Zeng Heng, Xie Mo, Huang Yong-Liang, Zhao Yifang, Xie Xiao-Jing, Bai Jian-Ping, Wan Meng-Yan, Krishna Rajamani, Lu Weigang, Li Dan
College of Chemistry and Materials Science, Jinan University, Guangzhou, 510632, P. R. China.
Van't Hoff Institute for Molecular Sciences, University of Amsterdam, Science Park 904, 1098 XH, Amsterdam, The Netherlands.
Angew Chem Int Ed Engl. 2019 Jun 17;58(25):8515-8519. doi: 10.1002/anie.201904160. Epub 2019 May 9.
Porous materials that can undergo pore-structure adjustment to better accommodate specific molecules are ideal for separation and purification. Here, we report a stable microporous metal-organic framework, JNU-1, featuring one-dimensional diamond-shaped channels with a high density of open metal sites arranged on the surface for the cooperative binding of acetylene. Together with its framework flexibility and appropriate pore geometry, JNU-1 exhibits an induced-fit behavior for acetylene. The specific binding sites and continuous framework adaptation upon increased acetylene pressure are validated by molecular modeling and in situ X-ray diffraction study. This unique induced-fit behavior endows JNU-1 with an unprecedented increase in the acetylene binding affinity (adsorption enthalpy: up to 47.6 kJ mol at ca. 2.0 mmol g loading).
能够进行孔结构调整以更好地容纳特定分子的多孔材料是分离和纯化的理想选择。在此，我们报道了一种稳定的微孔金属有机框架JNU-1，其具有一维菱形通道，在表面排列有高密度的开放金属位点，用于乙炔的协同结合。结合其框架灵活性和合适的孔几何形状，JNU-1对乙炔表现出诱导契合行为。通过分子模拟和原位X射线衍射研究验证了特定的结合位点以及随着乙炔压力增加而发生的连续框架适应性变化。这种独特的诱导契合行为使JNU-1的乙炔结合亲和力前所未有的增加（在约2.0 mmol g负载量下吸附焓高达47.6 kJ mol）。
