Parr Zachary S, Borges-González Jorge, Rashid Reem B, Thorley Karl J, Meli Dilara, Paulsen Bryan D, Strzalka Joseph, Rivnay Jonathan, Nielsen Christian B
Department of Chemistry, Queen Mary University of London, Mile End Road, London, E1 4NS, UK.
Department of Biomedical Engineering, Northwestern University, 2145 Sheridan Road, Evanston, IL, 60208, USA.
Adv Mater. 2022 Apr;34(14):e2107829. doi: 10.1002/adma.202107829. Epub 2022 Feb 23.
Organic mixed ionic and electronic conductors are of significant interest for bioelectronic applications. Here, three different isoindigoid building blocks are used to obtain polymeric mixed conductors with vastly different structural and electronic properties which can be further fine-tuned through the choice of comonomer unit. This work shows how careful design of the isoindigoid scaffold can afford highly planar polymer structures with high degrees of electronic delocalization, while subtle structural modifications can control the dominant charge carrier (hole or electron) when probed in organic electrochemical transistors. A combination of experimental and computational techniques is employed to probe electrochemical, structural, and mixed ionic and electronic properties of the polymer series which in turn allows the derivation of important structure-property relations for this promising class of materials in the context of organic bioelectronics. Ultimately, these findings are used to outline robust molecular-design strategies for isoindigo-based mixed conductors that can support efficient p-type, n-type, and ambipolar transistor operation in an aqueous environment.
有机混合离子和电子导体在生物电子应用中具有重大意义。在此，使用了三种不同的异吲哚类结构单元来获得具有截然不同的结构和电子性质的聚合物混合导体，这些性质可通过共聚单体单元的选择进一步微调。这项工作展示了如何精心设计异吲哚类支架，以提供具有高度电子离域的高度平面化聚合物结构，而细微的结构修饰在有机电化学晶体管中进行探测时，可以控制主要电荷载流子（空穴或电子）。采用实验和计算技术相结合的方法来探测聚合物系列的电化学、结构以及混合离子和电子性质，这反过来又使得在有机生物电子学背景下，能够推导这类有前景材料的重要结构 - 性质关系。最终，这些发现被用于勾勒基于异吲哚的混合导体的稳健分子设计策略，这些策略能够在水性环境中支持高效的p型、n型和双极性晶体管操作。
