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Surface-Immobilized Conjugated Polymers Incorporating Rhenium Bipyridine Motifs for Electrocatalytic and Photocatalytic CO <sub/>2</sub> Reduction
摘要： The solar-driven conversion of CO2 to value-added products provides a promising route for solar energy storage and atmospheric CO2 remediation. In this report, a variety of supporting electrode materials were successfully modified with a [2,2′-bipyridine]-5,5′-bis(diazonium) rhenium complex through a surface-localized electropolymerization method. Physical characterization of the resulting multilayer films confirms that the coordination environments of the rhenium bipyridine tricarbonyl sites are preserved upon immobilization and that the polymerized catalyst moieties exhibit long-range structural order with uniform film growth. UV?vis studies reveal additional absorption bands in the visible region for the polymeric films that are not present in the analogous rhenium bipyridine complexes. Electrochemical studies with modified graphite rod electrodes show that the electrocatalytic activity of these films increases with catalyst loading up to an optimal value, beyond which electron and mass transport through the material become rate-limiting. Electrocatalytic studies performed at ?2.25 V vs Fc/Fc+ for 2 h reveal CO production with faradaic efficiencies and turnover numbers up to 99% and 3606, respectively. Photocatalytic studies of the modified TiO2 devices demonstrate enhanced activity at low catalyst loadings, with turnover numbers up to 70 during 5 h of irradiation.
关键词： metallopolymers,surface modification,photocatalysis,rhenium bipyridine,solar energy conversion,electrocatalysis
更新于2025-09-23 15:23:52
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Metallopolymer Organohydrogels with Photoa??Controlled Coordination Crosslinks Work Properly Below 0 ?°C
摘要： Controlling the structures and functions of gels is important for both fundamental research and technological applications. Introducing photoresponsive units into gels enables remote control of their properties with light. However, existing gels show photoresponsiveness only at room temperature or elevated temperatures. The development of photoresponsive gels that work below 0 °C can expand their usage in cold environments. Here, photoresponsive metallopolymer organohydrogels that function even at ?20 °C are reported. The organohydrogels are prepared using photoresponsive Ru–thioether coordination bonds as reversible crosslinks to form polymer networks. A water/glycerol mixture is used as an anti-freezing solvent. At ?20 °C, the Ru–thioether coordination bonds are dissociated under light irradiation and reformed reversibly in the dark, which result in alternating crosslinking densities in the polymer networks. This process enables inducing reversible gel-to-sol transitions, healing damaged gels, controlling the mechanical properties and volumes of the gels, and rewriting microstructures on the gels below 0 °C.
关键词： photoresponsive materials,gels,crosslinks,anti-freezing,metallopolymers
更新于2025-09-23 15:19:57
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Comprehensive Supramolecular Chemistry II || Polymers and Molecular Wires as Chemical Sensors
摘要： Sensors provide a critical interface between humans and the world around them. A sensor, according to the Oxford English dictionary, is “a device that detects or measures a physical property and records, indicates, or otherwise responds to it.” A sensor responds to an external stimulus and converts it into a signal that can be recorded. The human body has at least ?ve sets of sensors, i.e., nose, tongue, ears, eyes, and skin; and human beings sense the world by their smell, taste, hearing, sight, and touch. Examples of some commercially available sensors include temperature sensors, pressure sensors, ?ow sensors, stress/strain sensors, and conductivity sensors.
关键词： Polymers,Fluorescent Sensors,Molecular Wires,Chemical Sensors,Metallopolymers
更新于2025-09-11 14:15:04