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Title: 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 O 2. 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 O 2 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 oxidationmore » 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.« less

Authors:
 [1];  [1]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [3]; ORCiD logo [1];  [1]; ORCiD logo [1]; ORCiD logo [4]; ORCiD logo [1]; ORCiD logo [1]
  1. Indiana Univ., Bloomington, IN (United States)
  2. Indiana Univ., Bloomington, IN (United States); NAVSEA Crane, IN (United States)
  3. Univ. of Central Florida, Orlando, FL (United States)
  4. Univ. of Central Florida, Orlando, FL (United States); Donostia International Physics Center (DIPC) (Spain)
Publication Date:
Research Org.:
Indiana Univ., Bloomington, IN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1416799
Alternate Identifier(s):
OSTI ID: 1505532
Grant/Contract Number:  
SC0016367
Resource Type:
Journal Article: Published Article
Journal Name:
Chemical Science
Additional Journal Information:
Journal Volume: 9; Journal Issue: 6; Journal ID: ISSN 2041-6520
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
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 States: 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 States. 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., and Tait, Steven L. Thu . "Redox-active ligand controlled selectivity of vanadium oxidation on Au(100)". United States. doi: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},
issn = {2041-6520},
number = 6,
volume = 9,
place = {United States},
year = {2018},
month = {1}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record at 10.1039/c7sc04752e

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Cited by: 7 works
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Figures / Tables:

Scheme 1 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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