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Developing silicalite-1 encapsulated Ni nanoparticles as sintering-/coking-resistant catalysts for dry reforming of methane

Xu, Shanshan, Slater, Thomas J.A. ORCID:, Huang, Hong, Zhou, Yangtao, Jiao, Yilai, Parlett, Christopher M.A., Guan, Shaoliang, Chansai, Sarayute, Xu, Shaojun, Wang, Xinrui, Hardacre, Christopher and Fan, Xiaolei 2022. Developing silicalite-1 encapsulated Ni nanoparticles as sintering-/coking-resistant catalysts for dry reforming of methane. Chemical Engineering Journal 446 (5) , 137439. 10.1016/j.cej.2022.137439

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The stability of catalysts in dry reforming of methane (DRM) is a known issue. In this paper an encapsulation strategy has been employed to improve the stability compared with conventional impregnation methods. Herein, nickel nanoparticles encapsulated in silicalite-1 were prepared using a range of methods including post treatment, direct hydrothermal and seed-directed methods to investigate the effect of synthesis protocol on the properties of catalysts, such as degree of encapsulation and Ni dispersion, and anti-coking/-sintering performance in DRM. The Ni@SiO2-S1 catalysts obtained by the seed-directed synthesis presented the full encapsulation of Ni NPs by the zeolite framework with small particle sizes (∼2.9 nm) and strong metal-support interaction, which could sterically hinder the migration/aggregation of Ni NPs and carbon deposition. Therefore, Ni@SiO2-S1 showed stable CO2/CH4 conversions of 80% and 73%, respectively, with negligible metal sintering and coking deposition (∼0.5 wt%) over 28 h, which outperformed the other catalysts prepared. In contrast, the catalysts developed by the post-treatment and ethylenediamine-protected hydrothermal methods showed the co-existence of Ni phase on the internal and external surfaces, i.e. incomplete encapsulation, with large Ni particles, contributing to Ni sintering and coking. The correlation of the synthesis-structure-performance in this study sheds light on the design of coking-/sintering-resistant encapsulated catalysts for DRM.

Item Type: Article
Date Type: Publication
Status: Published
Schools: Chemistry
Cardiff Catalysis Institute (CCI)
Additional Information: This is an open access article under the terms of the CC-BY Attribution 4.0 International license.
Publisher: Elsevier
ISSN: 1385-8947
Funders: EPSRC
Date of First Compliant Deposit: 26 July 2022
Date of Acceptance: 6 June 2022
Last Modified: 13 May 2023 17:15

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