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- Merte, Lindsay R., et al.
(författare)
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Structure of an Ultrathin Oxide on Pt3Sn(111) Solved by Machine Learning Enhanced Global Optimization
- 2022
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Ingår i: Angewandte Chemie International Edition. - : John Wiley & Sons. - 1433-7851 .- 1521-3773. ; 61:25, s. 1-7
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Tidskriftsartikel (refereegranskat)abstract
- Determination of the atomic structure of solid surfaces typically depends on comparison of measured properties with simulations based on hypothesized structural models. For simple structures, the models may be guessed, but for more complex structures there is a need for reliable theory-based search algorithms. So far, such methods have been limited by the combinatorial complexity and computational expense of sufficiently accurate energy estimation for surfaces. However, the introduction of machine learning methods has the potential to change this radically. Here, we demonstrate how an evolutionary algorithm, utilizing machine learning for accelerated energy estimation and diverse population generation, can be used to solve an unknown surface structure-the (4×4) surface oxide on Pt3Sn(111)-based on limited experimental input. The algorithm is efficient and robust, and should be broadly applicable in surface studies, where it can replace manual, intuition based model generation.
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| 2. |
- Merte, Lindsay R., et al.
(författare)
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Oxygen Storage by Tin Oxide Monolayers on Pt3Sn(111)
- 2023
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Ingår i: The Journal of Physical Chemistry C. - : American Chemical Society (ACS). - 1932-7447 .- 1932-7455. ; 127:6, s. 2988-2994
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Tidskriftsartikel (refereegranskat)abstract
- The high performance of platinum–tin catalysts for oxidation reactions has been linked to the formation of tin oxides at the metal surface, but little is known about the structure of these oxides or the chemical behavior that determines their catalytic properties. We show here how surface oxides on Pt3Sn(111) incorporate oxygen at the metal interface, which may be subsequently removed by reaction with CO. The storage mechanism, where oxygen uptake occurs without loss of interfacial Pt–Sn bonds, is enabled by the peculiar asymmetrical coordination state of Sn2+. O atoms are bound at pocket sites in the 2D oxide sheet between these outward-buckled Sn atoms and metallic Sn in the alloy surface below.
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