Effect of Residual Na+ on the Combustion of Methane over Co3O4 Bulk Catalysts Prepared by Precipitation

The effect of the presence of residual sodium (0.4 %wt) over a Co3O4 bulk catalyst for methane combustion was studied. Two samples, with and without residual sodium, were synthesized by precipitation and thoroughly characterised by X-ray diffraction (XRD), N-2 physisorption, Wavelength Dispersive X-...

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Detalhes bibliográficos
Autores: Choya Atencia, Andoni, De Rivas Martín, Beatriz, Gutiérrez Ortiz, José Ignacio, López Fonseca, Rubén
Formato: artículo
Fecha de publicación:2018
País:España
Recursos:Universidad del País Vasco
Repositorio:Addi. Archivo Digital para la Docencia y la Investigación
OAI Identifier:oai:addi.ehu.eus:10810/32301
Acesso em linha:http://hdl.handle.net/10810/32301
Access Level:acceso abierto
Palavra-chave:methane
catalytic oxidation
cobalt oxide
residual sodium
thermal stability
cobalt oxide catalysts
total oxidation
emissions abatement
N2O decomposition
no decomposition
nanoparticles
performance
behavior
account
MN
Descrição
Resumo:The effect of the presence of residual sodium (0.4 %wt) over a Co3O4 bulk catalyst for methane combustion was studied. Two samples, with and without residual sodium, were synthesized by precipitation and thoroughly characterised by X-ray diffraction (XRD), N-2 physisorption, Wavelength Dispersive X-ray Fluorescence (WDXRF), temperature-programmed reduction with hydrogen followed by temperature-programmed reduction with oxygen (H-2-TPR/O-2-TPO), temperature-programmed reaction with methane (CH4 -TPRe), ultraviolet-visible-near-infrared diffuse reflectance spectroscopy (UV-vis-NIR DRS), Raman spectroscopy and X-ray photoelectron spectroscopy (XPS). It was found that during calcination, a fraction of the sodium atoms initially deposited on the surface diffused and migrated into the spinel lattice, inducing a distortion that improved its textural and structural properties. However, surface sodium had an overall negative impact on the catalytic activity. It led to a reduction of surface Co3+ ions in favour of Co2+, thus ultimately decreasing the Co3+/Co2+ molar ratio (from 1.96 to 1.20) and decreasing the amount and mobility of active lattice oxygen species. As a result, the catalyst with residual sodium (T-90 = 545 degrees C) was notably less active than its clean counterpart (T-90 = 500 degrees C). All of this outlined the significance of a proper washing when synthesizing Co3O4 catalyst using a sodium salt as the precipitating agent.