Atomically Dispersed Pt1–Polyoxometalate Catalysts: How Does Metal–Support Interaction Affect Stability and Hydrogenation Activity?

多金属氧酸盐 催化作用 化学 密度泛函理论 吸附 金属 氧化物 Atom(片上系统) 铂金 物理化学 分子 纳米团簇 计算化学 无机化学 结晶学 有机化学 嵌入式系统 计算机科学
作者
Bin Zhang,Geng Sun,Shipeng Ding,Hiroyuki Asakura,Jia Zhang,Philippe Sautet,Ning Yan
出处
期刊:Journal of the American Chemical Society [American Chemical Society]
卷期号:141 (20): 8185-8197 被引量:176
标识
DOI:10.1021/jacs.9b00486
摘要

Unlike nanostructured metal catalysts, supported single-atom catalysts (SACs) contain only atomically dispersed metal atoms, hinting at much more pronounced metal–support effects. Herein, we take a series of polyoxometalate-supported Pt catalysts as examples to quantitatively investigate the stability of Pt atoms on oxide supports and how the Pt–support interaction influences the catalytic performance. For this entire series, we show that the Pt atoms prefer to stay at a 4-fold hollow site of one polyoxometalate molecule and that the least adsorption energy to obtain sintering-resistant Pt SACs is 5.50 eV, which exactly matches the cohesive energy of bulk Pt metal. Further, we compared their catalytic performance in several hydrogenation reactions and simulated the reaction pathways of propene hydrogenation by density functional theory (DFT) calculations. Both experimental and theoretical approaches suggest that despite the Pt1–support interactions being different, the reaction pathways of various Pt1–polyoxometalate catalysts are very similar and their effective reaction barriers are close to each other and as low as 24 kJ/mol, indicating the possibility of obtaining SACs with improved stability without compromising activity. DFT calculations show that all reaction elementary steps take place only on the Pt atom without involving neighboring O atoms and that hydrogenation proceeds from the molecularly adsorbed H2 species. Pt SACs give a weaker H2 adsorption energy than Pt clusters or surfaces, resulting in small adsorption equilibrium constants and small apparent activation barriers, which agree between experiment and theory.
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