Efficient catalytic combustion of propane at low temperature based on ignition effect caused by amorphous atomic-layer Pt clusters

丙烷 无定形固体 燃烧 活化能 催化作用 氧气 化学工程 铂金 分析化学(期刊) 无机化学 化学 物理化学 结晶学 有机化学 工程类
作者
Yangfei Fang,Kaijie Liu,Xin Shen,Daying Zheng,Xiaohui Chen,Bin Hu,Huaiyuan Wang,Mengyao Bian,Liwei Sun,Haijiao Xie,Yibo Zhang,Xiangguang Yang
出处
期刊:Fuel [Elsevier]
卷期号:367: 131509-131509 被引量:4
标识
DOI:10.1016/j.fuel.2024.131509
摘要

Developing highly active catalysts for hydrocarbon combustion at low temperatures is paramount but yet challenging. The crystal form of carrier and the dispersion degree of active species have great influence on propane combustion catalysts, but its internal mechanism is still unclear. In this study, the amorphous atomic-layer Pt clusters (AL) and Pt single atoms (SA) on TiO2 with various crystal phases were prepared and used as propane combustion catalysts, where the as-synthesized Pt/a-TiO2 catalyst with atomic-layer Pt clusters exhibited better catalytic performance. The Pt/a-TiO2-AL could achieve a 90 % propane conversion (T90) at 230 °C, with the highest reaction rate (39.57 × 10−7 mol g−1 s−1) and TOF value (7.72 × 10−2 s−1) at 240 °C. Kinetic studies showed that oxygen had a lower inhibitory effect on Pt/a-TiO2-AL compared to that on the Pt/p-TiO2-AL and Pt/r-TiO2-AL catalysts; simultaneously, the Pt/a-TiO2-AL catalyst presented lower apparent activation energy compared with Pt/a-TiO2-SA. DFT results showed that atomic-layer Pt clusters on TiO2 had the lower formation energy of oxygen vacancy than Pt single atoms due to the synergistic effect between adjacent exposed Pt atoms in the fully exposed atomic-layer Pt clusters, which had a higher activation capacity for oxygen and thus accelerated propane combustion through the ignition effect (rapid activation of oxygen and rapid combustion of propane). Our primary results provide a promising approach for the creation of high-efficiency Pt-based catalysts, specifically tailored for the catalytic combustion of volatile organic compounds (VOCs).

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