Covalently anchoring covalent organic framework on carbon nanotubes for highly efficient electrocatalytic CO2 reduction

被引:124
作者
Dong, Hong [1 ,2 ]
Lu, Meng [3 ]
Wang, Ya [1 ]
Tang, Hong-Liang [1 ]
Wu, Di [1 ]
Sun, Xiaojun [1 ]
Zhang, Feng-Ming [1 ]
机构
[1] Harbin Univ Sci & Technol, Sch Mat Sci & Chem Engn, Harbin 10040, Peoples R China
[2] Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China
[3] South China Normal Univ, Sch Chem, Guangzhou 510006, Peoples R China
基金
中国博士后科学基金;
关键词
Covalent-organic frameworks; Electrocatalysis CO2 reduction; NH2-MWCNT; Covalently connection; ELECTROCHEMICAL REDUCTION; ELECTROREDUCTION; DIOXIDE; CATALYSTS; SITES; PORPHYRIN;
D O I
10.1016/j.apcatb.2021.120897
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Porphyrin-based covalent organic frameworks (Por-COF) nanosheets were vertically anchored on carbon nanotubes (CNT) with covalent connection for efficient electrocatalytic CO2 reduction reaction (CO2RR). The CNT not only acts as ideal carriers for the dispersion of Pro-COF but also facilitates electron transfer along porphyrin planes to immobilized metal active sites. As a result, covalently linked MWCNT-Por-COF-M (M: Co, Ni, Fe) display improved electrocatalytic CO2-to-CO activity and selectivity compared to pure Por-COF-M and MWCNT@Por-COF-M without covalent connection between two components. In particular, MWCNT-Por-COF-Co exhibits superior activity (FECO: 99.3%), higher partial current density and good durability in 0.5 M KHCO3 by H type cell, while MWCNT-Por-COF-Cu exhibits the highest CH4 faradaic efficiency of 71.2% in 1.0 M KOH by flow cell. The results of HRTEM and Auger spectrum revealed that the high performance of MWCNT-Por-COF-Cu could be attributed to the generated Copper-based nanoclusters during the electrocatalytic CO2RR process.
引用
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页数:9
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