First-Principles Free-Energy Barriers for Photoelectrochemical Surface 
Reactions: Proton Abstraction at TiO2(110)

Stecher, Thomas; Reuter, Karsten; Oberhofer, Harald

doi:/10.1103/PhysRevLett.117.276001

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First-Principles Free-Energy Barriers for Photoelectrochemical Surface Reactions: Proton Abstraction at TiO₂(110)

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Stecher, T., Reuter, K., & Oberhofer, H. (2016). First-Principles Free-Energy Barriers for Photoelectrochemical Surface Reactions: Proton Abstraction at TiO₂(110). Physical Review Letters, 117(27): 276001. doi:/10.1103/PhysRevLett.117.276001.

Cite as: https://hdl.handle.net/21.11116/0000-000A-AC28-8

Abstract

We explicitly calculate the free-energy barrier for the initial proton abstraction in the water splitting reaction at rutile TiO₂(110) through ab initio molecular dynamics. Combining solid-state embedding, an energy based reaction coordinate and state-of-the-art free-energy reconstruction techniques renders the calculation tractable at the hybrid density-functional theory level. The obtained free-energy barrier of approximately 0.2 eV, depending slightly on the orientation of the first acceptor water molecule, suggests a hindered reaction on the pristine rutile surface.