Enhanced Redox Transformation Efficiency in Unconjugated Electroactive Polymer/Carbon Nanotube Hybrids

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• 作者：Xianwen Mao ; Esther H. Yan ; Gregory C. Rutledge ; T. Alan Hatton
• 刊名：Chemistry of Materials
• 出版年：2016
• 出版时间：January 26, 2016
• 年：2016
• 卷：28
• 期：2
• 页码：543-548
• 全文大小：417K
• ISSN：1520-5002

文摘

The mechanism for the redox activity of electroactive polymers (EAPs) with unconjugated backbones (e.g., polyvinylferrocene, PVFc) is fundamentally different from that of intrinsically conducting polymers. Here we investigate, for the first time, the redox transformation efficiency (RTE) of unconjugated EAPs with discrete electron donor/acceptors. We find that the RTE of PVFc can be modulated systematically by incorporation of carbon nanotubes (CNTs) via a facile and controllable solution process. Furthermore, we show that the improvement in the RTE of PVFc translated to enhanced performance of PVFc-based applications, such as energy storage, electrochemically responsive heterogeneous catalysis, and enzymatic biosensing. Our study provides valuable insights into the charge transport mechanism of unconjugated EAP/nanocarbon hybrids and the accelerated electron transfer kinetics by incorporation of materials with a high density of electronic states near the Fermi level. Moreover, this report suggests a generalizable strategy to modulate the accessibility and utilization of discrete redox moieties in unconjugated EAPs through creation of a heterogeneous nanostructure with a polymer-coated porous conducting framework that will simultaneously facilitate electron and ion transport processes.