State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, Beijing 100084, China.
State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, Beijing 100084, China.
Sci Total Environ. 2022 Oct 15;843:156904. doi: 10.1016/j.scitotenv.2022.156904. Epub 2022 Jun 23.
The biotreated effluent of landfill leachate still contains numerous refractory organic contaminants, which poses potential threats to human health and ecosystems. Influenced by landfill ages and other factors, the concentration of organic matter varies. Heterogeneous catalytic ozonation (HCO) is a promising technology for advanced wastewater treatment. Aiming to achieve the up-to-standard discharge of low-concentration landfill leachate (COD ≈ 108 mg·L) and improve the biodegradability of high-concentration landfill leachate (COD ≈ 1720 mg·L), the active component Fe was incorporated into a firm Ni-induced C-AlO-framework (CAF) composite support to synthesize a Fe-CAF catalyst for efficient catalytic ozonation. When the Fe-CAF dosage was 4 g·L, the gas flow rate was 0.5 L·min, and the ozone concentration was 20.0 mg·L, the COD of low-concentration landfill leachate effluent decreased to 43 mg·L, and the COD removal rate constant of low-concentration landfill leachate was 154% higher than that of pure ozone. For high-concentration landfill leachate with the BOD/COD of 0.058, the COD removal efficiency in Fe-CAF/O increased from 39% to 57% compared with ozonation, and the effluent BOD/COD increased to 0.282. Furthermore, the addition of hydrogen peroxide (HO) and peroxymonosulfate (PMS) can further enhance the treatment performance of Fe-CAF/O process and different strengthening mechanisms were revealed. The results indicated that surface hydroxyls on the Fe-CAF catalyst surface were the main catalytic sites for ozone, and hydroxyl radical (•OH) and singlet oxygen (O) were identified as the main reactive oxygen species for the removal of organics in landfill leachate. Adding HO can promote the generation of •OH for nonselective degradation of various organics, while PMS mainly enhanced the production of O to decompose macromolecular humus. This work highlighted an efficient Fe-CAF ozone catalyst and an innovative peroxide intensified HCO strategy for the advanced treatment of landfill leachate.
垃圾渗滤液经生物处理后仍含有大量难降解有机污染物,对人类健康和生态系统构成潜在威胁。受垃圾填埋场年龄等因素影响,有机物浓度存在差异。多相催化臭氧化(HCO)是一种很有前途的废水深度处理技术。本研究旨在实现低浓度垃圾渗滤液(COD≈108mg·L)达标排放,并提高高浓度垃圾渗滤液(COD≈1720mg·L)的可生化性,将活性组分 Fe 掺入到稳定的 Ni 诱导的 C-AlO 骨架(CAF)复合载体中,合成了一种用于高效催化臭氧化的 Fe-CAF 催化剂。当 Fe-CAF 剂量为 4g·L、气体流速为 0.5L·min 和臭氧浓度为 20.0mg·L 时,低浓度垃圾渗滤液的 COD 降低到 43mg·L,低浓度垃圾渗滤液的 COD 去除速率常数比纯臭氧高 154%。对于 BOD/COD 为 0.058 的高浓度垃圾渗滤液,Fe-CAF/O 中的 COD 去除效率从臭氧化的 39%提高到 57%,出水 BOD/COD 提高到 0.282。此外,添加过氧化氢(HO)和过一硫酸盐(PMS)可以进一步增强 Fe-CAF/O 工艺的处理性能,并揭示了不同的强化机制。结果表明,Fe-CAF 催化剂表面的表面羟基是臭氧的主要催化位点,而羟基自由基(•OH)和单线态氧(O)被确定为去除垃圾渗滤液中有机物的主要活性氧物种。添加 HO 可以促进•OH 的生成,实现对各种有机物的非选择性降解,而过一硫酸盐主要增强 O 的生成,以分解大分子腐殖质。这项工作突出了一种高效的 Fe-CAF 臭氧催化剂和一种创新的过氧化物强化 HCO 策略,用于垃圾渗滤液的深度处理。