CoN2O2 sites in carbon nanosheets by template-pyrolysis of COFs for CO2RR

被引：49

作者：

Miao, Qiyang ^{[1
,2
]}

Lu, Chengbao ^{[2
,3
]}

Xu, Qing ^{[2
,4
]}

Yang, Shuai ^{[4
,5
]}

Liu, Minghao ^{[2
,4
]}

Liu, Sijia ^{[2
,4
]}

Yu, Chengbing ^{[1
]}

Zhuang, Xiaodong ^{[2
]}

Jiang, Zheng ^{[4
,5
]}

Zeng, Gaofeng ^{[2
,4
]}

机构：

[1] Shanghai Univ, Dept Sch Mat Sci & Engn, Shanghai 200444, Peoples R China

[2] Chinese Acad Sci, Shanghai Adv Res Inst, CAS Key Lab Low Carbon Convers Sci & Engn, Shanghai 201800, Peoples R China

[3] Shanghai Jiao Tong Univ, Sch Chem & Chem Engn, Shanghai 200240, Peoples R China

[4] Univ Chinese Acad Sci, Sch Chem Engn, 19A Yuquan Rd, Beijing 100049, Peoples R China

[5] Chinese Acad Sci, Shanghai Adv Res Inst, Shanghai Synchrotron Radiat Facil, Shanghai, Peoples R China

来源：

CHEMICAL ENGINEERING JOURNAL | 2022年 / 450卷

基金：

上海市自然科学基金; 中国国家自然科学基金;

关键词：

Covalent organic frameworks; Two-dimensional carbons; Single atom catalysts; CO2; reduction; CoN2O2; sites; COVALENT ORGANIC FRAMEWORKS; LAYERED DOUBLE HYDROXIDE; REDUCTION; CATALYSIS; ELECTROREDUCTION;

D O I：

10.1016/j.cej.2022.138427

中图分类号：

X [环境科学、安全科学];

学科分类号：

08 ; 0830 ;

摘要：

Electrocatalytic CO2 reduction (CO2RR) is critical in addressing CO2 emissions. Single atom catalysts, are attracting considerable attention for CO2RR because of their high atom utilization efficiencies and tailored electron states. However, the catalytic sites remain limited and developing novel catalytic centers is a significant and challenge. Herein, for the first time, we fabricated CoN2O2 sites in 2D carbon for use in CO2RR via template pyrolysis of covalent organic frameworks (COFs). After forming the COF on the surface of Mg/Al-LDH, the obtained catalyst displayed a layered morphology with a thickness of approximately 36 nm and had abundant CoN2O2 sites (4.27 wt% Co). The catalyst showed a remarkable catalytic activity towards CO2RR, with Faradaic efficiencies of 80.2-96.5 % at applied potentials between -0.6 and -1.0 V. Theoretical calculations showed that the CoN2O2 sites favor the stretching and cleavage of COOH* at the Co active centers, accelerating the rate-determining step of COOH* formation.

引用

页数：7

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