Tailoring Co Coordination Mode in COF Nanosheets for Efficient Solar‐Driven Reduction of Non‐Neat CO<sub>2</sub> into Syngas
Abstract
AbstractPhotocatalytic conversion of CO2 into syngas is a promising approach to solving energy and environmental challenges. However, the current studies are mainly conducted by using neat CO2 where CO2 enrichment and purification is an energy‐intensive process. Herein, we report a Co‐COOH‐COF with an asymmetric tridentate ligand for syngas synthesis from different contents of CO2. The nanosheets of the resulting champion catalyst, Co17.7‐COOH‐COF enable an outstanding syngas production rate of 151.1 mmol g−1 h−1 from neat CO2 and 180.5 mmol g−1 h−1 from 40 vol% CO2 under visible light, while it is up to 112.3 mmol g−1 h−1 from neat CO2 and 116.0 mmol g−1 h−1 from 40 vol% CO2 under natural sunlight, which surpasses most of the previously reported state‐of‐the‐art photocatalysts. Impressively, the catalyst also exhibits a widely and continuously adjustable CO/H2 molar ratio from 4:1 to 1:21. Experimental and theoretical studies indicate that the asymmetric tridentate ligand with carboxyl groups increases Co loading in the covalent organic frame (COF) by the formation of atomically dispersed N–Co–O4 sites and enhances dissociation of water and CO2 adsorption by hydrogen bonding, thus facilitating CO2 transformation and hydrogen evolution. This work presents a new pathway for the design of high‐performance catalysts for the photoreduction of CO2 to syngas.
Article Details
Authors (7)
Yunjing Deng
Collaborative Innovation Center of Henan Province for Green Manufacturing of Fine Chemicals Key Laboratory of Green Chemical Media and Reactions Ministry of Education (China) School of Chemistry and Chemical Engineering Henan Normal University Xinxiang Henan 453007 P.R. China
Huiyong Wang
School of Chemistry and Chemical Engineering, Key Laboratory of Green Chemical Media and Reactions, Ministry of Education, Henan Normal University, 46 Jianshe Road, Xinxiang, Henan 453007, P. R. China
Qian Zhang
Shuaiqi Gao
Collaborative Innovation Center of Henan Province for Green Manufacturing of Fine Chemicals Key Laboratory of Green Chemical Media and Reactions Ministry of Education (China) School of Chemistry and Chemical Engineering Henan Normal University Xinxiang Henan 453007 P.R. China
Yun Ma
Hongshuai Gao
Zhejiang Engineering Research Center for Biological Control of Crop Pathogens and Insects, Zhejiang Key Laboratory of Biology and Ecological Regulation of Crop Pathogens and Insects, Ministry of Agriculture and Rural Affairs Key Lab of Molecular Biology of Crop Pathogens and Insect Pests, State Key Lab of Rice Biology and Breeding, Institute of Insect Sciences, College of Agriculture and Biotechnology, Zhejiang University
Jianji Wang
School of Chemistry and Chemical Engineering, Key Laboratory of Green Chemical Media and Reactions, Ministry of Education, Henan Normal University, 46 Jianshe Road, Xinxiang, Henan 453007, P. R. China