Component regulation in novel La-Co-O-C composite catalyst for boosted redox reactions and enhanced thermal stability in methane combustion

催化作用 化学 甲烷 X射线光电子能谱 解吸 吸附 活化能 热稳定性 氧气 傅里叶变换红外光谱 热脱附光谱法 氧化还原 无机化学 化学工程 物理化学 有机化学 工程类
作者
Peiqi Chu,Saifei Wang,Yi Zhang,Shiguang Zhao,Yahan Wang,Jiguang Deng,Erhong Duan
出处
期刊:Journal of Environmental Sciences-china [Elsevier BV]
卷期号:126: 459-469 被引量:11
标识
DOI:10.1016/j.jes.2022.04.002
摘要

• A novel La-Co-O-C composite (LC-C) is synthesized by co-hydrothermal route with oxides and glycerol. • The catalytic performance is optimized via component regulation for methane oxidation. • The catalytic mechanism of the composite changes from “Two-term” to “Rideal-Eley” with addition of Co. • The thermal stability of the La 2 O 2 CO 3 species is enhanced by component regulation. A novel La-Co-O-C (LC-C) composites were prepared via a facile co-hydrothermal route with oxides and glycerol and further optimized for methane catalytic activity and thermal stability via component regulation. It was demonstrated that Co 3 O 4 phase was the main component in regulation. The combined results of X-ray photoelectron spectroscopy (XPS), temperature-programmed desorption of oxygen (O 2 -TPD), temperature-programmed reduction of hydrogen (H 2 -TPR), temperature-programmed desorption of ammonia/carbon dioxide (NH 3 /CO 2 -TPD) revealed that component regulation led to more oxygen vacancies and exposure of surface Co 2+ , lower surface basicity and optimized acidity, which were beneficial for adsorption of active oxygen species and activation of methane molecules, resulting in the excellent catalytic oxidation performance. Especially, the (3.5)LC-C (3.5 is Co-to-La molar ratio) showed the optimum activity and the T 50 and T 90 (the temperature at which the CH 4 conversion rate was 50% and 90%, respectively) were 318 and 367°C, respectively. Using theoretical calculations and in situ diffuse reflection infrared Fourier transform spectroscopy characterization, it was also found that the catalytic mechanism changes from the “Rideal-Eley” mechanism to the “Two-term” mechanism depending on the temperature windows in which the reaction takes place. Besides, the use of the “Flynn-Wall-Ozawa” model in thermoanalytical kinetics revealed that component regulation simultaneously optimized the decomposition activation energy, further expanding the application scope of carbon-containing composites.
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