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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

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

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引用本文: 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 shu
Citation:  Chongbei Wu,  Feihong Chu,  Pengfei Kong,  Yuanxin Dong,  Gege Wang,  Lefan Wang,  Haitao Li,  Meixin Zhang,  Lifang Feng,  Xuan Li,  Jizhou Jiang. 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]. Acta Physico-Chimica Sinica, 2026, 42(11): 100385. doi: 10.1016/j.actphy.2026.100385 shu

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

  • 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

    • 通讯作者: 江吉周,E-mail:027wit@163.com
  • 基金项目:

    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。

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-Nx)。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。

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