Stability of single metal atoms on defective and doped diamond surfaces Shayantan Chaudhuri 1 , Andrew J. Logsdail 2 , Reinhard J. Maurer 1,3 1 Department of Chemistry, University of Warwick, UK, 2 Cardiff Catalysis Institute, Cardiff University, Cardiff, UK, 3 Department of Physics, University of Warwick, Coventry, UK Polycrystalline boron-doped diamond is widely used as a working electrode material in electrochemistry, and its properties such as a high stability make it an appealing support material for nanostructures for electrocatalytic applications. Recent experiments have shown that electrodeposition can lead to the creation of stable small nanoclusters and even single metal adatoms on boron-doped diamond surfaces. We investigate the adsorption energy and kinetic stability of single metal atoms adsorbed onto an atomistic model of boron-doped diamond surfaces using density-functional theory. The surface model is constructed using hybrid quantum/molecular mechanics embedding techniques and is based on an oxygen-termimated (110)-oriented diamond surface. As hybrid functionals are computationally intractable for large-scale periodic surface structures, we use the hybrid quantum mechanics/molecular mechanics (QM/MM) methodology to compare different density-functional approximations on equal footing, as well as model isolated point and charge defects. We explore the effect on adsorption energetics and diffusion barriers after the introduction of defects and dopants into the substrate. Our work forms the foundations for wider efforts to model hybrid metal/carbon-based interfaces, which can be facilitated by QM/MM approaches.
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© The Author(s), 2023
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