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:

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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,

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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,

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