10.1021/acs.jpca.5b04737.s001
Chen-Chi Lee
Chen-Chi
Lee
Hsin-Tsung Chen
Hsin-Tsung
Chen
Adsorption and Reaction of C<sub>2</sub>H<sub>4</sub> and O<sub>2</sub> on a Nanosized Gold Cluster: A Computational Study
American Chemical Society
2015
reaction mechanisms
38 nanoparticle
LH
C 2H
Nanosized Gold Cluster
eV
calculation results show
NEB
DFT
O 2
LDOS
ethylene
adsorption
2015-08-06 00:00:00
Journal contribution
https://acs.figshare.com/articles/journal_contribution/Adsorption_and_Reaction_of_C_sub_2_sub_H_sub_4_sub_and_O_sub_2_sub_on_a_Nanosized_Gold_Cluster_A_Computational_Study/2143504
We
have investigated the adsorption and reaction mechanisms of
C<sub>2</sub>H<sub>4</sub> and O<sub>2</sub> catalyzed by a Au<sub>38</sub> nanoparticle based on periodic density-functional theory
(DFT) calculations. The configurations of the adsorption of C<sub>2</sub>H<sub>4</sub>/Au<sub>38</sub>, O<sub>2</sub>/Au<sub>38</sub>, and O/Au<sub>38</sub> as well as the coadsorption of C<sub>2</sub>H<sub>4</sub>–O<sub>2</sub>/Au<sub>38</sub> were predicted.
The calculation results show that C<sub>2</sub>H<sub>4</sub>, O<sub>2</sub>, and O are preferably bound at top (T), bridge (B), and hexagonal
(h) sites with adsorption energies of −0.66, −0.99,
and −3.93 eV, respectively. The detailed reaction mechanisms
for ethylene epoxidation on the Au<sub>38</sub> nanoparticle has been
illustrated using the nudged elastic band (NEB) method. The oxidation
process takes place via the Langmuir–Hinshelwood (LH) mechanism
to generate ethylene oxide and acetaldehyde. The overall reaction
of C<sub>2</sub>H<sub>4</sub> + O<sub>2</sub> + Au<sub>38</sub> →
ethylene oxide + O/Au<sub>38</sub> is exothermic by 2.20–2.40
eV whereas those are 3.03–3.08 eV for the production of acetaldehyde
and O/Au<sub>38</sub>. The nature of the interaction between the adsorbate
and gold nanocluster has been analyzed by the detailed electronic
local density of states (LDOS) to understand the high catalytic activity
of the gold nanoclusters.