通过调控金属-有机框架中的金属-炔键化学相互作用克服 C H 吸附与分离性能之间的权衡。
Overcoming the Trade-Off between C H Sorption and Separation Performance by Regulating Metal-Alkyne Chemical Interaction in Metal-Organic Frameworks.
机构信息
State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, 350002, Fujian, P. R. China.
Fujian Science and Technology Innovation Laboratory for Optoelectronic Information of China, Fuzhou, 350108, Fujian, P. R. China.
出版信息
Angew Chem Int Ed Engl. 2023 May 22;62(22):e202302882. doi: 10.1002/anie.202302882. Epub 2023 Apr 25.
Designing porous materials for C H purification and safe storage is essential research for industrial utilization. We emphatically regulate the metal-alkyne interaction of Pd and Pt on C H sorption and C H /CO separation in two isostructural NbO metal-organic frameworks (MOFs), Pd/Cu-PDA and Pt/Cu-PDA. The experimental investigations and systematic theoretical calculations reveal that Pd in Pd/Cu-PDA undergoes spontaneous chemical reaction with C H , leading to irreversible structural collapse and loss of C H /CO sorption and separation. Contrarily, Pt in Pt/Cu-PDA shows strong di-σ bond interaction with C H to form specific π-complexation, contributing to high C H capture (28.7 cm g at 0.01 bar and 153 cm g at 1 bar). The reusable Pt/Cu-PDA efficiently separates C H from C H /CO mixtures with satisfying selectivity and C H capacity (37 min g ). This research provides valuable insight into designing high-performance MOFs for gas sorption and separation.
设计用于 CH 净化和安全储存的多孔材料是工业应用的重要研究方向。我们着重调控 Pd 和 Pt 的金属-炔键相互作用，以研究两种同构结构的 NbO 金属有机骨架（MOF）材料，即 Pd/Cu-PDA 和 Pt/Cu-PDA 中的 CH 吸附和 CH/CO 分离性能。实验研究和系统的理论计算表明，Pd/Cu-PDA 中的 Pd 与 CH 发生自发化学反应，导致不可逆的结构坍塌和 CH/CO 吸附和分离能力的丧失。相反，Pt/Cu-PDA 中的 Pt 与 CH 之间表现出强的二σ键相互作用，形成特定的π-络合作用，从而实现高 CH 捕获能力（在 0.01 bar 时为 28.7 cm 3 g -1 ，在 1 bar 时为 153 cm 3 g -1 ）。可重复使用的 Pt/Cu-PDA 能够有效地从 CH/CO 混合物中分离出 CH，具有令人满意的选择性和 CH 容量（37 min g -1 ）。这项研究为设计用于气体吸附和分离的高性能 MOF 提供了有价值的见解。
Zotero 插件