调节NNU-55(Fe)的<i>d</i>带中心以增强CO<sub>2</sub>吸附和光催化活性

引用本文: 杨雪琦, 赵俊涛, 叶家伟, 周德森, 狄廷敏, 张军. 调节NNU-55(Fe)的d带中心以增强CO₂吸附和光催化活性[J]. 物理化学学报, 2025, 41(7): 100074. doi: 10.1016/j.actphy.2025.100074 shu

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

调节NNU-55(Fe)的d带中心以增强CO₂吸附和光催化活性

杨雪琦 ^1, ,
赵俊涛 ^1, ,
叶家伟 ^{1,
,} ,
周德森 ^1, ,
狄廷敏 ^{2,
,} ,
张军 ^{1,
,}

1.
武汉工程大学, 化工与制药学院、绿色化工过程教育部重点实验室、新型反应器与绿色化学工艺湖北省重点实验室, 湖北武汉 430205
2.
武汉工程大学, 材料科学与工程学院、等离子体化学与新材料湖北省重点实验室, 湖北武汉 430205

通讯作者: 叶家伟, yejiawei@wit.edu.cn; 狄廷敏, ditingmin19@wit.edu.cn; 张军, junzhang@wit.edu.cn

基金项目:
国家自然科学基金 22308341

国家自然科学基金 22005228

武汉工程大学科学研究基金 K2024047

摘要: 光催化二氧化碳(CO₂)还原已成为一种有效的技术用于将CO₂转化为高价值的化学品。金属有机框架(MOFs)材料因其结构可调、比表面积大、催化性能好和光响应性优异等特点而展现出巨大的潜力。本文采用MOF材料NNU-55(Fe)将CO₂光催化转化为一氧化碳(CO)。通过改变无机阴离子配体调节金属活性中心(Fe-N4)的电子性质，可以轻松调控NNU-55(Fe) MOFs的光催化性能。研究表明，相较于SO₄²⁻和Cl⁻配位的催化剂，NO₃⁻配位的NNU-55(Fe)展现出更优异的催化性能，在3 h内实现了124 μmol∙g⁻¹的CO产量。NO₃⁻更强的电子供给能力提升了Fe中心的电子密度，降低了Fe的d带中心，并增强了吸附系统成键轨道的占据，从而提高了CO₂的吸附能力和还原活性。本研究通过改变金属位点的无机配体来调节MOFs电子结构和催化活性的策略，为开发高效光催化材料提供了新的思路。

关键词:

English

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

Xueqi Yang ^1, ,
Juntao Zhao ^1, ,
Jiawei Ye ^{1,
,} ,
Desen Zhou ^1, ,
Tingmin Di ^{2,
,} ,
Jun Zhang ^{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

Corresponding author: Email: yejiawei@wit.edu.cn (J. Ye); Email: ditingmin19@wit.edu.cn (T. Di); Email: junzhang@wit.edu.cn (J. Zhang)

Received Date: 26 January 2025
Accepted Date: 26 February 2025
Revised Date: 26 February 2025
Available Online: 15 July 2025
Fund Project:
the National Natural Science Foundation of China (NSFC)

the National Natural Science Foundation of China (NSFC)

the Scientific Research Foundation of Wuhan Institute of Technology

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.

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沈阳化工大学材料科学与工程学院沈阳 110142

调节NNU-55(Fe)的d带中心以增强CO₂吸附和光催化活性

通讯作者: 叶家伟, yejiawei@wit.edu.cn; 狄廷敏, ditingmin19@wit.edu.cn; 张军, junzhang@wit.edu.cn

English

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

Corresponding author: Email: yejiawei@wit.edu.cn (J. Ye); Email: ditingmin19@wit.edu.cn (T. Di); Email: junzhang@wit.edu.cn (J. Zhang)

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中国化学会秘书处

调节NNU-55(Fe)的d带中心以增强CO2吸附和光催化活性

通讯作者: 叶家伟, yejiawei@wit.edu.cn; 狄廷敏, ditingmin19@wit.edu.cn; 张军, junzhang@wit.edu.cn

English

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

Corresponding author: Email: yejiawei@wit.edu.cn (J. Ye); Email: ditingmin19@wit.edu.cn (T. Di); Email: junzhang@wit.edu.cn (J. Zhang)

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南： 你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

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CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

调节NNU-55(Fe)的d带中心以增强CO₂吸附和光催化活性

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