Hydrothermal Synthesis of Ruthenium Nanoparticles with a Metallic Core and a Ruthenium Carbide Shell for Low-Temperature Activation of CO2 to Methane

doi:10.1021/jacs.9b07088

機構典藏 > College of Engineering > Graduate Institute & Department of Electrical Engineering > Journal Article > Item 987654321/119826

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Title:	Hydrothermal Synthesis of Ruthenium Nanoparticles with a Metallic Core and a Ruthenium Carbide Shell for Low-Temperature Activation of CO2 to Methane
Authors:	Cored, Jorge;Andrea, García-Ortiz;Iborra, Sara;Climent, María J.;Liu, Lichen;Chuang, Cheng-Hao;Chan, Ting-Shan;Escudero, Carlos;Concepción, Patricia;Corma, Avelino
Date:	2019-11-27
Issue Date:	2021-01-06 12:10:28 (UTC+8)
Abstract:	Ruthenium nanoparticles with a core–shell structure formed by a core of metallic ruthenium and a shell of ruthenium carbide have been synthesized by a mild and easy hydrothermal treatment. The dual structure and composition of the nanoparticles have been determined by synchrotron X-ray photoelectron spectroscopy (XPS), near-edge X-ray absorption fine structure (NEXAFS) analysis, and transmission electron microscopy (TEM) imaging. According to depth profile synchrotron XPS and X-ray diffraction (XRD) analysis, metallic ruthenium species predominate in the inner layers of the material, ruthenium carbide species being located on the upper surface layers. The ruthenium carbon catalysts presented herein are able to activate both CO2 and H2, exhibiting exceptional high activity for CO2 hydrogenation at low temperatures (160–200 °C) with 100% selectivity to methane, surpassing by far the most active Ru catalysts reported up to now. On the basis of catalytic studies and isotopic 13CO/12CO2/H2 experiments, the active sites responsible for this unprecedented activity can be associated with surface ruthenium carbide (RuC) species, which enable CO2 activation and transformation to methane via a direct CO2 hydrogenation mechanism. Both the high activity and the absence of CO in the gas effluent confer relevance to these catalysts for the Sabatier reaction, a chemical process with renewed interest for storing surplus renewable energy in the form of methane.
Relation:	Journal of American Chemical Society 141(49), p.19304−19311
DOI:	10.1021/jacs.9b07088
Appears in Collections:	[Graduate Institute & Department of Electrical Engineering] Journal Article

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