Large-Scale Metal-Organic Framework Nanoparticle Monolayers with Controlled Orientation for Selective Transport of Rare-Earth Elements.
Large-Scale Metal-Organic Framework Nanoparticle Monolayers with Controlled Orientation for Selective Transport of Rare-Earth Elements.
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具有受控取向的大规模金属有机框架纳米粒子单层，用于稀土元素的选择性传输。
DOI：
10.1021/jacs.3c02716
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发表时间：
2023-05
影响因子：
15
通讯作者：
Ming Qiu;Zhongpeng Zhu;Dianyu Wang;Zhe Xu;Weining Miao;Lei Jiang;Ye Tian
中科院分区：
文献类型：
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作者：
Ming Qiu;Zhongpeng Zhu;Dianyu Wang;Zhe Xu;Weining Miao;Lei Jiang;Ye Tian
由多孔纳米粒子组成的长程有序膜在精确分离中已经被追求了很长时间。然而，大多数的制造方法受到有限的衬底或缺乏对晶体取向的精确控制的影响。在此，大规模的金属有机框架（MOF）单层膜的取向控制，通过界面自组装过程中所限制的超亲液基板。反应物微滴的超扩散导致在不混溶的油下形成一个封闭的反应器。伴随的M0 F（ZIF-8）颗粒自发地组装成具有受控取向的单层，所述受控取向由颗粒在液/液界面处的接触角确定，所述接触角可以通过溶剂组成来调节。其中，气体吸附和离子传输测试都证明了1111取向膜具有最小的传质阻力。所制备的膜对稀土元素具有选择性迁移能力，La ~（3+）/K ~+的选择性为14.3。分子动力学模拟表明，稀土选择性与离子膜结合能的明显差异，表明ZIF-8膜用于高效回收工业废物中的稀土的潜力。
Long-range ordered membranes comprised of porous nanoparticles have been pursued in precise separations for a long time. Yet most of the fabrication methods suffer from limited substrates or lack of precise control over crystal orientation. Herein, large-scale metal-organic framework (MOF) monolayer membranes with controlled orientations are prepared through an interfacial self-assembly process confined by superlyophilic substrates. The superspreading of reactant microdroplets results in an ultrathin liquid layer under an immiscible oil as a confined reactor. The concomitant MOF (ZIF-8) particles spontaneously assemble into monolayers with controlled orientations, determined by the particles' contact angles at the liquid/liquid interface, which can be regulated by solvent compositions. Therein both gas-adsorption and ion-transport tests prove that the ⟨111⟩-oriented membrane exhibits a minimized mass-transfer resistance. The as-prepared membrane can selectively transport rare-earth elements (REEs), and a La3+/K+ selectivity of 14.3 is achieved. Molecular dynamics simulations reveal that the REEs-selectivity is associated with the distinct difference in ion-membrane binding energies, demonstrating the potential of ZIF-8 membranes for use in high-efficiency recovery of REEs from industrial wastes.