Defect-Driven Restructuring of TiO2 Surface and Modified Reactivity Toward Deposited Gold Atoms

Park, Kenneth; Meunier, Vincent; Pan, Minghu; Plummer, Ward

doi:10.3390/catal3010276

Defect-Driven Restructuring of TiO₂ Surface and Modified Reactivity Toward Deposited Gold Atoms

Journal Article · Fri Mar 08 00:00:00 EST 2013 · Catalysts

DOI:https://doi.org/10.3390/catal3010276· OSTI ID:1381896

Park, Kenneth ^[1]; Meunier, Vincent ^[2]; Pan, Minghu ^[3]; Plummer, Ward ^[4]

Baylor Univ., Waco, TX (United States)
Rensselaer Polytechnic Inst., Troy, NY (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS)
Louisiana State Univ., Baton Rouge, LA (United States)

A partially reduced TiO₂ surface exhibits increasingly complex nature when forming various defects, whose stoichiometry, structure and properties are markedly different from those of bulk TiO₂. Using scanning tunneling microscopy and density functional theory, we investigate different types of surface defects formed by Ti interstitials on TiO₂ (110) and their reactivity toward deposited gold atoms. Sub-stoichiometric strands greatly enhance bonding of Au by transferring the excess charges from the reduced Ti³⁺ onto the strands. Thus the sub-stoichiometric strands behave as strong electron donor sites toward reactants. On the contrary, fully stoichiometric nanoclusters provide increased Au bonding through its 1-coordinated oxygen, which acts as a strong electron acceptor site. Specific interactions between Au and defects as well as the implication of electron donor/acceptor complexes for catalytic reactions are discussed.

View Accepted Manuscript (DOE)

Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Center for Atomic-Level Catalyst Design (CALCD); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Oak Ridge Leadership Computing Facility (OLCF)

Sponsoring Organization:: US Army Research Laboratory (USARL); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Scientific User Facilities Division

Grant/Contract Number:: AC05-00OR22725; SC0001058

OSTI ID:: 1381896

Alternate ID(s):: OSTI ID: 1105221

Journal Information:: Catalysts, Journal Name: Catalysts Journal Issue: 1 Vol. 3; ISSN CATACJ; ISSN 2073-4344

Publisher:: MDPICopyright Statement

Country of Publication:: United States

Language:: English

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Defect-Driven Restructuring of TiO2 Surface and Modified Reactivity Toward Deposited Gold Atoms

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Defect-Driven Restructuring of TiO₂ Surface and Modified Reactivity Toward Deposited Gold Atoms