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

中国化学工程学报 ›› 2023, Vol. 63 ›› Issue (11): 235-245.DOI: 10.1016/j.cjche.2023.04.025

• Full Length Article • 上一篇下一篇

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

Chang Yang, Juping Zhang, Jiakai Wang, Dongfang Li, Kongzhai Li, Xing Zhu

State Key Laboratory of Complex Nonferrous Metal Resources Clean Utilization, Faculty of Metallurgical and Energy Engineering, Kunming University of Science and Technology, Kunming 650093, China

收稿日期:2023-02-28 修回日期:2023-04-23 出版日期:2023-11-28 发布日期:2024-01-08
通讯作者: Xing Zhu,E-mail:zhuxing@kust.edu.cn
基金资助:
This work was supported by the National Natural Science Foundation of China (52066007, 22279048), Yunnan Major Scientific and Technological Projects (202202AG050017), and the Applied Basic Research Program of Yunnan Province (202101AT070076).

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

Chang Yang, Juping Zhang, Jiakai Wang, Dongfang Li, Kongzhai Li, Xing Zhu

State Key Laboratory of Complex Nonferrous Metal Resources Clean Utilization, Faculty of Metallurgical and Energy Engineering, Kunming University of Science and Technology, Kunming 650093, China

Received:2023-02-28 Revised:2023-04-23 Online:2023-11-28 Published:2024-01-08
Contact: Xing Zhu,E-mail:zhuxing@kust.edu.cn
Supported by:
This work was supported by the National Natural Science Foundation of China (52066007, 22279048), Yunnan Major Scientific and Technological Projects (202202AG050017), and the Applied Basic Research Program of Yunnan Province (202101AT070076).

摘要/Abstract

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

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

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]. 中国化学工程学报, 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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