Perovskite-supported Pt single atoms for methane activation

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...

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Bibliographic Details
Published in:Journal of materials chemistry. A, Materials for energy and sustainability Materials for energy and sustainability, 2020-02, Vol.8 (8), p.4362-4368
Main Authors: Wan, Qiang, Fung, Victor, Lin, Sen, Wu, Zili, Jiang, De-en
Format: Article
Language:English
Subjects:
Activation
Adsorption
Catalysts
Chemisorption
Compensation
Density functional theory
First principles
Methane
Organic chemistry
Perovskites
Single atom catalysts
Surface chemistry
Transition metals
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Summary: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 SrBO 3 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 SrBO 3 (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. Due to polar compensation, Pt 1 is negatively charged on the A termination of SrBO 3 (100) surfaces but positively charged on the B termination, which greatly impacts methane adsorption.
ISSN:2050-7488
2050-7496
DOI:10.1039/c9ta11712a