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Excess charge driven dissociative hydrogen adsorption on Ti2O4

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Abstract

The mechanism of dissociative D2 adsorption on Ti2O4, which serves as a model for an oxygen vacancy on a titania surface, is studied using infrared photodissociation spectroscopy in combination with density functional theory calculations and a recently developed single-component artificial force induced reaction method. Ti2O4 readily reacts with D2 under multiple collision conditions in a gas-filled ion trap held at 16 K forming a global minimum-energy structure (DO–Ti–(O)2–Ti(D)–O). The highly exergonic reaction proceeds quasi barrier-free via several intermediate species, involving heterolytic D2-bond cleavage followed by D-atom migration. We show that, compared to neutral Ti2O4, the excess negative charge in Ti2O4 is responsible for the substantial lowering of the D2 dissociation barrier, but does not affect the molecular D2 adsorption energy in the initial physisorption step.

Graphical abstract: Excess charge driven dissociative hydrogen adsorption on Ti2O4−

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Publication details

The article was received on 06 Jun 2017, accepted on 02 Aug 2017 and first published on 02 Aug 2017


Article type: Paper
DOI: 10.1039/C7CP03798H
Citation: Phys. Chem. Chem. Phys., 2017, Advance Article
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    Excess charge driven dissociative hydrogen adsorption on Ti2O4

    X. Song, M. R. Fagiani, S. Debnath, M. Gao, S. Maeda, T. Taketsugu, S. Gewinner, W. Schöllkopf, K. R. Asmis and A. Lyalin, Phys. Chem. Chem. Phys., 2017, Advance Article , DOI: 10.1039/C7CP03798H

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