Redox-active ligand controlled selectivity of vanadium oxidation on Au(100)
Abstract
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 VII to VIV, resulting in a single strongly bonded (DPTZ2-)VIVO 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 completemore »
- Authors:
-
[2];
[3];
[3];
[1];
[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
- Publication Date:
- Research Org.:
- Indiana Univ., Bloomington, IN (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1416799
- Alternate Identifier(s):
- OSTI ID: 1505532; OSTI ID: 1726279
- Grant/Contract Number:
- SC0016367
- Resource Type:
- Published Article
- Journal Name:
- Chemical Science
- Additional Journal Information:
- Journal Name: Chemical Science Journal Volume: 9 Journal Issue: 6; Journal ID: ISSN 2041-6520
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United Kingdom
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
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., and Tait, Steven L. Redox-active ligand controlled selectivity of vanadium oxidation on Au(100). United Kingdom: N. p., 2018.
Web. doi:10.1039/C7SC04752E.
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. Redox-active ligand controlled selectivity of vanadium oxidation on Au(100). United Kingdom. https://doi.org/10.1039/C7SC04752E
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., and Tait, Steven L. Mon .
"Redox-active ligand controlled selectivity of vanadium oxidation on Au(100)". United Kingdom. https://doi.org/10.1039/C7SC04752E.
@article{osti_1416799,
title = {Redox-active ligand controlled selectivity of vanadium oxidation on Au(100)},
author = {Tempas, Christopher D. and Morris, Tobias W. and Wisman, David L. and Le, Duy and Din, Naseem U. and Williams, Christopher G. and Wang, Miao and Polezhaev, Alexander V. and Rahman, Talat S. and Caulton, Kenneth G. and Tait, Steven L.},
abstractNote = {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 VII to VIV, resulting in a single strongly bonded (DPTZ2-)VIVO 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.},
doi = {10.1039/C7SC04752E},
journal = {Chemical Science},
number = 6,
volume = 9,
place = {United Kingdom},
year = {2018},
month = {1}
}
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https://doi.org/10.1039/C7SC04752E
https://doi.org/10.1039/C7SC04752E
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Cited by: 7 works
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Figures / Tables:
Scheme 1: Di-pyridinyltetrazine (DPTZ) and the M–L Polymer that forms after their redox assembly on the Au(100) surface.
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