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<p>Viologen-based ionic covalent organic polymers (V-iCOP) with higher dimensionality is promising for their various characteristics (porosity, redox potential, and color) owing to the tunability of their composition. In this work, 3 different viologen-based 2D cationic covalent organic polymer thin films (V-iCOP1, V-iCOP2, V-iCOP3) were synthesized by Zincke reaction with linkers of varying electron affinity: tris(4-aminophenyl)amine (TAPA), 1,3,5-tris(4-aminophenyl)benzene (TAPB), 1,3,5-tris-(4-aminophenyl)triazine (TAPT). The structural and electronic effects of the different linkers on the electrochromic device performances were investigated and compared with theoretical DFT calculations. Due to the cationic nature of the polymer thin film that promotes fast ionic diffusion, they overall show superior electrochromic performance in aqueous conditions. This is reflected from the rapid switching speed (&lt;10 s), high coloration efficiency (maximum CE of 836.08 cm<sup>2</sup>/C), low potential bias and multichromic properties with significant transmittance difference (ΔT%). The constructed V-iCOP electrochromic devices with quasi-solid hydrogel electrolyte exhibit long term cycling stability (92.5% at 2000 cycles). The acceptor-acceptor moiety of V-iCOP3 with the triazine linker exhibited the largest color modulation and highest coloration efficiency. This work showcases the versatile properties and promising molecular design prospectus of V-iCOP thin films for electrochromic devices.</p>

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Design of viologen-based 2D cationic covalent organic polymer for multi-colored electrochromic devices with tuneable redox potential

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年2月27日

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  • Jae Uk Choi,
  • Teck Lip Dexter Tam,
  • Jinwoo Park,
  • Yufei Zhang,
  • Pooi See Lee

摘要

Viologen-based ionic covalent organic polymers (V-iCOP) with higher dimensionality is promising for their various characteristics (porosity, redox potential, and color) owing to the tunability of their composition. In this work, 3 different viologen-based 2D cationic covalent organic polymer thin films (V-iCOP1, V-iCOP2, V-iCOP3) were synthesized by Zincke reaction with linkers of varying electron affinity: tris(4-aminophenyl)amine (TAPA), 1,3,5-tris(4-aminophenyl)benzene (TAPB), 1,3,5-tris-(4-aminophenyl)triazine (TAPT). The structural and electronic effects of the different linkers on the electrochromic device performances were investigated and compared with theoretical DFT calculations. Due to the cationic nature of the polymer thin film that promotes fast ionic diffusion, they overall show superior electrochromic performance in aqueous conditions. This is reflected from the rapid switching speed (<10 s), high coloration efficiency (maximum CE of 836.08 cm2/C), low potential bias and multichromic properties with significant transmittance difference (ΔT%). The constructed V-iCOP electrochromic devices with quasi-solid hydrogel electrolyte exhibit long term cycling stability (92.5% at 2000 cycles). The acceptor-acceptor moiety of V-iCOP3 with the triazine linker exhibited the largest color modulation and highest coloration efficiency. This work showcases the versatile properties and promising molecular design prospectus of V-iCOP thin films for electrochromic devices.