Processing–Structure–Performance Relationships of Microporous Metal–Organic Polymers for Size-Selective Separations
Processing–Structure–Performance Relationships of Microporous Metal–Organic Polymers for Size-Selective Separations
复制标题
用于尺寸选择性分离的微孔金属—有机聚合物的加工—结构—性能关系
DOI：
10.1021/acsami.0c14827
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发表时间：
2021
影响因子：
9.5
通讯作者：
Hanrath, Tobias
中科院分区：
文献类型：
--
作者：
Huang, Jen-Yu;Xu, Yuanze;Milner, Phillip J.;Hanrath, Tobias
小分子杂质，如N-亚硝基二甲胺（NDMA），已经渗透到仿制药行业，导致自2018年以来超过43个国家的常用处方血压和胃药召回，并直接影响数千万患者。从药物分子中去除小分子杂质如NDMA的一种有希望的策略是通过尺寸排阻，其中由于其较小的尺寸，通过选择性吸附到（微）多孔材料上来去除污染物。然而，目前的溶液相尺寸排阻分离主要受到通量-选择性权衡的限制。在这里，我们报告了一个生物启发的解决方案，以克服这些关键的挑战，利用组装成层次多孔结构的原子精确的积木。我们介绍了一种自下而上的方法，形成微孔，介孔，宏观超结构同时使用功能化的氧锆簇作为积木。此外，我们利用光聚合的最新进展来设计宏观流动结构以减轻背压。基于这些多尺度设计原则，我们设计了简单，廉价的设备，能够将NDMA从受污染的药物中分离出来。除了这个紧迫的模型系统，我们预计这种设计策略，以开辟迄今未开发的途径，纳米材料超结构制造的一系列尺寸排阻纯化策略。
Small-molecule impurities, such asN-nitrosodimethylamine (NDMA), have infiltrated the generic drug industry, leading to recalls in commonly prescribed blood pressure and stomach drugs in over 43 countries since 2018 and directly affecting tens of millions of patients. One promising strategy to remove small-molecule impurities like NDMA from drug molecules is by size exclusion, in which the contaminant is removed by selective adsorption onto a (micro)porous material due to its smaller size. However, current solution-phase size-exclusion separations are primarily limited by the throughput-selectivity trade-off. Here, we report a bioinspired solution to conquer these critical challenges by leveraging the assembly of atomically precise building blocks into hierarchically porous structures. We introduce a bottom-up approach to form micropores, mesopores, and macroscopic superstructures simultaneously using functionalized oxozirconium clusters as building blocks. Further, we leverage recent advances in photopolymerization to design macroscopic flow structures to mitigate backpressure. Based on these multiscale design principles, we engineer simple, inexpensive devices that are able to separate NDMA from contaminated drugs. Beyond this urgent model system, we expect this design strategy to open up hitherto unexplored avenues of nanomaterial superstructure fabrication for a range of size-exclusion purification strategies.