可溶液加工的原始 PEDOT 在掺杂状态下表现出优异的导电性、载流子迁移率和热稳定性,Macromolecular Chemistry and Physics

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可溶液加工的原始 PEDOT 在掺杂状态下表现出优异的导电性、载流子迁移率和热稳定性
Macromolecular Chemistry and Physics ( IF 2.5 ) Pub Date : 2021-06-26 , DOI: 10.1002/macp.202100123
Philip Schmode ₁ , Adrian Hochgesang ₁ , Mahima Goel ₁ , Florian Meichsner ₁ , John Mohanraj ₁ , Martina Fried ₁ , Mukundan Thelakkat _{1,

2}

Affiliation

PEDOT:PSS [聚（3,4-亚乙基二氧噻吩）聚苯乙烯磺酸盐] 是一种广泛使用的不溶性导电聚合物，因此由分散体加工而成。在这项工作中，PEDOT 均聚物（PEDOT-C ₆ C ₈ 1 和 2）在甲苯、四氢呋喃和氯仿等常用溶剂中的溶解度很高，使用 Kumada 催化剂转移聚合合成了一种新合成的高分子量和低分散性带有支链烷基取代基的 EDOT 单体。原始 PEDOT-C ₆ C ₈允许在具有 5 × 10 ⁻⁴ cm ² V ⁻¹ s ⁻¹的高电荷载流子迁移率的累积模式晶体管中使用. 此外，这些聚合物可以以受控方式掺杂，在掺杂剂 Spiro-MeOTAD(TFSI) ₂为 10 mol% 时达到 10 ^-3 S cm ^-1的电导率。掺杂状态非常稳定，在 100°C 的氮气下退火并暴露于环境气氛长达 12 小时后，仍保持初始值的 80%。在掺杂过程中，空穴注入势垒降低并在仅 2.5 mol% 掺杂剂负载下达到令人印象深刻的 130 meV 低值，而载流子迁移率没有损失；使用紫外光电子和阻抗光谱进行监测。这种新的设计概念导致具有良好控制的分子量的高溶解性聚合物以良好控制的方式提供可溶液加工的PEDOT。

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A Solution-Processable Pristine PEDOT Exhibiting Excellent Conductivity, Charge Carrier Mobility, and Thermal Stability in the Doped State

PEDOT:PSS [poly(3,4-ethylenedioxythiophene) polystyrene sulfonate] is a widely used insoluble conducting polymer, which is therefore processed from dispersions. In this work, PEDOT homopolymers (PEDOT-C₆C₈ 1 and 2) highly soluble in common solvents like toluene, tetrahydrofuran, and chloroform are synthesized with a high control of molecular weight and low dispersity using Kumada catalyst transfer polymerization of a newly synthesized EDOT monomer carrying a branched alkyl substituent. Pristine PEDOT-C₆C₈ allows the use in accumulation mode transistors with a high charge carrier mobility of 5 × 10⁻⁴ cm² V⁻¹ s⁻¹. Moreover, these polymers can be doped in a controlled fashion, reaching conductivities of 10⁻³ S cm⁻¹ at 10 mol% of a dopant, Spiro-MeOTAD(TFSI)₂. The doped state is remarkably stable, retaining 80% of the initial value after annealing under nitrogen at 100 °C and being exposed to ambient atmosphere for up to 12 h. During doping, the hole injection barrier decreases and reaches an impressively low value of 130 meV at only 2.5 mol% dopant loading without loss in carrier mobility; as monitored using ultraviolet photoelectron- and impedance spectroscopy. This new design concept leading to highly soluble polymers with well-controlled molecular weights provides solution-processable PEDOT dopable in a well-controlled fashion.

更新日期：2021-06-26

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