Department of Environmental Engineering, College of Ecology and Environment, Nanjing Forestry University, Nanjing 210037, China.
Department of Environmental Engineering, College of Ecology and Environment, Nanjing Forestry University, Nanjing 210037, China.
J Environ Manage. 2023 Dec 1;347:119187. doi: 10.1016/j.jenvman.2023.119187. Epub 2023 Oct 5.
Carbon materials used for catalysis in advanced oxidation processes tend to be obtained from cheap and readily available raw materials. We constructed a carbon material, OSC@FeO, by loading FeO onto the pyrolyzed hazardous waste oily sludge. OSC@FeO was then used to activate peroxymonosulfate (PMS) for the removal of tetracycline hydrochloride (TTCH) from water. At 298 K, 0.2 g⋅L of catalyst and 0.3 g⋅L of PMS, the reaction rate constant of the OSC@I-2/PMS system reached 0.079 min, with a TTCH removal efficiency of 92.6%. The degradation efficiency of TTCH remained at 81% after five cycles. The specific surface area and pore volume of OSC@I-2 were 263.9 m⋅g and 0.42 cm⋅g, respectively, which improved the porous structure of the carbon material and provided more active points, thus improving the catalytic performance. N and S were doped into the oily sludge carbon due to the presence of N- and S-containing compounds in the raw oily sludge. N and S doping led to more electron-rich sites with higher negative charges in OSC@I-2 and gave the oily sludge carbon a higher affinity to PMS, thereby promoting its ability to activate PMS. Sulfate radicals (SO‾) played a dominant role in the degradation of TTCH, with demethylation and the breaking of double bonds being a possible degradation pathway. A biotoxicity test showed that the microbial toxicity of the degradation intermediates was significantly reduced. This work provides a strategy for the application of PMS-based catalysts derived from waste carbon resources.
用于高级氧化过程中催化的碳材料往往是由廉价且易得的原材料制备得到的。我们通过将 FeO 负载到热解危险废物油泥上构建了一种碳材料 OSC@FeO。然后，OSC@FeO 用于激活过一硫酸盐（PMS）以去除水中的盐酸四环素（TTCH）。在 298 K 下，催化剂用量为 0.2 g⋅L 和 PMS 用量为 0.3 g⋅L 时，OSC@I-2/PMS 体系的反应速率常数达到 0.079 min，TTCH 的去除效率为 92.6%。TTCH 的降解效率在经过五次循环后仍保持在 81%。OSC@I-2 的比表面积和孔体积分别为 263.9 m⋅g 和 0.42 cm⋅g，这改善了碳材料的多孔结构，并提供了更多的活性点，从而提高了催化性能。由于原始油泥中含有含 N 和 S 的化合物，因此 N 和 S 被掺杂到油泥碳中。N 和 S 的掺杂导致 OSC@I-2 中具有更多富电子的位点和更高的负电荷，从而使油泥碳对 PMS 具有更高的亲和力，从而提高了其激活 PMS 的能力。硫酸盐自由基（SO‾）在 TTCH 的降解中起主导作用，可能的降解途径是脱甲基和双键断裂。生物毒性试验表明，降解中间体的微生物毒性显著降低。这项工作为基于废碳资源的 PMS 催化剂的应用提供了一种策略。
