Materials that combine magnetic order with other desirable physical attributes could find transformative applications in spintronics, quantum sensing, low-density magnets and gas separations. Among potential multifunctional magnetic materials, metal–organic frameworks, in particular, bear structures that offer intrinsic porosity, vast chemical and structural programmability, and the tunability of electronic properties. Nevertheless, magnetic order within metal–organic frameworks has generally been limited to low temperatures, owing largely to challenges in creating a strong magnetic exchange. Here we employ the phenomenon of itinerant ferromagnetism to realize magnetic ordering at T_C = 225 K in a mixed-valence chromium(ii/iii) triazolate compound, which represents the highest ferromagnetic ordering temperature yet observed in a metal–organic framework. The itinerant ferromagnetism proceeds through a double-exchange mechanism, which results in a barrierless charge transport below the Curie temperature and a large negative magnetoresistance of 23% at 5 K. These observations suggest applications for double-exchange-based coordination solids in the emergent fields of magnetoelectrics and spintronics.

将磁性顺序与其他理想物理属性相结合的材料可以在自旋电子学、量子传感、低密度磁体和气体分离中找到变革性应用。在潜在的多功能磁性材料中，尤其是金属-有机框架，具有提供固有孔隙率、巨大的化学和结构可编程性以及电子特性可调性的结构。然而，金属-有机框架内的磁性顺序通常仅限于低温，这主要是由于在创建强磁交换方面存在挑战。在这里，我们利用巡回铁磁性现象 在混合价铬（ii/iii）中实现T _{C = 225 K 时的磁性排序}三唑化合物，它代表了在金属 - 有机框架中观察到的最高铁磁有序温度。流动的铁磁性通过双交换机制进行，这导致低于居里温度的无势垒电荷传输和在 5 K 时 23% 的大负磁阻。这些观察表明基于双交换的配位固体在新兴领域中的应用磁电学和自旋电子学。