Open AccessNatural Kaolin-Based Ni Catalysts for CO2 Methanation: On the Effect of Ce Enhancement and Microwave-Assisted Hydrothermal Synthesis
Author(s) -
Kritchakorn Aimdate,
Atthapon Srifa,
Wanida KooAmornpattana,
Chularat Sakdaronnarong,
Wantana Klysubun,
Sirapassorn Kiatphuengporn,
Suttichai Assabumrungrat,
Suwimol Wongsakulphasatch,
Watchareeya Kaveevivitchai,
Masao Sudoh,
Ryo Watanabe,
Choji Fukuhara,
Sakhon Ratchahat
Publication year - 2021
Publication title -
acs omega
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 0.779
H-Index - 40
ISSN - 2470-1343
DOI - 10.1021/acsomega.1c01231
Subject(s) - methanation , catalysis , substitute natural gas , materials science , crystallite , scanning electron microscope , selectivity , chemical engineering , hydrothermal circulation , microwave , hydrothermal synthesis , inorganic chemistry , nuclear chemistry , syngas , chemistry , metallurgy , composite material , organic chemistry , physics , quantum mechanics , engineering
Natural kaolin-based Ni catalysts have been developed for low-temperature CO 2 methanation. The catalysts were prepared via a one-step co-impregnation of Ni and Ce onto a natural kaolin-derived metakaolin using a microwave-assisted hydrothermal method as an acid-/base-free synthesis method. The influences of microwave irradiation and Ce promotion on the catalytic enhancement including the CO 2 conversion, CH 4 selectivity, and CH 4 yield were experimentally investigated by a catalytic test of as-prepared catalysts in a fixed-bed tubular reactor. The relationship between the catalyst properties and its methanation activities was revealed by various characterization techniques including X-ray fluorescence, X-ray diffraction, Brunauer-Emmett-Teller, scanning electron microscopy, selected area electron diffraction, transmission electron microscopy, elemental mapping, H 2 temperature-programmed reduction, and X-ray absorption near-edge structure analyses. Among the two enhancement methods, microwave and Ce promotion, the microwave-assisted synthesis could produce a catalyst containing highly dispersed Ni particles with a smaller Ni crystallite size and higher catalyst reducibility, resulting in a higher CO 2 conversion from 1.6 to 7.5% and a better CH 4 selectivity from 76.3 to 79.9% at 300 °C. Meanwhile, the enhancement by Ce addition exhibited a great improvement on the catalyst activities. It was experimentally found that the CO 2 conversion increased approximately 7-fold from 7.5 to 52.9%, while the CH 4 selectivity significantly improved from 79.9 to 98.0% at 300 °C. Though the microwave-assisted synthesis could further improve the catalyst activities of Ce-promoted catalysts, the Ce addition exhibited a more prominent impact than the microwave enhancement. Cerium oxide (CeO 2 ) improved the catalyst activities through mechanisms of higher CO 2 adsorption capacity with its basic sites and the unique structure of CeO 2 with a reversible valence change of Ce 4+ and Ce 3+ and high oxygen vacancies. However, it was found that the catalyst prepared by microwave-assisted synthesis and Ce promotion proved to be the optimum catalyst in this study. Therefore, the present work demonstrated the potential to synthesize a nickel-based catalyst with improved catalytic activities by adding a small amount of Ce as a catalytic promoter and employing microwave irradiation for improving the Ni dispersion.