美国芝加哥大学Anderson John S.团队提出了非晶配位聚合物中玻璃-金属的本征转换。相关研究成果发表在2022年10月26日出版的《自然》。
导电有机材料，如掺杂的有机聚合物、分子导体和新兴的配位聚合物，支撑着从显示器到柔性电子的各种技术。要在传统绝缘有机材料中实现高导电性，就必须通过化学掺杂调整其电子结构。此外，即使是本质上导电的有机材料，如单组分分子导体，也需要结晶性才能实现金属行为。然而，导电聚合物通常是无定形的，以有助于耐久性和加工性。使用分子设计在未掺杂的无定形材料中产生高导电性，可在许多应用中实现可调且坚固的导电性，但没有本质导电的有机材料在无序时保持高导电性。
该文中，研究人员报道了一种非晶配位聚合物，四硫富瓦烯四硫代镍，它显示出显著的高电子电导率（高达1200Scm-1）和本征的玻璃金属行为。理论表明，这些性质是由对结构扰动鲁棒的分子重叠实现的。这一不寻常的特性导致高电导率，在pH值为0–14且温度高达140°C的潮湿空气中可稳定数周。这些发现表明，即使在高度无序的材料中，分子设计也可以实现金属导电性，这回答了关于没有周期性结构的金属传输如何存在的基本问题，并表明了这些材料令人兴奋的新应用。
附：英文原文
Title: Intrinsic glassy-metallic transport in an amorphous coordination polymer
Author: Xie, Jiaze, Ewing, Simon, Boyn, Jan-Niklas, Filatov, Alexander S., Cheng, Baorui, Ma, Tengzhou, Grocke, Garrett L., Zhao, Norman, Itani, Ram, Sun, Xiaotong, Cho, Himchan, Chen, Zhihengyu, Chapman, Karena W., Patel, Shrayesh N., Talapin, Dmitri V., Park, Jiwoong, Mazziotti, David A., Anderson, John S.
Issue&Volume: 2022-10-26
Abstract: Conducting organic materials, such as doped organic polymers1, molecular conductors2,3 and emerging coordination polymers4, underpin technologies ranging from displays to flexible electronics5. Realizing high electrical conductivity in traditionally insulating organic materials necessitates tuning their electronic structure through chemical doping6. Furthermore, even organic materials that are intrinsically conductive, such as single-component molecular conductors7,8, require crystallinity for metallic behaviour. However, conducting polymers are often amorphous to aid durability and processability9. Using molecular design to produce high conductivity in undoped amorphous materials would enable tunable and robust conductivity in many applications10, but there are no intrinsically conducting organic materials that maintain high conductivity when disordered. Here we report an amorphous coordination polymer, Ni tetrathiafulvalene tetrathiolate, which displays markedly high electronic conductivity (up to 1,200Scm1) and intrinsic glassy-metallic behaviour. Theory shows that these properties are enabled by molecular overlap that is robust to structural perturbations. This unusual set of features results in high conductivity that is stable to humid air for weeks, pH 0–14 and temperatures up to 140°C. These findings demonstrate that molecular design can enable metallic conductivity even in heavily disordered materials, raising fundamental questions about how metallic transport can exist without periodic structure and indicating exciting new applications for these materials.
DOI: 10.1038/s41586-022-05261-4
Source: https://www.nature.com/articles/s41586-022-05261-4