Unveiling the promotion effect of Zr species on SBA-15 supported nickel catalysts for CO2 methanation

被引:11
|
作者
Tang, Rui [1 ]
Ullah, Niamat [1 ]
Li, Zhenhua [1 ]
机构
[1] Tianjin Univ, Collaborat Innovat Ctr Chem Sci & Engn Tianjin, Sch Chem Engn & Technol, Key Lab Green Chem Technol,Minist Educ, Tianjin 300350, Peoples R China
基金
中国国家自然科学基金;
关键词
CO; 2; methanation; Ni; SBA-15; Promotion effect; Mechanism; ZrO2; SELECTIVE HYDROGENATION; NI/SBA-15; CATALYSTS; MESOPOROUS SILICA; NI/ZRO2; CATALYST; CARBON-DIOXIDE; CE; PERFORMANCE; RESISTANCE; INSIGHT; SURFACE;
D O I
10.1016/j.ijhydene.2022.11.011
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Introducing promoters on Ni-based catalysts for CO2 methanation have been proved to be positive for enhancing their performance. And the correlation of the promotion mecha-nism and the reaction pathway is significant for designing efficient catalysts. In this contribution, series of Zr species promoted SBA-15 supported Ni catalysts were prepared by citric acid complexation method under a range of Zr/Ni atomic ratios from 0 to 2.5. In situ and ex situ characterizations were carried out. It was found that the addition of citric acid was conductive to improve CH4 selectivity due to the higher concentrations of Ni0 confined in SBA-15, harvesting sufficient H atoms for CH4 formation following formate pathway via a formyl intermediate. Furthermore, a coverage layer of Zr species was found on the support at Zr/Ni = 1.7, which interacted with the Ni particles, providing higher concen-trations of medium basic sites for CO2 activation. Accordingly, the optimum catalytic performance was obtained on ZrNi-1.7(CI), achieving CO2 conversion as high as 78.1% and nearly 100% CH4 selectivity at 400 degrees C, following the formate hydrogenation pathway. In addition, the ZrNi-1.7(CI) showed good stability owing to the confinement effect of SBA-15 and the Ni-Zr interaction, no carbon deposits were detected after 50 h test.(c) 2022 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.
引用
收藏
页码:4694 / 4707
页数:14
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