Boosting CO2 methanation on ceria supported transition metal catalysts via chelation coupled wetness impregnation

Xuhui Zou; Zhangfeng Shen; Xi Li; Yongyong Cao; Qineng Xia; Siqian Zhang; Yanan Liu; Lingchang Jiang; Lifen Li; Lifeng Cui; Yangang Wang

doi:10.1016/j.jcis.2022.04.001

Boosting CO₂ methanation on ceria supported transition metal catalysts via chelation coupled wetness impregnation

J Colloid Interface Sci. 2022 Aug 15:620:77-85. doi: 10.1016/j.jcis.2022.04.001. Epub 2022 Apr 4.

Authors

Xuhui Zou¹, Zhangfeng Shen², Xi Li³, Yongyong Cao², Qineng Xia², Siqian Zhang², Yanan Liu², Lingchang Jiang², Lifen Li², Lifeng Cui⁴, Yangang Wang⁵

Affiliations

¹ Department of Environmental Science and Engineering, University of Shanghai for Science and Technology, Shanghai 200093, China; College of Biological Chemical Science and Engineering, Jiaxing University, Jiaxing 314001, China.
² College of Biological Chemical Science and Engineering, Jiaxing University, Jiaxing 314001, China.
³ College of Biological Chemical Science and Engineering, Jiaxing University, Jiaxing 314001, China. Electronic address: xili21@mail.zjxu.edu.cn.
⁴ Department of Environmental Science and Engineering, University of Shanghai for Science and Technology, Shanghai 200093, China. Electronic address: lifeng.cui@gmail.com.
⁵ College of Biological Chemical Science and Engineering, Jiaxing University, Jiaxing 314001, China. Electronic address: ygwang8136@mail.zjxu.edu.cn.

PMID: 35421755
DOI: 10.1016/j.jcis.2022.04.001

Abstract

The incipient wetness impregnation (IWI) method is widely used in the preparation of supported transition metal catalysts for its high throughput and cost-effective synthesis, yet suffers from poor metal-support interaction, restricting its further application at an industrial scale. Herein, a universal strategy of chelation coupled impregnation (CCI) is presented. The as-prepared Ni/CeO₂(CCI) showed superior catalytic performance for CO₂ conversion (84.3%) and CH₄ selectivity (100%) under the experimental conditions (WGHSV = 24,000 mL g^-1 h^-1 and H₂/CO₂ = 4:1) even at low temperatures (T = 275 °C). The surface characterization results confirmed that the agglomeration of metal active sites in Ni/CeO₂(CCI) was restricted and more surface oxygen vacancies were generated on CeO₂. Further, the in-situ diffuse reflectance infrared Fourier transform spectroscopy (in-situ DRIFTS) analysis suggested that the surface oxygen vacancies that served as active sites could facilitate the direct dissociation of CO₂ more favorably than the associative route, thus significantly promoting CO₂ methanation activity.

Keywords: CO(2) methanation; Ceria; Chelation coupled wetness impregnation; Oxygen vacancies; Supported transition metal catalysts.