As one of the core advanced oxidation processes, UV photo-Fenton technology demonstrates unique advantages in treating refractory organic wastewater. This study focuses on strontium zirconate-based catalysts with a perovskite structure. To address the high recombination rate of electron-hole pairs and weak visible-light response in conventional photocatalysts, an innovative iron-doped modification system was developed. A series of SrFexZr1-xO3-delta catalysts with gradient variations in Fe/Zr molar ratios were synthesized via a co-precipitation method, and their performance in the UV-H2O2 synergistic catalytic oxidation system for mcresol wastewater treatment was investigated. Experimental results demonstrated that SrFe0.25Zr0.75O3 exhibited optimal catalytic performance when x = 0.25. Subsequently, noble metals: Ag, Co, Pd were loaded onto the optimized catalyst surface using a sodium borohydride reduction method. XPS characterization confirmed that the metal loading effectively facilitated the directional migration of photogenerated electrons to the metal sites. Among the modified catalysts, Pd-SrFe0.25Zr0.75O3 displayed superior catalytic activity, with its apparent rate constant increasing by 43 % compared to the pristine material. This enhancement is attributed to the greater electronegativity of the metal element, which promotes the transfer of electrons from the metal to the catalyst, thus effectively decreasing the compounding rate of the electron-hole pairs and improving the photocatalytic effect of the catalysts. These findings not only provide novel insights into photocatalytic wastewater treatment but also offer valuable references for the modification of perovskite-type catalysts.
1,6-Hexamethylene diamino carbamate (HDC), i.e., a high-melting-point ester, is a precursor for the production of hexamethylene diisocyanate (HDI) via the non-phosgene process. Since HDI synthesis requires an anhydrous condition, the water content of raw HDC must be removed. Notably, the dehydration of solid organic esters at room temperature has been rarely reported. In this study, we systematically analyzed and investigated the physical properties of HDC, including its melting point, molten HDC viscosity, saturated vapor pressure, and solubility. Subsequently, the thermodynamic properties of HDC were characterized by thermogravimetric analysis-Fourier transform infrared spectroscopy (TG-FTIR), and differential scanning calorimetry (DSC) to investigate its thermal stability, enthalpy change, and thermal conductivity. HDC exhibited remarkable stability in an oxygen-free environment below 180 degrees C. Furthermore, molecular simulations were conducted to evaluate the binding force between HDC and water molecules. The binding energy of one HDC molecule with two water molecules was -37.56 kJ mol- 1, indicating a medium-strength hydrogen bond. Additionally, the spatial dimensions of the HDC molecule were 16.12 & Aring;, 7.91 & Aring;, and 5.59 & Aring;. Finally, two feasible drying methods, solid drying methods and new membrane dehydration after melting, along with critical control factors were proposed, offering novel insights into the selection of appropriate drying processes for materials with unique properties.
Evodiae Fructus (EF) is a hepatotoxic herbal medicine whose toxicity is linked to CYP3A4-mediated metabolic activation of evodiamine (EVD), as identified in our previous study using high-resolution MS platform. In clinic, EF is often combined with Licorice to enhance efficacy and reduce toxicity, but the detoxification mechanism is unknown. In this study, we developed an integrated analytical strategy combining multi-mass spectrometry techniques and biological experiments to investigate the detoxification mechanism of Licorice-EF combination. The changes in EVD serum contents, biochemical indexes and pathological sections in rats were monitored after Licorice administration, and correlation analysis was performed to clarify the detoxification effect of Licorice. In addition, the effect of the major components in Licorice on P450 enzymes and the electrophilic metabolites derived from EVD were investigated by combined application of UPLC-QQQ-MS/MS and UPLC-Q/TOF-MS/MS. Our study showed that the combined use of Licorice and EF in the ratio of 1:1 could significantly ameliorate EF-induced liver injury. The Licorice extract mainly inhibited the activities of CYP3A4, with isoliquiritigenin (ILG) exhibiting the most inhibitory potency with enzyme kinetics parameters kinact and KI at 0.034 min-1 and 0.63 μM, respectively. Furthermore, ILG not only significantly alleviated EVD-induced liver injury, but also obviously reduced the production of EVD-derived reactive metabolites. These results suggested that Licorice alleviated EF-induced liver injury by inhibition of metabolic activation of EF mediated by cytochrome P450s, providing stringent and scientific evidence for such combination from perspectives of metabolism-based interaction.
The conventional preparation of layered double hydroxide (LDH) often limits its catalytic effectiveness in advanced oxidation processes due to agglomeration and inadequate exposure of active sites. In this work, we present a simplified synthesis approach that utilizes zeolitic imidazolate frameworks (ZIF)-67 (Co) as a sacrificial template to in situ fabricate hollow polyhedral CoFe-LDH (HP-LDH), aimed at enhancing the degradation of dye contaminants in aqueous systems. The unique porous and polyhedral structure of HP-LDH, derived from the template, facilitates contact efficiency between the substrate and active metal sites, acting as an effective nanoreactor. The comparative degradation experiments of Acid Red 27 (AR27) in peroxymonosulfate (PMS) revealed that the degradation efficiency of HP-LDH was nearly twice that of conventional flake LDH (F-LDH). Under optimal conditions, the HP-LDH/PMS system attained a removal rate of 95% in just 15 min. The degradation of the dye relies on the action of both radical and non-radical species, particularly 1O2. Furthermore, the robust adaptability and versatility of HP-LDH/PMS to real water bodies, with a wide range of pH levels and coexisting inorganic anions, demonstrates its potential as a superior catalyst in wastewater treatment, offering a novel pathway for structural innovation of LDH materials in environmental applications.
The effective removal of toxic pollutants like m-cresol from wastewater remains challenging despite technological advancements. This study optimized total organic carbon (TOC) removal from m-cresol-contaminated wastewater using sodium percarbonate (SPC) oxidation through artificial neural network (ANN) and response surface methodology (RSM) modeling. TOC was selected as the optimization target due to its comprehensive representation of organic pollution levels. Six operational parameters were evaluated: initial pH, reaction time, SPC dosage, temperature, catalyst dosage, and initial m-cresol concentration. The ANN model demonstrated superior performance over RSM, achieving near-perfect R2 values with significant improvement in predictive accuracy. Under optimal ANN-derived conditions (pH 2.3, 35.7 min, 2.9 g L-1 SPC, 45.7 degrees C, 12.9 g L-1 catalyst, 75 mg L-1m-cresol), maximum experimental TOC removal reached 67.8%, significantly exceeding RSM's 38.2%. These findings demonstrate ANN's superior capability to model complex, nonlinear relationships in advanced oxidation processes, providing a robust optimization framework for enhancing wastewater treatment efficiency.
As chloride (Cl−) is a commonly found anion in natural water, it has a significant impact on electrocatalytic oxidation processes; yet, the mechanism of radical transformation on different types of anodes remains unexplored. Therefore, this study aims to investigate the influence of chlorine-containing environments on the electrocatalytic degradation performance of levofloxacin using BDD, Ti4O7, and Ru-Ti electrodes. The comparative analysis of the electrode performance demonstrated that the presence of Cl− improved the removal and mineralization efficiency of levofloxacin on all the electrodes. The enhancement was the most pronounced on the Ti4O7 electrode and the least significant on the Ru-Ti electrode. The evaluation experiments and EPR characterization revealed that the increased generation of hydroxyl radicals and active chlorine played a major role in the degradation process, particularly on the Ti4O7 anode. The electrochemical performance tests indicated that the concentration of Cl− affected the oxygen evolution potentials of the electrode and consequently influenced the formation of hydroxyl radicals. This study elucidates the mechanism of Cl− participation in the electrocatalytic degradation of chlorine-containing organic wastewater. Therefore, the highly chlorine-resistant electrocatalytic anode materials hold great potential for the promotion of the practical application of the electrocatalytic treatment of antibiotic wastewater.
MnO2-RuO2/carbon fiber cloth (MnO2-RuO2/CFC) composite electrode was successfully prepared by electrodeposition-calcination process and used to treat high-chlorine organic wastewater (HCOW). The MnO2-RuO2/CFC composite electrode showed excellent electrocatalysis oxidation ability compared with that of CFC electrode relying on the synergistic effect between MnO2 and RuO2. Under the optimal treatment condition of high-chlorine N,N-dimethylformamide (DMF) simulated wastewater (DMF initial concentration = 2000 mgL-1, current density = 100 mAcm(-2), electrode distance = 20 mm, initial pH = 7.0, and NaCl dosage = 8000 mgL-1), the removal rate of DMF was >80 % at 90 min, and the energy efficiency evaluation indicator was lower than 1.0 kWh m(-3). The active chlorine was the main oxidation species, while hydroxyl radical played the auxiliary role. DMF can be degraded into methylformamide, methanol, and hydrazine and then mineralized into N-2, CO2 and H2O. MnO2-RuO2/CFC composite electrode can be used at least 10 times in the treatment of high-chlorine real cephalosporin synthetic pharmaceutical wastewater, and the toxicity of the treated wastewater was significantly weakened, indicating the feasibility of the application of MnO2-RuO2/CFC composite electrode in the treatment of HCOW.
3DOMLaFeO(3) was prepared by template method combined with sol-gel method using monodisperse polystyrene (PS) microspheres as template, and Ag/3DOMLaFeO(3) perovskite catalyst was prepared by impregnation method combined with sodium borohydride reduction method. The catalysts were characterised by means of TG, XRD, SEM, BET, XPS, UV-vis DRS, etc. The photo-Fenton catalytic performance, stability and catalytic reaction mechanism of Ag/3DOMLaFeO(3) were studied with penicillin G potassium (PEN G) as the model pollutant. The results indicated that the as-prepared Ag/3DOMLaFeO(3) exhibited a three-dimensional ordered macroporous (3DOM) structure, and the light capture and mass transfer were enhanced through abundant pores and large specific surface area. Based on the surface plasmon resonance effect (SPR), Ag loading enhanced the absorption of the material in the visible light region, and inhibited the recombination of photogenerated carriers, which improved the photocatalytic performance of 3DOMLaFeO(3) under visible light. Under the conditions of hydrogen peroxide dosage of 1.5 mL center dot L-1, initial pH of 5, PEN G initial concentration of 100 mg center dot L-1, catalyst dosage of 300 mg center dot L-1, xenon lamp irradiation, the degration ratio of PEN G and the removal rate of TOC reached 99.99% and 85.45% within 120 min, respectively. In addition, it had a wide range of pH application, excellent stability and practical application value. The quenching experiment and ESR test showed that center dot OH and center dot O-2(-) were the reasons for high catalytic degradation. The least square method was used to fit the experimental data, and the results displayed that the degradation of PEN G was approximately in line with the first-order kinetic reaction.
BACKGROUND Wastewater containing m-cresol has become a global water environmental problem because its degradation is difficult, and it is highly toxic to plants, animals, and humans. The heterogeneous catalytic ozonation process has been widely used in the treatment of environmental pollution, so it is very important to study efficient catalysts. Perovskite catalysts have been widely investigated and applied in catalytic ozonation processes. Among them, strontium zirconate is a promising perovskite catalyst owing to its high oxidation efficiency and environmental friendliness. RESULTSS trontium zirconate was successfully synthesized via the co-precipitation method. To improve strontium zirconate catalytic performance, some methods such as changing the doping ratio of cobalt and iron, changing the amount of polyethylene glycol added, changing the calcination temperature, and changing the aging time were carried out during the synthesis process. Finally, the optimal conditions were determined. 0.4 g L-1 Sr2Co0.4Fe0.6ZrO6 prepared under the optimal conditions was used for catalytic ozonation of 100 ppm m-cresol, which achieved the optimum degradation (0.136 min(-1)), m-cresol conversion rate (92.2%) and total organic carbon removal rate (12.1%) within 20 min. CONCLUSION This work provides the best preparation conditions. The Sr2Co0.4Fe0.6ZrO6 catalyst, as prepared, is the optimal catalyst for catalytic ozonation of m-cresol among the investigated Sr(2)CoxFe(1-x)ZrO(6) catalysts. (c) 2024 Society of Chemical Industry (SCI).
Recently, visible-light-driven persulfate-based advanced oxidation processes (AOPs) employing heterogeneous catalysts to generate sulfate radicals (SO4·−) from peroxymonosulfate (PMS, HSO5−) have been extensively investigated in the field of water remediation, to remove organic contaminants. In this study, CeO2/2.0STO visible light photocatalyst with pore structure was synthesized by sol–gel method and impregnation method for photocatalytic methylene blue (MB) degradation via PMS activation. The MB degradation efficiency exhibited a high level at a broad pH range 2–12, and the presence of various organic matter and natural inorganic ions had no significant impact. When the PMS dosage was at 0–0.1 mM, the MB degradation efficiency still reached 100
Wastewater treatment, especially the efficient degradation of contaminants such as m-cresol, remains a pivotal challenge. This study investigates the application of artificial neural networks (ANN) in predicting total organic carbon (TOC) removal rates from m-cresol-contaminated wastewater by using the ultraviolet (UV)-Fenton oxidation process. Six key variables, namely, Fe2+ dosage, H2O2 dosage, catalyst quantity, reaction time, pH, and substrate concentration, were employed as inputs to the ANN model. Leveraging this multivariable input and a comprehensive data set, the ANN model projected a maximum TOC removal rate of 87.12%, validated by an efficiency of 86.26% achieved through experiments under the derived optimal conditions: Fe2+ dosage at 16.09 mg/L, H2O2 dosage at 1.40 mg/L, catalyst quantity at 0.11 g/L, reaction time of 29.80 min, initial pH of 3.66, and substrate concentration of 50 mg/L. Comparative analysis with other machine learning algorithms further revealed that the ANN model notably outperformed linear regression, support vector regression, and random forest in terms of precision. This work paves the way for resource-optimized experimental designs, fostering real-time wastewater monitoring and refining advanced oxidation process proficiency in industrial applications.
In this study, three-dimensional ordered microporous silica supported p-lanthanum ferrite and n-ceria (n-CeO2@p-LaFeO3/3DOM SiO2) was successfully synthesized as a visible lightdriven photocatalyst for activating peroxymonosulfate (PMS) to degrade Bisphenol A (BPA). In a wide pH range (2-12), the BPA degradation efficiency maintained at a high level, organic matter and natural inorganic ions had no significant negative impact. When the BPA concentration was as low as 2 mg$L-1, the removal rate in 60 min still reached 95.56%, indicating that the novel photocatalyst has potential application in the treatment of trace pollutants. The pore confinement effects of catalysts and the synergistic effect between LaFeO3 and CeO2 result in the excellent photocatalytic performance. We proposed the possible mechanism of BPA degradation, specifically involving the recognition and generation mechanism of reactive oxygen species (ROSs), adsorption processes and diffusion processes. In summary, the novel n-CeO2@p-LaFeO3/3DOM SiO2 would be a promising candidate photocatalytic material for practical sewage treatment. (c) 2023 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.
Highly efficient visible-light magnetic Fe3O4/3DOM LaMnO3 perovskite catalyst was prepared by sol–gel method and solvothermal method. The Fe3O4/3DOM LaMnO3 was adopted as catalyst to promote the photo-Fenton process, in which Penicillin G potassium (PEN G) was used as representative pollutant. The results showed that the catalyst exhibited excellent photo-Fenton oxidation degradation performances toward PEN G under visible light. Its application on degrading PEN G exhibited highly catalytic efficiency over a wide applicable pH range from 3 to 11. When the PEN G concentration was as low as 5 mg L−1, the PEN G degradation rate still reached 95.31
Membrane technology has been widely used to treat wastewater from a variety of industries, but it also results in a large amount of concentrated wastewater containing organic pollutants after membrane treatment, which is challenging to decompose. Here in this work, a series of perovskite SrFexZr1-xO3-δ catalysts were prepared via a modified co-precipitation method and evaluated for catalytic ozone oxidative degradation of m-cresol. An artificial neural intelligence networks (ANN) model was employed to train the experimental data to optimize the preparation parameters of catalysts, with SrFe0.13Zr0.87O3-δ being the optimal catalysts. The resultant catalysts before and after reduction were then thoroughly characterized and tested for m-cresol degradation. It was found that the co-doping of Fe and Zr at the B-site and the improvement of oxygen vacancies and oxygen active species by reduction dramatically increased TOC removal rates up to 5 times compared with ozone alone, with the conversion rate of m-cresol reaching 100%. We also proposed a possible mechanism for m-cresol degradation via investigating the intermediates using GC-MS, and confirmed the good versatility of the reduced SrFe0.13Zr0.87O3-δ catalyst to remove other common organic pollutants in concentrated wastewater. This work demonstrates new prospects for the use of perovskite materials in wastewater treatment.
As a high-performance liquid rocket fuel, unsymmetrical dimethylhydrazine (UDMH) will produce wastewater during transportation, storage and cleaning containers. The wastewater will have a bad impact on human health and ecological environment, and it must be properly handled. There are many reports about the technical feasibility of UDMH wastewater treatment. Less attention is paid to analyzing the impact on the environment during the treatment process. This paper quantifies the environmental impacts and economic benefits of four advanced oxidation processes for the treatment of UDMH wastewater based on life cycle assessment and life cycle costing methods. Taking the UDMH wastewater produced by an aerospace group of Tianjin, China as the research object, using Fenton method, UV-Fenton method, electro catalytic oxidation (EC) with ruthenium iridium titanium (Ti/TiO2-RuO2-IrO2) as electrode and electro catalytic oxidation with boron-doped diamond (BDD) as electrode as treatment methods, on the basis of the laboratory test, the industrialized device is adopted. The resource consumption, energy consumption, pollutant discharge and cost were compared when the TOC removal rate was the same, and a better method of treating unsymmetrical dimethyl hydrazine wastewater was discussed. The results show that the impact on most types of environments is as follows: UV-Fenton < Fenton < EC (BDD) < EC (Ti/TiO2-RuO2-IrO2), and the four advanced oxidation methods are all beneficial to reduce eutrophication. The life cycle cost of UV-Fenton is the lowest (US$1.53/m3). Combined with environmental and economic analysis, it can be seen that UV-Fenton is the best choice. Through sensitivity analysis, it can be seen that reducing chemical reagents and electricity consumption, and changing the way of generating electricity to renewable energy can significantly reduce the environmental and economic impact. The life cycle cost of EC(BDD) as the electrode is the highest (US$26.20/m3), but it can achieve a TOC removal rate of 97.75 %, so it is a better choice when only the removal rate is required regardless of cost.
为提升高盐废水生物处理效果,从制药厂二沉池中取活性污泥,采用逐步提高盐浓度的方法培养驯化出耐盐菌种.经筛选分离得到一株高耐盐菌M02,该菌株为Stenotrophomonas pavanii(寡养单胞菌)的一株潜在新菌,保藏号为CGMCC No.22898.单因素实验显示最适培养条件:pH值为7~8,温度为30℃,接种量为7%,盐的质量分数为1%~4%.菌株M02在实际高盐废水应用中,72 h COD去除率可达93.8%.该方法去除率明显高于普通活性污泥法(59.9%),具有实际应用价值.
以聚苯乙烯微球为模板,采用模板法联合溶胶-凝胶法制备了三维有序大孔(3DOM)材料La0.4Ce0.6FeO3(记作3DOM La0.4Ce0.6FeO3),并对其进行了表征.以亚甲基蓝为模型污染物,研究了3DOM La0.4Ce0.6FeO3的催化性能、稳定性和催化反应机理.实验结果表明,3DOM La0.4Ce0.6FeO3呈现3DOM结构,丰富的孔道和较大的比表面积增强了光的捕获与传质,Ce掺杂使Fe2+含量增加;与均相光催化剂相比,3DOM La0.4Ce0.6FeO3具有更广的pH适用范围、更低的铁泥产量及更高的双氧水利用率;重复使用5次后,3DOM La0.4Ce0.6FeO3对亚甲基蓝的降解效率维持在较高水平,表明催化剂稳定性较强;猝灭实验和ESR测试结果表明,亚甲基蓝的降解是在·OH和·O2-共同作用下完成的;结合XPS等分析结果提出了3DOM La0.4Ce0.6FeO3非均相光芬顿与光催化协同降解亚甲基蓝的机理.
工业生产过程中产生大量含有NaCl的高盐废水,易造成环境污染.探究了一种利用双极膜电渗析法从模拟NaCl废水中再生HCl和NaOH的工艺,在设定的实验条件下,分析NaCl初始浓度、电流密度等运行参数对酸、碱再生的影响.结果表明:NaCl溶液初始浓度过高,会导致膜堆电流过高,为保护膜堆,建议选择初始浓度相对较低的NaCl溶液;此外,对双极膜电渗析膜堆施加高电流强度可以缩短实验的运行时间.同时探索了使用高电通量运行双极膜电渗析装置的工程可行性,可为处理工业生产中的含氯废水提供参考.
The recyclable polyvinyl alcohol/strontium titanate/silver oxide (PVA/SrTiO3/Ag2O) composite with photocatalytic performance is successfully synthesized using the co-precipitation and sol–gel methods. The composition, morphology and optical properties on the composites are analyzed with the X-ray diffraction, scanning electron microscopy, transmission electron microscopy, energy-dispersive X-ray spectroscopy, X-ray photoelectron spectroscopy, ultraviolet–visible spectrophotometry, fluorescence spectrophotometry and electron paramagnetic resonance. The photocatalytic degradation efficiency of PVA/SrTiO3/Ag2O composite to 20 ppm methylene blue (MB) under UV light reaches 88%. The effects of the initial MB concentration and pH on the photocatalytic performance are analyzed. The recyclability of catalyst is evaluated.