Issue 14, 2025

Cobalt-ion center engineering in ZIF-67 for enhanced photothermal catalytic CO2 reduction: mechanistic insights into intermediate regulation and activity optimization

Abstract

Herein, a detailed study of ZIF-67 CO2 photothermal reduction catalysts was carried out, including the characterization of their physicochemical properties, photothermal catalytic performances and reaction mechanisms. Through the systematic characterization of ZIF-67 catalyst samples, the differences in their crystal structures, morphological features, specific surface areas and optical properties were investigated. In addition, the catalytic mechanism of the catalysts was investigated in detail by in situ DRIFTS and DFT calculations. The experimental results showed that among the ZIF-67 catalyst prepared with different ratios of Co2+ and 2-MI precursors, the ZIF-67 (8–1) catalyst exhibited an distinct crystal lattice structure, strongest photoelectron transfer ability, and largest specific surface area, resulting in an optimal catalytic activity (total yield = 4.71 μmol g−1 h−1). The band gap width of this material could be controlled by regulating the content of Co metal-ion centers to promote the photogenerated charge transfer in the adsorption–reduction process of CO2, corresponding to an enhancement in its catalytic activity. The mechanism of CO2 catalytic reduction showed that *COOH and *CHO are the key intermediates in the rate-controlling steps in the CO2 catalytic reduction reaction, and the energy barrier of the former controlled the reaction product yield, while that of the latter was the key to regulate product selectivity.

Graphical abstract: Cobalt-ion center engineering in ZIF-67 for enhanced photothermal catalytic CO2 reduction: mechanistic insights into intermediate regulation and activity optimization

Article information

Article type
Paper
Submitted
01 Apr 2025
Accepted
01 Jun 2025
First published
16 Jun 2025

Catal. Sci. Technol., 2025,15, 4303-4318

Cobalt-ion center engineering in ZIF-67 for enhanced photothermal catalytic CO2 reduction: mechanistic insights into intermediate regulation and activity optimization

B. Guan, J. Chen, L. Zhu, Z. Zhuang, X. Hu, C. Zhu, S. Zhao, K. Shu, H. Dang, J. Gao, L. Zhang, T. Zhu, W. Zeng, M. Qian, Z. Li, Y. Lu, S. Chen and Z. Huang, Catal. Sci. Technol., 2025, 15, 4303 DOI: 10.1039/D5CY00395D

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