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
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Kansas State Univ, Dept Chem Engn, Manhattan, KS 66506 USA
Univ Fed Rio de Janeiro, Chem Engn Program, COPPE, BR-21941972 Rio De Janeiro, RJ, Brazil
Natl Inst Technol, Catalysis Div, BR-20081312 Rio De Janeiro, RJ, BrazilKansas State Univ, Dept Chem Engn, Manhattan, KS 66506 USA
Cabral, Thiago Oliveira
[1
,2
,3
]
Noronha, Fabio Bellot
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Natl Inst Technol, Catalysis Div, BR-20081312 Rio De Janeiro, RJ, Brazil
Univ Artois, Univ Lille, UCCS Unite Catalyse & Chim Solide, CNRS,ENSCL,UMR 8181,Cent Lille, F-59000 Lille, FranceKansas State Univ, Dept Chem Engn, Manhattan, KS 66506 USA
Noronha, Fabio Bellot
[3
,4
]
Toniolo, Fabio Souza
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Univ Fed Rio de Janeiro, Chem Engn Program, COPPE, BR-21941972 Rio De Janeiro, RJ, BrazilKansas State Univ, Dept Chem Engn, Manhattan, KS 66506 USA
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
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.
机构:
Council Sci & Ind Res CSIR, Ctr Nanostruct & Adv Mat CeNAM, Chem Cluster, HySA Infrastruct Ctr Competence, ZA-0001 Pretoria, South Africa
North West Univ, Sch Chem & Minerals Engn, Ctr Excellence Carbon Based Fuels, Fac Engn, Private Bag X6001, ZA-2531 Potchefstroom, South AfricaCouncil Sci & Ind Res CSIR, Ctr Nanostruct & Adv Mat CeNAM, Chem Cluster, HySA Infrastruct Ctr Competence, ZA-0001 Pretoria, South Africa
Mbatha, Siphesihle
Thomas, Sebastien
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Univ Strasbourg UdS, CNRS, UMR 7515, Inst Chem & Proc Energy Environm & Hlth ICPEES, 25 Rue Becquerel, F-67087 Strasbourg 02, FranceCouncil Sci & Ind Res CSIR, Ctr Nanostruct & Adv Mat CeNAM, Chem Cluster, HySA Infrastruct Ctr Competence, ZA-0001 Pretoria, South Africa
Thomas, Sebastien
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Parkhomenko, Ksenia
Roger, Anne-Cecile
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Univ Strasbourg UdS, CNRS, UMR 7515, Inst Chem & Proc Energy Environm & Hlth ICPEES, 25 Rue Becquerel, F-67087 Strasbourg 02, FranceCouncil Sci & Ind Res CSIR, Ctr Nanostruct & Adv Mat CeNAM, Chem Cluster, HySA Infrastruct Ctr Competence, ZA-0001 Pretoria, South Africa
Roger, Anne-Cecile
Louis, Benoit
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Univ Strasbourg UdS, CNRS, UMR 7515, Inst Chem & Proc Energy Environm & Hlth ICPEES, 25 Rue Becquerel, F-67087 Strasbourg 02, FranceCouncil Sci & Ind Res CSIR, Ctr Nanostruct & Adv Mat CeNAM, Chem Cluster, HySA Infrastruct Ctr Competence, ZA-0001 Pretoria, South Africa
Louis, Benoit
Cui, Xiaoti
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Aalborg Univ, Dept Energy, Pontoppidanstr 111, DK-9220 Aalborg, DenmarkCouncil Sci & Ind Res CSIR, Ctr Nanostruct & Adv Mat CeNAM, Chem Cluster, HySA Infrastruct Ctr Competence, ZA-0001 Pretoria, South Africa
Cui, Xiaoti
Everson, Ray
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North West Univ, Sch Chem & Minerals Engn, Ctr Excellence Carbon Based Fuels, Fac Engn, Private Bag X6001, ZA-2531 Potchefstroom, South AfricaCouncil Sci & Ind Res CSIR, Ctr Nanostruct & Adv Mat CeNAM, Chem Cluster, HySA Infrastruct Ctr Competence, ZA-0001 Pretoria, South Africa
Everson, Ray
Langmi, Henrietta
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Univ Pretoria, Dept Chem, Private Bag X20, ZA-0028 Hatfield, South AfricaCouncil Sci & Ind Res CSIR, Ctr Nanostruct & Adv Mat CeNAM, Chem Cluster, HySA Infrastruct Ctr Competence, ZA-0001 Pretoria, South Africa
Langmi, Henrietta
Musyoka, Nicholas
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Council Sci & Ind Res CSIR, Ctr Nanostruct & Adv Mat CeNAM, Chem Cluster, HySA Infrastruct Ctr Competence, ZA-0001 Pretoria, South AfricaCouncil Sci & Ind Res CSIR, Ctr Nanostruct & Adv Mat CeNAM, Chem Cluster, HySA Infrastruct Ctr Competence, ZA-0001 Pretoria, South Africa
Musyoka, Nicholas
Ren, Jianwei
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Univ Johannesburg, Dept Mech Engn Sci, Cnr Kingsway & Univ Rd, ZA-2092 Johannesburg, South AfricaCouncil Sci & Ind Res CSIR, Ctr Nanostruct & Adv Mat CeNAM, Chem Cluster, HySA Infrastruct Ctr Competence, ZA-0001 Pretoria, South Africa
机构:
Moscow MV Lomonosov State Univ, Chem Dept, Moscow 119992, Russia
RAS, N D Zelinsky Inst Organ Chem, Moscow 119991, RussiaMoscow MV Lomonosov State Univ, Chem Dept, Moscow 119992, Russia
Tedeeva, Marina A.
Kustov, Alexander L.
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Moscow MV Lomonosov State Univ, Chem Dept, Moscow 119992, Russia
RAS, N D Zelinsky Inst Organ Chem, Moscow 119991, Russia
Natl Univ Sci & Technol MISiS, Inst Ecotechnol, Moscow 119071, RussiaMoscow MV Lomonosov State Univ, Chem Dept, Moscow 119992, Russia
Kustov, Alexander L.
Batkin, Alexander M.
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机构:
RAS, N D Zelinsky Inst Organ Chem, Moscow 119991, Russia
Natl Univ Sci & Technol MISiS, Inst Ecotechnol, Moscow 119071, RussiaMoscow MV Lomonosov State Univ, Chem Dept, Moscow 119992, Russia
Batkin, Alexander M.
Garifullina, Cholpan
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机构:
Almetievsk State Oil Inst AGNI, Kazan 423450, RussiaMoscow MV Lomonosov State Univ, Chem Dept, Moscow 119992, Russia
Garifullina, Cholpan
Zalyatdinov, Albert A.
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Almetievsk State Oil Inst AGNI, Kazan 423450, RussiaMoscow MV Lomonosov State Univ, Chem Dept, Moscow 119992, Russia
Zalyatdinov, Albert A.
Yang, Dan
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Nanjing Tech Univ, Sch Chem & Mol Engn, Nanjing 211816, Peoples R ChinaMoscow MV Lomonosov State Univ, Chem Dept, Moscow 119992, Russia
Yang, Dan
Dai, Yihu
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Nanjing Tech Univ, Sch Chem & Mol Engn, Nanjing 211816, Peoples R ChinaMoscow MV Lomonosov State Univ, Chem Dept, Moscow 119992, Russia
Dai, Yihu
Yang, Yanhui
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Nanjing Tech Univ, Sch Chem & Mol Engn, Nanjing 211816, Peoples R China
Minjiang Univ, Coll Mat & Chem Engn, Fuzhou 350108, Peoples R ChinaMoscow MV Lomonosov State Univ, Chem Dept, Moscow 119992, Russia
Yang, Yanhui
Kustov, Leonid M.
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h-index: 0
机构:
Moscow MV Lomonosov State Univ, Chem Dept, Moscow 119992, Russia
RAS, N D Zelinsky Inst Organ Chem, Moscow 119991, Russia
Natl Univ Sci & Technol MISiS, Inst Ecotechnol, Moscow 119071, RussiaMoscow MV Lomonosov State Univ, Chem Dept, Moscow 119992, Russia
机构:
Chemical Engineering, Competence Centre for Catalysis, Chalmers University of Technology, Gothenburg,SE - 41296, SwedenChemical Engineering, Competence Centre for Catalysis, Chalmers University of Technology, Gothenburg,SE - 41296, Sweden
Ghosh, Sreetama
Olsson, Louise
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Chemical Engineering, Competence Centre for Catalysis, Chalmers University of Technology, Gothenburg,SE - 41296, SwedenChemical Engineering, Competence Centre for Catalysis, Chalmers University of Technology, Gothenburg,SE - 41296, Sweden
Olsson, Louise
Creaser, Derek
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Chemical Engineering, Competence Centre for Catalysis, Chalmers University of Technology, Gothenburg,SE - 41296, SwedenChemical Engineering, Competence Centre for Catalysis, Chalmers University of Technology, Gothenburg,SE - 41296, Sweden
机构:
Council Sci & Ind Res CSIR, Ctr Nanostruct & Adv Mat CeNAM, Chem Cluster, HySA Infrastruct Ctr Competence, ZA-0001 Pretoria, South Africa
North West Univ, Sch Chem & Minerals Engn, Ctr Excellence Carbon Based Fuels, Fac Engn, Private Bag X6001, ZA-2531 Potchefstroom, South AfricaCouncil Sci & Ind Res CSIR, Ctr Nanostruct & Adv Mat CeNAM, Chem Cluster, HySA Infrastruct Ctr Competence, ZA-0001 Pretoria, South Africa
Mbatha, Siphesihle
Thomas, Sebastien
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h-index: 0
机构:
Univ Strasbourg UdS, CNRS, UMR 7515, Inst Chem & Proc Energy Environm & Hlth ICPEES, 25 Rue Becquerel, F-67087 Strasbourg 02, FranceCouncil Sci & Ind Res CSIR, Ctr Nanostruct & Adv Mat CeNAM, Chem Cluster, HySA Infrastruct Ctr Competence, ZA-0001 Pretoria, South Africa
Thomas, Sebastien
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Parkhomenko, Ksenia
Roger, Anne-Cecile
论文数: 0引用数: 0
h-index: 0
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Univ Strasbourg UdS, CNRS, UMR 7515, Inst Chem & Proc Energy Environm & Hlth ICPEES, 25 Rue Becquerel, F-67087 Strasbourg 02, FranceCouncil Sci & Ind Res CSIR, Ctr Nanostruct & Adv Mat CeNAM, Chem Cluster, HySA Infrastruct Ctr Competence, ZA-0001 Pretoria, South Africa
Roger, Anne-Cecile
Louis, Benoit
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Univ Strasbourg UdS, CNRS, UMR 7515, Inst Chem & Proc Energy Environm & Hlth ICPEES, 25 Rue Becquerel, F-67087 Strasbourg 02, FranceCouncil Sci & Ind Res CSIR, Ctr Nanostruct & Adv Mat CeNAM, Chem Cluster, HySA Infrastruct Ctr Competence, ZA-0001 Pretoria, South Africa
Louis, Benoit
Cui, Xiaoti
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h-index: 0
机构:
Aalborg Univ, Dept Energy, Pontoppidanstr 111, DK-9220 Aalborg, DenmarkCouncil Sci & Ind Res CSIR, Ctr Nanostruct & Adv Mat CeNAM, Chem Cluster, HySA Infrastruct Ctr Competence, ZA-0001 Pretoria, South Africa
Cui, Xiaoti
Everson, Ray
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h-index: 0
机构:
North West Univ, Sch Chem & Minerals Engn, Ctr Excellence Carbon Based Fuels, Fac Engn, Private Bag X6001, ZA-2531 Potchefstroom, South AfricaCouncil Sci & Ind Res CSIR, Ctr Nanostruct & Adv Mat CeNAM, Chem Cluster, HySA Infrastruct Ctr Competence, ZA-0001 Pretoria, South Africa
Everson, Ray
Langmi, Henrietta
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h-index: 0
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Univ Pretoria, Dept Chem, Private Bag X20, ZA-0028 Hatfield, South AfricaCouncil Sci & Ind Res CSIR, Ctr Nanostruct & Adv Mat CeNAM, Chem Cluster, HySA Infrastruct Ctr Competence, ZA-0001 Pretoria, South Africa
Langmi, Henrietta
Musyoka, Nicholas
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Council Sci & Ind Res CSIR, Ctr Nanostruct & Adv Mat CeNAM, Chem Cluster, HySA Infrastruct Ctr Competence, ZA-0001 Pretoria, South AfricaCouncil Sci & Ind Res CSIR, Ctr Nanostruct & Adv Mat CeNAM, Chem Cluster, HySA Infrastruct Ctr Competence, ZA-0001 Pretoria, South Africa
Musyoka, Nicholas
Ren, Jianwei
论文数: 0引用数: 0
h-index: 0
机构:
Univ Johannesburg, Dept Mech Engn Sci, Cnr Kingsway & Univ Rd, ZA-2092 Johannesburg, South AfricaCouncil Sci & Ind Res CSIR, Ctr Nanostruct & Adv Mat CeNAM, Chem Cluster, HySA Infrastruct Ctr Competence, ZA-0001 Pretoria, South Africa
机构:
Moscow MV Lomonosov State Univ, Chem Dept, Moscow 119992, Russia
RAS, N D Zelinsky Inst Organ Chem, Moscow 119991, RussiaMoscow MV Lomonosov State Univ, Chem Dept, Moscow 119992, Russia
Tedeeva, Marina A.
Kustov, Alexander L.
论文数: 0引用数: 0
h-index: 0
机构:
Moscow MV Lomonosov State Univ, Chem Dept, Moscow 119992, Russia
RAS, N D Zelinsky Inst Organ Chem, Moscow 119991, Russia
Natl Univ Sci & Technol MISiS, Inst Ecotechnol, Moscow 119071, RussiaMoscow MV Lomonosov State Univ, Chem Dept, Moscow 119992, Russia
Kustov, Alexander L.
Batkin, Alexander M.
论文数: 0引用数: 0
h-index: 0
机构:
RAS, N D Zelinsky Inst Organ Chem, Moscow 119991, Russia
Natl Univ Sci & Technol MISiS, Inst Ecotechnol, Moscow 119071, RussiaMoscow MV Lomonosov State Univ, Chem Dept, Moscow 119992, Russia
Batkin, Alexander M.
Garifullina, Cholpan
论文数: 0引用数: 0
h-index: 0
机构:
Almetievsk State Oil Inst AGNI, Kazan 423450, RussiaMoscow MV Lomonosov State Univ, Chem Dept, Moscow 119992, Russia
Garifullina, Cholpan
Zalyatdinov, Albert A.
论文数: 0引用数: 0
h-index: 0
机构:
Almetievsk State Oil Inst AGNI, Kazan 423450, RussiaMoscow MV Lomonosov State Univ, Chem Dept, Moscow 119992, Russia
Zalyatdinov, Albert A.
Yang, Dan
论文数: 0引用数: 0
h-index: 0
机构:
Nanjing Tech Univ, Sch Chem & Mol Engn, Nanjing 211816, Peoples R ChinaMoscow MV Lomonosov State Univ, Chem Dept, Moscow 119992, Russia
Yang, Dan
Dai, Yihu
论文数: 0引用数: 0
h-index: 0
机构:
Nanjing Tech Univ, Sch Chem & Mol Engn, Nanjing 211816, Peoples R ChinaMoscow MV Lomonosov State Univ, Chem Dept, Moscow 119992, Russia
Dai, Yihu
Yang, Yanhui
论文数: 0引用数: 0
h-index: 0
机构:
Nanjing Tech Univ, Sch Chem & Mol Engn, Nanjing 211816, Peoples R China
Minjiang Univ, Coll Mat & Chem Engn, Fuzhou 350108, Peoples R ChinaMoscow MV Lomonosov State Univ, Chem Dept, Moscow 119992, Russia
Yang, Yanhui
Kustov, Leonid M.
论文数: 0引用数: 0
h-index: 0
机构:
Moscow MV Lomonosov State Univ, Chem Dept, Moscow 119992, Russia
RAS, N D Zelinsky Inst Organ Chem, Moscow 119991, Russia
Natl Univ Sci & Technol MISiS, Inst Ecotechnol, Moscow 119071, RussiaMoscow MV Lomonosov State Univ, Chem Dept, Moscow 119992, Russia
机构:
Chemical Engineering, Competence Centre for Catalysis, Chalmers University of Technology, Gothenburg,SE - 41296, SwedenChemical Engineering, Competence Centre for Catalysis, Chalmers University of Technology, Gothenburg,SE - 41296, Sweden
Ghosh, Sreetama
Olsson, Louise
论文数: 0引用数: 0
h-index: 0
机构:
Chemical Engineering, Competence Centre for Catalysis, Chalmers University of Technology, Gothenburg,SE - 41296, SwedenChemical Engineering, Competence Centre for Catalysis, Chalmers University of Technology, Gothenburg,SE - 41296, Sweden
Olsson, Louise
Creaser, Derek
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h-index: 0
机构:
Chemical Engineering, Competence Centre for Catalysis, Chalmers University of Technology, Gothenburg,SE - 41296, SwedenChemical Engineering, Competence Centre for Catalysis, Chalmers University of Technology, Gothenburg,SE - 41296, Sweden