Tian Zhengbin, Wang Wenquan, Dong Chao, Deng Xiaohui, Wang Guang-Hui
Qingdao Institute of Bioenergy and Bioprocess Technology, Chinese Academy of Sciences, Qingdao 266101, China.
Shandong Energy Institute, Qingdao 266101, China.
ACS Nano. 2023 Feb 28;17(4):3889-3900. doi: 10.1021/acsnano.2c12168. Epub 2023 Feb 15.
Metal nanoparticles confined in porous carbon materials have been widely used in various heterogeneous catalytic processes due to their enhanced activity and stability. However, fabrication of such catalysts in a facile and scalable way remains challenging. Herein, we report a general and scalable thiol-assisted strategy to synthesize sulfur-doped mono-/bi-/trimetallic nanoparticles confined in mesoporous carbon (S-M@MC, M = Pt, Pd, Rh, Co, Zn, etc.), involving only two synthetic steps, i.e., a hydrothermal process and pyrolysis. The strategy is based on coordination chemistry and hydro-phobic interaction that the metal precursors coordinated with the hydrophobic thiol ligands are located at the hydrophobic core of micelles, in situ confined in the hydrothermally prepared mesostructured polymer, and then converted into sulfur-doped metal nanoparticles confined in MC after pyrolysis. It is demonstrated that the S-PtCo@MC exhibits enhanced catalytic activity and improved durability toward acidic hydrogen evolution reaction due to the confinement effect and S-doping.
由于其活性和稳定性增强，负载于多孔碳材料中的金属纳米颗粒已广泛应用于各种多相催化过程。然而，以简便且可扩展的方式制备此类催化剂仍然具有挑战性。在此，我们报道了一种通用且可扩展的硫醇辅助策略，用于合成负载于介孔碳中的硫掺杂单/双/三金属纳米颗粒（S-M@MC，M = Pt、Pd、Rh、Co、Zn等），该策略仅涉及两个合成步骤，即水热过程和热解。该策略基于配位化学和疏水相互作用，金属前驱体与疏水硫醇配体配位后位于胶束的疏水核心，原位负载于水热制备的介孔结构聚合物中，然后在热解后转化为负载于介孔碳中的硫掺杂金属纳米颗粒。结果表明，由于限域效应和硫掺杂，S-PtCo@MC对酸性析氢反应表现出增强的催化活性和更高的耐久性。
