催化作用
尖晶石
丙烷
材料科学
纳米颗粒
活化能
兴奋剂
氧气
傅里叶变换红外光谱
密度泛函理论
分子
光化学
无机化学
物理化学
化学工程
化学
纳米技术
计算化学
有机化学
冶金
工程类
光电子学
作者
Gaoyan Xiong,Chao Feng,Hsiao‐Chien Chen,Junxi Li,Fei Jiang,Shu Tao,Yunxia Wang,Yichuan Li,Yuan Pan
出处
期刊:Small methods
[Wiley]
日期:2023-03-31
卷期号:7 (7): e2300121-e2300121
被引量:21
标识
DOI:10.1002/smtd.202300121
摘要
Abstract This study adopts a facile and effective in situ encapsulation‐oxidation strategy for constructing a coupling catalyst composed of atomically dispersed Pt‐doped Co 3 O 4 spinel nanoparticles (NPs) embedded in polyhedron frames (PFs) for robust propane total oxidation. Benefiting from the abundant oxygen vacancies and more highly valent active Co 3+ species caused by the doping of Pt atoms as well as the confinement effect, the optimized 0.2Pt‐Co 3 O 4 NPs/PFs catalyst exhibits excellent propane catalytic activity with low T 90 (184 °C), superior apparent reaction rate (21.62×10 8 (mol g cat −1 s −1 )), low apparent activation energy ( E a = 17.89 kJ mol −1 ), high turnover frequency ( 811×10 7 (mol g cat −1 s −1 )) as well as good stability. In situ diffuse reflectance infrared Fourier transform spectroscopy and density functional theory calculations indicate that the doping of Pt atoms enhances the oxygen activation ability, and decreases the energy barrier required for CH bond breaking, thus improving the deep oxidation process of the intermediate species. This study opens up new ideas for constructing coupling catalysts from atomic scale with low cost to enhance the activation of oxygen molecules and the deep oxidation of linear short chain alkanes at low temperature.
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