Multi-electron Reduction Capacity and Multiple Binding Pockets in Metal–Organic Redox Assembly at Surfaces
Abstract
Abstract Metal–ligand complexation at surfaces utilizing redox‐active ligands has been demonstrated to produce uniform single‐site metals centers in regular coordination networks. Two key design considerations are the electron storage capacity of the ligand and the metal‐coordinating pockets on the ligand. In an effort to move toward greater complexity in the systems, particularly dinuclear metal centers, we designed and synthesized tetraethyltetra‐aza‐anthraquinone, TAAQ, which has superior electron storage capabilities and four ligating pockets in a diverging geometry. Cyclic voltammetry studies of the free ligand demonstrate its ability to undergo up to a four‐electron reduction. Solution‐based studies with an analogous ligand, diethyldi‐aza‐anthraquinone, demonstrate these redox capabilities in a molecular environment. Surface studies conducted on the Au(111) surface demonstrate TAAQ′s ability to complex with Fe. This complexation can be observed at different stoichiometric ratios of Fe:TAAQ as Fe 2p core level shifts in X‐ray photoelectron spectroscopy. Scanning tunneling microscopy experiments confirmed the formation of metal–organic coordination structures. The striking feature of these structures is their irregularity, which indicates the presence of multiple local binding motifs. Density functional theory calculations confirm several energetically accessible Fe:TAAQ isomers, which accounts for the non‐uniformity of the chains.
- Authors:
-
- Indiana Univ., Bloomington, IN (United States). Dept. of Chemistry
- Indiana Univ., Bloomington, IN (United States). Dept. of Physics
- Indiana Univ., Bloomington, IN (United States). Dept. of Chemistry; Naval Sea Systems Command (NAVSEA) Crane, IN (United States)
- Univ. of Central Florida, Orlando, FL (United States). Dept. of Physics
- Indiana Univ., Bloomington, IN (United States). Dept. of Chemistry and Physics
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1529239
- Alternate Identifier(s):
- OSTI ID: 1501742
- Grant/Contract Number:
- SC0016367
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Chemistry - A European Journal
- Additional Journal Information:
- Journal Volume: 25; Journal Issue: 21; Journal ID: ISSN 0947-6539
- Publisher:
- ChemPubSoc Europe
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Morris, Tobias W., Huerfano, I. J., Wang, Miao, Wisman, David L., Cabelof, Alyssa C., Din, Naseem U., Tempas, Christopher D., Le, Duy, Polezhaev, Alexander V., Rahman, Talat S., Caulton, Kenneth G., and Tait, Steven L. Multi-electron Reduction Capacity and Multiple Binding Pockets in Metal–Organic Redox Assembly at Surfaces. United States: N. p., 2019.
Web. doi:10.1002/chem.201900002.
Morris, Tobias W., Huerfano, I. J., Wang, Miao, Wisman, David L., Cabelof, Alyssa C., Din, Naseem U., Tempas, Christopher D., Le, Duy, Polezhaev, Alexander V., Rahman, Talat S., Caulton, Kenneth G., & Tait, Steven L. Multi-electron Reduction Capacity and Multiple Binding Pockets in Metal–Organic Redox Assembly at Surfaces. United States. https://doi.org/10.1002/chem.201900002
Morris, Tobias W., Huerfano, I. J., Wang, Miao, Wisman, David L., Cabelof, Alyssa C., Din, Naseem U., Tempas, Christopher D., Le, Duy, Polezhaev, Alexander V., Rahman, Talat S., Caulton, Kenneth G., and Tait, Steven L. Mon .
"Multi-electron Reduction Capacity and Multiple Binding Pockets in Metal–Organic Redox Assembly at Surfaces". United States. https://doi.org/10.1002/chem.201900002. https://www.osti.gov/servlets/purl/1529239.
@article{osti_1529239,
title = {Multi-electron Reduction Capacity and Multiple Binding Pockets in Metal–Organic Redox Assembly at Surfaces},
author = {Morris, Tobias W. and Huerfano, I. J. and Wang, Miao and Wisman, David L. and Cabelof, Alyssa C. and Din, Naseem U. and Tempas, Christopher D. and Le, Duy and Polezhaev, Alexander V. and Rahman, Talat S. and Caulton, Kenneth G. and Tait, Steven L.},
abstractNote = {Abstract Metal–ligand complexation at surfaces utilizing redox‐active ligands has been demonstrated to produce uniform single‐site metals centers in regular coordination networks. Two key design considerations are the electron storage capacity of the ligand and the metal‐coordinating pockets on the ligand. In an effort to move toward greater complexity in the systems, particularly dinuclear metal centers, we designed and synthesized tetraethyltetra‐aza‐anthraquinone, TAAQ, which has superior electron storage capabilities and four ligating pockets in a diverging geometry. Cyclic voltammetry studies of the free ligand demonstrate its ability to undergo up to a four‐electron reduction. Solution‐based studies with an analogous ligand, diethyldi‐aza‐anthraquinone, demonstrate these redox capabilities in a molecular environment. Surface studies conducted on the Au(111) surface demonstrate TAAQ′s ability to complex with Fe. This complexation can be observed at different stoichiometric ratios of Fe:TAAQ as Fe 2p core level shifts in X‐ray photoelectron spectroscopy. Scanning tunneling microscopy experiments confirmed the formation of metal–organic coordination structures. The striking feature of these structures is their irregularity, which indicates the presence of multiple local binding motifs. Density functional theory calculations confirm several energetically accessible Fe:TAAQ isomers, which accounts for the non‐uniformity of the chains.},
doi = {10.1002/chem.201900002},
journal = {Chemistry - A European Journal},
number = 21,
volume = 25,
place = {United States},
year = {Mon Mar 18 00:00:00 EDT 2019},
month = {Mon Mar 18 00:00:00 EDT 2019}
}
Web of Science
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