Experimental and computational studies of formic acid dehydrogenation over PdAu

Influence of ensemble and ligand effects on catalysis

Jin Hee Lee, Jinwon Cho, Mina Jeon, Muhammad Ridwan, Hyun S. Park, Sun Hee Choi, SukWoo Nam, Jonghee Han, Tae Hoon Lim, Hyung Chul Ham, Chang Won Yoon

Research output: Contribution to journalArticle

17 Citations (Scopus)

Abstract

The critical role of the ligand effect and ensemble effect in enhancing formic acid (FA) dehydrogenation over PdAu catalysts was highlighted by both experimental and theoretical studies. FA dehydrogenation energy was calculated by DFT on PdAu model catalysts of different surface atomic arrangements. The Pd3Au1 surface exhibited the lowest reaction energy and kinetic barrier for FA dehydrogenation among four different PdAu surfaces. The Pd trimer played a critical role in stabilizing reaction intermediates. The experimental FA dehydrogenation activity of three different PdAu catalysts supported the theoretical results. In addition, the electronic interaction between the surface and subsurface layers also proved to contribute to the improved catalytic activity of PdAu catalysts via modification of Pd d states.

Original languageEnglish
Pages (from-to)14141-14147
Number of pages7
JournalJournal of Materials Chemistry A
Volume4
Issue number37
DOIs
Publication statusPublished - 2016
Externally publishedYes

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formic acid
Formic acid
Dehydrogenation
Catalysis
Ligands
Catalysts
Reaction intermediates
Catalyst supports
Discrete Fourier transforms
Catalyst activity
Kinetics

ASJC Scopus subject areas

  • Chemistry(all)
  • Renewable Energy, Sustainability and the Environment
  • Materials Science(all)

Cite this

Experimental and computational studies of formic acid dehydrogenation over PdAu : Influence of ensemble and ligand effects on catalysis. / Lee, Jin Hee; Cho, Jinwon; Jeon, Mina; Ridwan, Muhammad; Park, Hyun S.; Choi, Sun Hee; Nam, SukWoo; Han, Jonghee; Lim, Tae Hoon; Ham, Hyung Chul; Yoon, Chang Won.

In: Journal of Materials Chemistry A, Vol. 4, No. 37, 2016, p. 14141-14147.

Research output: Contribution to journalArticle

Lee, Jin Hee ; Cho, Jinwon ; Jeon, Mina ; Ridwan, Muhammad ; Park, Hyun S. ; Choi, Sun Hee ; Nam, SukWoo ; Han, Jonghee ; Lim, Tae Hoon ; Ham, Hyung Chul ; Yoon, Chang Won. / Experimental and computational studies of formic acid dehydrogenation over PdAu : Influence of ensemble and ligand effects on catalysis. In: Journal of Materials Chemistry A. 2016 ; Vol. 4, No. 37. pp. 14141-14147.
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