Citation: Xueqi Yang, Juntao Zhao, Jiawei Ye, Desen Zhou, Tingmin Di, Jun Zhang. Modulating the d-band center of NNU-55(Fe) for enhanced CO₂ adsorption and photocatalytic activity[J]. Acta Physico-Chimica Sinica, ;2025, 41(7): 100074. doi: 10.1016/j.actphy.2025.100074 shu

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

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 Date: 26 January 2025
Revised Date: 26 February 2025
Accepted Date: 26 February 2025

Fund Project: This study was supported by the National Natural Science Foundation of China (NSFC) (22308341, 22005228) and the Scientific Research Foundation of Wuhan Institute of Technology (K2024047).

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, NO^-₃-coordinated NNU-55(Fe) demonstrated superior catalytic performance compared to SO₄^2-- and Cl^--coordinated catalysts, achieving a CO production of 124 μmol·g^-1 within 3 h. The stronger electron donation capacity of NO^-₃ 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.
- MOFs,
- Coordination structure,
- d-band center,
- CO₂ adsorption,
- Photoreduction
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通讯作者: 陈斌, bchen63@163.com

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沈阳化工大学材料科学与工程学院沈阳 110142

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

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通讯作者: 陈斌, bchen63@163.com

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