TY - JOUR
T1 - A computational study of alkane hydrogen-exchange reactions on zeolites
AU - Zheng, Xiaobo
AU - Blowers, Paul
N1 - Funding Information:
This work was funded by the State of Arizona through the Office of the Vice President for Research at the University of Arizona. Supercomputer time was provided by the National Computational Science Alliance and used the NCSA HP/Convex Exemplar SPP-2000 at the University of Illinois at Urbana-Champaign. Part of the supercomputer time was provided by National Partnership for Advanced Computational Infrastructure and used the IBM pSeries 690 and pSeries 655 at Boston University.
PY - 2005/12/1
Y1 - 2005/12/1
N2 - In this work, quantum chemical methods were applied to study light alkane hydrogen-exchange reactions on a zeolite cluster, RH + H3SiOAlH 2(OH′)SiH3 → RH′ + H3Si(OH) AlH2OSiH3. Methane, ethane, propane, and butane reactions were investigated. The reactants, products, and transition state structures were optimized using the B3LYP density functional theory method and the final energies were calculated using CBS-QB3, a complete basis set composite energy method. The computed activation barriers ranged from 28.32 kcal/mol for secondary hydrogen exchange of butane to 33.53 kcal/mol for methane. The relationship between activation energy and deprotonation energy was also investigated and a linear correlation was proposed in this work.
AB - In this work, quantum chemical methods were applied to study light alkane hydrogen-exchange reactions on a zeolite cluster, RH + H3SiOAlH 2(OH′)SiH3 → RH′ + H3Si(OH) AlH2OSiH3. Methane, ethane, propane, and butane reactions were investigated. The reactants, products, and transition state structures were optimized using the B3LYP density functional theory method and the final energies were calculated using CBS-QB3, a complete basis set composite energy method. The computed activation barriers ranged from 28.32 kcal/mol for secondary hydrogen exchange of butane to 33.53 kcal/mol for methane. The relationship between activation energy and deprotonation energy was also investigated and a linear correlation was proposed in this work.
KW - Alkane
KW - CBS method
KW - Hydrogen exchange
KW - Zeolite
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U2 - 10.1016/j.molcata.2005.07.029
DO - 10.1016/j.molcata.2005.07.029
M3 - Article
AN - SCOPUS:27744594241
VL - 242
SP - 18
EP - 25
JO - Journal of Molecular Catalysis A: Chemical
JF - Journal of Molecular Catalysis A: Chemical
SN - 1381-1169
IS - 1-2
ER -