Chemical functionalization is a powerful approach to tailor the physical and chemical properties of two-dimensional (2D) materials, increase their processability and stability, tune their functionalities and, even, create new 2D materials. This is typically achieved through post-synthetic functionalization by anchoring molecules on the surface of an exfoliated 2D crystal, but it inevitably alters the long-range structural order of the material. Here we present a pre-synthetic approach that allows the isolation of crystalline, robust and magnetic functionalized monolayers of coordination polymers. A series of five isostructural layered magnetic coordination polymers based on Fe(ii) centres and different benzimidazole derivatives (bearing a Cl, H, CH₃, Br or NH₂ side group) were first prepared. On mechanical exfoliation, 2D materials are obtained that retain their long-range structural order and exhibit good mechanical and magnetic properties. This combination, together with the possibility to functionalize their surface at will, makes them good candidates to explore magnetism in the 2D limit and to fabricate mechanical resonators for selective gas sensing.

化学功能化是一种强大的方法，可以定制二维（2D）材料的物理和化学特性，提高其可加工性和稳定性，调整其功能，甚至创建新的2D材料。这通常通过将分子锚定在片状2D晶体的表面上进行后合成功能化来实现，但不可避免地会改变该材料的远距离结构顺序。在这里，我们介绍了一种预合成方法，该方法可以隔离结晶，坚固且磁性官能化的配位聚合物单层。基于Fe（ii）中心和不同的苯并咪唑衍生物（带有Cl，H，CH ₃，Br或NH ₂）的一系列五种同构层状磁配位聚合物侧组）首先准备。机械剥离后，将获得2D材料，这些材料保留了其长期的结构顺序并显示出良好的机械和磁性能。这种结合以及随意对其表面进行功能化的可能性，使其成为探索2D极限磁场并制造用于选择性气体传感的机械谐振器的理想人选。