物理化学学报 >> 2025, Vol. 41 >> Issue (9): 100107.doi: 10.1016/j.actphy.2025.100107

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增强g-C3N4@BN范德华异质结界面上的三重态电子转移增强光催化合成H2O2

吴琦, 王长华*(), 李莹莹, 张昕彤*()   

  1. 东北师范大学, 中国教育部紫外发光材料与技术重点实验室, 吉林 长春 130024
  • 收稿日期:2025-03-31 修回日期:2025-05-25 录用日期:2025-05-25 发布日期:2025-07-04
  • 通讯作者: Email: wangch100@nenu.edu.cn (王长华)xtzhang@nenu.edu.cn (张昕彤)
  • 基金资助:
    吉林省科技发展计划项目(20220201073GX); 国家自然科学基金(52273236); 国家自然科学基金(U22A2078); 国家自然科学基金(91833303); 国家自然科学基金(51102001); 中央高校基本科研业务费专项资金(2412022QD035); 吉林省教育厅(JJKH20241426KJ)

Enhanced photocatalytic synthesis of H2O2 by triplet electron transfer at g-C3N4@BN van der Waals heterojunction interface

Qi Wu, Changhua Wang*(), Yingying Li, Xintong Zhang*()   

  1. Key Laboratory of UV-Emitting Materials and Technology of Chinese Ministry of Education, Northeast Normal University, Changchun 130024, Jilin Province, China
  • Received:2025-03-31 Revised:2025-05-25 Accepted:2025-05-25 Published:2025-07-04
  • Contact: Email: wangch100@nenu.edu.cn (Changhua Wang)xtzhang@nenu.edu.cn (Xintong Zhang)
  • Supported by:
    the Jilin Province Science and Technology Development Project(20220201073GX); the Natural Science Foundation of China(52273236); the Natural Science Foundation of China(U22A2078); the Natural Science Foundation of China(91833303); the Natural Science Foundation of China(51102001); the Fundamental Research Funds for the Central Universities(2412022QD035); the Education Department of Jilin Province(JJKH20241426KJ)

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摘要：

范德华异质结因其优异的电荷分离能力和在调节电子特性方面的显著灵活性而展现出卓越优势。本研究探讨了二维/二维(2D/2D) g-C3N4@BN范德华异质结在光催化合成过氧化氢(H2O2)中的潜在应用。基于该异质结，我们深入研究了三重态激子与单线态氧之间的能量转移过程，强调了催化剂结构对电荷分离和三重态电子稳定生成的重要性。通过构建电荷转移路径，异质结内的内置电场有效驱动了电荷载流子的定向迁移，显著延长了其寿命。我们采用了两种修饰策略来调控催化剂的激发态电子特性，包括调整层间排列以增强电荷传输能力，以及卤素修饰以提高材料的光响应性。实验验证表明，与CN相比，代表性的氯化-CN@BN有效抑制了激子复合，将激发态载流子的寿命延长了3.52倍。此外，H2O2的光催化产率提高了2.73倍。本研究为开发新型光催化剂提供了理论基础，并启发了从氧气直接合成H2O2的催化剂设计。

关键词: 2D/2D异质结界面, 光催化合成H2O2, 三重态电子转移, 能量转移

Abstract:

The van der Waals heterojunctions demonstrate exceptional advantages due to their outstanding charge separation capabilities and remarkable flexibility in tuning electronic properties. This study explores the potential application of the 2D/2D g-C3N4 @BN van der Waals heterojunction in the photocatalytic synthesis of hydrogen peroxide (H2O2). Based on this heterojunction, we investigated the energy transfer process between triplet excitons and singlet oxygen, emphasizing the importance of catalyst structure for charge separation and the stable generation of triplet electrons. By constructing a charge transfer pathway, the built-in electric field within the heterojunction effectively drives the directional migration of charge carriers, significantly extending their lifetime. We employed two modification strategies to regulate the excited state electronic properties of the catalyst, including adjusting the interlayer arrangement to enhance charge transport capability and halogen modification to improve the light responsiveness of materials. Experimental validation indicates that the representative chlorinated-CN@BN effectively suppresses exciton recombination compared to CN, extending the lifetime of excited-state carriers by 3.52 times. Furthermore, the photocatalytic yield of H2O2 is improved by 2.73 times. This study provides a theoretical basis for developing novel photocatalysts and inspires the design of catalysts for direct synthesis of H2O2 from oxygen.

Key words: 2D/2D heterojunction interface, Photocatalytic synthesis of H2O2, Triplet electron transfer, Energy transfer