Cho, Jinwon Lee, Sangheon Han, Jonghee Yoon, Sung Pil Nam, Suk Woo Choi, Sun Hee Hong, Seong-Ahn Lee, Kwan-Young Ham, Hyung Chul 2024-01-20T06:02:14Z 2024-01-20T06:02:14Z 2021-09-05 2015-10 1533-4880 https://pubs.kist.re.kr/handle/201004/124930 In this study, using spin-polarized density functional theory calculation we examined the origin of enhanced catalytic activity toward H-2 production from HCOOH in Ag-19@Pd-60 core shell nanoclusters (a 79-atom truncated octahedral cluster models). First, we find that the Pd monolayer shell on the Ag core can greatly enhance the selectivity to H-2 formation via HCOOH decomposition compared to the pure Pd-79 cluster by substantially reducing the binding energy of key intermediate HCOO and in turn the barrier for dehydrogenation. This activity enhancement is related to the modification of d states in the Pd monolayer shell by the strong ligand effect between Ag core and Pd shell, rather than the tensile strain effect by Ag core. In particular, the absence of dz(2)-r(2) density of states near the Fermi level in the Pd monolayer shell (which originated from the substantial charge transfer from Ag to Pd) is the main reason for the increased H-2 production from HCOOH decomposition. English AMER SCIENTIFIC PUBLISHERS FORMIC-ACID DECOMPOSITION HYDROGEN PD CATALYST DFT Enhanced Selectivity to H-2 Formation in Decomposition of HCOOH on the Ag-19@Pd-60 Core-Shell Nanocluster from First-Principles Article 10.1166/jnn.2015.11442 1 JOURNAL OF NANOSCIENCE AND NANOTECHNOLOGY, v.15, no.10, pp.8233 - 8237 JOURNAL OF NANOSCIENCE AND NANOTECHNOLOGY 15 10 8233 8237 scie scopus 000365554600150 2-s2.0-84947286928 Chemistry, Multidisciplinary Nanoscience & Nanotechnology Materials Science, Multidisciplinary Physics, Applied Physics, Condensed Matter Chemistry Science & Technology - Other Topics Materials Science Physics Article FORMIC-ACID DECOMPOSITION HYDROGEN PD CATALYST DFT First-Principles Ag-Pd Core-Shell H-2 Formation HCOOH Selectivity