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工程化多位点铂簇协同增强催化作用。

Engineering Multi-Site Platinum Ensembles Synergistically Boosts Catalysis.

作者信息

Dong Tao, Xiao Fei, Wu Xuanning, Ban Tao, Ji Jian, Liu Biyuan, Zhang Jiarui, Jiang Jiuxing, Zhang Dieqing, Yang Weixing, Liu Gaoyuan, Yang Xin, Huang Haibao

机构信息

School of Environmental Science and Engineering, Sun Yat-sen University, Guangzhou, 510006, China.

College of Ecology and Environment, School of Chemical Engineering and Technology, Xinjiang University, Urumqi, 830017, China.

出版信息

Adv Sci (Weinh). 2025 Apr;12(14):e2415937. doi: 10.1002/advs.202415937. Epub 2025 Feb 18.

Abstract

Engineering stable and efficient noble metal ensembles with multi-type active sites while understanding the role of each site at the atomic level remains a significant challenge in heterogeneous catalysis. Herein, a sub-nanometric Pt ensemble catalyst with a diverse array of active sites is constructed via a dual-confinement strategy, which exhibits superior activity and durability with minimal Pt loading (0.13 wt.%). Simultaneously, the roles of different Pt sites at the atomic scale are determined through in situ characterization methods and density functional theory (DFT) calculations. Specifically, Pt top sites predominantly serve as pivotal centers for O═O bond activation, whereas Pt-O-Si interfacial sites primarily govern the activation of H─OH and C─H bonds. The reactive oxygen species (O , O , and -OH) generated from O and HO activation synergistically enhance formaldehyde (HCHO) oxidation and shorten the reaction pathway. This study sheds light on a better understanding and rational design of catalyst active sites via precise synthesis of multi-site ensembles or discerning the distinct contributions of various catalytic sites.

摘要

在异相催化中,构建具有多类型活性位点的稳定高效贵金属团簇,同时在原子水平上理解每个位点的作用,仍然是一项重大挑战。在此,通过双限域策略构建了一种具有多种活性位点的亚纳米级铂团簇催化剂,该催化剂在最低铂负载量(0.13 wt.%)下表现出优异的活性和耐久性。同时,通过原位表征方法和密度泛函理论(DFT)计算确定了不同铂位点在原子尺度上的作用。具体而言,铂顶位主要作为O═O键活化的关键中心,而铂-氧-硅界面位主要控制H─OH和C─H键的活化。由O和HO活化产生的活性氧物种(O 、O 和-OH)协同增强甲醛(HCHO)氧化并缩短反应路径。这项研究通过精确合成多位点团簇或识别各种催化位点的不同贡献,为更好地理解和合理设计催化剂活性位点提供了思路。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0916/11984847/58a5e3e3e518/ADVS-12-2415937-g005.jpg

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