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Interlayer-confined two-dimensional manganese oxide-carbon nanotube catalytic ozonation membrane for efficient water purification

《化学科学与工程前沿（英文）》 2022年第16卷第5期页码 731-744 doi: 10.1007/s11705-021-2110-6

摘要： Catalytic ozonation technology has attracted copious attention in water purification owing to its favorable oxidative degradation of pollutants and mitigation of membrane fouling capacity. However, its extensive industrial application has been restricted by the low ozone utilization and limited mass transfer of the short-lived radical species. Interlayer space-confined catalysis has been theoretically proven to be a viable strategy for achieving high catalytic efficiency. Here, a two-dimensional MnO₂-incorporated ceramic membrane with tunable interspacing, which was obtained via the intercalation of a carbon nanotube, was designed as a catalytic ozonation membrane reactor for degrading methylene blue. Benefiting from the abundant catalytic active sites on the surface of two-dimensional MnO₂ as well as the ultralow mass transfer resistance of fluids due to the nanolayer confinement, an excellent mineralization effect, i.e., 1.2 mg O_3(aq) mg^–1 TOC removal (a total organic carbon removal rate of 71.5%), was achieved within a hydraulic retention time of 0.045 s of pollutant degradation. Further, the effects of hydraulic retention time and interlayer spacing on methylene blue removal were investigated. Moreover, the mechanism of the catalytic ozonation employing catalytic ozonation membrane was proposed based on the contribution of the Mn(III/IV) redox pair to electron transfer to generate the reactive oxygen species. This innovative two-dimensional confinement catalytic ozonation membrane could act as a nanoreactor and separator to efficiently oxidize organic pollutants and enhance the control of membrane fouling during water purification.

关键词： catalytic membrane reactor catalytic ozonation nanoconfinement two-dimensional manganese oxide

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利用商用凝胶型离子交换树脂实现超微纳米颗粒的大规模生产与高效水处理 Article

程思凯, 钱杰书, 张孝林, 鲁振达, 潘丙才

《工程（英文）》 2023年第23卷第4期页码 149-156 doi: 10.1016/j.eng.2021.09.010

摘要：

纳米技术为深度水处理提供了新的机遇。然而，高活性超微（<5 nm）纳米颗粒材料的大规模生产仍存在挑战，且超微材料在实际水处理中也存在操作困难等问题，阻碍了纳米技术在水污染控制领域的推广应用。针对这些问题，我们提出了一种简便的解决方法，即以商用凝胶型离子交换树脂N201 为载体合成超微纳米颗粒。N201 是一种季铵化的毫米级聚（苯乙烯二乙烯基苯共聚）小球。在N201 中通过简单的浸渍-沉淀获得了水合氧化铁（HFO）、水合氧化锰（HMO）、硫化镉（CdS）和零价铁（ZVI）等纳米颗粒，所有纳米颗粒的尺寸都小于5 nm。中试生产表明该合成方法方便放大，并制备了大量亚5 nm HFO颗粒。关于超微纳米颗粒的合成机理，我们认为每个在水中溶胀的N201 小球内都包含连续均匀水相，使反应物可快速地扩散到树脂球内部（7 s 内从小球表面扩散到中心），从而实现纳米颗粒的爆发成核，形成超窄尺寸分布的晶核。此外，交联聚合物链间还可形成狭窄的孔隙（直径<5 nm），可防止在其中形成的纳米颗粒过度生长。由于N201 载体具有毫米级尺寸，所制备的复合纳米材料可方便用于连续流装置中。批次实验和柱吸附测试表明，超微HFO颗粒对As(III/V)的吸附性能比约17 nm的HFO显著增强。本研究有望进一步促进纳米技术在实际水处理中的推广应用。

关键词：纳米尺寸效应纳米限域吸附内球配位再生