期刊
CHEMISTRY-A EUROPEAN JOURNAL
卷 25, 期 21, 页码 5565-5573出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.201900002
关键词
density functional calculations; metal-organic coordination; on-surface redox assembly; scanning tunneling microscopy; supramolecular self-assembly
资金
- National Science Foundation [CHE-1465105, CHE-1610984]
- US Department of Energy, Office of Basic Energy Sciences, Chemical Sciences program [DE-SC0016367]
- United States Department of Defense Naval Surface Warfare Center, Crane Division under the Naval Innovative Science and Engineering
- U.S. Department of Energy (DOE) [DE-SC0016367] Funding Source: U.S. Department of Energy (DOE)
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-anthraqui- none, 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.
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