CdS/DBTSO-BDTO S型异质结光催化制氢及其电荷转移动力学

doi:10.1016/j.actphy.2025.100084

物理化学学报 >> 2025, Vol. 41 >> Issue (8): 100084.doi: 10.1016/j.actphy.2025.100084

所属专题：光催化中的S型异质结

CdS/DBTSO-BDTO S型异质结光催化制氢及其电荷转移动力学

蔡家杰¹, 程畅², 刘博文¹, 张建军²^,*(), 姜传佳³^,*(), 程蓓¹^,*()

¹ 武汉理工大学材料合成与加工先进技术国家重点实验室, 湖北武汉 430070
² 中国地质大学(武汉)材料科学与化学学院, 太阳能燃料实验室, 湖北武汉 430078
³ 南开大学环境科学与工程学院, 天津 300350

收稿日期:2025-02-20 修回日期:2025-03-10 录用日期:2025-03-24 发布日期:2025-06-07
通讯作者: Email: zhangjianjun@cug.edu.cn (张建军)jiangcj@nankai.edu.cn (姜传佳)chengbei2013@whut.edu.cn (程蓓)
基金资助:
国家重点研发计划项目(2022YFB3803600); 国家自然科学基金项目(22238009); 国家自然科学基金项目(22361142704); 国家自然科学基金项目(22261142666); 国家自然科学基金项目(22278324); 国家自然科学基金项目(52073223); 湖北省自然科学基金项目(2022CFA001); 中央高校基本科研业务费项目(63241632)

CdS/DBTSO-BDTO S-scheme photocatalyst for H₂ production and its charge transfer dynamics

Jiajie Cai¹, Chang Cheng², Bowen Liu¹, Jianjun Zhang²^,*(), Chuanjia Jiang³^,*(), Bei Cheng¹^,*()

¹ State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan 430070, Hubei Province, China
² Laboratory of Solar Fuel, Faculty of Materials Science and Chemistry, China University of Geosciences, Wuhan 430078, Hubei Province, China
³ College of Environmental Science and Engineering, Nankai University, Tianjin 300350, China

Received:2025-02-20 Revised:2025-03-10 Accepted:2025-03-24 Published:2025-06-07
Contact: Email: zhangjianjun@cug.edu.cn (Jianjun Zhang)jiangcj@nankai.edu.cn (Chuanjia Jiang)chengbei2013@whut.edu.cn (Bei Cheng)
Supported by:
the National Key Research and Development Program of China(2022YFB3803600); the National Natural Science Foundation of China(22238009); the National Natural Science Foundation of China(22361142704); the National Natural Science Foundation of China(22261142666); the National Natural Science Foundation of China(22278324); the National Natural Science Foundation of China(52073223); the Natural Science Foundation of Hubei Province of China(2022CFA001); the Fundamental Research Funds for the Central Universities(63241632)

1. ACTPHY-2025.100084-SI-6p.pdf(1739KB)

摘要/Abstract

摘要：

光催化分解水产氢具有广阔的应用前景。然而，单一光催化剂由于光生电子与空穴易复合，导致光催化产氢效率较低，严重制约了该技术的实际应用。构建异质结是克服这些缺点的有效策略，最近S型异质结脱颖而出，显示出了高效的促进电子和空穴分离的能力，同时最大限度地提高光催化剂的氧化还原能力。其中，基于聚合物的S型光催化剂正在兴起，但无机-有机S型异质结中的载流子动力学仍有待阐明。在本工作中，我们制备了由共轭聚合物双氧硫芴苯并二噻吩二酮(dibenzothiophene-S, S-dioxide-alt-benzodithiophene, DBTSO-BDTO)和硫化镉(CdS)组成的S型异质结，并研究了其光催化制氢的性能和界面电荷传输机制。利用原位辐照X射线光电子能谱验证了S型电子转移机理，并利用飞秒瞬态吸收光谱深入分析了S型异质结中载流子的动力学，证实有大量光生电子发生了界面电荷转移。由于S型异质结对载流子效率的提高和氧化还原能力的增强，复合材料的性能超过了DBTSO-BDTO和CdS，并且最优化复合材料的析氢速率达到3313 μmol·h⁻¹·g⁻¹，约为纯CdS的3倍。本工作为S型异质结的电子转移机制提供了新的视角，并可指导用于太阳能燃料生产的聚合物基光催化剂的开发。

关键词: 光催化, 硫化镉, S型异质结, 产氢, 飞秒瞬态吸收光谱

Abstract:

Photocatalytic hydrogen (H₂) production is a clean energy technology, with great potential for addressing the global energy crisis and related environmental problems. However, single-component photocatalysts often suffer from low efficiency primarily due to fast charge carrier recombination and the tradeoff between light-absorbing capacity and redox capabilities. Constructing heterojunctions provides a promising strategy to overcome these drawbacks, and S-scheme heterojunctions have recently stood out, demonstrating the capability to efficiently facilitate electron/hole separation, while maximizing the redox capability. Among them, polymer-based S-scheme photocatalysts are emerging, though the charge carrier dynamics in inorganic-organic S-scheme heterojunctions remain to be elucidated. Herein, we fabricated an S-scheme heterojunction comprised of the conjugated polymer dibenzothiophene-S, S-dioxide-alt-benzodithiophene (DBTSO-BDTO) and cadmium sulfide (CdS) for photocatalytic H₂ production. The S-scheme mechanism was verified using in situ irradiated X-ray photoelectron spectroscopy, and the charge carrier transfer dynamics were analyzed in depth using femtosecond transient absorption spectroscopy, which revealed that a considerable fraction of electrons undergo interfacial charge transfer in the CdS/DBTSO-BDTO composite. Owing to the improved charge separation efficiency and redox capability, the performance of the composite surpassed that of DBTSO-BDTO and CdS, and the H₂ evolution rate of the optimized CdS/DBTSO-BDTO material reached 3313 μmol·h⁻¹·g⁻¹, three times that of pure CdS. The findings provide new insights into the electron transfer mechanisms of S-scheme heterojunctions, and can guide the design of polymer-based photocatalysts for solar fuel production.

Key words: Photocatalysis, Cadmium sulfide, S-scheme heterojunction, H₂ production, Femtosecond transient absorption spectroscopy

蔡家杰, 程畅, 刘博文, 张建军, 姜传佳, 程蓓. CdS/DBTSO-BDTO S型异质结光催化制氢及其电荷转移动力学[J]. 物理化学学报, 2025, 41(8), 100084. doi: 10.1016/j.actphy.2025.100084

Jiajie Cai, Chang Cheng, Bowen Liu, Jianjun Zhang, Chuanjia Jiang, Bei Cheng. CdS/DBTSO-BDTO S-scheme photocatalyst for H₂ production and its charge transfer dynamics[J]. Acta Phys. -Chim. Sin. 2025, 41(8), 100084. doi: 10.1016/j.actphy.2025.100084

链接本文: https://www.whxb.pku.edu.cn/CN/10.1016/j.actphy.2025.100084

https://www.whxb.pku.edu.cn/CN/Y2025/V41/I8/100084

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CdS/DBTSO-BDTO S型异质结光催化制氢及其电荷转移动力学

CdS/DBTSO-BDTO S-scheme photocatalyst for H₂ production and its charge transfer dynamics

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CdS/DBTSO-BDTO S型异质结光催化制氢及其电荷转移动力学

CdS/DBTSO-BDTO S-scheme photocatalyst for H2 production and its charge transfer dynamics

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CdS/DBTSO-BDTO S-scheme photocatalyst for H₂ production and its charge transfer dynamics