Ab initio energy calculations and macroscopic rate modeling of hydroformylation of higher alkenes by Rh-based catalyst

Ab initio quantum chemical computations have been done to determine the energetics and reaction pathways of hydroformylation of higher alkenes using a rhodium complex homogeneous catalyst. Calculation of fragments of the potential energy surfaces of the HRh(CO)(PPh<sub>3</sub>)<sub>...

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Main Authors: M.S., Shaharun, H., Mukhtar, B.K., Dutta
Format: Citation Index Journal
Language:English
Published: 2009
Subjects:
Online Access:http://scholars.utp.edu.my/id/eprint/234/
http://scholars.utp.edu.my/id/eprint/234/1/paper.pdf
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author M.S., Shaharun
H., Mukhtar
B.K., Dutta
author_facet M.S., Shaharun
H., Mukhtar
B.K., Dutta
author_sort M.S., Shaharun
building UTP Institutional Repository
collection Online Access
description Ab initio quantum chemical computations have been done to determine the energetics and reaction pathways of hydroformylation of higher alkenes using a rhodium complex homogeneous catalyst. Calculation of fragments of the potential energy surfaces of the HRh(CO)(PPh<sub>3</sub>)<sub>3</sub>-catalyzed hydroformylation of 1-decene, 1-dodecene, and styrene were performed by the restricted Hartree-Fock method at the second-order MØller-Plesset (MP2) level of perturbation theory and basis set of 6-31++G(d, p). Geometrically optimized structures of the intermediates and transition states were identified. Three generalized rate models were developed on the basis of above reaction path analysis as well as experimental findings reported in the literature. The kinetic and equilibrium parameters of the models were estimated by nonlinear least square regression of available literature data. The model based on H <sub>2</sub>-oxidative addition fitted the data best; it predicts the conversion of all the alkenes quite satisfactorily with an average deviation of 7.6% and a maximum deviation of 13%. © 2009 American Institute of Chemical Engineers.
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format Citation Index Journal
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institution Universiti Teknologi Petronas
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spelling oai:scholars.utp.edu.my:2342017-01-19T08:25:49Z http://scholars.utp.edu.my/id/eprint/234/ Ab initio energy calculations and macroscopic rate modeling of hydroformylation of higher alkenes by Rh-based catalyst M.S., Shaharun H., Mukhtar B.K., Dutta TP Chemical technology Ab initio quantum chemical computations have been done to determine the energetics and reaction pathways of hydroformylation of higher alkenes using a rhodium complex homogeneous catalyst. Calculation of fragments of the potential energy surfaces of the HRh(CO)(PPh<sub>3</sub>)<sub>3</sub>-catalyzed hydroformylation of 1-decene, 1-dodecene, and styrene were performed by the restricted Hartree-Fock method at the second-order MØller-Plesset (MP2) level of perturbation theory and basis set of 6-31++G(d, p). Geometrically optimized structures of the intermediates and transition states were identified. Three generalized rate models were developed on the basis of above reaction path analysis as well as experimental findings reported in the literature. The kinetic and equilibrium parameters of the models were estimated by nonlinear least square regression of available literature data. The model based on H <sub>2</sub>-oxidative addition fitted the data best; it predicts the conversion of all the alkenes quite satisfactorily with an average deviation of 7.6% and a maximum deviation of 13%. © 2009 American Institute of Chemical Engineers. 2009 Citation Index Journal NonPeerReviewed application/pdf en http://scholars.utp.edu.my/id/eprint/234/1/paper.pdf M.S., Shaharun and H., Mukhtar and B.K., Dutta (2009) Ab initio energy calculations and macroscopic rate modeling of hydroformylation of higher alkenes by Rh-based catalyst. [Citation Index Journal] http://www.scopus.com/inward/record.url?eid=2-s2.0-72149089349&partnerID=40&md5=a8b196c2afa18236ba346512711c55be 10.1002/aic.11936 10.1002/aic.11936 10.1002/aic.11936
spellingShingle TP Chemical technology
M.S., Shaharun
H., Mukhtar
B.K., Dutta
Ab initio energy calculations and macroscopic rate modeling of hydroformylation of higher alkenes by Rh-based catalyst
title Ab initio energy calculations and macroscopic rate modeling of hydroformylation of higher alkenes by Rh-based catalyst
title_full Ab initio energy calculations and macroscopic rate modeling of hydroformylation of higher alkenes by Rh-based catalyst
title_fullStr Ab initio energy calculations and macroscopic rate modeling of hydroformylation of higher alkenes by Rh-based catalyst
title_full_unstemmed Ab initio energy calculations and macroscopic rate modeling of hydroformylation of higher alkenes by Rh-based catalyst
title_short Ab initio energy calculations and macroscopic rate modeling of hydroformylation of higher alkenes by Rh-based catalyst
title_sort ab initio energy calculations and macroscopic rate modeling of hydroformylation of higher alkenes by rh-based catalyst
topic TP Chemical technology
url http://scholars.utp.edu.my/id/eprint/234/
http://scholars.utp.edu.my/id/eprint/234/
http://scholars.utp.edu.my/id/eprint/234/
http://scholars.utp.edu.my/id/eprint/234/1/paper.pdf