10.1021/acsomega.6b00462.s001
Ryan Lacdao Arevalo
Ryan Lacdao
Arevalo
Susan Meñez Aspera
Susan Meñez
Aspera
Mary Clare Sison Escaño
Mary
Clare Sison Escaño
Hiroshi Nakanishi
Hiroshi
Nakanishi
Hideaki Kasai
Hideaki
Kasai
Ru-Catalyzed Steam Methane Reforming:
Mechanistic Study from First Principles Calculations
American Chemical Society
2017
activation
Ru-Catalyzed Steam Methane Reforming
First Principles Calculations Elucidating
bond
formation
SMR
CH
catalyst
O-containing species
calculation
surface
conversion
dissociative adsorption process
2017-04-05 08:19:01
Journal contribution
https://acs.figshare.com/articles/journal_contribution/Ru-Catalyzed_Steam_Methane_Reforming_Mechanistic_Study_from_First_Principles_Calculations/4817998
Elucidating the reaction
mechanism of steam methane reforming (SMR)
is imperative for the rational design of catalysts for efficient hydrogen
production. In this paper, we provide mechanistic insights into SMR
on Ru surface using first principles calculations based on dispersion-corrected
density functional theory. Methane activation (i.e., C–H bond
cleavage) was found to proceed via a thermodynamically exothermic
dissociative adsorption process, resulting in (CH<sub><i>y</i></sub> + <i>z</i>H)* species (“*” denotes
a surface-bound state, and <i>y</i> + <i>z</i> = 4), with C* and CH* being the most stable adsorbates. The calculation
of activation barriers suggests that the conversion of C* into O-containing
species via C–O bond formation is kinetically slow, indicating
that the surface reaction of carbon intermediates with oxygen is a
possible rate-determining step. The results suggest the importance
of subsequent elementary reactions following methane activation in
determining the formation of stable carbon structures on the surface
that deactivates the catalyst or the conversion of carbon into O-containing
species.