物理化学学报 >> 2024, Vol. 40 >> Issue (11): 2406027.doi: 10.3866/PKU.WHXB202406027

所属专题： 太阳燃料制备

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ZnO/D-A共轭聚合物S型异质结高效光催化产H2O2及其电荷转移动力学研究

吴优1,2, 程畅2, 戚克振1,*(), 程蓓2,*(), 张建军3,*(), 余家国3, 张留洋3   

  1. 1 大理大学, 药学院, 云南 大理 671000
    2 武汉理工大学, 材料复合新技术国家重点实验室, 湖北 武汉 430070
    3 中国地质大学(武汉), 材料与化学学院太阳燃料实验室, 湖北 武汉 430078
  • 收稿日期:2024-06-21 修回日期:2024-07-25 录用日期:2024-07-26 发布日期:2024-10-14
  • 通讯作者: Email: qkzh2003@aliyun.com (戚克振)chengbei2013@whut.edu.cn (程蓓)zhangjianjun@cug.edu.cn (张建军)

Efficient Photocatalytic Production of H2O2 over ZnO/D-A Conjugated Polymer S-scheme Heterojunction and Charge Transfer Dynamics Investigation

You Wu1,2, Chang Cheng2, Kezhen Qi1,*(), Bei Cheng2,*(), Jianjun Zhang3,*(), Jiaguo Yu3, Liuyang Zhang3   

  1. 1 College of Pharmacy, Dali University, Dali 671000, Yunnan Province, China
    2 State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan 430070, China
    3 Laboratory of Solar Fuel, Faculty of Materials Science and Chemistry, China University of Geosciences, Wuhan 430078, China
  • Received:2024-06-21 Revised:2024-07-25 Accepted:2024-07-26 Published:2024-10-14
  • Contact: Email: qkzh2003@aliyun.com (Kezhen Qi)chengbei2013@whut.edu.cn (Bei Cheng)zhangjianjun@cug.edu.cn (Jianjun Zhang)
  • Supported by:
    Yunnan Provincial Science and Technology Plan Project(202305AF150116); the National Natural Science Foundation of China(22238009); the National Natural Science Foundation of China(U23A20102); the National Natural Science Foundation of China(52073223); the National Natural Science Foundation of China(22278324); the National Natural Science Foundation of China(22361142704); the Natural Science Foundation of Hubei Province of China(2022CFA001); the Fundamental Research Funds for the Central Universities, China University of Geosciences (Wuhan)(CUG22061)

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摘要：

光催化技术利用清洁、无污染的太阳能合成过氧化氢(H2O2)。本研究通过铃木-宫浦反应和水热法合成了ZnO/PBD S型异质结复合材料，其特点是在供体-受体共轭聚合物(PBD)基底上生长ZnO纳米颗粒。最佳ZnO/PBD复合材料的产H2O2效率为4.07 mmol∙g-1∙h-1，是原始ZnO的5.4倍。该性能的显著提高归功于S型异质结的形成。紫外可见漫反射吸收光谱和原位光照X射线光电子能谱证实了S型异质结的成功构建。稳态光致发光和飞秒瞬态吸收(fs-TA)光谱确定并验证了ZnO中缺陷态的存在。这些缺陷态会捕获光生电子，从而对光催化反应产生不利影响。然而，S型异质结有效地促进了电子的分离和转移，从而缓解了这一问题。通过拟合fs-TA衰减动力学曲线确定的这些缺陷态中光生电子的寿命，进一步证明了S型异质结中的载流子转移机制。该工作介绍了一种利用fs-TA光谱研究有机/无机S型异质结的新方法。

关键词: 光催化产H2O2, S型异质结, ZnO缺陷态, fs-TA光谱

Abstract:

Photocatalytic technology harnesses clean, non-polluting solar energy to synthesize hydrogen peroxide (H2O2). In this study, ZnO/PBD S-scheme heterojunction composites, featuring ZnO nanoparticles on a donor-acceptor conjugated polymer substrate (PBD), were synthesized via the Suzuki-Miyaura reaction and hydrothermal method. The optimal ZnO/PBD composite achieved an H2O2 production efficiency of 4.07 mmol·g-1·h-1, which is 5.4 times higher than that of pristine ZnO. This significant enhancement is attributed to the formation of S-scheme heterojunctions. The successful construction of S-scheme heterojunctions was confirmed through UV-visible absorption spectroscopy and in situ irradiated X-ray photoelectron spectroscopy. Steady-state photoluminescence and femtosecond transient absorption (fs-TA) spectroscopies identified and verified the presence of defect states in ZnO. These defect states trap photogenerated electrons, adversely affecting the photocatalytic reaction. However, the S-scheme heterojunction effectively promotes the separation and transfer of electrons, mitigating this issue. The measured lifetimes of photogenerated electrons in these defect states, as determined by fitted fs-TA decay kinetics, provided further evidence of the carrier transfer mechanism in S-scheme heterojunctions. This work introduces a novel approach for studying organic/inorganic S-scheme heterojunctions using fs-TA spectroscopy.

Key words: Photocatalytic production of H2O2, S-scheme heterojunction, ZnO defect states, fs-TA spectroscopy