催化作用
纳米颗粒
材料科学
离解(化学)
金属
化学工程
星团(航天器)
粒子(生态学)
粒径
纳米技术
分子
金属颗粒
Atom(片上系统)
多孔性
原子层沉积
多相催化
活化能
化学物理
过渡金属
催化氧化
无机化学
氧化还原
化学反应
小分子
反应中间体
分子动力学
反应机理
耐久性
吸附
沉积(地质)
作者
Jiankang Zhang,Ye Ma,Ye Ma,Jiawen Yang,Dan Feng,Xinshuo Zhao,Hao Xu,Shichao Zhao,Jinshu Tian,Yanhang Ma,Yanhang Ma,Yong Qin,Jiankang Zhang,Ye Ma,Jiawen Yang,Dan Feng,Xinshuo Zhao,Hao Xu,Shichao Zhao,Jinshu Tian
出处
期刊:ACS Nano
[American Chemical Society]
日期:2025-11-15
卷期号:19 (46): 39701-39713
标识
DOI:10.1021/acsnano.5c11282
摘要
Size-dependent catalysis is a classic and yet challenging issue in heterocatalysis because it is influenced by multiple factors such as varied metal loading and potential support effects. To the best of our knowledge, size-dependent catalytic research under the same metal loadings has rarely been reported. Herein, we designed and synthesized a series of unreducible SiO2-supported Pt-based catalysts with the same metal loadings (0.3 wt %) but different particle sizes from single atom (SA), cluster to nanoparticle by combining amino group-assisted atomic layer deposition with the designed activation strategy. Their catalytic properties were probed in the archetypal CO oxidation reaction. The catalytic activity boosts prominently with increased particle size, which is well consistent with the directly observed gradual aggregation-activation process during the reaction process tracked by in situ STEM and isotope-labeled surface reaction and rationalized by theoretical calculations. The dynamic size transform and surface-confinement effect of porous SiO2 also enable the Pt catalysts to achieve ultrahigh durability (> 2160 h) under the complete oxidation of CO, which is predominantly catalyzed by Pt nanoclusters/nanoparticles through the combined Mars-van Krevelen (66%) and Langmuir-Hinshelwood (34%) mechanisms. Similar phenomena were also found in catalytic hydrogenation and H2O2-involved oxidation reactions, i.e., SAs were poorly active, and nanoclusters/nanoparticles were clearly identified as the real active species. The dissociation energy of key small molecules (H2/O2/H2O2) is correlated with the particle size and catalytic activity, which can potentially act as a descriptor for the reaction activity. The present findings will afford deeper insights for deciphering the nature of size-dependent catalysis.
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