Institute of Environmental Engineering & Nano-Technology, Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen 518055, Guangdong, China; Guangdong Provincial Engineering Research Center for Urban Water Recycling and Environmental Safety, Tsinghua-Shenzhen International Graduate School, Tsinghua University, Shenzhen 518055, Guangdong, China; School of Environment, Tsinghua University, Beijing 100084, China.
Institute of Environmental Engineering & Nano-Technology, Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen 518055, Guangdong, China; College of Chemistry and Environmental Engineering, Shenzhen University, Shenzhen 518060, China.
Sci Total Environ. 2022 Mar 25;814:152698. doi: 10.1016/j.scitotenv.2021.152698. Epub 2021 Dec 30.
Heterogeneous advanced oxidation processes (AOPs) are commonly employed for the degradation of recalcitrant contaminants, however, practical application of heterogeneous AOPs has been limited by their low activation efficiency and inefficient utilization of radicals. Herein, this study demonstrates for the first time that 2D honeycomb-like holey membranes assembled by CoO nanosheets, serve as an excellent activator for peroxymonosulfate (PMS) and aid in rapid pollutant removal. The CoO membrane achieved 100% target pollutant ranitidine removal and a membrane retention time of only ~385 ms with the degradation rate 3-5 orders of magnitude faster than that achieved by conventional heterogeneous catalysis. Ranitidine degradation was maintained at >90% for 13 h of continuous-flow operation at a high flux of 176 L m h bar. Furthermore, the CoO membrane could also effectively degrade several recalcitrant pollutants, including pharmaceutical personal care products, phenols, and dyes. SO and •OH were identified as the primary reactive oxygen species in the CoO membrane/PMS system, with Co providing the active site for PMS activation. This strategy of membrane-based AOP treatment offers helpful guidance for the design of other efficient heterogeneous catalytic systems and presents a novel approach to overcoming the limitations of conventional heterogeneous catalysis.
多相高级氧化技术（AOPs）常用于降解难降解污染物，但因其自由基活化效率低和利用率低，实际应用受到限制。本研究首次表明，由 CoO 纳米片组装而成的二维蜂窝状多孔膜可作为过一硫酸盐（PMS）的高效活化剂，促进污染物的快速去除。CoO 膜在 385ms 内实现了 100%的目标污染物雷尼替丁去除率，降解速率比传统多相催化快 3-5 个数量级。在 176L·m-2·h-1 的高通量下连续运行 13h 后，雷尼替丁的降解率仍保持在>90%。此外，CoO 膜还可以有效降解几种难降解的污染物，包括药物个人护理产品、酚类和染料。SO 和 •OH 被确定为 CoO 膜/PMS 体系中的主要活性氧物质，Co 提供了 PMS 活化的活性位点。这种基于膜的 AOP 处理策略为设计其他高效多相催化体系提供了有益的指导，并为克服传统多相催化的局限性提供了一种新方法。
