DFT Mechanistic Study on the Complete Oxidation of Ethylene by the Silica-Supported Pt Catalyst: C=C Activation via the Ethylene Dioxide Intermediate

Ray Miyazaki, Naoki Nakatani, Sergey V. Levchenko, Takuro Yokoya, Kiyotaka Nakajima, Kenji Hara, Atsushi Fukuoka, Jun Ya Hasegawa

Research output: Contribution to journalArticlepeer-review

11 Citations (Scopus)

Abstract

Low-temperature complete oxidation of ethylene by the mesoporous silica-supported Pt catalyst is a forefront technology for food preservation. Public implementations of the Pt catalyst have already begun, and spectroscopy analyses on the catalytic mechanism have been reported. In this study, density functional theory calculations were conducted to clarify the potential energy profile and electronic mechanism of the catalytic reaction. Based on the experimental findings, a reaction pathway was proposed for ethylene oxidation up to CO2 formation via the HCHO intermediate. Among several possibilities, a reaction pathway via ethylene dioxide species is energetically plausible for the C-C bond cleavage to generate HCHO. Particular focus was given to the electronic effect of the silica support in the ethylene dioxide route. The reservoir effect, in which the siloxide groups take electrons from the Pt moiety, reduces the activation energy of the C-C bond cleavage step by taking electrons from the σ(C-C) orbital.

Original languageEnglish
Pages (from-to)12706-12715
Number of pages10
JournalJournal of Physical Chemistry C
Volume123
Issue number20
DOIs
Publication statusPublished - 23 May 2019

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