共价有机框架的双氧气还原中心促进光催化合成H2O2

doi:10.1016/S1872-2067(25)64740-1

催化学报 ›› 2025, Vol. 74: 329-340.DOI: 10.1016/S1872-2067(25)64740-1

共价有机框架的双氧气还原中心促进光催化合成H₂O₂

吴崇备^a^,¹, 楚飞鸿^a^,¹, 郝永超^c^,¹, 李璇^a, 贾晓月^a, 孙伊钒^a, 谷佳璇^a, 加鹏飞^a, 王傲冰^a, 江吉周^b^,^*()

^a河北科技工程职业技术大学, 河北省高校工业节能降耗与污染防治应用技术研发中心, 河北邢台 054000
^b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, 新型催化材料湖北省工程研究中心, 湖北武汉 430205
^c邢台学院化学工程与生物技术学院, 河北邢台 054000

收稿日期:2025-02-06 接受日期:2025-03-31 出版日期:2025-07-18 发布日期:2025-07-20
通讯作者: *电子信箱: 027wit@163.com (江吉周).
作者简介:¹共同第一作者.
基金资助:
河北省自然科学基金(B2023108012);河北省自然科学基金(A2023108002);河北省教育厅青年拔尖人才项目(BJK2024137);国家自然科学基金(62004143);湖北省重点研发计划(2022BAA084)

Dual O₂ reduction centers of COFs boosting H₂O₂ photosynthesis

Chongbei Wu^a^,¹, Feihong Chu^a^,¹, Yongchao Hao^c^,¹, Xuan Li^a, Xiaoyue Jia^a, Yifan Sun^a, Jiaxuan Gu^a, Pengfei Jia^a, Aobing Wang^a, Jizhou Jiang^b^,^*()

^aHebei 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, China
^bSchool 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, Wuhan Institute of Technology, Wuhan 430205, Hubei, China
^cSchool of Chemical Engineering and Biotechnology, Xingtai University, Xingtai, 054000, Hebei, China

Received:2025-02-06 Accepted:2025-03-31 Online:2025-07-18 Published:2025-07-20
Contact: *E-mail: 027wit@163.com (J. Jiang).
About author:¹Contributed equally to this work.
Supported by:
Hebei Province Natural Science Foundation(B2023108012);Hebei Province Natural Science Foundation(A2023108002);Science Research Project of Hebei Education Department(BJK2024137);National Natural Science Foundation of China(62004143);Key R&D Program of Hubei Province(2022BAA084)

摘要/Abstract

摘要：

过氧化氢(H₂O₂)广泛应用于造纸、电子制造和废水处理等领域. 传统蒽醌氧化法生产H₂O₂存在高能耗、环境污染等问题. 相比之下, 利用太阳能、水和氧气作为原料的光催化生产H₂O₂已成为一种有前途的可持续替代方案. 目前, 石墨相氮化碳(g-C₃N₄)、共价有机框架(COFs)等无金属有机半导体材料因其可调的分子结构设计, 展现出高效的光催化性能. 尽管g-C₃N₄在光合成H₂O₂中表现优异, 但其缓慢的电荷动力学和有限的O₂吸附活化位点限制了催化性能的提升. 因此, 利用COFs的分子结构可调性, 构筑具有高效的电荷转移动力学和双O₂吸附活化位点的COFs光催化剂以实现高效光催化合成H₂O₂是本文的主要研究思路.

基于COFs分子结构中偶极矩的理论预测表明, 引入吡嗪单元显著增强电荷迁移, 促进光生电荷的富集, 从而推动双位点两电子氧还原反应(2e^- ORR). 本文通过分子结构设计, 成功引入极性吡嗪单元, 构筑了三嗪-吡嗪交替排列的COFs光催化剂(TTDN-COFs), 其光催化合成H₂O₂的生成速率最高达到2757.6 µmol h^-1 g^-1. 理论计算和飞秒瞬态吸收光谱测试结果表明, 吡嗪单元的引入显著增强了材料的极化效应, 促进了光生载流子的分离, 并优化了电荷传输. 通过密度泛函理论(DFT)和时间依赖的密度泛函理论(TDDFT)计算得到的D-index进一步揭示了吡嗪单元引起的局部电荷极化效应, 显著提高了载流子分离与迁移能力. DFT计算表明, 三嗪和吡嗪位点不仅能够有效提高O₂的吸附能力, 而且促进了光生电子在三嗪和吡嗪位点的富集, 从而实现了O₂吸附的活化并构建了双位点反应机制. 结合原位红外光谱和DFT理论计算对催化机理分析, 吡嗪单元的引入有效降低了O₂的活化反应能垒, 促进了三嗪和吡嗪位点上1,4-内过氧化物活性中间体的生成, 进一步提高了2e^- ORR反应动力学和光催化效率. 以上结果表明, 功能基团介导的极化工程在开发基于COFs的H₂O₂光合反应中具有巨大潜力.

综上, 本研究在分子层面设计高性能无金属共价有机框架光催化剂提供了新思路, 并具有在人工光合作用和环境修复中的潜在应用.

关键词: 光催化合成过氧化氢, 三嗪-吡嗪基共价有机框架, 双活性位点, 极化效应

Abstract:

The two-electron oxygen reduction reaction (ORR) for H₂O₂ photosynthesis is often hindered by sluggish charge kinetics and a limited number of activation sites. Theoretical predictions based on dipole moment analysis indicate that introducing pyrazine units enhances charge migration, leading to increased accumulation of photoinduced electrons on these units, thereby facilitating the two-site, two-electron ORR. Inspired by these theoretical insights, this work designed and fabricated a triazine-pyrazine-based covalent organic framework materials (TTDN-COFs) for H₂O₂ photosynthesis via a polarity-functionalization strategy. The TTDN-COFs demonstrate a significant improvement in the photocatalytic H₂O₂ production rate, reaching 2757.6 μmol h^-1 g^-1 in pure water-3.2 times higher than that of the triazine-based COFs (TTPH-COFs). Experimental results and theoretical calculations confirm that the incorporation of pyrazine units not only enhances polarization, promoting the separation and migration of charge carriers, but also facilitates the formation of endoperoxide at both the triazine and pyrazine units. The dual adsorption activation sites lower the activation energy barrier for O₂, thereby accelerating the overall reaction kinetics. These findings highlight the potential of functional-group-mediated polarization engineering as a promising strategy for developing COFs-based H₂O₂ photosynthesis with dual activation sites.

Key words: H₂O₂ photosynthesis, Triazine-pyrazine-based COFs, Dual activation sites, Polarization

吴崇备, 楚飞鸿, 郝永超, 李璇, 贾晓月, 孙伊钒, 谷佳璇, 加鹏飞, 王傲冰, 江吉周. 共价有机框架的双氧气还原中心促进光催化合成H₂O₂[J]. 催化学报, 2025, 74: 329-340.

Chongbei Wu, Feihong Chu, Yongchao Hao, Xuan Li, Xiaoyue Jia, Yifan Sun, Jiaxuan Gu, Pengfei Jia, Aobing Wang, Jizhou Jiang. Dual O₂ reduction centers of COFs boosting H₂O₂ photosynthesis[J]. Chinese Journal of Catalysis, 2025, 74: 329-340.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(25)64740-1

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图/表 8

Fig. 1. (a) The synthetic routes schematics and DFT calculated dipole moments of TTPH-COFs, TTPN-COFs and TTDN-COFs. The D index (D index refers to the distance between the two centers of mass of electrons or holes) (b) and the O2 molecule adsorption energies (c) of COFs.

Fig. 2. FT-IR spectra (a), and solid-state 13C NMR spectra (b) of COFs. UV-vis absorption spectra (c) and electronic band structure (d) of COFs.

Fig. 3. (a) Time-dependent formation of H2O2 under O2-saturated pure water for COFs under illumination of a 300W Xe lamp. (b) Wavelength-dependent H2O2 yield and (c) the stability toward producing H2O2 of TTDN-COFs. (d) The H2O2 production performance of COFs under different sacrificial agent conditions. (e) The EPR spectra of TTDN-COFs recorded in ultrapure water under O2 atmosphere. (f) Photocatalytic yield of ?O2- by COFs detected by NBT method.

Fig. 4. The SPV spectroscopy (a), PL spectroscopy (b), and time-resolved PL decay measurements (c) of COFs. (d) Femtosecond transient absorption spectra of TTDN-COFs and TTPH-COFs. (e) Time profiles of normalized transient absorption kinetics of at 455 nm of TTDN-COFs and 515 nm of TTPH-COFs.

Fig. 5. (a) In-situ XPS spectra of N 1s spectra in TTDN-COFs photocatalysts. (b,c) In-situ DRIFT spectra of TTDN-COFs.

Fig. 6. PDOS plots of C 2p, N 2p in TTPH-COFs (a), TTPN-COFs (b) and TTDN-COFs (c). TDDFT-calculated absorption spectra for EDD of TTPH-COFs (d), TTPN-COFs (e) and TTDN-COFs (f).

Fig. 7. Electron and hole distribution for TTPH-COFs (a,d), TTPN-COFs (b,e), and TTDN-COFs (c,f).

Fig. 8. The weight difference index of fragments in (a) TTDN-COF, (b) TTPN-COF and (c) TTDN-COF. Calculated free energy diagrams of 2e- ORR pathway toward H2O2 production on different activation sites: (d) triazine sites in TTPH-COF, (e) pyrazine sites in TTPN-COF, (f) triazine sites in TTDN-COF and (g) pyrazine sites in TTDN-COF.

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共价有机框架的双氧气还原中心促进光催化合成H₂O₂

Dual O₂ reduction centers of COFs boosting H₂O₂ photosynthesis

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