Stabilizing Single-Atom and Small-Domain Platinum via Combining Organometallic Chemisorption and Atomic Layer Deposition

Shengsi Liu, J. Miles Tan, Ahmet Gulec, Lawrence A. Crosby, Tasha L. Drake, Neil M. Schweitzer, Massimiliano Delferro, Laurence D. Marks, Tobin J Marks, Peter C Stair

Research output: Contribution to journalArticle

7 Citations (Scopus)

Abstract

Oxide-supported single-atom Pt materials are prepared by combining surface organometallic chemisorption with atomic layer deposition (ALD). Here Pt is supported as a discrete monatomic "pincer" complex, stabilized by an atomic layer deposition (ALD) derived oxide overcoat, and then calcined at 400 °C under O2. ALD-derived Al2O3, TiO2, and ZnO overlayers are effective in suppressing Pt sintering and significantly stabilizing single Pt atoms. Furthermore, this procedure decreases the overall Pt nuclearity (∼1 nm average particle diameter) versus bare Pt (∼3.8 nm average diameter), as assayed by aberration corrected HAADF-STEM. The TiO2 and ZnO overcoats are significantly more effective at stabilizing single-atom Pt species and decreasing the overall Pt nuclearity than Al2O3 overcoats. Vibrational spectroscopy of adsorbed CO also shows that oxidized Pt species commonly thought to be single Pt atoms are inactive for catalytic oxidation of adsorbed CO. CO chemisorption measurements show site blockage by the ALD overcoats.

Original languageEnglish
Pages (from-to)818-828
Number of pages11
JournalOrganometallics
Volume36
Issue number4
DOIs
Publication statusPublished - Feb 27 2017

Fingerprint

Atomic layer deposition
Organometallics
Chemisorption
atomic layer epitaxy
Platinum
chemisorption
platinum
Carbon Monoxide
Atoms
Oxides
atoms
Vibrational spectroscopy
oxides
Catalytic oxidation
Aberrations
aberration
sintering
Sintering
oxidation
spectroscopy

ASJC Scopus subject areas

  • Physical and Theoretical Chemistry
  • Organic Chemistry
  • Inorganic Chemistry

Cite this

Stabilizing Single-Atom and Small-Domain Platinum via Combining Organometallic Chemisorption and Atomic Layer Deposition. / Liu, Shengsi; Tan, J. Miles; Gulec, Ahmet; Crosby, Lawrence A.; Drake, Tasha L.; Schweitzer, Neil M.; Delferro, Massimiliano; Marks, Laurence D.; Marks, Tobin J; Stair, Peter C.

In: Organometallics, Vol. 36, No. 4, 27.02.2017, p. 818-828.

Research output: Contribution to journalArticle

Liu, Shengsi ; Tan, J. Miles ; Gulec, Ahmet ; Crosby, Lawrence A. ; Drake, Tasha L. ; Schweitzer, Neil M. ; Delferro, Massimiliano ; Marks, Laurence D. ; Marks, Tobin J ; Stair, Peter C. / Stabilizing Single-Atom and Small-Domain Platinum via Combining Organometallic Chemisorption and Atomic Layer Deposition. In: Organometallics. 2017 ; Vol. 36, No. 4. pp. 818-828.
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