Redox-active ligand controlled selectivity of vanadium oxidation on Au(100)

Tempas, Christopher D.; Morris, Tobias W.; Wisman, David L.; Le, Duy; Din, Naseem U.; Williams, Christopher G.; Wang, Miao; Polezhaev, Alexander V.; Rahman, Talat S.; Caulton, Kenneth G.; Tait, Steven L.

doi:10.1039/C7SC04752E

Title: Redox-active ligand controlled selectivity of vanadium oxidation on Au(100)

Journal Article · Mon Jan 01 00:00:00 EST 2018 · Chemical Science

DOI:https://doi.org/10.1039/C7SC04752E· OSTI ID:1416799

Tempas, Christopher D. ^[1]; Morris, Tobias W. ^[1];

^[2];

^[3];

^[1]; Wang, Miao ^[4];

^[1];

^[5];

^[1];

^[6]

Department of Chemistry, Indiana University, Bloomington, USA
Department of Chemistry, Indiana University, Bloomington, USA, NAVSEA Crane
Department of Physics, University of Central Florida, Orlando, USA
Department of Physics, Indiana University, Bloomington, USA
Department of Physics, University of Central Florida, Orlando, USA, Donostia International Physics Center (DIPC)
Department of Chemistry, Indiana University, Bloomington, USA, Department of Physics

Metal–organic coordination networks at surfaces, formed by on-surface redox assembly, are of interest for designing specific and selective chemical function at surfaces for heterogeneous catalysts and other applications. The chemical reactivity of single-site transition metals in on-surface coordination networks, which is essential to these applications, has not previously been fully characterized. Here, we demonstrate with a surface-supported, single-site V system that not only are these sites active toward dioxygen activation, but the products of that reaction show much higher selectivity than traditional vanadium nanoparticles, leading to only one V-oxo product. We have studied the chemical reactivity of one-dimensional metal–organic vanadium – 3,6-di(2-pyridyl)-1,2,4,5-tetrazine (DPTZ) chains with O₂. The electron-rich chains self-assemble through an on-surface redox process on the Au(100) surface and are characterized by X-ray photoelectron spectroscopy, scanning tunneling microscopy, high-resolution electron energy loss spectroscopy, and density functional theory. Reaction of V-DPTZ chains with O₂ causes an increase in V oxidation state from V^II to V^IV, resulting in a single strongly bonded (DPTZ^2-)V^IVO product and spillover of O to the Au surface. DFT calculations confirm these products and also suggest new candidate intermediate states, providing mechanistic insight into this on-surface reaction. In contrast, the oxidation of ligand-free V is less complete and results in multiple oxygen-bound products. This demonstrates the high chemical selectivity of single-site metal centers in metal–ligand complexes at surfaces compared to metal nanoislands.

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Research Organization:: Indiana Univ., Bloomington, IN (United States)

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

Grant/Contract Number:: SC0016367

OSTI ID:: 1416799

Alternate ID(s):: OSTI ID: 1505532; OSTI ID: 1726279

Journal Information:: Chemical Science, Journal Name: Chemical Science Vol. 9 Journal Issue: 6; ISSN 2041-6520

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United Kingdom

Language:: English

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Cited by: 21 works

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