物理化学学报 >> 2025, Vol. 41 >> Issue (8): 100095.doi: 10.1016/j.actphy.2025.100095

所属专题： 光催化中的S型异质结

论文 上一篇    

优化氮化碳纳米片/球形共轭聚合物S型异质结界面电场以促进析氢反应

孟凡鹏1,†, 赵飞2,†, 林靖恺3, 赵金生1,*(), 张华阳3,*(), 王少彬3   

  1. 1 山东省化学储能与新型电池技术重点实验室, 聊城大学化学化工学院, 山东 聊城 252059
    2 泰山学院化学化工学院, 山东 泰安 271000
    3 School of Chemical Engineering, The University of Adelaide, Adelaide SA 5005, Australia
  • 收稿日期:2025-03-18 修回日期:2025-04-02 录用日期:2025-04-15 发布日期:2025-06-07
  • 通讯作者: Email: j.s.zhao@163.com (赵金生)huayang.zhang@adelaide.edu.au (张华阳)
  • 作者简介:

    †The authors contributed equally to the work.

  • 基金资助:
    国家自然科学基金(22302085); 国家自然科学基金(22172069); 山东省自然科学基金(ZR2024QB046); 山东省自然科学基金(ZR2021ME071); 聊城大学科研项目(318052272); 张华阳与王少彬获澳大利亚研究委员会发现项目(DP230102406); 张华阳与王少彬获澳大利亚研究委员会发现项目(DP240102787); 桂冠学者计划(FL230100178)

Optimizing interfacial electric fields in carbon nitride nanosheet/spherical conjugated polymer S-scheme heterojunction for hydrogen evolution

Fanpeng Meng1, Fei Zhao2, Jingkai Lin3, Jinsheng Zhao1,*(), Huayang Zhang3,*(), Shaobin Wang3   

  1. 1 Shandong Key Laboratory of Chemical Energy Storage and Novel Cell Technology, College of Chemistry and Chemical Engineering, Liaocheng University, Liaocheng 252059, Shandong Province, China
    2 College of Chemistry and Chemical Engineering, Taishan University, Taian 271000, Shandong Province, China
    3 School of Chemical Engineering, The University of Adelaide, Adelaide SA 5005, Australia
  • Received:2025-03-18 Revised:2025-04-02 Accepted:2025-04-15 Published:2025-06-07
  • Contact: Email: j.s.zhao@163.com (Jinsheng Zhao)huayang.zhang@adelaide.edu.au (Huayang Zhang)
  • Supported by:
    the National Natural Science Foundation of China(22302085); the National Natural Science Foundation of China(22172069); the Natural Science Foundation of Shandong Province(ZR2024QB046); the Natural Science Foundation of Shandong Province(ZR2021ME071); the Research Projects of Liaocheng University(318052272); H. Zhang and S. Wang acknowledges the support from Discovery Project(DP230102406); H. Zhang and S. Wang acknowledges the support from Discovery Project(DP240102787); Australian Laureate Fellowships from the Australian Research Council(FL230100178)

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摘要：

基于氮化碳设计异质结是提升光催化效率的有效途径。本研究通过简便高效的球磨技术，构建了由氮化碳纳米片(GCNNS)与供体-受体共轭聚合物(聚对氨基亚苄基异苯胺，PASO)组成的全有机S型无金属异质结。该异质结展现出优异的光催化产氢性能，优化后的GCNNS/PASO-10样品的产氢速率达到10.12 mmol·g−1·h−1，分别是GCNNS和PASO的5.9倍和19.5倍。这种提升源于独特的界面结合作用、增强的可见光吸收能力以及S型异质结强内建电场促进的高效电荷分离。理论计算与表征结果表明，该异质结的S型机制实现了能带最优匹配并推动了空间电荷的有效分离，从而显著提升了光催化活性。本工作揭示了全有机材料在异质结构建中的独特优势，为设计先进S型体系以实现可持续能源转化提供了新思路。

关键词: 全有机异质结, 氮化碳纳米片, S型异质结, 产氢, D-A共轭聚合物

Abstract:

Designing heterojunctions based on carbon nitride offers a promising pathway for enhancing photocatalytic efficiency. This study develops an all-organic S-scheme metal-free heterojunction uniquely composed of carbon nitride nanosheets (GCNNS) and a donor-acceptor conjugated polymer, poly p-aminobenzylidene-so-aniline (PASO), synthesized through a simple yet effective ball-milling technique. This heterojunction demonstrates excellent photocatalytic efficiency for hydrogen (H2) evolution. The optimized GCNNS/PASO-10 sample attains an H2 evolution rate of 10.12 mmol·g−1·h−1, which is about 5.9 times and 19.5 times greater than those of pure GCNNS and PASO, respectively. This improvement is due to the unique interfacial bonding, increased visible-light absorption, and efficient charge carrier separation facilitated by a strong internal electric field within the S-scheme. Theoretical calculations and characterization reveal that this heterojunction's S-scheme mechanism optimally aligns energy bands and promotes spatial charge separation, driving superior photocatalytic activity. This work presents the unique advantage of all-organic materials for heterojunction construction and provides insights into designing advanced S-scheme systems for sustainable energy conversion.

Key words: All-organic heterojunction, Carbon nitride nanosheets, S-scheme heterojunction, H2 evolution, D-A conjugated polymers