催化作用
甲烷
催化燃烧
化学
燃烧
氧气
Atom(片上系统)
甲烷厌氧氧化
材料科学
化学工程
无机化学
光化学
物理化学
有机化学
嵌入式系统
工程类
计算机科学
作者
Jinshu Tian,Ru Kong,Zhi Wang,Ling Fang,Tianyao He,Dong Jiang,Honggen Peng,Tulai Sun,Yihan Zhu,Yong Wang
出处
期刊:ACS Catalysis
[American Chemical Society]
日期:2023-12-13
卷期号:14 (1): 183-191
被引量:24
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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