Theoretical predictions for hexagonal BN based nanomaterials as electrocatalysts for the oxygen reduction reaction

概要

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The catalytic activity for oxygen reduction reaction (ORR) of the pristine and defected hexagonal boron nitride (h-BN) monolayer and H-terminated nanoribbon have been studied theoretically using density functional theory. It is demonstrated that inert h-BN monolayer can be functionalized and become catalytically active by nitrogen doping. It is shown that the energetics of adsorption of O2, O, OH, OOH, and H2O on N atom impurity in h-BN monolayer (N_[B]@h-BN) is quite similar to that known for Pt(111) surface. The specific mechanism of destructive and cooperative adsorption of ORR intermediates on the surface point defects is discussed. It is demonstrated that accounting for entropy and zero-point energy (ZPE) corrections results in destabilization of the ORR intermediates adsorbed on N_[B]@h-BN, while solvent effects lead to their stabilization. Therefore, entropy, ZPE and solvent effects partly cancel each other and have to be taken into account simultaneously. Analysis of the free energy changes along the ORR pathway allows us to suggest that N-doped h-BN monolayer can demonstrate catalytic properties for the ORR under condition that the electron transport to the catalytically active center is provided.
Royal Society of Chemistryの論文
2013-02-28