An ab initio investigation of the adsorption properties of water on binary AlSi clusters
文献情報
Alexandre C. R. Gomes, Tiago M. de Souza, Juarez L. F. Da Silva, Breno R. L. Galvão
The potential of doped aluminium clusters as catalysts for the water splitting reaction has attracted considerable scientific effort, however, the water–cluster interactions, which are a key step in the overall mechanism, are not fully understood. Here, we report an ab initio investigation of water adsorption on AlSi clusters at the MP2 level to elucidate the bonding and structural properties employing unary and binary 8- and 13-atom clusters, namely, Si8, Al2Si6, Al4Si4, Al8, Si13, Al2Si11, Al12Si, and Al13, which were selected by their relevance and energetic stability. We found that H2O binds via the O atom near to the on-top sites of the Si or Al atoms; in particular, there is a strong preference for the Al sites on the binary AlSi clusters, which is supported by the strong adsorption energy. Furthermore, we found a large enhancement of the adsorption energy on the Al2Si6 and Al2Si11 clusters, which can be explained by the cationic character of the Al site, which increases the Coulomb contribution to the Al+–O− interaction.
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Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.










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