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Dehydrogenation of Cyclohexane on Pt(111) in a Bulb Reactor

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Abstract

The dehydrogenation of cyclohexane on Pt (111) single crystal was investigated in a bulb reactor. The volume expansion associated with the dehydrogenation of cyclohexane into benzene causes a total pressure change which was used as an index of the extent of the reaction. The validity of this reactor for kinetic studies was tested by means of CO oxidation. The dehydrogenation of cyclohexane is a reversible reaction. High temperature is favorable for dehydrogenation. By switching the temperature, the cycles of cyclohexane dehydrogenation and benzene hydrogenation were observed in this bulb reactor. The formation of carbonaceous deposits on Pt(111) surface caused a progressive loss of total pressure during the reaction cycle. A Hougen-Watson model was used to model the dehydrogenation of cylohexane on Pt(111) single crystal in the absence of deactivation. The model parameters were statistically significant and satisfied the physicochemical criteria.

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Abbreviations

CH:

Cyclohexane

BZ:

Benzene

H:

Hydrogen

CH1 :

Cyclohexene

CH2 :

Cyclohexadiene

Ai :

Frequency factor for elementary reaction step i, S−1

Ei :

Activation energy for elementary reaction step i, J/kmol

ΔG0 :

The standard free energy for the reaction, J/mol K

ΔG0 :

The standard free energy of a reacting component, J/mol/K

ΔHr :

Heat of reaction, J/mol

ΔSa 0 :

Standard adsorption entropy, J/mol K

Sa 0 :

Entropy in the gas phase, J/mol K

Sg 0 :

Entropy in the adsorbed state, J/mol K

K:

Equilibrium constant of a reaction

ki :

Reaction rate coefficient, S−1

Ki :

Adsorption equilibrium constant, bar −1

ri :

Rate of elementary reaction step i expressed in terms of TOF, S−1

T:

Temperature, K or C

Tm :

Mean temperature, K

R:

Gas constant, J/mol K

Pt 0 :

Total pressure, torr

yi 0 :

Molar fraction of the component i

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Acknowledgements

The support of this work by the Fundamental Research Funds for the Central Universities of China (Grant No. 24720094028) is gratefully acknowledged. The authors are grateful to the late Prof. D.W. Goodman and to Dr. M.S. Chen for fruitful discussions and helpful suggestions regarding the experiments.

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Authors and Affiliations

  1. Department of Chemical Engineering, China University of Petroleum Huadong, Qingdao, Shandong, 266580, China

    Bo Wang

  2. Department of Chemical Engineering, Texas A&M University, College Station, TX, 77843-3122, USA

    Gilbert F. Froment

Authors
  1. Bo Wang
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  2. Gilbert F. Froment
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Correspondence to Bo Wang.

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Wang, B., Froment, G.F. Dehydrogenation of Cyclohexane on Pt(111) in a Bulb Reactor. Catal Lett 147, 663–673 (2017). https://doi.org/10.1007/s10562-016-1946-8

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