In this study, a facile hydrothermal approach was used to synthesize the MOFs materials [Mn-doped MIL-101 (Fe)]. These materials were subsequently subjected to high temperature annealing process via calcination to generate the MOFs derivatives (MnFeOx). The synthesized materials were utilized for the removal of sulfadiazine (SDZ) removal through activated peroxymonosulfate (PMS). At the optimum Mn doping, the removal ratio of SDZ could reach 98.9 % (at natural pH) within 20 min. In addition, the study investigated the influence of PMS dosage, catalyst dosage, initial pH, various inorganic anions, and humic acid (HA) on the degradation of SDZ. The activation processes of both free and non-free radicals in the MnFeOx/PMS system were examined by free radical quenching experiments and electron paramagnetic resonance (EPR) techniques. The analysis of the degradation products of SDZ was conducted by using high performance liquid chromatography-mass spectrometry (HPLC-MS), and the breakdown pathways of SDZ in the MnFeOx/PMS system were proposed.
Nano zero valent iron (nZVI) is widely used in traditional hydrogen peroxide (H2O2)-based Fenton reactions for the degradation of persistent organic pollutants in aqueous environments. How to restrain the blocked electron transfer aroused from thickening of the iron oxide passivation layer and reinforce the Fe(III)/Fe(II) dynamic cycling is essential for Fenton reactions. In this work, a novel core-shell structural nZVI@Fe2P was fabricated and employed for the degradation of sulfadiazine (SDZ). Compared to nZVI, the nZVI@Fe2P demonstrated a significant performance and stability in the degradation of SDZ. Completed SDZ removal is achieved in less than 15 min and the SDZ removal kept over 60% even in the ninth consecutive cycles. Although the SDZ removal decreased dramatically to only 27.4% in the tenth cycle, the value could be restored to 80.6% after a facile rephosphorization process. Both experimental and density function theory (DFT) calculation revealed the dominant role of Fe2P in promoting H2O2 activation and strengthening the Fe(III)/Fe(II) dynamic cycling. In the nZVI@Fe2P/H2O2 system, the low impedance and high proton conductivity of the Fe2P shell layer played a dual function, i.e., accelerating electron transfer and donating electrons for the continuous Fenton reaction. This implication of these findings provides a novel strategy by integrating the state-of-the-art material science, advanced oxidation process, and mechanism elucidation for practical environmental wastewater remediation.
Active chlorines (ACs) can selectively oxidize contaminants with benzene rings to recycle surfactants, which greatly facilitates the resource cycle. This paper firstly utilized Tween 80 to assist in ex-situ washing the ciprofloxacin (CI) contaminated soil, including the solubilization experiment, shake washing and soil column washing, all of which showed that 2 g/L of Tween 80 (TW 80) was the most effective in removing CI. Then electrochemically treated the collected soil washing effluent (SWE) at 10 V with an electrolyte of 20 mM NaCl + 10 mM Na2SO4; Pre-experiments screened the range of electrode spacing, pH and temperature, based on which an orthogonal design Table L9 (34) was designed. Visual analysis and ANOVA were performed on the ciprofloxacin removal efficiency and Tween 80 retention efficiency during the orthogonal experiments in 9 groups, and the results showed that CI was usually degraded within 30 min, and 50% of TW 80 was still present at the end of the experiment, and there was no significant effect of all three factors. LC-MS demonstrated that CI was mainly degraded synergistically by ·OH and ACs, and ·OH effectively reduced the biotoxicity of the SWE, so the mixed electrolyte may be more suitable for the electrochemical recycling system of ACs. This paper conducted the washing remediation study of CI-contaminated soil for the first time, and applied the theory of selective oxidation by ACs on benzene ring to treat the SWE, which provides a new treatment idea for antibiotic-contaminated soil.
针对被苯胺污染的土壤淋洗液的处理问题,以钌钛锡钛基板为阳极板,钛板为阴极板,对模拟污染土壤淋洗液中的苯胺和环糊精进行电化学处理,研究了电解质浓度,电流密度、环糊精浓度对苯胺和环糊精处理的效果,探究活性氯是否对苯胺有选择性氧化的作用.通过单因素试验和正交试验,所得的最佳降解条件为:环糊精浓度为160 mg/L,电流密度为20 mA/cm2,NaCl浓度为20 mmol/L.在最佳条件下,电解1 h苯胺的降解率达98.77%,苯胺的降解过程符合一级动力学方程(R2=0.93577).当淋洗液中的苯胺降解完全时,环糊精的保留率仅为2%,说明活性氯对苯胺选择性氧化作用不明显.
通过对厌氧颗粒污泥进行驯化,在(38±1)℃的条件下,探究了不同pH、不同聚乙二醇分子量对聚乙二醇废水的厌氧生物处理效果.在pH=6.0、7.0、8.0、9.0的条件下厌氧生物处理高质量浓度聚乙二醇废水,四个反应器中上清液COD初始质量浓度分别为11600、11200、11600、11800 mg/L,反应器稳定运行6 d后,各反应器内COD质量浓度分别降至1600、520、800、880 mg/L.在pH=7.5的条件下厌氧生物处理浓度为10.0 g/L的不同分子量的聚乙二醇废水,PEG-2000、PEG-4000、PEG-6000、PEG-10000四个反应器中上清液的初始COD浓度分别为11200、11600、12000、11200 mg/L,反应器稳定运行5 d后,四个反应器中COD分别降至200、240、280、400 mg/L.