Kinetic and DRIFTS studies of the CO2 catalytic hydrogenation on Ru/SiO2: A comprehensive and strategic investigation of CO2 methanation mechanisms by kinetic modeling and data regression

被引:5
作者
Cabral, Thiago Oliveira [1 ,2 ,3 ]
Noronha, Fabio Bellot [3 ,4 ]
Toniolo, Fabio Souza [2 ]
机构
[1] Kansas State Univ, Dept Chem Engn, Manhattan, KS 66506 USA
[2] Univ Fed Rio de Janeiro, Chem Engn Program, COPPE, BR-21941972 Rio De Janeiro, RJ, Brazil
[3] Natl Inst Technol, Catalysis Div, BR-20081312 Rio De Janeiro, RJ, Brazil
[4] Univ Artois, Univ Lille, UCCS Unite Catalyse & Chim Solide, CNRS,ENSCL,UMR 8181,Cent Lille, F-59000 Lille, France
关键词
CO; 2; methanation; Infrared spectroscopy; Kinetic assessment; Langmuir-Hinshelwood modeling; Non-linear regression; DENSITY-FUNCTIONAL THEORY; CARBON-DIOXIDE; LOW-TEMPERATURE; STRUCTURE SENSITIVITY; PARTICLE-SIZE; DFT; NI; SURFACE; INSIGHT; NANOPARTICLES;
D O I
10.1016/j.cej.2024.149716
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
The kinetics of the CO2 hydrogenation/methanation is investigated on a Ru/SiO2 catalyst. Diffuse reflectance infrared Fourier transform spectroscopy experiments attest the presence of linearly adsorbed and bridge-bonded carbonyls on the metallic sites, as well as bicarbonate and formate species. Kinetic assessments at different temperatures and partial pressures show a direct relationship between methane turnover frequency and H2 pressure, suggesting that H* is involved in the rate-determining step. Contrariwise, increases in CO2 pressure inhibited methane formation. Applying Langmuir-Hinshelwood kinetics and non-linear regression, strategic kinetic models for CH4 formation rate were conceived and tested. The best model indicates that methanation starts off with CO2 dissociation into CO*reactive, proceeding along a H*-assisted pathway. The model also points out that competing oxygenated species (O*, HO*), intrinsically generated by CO2 activation, are hydrogenated faster on key sites, hindering the hydrogenation of carbon intermediates, which explained the inhibitory effect observed when CO2 pressure was increased.
引用
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页数:16
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