Acta Phys. -Chim. Sin. ›› 2025, Vol. 41 ›› Issue (7): 100074.doi: 10.1016/j.actphy.2025.100074

Special Issue: S-scheme heterojunction in photocatalysis

• ARTICLE • Previous Articles     Next Articles

Modulating the d-band center of NNU-55(Fe) for enhanced CO2 adsorption and photocatalytic activity

Xueqi Yang1, Juntao Zhao1, Jiawei Ye1,*(), Desen Zhou1, Tingmin Di2,*(), Jun Zhang1,*()   

  1. 1 Key Laboratory of Green Chemical Process of Ministry of Education, Hubei Key Laboratory of Novel Reactor and Green Chemical Technology, School of Chemical Engineering and Pharmacy, Wuhan Institute of Technology, Wuhan 430205, Hubei Province, China
    2 Hubei Key Laboratory of Plasma Chemistry and Advanced Materials, School of Materials Science and Engineering, Wuhan Institute of Technology, Wuhan 430205, Hubei Province, China
  • Received:2025-01-26 Revised:2025-02-26 Accepted:2025-02-26 Published:2025-05-22
  • Contact: Email: yejiawei@wit.edu.cn (Jiawei Ye)ditingmin19@wit.edu.cn (Tingmin Di)junzhang@wit.edu.cn (Jun Zhang)
  • Supported by:
    the National Natural Science Foundation of China (NSFC)(22308341); the National Natural Science Foundation of China (NSFC)(22005228); the Scientific Research Foundation of Wuhan Institute of Technology(K2024047)

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Abstract:

Photocatalytic reduction of carbon dioxide (CO2) has emerged as an effective technology to transform CO2 into valuable chemicals. Metal-organic frameworks (MOFs) show great promise due to their adjustable structures, huge specific surface areas, excellent catalytic properties, and remarkable photo responsiveness. Herein, the MOF material NNU-55(Fe) was employed for the photocatalytic transformation of CO2 into carbon monoxide (CO). Through electronic modulation of the active metal center (Fe-N4) via inorganic anionic ligand tuning, the photocatalytic performance of NNU-55(Fe) MOFs can be easily regulated. Notably, NO3−-coordinated NNU-55(Fe) demonstrated superior catalytic performance compared to SO42−- and Cl−-coordinated catalysts, achieving a CO production of 124 μmol∙g−1 within 3 h. The stronger electron donation capacity of NO3− leads to an improved electron density of Fe centers, which lowers the Fe d-band center and enhances the bonding orbital occupancy in the adsorption system, thereby increasing the adsorption strength of CO2 and reduction activity. This study highlights a simple strategy for altering the catalytic activity and electrical structure of MOFs by altering the coordinated inorganic ligands of metal sites, offering a novel approach to developing efficient photocatalytic materials.

Key words: MOFs, Coordination structure, d-band center, CO2 adsorption, Photoreduction