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首页> 外文期刊>ACS applied materials & interfaces >Controlled Radical Polymerization and Quantification of Solid State Electrical Conductivities of Macromolecules Bearing Pendant Stable Radical Groups
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Controlled Radical Polymerization and Quantification of Solid State Electrical Conductivities of Macromolecules Bearing Pendant Stable Radical Groups

机译：带有侧基稳定基团的大分子的受控自由基聚合和固态电导率的定量

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摘要

Macromolecules with aliphatic backbones that bear pendant stable radical groups (i.e., radical polymers) have attracted much attention in applications where a supporting electrolyte is capable of aiding charge transport in solution; however, the utilization of these materials in solid state applications has been limited. Here, we synthesize a model radical polymer, poly(2,2,6,6-tetramethylpiperidinyloxy meth-acrylate) (PTMA), through a controlled reversible addition-fragmentation chain transfer (RAFT) mediated polymerization mechanism to generate well-defined and easily-tunable functional polymers. These completely amorphous, electronically-active polymers demonstrate relatively high glass transition temperatures (T_g ～170 °C) and, because of the aliphatic nature of the backbone of the radical polymers, are almost completely transparent in the visible region of the electromagnetic spectrum. Additionally, we quantify the conductivity of PTMA (～1 X 10~(-6) S cm~(-1)) and find it to be on par with pristine π-conjugated polymers such as poly(phenylene vinylenes) (PPVs) and poly(3-alkylthiophenes) (P3ATs). Furthermore, we demonstrate that the addition of small molecules bearing stable radical groups provides for more solid state charge hopping sites without altering the chemical nature of radical polymers; this, in turn, allows for an increase in the conductivity of PTMA relative to neat PTMA thin films while still retaining the same high degree of optical transparency and device stability. Because of the synthetic flexibility and easily-controlled doping mechanisms (that do not alter the PTMA chemistry), radical polymers present themselves as promising and tunable materials for transparent solid-state plastic electronic applications.
机译：具有脂肪族主链并带有稳定的侧基的侧基的大分子（即自由基聚合物）在支持电解质能够帮助溶液中电荷迁移的应用中引起了很多关注。然而，在固态应用中这些材料的利用受到限制。在这里，我们通过受控的可逆加成-断裂链转移（RAFT）介导的聚合机理合成了模型自由基聚合物聚（2,2,6,6-四甲基哌啶基氧基甲基丙烯酸酯）（PTMA），以生成定义明确且容易可调节的功能聚合物。这些完全无定形的电子活性聚合物表现出较高的玻璃化转变温度（T_g〜170°C），并且由于自由基聚合物主链的脂族性质，在电磁光谱的可见光区域几乎是完全透明的。此外，我们对PTMA的电导率进行了量化（〜1 X 10〜（-6）S cm〜（-1）），发现它与原始的π-共轭聚合物，例如聚亚苯基亚乙烯基（PPV）和聚（3-烷基噻吩）（P3AT）。此外，我们证明，带有稳定自由基基团的小分子的添加可提供更多的固态电荷跳跃点，而不会改变自由基聚合物的化学性质;相对于纯PTMA薄膜，这又可以增加PTMA的电导率，同时仍保持相同的高度光学透明性和器件稳定性。由于合成的灵活性和易于控制的掺杂机制（不会改变PTMA化学性质），自由基聚合物作为透明固态塑料电子应用的有希望和可调谐的材料而呈现。

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