{"title":"Precisely Regulating Interchain Aggregation and Film Crystallinity of Quinoidal Terpolymers for High-Performance Eco-friendly Transistors","authors":"Runze Xie, Quanfeng Zhou, Pingzhong Guan, Jinlun Li, Cheng Liu, Miao Qi, Chongqing Yang, Xuanchen Liu, Junkai Xiong, Xiang Ge, Pengfei Zhou, Lianjie Zhang, Junwu Chen, Yi Liu, Xuncheng Liu","doi":"10.1021/acs.macromol.4c02672","DOIUrl":null,"url":null,"abstract":"The widespread use of toxic halogenated solvents in processing high-performance conjugated polymers raises environmental concerns and hinders large-scale organic electronics production. While the terpolymer approach has improved the donor–acceptor polymer performance, it remains unexplored in quinoidal systems. This study pioneers a terpolymer strategy for quinoidal polymers to enable eco-friendly processing by fine-tuning interchain aggregation and film crystallinity, leading to improved charge mobility and stability in organic field-effect transistors (OFETs). A series of <i>para</i>-azaquinodimethane-based random terpolymers with varied ratios of terthiophene (3T) and quaterthiophene (4T) units are developed, demonstrating that higher 4T content enhances interchain aggregation but reduces solubility, dramatically affecting molecular packing and OFET performance. When processed from chlorobenzene, all terpolymers outperformed reference alternating copolymers, with PA-3T25-4T75 containing 75% 4T achieving the highest hole mobility of 2.26 cm<sup>2</sup> V<sup>–1</sup> s<sup>–1</sup> due to its most ordered microstructure. Notably, PA-3T75-4T25 with 25% 4T achieves an impressive hole mobility of 2.09 cm<sup>2</sup> V<sup>–1</sup> s<sup>–1</sup> with tetrahydrofuran as the solvent, marking a record high value for quinoidal polymers processed from eco-friendly solvents. This work underscores the potential of terpolymer design in enhancing both OFET performance and environmental sustainability of quinoidal polymers, contributing to the development of eco-friendly organic electronics.","PeriodicalId":51,"journal":{"name":"Macromolecules","volume":"33 1","pages":""},"PeriodicalIF":5.2000,"publicationDate":"2025-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Macromolecules","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1021/acs.macromol.4c02672","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"POLYMER SCIENCE","Score":null,"Total":0}
引用次数: 0
Abstract
The widespread use of toxic halogenated solvents in processing high-performance conjugated polymers raises environmental concerns and hinders large-scale organic electronics production. While the terpolymer approach has improved the donor–acceptor polymer performance, it remains unexplored in quinoidal systems. This study pioneers a terpolymer strategy for quinoidal polymers to enable eco-friendly processing by fine-tuning interchain aggregation and film crystallinity, leading to improved charge mobility and stability in organic field-effect transistors (OFETs). A series of para-azaquinodimethane-based random terpolymers with varied ratios of terthiophene (3T) and quaterthiophene (4T) units are developed, demonstrating that higher 4T content enhances interchain aggregation but reduces solubility, dramatically affecting molecular packing and OFET performance. When processed from chlorobenzene, all terpolymers outperformed reference alternating copolymers, with PA-3T25-4T75 containing 75% 4T achieving the highest hole mobility of 2.26 cm2 V–1 s–1 due to its most ordered microstructure. Notably, PA-3T75-4T25 with 25% 4T achieves an impressive hole mobility of 2.09 cm2 V–1 s–1 with tetrahydrofuran as the solvent, marking a record high value for quinoidal polymers processed from eco-friendly solvents. This work underscores the potential of terpolymer design in enhancing both OFET performance and environmental sustainability of quinoidal polymers, contributing to the development of eco-friendly organic electronics.
期刊介绍：
Macromolecules publishes original, fundamental, and impactful research on all aspects of polymer science. Topics of interest include synthesis (e.g., controlled polymerizations, polymerization catalysis, post polymerization modification, new monomer structures and polymer architectures, and polymerization mechanisms/kinetics analysis); phase behavior, thermodynamics, dynamic, and ordering/disordering phenomena (e.g., self-assembly, gelation, crystallization, solution/melt/solid-state characteristics); structure and properties (e.g., mechanical and rheological properties, surface/interfacial characteristics, electronic and transport properties); new state of the art characterization (e.g., spectroscopy, scattering, microscopy, rheology), simulation (e.g., Monte Carlo, molecular dynamics, multi-scale/coarse-grained modeling), and theoretical methods. Renewable/sustainable polymers, polymer networks, responsive polymers, electro-, magneto- and opto-active macromolecules, inorganic polymers, charge-transporting polymers (ion-containing, semiconducting, and conducting), nanostructured polymers, and polymer composites are also of interest. Typical papers published in Macromolecules showcase important and innovative concepts, experimental methods/observations, and theoretical/computational approaches that demonstrate a fundamental advance in the understanding of polymers.
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