通过电子给体酚羟基调控芘-COFs的反键轨道占据以促进光催化产氢

引用本文: 刘永康, 余守希, 陈丽, 王中辽, 张美玉, 张金峰. 通过电子给体酚羟基调控芘-COFs的反键轨道占据以促进光催化产氢[J]. 物理化学学报, 2026, 42(10): 100338. doi: 10.1016/j.actphy.2026.100338 shu

Citation: Yongkang Liu, Shouxi Yu, Li Chen, Zhongliao Wang, Meiyu Zhang, Jinfeng Zhang. Tuning antibonding-orbital occupancy in pyrene-COFs via electron-donating phenolic -OH for boosted photocatalytic H₂ evolution[J]. Acta Physico-Chimica Sinica, 2026, 42(10): 100338. doi: 10.1016/j.actphy.2026.100338 shu

通过电子给体酚羟基调控芘-COFs的反键轨道占据以促进光催化产氢

刘永康 ^1, ,
余守希 ^2, ,
陈丽 ^2, ,
王中辽 ^{2,
,} ,
张美玉 ^{3,
,} ,
张金峰 ^{1,
,}

1.
淮北师范大学物理与电子信息学院, 安徽省智能计算与应用重点实验室, 安徽淮北 235000;
2.
淮北师范大学能源科学与工程学院, 安徽淮北 235000;
3.
聊城大学化学化工学院, 山东省化学储能与新型电池技术重点实验室, 山东聊城 252059

通讯作者: 王中辽,E-mail:wangzl@chnu.edu.cn; 张美玉,E-mail:zhangmeiyu@lcu.edu.cn; 张金峰,E-mail:jfzhang@chnu.edu.cn

基金项目:
本研究得到国家自然科学基金(项目编号：52402116)、山东省自然科学基金(项目编号：ZR2023QB203)以及安徽省学科(专业)带头人培养项目(项目编号：DTR2024015)的资助。

摘要: 共价有机框架(COF)作为析氢反应(HER)的光催化剂被广泛研究，但多数设计策略聚焦于光吸收或电荷分离，而非催化位点本身的H*脱附能垒。本研究从键分辨视角重新审视该问题：采用晶体轨道哈密顿布居(COHP)方法，将N-H反键轨道的占据程度作为量化描述符，用于评估希夫碱COF中亚胺氮原子对H*的结合强度。通过合成两种芘基COF (PY-BD与PY-DHBD)验证该描述符：在二醛连接体中引入两个酚羟基后，反键轨道占据率提升(ICOHP从-7.52增至-7.18 eV)，N-H键弱化，ΔG_H*从-0.22 eV优化至0.04 eV (接近热中性)。可见光驱动的产氢速率相应从450 μmol g^-1 h^-1提升至1127 μmol g^-1 h^-1，达到PY-BD的2.5倍。该研究将COHP解析的反键占据率与金属催化中经典的d带中心理论并列，为调控富氮COF活性位点的HER性能提供了定量描述框架。

关键词:

芘-COFs
/ 给电子
/ 酚羟基
/ 光催化析氢
/ COHP

English

Tuning antibonding-orbital occupancy in pyrene-COFs via electron-donating phenolic -OH for boosted photocatalytic H₂ evolution

Yongkang Liu ^1, ,
Shouxi Yu ^2, ,
Li Chen ^2, ,
Zhongliao Wang ^{2,
,} ,
Meiyu Zhang ^{3,
,} ,
Jinfeng Zhang ^{1,
,}

1.
Anhui Province Key Laboratory of Intelligent Computing and Applications, College of Physics and Electronic Engineering, Huaibei Normal University, Huaibei 235000, Anhui Province, China;
2.
College of Energy Science and Engineering, Huaibei Normal University, Huaibei 235000, Anhui Province, China;
3.
Shandong Provincial Key Laboratory of Chemical Energy Storage and Novel Cell Technology, School of Chemistry & Chemical Engineering, Liaocheng University, Liaocheng 252059, Shandong Province, China

Corresponding author: Zhongliao Wang, ; Meiyu Zhang, ; Jinfeng Zhang,

Received Date: 04 May 2026
Accepted Date: 01 June 2026
Revised Date: 30 May 2026

Abstract: Covalent organic frameworks (COFs) are widely studied as photocatalysts for the hydrogen evolution reaction (HER), yet most design strategies target light absorption or charge separation rather than the H* desorption barrier at the catalytic site itself. We re-examine the problem from a bond-resolved view: the crystal orbital Hamilton population (COHP) is used to treat the occupancy of the N-H antibonding manifold as a quantitative descriptor of how strongly the imine nitrogen of a Schiff-base COF binds H*. Two pyrene-based COFs, PY-BD and PY-DHBD, are synthesized to test the descriptor. Adding two phenolic -OH groups to the dialdehyde linker raises the antibonding occupancy (ICOHP from -7.52 to -7.18 eV), weakens the N-H bond, and shifts ΔG_H* from -0.22 to 0.04 eV, close to thermoneutrality. The visible-light HS₂^-evolution rate accordingly rises from 450 to 1127 μmol g^-1 h^-1, 2.5-fold the rate of PY-BD. The work places COHP-resolved antibonding occupancy alongside the d-band-centre framework familiar from metal catalysis as a quantitative descriptor for tuning HER on N-rich COF active sites.

Key words:

1. [1]
  C. Bie, L. Wang, J. Yu, Chem 8(2022) 1567, https://doi.org/10.1016/j.chempr.2022.04.013.C. Bie, L. Wang, J. Yu, Chem 8(2022) 1567, https://doi.org/10.1016/j.chempr.2022.04.013.
2. [2]
  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.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.
3. [3]
  K. Meng, J. Zhang, B. Cheng, X. Ren, Z. Xia, F. Xu, L. Zhang, J. Yu, Adv. Mater. 36(2024) 2406460, https://doi.org/10.1002/adma.202406460.K. Meng, J. Zhang, B. Cheng, X. Ren, Z. Xia, F. Xu, L. Zhang, J. Yu, Adv. Mater. 36(2024) 2406460, https://doi.org/10.1002/adma.202406460.
4. [4]
  K. Meng, J. Zhang, B. Zhu, C. Jiang, H. García, J. Yu, Adv. Mater. 37(2025) 2505088, https://doi.org/10.1002/adma.202505088.K. Meng, J. Zhang, B. Zhu, C. Jiang, H. García, J. Yu, Adv. Mater. 37(2025) 2505088, https://doi.org/10.1002/adma.202505088.
5. [5]
  J. Xu, W. Zhong, F. Chen, X. Wang, H. Yu, Appl. Catal. B: Environ. 328(2023) 122493, https://doi.org/10.1016/j.apcatb.2023.122493.J. Xu, W. Zhong, F. Chen, X. Wang, H. Yu, Appl. Catal. B: Environ. 328(2023) 122493, https://doi.org/10.1016/j.apcatb.2023.122493.
6. [6]
  H. Ran, X. Liu, L. Ye, J. Fan, B. Zhu, Q. Xu, Y. Wei, J. Mater. Sci. Technol. 234(2025) 24, https://doi.org/10.1016/j.jmst.2024.12.089.H. Ran, X. Liu, L. Ye, J. Fan, B. Zhu, Q. Xu, Y. Wei, J. Mater. Sci. Technol. 234(2025) 24, https://doi.org/10.1016/j.jmst.2024.12.089.
7. [7]
  D. Liu, Z. Tang, H. Wang, X. Li, J. Li, C. Zhu, S. Ding, Y.-S. Cheng, H. Zhang, P. Li, J. Wu, G. Yuan, Chin. J. Struct. Chem. 45(2026) 100762, https://doi.org/10.1016/j.cjsc.2025.100762.D. Liu, Z. Tang, H. Wang, X. Li, J. Li, C. Zhu, S. Ding, Y.-S. Cheng, H. Zhang, P. Li, J. Wu, G. Yuan, Chin. J. Struct. Chem. 45(2026) 100762, https://doi.org/10.1016/j.cjsc.2025.100762.
8. [8]
  S. Cao, B. Zhong, C. Bie, B. Cheng, F. Xu, Acta Phys. Chim. Sin. 40(2024) 2307016, https://doi.org/10.3866/pku.whxb202307016.S. Cao, B. Zhong, C. Bie, B. Cheng, F. Xu, Acta Phys. Chim. Sin. 40(2024) 2307016, https://doi.org/10.3866/pku.whxb202307016.
9. [9]
  G. Chen, Z. Zheng, W. Zhong, G. Wang, X. Wu, Acta Phys. Chim. Sin. 40(2024) 2406021, https://doi.org/10.3866/pku.whxb202406021.G. Chen, Z. Zheng, W. Zhong, G. Wang, X. Wu, Acta Phys. Chim. Sin. 40(2024) 2406021, https://doi.org/10.3866/pku.whxb202406021.
10. [10]
  W. Yu, C. Bie, Acta Phys. Chim. Sin. 40(2024) 2307022, https://doi.org/10.3866/pku.whxb202307022.W. Yu, C. Bie, Acta Phys. Chim. Sin. 40(2024) 2307022, https://doi.org/10.3866/pku.whxb202307022.
11. [11]
  B. Zhu, J. Sun, Y. Zhao, L. Zhang, J. Yu, Adv. Mater. 36(2024) 2310600, https://doi.org/10.1002/adma.202310600.B. Zhu, J. Sun, Y. Zhao, L. Zhang, J. Yu, Adv. Mater. 36(2024) 2310600, https://doi.org/10.1002/adma.202310600.
12. [12]
  L. Zhang, J. Zhang, J. Yu, Chem 12(2026) 102719, https://doi.org/10.1016/j.chempr.2025.102719.L. Zhang, J. Zhang, J. Yu, Chem 12(2026) 102719, https://doi.org/10.1016/j.chempr.2025.102719.
13. [13]
  C. Zhang, Y. Zhong, X. Wang, Y. Chen, C. Jiang, T. Majozi, Z. Wang, F. Karadas, J. Low, Y. Xiong, J. Mater. Sci. Technol. 254(2026) 258, https://doi.org/10.1016/j.jmst.2025.07.058.C. Zhang, Y. Zhong, X. Wang, Y. Chen, C. Jiang, T. Majozi, Z. Wang, F. Karadas, J. Low, Y. Xiong, J. Mater. Sci. Technol. 254(2026) 258, https://doi.org/10.1016/j.jmst.2025.07.058.
14. [14]
  F. Xu, L. Zheng, J. Zhang, Y. He, H. Cao, X. Zheng, H. García, J. Yu, Nat. Catal. 9(2026) 73, https://doi.org/10.1038/s41929-025-01471-x.F. Xu, L. Zheng, J. Zhang, Y. He, H. Cao, X. Zheng, H. García, J. Yu, Nat. Catal. 9(2026) 73, https://doi.org/10.1038/s41929-025-01471-x.
15. [15]
  W. Yu, M.H. Richter, P. Buabthong, I.A. Moreno-Hernandez, C.G. Read, E. Simonoff, B.S. Brunschwig, N.S. Lewis, Energy Environ. Sci. 14(2021) 6007, https://doi.org/10.1039/d1ee02809j.W. Yu, M.H. Richter, P. Buabthong, I.A. Moreno-Hernandez, C.G. Read, E. Simonoff, B.S. Brunschwig, N.S. Lewis, Energy Environ. Sci. 14(2021) 6007, https://doi.org/10.1039/d1ee02809j.
16. [16]
  Y. Shao, R. Shen, S. Wang, S. Li, P. Zhang, X. Li, Acta Phys. Chim. Sin. 41(2025) 100176, https://doi.org/10.1016/j.actphy.2025.100176.Y. Shao, R. Shen, S. Wang, S. Li, P. Zhang, X. Li, Acta Phys. Chim. Sin. 41(2025) 100176, https://doi.org/10.1016/j.actphy.2025.100176.
17. [17]
  H. Dong, C. Qu, C. Li, B. Hu, X. Li, G. Liang, J. Jiang, Chin. J. Catal. 70(2025) 142, https://doi.org/10.1016/S1872-2067(24)60184-1.H. Dong, C. Qu, C. Li, B. Hu, X. Li, G. Liang, J. Jiang, Chin. J. Catal. 70(2025) 142, https://doi.org/10.1016/S1872-2067(24)60184-1.
18. [18]
  X. Lin, J. Zheng, L. Wang, J. Wang, D. Jiang, Y. Yamauchi, C. Zhang, Z. Yuan, ACS Catal. 16(2026) 57, https://doi.org/10.1021/acscatal.5c06316.X. Lin, J. Zheng, L. Wang, J. Wang, D. Jiang, Y. Yamauchi, C. Zhang, Z. Yuan, ACS Catal. 16(2026) 57, https://doi.org/10.1021/acscatal.5c06316.
19. [19]
  S. Manzoor, M.A. Younis, Y. Yao, Q.-u.-n. Tariq, B. Zhang, B. Tian, L. Yan, C. Qiu, Coord. Chem. Rev. 541(2025) 216840, https://doi.org/10.1016/j.ccr.2025.216840.S. Manzoor, M.A. Younis, Y. Yao, Q.-u.-n. Tariq, B. Zhang, B. Tian, L. Yan, C. Qiu, Coord. Chem. Rev. 541(2025) 216840, https://doi.org/10.1016/j.ccr.2025.216840.
20. [20]
  Y. Li, J. Yang, W. Si, Y. Cao, J. Shi, W. Han, J. Qian, W. Qin, Sep. Purif. Technol. 356(2025) 129809, https://doi.org/10.1016/j.seppur.2024.129809.Y. Li, J. Yang, W. Si, Y. Cao, J. Shi, W. Han, J. Qian, W. Qin, Sep. Purif. Technol. 356(2025) 129809, https://doi.org/10.1016/j.seppur.2024.129809.
21. [21]
  A.T. Partho, M. Tahir, B. Tahir, Int. J. Hydrogen Energy 47(2022) 34323, https://doi.org/10.1016/j.ijhydene.2022.08.060.A.T. Partho, M. Tahir, B. Tahir, Int. J. Hydrogen Energy 47(2022) 34323, https://doi.org/10.1016/j.ijhydene.2022.08.060.
22. [22]
  J. Guo, L. Xue, F. Song, C. Li, Z. Chen, L. Wen, Acta Phys. Chim. Sin. 42(2026) 100177, https://doi.org/10.1016/j.actphy.2025.100177.J. Guo, L. Xue, F. Song, C. Li, Z. Chen, L. Wen, Acta Phys. Chim. Sin. 42(2026) 100177, https://doi.org/10.1016/j.actphy.2025.100177.
23. [23]
  M. Wang, Y. Li, D. Yan, H. Hu, Y. Song, X. Su, J. Sun, S. Xiao, Y. Gao, Chin. J. Catal. 65(2024) 103, https://doi.org/10.1016/S1872-2067(24)60113-0.M. Wang, Y. Li, D. Yan, H. Hu, Y. Song, X. Su, J. Sun, S. Xiao, Y. Gao, Chin. J. Catal. 65(2024) 103, https://doi.org/10.1016/S1872-2067(24)60113-0.
24. [24]
  L. Zhang, H. Zhang, D. Zhu, Z. Fu, S. Dong, C. Lyu, Chin. J. Catal. 66(2024) 181, https://doi.org/10.1016/S1872-2067(24)60132-4.L. Zhang, H. Zhang, D. Zhu, Z. Fu, S. Dong, C. Lyu, Chin. J. Catal. 66(2024) 181, https://doi.org/10.1016/S1872-2067(24)60132-4.
25. [25]
  L. Wang, W. Cheng, J. Wang, J. Yang, Q. Liu, Chin. J. Catal. 58(2024) 194, https://doi.org/10.1016/S1872-2067(23)64602-9.L. Wang, W. Cheng, J. Wang, J. Yang, Q. Liu, Chin. J. Catal. 58(2024) 194, https://doi.org/10.1016/S1872-2067(23)64602-9.
26. [26]
  Y.-Y. Gu, J. Wang, Q. Tang, H. Wei, J. Ning, X. Lan, X. Wang, X. Li, Y. Jia, S. Wang, L. Hao, ACS Catal. 14(2024) 11262, https://doi.org/10.1021/acscatal.4c02827.Y.-Y. Gu, J. Wang, Q. Tang, H. Wei, J. Ning, X. Lan, X. Wang, X. Li, Y. Jia, S. Wang, L. Hao, ACS Catal. 14(2024) 11262, https://doi.org/10.1021/acscatal.4c02827.
27. [27]
  J. Yang, X. Zhang, W. Si, Y. Cao, J. Qian, Y. Li, B. Li, W. Qin, ACS Catal. 14(2024) 2022, https://doi.org/10.1021/acscatal.3c03034.J. Yang, X. Zhang, W. Si, Y. Cao, J. Qian, Y. Li, B. Li, W. Qin, ACS Catal. 14(2024) 2022, https://doi.org/10.1021/acscatal.3c03034.
28. [28]
  B. Qi, R. Shen, Z. Ren, Y. Teng, H. Ding, X. Zhang, Y. Zhang, L. Hao, X. Li, J. Mater. Sci. Technol. 232(2025) 65, https://doi.org/10.1016/j.jmst.2025.03.003.B. Qi, R. Shen, Z. Ren, Y. Teng, H. Ding, X. Zhang, Y. Zhang, L. Hao, X. Li, J. Mater. Sci. Technol. 232(2025) 65, https://doi.org/10.1016/j.jmst.2025.03.003.
29. [29]
  Y. He, L. Zheng, W. Mei, J. Zhang, C. Bie, J. Yu, H. García, F. Xu, Adv. Funct. Mater. 36(2026) e18330, https://doi.org/10.1002/adfm.202518330.Y. He, L. Zheng, W. Mei, J. Zhang, C. Bie, J. Yu, H. García, F. Xu, Adv. Funct. Mater. 36(2026) e18330, https://doi.org/10.1002/adfm.202518330.
30. [30]
  Y.-Q. Xia, S.-M. Jing, L.-M. Chang, Z.-G. Gu, J. Zhang, Chin. J. Struct. Chem. 45(2026) 100731, https://doi.org/10.1016/j.cjsc.2025.100731.Y.-Q. Xia, S.-M. Jing, L.-M. Chang, Z.-G. Gu, J. Zhang, Chin. J. Struct. Chem. 45(2026) 100731, https://doi.org/10.1016/j.cjsc.2025.100731.
31. [31]
  X. Chen, W. Huang, X. Zhao, S. Zhang, X. Miao, Chin. J. Struct. Chem. 44(2025) 100604, https://doi.org/10.1016/j.cjsc.2025.100604.X. Chen, W. Huang, X. Zhao, S. Zhang, X. Miao, Chin. J. Struct. Chem. 44(2025) 100604, https://doi.org/10.1016/j.cjsc.2025.100604.
32. [32]
  T. Dong, X. Wen, X. Wu, Y. Jiang, C. Wang, R. Liu, J. Li, W. Zhou, Y. Song, X. Shi, et al., Chin. J. Struct. Chem. 44(2025) 100733, https://doi.org/10.1016/j.cjsc.2025.100733.T. Dong, X. Wen, X. Wu, Y. Jiang, C. Wang, R. Liu, J. Li, W. Zhou, Y. Song, X. Shi, et al., Chin. J. Struct. Chem. 44(2025) 100733, https://doi.org/10.1016/j.cjsc.2025.100733.
33. [33]
  L. Zhao, K. Xu, C. Bie, Acta Phys. Chim. Sin. 42(2026) 100216, https://doi.org/10.1016/j.actphy.2025.100216.L. Zhao, K. Xu, C. Bie, Acta Phys. Chim. Sin. 42(2026) 100216, https://doi.org/10.1016/j.actphy.2025.100216.
34. [34]
  J. Qiu, C. Cheng, H. García, G. Liang, B. Zhu, L. Zhang, J. Yu, Angew. Chem. Int. Ed. 64(2025) e202515898, https://doi.org/10.1002/anie.202515898.J. Qiu, C. Cheng, H. García, G. Liang, B. Zhu, L. Zhang, J. Yu, Angew. Chem. Int. Ed. 64(2025) e202515898, https://doi.org/10.1002/anie.202515898.
35. [35]
  Y. He, P. Hu, J. Zhang, G. Liang, J. Yu, F. Xu, ACS Catal. 14(2024) 1951, https://doi.org/10.1021/acscatal.4c00026.Y. He, P. Hu, J. Zhang, G. Liang, J. Yu, F. Xu, ACS Catal. 14(2024) 1951, https://doi.org/10.1021/acscatal.4c00026.
36. [36]
  X. Zhao, Y. Cao, M. Lei, Z. Jin, N. Tsubaki, Acta Phys. Chim. Sin. 41(2025) 100152, https://doi.org/10.1016/j.actphy.2025.100152.X. Zhao, Y. Cao, M. Lei, Z. Jin, N. Tsubaki, Acta Phys. Chim. Sin. 41(2025) 100152, https://doi.org/10.1016/j.actphy.2025.100152.
37. [37]
  G. Tang, J. Zhang, C. Bie, X. Zheng, C. Jiang, J. Yu, Adv. Mater. 37(2025) e14576, https://doi.org/10.1002/adma.202514576.G. Tang, J. Zhang, C. Bie, X. Zheng, C. Jiang, J. Yu, Adv. Mater. 37(2025) e14576, https://doi.org/10.1002/adma.202514576.
38. [38]
  J. Pan, A. Zhang, L. Zhang, P. Dong, Chin. J. Catal. 58(2024) 180, https://doi.org/10.1016/S1872-2067(23)64609-1.J. Pan, A. Zhang, L. Zhang, P. Dong, Chin. J. Catal. 58(2024) 180, https://doi.org/10.1016/S1872-2067(23)64609-1.
39. [39]
  X. Wu, M. Sayed, G. Wang, W. Yu, B. Zhu, Adv. Mater. 38(2026) e11322, https://doi.org/10.1002/adma.202511322.X. Wu, M. Sayed, G. Wang, W. Yu, B. Zhu, Adv. Mater. 38(2026) e11322, https://doi.org/10.1002/adma.202511322.
40. [40]
  Y. Kobayashi, I. Tateishi, M. Uzzaman, H. Katsumata, M. Furukawa, S. Kaneco, Solid State Sci. 169(2025) 108084, https://doi.org/10.1016/j.solidstatesciences.2025.108084.Y. Kobayashi, I. Tateishi, M. Uzzaman, H. Katsumata, M. Furukawa, S. Kaneco, Solid State Sci. 169(2025) 108084, https://doi.org/10.1016/j.solidstatesciences.2025.108084.
41. [41]
  A. Rodríguez-Camargo, M.W. Terban, M. Paetsch, E.A. Rico, D. Graf, R. Hirpara, V. Duppel, I. Moudrakovski, M. Etter, N. Guijarro, et al., Nat. Synth. 4(2025) 710, https://doi.org/10.1038/s44160-024-00731-1.A. Rodríguez-Camargo, M.W. Terban, M. Paetsch, E.A. Rico, D. Graf, R. Hirpara, V. Duppel, I. Moudrakovski, M. Etter, N. Guijarro, et al., Nat. Synth. 4(2025) 710, https://doi.org/10.1038/s44160-024-00731-1.
42. [42]
  C. Zhao, Z. Li, D. Wu, X. Yang, Acta Phys. Chim. Sin. 42(2026) 100149, https://doi.org/10.1016/j.actphy.2025.100149.C. Zhao, Z. Li, D. Wu, X. Yang, Acta Phys. Chim. Sin. 42(2026) 100149, https://doi.org/10.1016/j.actphy.2025.100149.
43. [43]
  Z. Lin, W. Xie, M. Zhu, C. Wang, J. Guo, Chin. J. Catal. 64(2024) 87, https://doi.org/10.1016/S1872-2067(24)60107-5.Z. Lin, W. Xie, M. Zhu, C. Wang, J. Guo, Chin. J. Catal. 64(2024) 87, https://doi.org/10.1016/S1872-2067(24)60107-5.
44. [44]
  J.-Z. Xiao, Z.-H. Zhao, N.-N. Zhang, H.-T. Che, X. Qiao, G.-Y. Zhang, X. Chu, Y. Wang, H. Dong, F.-M. Zhang, Chin. J. Catal. 69(2025) 219, https://doi.org/10.1016/S1872-2067(24)60195-6.J.-Z. Xiao, Z.-H. Zhao, N.-N. Zhang, H.-T. Che, X. Qiao, G.-Y. Zhang, X. Chu, Y. Wang, H. Dong, F.-M. Zhang, Chin. J. Catal. 69(2025) 219, https://doi.org/10.1016/S1872-2067(24)60195-6.
45. [45]
  H. Wu, X. He, X. Du, D. Wang, W. Li, H. Chen, W. Fang, L. Zhao, Small 19(2023) 2304367, https://doi.org/10.1002/smll.202304367.H. Wu, X. He, X. Du, D. Wang, W. Li, H. Chen, W. Fang, L. Zhao, Small 19(2023) 2304367, https://doi.org/10.1002/smll.202304367.
46. [46]
  W. Li, Y. Wang, L. Li, X. Huang, M. Liu, B. Gui, X. Lang, C. Wang, Chin. J. Struct. Chem. 43(2024) 100299, https://doi.org/10.1016/j.cjsc.2024.100299.W. Li, Y. Wang, L. Li, X. Huang, M. Liu, B. Gui, X. Lang, C. Wang, Chin. J. Struct. Chem. 43(2024) 100299, https://doi.org/10.1016/j.cjsc.2024.100299.
47. [47]
  X. Sun, K. Kong, J. Liang, D. Wang, B. Dong, R. Wang, Chin. J. Struct. Chem. 44(2025) 100652, https://doi.org/10.1016/j.cjsc.2025.100652.X. Sun, K. Kong, J. Liang, D. Wang, B. Dong, R. Wang, Chin. J. Struct. Chem. 44(2025) 100652, https://doi.org/10.1016/j.cjsc.2025.100652.
48. [48]
  H. Hu, X. Sun, H. Li, H. Pan, Y. Ma, H. Huang, T. Ma, Small 21(2025) 2407117, https://doi.org/10.1002/smll.202407117.H. Hu, X. Sun, H. Li, H. Pan, Y. Ma, H. Huang, T. Ma, Small 21(2025) 2407117, https://doi.org/10.1002/smll.202407117.
49. [49]
  Z. Wang, C. Bie, J. Mater. Sci. Technol. 243(2026) 206, https://doi.org/10.1016/j.jmst.2025.04.028.Z. Wang, C. Bie, J. Mater. Sci. Technol. 243(2026) 206, https://doi.org/10.1016/j.jmst.2025.04.028.
50. [50]
  P. Das, G. Chakraborty, J. Yang, J. Roeser, H. Küçükkeçeci, A.D. Nguyen, M. Schwarze, J. Gabriel, C. Penschke, S. Du, et al., Adv. Energy Mater. 16(2026) 2501193, https://doi.org/10.1002/aenm.202501193.P. Das, G. Chakraborty, J. Yang, J. Roeser, H. Küçükkeçeci, A.D. Nguyen, M. Schwarze, J. Gabriel, C. Penschke, S. Du, et al., Adv. Energy Mater. 16(2026) 2501193, https://doi.org/10.1002/aenm.202501193.
51. [51]
  H. Wang, W.-N. Jiao, W.-D. Zhu, S. Huang, X.-C. Lin, T. Chen, Y. Fan, F. Chen, H.-S. Xu, M. Pan, et al., Angew. Chem. Int. Ed. 64(2025) e202511559, https://doi.org/10.1002/anie.202511559.H. Wang, W.-N. Jiao, W.-D. Zhu, S. Huang, X.-C. Lin, T. Chen, Y. Fan, F. Chen, H.-S. Xu, M. Pan, et al., Angew. Chem. Int. Ed. 64(2025) e202511559, https://doi.org/10.1002/anie.202511559.
52. [52]
  Y. Xiang, W. Dong, P. Wang, S. Wang, X. Ding, F. Ichihara, Z. Wang, Y. Wada, S. Jin, Y. Weng, et al., Appl. Catal. B: Environ. 274(2020) 119096, https://doi.org/10.1016/j.apcatb.2020.119096.Y. Xiang, W. Dong, P. Wang, S. Wang, X. Ding, F. Ichihara, Z. Wang, Y. Wada, S. Jin, Y. Weng, et al., Appl. Catal. B: Environ. 274(2020) 119096, https://doi.org/10.1016/j.apcatb.2020.119096.
53. [53]
  J. Ma, L. Li, Y. Zhang, J. Qian, X. Wang, Chin. J. Struct. Chem. 43(2024) 100466, https://doi.org/10.1016/j.cjsc.2024.100466.J. Ma, L. Li, Y. Zhang, J. Qian, X. Wang, Chin. J. Struct. Chem. 43(2024) 100466, https://doi.org/10.1016/j.cjsc.2024.100466.
54. [54]
  J. Ning, J. Huang, Y. Liu, Y. Chen, Q. Niu, Q. Lin, Y. He, Z. Liu, Y. Yu, L. Li, Chin. J. Struct. Chem. 43(2024) 100453, https://doi.org/10.1016/j.cjsc.2024.100453.J. Ning, J. Huang, Y. Liu, Y. Chen, Q. Niu, Q. Lin, Y. He, Z. Liu, Y. Yu, L. Li, Chin. J. Struct. Chem. 43(2024) 100453, https://doi.org/10.1016/j.cjsc.2024.100453.
55. [55]
  A. Chakraborty, A. Alam, U. Pal, A. Sinha, S. Das, T. Saha-Dasgupta, P. Pachfule, Nat. Commun. 16(2025) 503, https://doi.org/10.1038/s41467-025-55894-y.A. Chakraborty, A. Alam, U. Pal, A. Sinha, S. Das, T. Saha-Dasgupta, P. Pachfule, Nat. Commun. 16(2025) 503, https://doi.org/10.1038/s41467-025-55894-y.
56. [56]
  F. Xie, C. Yuan, H. Tan, A.Z. Moshfegh, B. Zhu, J. Yu, Acta Phys. Chim. Sin. 40(2024) 2407013, https://doi.org/10.3866/pku.whxb202407013.F. Xie, C. Yuan, H. Tan, A.Z. Moshfegh, B. Zhu, J. Yu, Acta Phys. Chim. Sin. 40(2024) 2407013, https://doi.org/10.3866/pku.whxb202407013.
57. [57]
  X. Xiang, B. Cheng, B. Zhu, C. Jiang, G. Liang, Chin. J. Catal. 68(2025) 326, https://doi.org/10.1016/S1872-2067(24)60167-1.X. Xiang, B. Cheng, B. Zhu, C. Jiang, G. Liang, Chin. J. Catal. 68(2025) 326, https://doi.org/10.1016/S1872-2067(24)60167-1.
58. [58]
  W. Zhong, A. Meng, X. Cai, Y. Gan, J. Wang, Y. Su, Chin. J. Catal. 76(2025) 108, https://doi.org/10.1016/S1872-2067(25)64747-4.W. Zhong, A. Meng, X. Cai, Y. Gan, J. Wang, Y. Su, Chin. J. Catal. 76(2025) 108, https://doi.org/10.1016/S1872-2067(25)64747-4.
59. [59]
  S. Zhang, C. Bie, Rare Met. 44(2025) 9289, https://doi.org/10.1007/s12598-025-03584-5.S. Zhang, C. Bie, Rare Met. 44(2025) 9289, https://doi.org/10.1007/s12598-025-03584-5.
60. [60]
  D. Gao, H. Yu, H. García, J. Yu, Prog. Mater. Sci. 159(2026) 101663, https://doi.org/10.1016/j.pmatsci.2026.101663.D. Gao, H. Yu, H. García, J. Yu, Prog. Mater. Sci. 159(2026) 101663, https://doi.org/10.1016/j.pmatsci.2026.101663.
61. [61]
  M. Bi, Y. Ma, J. Chai, Y. Su, Y. Xia, Sep. Purif. Technol. 375(2025) 133810, https://doi.org/10.1016/j.seppur.2025.133810.M. Bi, Y. Ma, J. Chai, Y. Su, Y. Xia, Sep. Purif. Technol. 375(2025) 133810, https://doi.org/10.1016/j.seppur.2025.133810.
62. [62]
  Z. Lu, H. Lv, Q. Liu, Z. Wang, Acta Phys. Chim. Sin. 40(2024) 2405005, https://doi.org/10.3866/pku.whxb202405005.Z. Lu, H. Lv, Q. Liu, Z. Wang, Acta Phys. Chim. Sin. 40(2024) 2405005, https://doi.org/10.3866/pku.whxb202405005.
63. [63]
  Q. Liao, Q. Sun, H. Xu, Y. Wang, Y. Xu, Z. Li, J. Hu, D. Wang, H. Li, K. Xi, Angew. Chem. Int. Ed. 62(2023) e202310556, https://doi.org/10.1002/anie.202310556.Q. Liao, Q. Sun, H. Xu, Y. Wang, Y. Xu, Z. Li, J. Hu, D. Wang, H. Li, K. Xi, Angew. Chem. Int. Ed. 62(2023) e202310556, https://doi.org/10.1002/anie.202310556.
64. [64]
  D. Gao, P. Deng, J. Zhang, L. Zhang, X. Wang, H. Yu, J. Yu, Angew. Chem. Int. Ed. 62(2023) e202304559, https://doi.org/10.1002/anie.202304559.D. Gao, P. Deng, J. Zhang, L. Zhang, X. Wang, H. Yu, J. Yu, Angew. Chem. Int. Ed. 62(2023) e202304559, https://doi.org/10.1002/anie.202304559.
65. [65]
  H. Long, X. Zhang, Z. Zhang, J. Zhang, J. Yu, H. Yu, Nat. Commun. 16(2025) 946, https://doi.org/10.1038/s41467-025-56306-x.H. Long, X. Zhang, Z. Zhang, J. Zhang, J. Yu, H. Yu, Nat. Commun. 16(2025) 946, https://doi.org/10.1038/s41467-025-56306-x.
66. [66]
  H. Long, R. Li, C. Bie, J. Zhang, J. Yu, H. García, H. Yu, J. Am. Chem. Soc. 148(2026) 17146, https://doi.org/10.1021/jacs.6c01844.H. Long, R. Li, C. Bie, J. Zhang, J. Yu, H. García, H. Yu, J. Am. Chem. Soc. 148(2026) 17146, https://doi.org/10.1021/jacs.6c01844.
67. [67]
  D. Gao, J. Zhang, H. Yu, C. Jiang, H. García, J. Yu, Angew. Chem. Int. Ed. 65(2026) e2317803, https://doi.org/10.1002/anie.2317803.D. Gao, J. Zhang, H. Yu, C. Jiang, H. García, J. Yu, Angew. Chem. Int. Ed. 65(2026) e2317803, https://doi.org/10.1002/anie.2317803.
68. [68]
  C. Sun, Y. Han, H. Guo, R. Zhao, Y. Liu, Z. Lin, Z. Xiao, Z. Sun, M. Luo, S. Guo, Adv. Mater. 37(2025) 2502990, https://doi.org/10.1002/adma.202502990.C. Sun, Y. Han, H. Guo, R. Zhao, Y. Liu, Z. Lin, Z. Xiao, Z. Sun, M. Luo, S. Guo, Adv. Mater. 37(2025) 2502990, https://doi.org/10.1002/adma.202502990.
69. [69]
  X. Zhou, Y. Huo, S. Yang, B. He, X. Wang, Z. Wu, J. Zhang, Acta Phys. Chim. Sin. 41(2025) 100160, https://doi.org/10.1016/j.actphy.2025.100160.X. Zhou, Y. Huo, S. Yang, B. He, X. Wang, Z. Wu, J. Zhang, Acta Phys. Chim. Sin. 41(2025) 100160, https://doi.org/10.1016/j.actphy.2025.100160.
70. [70]
  G. Kresse, J. Furthmüller, Phys. Rev. B 54(1996) 11169, https://doi.org/10.1103/physrevb.54.11169.G. Kresse, J. Furthmüller, Phys. Rev. B 54(1996) 11169, https://doi.org/10.1103/physrevb.54.11169.
71. [71]
  G. Kresse, D. Joubert, Phys. Rev. B 59(1999) 1758, https://doi.org/10.1103/physrevb.59.1758.G. Kresse, D. Joubert, Phys. Rev. B 59(1999) 1758, https://doi.org/10.1103/physrevb.59.1758.
72. [72]
  J.P. Perdew, K. Burke, M. Ernzerhof, Phys. Rev. Lett. 77(1996) 3865, https://doi.org/10.1103/physrevlett.77.3865.J.P. Perdew, K. Burke, M. Ernzerhof, Phys. Rev. Lett. 77(1996) 3865, https://doi.org/10.1103/physrevlett.77.3865.
73. [73]
  J.K. Nørskov, T. Bligaard, Á. Logadóttir, J.R. Kitchin, J.G. Chen, S. Pandelov, U. Stimming, J. Electrochem. Soc. 152(2005) J23, https://doi.org/10.1149/1.1856988.J.K. Nørskov, T. Bligaard, Á. Logadóttir, J.R. Kitchin, J.G. Chen, S. Pandelov, U. Stimming, J. Electrochem. Soc. 152(2005) J23, https://doi.org/10.1149/1.1856988.
74. [74]
  S. Grimme, J. Antony, S. Ehrlich, H. Krieg, J. Chem. Phys. 132(2010) 154104, https://doi.org/10.1063/1.3382344.S. Grimme, J. Antony, S. Ehrlich, H. Krieg, J. Chem. Phys. 132(2010) 154104, https://doi.org/10.1063/1.3382344.
75. [75]
  V. Wang, N. Xu, J.-C. Liu, G. Tang, W.-T. Geng, Comput. Phys. Commun. 267(2021) 108033, https://doi.org/10.1016/j.cpc.2021.108033.V. Wang, N. Xu, J.-C. Liu, G. Tang, W.-T. Geng, Comput. Phys. Commun. 267(2021) 108033, https://doi.org/10.1016/j.cpc.2021.108033.
76. [76]
  W. Tang, E. Sanville, G. Henkelman, J. Phys.: Condens. Matter 21(2009) 084204, https://doi.org/10.1088/0953-8984/21/8/084204.W. Tang, E. Sanville, G. Henkelman, J. Phys.: Condens. Matter 21(2009) 084204, https://doi.org/10.1088/0953-8984/21/8/084204.
77. [77]
  S. Maintz, V.L. Deringer, A.L. Tchougréeff, R. Dronskowski, J. Comput. Chem. 37(2016) 1030, https://doi.org/10.1002/jcc.24300.S. Maintz, V.L. Deringer, A.L. Tchougréeff, R. Dronskowski, J. Comput. Chem. 37(2016) 1030, https://doi.org/10.1002/jcc.24300.
78. [78]
  Y. Li, C. Wang, S. Ma, H. Zhang, J. Ou, Y. Wei, M. Ye, ACS Appl. Mater. Interfaces 11(2019) 11706, https://doi.org/10.1021/acsami.8b18502.Y. Li, C. Wang, S. Ma, H. Zhang, J. Ou, Y. Wei, M. Ye, ACS Appl. Mater. Interfaces 11(2019) 11706, https://doi.org/10.1021/acsami.8b18502.
79. [79]
  V.S. Vyas, F. Haase, L. Stegbauer, G. Savasci, F. Podjaski, C. Ochsenfeld, B.V. Lotsch, Nat. Commun. 6(2015) 8508, https://doi.org/10.1038/ncomms9508.V.S. Vyas, F. Haase, L. Stegbauer, G. Savasci, F. Podjaski, C. Ochsenfeld, B.V. Lotsch, Nat. Commun. 6(2015) 8508, https://doi.org/10.1038/ncomms9508.
80. [80]
  S.A. Hashemi, A. Ghaffarkhah, A.A. Isari, M. Panahi-Sarmad, F. Jiang, O.J. Rojas, S. Wuttke, M. Dincă, M. Arjmand, Adv. Mater. 37(2025) 2411617, https://doi.org/10.1002/adma.202411617.S.A. Hashemi, A. Ghaffarkhah, A.A. Isari, M. Panahi-Sarmad, F. Jiang, O.J. Rojas, S. Wuttke, M. Dincă, M. Arjmand, Adv. Mater. 37(2025) 2411617, https://doi.org/10.1002/adma.202411617.
81. [81]
  Y. Wu, H. Lv, X. Wu, Chin. J. Struct. Chem. 43(2024) 100375, https://doi.org/10.1016/j.cjsc.2024.100375.Y. Wu, H. Lv, X. Wu, Chin. J. Struct. Chem. 43(2024) 100375, https://doi.org/10.1016/j.cjsc.2024.100375.
82. [82]
  L. Geng, W.-H. Fang, Chin. J. Struct. Chem. 45(2026) 100746, https://doi.org/10.1016/j.cjsc.2025.100746.L. Geng, W.-H. Fang, Chin. J. Struct. Chem. 45(2026) 100746, https://doi.org/10.1016/j.cjsc.2025.100746.

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: 1

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

通过电子给体酚羟基调控芘-COFs的反键轨道占据以促进光催化产氢

通讯作者: 王中辽,E-mail:wangzl@chnu.edu.cn; 张美玉,E-mail:zhangmeiyu@lcu.edu.cn; 张金峰,E-mail:jfzhang@chnu.edu.cn

English

Tuning antibonding-orbital occupancy in pyrene-COFs via electron-donating phenolic -OH for boosted photocatalytic H₂ evolution

Corresponding author: Zhongliao Wang, ; Meiyu Zhang, ; Jinfeng Zhang,

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

通过电子给体酚羟基调控芘-COFs的反键轨道占据以促进光催化产氢

通讯作者: 王中辽,E-mail:wangzl@chnu.edu.cn; 张美玉,E-mail:zhangmeiyu@lcu.edu.cn; 张金峰,E-mail:jfzhang@chnu.edu.cn

English

Tuning antibonding-orbital occupancy in pyrene-COFs via electron-donating phenolic -OH for boosted photocatalytic H2 evolution

Corresponding author: Zhongliao Wang, ; Meiyu Zhang, ; Jinfeng Zhang,

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

文章相关

通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

Tuning antibonding-orbital occupancy in pyrene-COFs via electron-donating phenolic -OH for boosted photocatalytic H₂ evolution

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs