| Title: | Fischer-Tropsch Product Selectivity Modulation via an FeRh Nanocluster Composition Design |
| Authors: | Jhan, SM (Jhan, Sin-Mu)
Hsu, HL (Hsu, Ho-Liang)
Chang, CC (Chang, Chun-Chih)
Li, EY (Li, Elise Y.) |
| Contributors: | 化材系 |
| Keywords: | ELECTRONIC-STRUCTURE
ETHANOL SYNTHESIS
CO
IRON
NANOPARTICLES
MECHANISM
CATALYSTS
CLUSTERS
DFT
REACTIVITY |
| Date: | 2020-07-16 |
| Issue Date: | 2020-10-30 13:42:32 (UTC+8) |
| Abstract: | The reaction mechanism of *CHx formation in Fischer-Tropsch synthesis on various FeRh nanoclusters is studied using DFT calculations. We find that the energy barrier of *CH2 formation from hydrogen-assisted *CH2O dissociation can be directly modulated using the Fe/Rh composition ratio. Thermodynamic investigations and the natural bond orbital (NBO) analysis indicate that the barrier dropping of C-O bond scission in *CH2O can be ascribed to the interaction between the Fe and the O atoms. In particular, the *CH2 formation can be selectively stabilized with respect to the *CH3O formation using a local tri-Fe configuration on the FeRh nanocluster when the Fe ratio exceeds 50%. An optimal barrier may be achieved by carefully balancing the number of Rh and Fe atoms in the local configuration of the active site to stabilize both ends of the intermediates. |
| Relation: | JOURNAL OF PHYSICAL CHEMISTRY C 卷冊: 124 期: 28 頁數: 15225-15230 |
| Appears in Collections: | [Department of Chemical & Materials Engineering] journal articles
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