CdS/DBTSO-BDTO S型异质结光催化制氢及其电荷转移动力学

引用本文: 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 shu

Citation: 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 Physico-Chimica Sinica, 2025, 41(8): 100084. doi: 10.1016/j.actphy.2025.100084 shu

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

通讯作者: 张建军, zhangjianjun@cug.edu.cn; 姜传佳, jiangcj@nankai.edu.cn; 程蓓, chengbei2013@whut.edu.cn

基金项目:
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

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:

English

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

Jiajie Cai ^1, ,
Chang Cheng ^2, ,
Bowen Liu ^1, ,
Jianjun Zhang ^{2,
,} ,
Chuanjia Jiang ^{3,
,} ,
Bei Cheng ^{1,
,}

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

Corresponding author: Email: zhangjianjun@cug.edu.cn (J.J. Zhang); Email: jiangcj@nankai.edu.cn (C.J. Jiang); Email: chengbei2013@whut.edu.cn (B. Cheng)

Received Date: 20 February 2025
Accepted Date: 24 March 2025
Revised Date: 10 March 2025
Available Online: 15 August 2025
Fund Project:
the National Key Research and Development Program of China

the National Natural Science Foundation of China

the National Natural Science Foundation of China

the National Natural Science Foundation of China

the National Natural Science Foundation of China

the National Natural Science Foundation of China

the Natural Science Foundation of Hubei Province of China

the Fundamental Research Funds for the Central Universities

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

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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

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