物理化学学报 >> 2024, Vol. 40 >> Issue (10): 2311016.doi: 10.3866/PKU.WHXB202311016

所属专题: 太阳燃料光催化剂

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内建电场与偶极场协同增强SnNb2O6/富氮C3N5 S型异质结光催化性能

刘倩倩1,†,*(), 杜兴1,†, 李宛飞1,2, 戴维林3,*(), 刘波1,*()   

  1. 1 苏州科技大学材料科学与工程学院, 苏州市微纳光电材料与传感器重点实验室, 江苏 苏州 215009
    2 姑苏实验室, 江苏 苏州 215123
    3 复旦大学化学系, 上海市分子催化与创新材料重点实验室, 上海 200433
  • 收稿日期:2023-11-10 修回日期:2023-12-15 录用日期:2023-12-18 发布日期:2024-03-13
  • 通讯作者: Email: liuqianqian@usts.edu.cn. Tel.: +86-15995837516 (刘倩倩)wldai@fudan.edu.cn. Tel.: +86-512-68097107 (戴维林)liubo@mail.usts.edu.cn (戴维林)
  • 作者简介:

    †These authors contributed equally to this paper.

  • 基金资助:
    国家自然科学基金项目(22002102); 国家自然科学基金项目(61904118); 国家自然科学基金项目(62205231); 江苏省研究生科研与实践创新项目(SJCX22_1555); 江苏省环境功能材料重点实验室

Synergistic Effects of Internal Electric and Dipole Fields in SnNb2O6/Nitrogen-Enriched C3N5 S-Scheme Heterojunction for Boosting Photocatalytic Performance

Qianqian Liu1,*(), Xing Du1, Wanfei Li1,2, Wei-Lin Dai3,*(), Bo Liu1,*()   

  1. 1 Suzhou Key Laboratory for Nanophotonic and Nanoelectronic Materials and Its Devices, School of Materials Science and Engineering, Suzhou University of Science and Technology, Suzhou 215009, Jiangsu Province, China
    2 Gusu Lab Mat, Suzhou 215123, Jiangsu Province, China
    3 Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, Shanghai 200433, China
  • Received:2023-11-10 Revised:2023-12-15 Accepted:2023-12-18 Published:2024-03-13
  • Contact: Email: liuqianqian@usts.edu.cn. Tel.: +86-15995837516 (Qianqian Liu)wldai@fudan.edu.cn. Tel.: +86-512-68097107 (Wei-Lin Dai)liubo@mail.usts.edu.cn (Bo Liu)
  • Supported by:
    National Natural Science Foundation of China(22002102); National Natural Science Foundation of China(61904118); National Natural Science Foundation of China(62205231); Postgraduate Research & Practice Innovation Program of Jiangsu Province(SJCX22_1555); Jiangsu Key Laboratory for Environment Functional Materials

摘要:

定向电荷转移是调控光生载流子分离动力学的一种极具吸引力的策略。本文通过在SnNb2O6纳米片上原位生长C3N5纳米棒,设计一种具有强内建电场(IEF)和偶极场(DF)的新型2D/1D SnNb2O6/富氮C3N5 S型异质结。通过构筑S型异质结,在界面处产生IEF,促进电荷从SnNb2O6向C3N5的定向迁移。与此同时,C3N5中的DF提供一种驱动力,将光生电子定向转移至活性位点。通过IEF和DF的协同效应,SnNb2O6/C3N5异质结实现了快速的定向电子转移,从而显著提高了电荷分离效率。研究结果表明,SnNb2O6/C3N5异质结的最佳产氢速率高达1090.0 μmol∙g−1·h−1 (反应过程中持续释放H2气泡),分别是SnNb2O6和C3N5的38.8和10.7倍。此外,SnNb2O6/C3N5异质结在去除罗丹明B、四环素和Cr(Ⅵ)方面也表现出优异的光催化性能。通过电子顺磁共振(EPR)、时间分辨光致发光光谱(TPRL)和密度泛函理论(DFT)计算,本文系统探讨了SnNb2O6/C3N5异质结的定向电荷转移机制。这项研究为开发高效异质结光催化剂提供了一种可行的方法。

关键词: SnNb2O6/C3N5, 内建电场, 偶极场, 光催化性能, 定向电荷转移

Abstract:

Directional electron transfer is an appealing strategy for harnessing photogenerated charge separation kinetics. Herein, a novel 2D/1D SnNb2O6/nitrogen-enriched C3N5 S-scheme heterojunction with strong internal electric field (IEF) and dipole field (DF) is designed through in situ growth of C3N5 nanorods on SnNb2O6 nanosheets. The IEF generated at the interface via the formation of the S-scheme heterojunction induces directional charge transfer from SnNb2O6 to C3N5. Simultaneously, the DF within C3N5 provides the impetus to guide photo-excited electrons to the active sites. Consequently, the synergistic effects of IEF and DF facilitate swift directional electron transfer. The optimized SnNb2O6/C3N5 heterojunction demonstrates a remarkable H2 production rate of 1090.0 μmol∙g−1∙h−1 with continuous release of H2 bubbles. This performance surpasses that of SnNb2O6 and C3N5 by 38.8 and 10.7 times, respectively. Additionally, the SnNb2O6/C3N5 heterojunction exhibits superior activity in the removal of Rhodamine B, tetracycline, and Cr(Ⅵ). Based on electron paramagnetic resonance (EPR), time-resolved photoluminescence (TPRL) and density functional theory (DFT) calculations, etc., the directional charge transfer mechanism was systematically explored. The research furnishes a plausible approach to construct effective heterojunction photocatalysts for applications in energy and environmental domains.

Key words: SnNb2O6/C3N5, Internal electric field, Dipole field, Photocatalytic performance, Directional charge transfer