Density Functional Theory Study of the Zeolite-Catalyzed Methylation of Benzene with Methanol
Abstract The reaction coordinates based on Gibbs free energies for the methylation of benzene with methanol over HZSM-5 and Hβ, both concerted and stepwise pathway, were investigated by applying density functional theory. From the estimated adsorption energies of benzene and methanol on these zeolit...
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| Autor*in: |
Wen, Zhenhao [verfasserIn] Zhu, Huayu [verfasserIn] Zhu, Xuedong [verfasserIn] |
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| Format: |
E-Artikel |
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| Sprache: |
Englisch |
| Erschienen: |
2019 |
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| Schlagwörter: |
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| Übergeordnetes Werk: |
Enthalten in: Catalysis letters - Dordrecht [u.a.] : Springer Science + Business Media B.V, 1988, 150(2019), 1 vom: 29. Aug., Seite 21-30 |
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| Übergeordnetes Werk: |
volume:150 ; year:2019 ; number:1 ; day:29 ; month:08 ; pages:21-30 |
| Links: |
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| DOI / URN: |
10.1007/s10562-019-02931-3 |
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| Katalog-ID: |
SPR011357398 |
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| 245 | 1 | 0 | |a Density Functional Theory Study of the Zeolite-Catalyzed Methylation of Benzene with Methanol |
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| 520 | |a Abstract The reaction coordinates based on Gibbs free energies for the methylation of benzene with methanol over HZSM-5 and Hβ, both concerted and stepwise pathway, were investigated by applying density functional theory. From the estimated adsorption energies of benzene and methanol on these zeolites, stronger guest–host interactions were observed in HZSM-5 compared to Hβ. We find that at low temperatures, the concerted mechanism dominates, however, the mechanism converts to the stepwise pathway at higher temperatures. The formation of methoxy group is found to be the rate-determining step for the stepwise pathway, and the calculated free energy barriers at 673 K were 138 kJ/mol for HZSM-5 and 149 kJ/mol for Hβ, lower than those in the concerted pathway (165 kJ/mol for HZSM-5 and 168 kJ/mol for Hβ), indicating that the stepwise pathway is kinetically favored for the methylation of benzene with methanol at 673 K. Gaseous methane can be produced via one intramolecular hydrogen transfer from the ring carbon to the carbon of methyl group in the protonated toluene species, and the calculated free energy barriers for forming methane over HZSM-5 and Hβ are 112 and 100 kJ/mol, respectively, suggesting that methane is more easily formed over 12-ring Hβ catalyst. Graphic Abstract The stepwise pathway is kinetically favored for the methylation of benzene with methanol compared to concerted pathway. | ||
| 650 | 4 | |a Methylation of benzene |7 (dpeaa)DE-He213 | |
| 650 | 4 | |a Methanol conversion |7 (dpeaa)DE-He213 | |
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| 650 | 4 | |a Hβ |7 (dpeaa)DE-He213 | |
| 650 | 4 | |a DFT |7 (dpeaa)DE-He213 | |
| 700 | 1 | |a Zhu, Huayu |e verfasserin |4 aut | |
| 700 | 1 | |a Zhu, Xuedong |e verfasserin |4 aut | |
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10.1007/s10562-019-02931-3 doi (DE-627)SPR011357398 (SPR)s10562-019-02931-3-e DE-627 ger DE-627 rakwb eng 540 660 ASE 35.17 bkl Wen, Zhenhao verfasserin aut Density Functional Theory Study of the Zeolite-Catalyzed Methylation of Benzene with Methanol 2019 Text txt rdacontent Computermedien c rdamedia Online-Ressource cr rdacarrier Abstract The reaction coordinates based on Gibbs free energies for the methylation of benzene with methanol over HZSM-5 and Hβ, both concerted and stepwise pathway, were investigated by applying density functional theory. From the estimated adsorption energies of benzene and methanol on these zeolites, stronger guest–host interactions were observed in HZSM-5 compared to Hβ. We find that at low temperatures, the concerted mechanism dominates, however, the mechanism converts to the stepwise pathway at higher temperatures. The formation of methoxy group is found to be the rate-determining step for the stepwise pathway, and the calculated free energy barriers at 673 K were 138 kJ/mol for HZSM-5 and 149 kJ/mol for Hβ, lower than those in the concerted pathway (165 kJ/mol for HZSM-5 and 168 kJ/mol for Hβ), indicating that the stepwise pathway is kinetically favored for the methylation of benzene with methanol at 673 K. Gaseous methane can be produced via one intramolecular hydrogen transfer from the ring carbon to the carbon of methyl group in the protonated toluene species, and the calculated free energy barriers for forming methane over HZSM-5 and Hβ are 112 and 100 kJ/mol, respectively, suggesting that methane is more easily formed over 12-ring Hβ catalyst. Graphic Abstract The stepwise pathway is kinetically favored for the methylation of benzene with methanol compared to concerted pathway. Methylation of benzene (dpeaa)DE-He213 Methanol conversion (dpeaa)DE-He213 HZSM-5 (dpeaa)DE-He213 Hβ (dpeaa)DE-He213 DFT (dpeaa)DE-He213 Zhu, Huayu verfasserin aut Zhu, Xuedong verfasserin aut Enthalten in Catalysis letters Dordrecht [u.a.] : Springer Science + Business Media B.V, 1988 150(2019), 1 vom: 29. Aug., Seite 21-30 (DE-627)306717638 (DE-600)1501518-X 1572-879X nnns volume:150 year:2019 number:1 day:29 month:08 pages:21-30 https://dx.doi.org/10.1007/s10562-019-02931-3 lizenzpflichtig Volltext GBV_USEFLAG_A SYSFLAG_A GBV_SPRINGER SSG-OLC-PHA GBV_ILN_11 GBV_ILN_20 GBV_ILN_22 GBV_ILN_23 GBV_ILN_24 GBV_ILN_31 GBV_ILN_32 GBV_ILN_39 GBV_ILN_40 GBV_ILN_60 GBV_ILN_62 GBV_ILN_63 GBV_ILN_65 GBV_ILN_69 GBV_ILN_70 GBV_ILN_73 GBV_ILN_74 GBV_ILN_90 GBV_ILN_95 GBV_ILN_100 GBV_ILN_101 GBV_ILN_105 GBV_ILN_110 GBV_ILN_120 GBV_ILN_138 GBV_ILN_150 GBV_ILN_151 GBV_ILN_152 GBV_ILN_161 GBV_ILN_170 GBV_ILN_171 GBV_ILN_187 GBV_ILN_213 GBV_ILN_224 GBV_ILN_230 GBV_ILN_250 GBV_ILN_281 GBV_ILN_285 GBV_ILN_293 GBV_ILN_370 GBV_ILN_602 GBV_ILN_636 GBV_ILN_702 GBV_ILN_2001 GBV_ILN_2003 GBV_ILN_2004 GBV_ILN_2005 GBV_ILN_2006 GBV_ILN_2007 GBV_ILN_2008 GBV_ILN_2009 GBV_ILN_2010 GBV_ILN_2011 GBV_ILN_2014 GBV_ILN_2015 GBV_ILN_2020 GBV_ILN_2021 GBV_ILN_2025 GBV_ILN_2026 GBV_ILN_2027 GBV_ILN_2031 GBV_ILN_2034 GBV_ILN_2037 GBV_ILN_2038 GBV_ILN_2039 GBV_ILN_2044 GBV_ILN_2048 GBV_ILN_2049 GBV_ILN_2050 GBV_ILN_2055 GBV_ILN_2057 GBV_ILN_2059 GBV_ILN_2061 GBV_ILN_2064 GBV_ILN_2065 GBV_ILN_2068 GBV_ILN_2070 GBV_ILN_2086 GBV_ILN_2088 GBV_ILN_2093 GBV_ILN_2106 GBV_ILN_2107 GBV_ILN_2108 GBV_ILN_2110 GBV_ILN_2111 GBV_ILN_2112 GBV_ILN_2113 GBV_ILN_2116 GBV_ILN_2118 GBV_ILN_2119 GBV_ILN_2122 GBV_ILN_2129 GBV_ILN_2143 GBV_ILN_2144 GBV_ILN_2147 GBV_ILN_2148 GBV_ILN_2152 GBV_ILN_2153 GBV_ILN_2188 GBV_ILN_2190 GBV_ILN_2232 GBV_ILN_2336 GBV_ILN_2446 GBV_ILN_2470 GBV_ILN_2472 GBV_ILN_2507 GBV_ILN_2522 GBV_ILN_2548 GBV_ILN_4035 GBV_ILN_4037 GBV_ILN_4046 GBV_ILN_4112 GBV_ILN_4125 GBV_ILN_4242 GBV_ILN_4246 GBV_ILN_4249 GBV_ILN_4251 GBV_ILN_4305 GBV_ILN_4306 GBV_ILN_4307 GBV_ILN_4313 GBV_ILN_4322 GBV_ILN_4323 GBV_ILN_4324 GBV_ILN_4325 GBV_ILN_4326 GBV_ILN_4333 GBV_ILN_4334 GBV_ILN_4335 GBV_ILN_4336 GBV_ILN_4338 GBV_ILN_4393 GBV_ILN_4700 35.17 ASE AR 150 2019 1 29 08 21-30 |
| spelling |
10.1007/s10562-019-02931-3 doi (DE-627)SPR011357398 (SPR)s10562-019-02931-3-e DE-627 ger DE-627 rakwb eng 540 660 ASE 35.17 bkl Wen, Zhenhao verfasserin aut Density Functional Theory Study of the Zeolite-Catalyzed Methylation of Benzene with Methanol 2019 Text txt rdacontent Computermedien c rdamedia Online-Ressource cr rdacarrier Abstract The reaction coordinates based on Gibbs free energies for the methylation of benzene with methanol over HZSM-5 and Hβ, both concerted and stepwise pathway, were investigated by applying density functional theory. From the estimated adsorption energies of benzene and methanol on these zeolites, stronger guest–host interactions were observed in HZSM-5 compared to Hβ. We find that at low temperatures, the concerted mechanism dominates, however, the mechanism converts to the stepwise pathway at higher temperatures. The formation of methoxy group is found to be the rate-determining step for the stepwise pathway, and the calculated free energy barriers at 673 K were 138 kJ/mol for HZSM-5 and 149 kJ/mol for Hβ, lower than those in the concerted pathway (165 kJ/mol for HZSM-5 and 168 kJ/mol for Hβ), indicating that the stepwise pathway is kinetically favored for the methylation of benzene with methanol at 673 K. Gaseous methane can be produced via one intramolecular hydrogen transfer from the ring carbon to the carbon of methyl group in the protonated toluene species, and the calculated free energy barriers for forming methane over HZSM-5 and Hβ are 112 and 100 kJ/mol, respectively, suggesting that methane is more easily formed over 12-ring Hβ catalyst. Graphic Abstract The stepwise pathway is kinetically favored for the methylation of benzene with methanol compared to concerted pathway. Methylation of benzene (dpeaa)DE-He213 Methanol conversion (dpeaa)DE-He213 HZSM-5 (dpeaa)DE-He213 Hβ (dpeaa)DE-He213 DFT (dpeaa)DE-He213 Zhu, Huayu verfasserin aut Zhu, Xuedong verfasserin aut Enthalten in Catalysis letters Dordrecht [u.a.] : Springer Science + Business Media B.V, 1988 150(2019), 1 vom: 29. Aug., Seite 21-30 (DE-627)306717638 (DE-600)1501518-X 1572-879X nnns volume:150 year:2019 number:1 day:29 month:08 pages:21-30 https://dx.doi.org/10.1007/s10562-019-02931-3 lizenzpflichtig Volltext GBV_USEFLAG_A SYSFLAG_A GBV_SPRINGER SSG-OLC-PHA GBV_ILN_11 GBV_ILN_20 GBV_ILN_22 GBV_ILN_23 GBV_ILN_24 GBV_ILN_31 GBV_ILN_32 GBV_ILN_39 GBV_ILN_40 GBV_ILN_60 GBV_ILN_62 GBV_ILN_63 GBV_ILN_65 GBV_ILN_69 GBV_ILN_70 GBV_ILN_73 GBV_ILN_74 GBV_ILN_90 GBV_ILN_95 GBV_ILN_100 GBV_ILN_101 GBV_ILN_105 GBV_ILN_110 GBV_ILN_120 GBV_ILN_138 GBV_ILN_150 GBV_ILN_151 GBV_ILN_152 GBV_ILN_161 GBV_ILN_170 GBV_ILN_171 GBV_ILN_187 GBV_ILN_213 GBV_ILN_224 GBV_ILN_230 GBV_ILN_250 GBV_ILN_281 GBV_ILN_285 GBV_ILN_293 GBV_ILN_370 GBV_ILN_602 GBV_ILN_636 GBV_ILN_702 GBV_ILN_2001 GBV_ILN_2003 GBV_ILN_2004 GBV_ILN_2005 GBV_ILN_2006 GBV_ILN_2007 GBV_ILN_2008 GBV_ILN_2009 GBV_ILN_2010 GBV_ILN_2011 GBV_ILN_2014 GBV_ILN_2015 GBV_ILN_2020 GBV_ILN_2021 GBV_ILN_2025 GBV_ILN_2026 GBV_ILN_2027 GBV_ILN_2031 GBV_ILN_2034 GBV_ILN_2037 GBV_ILN_2038 GBV_ILN_2039 GBV_ILN_2044 GBV_ILN_2048 GBV_ILN_2049 GBV_ILN_2050 GBV_ILN_2055 GBV_ILN_2057 GBV_ILN_2059 GBV_ILN_2061 GBV_ILN_2064 GBV_ILN_2065 GBV_ILN_2068 GBV_ILN_2070 GBV_ILN_2086 GBV_ILN_2088 GBV_ILN_2093 GBV_ILN_2106 GBV_ILN_2107 GBV_ILN_2108 GBV_ILN_2110 GBV_ILN_2111 GBV_ILN_2112 GBV_ILN_2113 GBV_ILN_2116 GBV_ILN_2118 GBV_ILN_2119 GBV_ILN_2122 GBV_ILN_2129 GBV_ILN_2143 GBV_ILN_2144 GBV_ILN_2147 GBV_ILN_2148 GBV_ILN_2152 GBV_ILN_2153 GBV_ILN_2188 GBV_ILN_2190 GBV_ILN_2232 GBV_ILN_2336 GBV_ILN_2446 GBV_ILN_2470 GBV_ILN_2472 GBV_ILN_2507 GBV_ILN_2522 GBV_ILN_2548 GBV_ILN_4035 GBV_ILN_4037 GBV_ILN_4046 GBV_ILN_4112 GBV_ILN_4125 GBV_ILN_4242 GBV_ILN_4246 GBV_ILN_4249 GBV_ILN_4251 GBV_ILN_4305 GBV_ILN_4306 GBV_ILN_4307 GBV_ILN_4313 GBV_ILN_4322 GBV_ILN_4323 GBV_ILN_4324 GBV_ILN_4325 GBV_ILN_4326 GBV_ILN_4333 GBV_ILN_4334 GBV_ILN_4335 GBV_ILN_4336 GBV_ILN_4338 GBV_ILN_4393 GBV_ILN_4700 35.17 ASE AR 150 2019 1 29 08 21-30 |
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10.1007/s10562-019-02931-3 doi (DE-627)SPR011357398 (SPR)s10562-019-02931-3-e DE-627 ger DE-627 rakwb eng 540 660 ASE 35.17 bkl Wen, Zhenhao verfasserin aut Density Functional Theory Study of the Zeolite-Catalyzed Methylation of Benzene with Methanol 2019 Text txt rdacontent Computermedien c rdamedia Online-Ressource cr rdacarrier Abstract The reaction coordinates based on Gibbs free energies for the methylation of benzene with methanol over HZSM-5 and Hβ, both concerted and stepwise pathway, were investigated by applying density functional theory. From the estimated adsorption energies of benzene and methanol on these zeolites, stronger guest–host interactions were observed in HZSM-5 compared to Hβ. We find that at low temperatures, the concerted mechanism dominates, however, the mechanism converts to the stepwise pathway at higher temperatures. The formation of methoxy group is found to be the rate-determining step for the stepwise pathway, and the calculated free energy barriers at 673 K were 138 kJ/mol for HZSM-5 and 149 kJ/mol for Hβ, lower than those in the concerted pathway (165 kJ/mol for HZSM-5 and 168 kJ/mol for Hβ), indicating that the stepwise pathway is kinetically favored for the methylation of benzene with methanol at 673 K. Gaseous methane can be produced via one intramolecular hydrogen transfer from the ring carbon to the carbon of methyl group in the protonated toluene species, and the calculated free energy barriers for forming methane over HZSM-5 and Hβ are 112 and 100 kJ/mol, respectively, suggesting that methane is more easily formed over 12-ring Hβ catalyst. Graphic Abstract The stepwise pathway is kinetically favored for the methylation of benzene with methanol compared to concerted pathway. Methylation of benzene (dpeaa)DE-He213 Methanol conversion (dpeaa)DE-He213 HZSM-5 (dpeaa)DE-He213 Hβ (dpeaa)DE-He213 DFT (dpeaa)DE-He213 Zhu, Huayu verfasserin aut Zhu, Xuedong verfasserin aut Enthalten in Catalysis letters Dordrecht [u.a.] : Springer Science + Business Media B.V, 1988 150(2019), 1 vom: 29. Aug., Seite 21-30 (DE-627)306717638 (DE-600)1501518-X 1572-879X nnns volume:150 year:2019 number:1 day:29 month:08 pages:21-30 https://dx.doi.org/10.1007/s10562-019-02931-3 lizenzpflichtig Volltext GBV_USEFLAG_A SYSFLAG_A GBV_SPRINGER SSG-OLC-PHA GBV_ILN_11 GBV_ILN_20 GBV_ILN_22 GBV_ILN_23 GBV_ILN_24 GBV_ILN_31 GBV_ILN_32 GBV_ILN_39 GBV_ILN_40 GBV_ILN_60 GBV_ILN_62 GBV_ILN_63 GBV_ILN_65 GBV_ILN_69 GBV_ILN_70 GBV_ILN_73 GBV_ILN_74 GBV_ILN_90 GBV_ILN_95 GBV_ILN_100 GBV_ILN_101 GBV_ILN_105 GBV_ILN_110 GBV_ILN_120 GBV_ILN_138 GBV_ILN_150 GBV_ILN_151 GBV_ILN_152 GBV_ILN_161 GBV_ILN_170 GBV_ILN_171 GBV_ILN_187 GBV_ILN_213 GBV_ILN_224 GBV_ILN_230 GBV_ILN_250 GBV_ILN_281 GBV_ILN_285 GBV_ILN_293 GBV_ILN_370 GBV_ILN_602 GBV_ILN_636 GBV_ILN_702 GBV_ILN_2001 GBV_ILN_2003 GBV_ILN_2004 GBV_ILN_2005 GBV_ILN_2006 GBV_ILN_2007 GBV_ILN_2008 GBV_ILN_2009 GBV_ILN_2010 GBV_ILN_2011 GBV_ILN_2014 GBV_ILN_2015 GBV_ILN_2020 GBV_ILN_2021 GBV_ILN_2025 GBV_ILN_2026 GBV_ILN_2027 GBV_ILN_2031 GBV_ILN_2034 GBV_ILN_2037 GBV_ILN_2038 GBV_ILN_2039 GBV_ILN_2044 GBV_ILN_2048 GBV_ILN_2049 GBV_ILN_2050 GBV_ILN_2055 GBV_ILN_2057 GBV_ILN_2059 GBV_ILN_2061 GBV_ILN_2064 GBV_ILN_2065 GBV_ILN_2068 GBV_ILN_2070 GBV_ILN_2086 GBV_ILN_2088 GBV_ILN_2093 GBV_ILN_2106 GBV_ILN_2107 GBV_ILN_2108 GBV_ILN_2110 GBV_ILN_2111 GBV_ILN_2112 GBV_ILN_2113 GBV_ILN_2116 GBV_ILN_2118 GBV_ILN_2119 GBV_ILN_2122 GBV_ILN_2129 GBV_ILN_2143 GBV_ILN_2144 GBV_ILN_2147 GBV_ILN_2148 GBV_ILN_2152 GBV_ILN_2153 GBV_ILN_2188 GBV_ILN_2190 GBV_ILN_2232 GBV_ILN_2336 GBV_ILN_2446 GBV_ILN_2470 GBV_ILN_2472 GBV_ILN_2507 GBV_ILN_2522 GBV_ILN_2548 GBV_ILN_4035 GBV_ILN_4037 GBV_ILN_4046 GBV_ILN_4112 GBV_ILN_4125 GBV_ILN_4242 GBV_ILN_4246 GBV_ILN_4249 GBV_ILN_4251 GBV_ILN_4305 GBV_ILN_4306 GBV_ILN_4307 GBV_ILN_4313 GBV_ILN_4322 GBV_ILN_4323 GBV_ILN_4324 GBV_ILN_4325 GBV_ILN_4326 GBV_ILN_4333 GBV_ILN_4334 GBV_ILN_4335 GBV_ILN_4336 GBV_ILN_4338 GBV_ILN_4393 GBV_ILN_4700 35.17 ASE AR 150 2019 1 29 08 21-30 |
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10.1007/s10562-019-02931-3 doi (DE-627)SPR011357398 (SPR)s10562-019-02931-3-e DE-627 ger DE-627 rakwb eng 540 660 ASE 35.17 bkl Wen, Zhenhao verfasserin aut Density Functional Theory Study of the Zeolite-Catalyzed Methylation of Benzene with Methanol 2019 Text txt rdacontent Computermedien c rdamedia Online-Ressource cr rdacarrier Abstract The reaction coordinates based on Gibbs free energies for the methylation of benzene with methanol over HZSM-5 and Hβ, both concerted and stepwise pathway, were investigated by applying density functional theory. From the estimated adsorption energies of benzene and methanol on these zeolites, stronger guest–host interactions were observed in HZSM-5 compared to Hβ. We find that at low temperatures, the concerted mechanism dominates, however, the mechanism converts to the stepwise pathway at higher temperatures. The formation of methoxy group is found to be the rate-determining step for the stepwise pathway, and the calculated free energy barriers at 673 K were 138 kJ/mol for HZSM-5 and 149 kJ/mol for Hβ, lower than those in the concerted pathway (165 kJ/mol for HZSM-5 and 168 kJ/mol for Hβ), indicating that the stepwise pathway is kinetically favored for the methylation of benzene with methanol at 673 K. Gaseous methane can be produced via one intramolecular hydrogen transfer from the ring carbon to the carbon of methyl group in the protonated toluene species, and the calculated free energy barriers for forming methane over HZSM-5 and Hβ are 112 and 100 kJ/mol, respectively, suggesting that methane is more easily formed over 12-ring Hβ catalyst. Graphic Abstract The stepwise pathway is kinetically favored for the methylation of benzene with methanol compared to concerted pathway. Methylation of benzene (dpeaa)DE-He213 Methanol conversion (dpeaa)DE-He213 HZSM-5 (dpeaa)DE-He213 Hβ (dpeaa)DE-He213 DFT (dpeaa)DE-He213 Zhu, Huayu verfasserin aut Zhu, Xuedong verfasserin aut Enthalten in Catalysis letters Dordrecht [u.a.] : Springer Science + Business Media B.V, 1988 150(2019), 1 vom: 29. Aug., Seite 21-30 (DE-627)306717638 (DE-600)1501518-X 1572-879X nnns volume:150 year:2019 number:1 day:29 month:08 pages:21-30 https://dx.doi.org/10.1007/s10562-019-02931-3 lizenzpflichtig Volltext GBV_USEFLAG_A SYSFLAG_A GBV_SPRINGER SSG-OLC-PHA GBV_ILN_11 GBV_ILN_20 GBV_ILN_22 GBV_ILN_23 GBV_ILN_24 GBV_ILN_31 GBV_ILN_32 GBV_ILN_39 GBV_ILN_40 GBV_ILN_60 GBV_ILN_62 GBV_ILN_63 GBV_ILN_65 GBV_ILN_69 GBV_ILN_70 GBV_ILN_73 GBV_ILN_74 GBV_ILN_90 GBV_ILN_95 GBV_ILN_100 GBV_ILN_101 GBV_ILN_105 GBV_ILN_110 GBV_ILN_120 GBV_ILN_138 GBV_ILN_150 GBV_ILN_151 GBV_ILN_152 GBV_ILN_161 GBV_ILN_170 GBV_ILN_171 GBV_ILN_187 GBV_ILN_213 GBV_ILN_224 GBV_ILN_230 GBV_ILN_250 GBV_ILN_281 GBV_ILN_285 GBV_ILN_293 GBV_ILN_370 GBV_ILN_602 GBV_ILN_636 GBV_ILN_702 GBV_ILN_2001 GBV_ILN_2003 GBV_ILN_2004 GBV_ILN_2005 GBV_ILN_2006 GBV_ILN_2007 GBV_ILN_2008 GBV_ILN_2009 GBV_ILN_2010 GBV_ILN_2011 GBV_ILN_2014 GBV_ILN_2015 GBV_ILN_2020 GBV_ILN_2021 GBV_ILN_2025 GBV_ILN_2026 GBV_ILN_2027 GBV_ILN_2031 GBV_ILN_2034 GBV_ILN_2037 GBV_ILN_2038 GBV_ILN_2039 GBV_ILN_2044 GBV_ILN_2048 GBV_ILN_2049 GBV_ILN_2050 GBV_ILN_2055 GBV_ILN_2057 GBV_ILN_2059 GBV_ILN_2061 GBV_ILN_2064 GBV_ILN_2065 GBV_ILN_2068 GBV_ILN_2070 GBV_ILN_2086 GBV_ILN_2088 GBV_ILN_2093 GBV_ILN_2106 GBV_ILN_2107 GBV_ILN_2108 GBV_ILN_2110 GBV_ILN_2111 GBV_ILN_2112 GBV_ILN_2113 GBV_ILN_2116 GBV_ILN_2118 GBV_ILN_2119 GBV_ILN_2122 GBV_ILN_2129 GBV_ILN_2143 GBV_ILN_2144 GBV_ILN_2147 GBV_ILN_2148 GBV_ILN_2152 GBV_ILN_2153 GBV_ILN_2188 GBV_ILN_2190 GBV_ILN_2232 GBV_ILN_2336 GBV_ILN_2446 GBV_ILN_2470 GBV_ILN_2472 GBV_ILN_2507 GBV_ILN_2522 GBV_ILN_2548 GBV_ILN_4035 GBV_ILN_4037 GBV_ILN_4046 GBV_ILN_4112 GBV_ILN_4125 GBV_ILN_4242 GBV_ILN_4246 GBV_ILN_4249 GBV_ILN_4251 GBV_ILN_4305 GBV_ILN_4306 GBV_ILN_4307 GBV_ILN_4313 GBV_ILN_4322 GBV_ILN_4323 GBV_ILN_4324 GBV_ILN_4325 GBV_ILN_4326 GBV_ILN_4333 GBV_ILN_4334 GBV_ILN_4335 GBV_ILN_4336 GBV_ILN_4338 GBV_ILN_4393 GBV_ILN_4700 35.17 ASE AR 150 2019 1 29 08 21-30 |
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10.1007/s10562-019-02931-3 doi (DE-627)SPR011357398 (SPR)s10562-019-02931-3-e DE-627 ger DE-627 rakwb eng 540 660 ASE 35.17 bkl Wen, Zhenhao verfasserin aut Density Functional Theory Study of the Zeolite-Catalyzed Methylation of Benzene with Methanol 2019 Text txt rdacontent Computermedien c rdamedia Online-Ressource cr rdacarrier Abstract The reaction coordinates based on Gibbs free energies for the methylation of benzene with methanol over HZSM-5 and Hβ, both concerted and stepwise pathway, were investigated by applying density functional theory. From the estimated adsorption energies of benzene and methanol on these zeolites, stronger guest–host interactions were observed in HZSM-5 compared to Hβ. We find that at low temperatures, the concerted mechanism dominates, however, the mechanism converts to the stepwise pathway at higher temperatures. The formation of methoxy group is found to be the rate-determining step for the stepwise pathway, and the calculated free energy barriers at 673 K were 138 kJ/mol for HZSM-5 and 149 kJ/mol for Hβ, lower than those in the concerted pathway (165 kJ/mol for HZSM-5 and 168 kJ/mol for Hβ), indicating that the stepwise pathway is kinetically favored for the methylation of benzene with methanol at 673 K. Gaseous methane can be produced via one intramolecular hydrogen transfer from the ring carbon to the carbon of methyl group in the protonated toluene species, and the calculated free energy barriers for forming methane over HZSM-5 and Hβ are 112 and 100 kJ/mol, respectively, suggesting that methane is more easily formed over 12-ring Hβ catalyst. Graphic Abstract The stepwise pathway is kinetically favored for the methylation of benzene with methanol compared to concerted pathway. Methylation of benzene (dpeaa)DE-He213 Methanol conversion (dpeaa)DE-He213 HZSM-5 (dpeaa)DE-He213 Hβ (dpeaa)DE-He213 DFT (dpeaa)DE-He213 Zhu, Huayu verfasserin aut Zhu, Xuedong verfasserin aut Enthalten in Catalysis letters Dordrecht [u.a.] : Springer Science + Business Media B.V, 1988 150(2019), 1 vom: 29. Aug., Seite 21-30 (DE-627)306717638 (DE-600)1501518-X 1572-879X nnns volume:150 year:2019 number:1 day:29 month:08 pages:21-30 https://dx.doi.org/10.1007/s10562-019-02931-3 lizenzpflichtig Volltext GBV_USEFLAG_A SYSFLAG_A GBV_SPRINGER SSG-OLC-PHA GBV_ILN_11 GBV_ILN_20 GBV_ILN_22 GBV_ILN_23 GBV_ILN_24 GBV_ILN_31 GBV_ILN_32 GBV_ILN_39 GBV_ILN_40 GBV_ILN_60 GBV_ILN_62 GBV_ILN_63 GBV_ILN_65 GBV_ILN_69 GBV_ILN_70 GBV_ILN_73 GBV_ILN_74 GBV_ILN_90 GBV_ILN_95 GBV_ILN_100 GBV_ILN_101 GBV_ILN_105 GBV_ILN_110 GBV_ILN_120 GBV_ILN_138 GBV_ILN_150 GBV_ILN_151 GBV_ILN_152 GBV_ILN_161 GBV_ILN_170 GBV_ILN_171 GBV_ILN_187 GBV_ILN_213 GBV_ILN_224 GBV_ILN_230 GBV_ILN_250 GBV_ILN_281 GBV_ILN_285 GBV_ILN_293 GBV_ILN_370 GBV_ILN_602 GBV_ILN_636 GBV_ILN_702 GBV_ILN_2001 GBV_ILN_2003 GBV_ILN_2004 GBV_ILN_2005 GBV_ILN_2006 GBV_ILN_2007 GBV_ILN_2008 GBV_ILN_2009 GBV_ILN_2010 GBV_ILN_2011 GBV_ILN_2014 GBV_ILN_2015 GBV_ILN_2020 GBV_ILN_2021 GBV_ILN_2025 GBV_ILN_2026 GBV_ILN_2027 GBV_ILN_2031 GBV_ILN_2034 GBV_ILN_2037 GBV_ILN_2038 GBV_ILN_2039 GBV_ILN_2044 GBV_ILN_2048 GBV_ILN_2049 GBV_ILN_2050 GBV_ILN_2055 GBV_ILN_2057 GBV_ILN_2059 GBV_ILN_2061 GBV_ILN_2064 GBV_ILN_2065 GBV_ILN_2068 GBV_ILN_2070 GBV_ILN_2086 GBV_ILN_2088 GBV_ILN_2093 GBV_ILN_2106 GBV_ILN_2107 GBV_ILN_2108 GBV_ILN_2110 GBV_ILN_2111 GBV_ILN_2112 GBV_ILN_2113 GBV_ILN_2116 GBV_ILN_2118 GBV_ILN_2119 GBV_ILN_2122 GBV_ILN_2129 GBV_ILN_2143 GBV_ILN_2144 GBV_ILN_2147 GBV_ILN_2148 GBV_ILN_2152 GBV_ILN_2153 GBV_ILN_2188 GBV_ILN_2190 GBV_ILN_2232 GBV_ILN_2336 GBV_ILN_2446 GBV_ILN_2470 GBV_ILN_2472 GBV_ILN_2507 GBV_ILN_2522 GBV_ILN_2548 GBV_ILN_4035 GBV_ILN_4037 GBV_ILN_4046 GBV_ILN_4112 GBV_ILN_4125 GBV_ILN_4242 GBV_ILN_4246 GBV_ILN_4249 GBV_ILN_4251 GBV_ILN_4305 GBV_ILN_4306 GBV_ILN_4307 GBV_ILN_4313 GBV_ILN_4322 GBV_ILN_4323 GBV_ILN_4324 GBV_ILN_4325 GBV_ILN_4326 GBV_ILN_4333 GBV_ILN_4334 GBV_ILN_4335 GBV_ILN_4336 GBV_ILN_4338 GBV_ILN_4393 GBV_ILN_4700 35.17 ASE AR 150 2019 1 29 08 21-30 |
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Wen, Zhenhao @@aut@@ Zhu, Huayu @@aut@@ Zhu, Xuedong @@aut@@ |
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From the estimated adsorption energies of benzene and methanol on these zeolites, stronger guest–host interactions were observed in HZSM-5 compared to Hβ. We find that at low temperatures, the concerted mechanism dominates, however, the mechanism converts to the stepwise pathway at higher temperatures. The formation of methoxy group is found to be the rate-determining step for the stepwise pathway, and the calculated free energy barriers at 673 K were 138 kJ/mol for HZSM-5 and 149 kJ/mol for Hβ, lower than those in the concerted pathway (165 kJ/mol for HZSM-5 and 168 kJ/mol for Hβ), indicating that the stepwise pathway is kinetically favored for the methylation of benzene with methanol at 673 K. Gaseous methane can be produced via one intramolecular hydrogen transfer from the ring carbon to the carbon of methyl group in the protonated toluene species, and the calculated free energy barriers for forming methane over HZSM-5 and Hβ are 112 and 100 kJ/mol, respectively, suggesting that methane is more easily formed over 12-ring Hβ catalyst. 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| author |
Wen, Zhenhao |
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Wen, Zhenhao ddc 540 bkl 35.17 misc Methylation of benzene misc Methanol conversion misc HZSM-5 misc Hβ misc DFT Density Functional Theory Study of the Zeolite-Catalyzed Methylation of Benzene with Methanol |
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540 660 ASE 35.17 bkl Density Functional Theory Study of the Zeolite-Catalyzed Methylation of Benzene with Methanol Methylation of benzene (dpeaa)DE-He213 Methanol conversion (dpeaa)DE-He213 HZSM-5 (dpeaa)DE-He213 Hβ (dpeaa)DE-He213 DFT (dpeaa)DE-He213 |
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ddc 540 bkl 35.17 misc Methylation of benzene misc Methanol conversion misc HZSM-5 misc Hβ misc DFT |
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ddc 540 bkl 35.17 misc Methylation of benzene misc Methanol conversion misc HZSM-5 misc Hβ misc DFT |
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Density Functional Theory Study of the Zeolite-Catalyzed Methylation of Benzene with Methanol |
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Density Functional Theory Study of the Zeolite-Catalyzed Methylation of Benzene with Methanol |
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Wen, Zhenhao |
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Wen, Zhenhao Zhu, Huayu Zhu, Xuedong |
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density functional theory study of the zeolite-catalyzed methylation of benzene with methanol |
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Density Functional Theory Study of the Zeolite-Catalyzed Methylation of Benzene with Methanol |
| abstract |
Abstract The reaction coordinates based on Gibbs free energies for the methylation of benzene with methanol over HZSM-5 and Hβ, both concerted and stepwise pathway, were investigated by applying density functional theory. From the estimated adsorption energies of benzene and methanol on these zeolites, stronger guest–host interactions were observed in HZSM-5 compared to Hβ. We find that at low temperatures, the concerted mechanism dominates, however, the mechanism converts to the stepwise pathway at higher temperatures. The formation of methoxy group is found to be the rate-determining step for the stepwise pathway, and the calculated free energy barriers at 673 K were 138 kJ/mol for HZSM-5 and 149 kJ/mol for Hβ, lower than those in the concerted pathway (165 kJ/mol for HZSM-5 and 168 kJ/mol for Hβ), indicating that the stepwise pathway is kinetically favored for the methylation of benzene with methanol at 673 K. Gaseous methane can be produced via one intramolecular hydrogen transfer from the ring carbon to the carbon of methyl group in the protonated toluene species, and the calculated free energy barriers for forming methane over HZSM-5 and Hβ are 112 and 100 kJ/mol, respectively, suggesting that methane is more easily formed over 12-ring Hβ catalyst. Graphic Abstract The stepwise pathway is kinetically favored for the methylation of benzene with methanol compared to concerted pathway. |
| abstractGer |
Abstract The reaction coordinates based on Gibbs free energies for the methylation of benzene with methanol over HZSM-5 and Hβ, both concerted and stepwise pathway, were investigated by applying density functional theory. From the estimated adsorption energies of benzene and methanol on these zeolites, stronger guest–host interactions were observed in HZSM-5 compared to Hβ. We find that at low temperatures, the concerted mechanism dominates, however, the mechanism converts to the stepwise pathway at higher temperatures. The formation of methoxy group is found to be the rate-determining step for the stepwise pathway, and the calculated free energy barriers at 673 K were 138 kJ/mol for HZSM-5 and 149 kJ/mol for Hβ, lower than those in the concerted pathway (165 kJ/mol for HZSM-5 and 168 kJ/mol for Hβ), indicating that the stepwise pathway is kinetically favored for the methylation of benzene with methanol at 673 K. Gaseous methane can be produced via one intramolecular hydrogen transfer from the ring carbon to the carbon of methyl group in the protonated toluene species, and the calculated free energy barriers for forming methane over HZSM-5 and Hβ are 112 and 100 kJ/mol, respectively, suggesting that methane is more easily formed over 12-ring Hβ catalyst. Graphic Abstract The stepwise pathway is kinetically favored for the methylation of benzene with methanol compared to concerted pathway. |
| abstract_unstemmed |
Abstract The reaction coordinates based on Gibbs free energies for the methylation of benzene with methanol over HZSM-5 and Hβ, both concerted and stepwise pathway, were investigated by applying density functional theory. From the estimated adsorption energies of benzene and methanol on these zeolites, stronger guest–host interactions were observed in HZSM-5 compared to Hβ. We find that at low temperatures, the concerted mechanism dominates, however, the mechanism converts to the stepwise pathway at higher temperatures. The formation of methoxy group is found to be the rate-determining step for the stepwise pathway, and the calculated free energy barriers at 673 K were 138 kJ/mol for HZSM-5 and 149 kJ/mol for Hβ, lower than those in the concerted pathway (165 kJ/mol for HZSM-5 and 168 kJ/mol for Hβ), indicating that the stepwise pathway is kinetically favored for the methylation of benzene with methanol at 673 K. Gaseous methane can be produced via one intramolecular hydrogen transfer from the ring carbon to the carbon of methyl group in the protonated toluene species, and the calculated free energy barriers for forming methane over HZSM-5 and Hβ are 112 and 100 kJ/mol, respectively, suggesting that methane is more easily formed over 12-ring Hβ catalyst. Graphic Abstract The stepwise pathway is kinetically favored for the methylation of benzene with methanol compared to concerted pathway. |
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Density Functional Theory Study of the Zeolite-Catalyzed Methylation of Benzene with Methanol |
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https://dx.doi.org/10.1007/s10562-019-02931-3 |
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Zhu, Huayu Zhu, Xuedong |
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Zhu, Huayu Zhu, Xuedong |
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10.1007/s10562-019-02931-3 |
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2024-07-03T22:08:53.462Z |
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From the estimated adsorption energies of benzene and methanol on these zeolites, stronger guest–host interactions were observed in HZSM-5 compared to Hβ. We find that at low temperatures, the concerted mechanism dominates, however, the mechanism converts to the stepwise pathway at higher temperatures. The formation of methoxy group is found to be the rate-determining step for the stepwise pathway, and the calculated free energy barriers at 673 K were 138 kJ/mol for HZSM-5 and 149 kJ/mol for Hβ, lower than those in the concerted pathway (165 kJ/mol for HZSM-5 and 168 kJ/mol for Hβ), indicating that the stepwise pathway is kinetically favored for the methylation of benzene with methanol at 673 K. 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| score |
7.3997297 |