Shao Kai, Wen Hui-Min, Liang Cong-Cong, Xiao Xiaoyan, Gu Xiao-Wen, Chen Banglin, Qian Guodong, Li Bin
State Key Laboratory of Silicon Materials, School of Materials Science and Engineering, Zhejiang University, Hangzhou, 310027, China.
College of Chemical Engineering, Zhejiang University of Technology, Hangzhou, 310014, China.
Angew Chem Int Ed Engl. 2022 Oct 10;61(41):e202211523. doi: 10.1002/anie.202211523. Epub 2022 Sep 2.
Developing porous materials to overcome the trade-off between adsorption capacity and selectivity for C H /CO separation remains a challenge. Herein, we report a stable HKUST-1-like MOF (ZJU-50a), featuring large cages decorated with high density of supramolecular binding sites to achieve both high C H storage and selectivity. ZJU-50a exhibits one of the highest C H storage capacity (192 cm g ) and concurrently high C H /CO selectivity (12) at 298 K and 1 bar. Single-crystal X-ray diffraction studies on gas-loaded ZJU-50a crystal unveil that the incorporated supramolecular binding sites can selectively take up C H molecule but not CO to result in both high C H storage and selectivity. Breakthrough experiments validated its separation performance for C H /CO mixtures, providing a high C H recovery capacity of 84.2 L kg with 99.5 % purity. This study suggests a novel strategy of engineering supramolecular binding sites into MOFs to overcome the trade-off for this separation.
开发多孔材料以克服在CH/CO分离中吸附容量和选择性之间的权衡仍然是一项挑战。在此，我们报道了一种稳定的类HKUST-1金属有机框架（ZJU-50a），其具有装饰有高密度超分子结合位点的大笼子，以实现高CH储存量和选择性。ZJU-50a在298K和1巴下表现出最高的CH储存容量之一（192 cm g ），同时具有高的CH/CO选择性（12）。对负载气体的ZJU-50a晶体进行的单晶X射线衍射研究表明，引入的超分子结合位点可以选择性地吸收CH分子而不是CO分子，从而实现高CH储存量和选择性。突破实验验证了其对CH/CO混合物的分离性能，提供了84.2 L kg的高CH回收容量，纯度为99.5%。这项研究提出了一种将超分子结合位点工程化到金属有机框架中的新策略，以克服这种分离中的权衡。
