Morphology and reactivity of size-selected titanium oxide nanoclusters on Au(111)

Goodman, Kenneth R.; Wang, Jason; Ma, Yilin; Tong, Xiao; Stacchiola, Dario J.; White, Michael G.

doi:10.1063/1.5134453

Morphology and reactivity of size-selected titanium oxide nanoclusters on Au(111)

Journal Article · Tue Feb 04 00:00:00 EST 2020 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.5134453· OSTI ID:1631942

Goodman, Kenneth R. ^[1]; Wang, Jason ^[1]; Ma, Yilin ^[1]; ^[2]; ^[2]; ^[3]

Stony Brook Univ., NY (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States)
Stony Brook Univ., NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)

The morphology and reactivity of mass-selected titania clusters, Ti₃O₆ and Ti₃O₅, deposited onto Au(111) were studied by scanning tunneling microscopy (STM) and temperature programmed desorption (TPD). Despite differing by only one oxygen atom, the stoichiometric Ti₃O₆ and the sub-stoichiometric (“reduced”) Ti₃O₅ clusters exhibit very different structures and preferred binding sites. The Ti₃O₆ clusters preferentially bind at step edges and form small assemblies (2-4 clusters) on Au terraces, while the “reduced” Ti₃O₅ clusters form much larger fractal-like assemblies that can extend across step boundaries. Annealing the Ti₃O_5,6/Au(111) systems to higher temperatures causes changes in the size-distributions of cluster assemblies but does not lead to the formation of TiO_x nanoislands for temperatures ≤ 700 K. Reactivity studies show that the reduced Ti₃O₅ cluster has higher activity than Ti₃O₆ for 2-propanol dehydration, although both clusters exhibit substantial activity for dehydrogenation to acetone. Calculations using DFT+U suggest that the differences in aggregate morphology and reactivity are associated with the number of undercoordinated Ti_3c sites in the supported clusters.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States); Energy Frontier Research Centers (EFRC) (United States). Integrated Mesoscale Architectures for Sustainable Catalysis (IMASC)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: SC0012573; SC0012704

OSTI ID:: 1631942

Alternate ID(s):: OSTI ID: 1597145

Report Number(s):: BNL--215990-2020-JAAM

Journal Information:: Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 5 Vol. 152; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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