CO 2 Adsorption on Anatase TiO 2 (101) Surfaces in the Presence of Subnanometer Ag/Pt Clusters: Implications for CO 2 Photoreduction

Yang, Chi-Ta; Wood, Brandon C.; Bhethanabotla, Venkat R.; Joseph, Babu

doi:10.1021/jp509219n

Title: CO ₂ Adsorption on Anatase TiO ₂ (101) Surfaces in the Presence of Subnanometer Ag/Pt Clusters: Implications for CO ₂ Photoreduction

Journal Article · Mon Oct 20 00:00:00 EDT 2014 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/jp509219n· OSTI ID:1325872

Yang, Chi-Ta ^[1]; Wood, Brandon C. ^[2]; Bhethanabotla, Venkat R. ^[1]; Joseph, Babu ^[1]

Univ. of South Florida, Tampa, FL (United States). Dept. of Chemical and Biomedical Engineering
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States). Quantum Simulations Group

We show how CO₂ adsorption on perfect and reduced anatase TiO₂ (101) surfaces can be substantially modified by the presence of surface Ag and Pt octamer clusters, using density functional theory calculations. Furthermore, we found that adsorption was affected even at sites where the adsorbate was not in direct contact with the octamer, which we attributed to charge donation to CO₂ from the Ag/Pt-modified surface, as well as an electrostatic competition between attractive (Ti–O) and repulsive (Ti–C) interactions. Additionally, TiO₂-supported Pt octamers offer key advantages that could be leveraged for CO₂ photoreduction, including providing additional stable adsorption sites for bent CO₂ species and facilitating charge transfer to aid in CO₂– anion formation. Electronic structure analysis suggests these factors arise primarily from the hybridization of the bonding molecular orbitals of CO₂ with d orbitals of the Pt atoms. Our results show that, for adsorption on TiO₂-supported Pt octamers, the O–C–O bending and C–O asymmetric stretching frequencies can be used as reliable indicators of the presence of the CO₂– anion intermediate as well as to distinguish unique adsorption geometries or sites. Finally, we suggest a possible pathway for subsequent CO₂ dissociation to CO at the surface of a reduced anatase TiO₂ (101)-supported Pt octamer, which has a computed energy barrier of 1.01 eV.

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Research Organization:: Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC52-07NA27344

OSTI ID:: 1325872

Report Number(s):: LLNL-JRNL-659615

Journal Information:: Journal of Physical Chemistry. C, Vol. 118, Issue 45; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 53 works

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Title: CO 2 Adsorption on Anatase TiO 2 (101) Surfaces in the Presence of Subnanometer Ag/Pt Clusters: Implications for CO 2 Photoreduction

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Title: CO ₂ Adsorption on Anatase TiO ₂ (101) Surfaces in the Presence of Subnanometer Ag/Pt Clusters: Implications for CO ₂ Photoreduction