在新型电子学材料和绿色能源技术的研发领域，共轭配位聚合物（conjugated coordination polymers, c-CPs）近年来引起了广泛关注。这些由平面共轭配体和过渡金属组装形成的新型有机无机杂合材料，不仅具有优异的电学性质还具有可设计的分子孔洞、可调控的能级结构和电化学活性，在高性能、多功能先进光电器件及绿色能源器件的构建上展示了广泛的应用潜力。近年来，平面共轭配体，如六取代苯和六取代三亚苯等(取代基为巯基、氨基、羟基，硒基)，已发展成为构建高电导率和高迁移率c-CPs的重要组成。然而，上述单一取代的共轭配体在构建能带结构可调的半导体c-CPs方面存在局限。如何实现配位聚合物半导体能带结构的大范围调制仍具挑战性。
近日，德累斯顿工业大学冯新亮教授、山东大学董人豪教授、中国科学院化学研究所徐伟研究员与南京大学黎建教授开展合作研究，突破了这一局限。他们基于新型“4+2”构型苯基配体构筑了两个具有相同拓扑结构、不同氧化态的银基共轭配位聚合物（c-CPs）单晶，包括Ag
4TTHQ和Ag
4TTBQ（TTHQ为四巯基对氢醌，TTBQ为四巯基对苯醌）。研究团队发现，通过对聚合物骨架中氢醌/苯醌(HQ/BQ)氧化态的调节能够显著改变能带结构，可以实现电子带隙从0.5 eV到1.5 eV的大幅变化。在不同半导体能带结构状态下，两种c-CPs均展示出了数值可达10
2 cm
2/V·s的高载流子迁移率。该工作由此发展了一种通过改变氧化态调节能带结构的化学策略。
首先，利用对反应条件的细微控制可以分别合成具有氢醌单元的Ag
4TTHQ和具有苯醌单元的Ag
4TTBQ。关于Ag
4TTBQ的合成过程如下：使用硝酸银和TTHQ作为原料在氯苯/水界面合成，利用原位生成稀硝酸带来的氧化环境进行慢速合成，可使TTHQ逐步氧化为TTBQ，最终得到Ag
4TTBQ。而利用无法生成氧化性酸的醋酸银和TTHQ在惰性气氛下、甲醇中快速反应得到的是Ag
4TTHQ。通过紫外光谱分析发现，相比Ag
4TTBQ（0.5 eV），Ag
4TTHQ（1.5 eV）具有更宽的光学带隙。
利用旋转电子衍射技术对单晶结构进行解析发现Ag
4TTHQ和Ag
4TTBQ具有相似的由Ag 原子层和有机层构建的层状杂合结构。单晶结构显示两者具有同样的拓扑连接方式和相似的无机层原子排布，但有机层中C-O键长度不同。结合拉曼光谱中碳氧双键特征峰的分析，研究者揭示了Ag
4TTHQ和Ag
4TTBQ分别具有氢醌（HQ）和苯醌（BQ）单元。
基于Ag
4TTHQ和Ag
4TTBQ的能带结构理论计算可知，氢醌/苯醌单元对费米面附近由大量C、O轨道形成的能带有调制作用，可以作为能带开关的旋钮。而对于材料电导率（0.4 S/cm
vs. 10 S/cm）和塞贝克系数（330 μV/K
vs. 50 μV/K）的测试揭示了能带变化对两者的显著影响。
利用时间分辨太赫兹光谱研究了 Ag
4TTHQ 和 Ag
4TTBQ 中光生载流子动力学和微观电荷传输机制。光激发后，Ag
4TTHQ 和 Ag
4TTBQ 展现出截然不同的光生载流子动力学：Ag
4TTHQ 显示出与泵注量无关的光电导衰减率，光电导衰减由缺陷辅助复合机制主导；而 Ag
4TTBQ 在泵注量升高时表现出更高的光电导衰减率，光电导衰减受缺陷辅助复合机制和电子-空穴重组机制共同影响。其频率分辨复合光电导符合Drude-Smith传输模型，拟合分析可以得到Ag
4TTHQ 和 Ag
4TTBQ的直流载流子迁移率，分别为137 ± 7 cm
2/V·s和130 ± 9 cm
2/V·s。
这项研究不仅为构建高载流子迁移率且具有可调控能级结构的配位聚合物半导体提供了新的思路，而且也展现出了Ag
4TTBQ和Ag
4TTHQ在高性能光电器件和电化学储能应用方面的巨大的潜力。黄幸博士（德累斯顿工业大学）是本工作的第一。李洋博士（中国科学院化学研究所）和付帅博士（德累斯顿工业大学）为本工作的共同一作。文章发表在
Angew. Chem. Int. Ed.2024, DOI：10.1002/anie.202320091
文章链接：
https://onlinelibrary.wiley.com/doi/10.1002/anie.202320091
来源：高分子科学前沿
声明：仅代表个人观点，水平有限，如有不科学之处，请在下方留言指正！
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