A Covalent Organic Framework Bearing Single Ni Sites as a Synergistic Photocatalyst for Selective Photoreduction of CO 2 to CO
Photocatalytic reduction of CO into energy-rich carbon compounds has attracted increasing attention. However, it is still a challenge to selectively and effectively convert CO to a desirable reaction product. Herein, we report a design of a synergistic photocatalyst for selective reduction of CO to...
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| Published in | Journal of the American Chemical Society Vol. 141; no. 18; pp. 7615 - 7621 |
|---|---|
| Main Authors | , , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
United States
08.05.2019
|
| Online Access | Get full text |
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| Abstract | Photocatalytic reduction of CO
into energy-rich carbon compounds has attracted increasing attention. However, it is still a challenge to selectively and effectively convert CO
to a desirable reaction product. Herein, we report a design of a synergistic photocatalyst for selective reduction of CO
to CO by using a covalent organic framework bearing single Ni sites (Ni-TpBpy), in which electrons transfer from photosensitizer to Ni sites for CO production by the activated CO
reduction under visible-light irradiation. Ni-TpBpy exhibits an excellent activity, giving a 4057 μmol g
of CO in a 5 h reaction with a 96% selectivity over H
evolution. More importantly, when the CO
partial pressure was reduced to 0.1 atm, 76% selectivity for CO production is still obtained. Theoretical calculations and experimental results suggest that the promising catalytic activity and selectivity are ascribed to synergistic effects of single Ni catalytic sites and TpBpy, in which the TpBpy not only serves as a host for CO
molecules and Ni catalytic sites but also facilitates the activation of CO
and inhibits the competitive H
evolution. |
|---|---|
| AbstractList | Photocatalytic reduction of CO
into energy-rich carbon compounds has attracted increasing attention. However, it is still a challenge to selectively and effectively convert CO
to a desirable reaction product. Herein, we report a design of a synergistic photocatalyst for selective reduction of CO
to CO by using a covalent organic framework bearing single Ni sites (Ni-TpBpy), in which electrons transfer from photosensitizer to Ni sites for CO production by the activated CO
reduction under visible-light irradiation. Ni-TpBpy exhibits an excellent activity, giving a 4057 μmol g
of CO in a 5 h reaction with a 96% selectivity over H
evolution. More importantly, when the CO
partial pressure was reduced to 0.1 atm, 76% selectivity for CO production is still obtained. Theoretical calculations and experimental results suggest that the promising catalytic activity and selectivity are ascribed to synergistic effects of single Ni catalytic sites and TpBpy, in which the TpBpy not only serves as a host for CO
molecules and Ni catalytic sites but also facilitates the activation of CO
and inhibits the competitive H
evolution. |
| Author | Sa, Rongjian Bi, Jinhong Li, Lingyun Zhuang, Zanyong Yu, Yan Li, Liuyi He, Yajun Zou, Zhigang Zhong, Wanfu |
| Author_xml | – sequence: 1 givenname: Wanfu surname: Zhong fullname: Zhong, Wanfu organization: Key Laboratory of Eco-materials Advanced Technology, College of Materials Science and Engineering , Fuzhou University , Fuzhou 350108 , China – sequence: 2 givenname: Rongjian surname: Sa fullname: Sa, Rongjian organization: Institute of Oceanography, Ocean College , Minjiang University , Fuzhou , Fujian 350108 , China – sequence: 3 givenname: Liuyi orcidid: 0000-0002-3066-2991 surname: Li fullname: Li, Liuyi organization: Key Laboratory of Eco-materials Advanced Technology, College of Materials Science and Engineering , Fuzhou University , Fuzhou 350108 , China – sequence: 4 givenname: Yajun surname: He fullname: He, Yajun organization: Key Laboratory of Eco-materials Advanced Technology, College of Materials Science and Engineering , Fuzhou University , Fuzhou 350108 , China – sequence: 5 givenname: Lingyun orcidid: 0000-0003-0450-097X surname: Li fullname: Li, Lingyun organization: Key Laboratory of Eco-materials Advanced Technology, College of Materials Science and Engineering , Fuzhou University , Fuzhou 350108 , China – sequence: 6 givenname: Jinhong orcidid: 0000-0002-8141-7742 surname: Bi fullname: Bi, Jinhong organization: Key Laboratory of Eco-materials Advanced Technology, College of Materials Science and Engineering , Fuzhou University , Fuzhou 350108 , China – sequence: 7 givenname: Zanyong orcidid: 0000-0002-6367-3726 surname: Zhuang fullname: Zhuang, Zanyong organization: Key Laboratory of Eco-materials Advanced Technology, College of Materials Science and Engineering , Fuzhou University , Fuzhou 350108 , China – sequence: 8 givenname: Yan orcidid: 0000-0001-6748-2620 surname: Yu fullname: Yu, Yan organization: Key Laboratory of Eco-materials Advanced Technology, College of Materials Science and Engineering , Fuzhou University , Fuzhou 350108 , China – sequence: 9 givenname: Zhigang surname: Zou fullname: Zou, Zhigang organization: Eco-materials and Renewable Energy Research Center, College of Engineering and Applied Sciences , Nanjing University , Nanjing 210093 , China |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/30998334$$D View this record in MEDLINE/PubMed |
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