TY - JOUR
T1 - Adsorption and dehydrogenation of ethane, propane and butane on Rh13 clusters supported on unzipped graphene oxide and TiO2(110) - A DFT study
AU - Chang, Chun Chih
AU - Liu, Chi You
AU - Wu, Shiuan Yau
AU - Tsai, Ming Kang
N1 - Publisher Copyright:
© the Owner Societies 2017.
PY - 2017
Y1 - 2017
N2 - The catalytic activity for the adsorption and dehydrogenation of alkanes (CnH2n+2, n = 2, 3, 4) on a low-symmetry Rh13 cluster (Rh13-Ls) is compared with a system consisting of the same cluster (Rh13-Ls) supported on either an unzipped graphene-oxide (UGO) sheet (Rh13-Ls/UGO) or a TiO2(110) surface (Rh13-Ls/TiO2). The adsorption energies of these alkanes, calculated using density-functional theory, follow the order Rh13-Ls/TiO2 ≈ Rh13-Ls/UGO > Rh13-Ls. Our proposed reaction path for the dehydrogenation of ethane, propane and butane on Rh13-Ls/UGO has first barrier heights of 0.21, 0.22 and 0.16 eV for the dissociation of a terminal C-H bond to form -C2H5, -C3H7 and -C4H9, respectively. Compared with the barriers on Rh13-Ls and Rh13-Ls/TiO2, the barrier on Rh13-Ls/UGO is the lowest for all alkanes. The calculated data, including the electronic distribution and the density of states of alkanes adsorbed on Rh13-Ls/UGO, Rh13-Ls and Rh13-Ls/TiO2, to support our results are presented.
AB - The catalytic activity for the adsorption and dehydrogenation of alkanes (CnH2n+2, n = 2, 3, 4) on a low-symmetry Rh13 cluster (Rh13-Ls) is compared with a system consisting of the same cluster (Rh13-Ls) supported on either an unzipped graphene-oxide (UGO) sheet (Rh13-Ls/UGO) or a TiO2(110) surface (Rh13-Ls/TiO2). The adsorption energies of these alkanes, calculated using density-functional theory, follow the order Rh13-Ls/TiO2 ≈ Rh13-Ls/UGO > Rh13-Ls. Our proposed reaction path for the dehydrogenation of ethane, propane and butane on Rh13-Ls/UGO has first barrier heights of 0.21, 0.22 and 0.16 eV for the dissociation of a terminal C-H bond to form -C2H5, -C3H7 and -C4H9, respectively. Compared with the barriers on Rh13-Ls and Rh13-Ls/TiO2, the barrier on Rh13-Ls/UGO is the lowest for all alkanes. The calculated data, including the electronic distribution and the density of states of alkanes adsorbed on Rh13-Ls/UGO, Rh13-Ls and Rh13-Ls/TiO2, to support our results are presented.
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U2 - 10.1039/c6cp07130a
DO - 10.1039/c6cp07130a
M3 - Article
C2 - 27942646
AN - SCOPUS:85014305655
SN - 1463-9076
VL - 19
SP - 4989
EP - 4996
JO - Physical Chemistry Chemical Physics
JF - Physical Chemistry Chemical Physics
IS - 7
ER -