Dai Shan, Nouar Farid, Zhang Sanjun, Tissot Antoine, Serre Christian
Institut des Matériaux Poreux de Paris, UMR 8004 Ecole Normale Supérieure, ESPCI Paris, CNRS, PSL University, 75005, Paris, France.
State Key Laboratory of Precision Spectroscopy, East China Normal University, No. 3663, North Zhongshan Road, Shanghai, 200062, China.
Angew Chem Int Ed Engl. 2021 Feb 19;60(8):4282-4288. doi: 10.1002/anie.202014184. Epub 2020 Dec 23.
Room-temperature syntheses of metal-organic frameworks (MOFs) are of interest to meet the demand of the sustainable chemistry and are a pre-requisite for the incorporation of functional compounds in water-stable MOFs. However, only few routes under ambient conditions have been reported to produce metal(IV)-based MOFs. Reported here is a new versatile one-step synthesis of a series of highly porous M -oxocluster-based MOFs (M=Zr, Hf, Ce) at room temperature, including 8- or 12-connected micro/mesoporous solids with different functionalized organic ligands. The compounds show varying degrees of defects, particularly for 12-connected phases, while maintaining the chemical stability of the parent MOFs. Proposed here are first insights into in situ kinetics observations for efficient MOF preparation. Remarkably, the synthesis has a high space-time yield and also provides the possibility to tune the particle size, therefore paving the way for their practical use.
金属有机框架材料（MOFs）的室温合成对于满足可持续化学的需求具有重要意义，并且是将功能化合物掺入水稳定MOFs中的先决条件。然而，据报道在环境条件下只有少数方法可用于制备基于金属（IV）的MOFs。本文报道了一种新型通用的一步法，可在室温下合成一系列高度多孔的基于M-氧簇的MOFs（M = Zr、Hf、Ce），包括具有不同功能化有机配体的8或12连接的微孔/介孔固体。这些化合物表现出不同程度的缺陷，特别是对于12连接相，同时保持了母体MOFs的化学稳定性。本文首次提出了关于高效制备MOF的原位动力学观察的见解。值得注意的是，该合成方法具有较高的时空产率，并且还提供了调节粒径的可能性，因此为它们的实际应用铺平了道路。
