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

DOI: 10.1016/j.cej.2022.137439 DOI Help

Authors: Shanshan Xu (The University of Manchester) , Thomas J. A. Slater (Diamond Light Source) , Hong Huang (Electrochemical Process Engineering (IEK-14), Forschungszentrum Jülich) , Yangtao Zhou (Institute of Metal Research, Chinese Academy of Sciences) , Yilai Jiao (Institute of Metal Research, Chinese Academy of Sciences) , Christopher M. A. Parlett (The University of Manchester; Diamond Light Source; UK Catalysis Hub, Research Complex at Harwell; University of Manchester at Harwell) , Shaoliang Guan (Harwell XPS–The EPSRC National Facility for Photoelectron Spectroscopy, Research Complex at Harwell) , Sarayute Chansai (The University of Manchester) , Shaojun Xu (UK Catalysis Hub, Research Complex at Harwell; Cardiff University) , Xinrui Wang (The University of Manchester) , Christopher Hardacre (The University of Manchester) , Xiaolei Fan (The University of Manchester)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Chemical Engineering Journal , VOL 5

State: Published (Approved)
Published: June 2022
Diamond Proposal Number(s): 29468

Open Access Open Access

Abstract: 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.

Journal Keywords: Silicalite-1; Encapsulated Ni catalyst; Dry reforming of methane; Anti-sintering; Anti-coking

Subject Areas: Chemistry, Materials, Environment

Diamond Offline Facilities: Electron Physical Sciences Imaging Centre (ePSIC)
Instruments: E01-JEM ARM 200CF

Added On: 09/06/2022 10:45


Discipline Tags:

Zeolites Earth Sciences & Environment Climate Change Physical Chemistry Catalysis Chemistry Materials Science Chemical Engineering Engineering & Technology Nanoscience/Nanotechnology

Technical Tags:

Microscopy Electron Microscopy (EM) Scanning Transmission Electron Microscopy (STEM)