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Constructing the Ni-O-Ce interface to enhance the activity and stability for partial oxidation of methane to syngas under high temperatures

Journal 2024 · IF 6.5 · 发表于 2024 年 5 月 12 日
作者: Yuanjie Xu,Rong Chen,Hongqiao Lin,Qian Lv,Bo Liu,Lizhi Wu,Li Tan,Yihu Dai,Xupeng Zong,Yu Tang
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摘要

Catalyst interface determines the activity and stability of partial oxidation of methane (POM) toward syngas under high temperatures crucially. Herein, Ni catalysts supported on CeO 2 were prepared under different pretreatment atmospheres to construct an optimal and robust interface. Ni/CeO 2 catalyst pretreated in H 2 (Ni/CeO 2 -H 2 ) exhibits the higher activity and the better stability than Ni/CeO 2 -Ar and Ni/CeO 2 -air catalysts. The Ni-O-Ce interfacial site in Ni/CeO 2 -H 2 catalyst shows the lower reduction temperature, indicating the enhanced H-spillover effect and enhanced oxidation resistance of Ni under POM conditions. Moreover, the XPS and in situ Raman results show that Ni/CeO 2 -H 2 contains more surface oxygen vacancies for adsorbing and activating oxygen, further contributing to the reaction activity. The in situ DRIFTS results indicate that the CH 4 could react with the lattice oxygen to form formate and carbonate, and further decompose to CO and CO 2 . These findings deepen the fundamental understanding of Ni/CeO 2 catalysts for POM reaction.

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