Photocatalytic CO2 conversion over single-atom MoN2 sites of covalent organic framework

被引:202
作者
Kou, Mingpu [1 ,2 ]
Liu, Wei [1 ]
Wang, Yongye [1 ]
Huang, Jindi [2 ]
Chen, Yanli [2 ]
Zhou, Ying [3 ]
Chen, Yi [3 ]
Ma, Minzhi [3 ]
Lei, Kai [4 ]
Xie, Haiquan [2 ]
Wong, Po Keung [5 ]
Ye, Liqun [1 ]
机构
[1] China Three Gorges Univ, Coll Mat & Chem Engn, Key Lab Inorgan Nonmetall Crystalline & Energy Co, Yichang 443002, Peoples R China
[2] Nanyang Normal Univ, Coll Chem & Pharmaceut Engn, Engn Technol Res Ctr Henan Prov Solar Catalysis, Nanyang 473061, Peoples R China
[3] Southwest Petr Univ, Sch Oil & Nat Gas Engn, State Key Lab Oil & Gas Reservoir Geol & Exploita, Chengdu 610500, Peoples R China
[4] Huazhong Univ Sci & Technol HUST, Wuhan Natl Lab Optoelect, Sch Chem & Chem Engn,Hubei Key Lab Mat Chem & Ser, Minist Educ,Key Lab Mat Chem Energy Convers & Sto, Luoyu Rd, Wuhan 430074, Peoples R China
[5] Chinese Univ Hong Kong, Sch Life Sci, Shatin, Hong Kong 999007, Peoples R China
基金
中国国家自然科学基金;
关键词
Covalent organic framework; Photocatalysis; CO2; Single atom; REDUCTION; PHASE; WATER;
D O I
10.1016/j.apcatb.2021.120146
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
The application of covalent organic framework (COF) for photocatalytic CO2 conversion has received more and more attention. However, it is still a challenge for photocatalytic conversion of CO2 with atmosphere concentration to high added value hydrocarbons products (CxHy) such as CH4 and C2H4. Here, integrating the advantages of micropore structure and single atom catalysis, we introduced single- atom MoN2 sites into COF to construct Mo-COF materials. The aberration-COrrected high-angle annular dark-field scanning transmission electron microscopy (HAADF- STEM) confirms that Mo single atom on COF. Mo-COF can reduce CO2 to CxHy under visible light with a selectivity of 42.92 % and C2H4 product was found for the the first time. In-situ fourier transform infrared spectrometer (In situ FT-IR) and theoretical calculation showed that the introduction of single-atom MoN2 sites is the key to improving the catalysis performance. It also provides a new idea for converting CO2 into high added value CxHy products.
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页数:8
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