm Sci & Engn, Beijing 100081, Peoples R China Beijing Inst Technol, Sch Mat Sci & Engn, Beijing Key Lab Environm Sci & Engn, Beijing 100081, Peoples R China

Ren, Jingjie
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Beijing Inst Technol, Sch Mat Sci & Engn, Beijing Key Lab Environm Sci & Engn, Beijing 100081, Peoples R China Beijing Inst Technol, Sch Mat Sci & Engn, Beijing Key Lab Environm Sci & Engn, Beijing 100081, Peoples R China

Hu, Xinrong
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Beijing Inst Technol, Sch Mat Sci & Engn, Beijing Key Lab Environm Sci & Engn, Beijing 100081, Peoples R China Beijing Inst Technol, Sch Mat Sci & Engn, Beijing Key Lab Environm Sci & Engn, Beijing 100081, Peoples R China

Wu, Feng
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Beijing Inst Technol, Sch Mat Sci & Engn, Beijing Key Lab Environm Sci & Engn, Beijing 100081, Peoples R China
Beijing Inst Technol, Chongqing Innovat Ctr, Chongqing 401120, Peoples R China Beijing Inst Technol, Sch Mat Sci & Engn, Beijing Key Lab Environm Sci & Engn, Beijing 100081, Peoples R China

Zhang, Shanqing
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Griffith Univ, Ctr Clean Environm & Energy, Sch Environm & Sci, Gold Coast Campus, Gold Coast, Qld 4222, Australia Beijing Inst Technol, Sch Mat Sci & Engn, Beijing Key Lab Environm Sci & Engn, Beijing 100081, Peoples R China

Wu, Junxiu
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h-index: 0
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Zhejiang Univ, Coll Chem & Biol Engn, Hangzhou 310027, Peoples R China Beijing Inst Technol, Sch Mat Sci & Engn, Beijing Key Lab Environm Sci & Engn, Beijing 100081, Peoples R China

Lu, Jun
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h-index: 0
机构:
Zhejiang Univ, Coll Chem & Biol Engn, Hangzhou 310027, Peoples R China Beijing Inst Technol, Sch Mat Sci & Engn, Beijing Key Lab Environm Sci & Engn, Beijing 100081, Peoples R China
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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