The effects of near-surface atomic order on the catalytic properties of Cu3Au and CuAu3 intermetallics for the CO2 reduction reaction
文献信息
Yunzhe Wang, Juarez L. F. Da Silva, Tim Mueller
Density functional theory (DFT) calculations combined with cluster expansions (CE) were employed to explore the catalytic activity of stoichiometric and non-stoichiometric Cu3Au(100), Cu3Au(111), CuAu3(100), and CuAu3(111) surfaces for CO2 reduction to CO. We identified several adsorption sites which otherwise would not be considered using slab models generated by cleaving ordered bulk structures. For Cu3Au(111) and CuAu3(111), the adsorption sites with the highest and lowest estimated onset potential values found through our approach would be missed if modeled from bulk-derived slabs, showing the ability of our strategy to explore the richness of alloy catalysts that arises from the formation of near-surface atomic ordering effects. Finally, we performed simulated annealing calculations based on CE fit to predict CO and COOH adsorption energies. This analysis led us to find adsorption site ensembles that can deviate from the linear scaling relationship that usually hinders the discovery of more active and selective catalysts for CO production.
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Catalysis Science & Technology

Catalysis Science & Technology is committed to publishing research reporting high-quality, cutting-edge developments across the catalysis community at large. The journal places equal focus on publications from the heterogeneous, homogeneous, thermo-, electro-, photo-, organo- and biocatalysis communities. Works published in the journal feature a balanced mix of fundamental, technology-oriented, experimental, computational, digital and data-driven original research, thus appealing to catalysis practitioners in both academic and industrial environments. Original research articles published in the journal must demonstrate new catalytic discoveries and/or methodological advances that represent a significant advance on previously published work, from the molecular to the process scales. We welcome rigorous research in a wide range of timely or emerging applications related to the environment, health, energy and materials. Catalysis Science & Technology publishes Communications, Articles, Reviews and Perspectives. More details regarding manuscript types may be found in the Information for Authors section.













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