Submonolayer Is Enough: Switching Reaction Channels on Pt/SiO2 by Atomic Layer Deposition

Tang, Xin; Liu, Chao; Long, Edmund A.; Lin, Wei; Hackler, Ryan A.; Wang, Xiang; Marks, Laurence D.; Notestein, Justin M.; Stair, Peter C.

doi:10.1021/acs.jpcc.1c04972

Title: Submonolayer Is Enough: Switching Reaction Channels on Pt/SiO₂ by Atomic Layer Deposition

Journal Article · 23 August 2021 · Journal of Physical Chemistry. C

DOI: https://doi.org/10.1021/acs.jpcc.1c04972 · OSTI ID:2482454

Tang, Xin ^[1]; Liu, Chao ^[1]; Long, Edmund A. ^[1];

^[1];

^[1]

Northwestern University, Evanston, IL (United States)

The reaction mechanism of CO₂ with H₂ is studied on platinum nanoparticles supported on fumed silica. It is found that platinum nanoparticle size, reaction temperature, and metal oxide promoters play important roles in determining the reaction rate and the mechanism of forming surface carbonyl species. Metal oxide promoters consist of sub-monolayer titanium oxide or aluminum oxide overcoated onto the catalysts by atomic layer deposition (ALD). Furthermore, these alter the CO formation rate, influence the adsorption and desorption behavior, and switch the surface reaction channel from Eley-Rideal to Langmuir-Hinshelwood mechanism due to an enhancement of CO₂ affinity to the metal-metal oxide interface. At the temperatures relevant for catalytic turnover, ALD overcoating significantly increases catalytic activity in CO₂ hydrogenation to CH₄ and CO, while the identity of the oxide overcoat helps control product selectivity.

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Research Organization:: Northwestern University, Evanston, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: FG02-03ER15457

OSTI ID:: 2482454

Journal Information:: Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Journal Issue: 34 Vol. 125; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Title: Submonolayer Is Enough: Switching Reaction Channels on Pt/SiO2 by Atomic Layer Deposition

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Title: Submonolayer Is Enough: Switching Reaction Channels on Pt/SiO₂ by Atomic Layer Deposition