Single Crystals of a Highly Conductive Three-Dimensional Conjugated Coordination Polymer,Journal of the American Chemical Society

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Single Crystals of a Highly Conductive Three-Dimensional Conjugated Coordination Polymer
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2023-05-19 , DOI: 10.1021/jacs.3c02378
Kun Fan _{1,

2} , Jian Li ₃ , Yongshan Xu ₄ , Cheng Fu ₃ , Yuan Chen _{1,

2} , Chenyang Zhang ₁ , Guoqun Zhang ₁ , Jing Ma ₃ , Tianyou Zhai ₄ , Chengliang Wang _{1,

2}

Affiliation

Conjugated coordination polymers (CCPs), which possess long-range planar π–d conjugation, are fascinating for various applications because they inherit the merits of both metal–organic frameworks (MOFs) and conducting polymers. However, only one-dimensional (1D) and two-dimensional (2D) CCPs have been reported so far. The synthesis of three-dimensional (3D) CCPs is challenging and even seems theoretically infeasible because conjugation implies 1D or 2D structure. Besides, the redox activity of the conjugated ligands and the π–d conjugation makes the synthesis of CCPs very complicated, and hence, single crystals of CCPs are rarely achieved. Herein, we reported the first 3D CCP and its single crystals with atomically precise structures. The synthesis process involves complicated in situ dimerization, deprotonation of ligands, oxidation/reduction of both ligands and metal ions, and precise coordination between them. The crystals contain in-plane 1D π–d conjugated chains and close π–π interactions between the adjacent chains that are bridged by another column of stacked chains, thus forming 3D CCP with high conductivity (400 S m^–1 at room temperature and 3100 S m^–1 at 423 K) and potential applications as cathodes in sodium-ion batteries with high capacity, rate capability, and cyclability.

中文翻译：

高导电三维共轭配位聚合物的单晶

具有长程平面 π-d 共轭的共轭配位聚合物 (CCP) 在各种应用中都很有吸引力，因为它们继承了金属有机骨架 (MOF) 和导电聚合物的优点。然而，到目前为止，仅报道了一维 (1D) 和二维 (2D) CCP。三维 (3D) CCP 的合成具有挑战性，甚至在理论上似乎是不可行的，因为共轭意味着 1D 或 2D 结构。此外，共轭配体的氧化还原活性和π-d共轭使得CCPs的合成非常复杂，因此很少能实现CCPs的单晶。在此，我们报道了第一个 3D CCP 及其具有原子精确结构的单晶。合成过程涉及复杂的原位二聚化、配体去质子化、配体和金属离子的氧化/还原，以及它们之间的精确配位。晶体包含面内 1D π-d 共轭链和相邻链之间的紧密 π-π 相互作用，相邻链由另一列堆叠链桥接，从而形成具有高导电性的 3D CCP（400 S m^–1在室温下和 3100 S m ^–1在 423 K 下）以及在具有高容量、倍率性能和循环能力的钠离子电池中作为阴极的潜在应用。

更新日期：2023-05-19

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