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

Junxin Chen, Shengyu Cong, Lewen Wang, Yazhou Wang, Liuyuan Lan, Chaoyue Chen, Yecheng Zhou, Zhengke Li, Iain McCulloch, Wan Yue

Research output: Contribution to journalArticlepeer-review

11 Scopus citations

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.
Original languageEnglish (US)
Pages (from-to)607-618
Number of pages12
JournalMaterials Horizons
Volume10
Issue number2
DOIs
StatePublished - Dec 2 2022
Externally publishedYes

Bibliographical note

Generated from Scopus record by KAUST IRTS on 2023-09-21

ASJC Scopus subject areas

  • Mechanics of Materials
  • Process Chemistry and Technology
  • General Materials Science
  • Electrical and Electronic Engineering

Fingerprint

Dive into the research topics of 'Backbone coplanarity manipulation via hydrogen bonding to boost the n-type performance of polymeric mixed conductors operating in aqueous electrolyte'. Together they form a unique fingerprint.

Cite this