催化作用
甲烷
催化燃烧
化学
燃烧
氧气
Atom(片上系统)
钯
化学工程
无机化学
物理化学
有机化学
计算机科学
工程类
嵌入式系统
作者
Jinshu Tian,Ran Kong,Zhi Wang,Ling Fang,Tianyao He,Dong Jiang,Honggen Peng,Tulai Sun,Yihan Zhu,Yong Wang
标识
DOI:10.1021/acscatal.3c02167
摘要
Reducing methane emissions is crucial for mitigating global warming. Developing highly efficient catalysts for low-temperature methane combustion is of great importance. Supported single-atom catalysts (SACs) have received significant attention in this regard. However, their long-term stability and activity remain challenging. In this study, we present a method for creating a highly active and thermally stable Pd1/CeO2 catalyst by using thermal-shock synthesis (Pd1/CeO2-TS). By subjecting isolated Pd2+ ions to ultrafast shockwaves, we control their local environment, resulting in unique electronic structures and the geometry of the Pd single atoms. Compared with the single-atom Pd1/CeO2 catalyst formed through atom trapping (Pd1/CeO2-AT), Pd1/CeO2-TS showed improved activity for methane combustion with a nearly 20-fold increase in turnover frequency and reversible stability against water. This increase in activity is attributed to the presence of coordination-unsaturated Pd–O species and surface hydroxyls on ceria. These factors enhance the oxygen activity and reduce the barrier for C–H bond activation, resulting in increased catalytic performance.
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