Enhancing CO <sub>2</sub> Photoreduction Efficiency Through Improved Interaction Enabled by a Decorated Covalent‐Organic Framework
Abstract
Abstract Photoreduction of CO 2 is often hindered by the sluggish kinetics for its activation. Refinement of host–guest interactions is an effective strategy to overcome this barrier. Here, we report the immobilization of active Co(II) sites within a covalent‐organic framework (COF) with a one‐dimensional (1D) chain structure, Co‐PyPDA‐COF, which demonstrates a remarkable CO generation rate of 30.5 mmol g −1 h −1 and a high CO selectivity of 95.8% in 2 h for CO 2 photoreduction at room temperature. The pore size of Co‐PyPDA‐COF is comparable to the diameter of CO 2 , which allows simultaneous interaction of a single CO 2 molecule with the two Co(II) sites. The enhanced interaction result in increased local CO 2 pressure, limited CO 2 diffusion after adsorption, shortened distance for photoelectron transfer, and reduced energy barrier for the rate‐determining step in CO 2 reduction, promoting CO 2 activation and conversion. This work opens a new way to design efficient catalysts by optimizing the pore size of the host.
Article Details
Authors (16)
Wenling Zhao
Beijing National Laboratory for Molecular Sciences, CAS Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Centre for Excellence in Molecular Sciences, Centre for Carbon Neutral Chemistry
Jiangnan Li
College of Chemistry and Molecular Engineering, Beijing National Laboratory for Molecular Sciences
Ke Li
Jiapeng Jiao
Shanghai Key Laboratory of Green Chemistry and Chemical Processes, State Key Laboratory of Petroleum Molecular & Process Engineering, School of Chemistry and Molecular Engineering
Shiqiang Liu
Beijing National Laboratory for Molecular Sciences, CAS Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Centre for Excellence in Molecular Sciences, Centre for Carbon Neutral Chemistry
Jiahao Yang
Xiamen University , , ,
Mark D. Frogley
Diamond Light Source, Harwell Science Campus, Oxfordshire OX11 0DE, U.K.
Yaguang Peng
Beijing National Laboratory for Molecular Sciences, CAS Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Centre for Excellence in Molecular Sciences, Centre for Carbon Neutral Chemistry
Yiyong Wang
Beijing National Laboratory for Molecular Sciences, CAS Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Centre for Excellence in Molecular Sciences, Centre for Carbon Neutral Chemistry
Hengan Wang
Beijing National Laboratory for Molecular Sciences, CAS Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Centre for Excellence in Molecular Sciences, Centre for Carbon Neutral Chemistry
Shipeng Zhang
Beijing National Laboratory for Molecular Sciences, CAS Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Centre for Excellence in Molecular Sciences, Centre for Carbon Neutral Chemistry
Lihong Jing
Beijing National Laboratory for Molecular Sciences, CAS Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Center for Excellence in Molecular Sciences, Center for Carbon Neutral Chemistry
Chengcheng Liu
Institute of Frontier Chemistry, School of Chemistry and Chemical Engineering
Sihai Yang
Peking University , , ,
Xinchen Kang
Institute of Chemistry, Chinese Academy of Sciences , , ,
Buxing Han
Institute of Chemistry, Chinese Academy of Sciences , , ,