CuO与有机羧酸在室温条件下利用水蒸汽辅助老化法合成金属有机框架SNU-50

Efficient Vapor-assisted aging Synthesis of a Metal-Organic Framework, SNU-50,from CuO

氧化铜(CuO)作为一种高晶格能的金属氧化物,由于其高稳定性和难溶解性,通常难以直接作为反应原料来合成相应的含铜的功能材料。在这里,我们直接利用氧化铜作为反应原料与合成得到的N-N’-二(3,5-二羧基苯基)均苯四甲酸二酰亚胺(H4BDCPPI,简称四羧酸),在绿色温和的蒸汽辅助老化法合成条件下,成功的得到了相应的金属有机框架材料SNU-50。首先,我们利用预盐湿磨(pre-ionic and liquid assisted grinding,简称pre-ILAG)的预处理方法,将称取的氧化铜,四羧酸,一定量的催化剂氯化铵和微量溶剂(水,乙醇和DMF)混合并研磨一分钟,然后取出样品放置于不同的溶剂蒸汽中(水,乙醇和DMF)中进行熏蒸老化。我们发现在水蒸气熏蒸上述混合物12小时后,成功合成得到SNU-50材料。相应地,我们利用PXRD和BET孔材料等分析方法进行了相应的产物的结构表征。此外,我们还探讨了催化剂氯化铵的用量对于反应过程的影响。

Copper oxide,CuO,a starting material with high crystalline energy and stability,is very difficult to be used to synthesize copper-based functional materials directly.Herein,by the method of vapor-assisted aging,a green and mild synthesis,we obtained a Metal-Organic Framewor SNU-50 successfully from CuO and the as-synthesized N,N’-bis(3,5-dicarboxyphenyl)pyromellitic diimide(H4BDCPPI).Firstly,the mixture of CuO,H4BDCPPI,NH4Cl with liquid(μL)pre-ground together in a ball mill at 25 Hz for only 1 minute,then was placed in a solvent atmosphere for room temperature aging.It was found that when the adding amount of NH4Cl is 15%,the reaction took 12 hours to complete under water vapor aging.Furthermore,PXRD and BET specific area was used to structural characterize the product.Also,the effect of the amount of the catalytic ammonium chloride on the reaction rate had been studied.