Perovskite-supported Pt single atoms for methane activation
- 27 February 2020
- journal article
- research article
- Published by Royal Society of Chemistry (RSC) in Journal of Materials Chemistry A
- Vol. 8 (8), 4362-4368
- https://doi.org/10.1039/c9ta11712a
Abstract
ABO(3) perovskites are increasingly being explored as catalysts, but it is unclear how they behave as supports for single atoms and how the subsequent single-atom catalysts can be employed for important reactions such as methane activation. Here we examine the stability of Pt single atoms (Pt-1) on the commonly exposed (100) surfaces of SrBO3 perovskites (B = 3d transition metals) and their methane-adsorption properties by first principles density functional theory. We find that the stability and charge state of Pt-1 on the SrBO3(100) surfaces are termination-sensitive. Due to polar compensation, Pt-1 is negatively charged on the A termination but positively charged on the B termination. This charge state greatly impacts methane adsorption: negatively charged Pt-1 on the A-termination chemisorbs methane (in some cases, dissociatively), but positively charged Pt-1 on the B-termination adsorbs methane physically. Analysis of the density of states of the negatively charged Pt-1 reveals that its sp states are key to methane chemisorption and C-H activation. Our work shows that polar compensation on the perovskite surfaces can be used to tune the charge state of a single atom for methane chemisorption and C-H activation.Keywords
Funding Information
- Basic Energy Sciences
- U.S. Department of Energy (DE-AC02-05CH11231)
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