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Topochemical Polymerization of a Supramolecular Polymer and Prominent Ambipolar Charge-Carrier Mobility
Macromolecules ( IF 5.1 ) Pub Date : 2024-12-16 , DOI: 10.1021/acs.macromol.4c02090
Atish Nag, Rajendra Prasad Paitandi, Shu Seki, Suhrit Ghosh

This study reports the topochemical polymerization of a supramolecular polymer of the n-type semiconducting naphthalene-diimide (NDI)-appended diacetylene (DA) building block NDI-DA. It exhibits H-bonding-driven supramolecular polymerization in a nonpolar solvent, producing a fibrillar gel, in which the polymerizable DA units are spatially organized in a manner that facilitates topochemical polymerization. Upon photoirradiation, topochemical polymerization proceeds efficiently, producing the p-type semiconducting polydiacetylene (PDA) backbone with appended n-type NDI chromophores. The resulting polymer (NDI-PDA) was isolated as a red solid and showed a very high molecular weight (Mn) of 232,000 g mol–1 with a narrow dispersity (Đ) of 1.1. The UV/vis spectrum of NDI-PDA, even in a good solvent, showed prominent π-stacking despite the absence of H-bonding among the amide groups, suggesting indeed that the topochemical polymerization had stabilized the NDI stack, as desired. Electron- and hole-transporting pathways along the peripheral NDI array and the PDA backbone, respectively, lead to a significantly high ambipolar charge-carrier mobility of 6.0 × 10–4 cm2 V–1 s–1, estimated by flash photolysis time-resolved microwave conductivity in combination with transient absorption spectroscopy studies.

中文翻译:


超分子聚合物的拓扑化学聚合和突出的双极电荷载流子迁移率



本研究报道了 n 型半导体萘-二酰亚胺 (NDI) 附加的二乙炔 (DA) 结构单元 NDI-DA 的超分子聚合物的拓扑化学聚合。它在非极性溶剂中表现出 H 键驱动的超分子聚合,产生纤维状凝胶,其中可聚合的 DA 单元在空间上以有利于拓扑化学聚合的方式组织。在光照射下,拓扑化学聚合有效地进行,产生带有附加 n 型 NDI 发色团的 p 型半导体聚二乙炔 (PDA) 骨架。所得聚合物 (NDI-PDA) 被分离为红色固体,显示出 232,000 g mol–1 的极高分子量 (Mn),窄分散度 (Đ) 为 1.1。尽管酰胺基团之间没有氢键,但 NDI-PDA 的紫外/可见光谱即使在良好的溶剂中也显示出明显的π堆叠,这表明拓扑化学聚合确实如预期般稳定了 NDI 堆栈。沿外周 NDI 阵列和 PDA 主链的电子和空穴传输途径分别导致 6.0 × 10-4 cm2 V-1 s-1 的显着高双极电荷载流子迁移率,通过闪光光解时间分辨微波电导率结合瞬态吸收光谱研究估计。
更新日期:2024-12-17
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