Atomic-Scale Structure and Catalysis on Positively Charged Bimetallic Sites for Generation of H2

Yu Tang, Shiran Zhang, Takat B. Rawal, Luan Nguyen, Yasuhiro Iwasawa, Shree R. Acharya, Jingyue Liu, Sampyo Hong, Talat S. Rahman, Franklin Tao

Research output: Contribution to journalArticlepeer-review

8 Scopus citations


Here, we report that a cationic bimetallic site consisting of one Pd and three Zn atoms (Pd1Zn3) supported on ZnO (Pd1Zn3/ZnO) exhibits an extraordinarily high catalytic activity for the generation of H2 through methanol partial oxidation (MPO) that is 2-3 orders of magnitude higher than that of a metallic Pd-Zn site on Pd-Zn nanoalloy (Pd-Zn/ZnO). Computational studies uncovered that the positively charged Pd atom of the subnanometer Pd1Zn3 bimetallic site largely decreases the activation barrier for dehydrogenation of methanol as compared to a metallic Pd atom of Pd-Zn alloy, thus switching the rate-determining step of MPO from methanol dehydrogenation over a Pd-Zn alloy with high barrier to the O2 dissociation step on a cationic Pd1Zn3 site with a low barrier, which is supported by our kinetics studies. The significantly higher catalytic activity and selectivity for H2 production over a cationic bimetallic site suggest a new approach to design bimetallic catalysts.

Original languageEnglish (US)
Pages (from-to)6255-6262
Number of pages8
JournalNano Letters
Issue number9
StatePublished - Sep 9 2020


  • bimetallic site
  • catalytic activity
  • hydrogen
  • nanocatalysis
  • palladium
  • single-atom catalyst

ASJC Scopus subject areas

  • Bioengineering
  • Chemistry(all)
  • Materials Science(all)
  • Condensed Matter Physics
  • Mechanical Engineering


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