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

引用本文: 吴琦, 王长华, 李莹莹, 张昕彤. 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[J]. 物理化学学报, 2025, 41(9): 100107. doi: 10.1016/j.actphy.2025.100107 shu

Citation: Qi Wu, Changhua Wang, Yingying Li, Xintong Zhang. Enhanced photocatalytic synthesis of H₂O₂ by triplet electron transfer at g-C₃N₄@BN van der Waals heterojunction interface[J]. Acta Physico-Chimica Sinica, 2025, 41(9): 100107. doi: 10.1016/j.actphy.2025.100107 shu

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

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

通讯作者: 王长华, wangch100@nenu.edu.cn; 张昕彤, xtzhang@nenu.edu.cn

基金项目:
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

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:

English

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

Key Laboratory of UV-Emitting Materials and Technology of Chinese Ministry of Education, Northeast Normal University, Changchun 130024, Jilin Province, China

Corresponding author: Email: wangch100@nenu.edu.cn (C.W.); Email: xtzhang@nenu.edu.cn (X.Z.)

Received Date: 31 March 2025
Accepted Date: 25 May 2025
Revised Date: 25 May 2025
Available Online: 15 September 2025
Fund Project:
the Jilin Province Science and Technology Development Project

the Natural Science Foundation of China

the Natural Science Foundation of China

the Natural Science Foundation of China

the Natural Science Foundation of China

the Fundamental Research Funds for the Central Universities

the Education Department of Jilin Province

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:

1. [1]
  F. He, Y. Lu, Y. Wu, S. Wang, Y. Zhang, P. Dong, Y. Wang, C. Zhao, S. Wang, J. Zhang, Adv. Mater. 36 (2023), 2307490, https://doi.org/10.1002/adma.202307490. doi: 10.1002/adma.202307490
2. [2]
  G. Chen, Z. Zheng, W. Zhong, G. Wang, X. Wu, Acta Phys. -Chim. Sin. 40 (2024), 2406021, https://doi.org/10.3866/PKU.WHXB202406021. doi: 10.3866/PKU.WHXB202406021
3. [3]
  W. Liu, P. Wang, J. Chen, X. Gao, H. Che, B. Liu, Y. Ao, Adv. Funct. Mater. 32 (2022), 2205119, https://doi.org/10.1002/adfm.202205119. doi: 10.1002/adfm.202205119
4. [4]
  S. Qu, H. Wu, Y.H. Ng, Adv. Energy Mater. 13 (2023), 2301047, https://doi.org/10.1002/aenm.202301047. doi: 10.1002/aenm.202301047
5. [5]
  T.C. Khiem, N.N. Huy, E. Kwon, J. Lee, W.D. Oh, X. Duan, S. Wacławek, H. Wang, G. Lisak, F. Ghanbari, K. -Y.A. Lin, Appl. Catal., B 343 (2024), 123490, https://doi.org/10.1016/j.apcatb.2023.123490. doi: 10.1016/j.apcatb.2023.123490
6. [6]
  P. Dong, H. Lv, R. Luo, Z. Li, X. Wu, J. Lei, Chem. Eng. J. 461 (2023), 141817, https://doi.org/10.1016/j.cej.2023.141817. doi: 10.1016/j.cej.2023.141817
7. [7]
  W. Zhang, W. Huang, J. Jin, Y. Gan, S. Zhang, Appl. Catal., B 292 (2021), 120197, https://doi.org/10.1016/j.apcatb.2021.120197. doi: 10.1016/j.apcatb.2021.120197
8. [8]
  D. Li, K. Wang, J. Tang, Y. Zhao, H. Elhaes, M. Tahir, M.A. Ibrahim, Y. Li, Appl. Surf. Sci. 613 (2023), 155991, https://doi.org/10.1016/j.apsusc.2022.155991. doi: 10.1016/j.apsusc.2022.155991
9. [9]
  A.K. Pal, A. Datta, J. Chem. Phys. 160 (2024), 164720, https://doi.org/10.1063/5.0196557. doi: 10.1063/5.0196557
10. [10]
  S. Jin, W. Shao, X. Luo, H. Wang, X. Sun, X. He, X. Zhang, Y. Xie, Adv. Mater. 34 (2022), 2206516, https://doi.org/10.1002/adma.202206516. doi: 10.1002/adma.202206516
11. [11]
  G. Li, T. Qiu, Q. Wu, Z. Zhao, L. Wang, Y. Li, Y. Geng, H. Tan, Angew. Chem. Int. Ed. 63 (2024), e202405396, https://doi.org/10.1002/anie.202405396. doi: 10.1002/anie.202405396
12. [12]
  Y. Shen, Y. Yao, C. Zhu, J. Wu, L. Chen, Q. Fang, S. Song, Chem. Eng. J. 475 (2023), 146383, https://doi.org/10.1016/j.cej.2023.146383. doi: 10.1016/j.cej.2023.146383
13. [13]
  X. Zeng, T. Wang, Z. Wang, M. Tebyetekerwa, Y. Liu, Z. Liu, G. Wang, A.A. Wibowo, G. Pierens, Q. Gu, X. Zhang, ACS Catal. 14 (2024), 9955, https://doi.org/10.1021/acscatal.4c01591. doi: 10.1021/acscatal.4c01591
14. [14]
  J. Cheng, S. Wan, S. Cao, Angew. Chem. Int. Ed. 62 (2023), e202310476, https://doi.org/10.1002/anie.202310476. doi: 10.1002/anie.202310476
15. [15]
  S. Pullen, Chem Catal. 3 (2023), 100861, https://doi.org/10.1016/j.checat.2023.100861. doi: 10.1016/j.checat.2023.100861
16. [16]
  M. Schmitz, M. -S. Bertrams, A.C. Sell, F. Glaser, C. Kerzig, J. Am. Chem. Soc. 146 (2024), 25799, https://doi.org/10.1021/jacs.4c08551. doi: 10.1021/jacs.4c08551
17. [17]
  H. Yersin, R. Czerwieniec, U. Monkowius, R. Ramazanov, R. Valiev, M.Z. Shafikov, W. -M. Kwok, C. Ma, Coord. Chem. Rev. 478 (2023), 214975, https://doi.org/10.1016/j.ccr.2022.214975. doi: 10.1016/j.ccr.2022.214975
18. [18]
  J.A. Kübler, B. Pfund, O.S. Wenger, JACS Au 2 (2022), 2367, https://doi.org/10.1021/jacsau.2c00442. doi: 10.1021/jacsau.2c00442
19. [19]
  T. Jin, S. He, Y. Zhu, E. Egap, T. Lian, Nano Lett. 22 (2022), 3897, https://doi.org/10.1021/acs.nanolett.2c00017. doi: 10.1021/acs.nanolett.2c00017
20. [20]
  Y. Zhao, X. Yu, T. Bao, Y. Guo, Y. Su, J. Zhao, Nano Lett. 24 (2024), 13534, https://doi.org/10.1021/acs.nanolett.4c02986. doi: 10.1021/acs.nanolett.4c02986
21. [21]
  P. Li, Y. Cui, Z. Wang, G. Dawson, C. Shao, K. Dai, Acta Phys. -Chim. Sin. 41 (2025), 100065, https://doi.org/10.1016/j.actphy.2025.100065. doi: 10.1016/j.actphy.2025.100065
22. [22]
  Y. Liu, C. Chen, G. Dawson, J. Zhang, C. Shao, K. Dai, J. Mater. Sci. Technol. 233 (2025), 10, https://doi.org/10.1016/j.jmst.2024.12.094. doi: 10.1016/j.jmst.2024.12.094
23. [23]
  Z. Wang, S. Hu, F. Deng, H. Shi, X. Li, S. Zhang, J. Zou, X. Luo, Sep. Purif. Technol. 330 (2024), 125287, https://doi.org/10.1016/j.seppur.2023.125287. doi: 10.1016/j.seppur.2023.125287
24. [24]
  Z. Wang, B. Cheng, L. Zhang, J. Yu, Y. Li, S. Wageh, A.A. Al-Ghamdi, Chin. J. Catal. 43 (2022), 1657, https://doi.org/10.1016/S1872-2067(21)64010-X. doi: 10.1016/S1872-2067(21)64010-X
25. [25]
  H. Zhang, C. Shao, Z. Wang, J. Zhang, K. Dai, J. Mater. Sci. Technol. 195 (2024), 146, https://doi.org/10.1016/j.jmst.2023.11.081. doi: 10.1016/j.jmst.2023.11.081
26. [26]
  Y. Cui, J. Zhang, H. Chu, L. Sun, K. Dai, Acta Phys. -Chim. Sin. 40 (2024), 2405016, https://doi.org/10.3866/PKU.WHXB202405016. doi: 10.3866/PKU.WHXB202405016
27. [27]
  K. Dong, C. Shen, R. Yan, Y. Liu, C. Zhuang, S. Li, Acta Phys. -Chim. Sin. 40 (2024), 2310013, https://doi.org/10.3866/PKU.WHXB202310013. doi: 10.3866/PKU.WHXB202310013
28. [28]
  Z. Fang, J. Qi, Y. Xu, Y. Liu, T. Qi, L. Xing, Q. Dai, L. Wang, Chem. Eng. J. 441 (2022), 136051, https://doi.org/10.1016/j.cej.2022.136051. doi: 10.1016/j.cej.2022.136051
29. [29]
  A. Savateev, N.V. Tarakina, V. Strauss, T. Hussain, K. ten Brummelhuis, J.M. Sánchez Vadillo, Y. Markushyna, S. Mazzanti, A.P. Tyutyunnik, R. Walczak, M. Oschatz, D.M. Guldi, A. Karton, M. Antonietti, Angew. Chem. Int. Ed. 59 (2020), 15061, https://doi.org/10.1002/anie.202004747. doi: 10.1002/anie.202004747
30. [30]
  S. Liang, Q. Wu, C. Wang, R. Wang, D. Li, Y. Xing, D. Jin, H. Ma, Y. Liu, P. Zhang, X. Zhang, Proc. Natl. Acad. Sci 121 (2024), e2410504121, https://doi.org/10.1073/pnas.2410504121. doi: 10.1073/pnas.2410504121
31. [31]
  Y. Luo, H. Zheng, X. Li, F. Li, H. Tang, X. She, Acta Phys. -Chim. Sin. 41 (2025), 100052, https://doi.org/10.1016/j.actphy.2025.100052. doi: 10.1016/j.actphy.2025.100052
32. [32]
  C. You, C. Wang, M. Cai, Y. Liu, B. Zhu, S. Li, Acta Phys. -Chim. Sin. 40 (2024), 2407014, https://doi.org/10.3866/PKU.WHXB202407014. doi: 10.3866/PKU.WHXB202407014
33. [33]
  M. Cai, Y. Liu, K. Dong, X. Chen, S. Li, Chin. J. Catal. 52 (2023), 239, https://doi.org/10.1016/S1872-2067(23)64496-1. doi: 10.1016/S1872-2067(23)64496-1
34. [34]
  J. Zhang, G. Yu, C. Yang, S. Li, Curr. Opin. Chem. Eng. 45 (2024), 101040, https://doi.org/10.1016/j.coche.2024.101040. doi: 10.1016/j.coche.2024.101040
35. [35]
  K. Li, C. Liu, J. Li, G. Wang, K. Wang, Acta Phys. -Chim. Sin. 40 (2024), 2403009, https://doi.org/10.3866/PKU.WHXB202403009. doi: 10.3866/PKU.WHXB202403009
36. [36]
  W. Zhong, D. Zheng, Y. Ou, A. Meng, Y. Su, Acta Phys. -Chim. Sin. 40 (2024), 2406005, https://doi.org/10.3866/PKU.WHXB202406005. doi: 10.3866/PKU.WHXB202406005
37. [37]
  Z. Xiu, W. Mu, X. Zhou, X. Han, Chin. J. Catal. 65 (2024), 126, https://doi.org/10.1016/S1872-2067(24)60114-2. doi: 10.1016/S1872-2067(24)60114-2
38. [38]
  L. Zhang, J. Zhang, J. Yu, H. García, Nat. Rev. Chem. 9 (2025), 328, https://doi.org/10.1038/s41570-025-00698-3. doi: 10.1038/s41570-025-00698-3
39. [39]
  L. Acharya, S.P. Pattnaik, A. Behera, R. Acharya, K. Parida, Inorg. Chem. 60 (2021), 5021, https://doi.org/10.1021/acs.inorgchem.1c00062. doi: 10.1021/acs.inorgchem.1c00062
40. [40]
  H. Sohrabi, O. Arbabzadeh, M. Falaki, V. Vatanpour, M.R. Majidi, N. Kudaibergenov, S.W. Joo, A. Khataee, Surf. Interfaces 41 (2023), 103152, https://doi.org/10.1016/j.surfin.2023.103152. doi: 10.1016/j.surfin.2023.103152
41. [41]
  C. Chen, J. Zhang, H. Chu, L. Sun, G. Dawson, K. Dai, Chin. J. Catal. 63 (2024), 81, https://doi.org/10.1016/S1872-2067(24)60072-0. doi: 10.1016/S1872-2067(24)60072-0
42. [42]
  T. Yang, J. Wang, Z. Wang, J. Zhang, K. Dai, Chin. J. Catal. 58 (2024), 157, https://doi.org/10.1016/S1872-2067(23)64607-8. doi: 10.1016/S1872-2067(23)64607-8
43. [43]
  L. Jiang, X. Yuan, G. Zeng, Z. Wu, J. Liang, X. Chen, L. Leng, H. Wang, H. Wang, Appl. Catal., B. 221 (2018), 715, https://doi.org/10.1016/j.apcatb.2017.09.059. doi: 10.1016/j.apcatb.2017.09.059
44. [44]
  Q. Wu, Y. Lin, Y. Ou, C. Wang, H. Ma, R. Wang, Y. Li, X. Zhang, J. Mater. Chem. A 12 (2024), 14302, https://doi.org/10.1039/D4TA02059F. doi: 10.1039/D4TA02059F
45. [45]
  H. He, Z. Wang, J. Zhang, C. Shao, K. Dai, K. Fan, Adv. Funct. Mater. 34 (2024), 2315426, https://doi.org/10.1002/adfm.202315426. doi: 10.1002/adfm.202315426
46. [46]
  M.J. Frisch, G.W. Trucks, H.B. Schlegel, G.E. Scuseria, M.A. Robb, J.R. Cheeseman, G. Scalmani, V. Barone, G.A. Petersson, H. Nakatsuji, et al. Gaussian 16 Rev. B. 01[Z]. Wallingford, CT. 2016
47. [47]
  Z. Liu, X. Wang, T. Lu, A. Yuan, X. Yan, Carbon 187 (2022), 78, https://doi.org/10.1016/j.carbon.2021.11.005. doi: 10.1016/j.carbon.2021.11.005
48. [48]
  T. Lu, F. Chen, J. Comput. Chem. 33 (2012), 580, https://doi.org/10.1002/jcc.22885. doi: 10.1002/jcc.22885
49. [49]
  F. Neese, WIREs Comput. Mol. Sci. 2 (2012), 73, https://doi.org/10.1002/wcms.81. doi: 10.1002/wcms.81
50. [50]
  T. Lu, Q. Chen, J. Comput. Chem. 43 (2022), 539, https://doi.org/10.1002/jcc.26812. doi: 10.1002/jcc.26812
51. [51]
  R.A. Marcus, N. Sutin, Biochim. Biophys. Acta 811 (1985), 265. doi: 10.1016/0304-4173(85)90014-X
52. [52]
  A.A. Peterson, F. Abild-Pedersen, F. Studt, J. Rossmeisl, J.K. Nrskov, Energy Environ. Sci. 3 (2010), 1311, https://doi.org/10.1039/C0EE00071J. doi: 10.1039/c0ee00071j
53. [53]
  X. Wang, B. Liu, S. Ma, Y. Zhang, L. Wang, G. Zhu, W. Huang, S. Wang, Nat. Commun. 15 (2024), 2600, https://doi.org/10.1038/s41467-024-47022-z. doi: 10.1038/s41467-024-47022-z
54. [54]
  S. Guo, Y. Park, E. Park, S. Jin, L. Chen, Y.M. Jung, Angew. Chem., Int. Ed. 62 (2023), e202306709, https://doi.org/10.1002/anie.202306709. doi: 10.1002/anie.202306709
55. [55]
  C.A. Ullrich, Z.-H. Yang, Braz. J. Phys. 44 (2014), 154, https://doi.org/10.1007/s13538-013-0141-2. doi: 10.1007/s13538-013-0141-2
56. [56]
  Z. Liu, T. Lu, Q. Chen, Carbon 165 (2020), 461, https://doi.org/10.1016/j.carbon.2020.05.023. doi: 10.1016/j.carbon.2020.05.023
57. [57]
  C.A. Guido, P. Cortona, B. Mennucci, C. Adamo, J. Chem. Theory Comput. 9 (2013), 3118, https://doi.org/10.1021/ct400337e. doi: 10.1021/ct400337e
58. [58]
  R.A. House, G.J. Rees, K. McColl, J.-J. Marie, M. Garcia-Fernandez, A. Nag, K.-J. Zhou, S. Cassidy, B.J. Morgan, M. Saiful Islam, P.G. Bruce, Nat. Energy 8 (2023), 351, https://doi.org/10.1038/s41560-023-01211-0. doi: 10.1038/s41560-023-01211-0
59. [59]
  C. Duan, J. Li, C. Han, D. Ding, H. Yang, Y. Wei, H. Xu, Chem. Mater. 28 (2016), 5667, https://doi.org/10.1021/acs.chemmater.6b01691. doi: 10.1021/acs.chemmater.6b01691
60. [60]
  T.J. Penfold, J. Phys. Chem. C 119 (2015), 13535, https://doi.org/10.1021/acs.jpcc.5b03530. doi: 10.1021/acs.jpcc.5b03530
61. [61]
  Y. Yang, X. Zhou, M. Gu, B. Cheng, Z. Wu, J. Zhang, Acta Phys. -Chim. Sin. 41 (2025), 100064, https://doi.org/10.1016/j.actphy.2025.100064. doi: 10.1016/j.actphy.2025.100064
62. [62]
  J. Yan, J. Zhang, J. Mater. Sci. Technol. 193 (2024), 18, https://doi.org/10.1016/j.jmst.2023.12.054. doi: 10.1016/j.jmst.2023.12.054

扫一扫看文章

计量

PDF下载量: 0
文章访问数: 9
HTML全文浏览量: 2

通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142

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

通讯作者: 王长华, wangch100@nenu.edu.cn; 张昕彤, xtzhang@nenu.edu.cn

English

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

Corresponding author: Email: wangch100@nenu.edu.cn (C.W.); Email: xtzhang@nenu.edu.cn (X.Z.)

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

计量

通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处