Department of Civil Engineering , The University of Hong Kong , Pokfulam , Hong Kong.
UNESCO Centre for Membrane Science and Technology, School of Chemical Engineering , University of New South Wales , Sydney , New South Wales 2052 , Australia.
Environ Sci Technol. 2019 May 7;53(9):5301-5308. doi: 10.1021/acs.est.9b00473. Epub 2019 Apr 18.
Thin-film nanocomposite (TFN) membranes have been widely studied over the past decade for their desalination applications. For some cases, the incorporation of nonporous hydrophilic nanofillers has been reported to greatly enhance membrane separation performance, yet the underlying mechanism is poorly understood. The current study systematically investigates TFN membranes incorporated with silver nanoparticles (AgNPs). For the first time, we reveal the formation of nanochannels of approximately 2.5 nm in size around the AgNPs, which can be attributed to the hydrolysis of trimesoyl chloride monomers and thus the termination of interfacial polymerization by the water layer around each hydrophilic nanoparticle. These nanochannels nearly tripled the membrane water permeability for the optimal membrane. In addition, this membrane showed increased rejection against NaCl, boron, and a set of small-molecular organic compounds (e.g., propylparaben, norfloxacin, and ofloxacin), thanks to its combined effects of improved size exclusion, enhanced Donnan exclusion, and suppressed hydrophobic interaction. Our work provides fundamental insights into the formation and transport mechanisms involved in solid-filler incorporated TFN membranes. Future studies should take advantage of this spontaneous nanochannel formation in the design of TFN to overcome the classical membrane permeability-selectivity trade-off.
在过去的十年中,人们广泛研究了用于脱盐应用的薄膜纳米复合(TFN)膜。在某些情况下,已经报道了掺入无孔亲水性纳米填料可以极大地提高膜分离性能,但基础机制仍了解甚少。本研究系统地研究了掺入银纳米颗粒(AgNPs)的 TFN 膜。我们首次揭示了在 AgNPs 周围形成了大约 2.5nm 大小的纳米通道,这归因于三酰氯单体的水解,以及每个亲水性纳米颗粒周围的水层终止了界面聚合。对于最佳膜,这些纳米通道使膜水透过率几乎增加了两倍。此外,由于改进的尺寸排阻、增强的Donnan 排斥和抑制的疏水相互作用,该膜对 NaCl、硼以及一组小分子有机化合物(例如对羟基苯甲酸丙酯、诺氟沙星和氧氟沙星)的截留率增加。我们的工作为固体填充 TFN 膜中涉及的形成和传输机制提供了基本的见解。未来的研究应该利用这种自发的纳米通道形成来设计 TFN,以克服经典的膜渗透性-选择性权衡。