| 학회 |
한국화학공학회 |
| 학술대회 |
2014년 가을 (10/22 ~ 10/24, 대전 DCC) |
| 권호 |
20권 2호, p.2261 |
| 발표분야 |
촉매 및 반응공학 |
| 제목 |
The First-Principles approach to the interplay of Ligand Effect in Enhanced Dehydrogenation of HCOOH on the Bimetallic Pd-M Catalyst |
| 초록 |
The critical role of the Ag-Pd ligand effect (which is tuned by changing the number of Pd atomic layers) in determining the dehydrogenation and dehydration of HCOOH on the bimetallic Pd/Ag catalysts was elucidated by using the spin-polarized density functional theory (DFT) calculations. Our calculations suggest that the productivity and selectivity to H2 production from HCOOH on the bimetallic Pd/Ag catalysts strongly depends on the Pd atomic layer thickness at near surface. In particular, the thinnest Pd monolayer in the Pd/Ag system is responsible for enhancing the dehydrogenation of HCOOH toward H2 production by reducing the surface binding strength of specific intermediates such as HCOO and HCO. The dominant Ag-Pd ligand effect by the substantial charge donation to the Pd surface from the subsurface Ag [which significantly reduce the density of state (particularly, dz2–r2 orbital) near the Fermi level] proves to be a key factor for the enhanced kinetics of dehydrogenation, whereas the expansive (tensile) strain imposed by the underlying Ag substrate plays a minor role. This work hints on the importance of properly engineering the surface activity of the Ag-Pd core-shell catalysts by the interplay between ligand and strain effects. |
| 저자 |
조진원1, 이상헌1, 한종희1, 이관영2, 함형철1
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| 소속 |
1한국과학기술(연), 2고려대 |
| 키워드 |
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| E-Mail |
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| 원문파일 |
초록 보기 |
