二面角工程调控四嗪COFs层间作用强化电荷转移促进光合成H2O2

doi:10.1016/j.actphy.2026.100385

物理化学学报 >> 2026, Vol. 42 >> Issue (11): 100385.doi: 10.1016/j.actphy.2026.100385

所属专题： 2026年度《物理化学学报》“新锐科学家”专刊

论文上一篇

二面角工程调控四嗪COFs层间作用强化电荷转移促进光合成H₂O₂

吴崇备¹, 楚飞鸿¹, 孔鹏飞¹, 董原欣¹, 王格格¹, 王乐凡¹, 李海涛¹, 张美鑫¹, 冯丽芳¹, 李璇¹, 江吉周^2,3

1 河北科技工程职业技术大学, 河北省高校工业节能与污染防治应用技术研发中心, 河北省人机环境热控制技术与装备重点实验室, 河北邢台 054000, 河北省, 中国;
2 武汉工程大学材料科学与工程学院, 磷矿及其共伴生资源绿色高效开发利用全国重点实验室, 磷资源开发利用教育部工程研究中心, 绿色化工过程教育部重点实验室, 等离子体化学与先进材料湖北省重点实验室, 新型催化材料湖北省工程研究中心, 湖北武汉 430205;
3 FTSCI先进化学与新材料工业技术研究院, 湖北武汉 430080

收稿日期:2026-06-29 修回日期:2026-08-09 录用日期:2026-08-09 发布日期:2026-09-29
通讯作者: 江吉周 E-mail:027wit@163.com
基金资助:
本工作得到了国家自然科学基金(22502052、12504202)，河北省教育厅科学研究项目(BJ2025105)，湖北省教育厅科研计划重点项目(D20241501)以及邢台市科技计划(2025ZC271、2025ZC270)的资助。飞秒时间分辨瞬态吸收光谱在中国科学院物理研究所陈海龙和翁羽翔实验室完成。我们感谢王专研究员在样品制备和TAS数据采集方面的帮助。

Interlayer interaction modulation via dihedral angle engineering in tetrazine COFs boosts charge transfer for photocatalytic H₂O₂ production

Chongbei Wu¹, Feihong Chu¹, Pengfei Kong¹, Yuanxin Dong¹, Gege Wang¹, Lefan Wang¹, Haitao Li¹, Meixin Zhang¹, Lifang Feng¹, Xuan Li¹, Jizhou Jiang^2,3

1 Hebei Center for Industrial Energy-Saving and Pollution Control Research, Hebei Key Laboratory of Man-Machine Environmental Thermal Control Technology and Equipment, Hebei Vocational University of Technology and Engineering, Xingtai 054000, Hebei Province, China;
2 School of Materials Science and Engineering, State Key Laboratory of Green and Efficient Development of Phosphorus Resources, Engineering Research Center of Phosphorus Resources Development and Utilization of Ministry of Education, Key Laboratory of Green Chemical Engineering Process of Ministry of Education, Hubei Key Laboratory of Plasma Chemistry and Advanced Materials, Novel Catalytic Materials of Hubei Engineering Research Center, Wuhan Institute of Technology, Wuhan 430205, Hubei Province, China;
3 FTSCI Institute of Industrial Technology for Advanced Chemical and New Materials, Wuhan 430080, Hubei Province, China

Received:2026-06-29 Revised:2026-08-09 Accepted:2026-08-09 Published:2026-09-29
Contact: Jizhou Jiang E-mail:027wit@163.com

1. 2026.100385-ACTPHY-D-26-00451-51p-2# SI.pdf(4138KB)

摘要/Abstract

摘要： 共价有机框架(COFs)在太阳能驱动过氧化氢(H₂O₂)光合作用中展现出潜力，但受限于层间电荷传输效率低下。本研究通过空间位阻产生的非共价相互作用，逐步用氮原子替代三苯基芳烃平台中心芳环上的交替碳原子，从而设计并合成了一系列基于四嗪的COFs (Tz-COF-N_x)。结果表明，随着COFs骨架中氮原子数量的增加，相邻芳环之间的二面角逐渐减小。增强的层间π-π相互作用缩短了层间电子迁移距离，并显著提高了光生电荷载流子的分离和迁移效率。层间电子转移数遵循以下趋势：Tz-COF-N₃ (0.021 e^-) > Tz-COF-N₂ (0.011 e^-) > Tz-COF-N₁ (0.006 e^-) > Tz-COF-N₀ (0.001 e^-)。因此，Tz-COF-N₃在纯水中实现了6316.4 μmol g^-1 h^-1的光催化H₂O₂产率，是苯-四嗪COF (Tz-COF-N₀)的5.3倍。本研究通过调节空间构型以优化层间相互作用并促进层间电荷传输，为设计高效的COF基光催化剂提供了一种可行策略。

关键词: 共价有机框架, 光催化H₂O₂生产, 层间电子转移, 二面角

Abstract: Covalent organic frameworks (COFs) show promise for solar-driven hydrogen peroxide (H₂O₂) photosynthesis, but are limited by inefficient interlayer charge transport. Here, this study leverages non-covalent interactions arising from steric hindrance to gradually replace alternating C atoms in the central aryl ring of a triphenylarene platform with N atoms, thereby designing and synthesizing a series of tetrazine-based COFs (Tz-COF-N_x). The results show that as the number of N atoms in the COFs backbone increases, the dihedral angle between adjacent aromatic rings progressively decreases. The strengthened interlayer π-π interactions shorten the electron migration distance between layers and significantly improve the separation and migration efficiency of photogenerated charge carriers. The interlayer electron transfer numbers follow the trend: Tz-COF-N₃ (0.021 e^-) > Tz-COF-N₂ (0.011 e^-) > Tz-COF-N₁ (0.006 e^-) > Tz-COF-N₀ (0.001 e^-). Consequently, Tz-COF-N₃ achieves a photocatalytic H₂O₂ production rate of 6316.4 μmol g^-1 h^-1 in pure water, which is 5.3 times higher than that of the benzene-tetrazine COF (Tz-COF-N₀). This study provides a feasible strategy for designing efficient COF-based photocatalysts by tuning the spatial configuration to optimize interlayer interactions and promote interlayer charge transport.

Key words: Covalent organic frameworks, Photocatalytic H₂O₂ production, Interlayer electron transfer, Dihedral angle

吴崇备, 楚飞鸿, 孔鹏飞, 董原欣, 王格格, 王乐凡, 李海涛, 张美鑫, 冯丽芳, 李璇, 江吉周. 二面角工程调控四嗪COFs层间作用强化电荷转移促进光合成H₂O₂[J]. 物理化学学报, 2026, 42(11), 100385. doi: 10.1016/j.actphy.2026.100385

Chongbei Wu, Feihong Chu, Pengfei Kong, Yuanxin Dong, Gege Wang, Lefan Wang, Haitao Li, Meixin Zhang, Lifang Feng, Xuan Li, Jizhou Jiang. Interlayer interaction modulation via dihedral angle engineering in tetrazine COFs boosts charge transfer for photocatalytic H₂O₂ production[J]. Acta Phys. -Chim. Sin. 2026, 42(11), 100385. doi: 10.1016/j.actphy.2026.100385

链接本文: https://www.whxb.pku.edu.cn/CN/10.1016/j.actphy.2026.100385

https://www.whxb.pku.edu.cn/CN/Y2026/V42/I11/100385

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二面角工程调控四嗪COFs层间作用强化电荷转移促进光合成H₂O₂

Interlayer interaction modulation via dihedral angle engineering in tetrazine COFs boosts charge transfer for photocatalytic H₂O₂ production

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