Abstract
We developed an efficient and convenient electrochemical method to synthesize π-conjugated redox metal-complex linear polymer wires composed of azobenzene-bridged bis(terpyridine)metal (2-M, M = Fe, Ru) units covalently immobilized on glassy carbon (GC). Polymerization proceeds by electrochemical oxidation of bis(4′-(4-anilino)-2,2′:6′,2″-terpyridine)metal (1-M) in a water–acetonitrile–HClO4 solution, affording ultralong wires up to 7400 mers (corresponding to ca. 15 μm). Both 2-Fe and 2-Ru undergo reversible redox reactions, and their redox behaviors indicate remarkably fast redox conduction. Anisotropic hetero-metal-complex polymer wires with Fe and Ru centers are constructed via stepwise electropolymerization. The cyclic voltammograms of two hetero-metal-complex polymer wires, GC/[2-Fe]–[2-Ru] (3) and GC/[2-Ru]–[2-Fe] (4), show irreversible redox reactions with opposite electron transfer characteristics, indicating redox diodelike behavior. In short, the present electrochemical method is useful to synthesize polymer wire arrays and to integrate functional molecules on carbon.
Highlights
IntroductionMolecular wires are long molecules that allow electrons or holes to flow smoothly within them, thereby acting as molecular-scale, electrically conductive wires
Molecular wires are long molecules that allow electrons or holes to flow smoothly within them, thereby acting as molecular-scale, electrically conductive wires. They are one of the most important components of molecular-scale electronics for molecular or quantum computing [1,2,3,4,5,6,7,8,9]. Their preparation faces two major challenges: achieving precise control of their lengths and structures when immobilized on electrodes and synthesizing wires long enough to link and integrate large numbers of functional molecular units to obtain high-performance devices [10,11,12,13,14,15,16,17,18,19,20,21,22,23,24,25,26,27,28,29,30,31,32]
We describe the electrochemical synthesis, characterization, and elecelectrochemical properties of π-conjugated homohetero-metal-complex linear polytrochemical properties of π-conjugated homoandand hetero-metal-complex linear polymer mer wires to demonstrate the general versatility of this method to construct polymer wires to demonstrate the general versatility of this method to construct polymer wirewire ararrays with integrated functionalities on carbon
Summary
Molecular wires are long molecules that allow electrons or holes to flow smoothly within them, thereby acting as molecular-scale, electrically conductive wires. Stepwise coordination is a good solution to the first challenge It involves synthesis of a series of linear and branched π-conjugated bis(terpyridine)metal complex oligomer wires with precise lengths and specific structures on gold or silicon electrodes [33,34,35,36,37,38,39,40]. These wires have shown excellent long-range electron transfer, high redox conductivity, and good redox cyclability, making them promising components for molecular electronics. It is essential to find new, simpler methods to construct long molecular wires
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