通过间接两电子还原的HOF/BiVO4 (010) S型光催化剂增强H2O2生产性能

引用本文: 周玲, 李龙, 黄礼文, 吴艳. 通过间接两电子还原的HOF/BiVO₄ (010) S型光催化剂增强H₂O₂生产性能[J]. 物理化学学报, 2026, 42(3): 100172. doi: 10.1016/j.actphy.2025.100172 shu

Citation: Ling Zhou, Long Li, Liwen Huang, Yan Wu. Enhanced H₂O₂ production performance via indirect two-electron reduction of HOF/BiVO₄ (010) S-scheme photocatalyst[J]. Acta Physico-Chimica Sinica, 2026, 42(3): 100172. doi: 10.1016/j.actphy.2025.100172 shu

通过间接两电子还原的HOF/BiVO₄ (010) S型光催化剂增强H₂O₂生产性能

周玲 ^{1, †,} ,
李龙 ^{1, †,} ,
黄礼文 ^{2,
,} ,
吴艳 ^{1,
,}

1.
中国地质大学(武汉), 材料与化学学院, 湖北武汉 430078
2.
湖北工程学院, 化学与材料科学学院, 湖北孝感 432000

通讯作者: hlw@hbeu.edu.cn (黄礼文); Email: wuyan@cug.edu.cn (吴艳)

摘要: 太阳能驱动的氧还原制取H₂O₂为传统工业蒽醌法和直接H₂/O₂合成法提供了一种绿色、高效且环境友好的替代方案。本研究通过定向晶面工程，将氢键有机框架(HOF)选择性锚定在BiVO₄的(010)晶面上，构建了以HOF为还原端、通过氧还原反应生成H₂O₂的S型异质结。该结构使H₂O₂产率显著提升至555 μmol g⁻¹ h⁻¹，较随机锚定的HOF/BiVO₄体系提高约37%。原位开尔文探针力显微镜(KPFM)揭示了原始BiVO₄的(110)与(010)晶面间存在内建电场，且(010)晶面在光照下富集电子。对HOF定向锚定于BiVO₄ (010)晶面的材料研究表明，两组分间还建立了额外的内建电场。由此，我们提出了一种在异质结中具有双内建电场的新型HOF/BiVO₄ (010)光催化材料，这种结构显著促进了单晶BiVO₄不同晶面与S型异质结界面的双向定向电荷转移。原位X射线光电子(XPS)进一步证实了S型异质结的电子转移机制。通过引入电子清除剂与空穴捕获剂，我们证实该异质结介导的光催化过程遵循两电子氧还原反应(ORR)路径。电子顺磁共振(EPR)光谱检测到超氧自由基(∙O₂⁻)的存在，表明ORR通过间接两电子转移机制进行。双内建电场、S型异质结结构与两电子ORR路径的协同效应共同促成了该体系优异的光催化性能。

关键词:

English

Enhanced H₂O₂ production performance via indirect two-electron reduction of HOF/BiVO₄ (010) S-scheme photocatalyst

Ling Zhou ^{1, †,} ,
Long Li ^{1, †,} ,
Liwen Huang ^{2,
,} ,
Yan Wu ^{1,
,}

1.
Faculty of Materials Science and Chemistry, China University of Geosciences (Wuhan), Wuhan 430078, Hubei Province, China
2.
College of Chemistry and Materials Science, Hubei Engineering University, Xiaogan 432000, Hubei Province, China

Corresponding author: hlw@hbeu.edu.cn (Liwen Huang); Email: wuyan@cug.edu.cn (Yan Wu)

Received Date: 15 July 2025
Accepted Date: 24 August 2025
Revised Date: 20 August 2025
Available Online: 15 March 2026
^† Equally contributed to this work.

Abstract: Solar-driven oxygen reduction for H₂O₂ production offers a green, efficient, and environmentally friendly alternative to the conventional industrial anthraquinone process and direct H₂/O₂ synthesis. In this study, through targeted crystal facet engineering, a hydrogen-bonded organic framework (HOF) was selectively anchored onto the (010) facet of BiVO₄, forming an S-scheme heterojunction where the HOF is the reducing side and oxygen reduction occurs to produce H₂O₂. This configuration significantly enhanced the H₂O₂ yield to 555 μmol g⁻¹ h⁻¹, representing a ~37% improvement compared to randomly contacted HOF/BiVO₄ systems. In situ Kelvin probe force microscopy (KPFM) revealed the formation of an intrinsic electric field between the (110) and (010) facets of pristine BiVO₄, with the (010) facet becoming electron-rich under illumination. Further investigation of the HOF/BiVO₄ (010) material, where HOF is directionally anchored to the (010) facet of BiVO₄, demonstrated the establishment of an additional built-in electric field between the two components. Thus, we propose a novel HOF/BiVO₄ (010) photocatalytic material featuring dual built-in electric fields in the heterojunctions, which significantly promote the dual directed charge transfer in the different facets of single crystal BiVO₄ and the interface of the S-scheme heterojunction. In situ X-ray Photoelectron Spectroscopy (XPS) further confirmed the S-scheme heterojunction electron transfer mechanism. By introducing electron scavengers and hole trappers, we conclusively verified that the heterojunction-mediated photocatalytic process follows a two-electron Oxygen Reduction Reaction (ORR) pathway. Electron Paramagnetic Resonance (EPR) spectroscopy detected the presence of superoxide radicals (∙O₂⁻), indicating that the ORR proceeds via an indirect two-electron transfer mechanism. The synergistic effects of the dual built-in electric fields, S-scheme heterojunction structure, and two-electron ORR pathway collectively contribute to the superior photocatalytic performance of this system.

Key words:

1. [1]
  J. Qiu, D. Dai, J. Yao, Coord Chem. Rev. 501 (2024) 215597, https://doi.org/10.1016/j.ccr.2023.215597. doi: 10.1016/j.ccr.2023.215597
2. [2]
  J. Ji, Z. Wang, Q. Xu, Q. Zhu, M. Xing, Chem. Eur. J. 29 (2023) e202203921.https://doi.org/10.1002/chem.202203921. doi: 10.1002/chem.202203921
3. [3]
  B. Liu, J. Zhang, H. Li, B. Cheng, C. Bie, Acta Phys. Chim. Sin. 41 (2025) 100084, https://doi.org/10.1016/j.actphy.2025.100084. doi: 10.1016/j.actphy.2025.100084
4. [4]
  H. Li, W. Wang, K. Xu, B. Cheng, J. Xu, S. Cao, Chin. J. Catal. 72 (2025) 24, https://doi.org/10.1016/S1872-2067(24)60257-3. doi: 10.1016/S1872-2067(24)60257-3
5. [5]
  X. Ruan, M. Xu, C. Ding, J. Leng, G. Fang, D. Meng, W. Zhang, Z. Jiang, S. Ravi, X. Cui, et al., Adv. Energy Mater. 15 (2025) 2405478, https://doi.org/10.1002/aenm.202405478. doi: 10.1002/aenm.202405478
6. [6]
  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
7. [7]
  M. Sayed, K. Qi, X. Wu, L. Zhang, H. García, J. Yu, Chem. Soc. Rev. 54 (2025) 4874, https://doi.org/10.1039/D4CS01091D. doi: 10.1039/D4CS01091D
8. [8]
  J. Li, N. Xu, Y. Zhang, H. Dong, C. Li, Chin. Chem. Lett. (2024) 110470, https://doi.org/10.1016/j.cclet.2024.110470. doi: 10.1016/j.cclet.2024.110470
9. [9]
  X. Cheng, L. Liang, J. Ye, N. Li, B. Yan, G. Chen, Sci. Total Environ. 888 (2023) 164086, https://doi.org/10.1016/j.scitotenv.2023.164086. doi: 10.1016/j.scitotenv.2023.164086
10. [10]
  B. Xia, G. Liu, K. Fan, R. Chen, X. Liu, L. Li, Chin. J. Catal. 69 (2025) 315, https://doi.org/10.1016/S1872-2067(24)60210-X. doi: 10.1016/S1872-2067(24)60210-X
11. [11]
  Z. Jiang, J. Zhang, B. Cheng, Y. Zhang, J. Yu, L. Zhang, Small 21 (2025) 2409079, https://doi.org/10.1002/smll.202409079. doi: 10.1002/smll.202409079
12. [12]
  Y. Wu, C. Cheng, K. Qi, B. Cheng, J. Zhang, J. Yu, L. Zhang, Acta Phys. Chim. Sin. 40 (2024) 2406027, https://doi.org/10.3866/PKU.WHXB202406027. doi: 10.3866/PKU.WHXB202406027
13. [13]
  Y. Zhao, C. Yang, S. Zhang, G. Sun, B. Zhu, L. Wang, J. Zhang, Chin. J. Catal. 63 (2024) 258, https://doi.org/10.1016/S1872-2067(24)60069-0. doi: 10.1016/S1872-2067(24)60069-0
14. [14]
  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
15. [15]
  G. Liu, R. Chen, B. Xia, Z. Wu, S. Liu, A. Talebian-Kiakalaieh, J. Ran, Chin. J. Catal. 61 (2024) 97, https://doi.org/10.1016/S1872-2067(24)60014-8. doi: 10.1016/S1872-2067(24)60014-8
16. [16]
  Z. Lu, R. Chen, G. Liu, B. Xia, K. Fan, T. Liu, Y. Xia, S. Liu, B. You, Adv. Funct. Mater. (2025) 2500944, https://doi.org/10.1002/adfm.202500944. doi: 10.1002/adfm.202500944
17. [17]
  B. Xia, G. Liu, K. Fan, R. Chen, X. Liu, L. Li, Chin. J. Catal. 69 (2025) 315, https://doi.org/10.1016/S1872-2067(24)60210-X. doi: 10.1016/S1872-2067(24)60210-X
18. [18]
  Z. Xie, H. Tan, H. Wu, R. Amal, J. Scott, Y. Ng, Mater. Today Energy 26 (2022) 100986, https://doi.org/10.1016/j.mtener.2022.100986. doi: 10.1016/j.mtener.2022.100986
19. [19]
  G. Wang, H. Cheng, Sep. Purif. Technol. 318 (2023) 123949, https://doi.org/10.1016/j.seppur.2023.123949. doi: 10.1016/j.seppur.2023.123949
20. [20]
  Y. Zhao, Q. Jia, Z. Tian, Y. Wang, J. Li, S. Song, T. Fu, X. Cui, G. Liu, X. Zhou, L. Jiang, J. Energy Chem. 103 (2025) 877, https://doi.org/10.1016/j.jechem.2024.12.003. doi: 10.1016/j.jechem.2024.12.003
21. [21]
  D. Seo, V. Somjit, D.H. Wi, G. Galli, K. Choi, J. Am. Chem. Soc. 147 (2025) 3261, https://doi.org/10.1021/jacs.4c13290. doi: 10.1021/jacs.4c13290
22. [22]
  K. Wang, M. Wang, J. Yu, D. Liao, H. Shi, X. Wang, H. Yu, ACS Appl. Nano Mater. 4 (2021) 13158, https://doi.org/10.1021/acsanm.1c02688. doi: 10.1021/acsanm.1c02688
23. [23]
  X. Wang, D. Liao, H. Yu, J. Yu, Dalton Trans. 47 (2018) 6370, https://doi.org/10.1039/C8DT00780B. doi: 10.1039/C8DT00780B
24. [24]
  X. Liu, G. Liu, T. Fu, K. Ding, J. Guo, Z. Wang, W. Xia, H. Shangguan, Adv. Sci. 11 (2024) 2400101, https://doi.org/10.1002/advs.202400101. doi: 10.1002/advs.202400101
25. [25]
  Y. Yao, Q. Wu, S. Ren, Y. Zhao, L. Guan, Adv. Opt. Mater. 13 (2025) 2402260, https://doi.org/10.1002/adom.202402260. doi: 10.1002/adom.202402260
26. [26]
  X. Li, Z. Su, H. Jiang, J. Liu, L. Zheng, H. Zheng, S. Wu, X. Shi, Small 20 (2024) 2400617, https://doi.org/10.1002/smll.202400617. doi: 10.1002/smll.202400617
27. [27]
  Y. Lin, X. Jiang, S.T. Kim, S. Alahakoon, X. Hou, Z. Zhang, C. Thompson, R.A. Smaldone, C. Ke, J. Am. Chem. Soc. 139 (2017) 7172, https://doi.org/10.1021/jacs.7b03204. doi: 10.1021/jacs.7b03204
28. [28]
  C. Ban, Y. Wang, Y. Feng, Z. Zhu, Y. Duan, J. Ma, X. Zhang, X. Liu, K. Zhou, H. Zou, D. Yu, X. Tao, L. Gan, G. Han, X. Zhou, Energy Environ. Sci. 17 (2024) 518, https://doi.org/10.1039/D3EE02800C. doi: 10.1039/D3EE02800C
29. [29]
  Q. Zhang, G. Liu, T. Liu, ACS Sustain. Chem. Eng. 12 (2024) 5675, https://doi.org/10.1021/acssuschemeng.4c00637. doi: 10.1021/acssuschemeng.4c00637
30. [30]
  Q. Zhou, Y. Guo, Y. Zhu, Nat. Catal. 6 (2023) 574, https://doi.org/10.1038/s41929-023-00972-x. doi: 10.1038/s41929-023-00972-x
31. [31]
  J. Wang, J. Bai, Y. Zhang, L. Li, C. Zhou, T. Zhou, J. Li, H. Zhu, B. Zhou, ACS Appl. Mater. Interfaces 15 (2023) 14359, https://doi.org/10.1021/acsami.2c23169. doi: 10.1021/acsami.2c23169
32. [32]
  X. Luo, S. Yang, Z. Wang, Y. Xu, Sep. Purif. Technol. 318 (2023) 123966, https://doi.org/10.1016/j.seppur.2023.123966. doi: 10.1016/j.seppur.2023.123966
33. [33]
  N. Zhang, Q. Yin, S. Guo, K. Chen, T. Liu, P. Wang, Z. Zhang, T. Lu, Appl. Catal. B Environ. 296 (2021) 120337, https://doi.org/10.1016/j.apcatb.2021.120337. doi: 10.1016/j.apcatb.2021.120337
34. [34]
  H. Shi, Y. Li, X. Wang, H. Yu, J. Yu, Appl. Catal. B Environ. 297 (2021) 120414, https://doi.org/10.1016/j.apcatb.2021.120414. doi: 10.1016/j.apcatb.2021.120414
35. [35]
  H. Shi, Y. Li, K. Wang, S. Li, X. Wang, P. Wang, F. Chen, H. Yu, Chem. Eng. J. 443 (2022) 136429, https://doi.org/10.1016/j.cej.2022.136429. doi: 10.1016/j.cej.2022.136429
36. [36]
  X. Zhang, D. Gao, B. Zhu, B. Cheng, J. Yu, H. Yu, Nat. Commun. 15 (2024) 3212, https://doi.org/10.1038/s41467-024-47624-7. doi: 10.1038/s41467-024-47624-7
37. [37]
  W. Wang, Z. Chen, C. Li, B. Cheng, K. Yang, S. Zhang, G. Luo, J. Yu, S. Cao, Adv. Funct. Mater. (2025) 2422307.https://doi.org/10.1002/adfm.202422307. doi: 10.1002/adfm.202422307
38. [38]
  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
39. [39]
  W. Zhong, A. Meng, Y. Su, H. Yu, P. Han, J. Yu, Angew. Chem. Int. Ed. 64 (2025) e202425038, https://doi.org/10.1002/anie.202425038. doi: 10.1002/anie.202425038
40. [40]
  H. Tan, C. Chai, J. Heng, Q.V. Thi, X. Wu, Y.H. Ng, E. Ye, Adv. Sci. 12 (2025) 2407801, https://doi.org/10.1002/advs.202407801. doi: 10.1002/advs.202407801
41. [41]
  L. Jian, Y. Dong, H. Zhao, C. Pan, G. Wang, Y. Zhu, Appl. Catal. B Environ. 342 (2024) 123340, https://doi.org/10.1016/j.apcatb.2023.123340. doi: 10.1016/j.apcatb.2023.123340
42. [42]
  L. Ding, Z. Pan, Q. Wang, Chin. Chem. Lett. 35 (2024) 110125, https://doi.org/10.1016/j.cclet.2024.110125. doi: 10.1016/j.cclet.2024.110125
43. [43]
  H. Luo, T. Shan, J. Zhou, L. Huang, L. Chen, R. Sa, Y. Yamauchi, J. You, Y. Asakura, Z. Yuan, et al., Appl. Catal. B Environ. 337 (2023) 122933, https://doi.org/10.1016/j.apcatb.2023.122933. doi: 10.1016/j.apcatb.2023.122933
44. [44]
  L. Lin, Y. Ma, J. Vequizo, M. Nakabayashi, C. Gu, X. Tao, H. Yoshida, Y. Pihosh, Y. Nishina, A. Yamakata, et al., Nat. Commun. 15 (2024) 397, https://doi.org/10.1038/s41467-024-44706-4. doi: 10.1038/s41467-024-44706-4
45. [45]
  Q. Zhang, B. Wang, H. Miao, J. Fan, T. Sun, E. Liu, Chem. Eng. J. 482 (2024) 148844, https://doi.org/10.1016/j.cej.2024.148844. doi: 10.1016/j.cej.2024.148844
46. [46]
  X. Wang, S. Yuan, B. Feng, X. Qiu, C. Yu, W. Lu, X. Xu, Y. Hu, Y. Shi, J. Colloid Interface Sci. 691 (2025) 137371, https://doi.org/10.1016/j.jcis.2025.137371. doi: 10.1016/j.jcis.2025.137371
47. [47]
  J. Zhou, T. Shan, S. Wu, J. Li, F. Zhang, L. Huang, L. Chen, H. Xiao, Chem. Eng. J. 492 (2024) 152441, https://doi.org/10.1016/j.cej.2024.152441. doi: 10.1016/j.cej.2024.152441
48. [48]
  J. Tang, X. Wang, Y. Huang, X. Du, Z. He, D. Wang, S. Song, Chem. Eng. J. 499 (2024) 156055, https://doi.org/10.1016/j.cej.2024.156055. doi: 10.1016/j.cej.2024.156055
49. [49]
  K. Wang, Y. Yang, S. Farhan, Y. Wu, W. Lin, Chem. Eng. J. 490 (2024) 151408, https://doi.org/10.1016/j.cej.2024.151408. doi: 10.1016/j.cej.2024.151408
50. [50]
  W. Fu, S. Wang, Y. Zhang, B. Cheng, Y. Wu, J. Mater. Sci. Technol. 232 (2025) 181, https://doi.org/10.1016/j.jmst.2024.12.081. doi: 10.1016/j.jmst.2024.12.081
51. [51]
  S. Yang, K. Wang, Q. Chen, Y. Wu, J. Mater. Sci. Technol. 175 (2024) 104, https://doi.org/10.1016/j.jmst.2023.07.044. doi: 10.1016/j.jmst.2023.07.044
52. [52]
  S. Yang, K. Wang, Z. Wu, Y. Wu, J. Mater. Sci. Technol. 200 (2024) 253, https://doi.org/10.1016/j.jmst.2024.02.055. doi: 10.1016/j.jmst.2024.02.055
53. [53]
  R. Gao, R. Shen, C. Huang, K. Huang, G. Liang, P. Zhang, X. Li, Angew. Chem. Int. Ed. 64 (2025) e202414229, https://doi.org/10.1002/anie.202414229. doi: 10.1002/anie.202414229
54. [54]
  M. Gu, Y. Yang, L. Zhang, B. Zhu, G. Liang, J. Yu, App. Catal. B: Environ. 324 (2023) 122227, https://doi.org/10.1016/j.apcatb.2022.122227. doi: 10.1016/j.apcatb.2022.122227

扫一扫看文章

计量

PDF下载量: 0
文章访问数: 85
HTML全文浏览量: 12

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

通过间接两电子还原的HOF/BiVO₄ (010) S型光催化剂增强H₂O₂生产性能

通讯作者: hlw@hbeu.edu.cn (黄礼文); Email: wuyan@cug.edu.cn (吴艳)

English

Enhanced H₂O₂ production performance via indirect two-electron reduction of HOF/BiVO₄ (010) S-scheme photocatalyst

Corresponding author: hlw@hbeu.edu.cn (Liwen Huang); Email: wuyan@cug.edu.cn (Yan Wu)

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