TiO<sub>2</sub>/CdS S型异质结促进光催化CO<sub>2</sub>甲烷化及其飞秒瞬态吸收光谱机理研究

引用本文: 霍怡廷, 周欣, 赵非凡, 艾陈斌, 吴珍, 常志东, 朱必成. TiO₂/CdS S型异质结促进光催化CO₂甲烷化及其飞秒瞬态吸收光谱机理研究[J]. 物理化学学报, 2025, 41(11): 100148. doi: 10.1016/j.actphy.2025.100148 shu

Citation: Yiting Huo, Xin Zhou, Feifan Zhao, Chenbin Ai, Zhen Wu, Zhidong Chang, Bicheng Zhu. Boosting photocatalytic CO₂ methanation through TiO₂/CdS S-scheme heterojunction and fs-TAS mechanism study[J]. Acta Physico-Chimica Sinica, 2025, 41(11): 100148. doi: 10.1016/j.actphy.2025.100148 shu

TiO₂/CdS S型异质结促进光催化CO₂甲烷化及其飞秒瞬态吸收光谱机理研究

霍怡廷 ^{1, 2, 3,} ,
周欣 ^2, ,
赵非凡 ^3, ,
艾陈斌 ^3, ,
吴珍 ^2, ,
常志东 ^{1,
,} ,
朱必成 ^{3,
,}

1.
北京科技大学化学与生物工程学院, 北京 100083
2.
鄂尔多斯应用技术学院化学工程学院, 内蒙古鄂尔多斯 017000
3.
中国地质大学材料与化学学院太阳燃料实验室, 湖北武汉 430078

通讯作者: 常志东, zdchang@ustb.edu.cn; 朱必成, zhubicheng@cug.edu.cn

基金项目:
国家自然科学基金 52173065

国家自然科学基金 22469001

内蒙古自然科学基金 2025QN05107

内蒙古自然科学基金 2025ZDLH002

摘要: 通过光催化将CO₂转化为高附加值碳氢化合物在可持续能源领域具有巨大潜力，但实现高活性和选择性仍然具有挑战性。本文中，一种新型的TiO₂/CdS异质结光催化剂在光催化CO₂还原中表现出优异的性能。优化后的催化剂的CH₄产率比纯TiO₂提高了4.2倍，且对CH₄的选择性高达65.4% (CO为34.6%)。其增强的活性源于独特的形貌，促进了CO₂的吸附和传质，以及CdS与TiO₂之间形成紧密的S型异质结，这提高了电荷分离效率，同时保持了强氧化还原电位。并且，飞秒瞬态吸收光谱(fs-TAS)与原位漫反射红外傅里叶变换光谱(DRIFTS)相结合，为光催化二氧化碳还原路径提供了直接证据，并确定了CdS上的硫位点是稳定*CH₃O、*CHO和*CO中间体的关键，从而促进选择性生成CH₄。此外，基于密度泛函理论(DFT)的理论计算进一步补充了实验结果。计算证实了S型异质结的电子结构特征，揭示了原子尺度上的能级和电荷转移机制。这不仅加深了我们对光催化过程的理解，还为进一步优化光催化剂设计提供了理论基础。总体而言，我们的工作展示了TiO₂/CdS异质结光催化剂在光催化CO₂还原中的优异性能。

关键词:

English

Boosting photocatalytic CO₂ methanation through TiO₂/CdS S-scheme heterojunction and fs-TAS mechanism study

1.
School of Chemistry and Biological Engineering, University of Science and Technology Beijing, Beijing, 100083, China
2.
School of Chemical Engineering, Ordos Institute of Technology, Ordos, 017000, Inner Mongolia, China
3.
Laboratory of Solar Fuel, Faculty of Materials Science and Chemistry, China University of Geosciences, Wuhan 430078, Hubei Province, China

Corresponding author: Email: zdchang@ustb.edu.cn (Z.C.); Email: zhubicheng@cug.edu.cn (B.Z.)

Received Date: 16 July 2025
Accepted Date: 03 August 2025
Revised Date: 30 July 2025
Available Online: 15 November 2025
Fund Project:
the National Natural Science Foundation of China

the National Natural Science Foundation of China

Natural Science Foundation of Inner Mongolia Autonomous Region of China

Natural Science Foundation of Inner Mongolia Autonomous Region of China

Abstract: The conversion of CO₂ into value-added hydrocarbons via photocatalysis holds great promise for sustainable energy, yet achieving high activity and selectivity remains challenging. Herein, a novel TiO₂/CdS heterostructured photocatalyst exhibits exceptional performance in CO₂ photoreduction. The optimized catalyst delivers a 4.2-fold increase in CH₄ production rate compared to pristine TiO₂, with a remarkable 65.4% selectivity toward CH₄ (34.6% CO). The enhanced activity arises from the unique morphology, facilitating CO₂ adsorption and mass transfer, and the intimate S-scheme heterojunction between CdS and TiO₂, which boosts charge separation while preserving strong redox potentials. Critically, femtosecond transient absorption spectroscopy (fs-TAS) combined with in situ DRIFTS provides direct evidence for the S-scheme pathway and identifies sulfur sites on CdS as key for stabilizing *CH₃O, *CHO and *CO intermediates, steering selectivity toward CH₄. In addition, theoretical calculations based on density functional theory (DFT) further complement the experimental findings. The calculations confirm the electronic structure characteristics of the S-scheme heterojunction, revealing the energy levels and charge transfer mechanisms at the atomic scale. This not only deepens our understanding of the photocatalytic process but also provides a theoretical basis for further optimizing the photocatalyst design. Overall, our work demonstrates the outstanding performance of the TiO₂/CdS heterostructured photocatalyst in CO₂ photoreduction.

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沈阳化工大学材料科学与工程学院沈阳 110142

TiO₂/CdS S型异质结促进光催化CO₂甲烷化及其飞秒瞬态吸收光谱机理研究

通讯作者: 常志东, zdchang@ustb.edu.cn; 朱必成, zhubicheng@cug.edu.cn

English

Boosting photocatalytic CO₂ methanation through TiO₂/CdS S-scheme heterojunction and fs-TAS mechanism study

Corresponding author: Email: zdchang@ustb.edu.cn (Z.C.); Email: zhubicheng@cug.edu.cn (B.Z.)

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TiO2/CdS S型异质结促进光催化CO2甲烷化及其飞秒瞬态吸收光谱机理研究

通讯作者: 常志东, zdchang@ustb.edu.cn; 朱必成, zhubicheng@cug.edu.cn

English

Boosting photocatalytic CO2 methanation through TiO2/CdS S-scheme heterojunction and fs-TAS mechanism study

Corresponding author: Email: zdchang@ustb.edu.cn (Z.C.); Email: zhubicheng@cug.edu.cn (B.Z.)

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

TiO₂/CdS S型异质结促进光催化CO₂甲烷化及其飞秒瞬态吸收光谱机理研究

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