自光敏金属配合物用于光催化析氢

doi:10.1016/S1872-2067(26)65050-4

催化学报

• • 下一篇

自光敏金属配合物用于光催化析氢

马明宇^a,1, 刘棕阳^a,1, 袁阔^a,1, 刘哲源^b,1, 王嘉新^a, 林清清^b, 钟地长^a,*, 鲁统部^a,*

^a天津理工大学材料科学与工程学院, 新能源材料与低碳技术研究院, 天津 300384;
^b福州大学材料科学与工程学院, 先进材料技术国际(港澳台)联合实验室, 先进材料技术重点实验室, 福建福州 350108

收稿日期:2025-09-30 接受日期:2025-09-30
通讯作者: *电子信箱: dczhong@email.tjut.edu.cn (钟地长), lutongbu@tjut.edu.cn (鲁统部).
作者简介:¹共同第一作者.
基金资助:
国家自然科学基金(22571228, 22531007, 22271218, 22205162, 22575173); 天津市自然科学基金重点项目(24JCZDJC00220, 25JCQNJC00150).

Self-photosensitizing metal complexes for photocatalytic hydrogen evolution

Mingyu Ma^a,1, Zongyang Liu^a,1, Kuo Yuan^a,1, Zheyuan Liu^b,1, Jiaxin Wang^a, Qingqing Lin^b, Di-Chang Zhong^a,*, Tong-Bu Lu^a,*

^aInstitute for New Energy Materials and Low Carbon Technologies, School of Materials Science and Engineering, Tianjin University of Technology, Tianjin 300384, China;
^bKey Laboratory of Advanced Materials Technologies, International (Hong Kong Macao and Taiwan) Joint Laboratory on Advanced Materials Technologies, School of Materials Science and Engineering, Fuzhou University, Fuzhou 350108, Fujian, China

Received:2025-09-30 Accepted:2025-09-30
Contact: *E-mail: dczhong@email.tjut.edu.cn (D.-C. Zhong), lutongbu@tjut.edu.cn (T.-B. Lu).
About author:¹Contributed equally to this work.
Supported by:
National Natural Science Foundation of China (22571228, 22531007, 22271218, 22205162, 22575173) and Tianjin Natural Science Foundation (24JCZDJC00220, 25JCQNJC00150).

摘要/Abstract

摘要： 化石能源的过度消耗导致了全球变暖、环境污染和能源危机等一系列问题, 开发绿色清洁能源已成为当下的迫切需求. 氢能具有燃烧产物单一、能量密度高等优势, 被视为可持续能源体系的重要组成部分, 其中光催化析氢手段因其利用太阳能驱动、过程温和且环境友好而受到广泛关注. 金属配合物因结构明确、可设计性强, 在光催化析氢研究中展现出巨大潜力. 但现有研究主要集中于通过调控单核金属中心的配位环境来提高催化活性, 提高活性, 而关于通过构筑双核金属位点产生协同效应以提升光催化性能的研究较为缺乏. 此外, 传统体系普遍依赖贵金属光敏剂(如Ru, Rh, Os配合物)提供光生电子, 催化剂与光敏剂通过物理混合实现电子转移, 界面相互作用较弱, 导致电荷分离与传递效率受限, 从而限制了整体光催化性能的进一步提升. 因此, 开发一种兼具光敏功能与高效双核金属催化中心, 且能促进快速电荷转移的分子光催化体系, 对于构筑高性能光催化析氢催化剂具有重要意义.
本研究基于分子催化剂结构可设计的优势, 通过共价键将光敏基元与双核金属中心精确耦合, 成功构建了一种自光敏化芘修饰的双核钴(II)分子催化剂(Co₂(pyrene-L)₂). 核磁、质谱、红外和粉末衍射等表征结果均证明了目标结构的成功制备. 得益于共价连接的芘基光敏中心, Co₂(pyrene-L)₂可在无任何外加贵金属光敏剂的条件下实现高效光催化产氢, 充分发挥了分子层面精准整合光敏与催化功能的策略优势. 光催化实验表明, Co₂(pyrene-L)₂的产氢活性是物理混合样品Co₂L₂&pyrene的三倍以上, 同时其活性也优于使用贵金属光敏剂[Ru(phen)₃]²⁺的对照体系. 进一步与单核光催化剂Co(pyrene-L)₂比较, Co₂(pyrene-L)₂的催化性能提升近十倍, 证明双核金属中心之间存在显著的协同催化效应. 机理研究表明, 芘基团可在光照下产生光生电子并高效地向双核Co(II)中心传递电子, 使Co₂(pyrene-L)₂光催化剂完成对光敏、光还原与光氧化功能的多重整合, 从而大幅提升体系的电子分离与传输效率. 时间分辨荧光寿命测试表明, Co₂(pyrene-L)₂的平均荧光寿命(τ_ave = 0.112 ns)相比物理混合样品Co₂L₂&pyrene (11.609 ns)大幅缩短, 表明其激发态发生了更快速的猝灭过程. 这清晰说明芘光敏基元与双核Co₂L₂之间的共价连接可有效加速电子转移. 同时, 密度泛函理论与激发态电子分布计算进一步揭示Co₂(pyrene-L)₂中电子由芘光敏中心向双核金属中心迁移的优势通道, 证明了共价连接策略对电荷分离的显著促进作用.
综上, 本工作通过分子层面上的共价集成策略, 实现了光敏与双核催化中心的结构一体化设计, 显著提升了电子转移效率和光催化析氢性能, 为设计高性能分子催化剂开辟了新途径.

关键词: 双核金属配合物, 光催化析氢, 协同催化, 自光敏, 芘

Abstract: Combining organic photosensitive center with dinuclear-metal catalytic center through covalent bonds to synthesize supramolecular catalysts for photocatalytic hydrogen evolution is a cost-efficient approach to convert solar to hydrogen energy, while it has been rarely explored. Herein, we constructed a self-photosensitizing pyrene-decorated dinuclear cobalt(II) molecular photocatalyst [Co₂(pyrene-L)₂] via covalent bonds, which can accelerate photogenerated electron transfer from pyrene center to dinuclear cobalt(II) center, achieving efficiently photocatalytic hydrogen evolution in the absence of any noble metal photosensitizers. The photocatalytic activity of Co₂(pyrene-L)₂ is more than 3-fold over that of the physically mixed sample. Moreover, owing to the synergistic effect of dinuclear cobalt(II) centers, the activity of Co₂(pyrene-L)₂ is 10-fold higher than that of mononuclear counterpart (Co(pyrene-L)₂). As the first example of self-photosensitizing pyrene-decorated dinuclear metal molecular catalyst, it not only features multi-functions of photosensitivity, photoreduction and photooxidation, but also possesses synergistic dinuclear metal centers to improve catalytic activity, which gives new insights for researchers in designing high-performance photocatalysts for hydrogen evolution.

Key words: Dinuclear metal complex, Photocatalytic hydrogen evolution, Synergistic catalysis, Self-photosensitizing, Pyrene

马明宇, 刘棕阳, 袁阔, 刘哲源, 王嘉新, 林清清, 钟地长, 鲁统部. 自光敏金属配合物用于光催化析氢[J]. 催化学报, DOI: 10.1016/S1872-2067(26)65050-4.

Mingyu Ma, Zongyang Liu, Kuo Yuan, Zheyuan Liu, Jiaxin Wang, Qingqing Lin, Di-Chang Zhong, Tong-Bu Lu. Self-photosensitizing metal complexes for photocatalytic hydrogen evolution[J]. Chinese Journal of Catalysis, DOI: 10.1016/S1872-2067(26)65050-4.

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自光敏金属配合物用于光催化析氢

Self-photosensitizing metal complexes for photocatalytic hydrogen evolution

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