A kinetic study of vapor-phase cyclohexene epoxidation by H2O2 over mesoporous TS-1

Stephanie Kwon, Neil M. Schweitzer, Sunyoung Park, Peter C Stair, Randall Q. Snurr

Research output: Contribution to journalArticle

25 Citations (Scopus)

Abstract

A kinetic analysis of gas-phase cyclohexene epoxidation by H2O2 over mesoporous TS-1 was performed. The production of cyclohexene oxide was very stable with high selectivity. Based on the kinetic analysis, the gas-phase mechanism is proposed to be similar to that of the liquid-phase reaction: an Eley-Rideal type mechanism, in which the reaction between a Ti-OOH intermediate and the physisorbed alkene is the rate-determining step. When the partial pressure of water or H2O2 was varied, a compensation effect was observed. Based on the kinetic model, the compensation effect is attributed to variations in the surface coverage of intermediates, specifically the competitive adsorption of water and H2O2 at the Ti active sites. A meaningful activation energy can only be obtained at high surface coverages of H2O2 and was determined to be 40 ± 2 kJ/mol.

Original languageEnglish
Pages (from-to)107-115
Number of pages9
JournalJournal of Catalysis
Volume326
DOIs
Publication statusPublished - Jun 1 2015

Fingerprint

epoxidation
Epoxidation
Vapors
vapor phases
Kinetics
kinetics
Gases
Water
Alkenes
Partial pressure
water
alkenes
Olefins
partial pressure
liquid phases
Activation energy
selectivity
activation energy
Adsorption
adsorption

Keywords

  • Alkene
  • Compensation effect
  • Hydrogen peroxide
  • Oxidation
  • Zeolite

ASJC Scopus subject areas

  • Catalysis
  • Physical and Theoretical Chemistry

Cite this

A kinetic study of vapor-phase cyclohexene epoxidation by H2O2 over mesoporous TS-1. / Kwon, Stephanie; Schweitzer, Neil M.; Park, Sunyoung; Stair, Peter C; Snurr, Randall Q.

In: Journal of Catalysis, Vol. 326, 01.06.2015, p. 107-115.

Research output: Contribution to journalArticle

Kwon, Stephanie ; Schweitzer, Neil M. ; Park, Sunyoung ; Stair, Peter C ; Snurr, Randall Q. / A kinetic study of vapor-phase cyclohexene epoxidation by H2O2 over mesoporous TS-1. In: Journal of Catalysis. 2015 ; Vol. 326. pp. 107-115.
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