School of Chemical Engineering, Sichuan University, Chengdu, 610065, China.
School of Chemical Engineering, Sichuan University, Chengdu, 610065, China.
Environ Pollut. 2021 Jan 1;268(Pt B):115930. doi: 10.1016/j.envpol.2020.115930. Epub 2020 Oct 31.
Advanced oxidation processes (AOPs) based on peroxymonosulfate (PMS) activation have attracted increasing attention in recent years for organic pollutants removal. Herein, we put forward a facile method to form cobalt phosphide/carbon composite for PMS activation. Combining impregnation approach with pyrolysis treatment enabled the formation of CoP/biochar composites using baker's yeast and Co as precursors. The as-synthesized products exhibited excellent catalytic activity for sulfamethoxazole (SMX) degradation over the pH range 3.0-9.0 b y activating PMS. For example, 100% of SMX (20 mg L) removal was achieved in 20 min with catalyst dosage of 0.4 g L and PMS loading of 0.4 g L. Near zero Co leaching was observed during catalytic reaction, which remarkably lowered the toxic risk of transition metal ion in water. Meanwhile, the reusability of catalyst could be attained by thermal treatment. SMX degradation intermediates were identified by liquid chromatography-mass spectrometry (LC-MS), which facilitated the proposal of possible SMX degradation pathways. Ecological Structure Activity Relationships (ECOSAR) analysis indicated that SMX degradation intermediates may not pose ecological toxicity to the environment. Further investigation verified that CoP/biochar composites could set off PMS activation not only for the degradation of SMX but also for other sulfonamides. In this study, we not only developed a facile method of utilizing environmental-benign biomass for transition metal phosphide/carbon composite formation, but also achieved highly efficient antibiotic elimination by PMS-based AOP.
基于过一硫酸盐(PMS)活化的高级氧化工艺(AOPs)近年来在去除有机污染物方面受到了越来越多的关注。在此,我们提出了一种简便的方法来制备用于 PMS 活化的磷化钴/碳复合材料。通过浸渍法和热解处理相结合,使用面包酵母和 Co 作为前体制备了 CoP/生物炭复合材料。所合成的产物在 pH 值为 3.0-9.0 的范围内通过活化 PMS 对磺胺甲恶唑(SMX)的降解表现出优异的催化活性。例如,在催化剂用量为 0.4 g/L 和 PMS 用量为 0.4 g/L 的条件下,仅需 20 min 即可实现 100%的 SMX(20 mg/L)去除。在催化反应过程中几乎没有观察到 Co 浸出,这显著降低了水中过渡金属离子的毒性风险。同时,通过热处理可以实现催化剂的重复使用。通过液相色谱-质谱(LC-MS)鉴定了磺胺甲恶唑的降解中间产物,这有助于提出磺胺甲恶唑的可能降解途径。生态结构活性关系(ECOSAR)分析表明,磺胺甲恶唑降解中间产物对环境可能没有生态毒性。进一步的研究验证了 CoP/生物炭复合材料不仅可以引发 PMS 活化,用于 SMX 的降解,还可以用于其他磺胺类抗生素的去除。在本研究中,我们不仅开发了一种利用环境友好型生物质制备过渡金属磷化物/碳复合材料的简便方法,而且通过基于 PMS 的 AOP 实现了高效去除抗生素。