PCCP RSCPublishing
ARTICLE
This journal is © The Royal Society of Chemistry 2013 J. Name ., 2013, 00, 1-3 | 1
Cite this: DOI: 10.1039/x0xx00000x
Received 00th January 2012,
Accepted 00th January 2012
DOI: 10.1039/x0xx00000x
www.rsc.org/
Modification of catalytic properties of the Au
4
nanocluster for the conversion of methane-to-
methanol: Synergic effects of metallic adatoms and
defective graphene support
J. Sirijaraensre
a,b
and J. Limtrakul
a,b,c,*
Table S1. ZPE-corrected relative energies of the system along the steps of the catalytic cycle for the partial oxidation of methane by N
2
O over the graphene-
deposited Au
5
catalyst. The energy of the isolated subsystems in their lowest-energy spin state is taken as zero.
Relative Energy (kcal·mol
-1
)
Steps
Doublet spin-state Quartet spin-state
Isolated systems 0.0 18.8
N
2
O adsorption -4.5 14.1
N
2
O decomposition transition state (TS1) 11.6 21.7
N
2
adsorption on Au
5
O -9.2 -2.1
N
2
desorption -5.9 1.4
CH
4
adsorption -9.4 2.0
C-H bond activation transition state (TS2) 5.9 16.8
Intermediate of C-H bond activation -32.8 -25.0
Two-centered recombination
C-O formation transition state (TS3) 7.2 10.6
One-centered recombination
CH
3
Shift transition state (TS3
B1
) -17.3 -10.1
IV
B
intermediate -20.1 -34.5
C-O formation transition state (TS3
B2
) 5.9 18.5
CH
3
OH adsorption -39.4 -20.6
CH
3
OH desorption -28.9 -10.1
Electronic Supplementary Material (ESI) for Physical Chemistry Chemical Physics.
This journal is © the Owner Societies 2015