adsorption;
catalysis;
methanol conversion;
temperature programmed reaction;
zeolite;
D O I:
10.1002/bbpc.199500118
中图分类号:
O64 [物理化学(理论化学)、化学物理学];
学科分类号:
070304 ;
081704 ;
摘要:
The methanol to gasoline conversion over ZSM-5 has been studied by the Temperature Programmed Surface Reaction (TPSR) technique. The technique is able to delineate the two steps in the process: the dehydration of methanol to dimethyl ether and the subsequent conversion of dimethyl ether to hydrocarbons. The activation barriers associated with each step was evaluated from the TPSR profiles and are 108 kJ/mol and 195 kJ/mol respectively. The methanol desorption profile shows considerable change with the amount of methanol molecules adsorbed per Bronsted site of the zeolite. The energy associated with the desorption process, (CH3OHH+-ZSM-5-->(CH3OHH+-ZSM-5+CH3OH, shows a spectrum of values depending on n. The spectrum is not continuous and has a gap for n=1. The trend is similar to that for the corresponding gas-phase reaction, (CH3OHH+-->(CH3OHH++CH3OH. The present investigation highlights the importance of the protonated methanol cluster, (CH3OHH+-ZSM-5, in the primary step of the MTG process, the formation of dimethyl ether. The reaction is compared with the corresponding gas phase ion-molecule reaction of CH3OH2+.
机构:
Univ Western Australia, Ctr Energy M473, 35 Stirling Highway, Crawley, WA 6009, AustraliaUniv Western Australia, Ctr Energy M473, 35 Stirling Highway, Crawley, WA 6009, Australia
Wan, Zhijian
Li, Gang
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Univ Western Australia, Ctr Energy M473, 35 Stirling Highway, Crawley, WA 6009, AustraliaUniv Western Australia, Ctr Energy M473, 35 Stirling Highway, Crawley, WA 6009, Australia
Li, Gang
Wang, Chuanfu
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Univ Western Australia, Ctr Energy M473, 35 Stirling Highway, Crawley, WA 6009, AustraliaUniv Western Australia, Ctr Energy M473, 35 Stirling Highway, Crawley, WA 6009, Australia
Wang, Chuanfu
Yang, Hong
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Univ Western Australia, Ctr Energy M473, 35 Stirling Highway, Crawley, WA 6009, AustraliaUniv Western Australia, Ctr Energy M473, 35 Stirling Highway, Crawley, WA 6009, Australia
Yang, Hong
Zhang, Dongke
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Univ Western Australia, Ctr Energy M473, 35 Stirling Highway, Crawley, WA 6009, AustraliaUniv Western Australia, Ctr Energy M473, 35 Stirling Highway, Crawley, WA 6009, Australia
机构:
UCL, Dept Chem, London WC1 HOAJ, England
STFC Rutherford Appleton Lab, UK Catalysis Hub, Res Complex Harwell, Chilton OX11 0FA, EnglandUCL, Dept Chem, London WC1 HOAJ, England
Matam, S. K.
O'Malley, A. J.
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STFC Rutherford Appleton Lab, UK Catalysis Hub, Res Complex Harwell, Chilton OX11 0FA, England
Cardiff Univ, Sch Chem, Cardiff Catalysis Inst, Cardiff CF10 3AT, S Glam, WalesUCL, Dept Chem, London WC1 HOAJ, England
O'Malley, A. J.
Catlow, C. R. A.
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STFC Rutherford Appleton Lab, UK Catalysis Hub, Res Complex Harwell, Chilton OX11 0FA, England
Cardiff Univ, Sch Chem, Cardiff Catalysis Inst, Cardiff CF10 3AT, S Glam, WalesUCL, Dept Chem, London WC1 HOAJ, England
Catlow, C. R. A.
Suwardiyanto
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Univ Jember, Dept Chem, Jember 68121, IndonesiaUCL, Dept Chem, London WC1 HOAJ, England
Suwardiyanto
Collier, P.
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Johnson Matthey Technol Ctr, Reading RG34 9NH, Berks, EnglandUCL, Dept Chem, London WC1 HOAJ, England
Collier, P.
Hawkins, A. P.
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Univ Glasgow, Sch Chem, Glasgow G12 8QQ, Lanark, ScotlandUCL, Dept Chem, London WC1 HOAJ, England
Hawkins, A. P.
Zachariou, A.
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Univ Glasgow, Sch Chem, Glasgow G12 8QQ, Lanark, ScotlandUCL, Dept Chem, London WC1 HOAJ, England
Zachariou, A.
Lennon, D.
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Univ Glasgow, Sch Chem, Glasgow G12 8QQ, Lanark, ScotlandUCL, Dept Chem, London WC1 HOAJ, England
Lennon, D.
Silverwood, I.
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STFC Rutherford Appleton Lab, ISIS Facil, Didcot OX11 0QX, Oxon, EnglandUCL, Dept Chem, London WC1 HOAJ, England
Silverwood, I.
Parker, S. F.
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STFC Rutherford Appleton Lab, UK Catalysis Hub, Res Complex Harwell, Chilton OX11 0FA, England
STFC Rutherford Appleton Lab, ISIS Facil, Didcot OX11 0QX, Oxon, EnglandUCL, Dept Chem, London WC1 HOAJ, England
Parker, S. F.
Howe, R. F.
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Univ Aberdeen, Dept Chem, Aberdeen AB24 3UE, ScotlandUCL, Dept Chem, London WC1 HOAJ, England