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 · 04 January 2018 · Chemical Science

DOI: https://doi.org/10.1039/c7sc04752e · OSTI ID:1416799

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

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^[3];

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

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Indiana Univ., Bloomington, IN (United States)
Indiana Univ., Bloomington, IN (United States); NAVSEA Crane, IN (United States)
Univ. of Central Florida, Orlando, FL (United States)
Univ. of Central Florida, Orlando, FL (United States); Donostia International Physics Center (DIPC) (Spain)

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, Vol. 9, Issue 6; ISSN 2041-6520

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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