Zhong Shilong, Shi Haixian, Xiao Chengwei, Gu Xirui, Wu Jing, Lu Shaolin, Yuan Zhongke, Yang Yuzhao, Yu Dingshan, Chen Xudong
School of Chemical Engineering and Light Industry, Guangdong University of Technology, Guangzhou 510006, China; Guangdong Laboratory of Chemistry and Chemical Engineering Jieyang Center, Jieyang 515200, China.
Key Laboratory for Polymeric Composite and Functional Materials of Ministry of Education, Guangdong Engineering Technology Research Center for High-performance Organic and Polymer Photoelectric Functional Films, School of Chemistry, Sun Yat-sen University, Guangzhou 510275, China.
J Colloid Interface Sci. 2025 Feb;679(Pt B):91-101. doi: 10.1016/j.jcis.2024.10.092. Epub 2024 Oct 18.
Constructing single-atom catalysts (SACs) using organic porous framework materials as supports presents a promising approach for developing highly efficient photocatalysts for hydrogen evolution. However, the fabrication of SACs that are both highly stable and active poses a significant challenge, particularly in the precise anchoring of metal single atoms. In this study, we utilized 1,3,6,8-tetra (p-methyl benzoate) pyrene as a ligand to synthesize pyrene-based hydrogen-bonded organic frameworks (denoted as PFC-1) through a self-assembly approach. Subsequently, a liquid-phase photoreduction process was employed to deposit noble metal platinum (Pt) onto PFC-1, resulting in the fabrication of SACs (PFC-1@Pt). Characterization results confirmed that Pt existed in a monatomic state, anchored through PtC and PtO coordination bonds with PFC-1. Serving as electron capture and separation centers, the Pt single atoms effectively suppressed electron-hole recombination, thereby prolonging carrier lifetimes. Consequently, the PFC-1@Pt SAC exhibited efficient hydrogen evolution performance with a rate of 2202.5 μmol g h and maintained photocatalytic activity for over 40 h. Our findings provide a systematic approach for developing efficient and stable SACs based on HOFs, expanding the potential applications of HOF materials in photocatalysis.
使用有机多孔框架材料作为载体构建单原子催化剂（SACs），为开发高效的析氢光催化剂提供了一种很有前景的方法。然而，制备既高度稳定又具有活性的SACs面临重大挑战，特别是在金属单原子的精确锚定方面。在本研究中，我们利用1,3,6,8-四（对甲基苯甲酸酯）芘作为配体，通过自组装方法合成了芘基氢键有机框架（记为PFC-1）。随后，采用液相光还原过程将贵金属铂（Pt）沉积到PFC-1上，从而制备出SACs（PFC-1@Pt）。表征结果证实，Pt以单原子状态存在，通过PtC和PtO配位键与PFC-1锚定。作为电子捕获和分离中心，Pt单原子有效地抑制了电子-空穴复合，从而延长了载流子寿命。因此，PFC-1@Pt SAC表现出高效的析氢性能，速率为2202.5 μmol g h，并且保持光催化活性超过40小时。我们的研究结果为基于氢键有机框架开发高效稳定的SACs提供了一种系统方法，扩展了氢键有机框架材料在光催化中的潜在应用。
