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Hydrothermal Synthesis of Ruthenium Nanoparticles with a Metallic Core and a Ruthenium Carbide Shell for Low-Temperature Activation of CO2 to Methane.
Cored, Jorge; García-Ortiz, Andrea; Iborra, Sara; Climent, María J; Liu, Lichen; Chuang, Cheng-Hao; Chan, Ting-Shan; Escudero, Carlos; Concepción, Patricia; Corma, Avelino.
Afiliação
  • Cored J; Instituto de Tecnología Química , Universitat Politècnica de València-Consejo Superior de Investigaciones Científicas (UPV-CSIC) , Avenida de los Naranjos s/n , 46022 Valencia , Spain.
  • García-Ortiz A; Instituto de Tecnología Química , Universitat Politècnica de València-Consejo Superior de Investigaciones Científicas (UPV-CSIC) , Avenida de los Naranjos s/n , 46022 Valencia , Spain.
  • Iborra S; Instituto de Tecnología Química , Universitat Politècnica de València-Consejo Superior de Investigaciones Científicas (UPV-CSIC) , Avenida de los Naranjos s/n , 46022 Valencia , Spain.
  • Climent MJ; Instituto de Tecnología Química , Universitat Politècnica de València-Consejo Superior de Investigaciones Científicas (UPV-CSIC) , Avenida de los Naranjos s/n , 46022 Valencia , Spain.
  • Liu L; Instituto de Tecnología Química , Universitat Politècnica de València-Consejo Superior de Investigaciones Científicas (UPV-CSIC) , Avenida de los Naranjos s/n , 46022 Valencia , Spain.
  • Chuang CH; Department of Physics , Tamkang University , Tamsui 25137 New Taipei City , Taiwan.
  • Chan TS; Research Center for X-Ray Science , Tamkang University , Tamsui 25137 , New Taipei City , Taiwan.
  • Escudero C; National Synchrotron Radiation Research Center , Hsinchu 30076 , Taiwan.
  • Concepción P; ALBA Synchrotron Light Source , Carrer de la Llum 2-26 , 08290 Cerdanyola del Vallès , Spain.
  • Corma A; Instituto de Tecnología Química , Universitat Politècnica de València-Consejo Superior de Investigaciones Científicas (UPV-CSIC) , Avenida de los Naranjos s/n , 46022 Valencia , Spain.
J Am Chem Soc ; 141(49): 19304-19311, 2019 Dec 11.
Artigo em Inglês | MEDLINE | ID: mdl-31774282
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.

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Texto completo: Disponível Coleções: Bases de dados internacionais Base de dados: MEDLINE Idioma: Inglês Revista: J Am Chem Soc Ano de publicação: 2019 Tipo de documento: Artigo País de afiliação: Espanha