Issue 2, 2023

Backbone coplanarity manipulation via hydrogen bonding to boost the n-type performance of polymeric mixed conductors operating in aqueous electrolyte

Abstract

The development of high-performance n-type semiconducting polymers remains a significant challenge. Reported here is the construction of a coplanar backbone via intramolecular hydrogen bonds to dramatically enhance the performance of n-type polymeric mixed conductors operating in aqueous electrolyte. Specifically, glycolated naphthalene tetracarboxylicdiimide (gNDI) couples with vinylene and thiophene to give gNDI-V and gNDI-T, respectively. The hydrogen bonding functionalities are fused to the backbone to ensure a more coplanar backbone and much tighter π–π stacking of gNDI-V than gNDI-T, which is evidenced by density functional theory simulations and grazing-incidence wide-angle X-ray scattering. Importantly, these copolymers are fabricated as the active layer of the aqueous-based electrochromic devices and organic electrochemical transistors (OECTs). gNDI-V exhibits a larger electrochromic contrast (ΔT = 30%) and a higher coloration efficiency (1988 cm2 C−1) than gNDI-T owing to its more efficient ionic–electronic coupling. Moreover, gNDI-V gives the highest electron mobility (0.014 cm2 V−1 s−1) and μC* (2.31 FV−1 cm−1 s−1) reported to date for NDI-based copolymers in OECTs, attributed to the improved thin-film crystallinity and molecular packing promoted by hydrogen bonds. Overall, this work marks a remarkable advance in the n-type polymeric mixed conductors and the hydrogen bond functionalization strategy opens up an avenue to access desirable performance metrics for aqueous-based electrochemical devices.

Graphical abstract: Backbone coplanarity manipulation via hydrogen bonding to boost the n-type performance of polymeric mixed conductors operating in aqueous electrolyte

Supplementary files

Article information

Article type
Communication
Submitted
02 Sep 2022
Accepted
30 Nov 2022
First published
02 Dec 2022

Mater. Horiz., 2023,10, 607-618

Backbone coplanarity manipulation via hydrogen bonding to boost the n-type performance of polymeric mixed conductors operating in aqueous electrolyte

J. Chen, S. Cong, L. Wang, Y. Wang, L. Lan, C. Chen, Y. Zhou, Z. Li, I. McCulloch and W. Yue, Mater. Horiz., 2023, 10, 607 DOI: 10.1039/D2MH01100J

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