Zhang Zhongzheng, Sun Nannan, Wei Wei, Sun Yuhan
CAS Key Laboratory of Low-Carbon Conversion Science and Engineering, Shanghai Advanced Research Institute, Chinese Academy of Science Shanghai 201203 China
School of Physical Science and Technology, Shanghai Tech University Shanghai 201210 China.
RSC Adv. 2018 Jun 12;8(38):21460-21471. doi: 10.1039/c8ra03349h. eCollection 2018 Jun 8.
A new strategy for controlled synthesis of a MOF composite with a core-shell structure, ZIF-8@resorcinol-urea-formaldehyde resin (ZIF@RUF), is reported for the first time through growth of RUF on the surface of ZIF-8 nanoparticles an organic-organic self-assembly process by using hexamethylenetetramine as a formaldehyde-releasing source to effectively control the formation rate of RUF, providing the best opportunity for RUF to selectively grow around the nucleation seeds ZIF-8. Compared with the widely reported method for MOF composite synthesis, our strategy not only avoids the difficulty of incorporating MOF crystals into small pore sized materials because of pore limitation, but also effectively guarantees the formation of a MOF composite with a MOF as the core. After carbonization, a morphology-retaining N-doped hierarchical porous carbon characterized by its highly developed microporosity in conjunction with ordered mesoporosity was obtained. Thanks to this unique microporous core-mesoporous shell structure and significantly enhanced porosity, simultaneous improvements of CO adsorption capacity and kinetics were achieved. This strategy not only paves a way to the design of other core-shell structured MOF composites, but also provides a promising method to prepare capacity- and kinetics-increased carbon materials for CO capture.
首次报道了一种用于可控合成具有核壳结构的金属有机框架(MOF)复合材料——ZIF-8@间苯二酚-尿素-甲醛树脂(ZIF@RUF)的新策略,该策略是通过在ZIF-8纳米颗粒表面生长RUF,利用六亚甲基四胺作为甲醛释放源,通过有机-有机自组装过程有效控制RUF的形成速率,为RUF在成核种子ZIF-8周围选择性生长提供了最佳机会。与广泛报道的MOF复合材料合成方法相比,我们的策略不仅避免了由于孔限制而将MOF晶体掺入小孔径材料的困难,而且有效地保证了以MOF为核心的MOF复合材料的形成。碳化后,获得了一种形态保留的氮掺杂分级多孔碳,其特征在于高度发达的微孔与有序介孔相结合。由于这种独特的微孔核-介孔壳结构和显著增强的孔隙率,实现了CO吸附容量和动力学的同时提高。该策略不仅为设计其他核壳结构的MOF复合材料铺平了道路,而且为制备用于CO捕获的容量和动力学增加的碳材料提供了一种有前景的方法。