Oxygen vacancies enriched Ni-Co/SiO2@CeO2 redox catalyst for cycling methane partial oxidation and CO2 splitting

doi:10.1016/j.cjche.2023.04.025

Abstract

Abstract: Redox catalysts play a vital role in the interconversion of two significant greenhouse gases, CO₂ and CH₄, via chemical looping methane dry reforming technology. Herein, a series of transition metals-alloyed and core-shell structured Ni-M/SiO₂@CeO₂ (M = Fe, Co, Cu, Mn, Zr) redox catalyst were fabricated and evaluated in a gas-solid fixed-bed reactor for cycling CH₄ partial oxidation (POx) and CO₂ splitting. The catalysts are composed of spherical SiO₂ core and CeO₂ shell, and the highly dispersed Ni alloy nanoparticles are the interlayer between core and shell. The oxygen vacancy concentration of Ni-M/SiO₂@CeO₂ followed the order of Co > Cu > Fe > Mn > Zr, and Ni alloying with transition metals significantly enhanced oxygen storage capacity (OSC). Ni-Co/SiO₂@CeO₂ catalyst with abundant oxygen vacancies and a high OSC showed the lowest temperatures of CH₄ activation (610 ℃) and CO₂ decomposition (590 ℃), thus demonstrating excellent redox reactivity. The catalyst exhibited superior activity and structural stability in the continuous CH₄/CO₂ redox cycles at 615 ℃, achieving 87% CH₄ conversion and 83% CO selectivity. The proposed catalyst shows great potential for the utilization of CH₄ and CO₂ in a redox mode, providing a new sight for design redox catalyst in chemical looping or related fields.

Key words: Chemical looping, Methane, Dry reforming, Catalyst, Partial Oxidation

摘要： Redox catalysts play a vital role in the interconversion of two significant greenhouse gases, CO₂ and CH₄, via chemical looping methane dry reforming technology. Herein, a series of transition metals-alloyed and core-shell structured Ni-M/SiO₂@CeO₂ (M = Fe, Co, Cu, Mn, Zr) redox catalyst were fabricated and evaluated in a gas-solid fixed-bed reactor for cycling CH₄ partial oxidation (POx) and CO₂ splitting. The catalysts are composed of spherical SiO₂ core and CeO₂ shell, and the highly dispersed Ni alloy nanoparticles are the interlayer between core and shell. The oxygen vacancy concentration of Ni-M/SiO₂@CeO₂ followed the order of Co > Cu > Fe > Mn > Zr, and Ni alloying with transition metals significantly enhanced oxygen storage capacity (OSC). Ni-Co/SiO₂@CeO₂ catalyst with abundant oxygen vacancies and a high OSC showed the lowest temperatures of CH₄ activation (610 ℃) and CO₂ decomposition (590 ℃), thus demonstrating excellent redox reactivity. The catalyst exhibited superior activity and structural stability in the continuous CH₄/CO₂ redox cycles at 615 ℃, achieving 87% CH₄ conversion and 83% CO selectivity. The proposed catalyst shows great potential for the utilization of CH₄ and CO₂ in a redox mode, providing a new sight for design redox catalyst in chemical looping or related fields.

关键词: Chemical looping, Methane, Dry reforming, Catalyst, Partial Oxidation

Chang Yang, Juping Zhang, Jiakai Wang, Dongfang Li, Kongzhai Li, Xing Zhu. Oxygen vacancies enriched Ni-Co/SiO₂@CeO₂ redox catalyst for cycling methane partial oxidation and CO₂ splitting[J]. Chinese Journal of Chemical Engineering, 2023, 63(11): 235-245.

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Oxygen vacancies enriched Ni-Co/SiO₂@CeO₂ redox catalyst for cycling methane partial oxidation and CO₂ splitting

Oxygen vacancies enriched Ni-Co/SiO₂@CeO₂ redox catalyst for cycling methane partial oxidation and CO₂ splitting

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