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Solvent-free synthesis of ZIFs: a route towards the elusive Fe(II) analogue of ZIF-8
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2019-04-11 , DOI: 10.1021/jacs.9b02686
Javier López-Cabrelles 1 , Jorge Romero 1 , Gonzalo Abellán 1, 2, 3 , Mónica Giménez-Marqués 1 , Miguel Palomino 4 , Susana Valencia 4 , Fernando Rey 4 , Guillermo Mínguez Espallargas 1
Affiliation  

Herein we report the synthesis of an elusive metal-organic framework, the iron(II) analogue of ZIF-8 with the formula Fe(2-methylimidazolate)2, here denoted as MUV-3. The preparation of this highly interesting porous material, inaccessible by common synthetic procedures, occurs in a solvent-free reaction upon addition of an easily detachable template molecule, yielding single crystals of MUV-3. This methodology can be extended to other metals and imidazolate derivatives, allowing the preparation of ZIF-8, ZIF-67, and the unprecedented iron(II) ZIFs Fe(2-ethylimidazolate)2 and Fe(2-methylbenzimidazolate)2. The different performance of MUV-3 toward NO sorption, in comparison to ZIF-8, results from the chemisorption of NO molecules, which also causes a gate-opening behavior. Finally, the controlled pyrolysis of MUV-3 results in a N-doped graphitic nanocomposite that exhibits extraordinary performance for the oxygen evolution reaction (OER), with low overpotential at different current densities (316 mV at 10 mA cm-2), low Tafel slope (37 mV per decade), high maximum current density (710 mA cm-2 at 2.0 V vs RHE), and great durability (15 h).

中文翻译:

ZIF 的无溶剂合成:通往 ZIF-8 难以捉摸的 Fe(II) 类似物的途径

在本文中,我们报告了难以捉摸的金属有机骨架的合成,即 ZIF-8 的铁 (II) 类似物,分子式为 Fe(2-methylimidazolate)2,此处表示为 MUV-3。这种非常有趣的多孔材料的制备是普通合成程序无法获得的,在添加易于分离的模板分子后,在无溶剂反应中发生,产生 MUV-3 单晶。这种方法可以扩展到其他金属和咪唑衍生物,允许制备 ZIF-8、ZIF-67 和前所未有的铁 (II) ZIF Fe(2-ethylimidazolate)2 和 Fe(2-methylbenzimidazolate)2。与 ZIF-8 相比,MUV-3 对 NO 吸附的不同性能是由 NO 分子的化学吸附引起的,这也会导致门打开行为。最后,
更新日期:2019-04-11
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