Search Results (15)

With the increasing detection of antibiotics such as sulfamethoxazole (SMX) in water bodies, developing efficient and eco-friendly treatment technologies is critical. This study employs a hydrothermal impregnation method to prepare a NiFe₂O₄/granular activated carbon (GAC) composite catalyst, optimized for use in a proton exchange membrane (PEM) electrolytic ozonation system to degrade SMX. Single-factor experiments optimized preparation conditions with a Fe:Ni molar ratio of 3:1, a GAC:Fe + Ni mass ratio of 2:1, and calcination at 500 °C for 3 h. The catalyst was characterized using XRD, SEM, TEM, XPS, and FT-IR, confirming a spinel NiFe₂O₄ structure (crystal size ~15.2 nm) uniformly dispersed on GAC, with an Fe:Ni atomic ratio of ~2.1:1. In the PEM system, the optimized catalyst achieved a 99.15% ± 0.3% SMX degradation rate (50 mg/L) within 25 min, compared to 95.06% ± 0.6% in 30 min without a catalyst. The catalyst maintained 98.45% ± 0.5% efficiency after three cycles, demonstrating excellent stability. The synergy between GAC adsorption and NiFe₂O₄ catalysis, driven by Fe³⁺/Fe²⁺ redox cycling, enhances ·OH generation from ozone decomposition, boosting SMX degradation. This work provides a robust catalyst for antibiotic wastewater treatment and a foundation for scaling up catalytic ozonation. Full article

As a highly energy-intensive and carbon-emitting industry with significant emissions of volatile organic compounds (VOCs), the petroleum and chemical industry is a major contributor to the global greenhouse effect and ozone layer destruction. Improper treatment of petrochemical waste gas (PWG) seriously harms human health and the natural environment. This study uses CiteSpace and VOSviewer to conduct a scientometric analysis of 1384 scholarly works on PWG and carbon sequestration published between 1981 and 2022, revealing the basic characteristics, knowledge base, research topic evolution, and research hotspots of the field. The results show the following: (1) In the early stages of the petrochemical industry, it was processed tail gas, plant leakage waste gas, and combustion flue gas that were investigated in PWG research. (2) Later, green environmental protection technology was widely studied in the field of PWG treatment, such as biotechnology, catalytic oxidation technology, membrane separation technology, etc., in order to achieve efficient, low energy consumption and low emissions of waste gas treatment, and the number of publications related to this topic has increased rapidly. In addition, researchers studied the internet of things and technology integration, such as the introduction of artificial intelligence, big data analysis, and other technologies, to improve the accuracy and efficiency of exhaust gas monitoring, control, and management. (3) The department has focused on how to reduce emissions by optimizing petrochemical process lines or improving energy efficiency. Emission reduction and low-carbon transition in the petrochemical industry will become the main trend in the future. Switching from renewable carbon to feedstock carbon derived from captured carbon dioxide, biomass, or recycled chemicals has become an attractive strategy to help curb emissions from the chemical industry. The results of our analysis can provide funding agencies and research groups with information to better understand the global trends and directions that have emerged in this field from 1981 to 2022 and serve as a reference for future research. Full article

The removal of persistent organic micropollutants (OMPs) from secondary effluent in wastewater treatment plants is critical for meeting water reuse standards. Traditional treatment methods often fail to adequately degrade these contaminants. This study explored the efficacy of a hybrid ozonation membrane filtration (HOMF) process using CeO₂ and CeTiO_x-doped ceramic crossflow ultrafiltration ceramic membranes for the degradation of OMPs. Hollow ceramic membranes (CM) with a 300 kDa molecular weight cut-off (MWCO) were modified to serve as substrates for catalytic nanosized metal oxides in a crossflow and inside-out operational configuration. Three types of depositions were tested: a single layer of CeO₂, a single layer of CeTiO_x, and a combined layer of CeO₂ + CeTiO_x. These catalytic nanoparticles were distributed uniformly using a solution-based method supported by vacuum infiltration to ensure high-throughput deposition. The results demonstrated successful infiltration of the metal oxides, although the yield permeability and transmembrane flow varied, following this order: pristine > CeTiO_x > CeO₂ > CeO₂ + CeTiO_x. Four OMPs were examined: two easily degraded by ozone (carbamazepine and diclofenac) and two recalcitrant (ibuprofen and pCBA). The highest OMP degradation was observed in demineralized water, particularly with the CeO₂ + CeTiO_x modification, suggesting O₃ decomposition to hydroxyl radicals. The increased resistance in the modified membranes contributed to the adsorption phenomena. The degradation efficiency decreased in secondary effluent due to competition with the organic and inorganic load, highlighting the challenges in complex water matrices. Full article

The present study evaluates the application of heterogeneous catalytic ozonation for the removal of micropollutants from wastewater effluent in a pre-industrial-scale unit, consisting of a post-filtration, an ozone dilution, a catalytic ozonation, and a final biological stabilization step. The important step of ozone dilution is optimized by the use of a hollow fiber membrane that minimizes the loss of ozone gas due to the transfer of ozone to the liquid phase mainly by diffusion. It is observed that the efficiency of this sub-system is maximized for the dead-end operation of the membrane and the introduction of ozone gas to the shell side and liquid phase to the lumen side of the membrane module. Under these conditions, the concentration of dissolved ozone is directly dependent on the ratio of ozone gas feed to the wastewater flow subjected to post-treatment. Regarding the removal of MPs, part of their degradation already takes place at this stage (i.e., during ozone dilution), while after the post-treatment of wastewater effluent in the catalytic ozonation bed, the MP degradation yield ranges from 35% up to complete removal, depending on the type and properties of the specific MP. The addition of a final biological filtration bed to the overall treatment unit significantly increased its performance, regarding the removal of MPs, enhancing it by an additional removal rate that can reach up to 30%. Full article

In the treatment of drinking water, the ibuprofen (IBP) disinfection by-products, toxicity, and its impact on drinking water safety have caused widespread attention in domestic and overseas research areas. We studied the removal efficiency of IBP under the following conditions: combination of good catalytic activity of a silicate-based microfiltration membrane with the strong oxidizing ability of ozone in the continuous flow experiment mode and various influencing factors. This research revealed that with the increase of pH and hydraulic retention time, the removal efficiency of IBP exhibited an increasing trend; with the increase of alkalinity and humic acid concentration in water, the removal efficiency of IBP was obviously inhibited. Free radical inhibitors and electron spin resonance (ESR) analysis demonstrated that hydroxyl radical (∙OH) is an important active species during the reaction of ozone-catalyzed IBP with the silicate-based microfiltration membrane. Full article

The present study evaluates the removal of micropollutants from water/wastewater contaminated sources through the application of a heterogeneous catalytic ozonation process, using a pilot-scale continuous operation unit, composed of a membrane module for the diffusion and effective dilution of ozone into the liquid phase to be treated and a plug flow reactor/continuous stirred tank reactor (PFR/CSTR) contact reactor system in series, where the catalyst is recirculated in dispersion mode. The solid materials tested as catalysts are natural and calcined zeolite, Bayoxide and alumina, whereas the examined micropollutants, used in this case as probe compounds, are p-chlorobenzoic acid (p-CBA), atrazine, benzotriazole and carbamazepine. A high-performance liquid chromatography system was used to determine the removal of micropollutants. In the case of p-CBA, an ozone-resistant compound, the addition of catalyst was found to significantly enhance its degradation rate, leading to >99% removal under the optimum defined conditions, i.e., in terms of catalyst concentration, pH, temperature, and process time. On the other hand, in the case of atrazine, a different ozone-resistant compound, the introduction of examined catalysts in the ozonation process was found to reduce the degradation of micropollutant, when compared with the application of single ozonation, indicating the importance of specific affinity between the pollutant and the solid material used as catalyst. Benzotriazole, a moderately ozone-reactive compound was degraded by more than 95% under all experimental conditions and catalysts tested in the pilot unit, while carbamazepine, a highly ozone-reactive compound, was completely removed even during the first stage of treatment process (i.e., at the membrane contactor). When increasing the pH value (in the range 6–8) and the contact time, the performance of catalytic ozonation process also improved. Full article

With the continuous expansion of industrial enterprises, a large amount of high-salt wastewater with complex components is produced. Direct discharge will cause great harm to the ecosystem and waste a large amount of potential salt resources. This paper summarizes the source, water quality characteristics, and environmental impact of high-salinity wastewater, and introduces the desalination and treatment technologies of high-salinity wastewater. The desalination technology of high-salinity wastewater mainly includes two processes: concentration and crystallization, obtaining concentrated solution through membrane concentration or thermal concentration and then carrying out crystallization treatment on the concentrated solution, thereby realizing the recovery of salt. The advanced treatment technologies of high-salinity wastewater were analyzed, including physicochemical treatment, biological treatment, and coupling treatment. Catalytic ozonation is one of the most widely used physicochemical technologies for the advanced treatment of high-salinity wastewater. Biological treatment processes operating in the presence of halotolerant bacteria show excellent performance at high salinity. High salinity has a negative impact on the performance of various physicochemical processes and biological treatment technologies. However, high salinity has little effect on the performance of a coupled system designed to treat high-salinity wastewater. In this review, the effect of salinity on the scaling and corrosion of equipment is also illustrated. It is suggested that the research direction of high-salinity wastewater should be to develop new membrane materials and catalysts, develop salt-tolerant microorganisms, explore high-efficiency and energy-saving physico–chemical–biochemical combination processes, improve the treatment efficiency of high-salinity organic wastewater, and reduce treatment costs. Full article

In order to efficiently remove NOMs in natural surface water and alleviate membrane pollution at the same time, a flat microfiltration ceramic membrane (CM) was modified with MnFeO_X (Mn-Fe-CM), and a coagulation–precipitation–sand filtration pretreatment coupled with an in situ ozonation-ceramic membrane filtration system (Pretreatment/O₃/Mn-Fe-CM) was constructed for this study. The results show that the removal rates of dissolved organic carbon (DOC), specific ultraviolet absorption (SUVA) and NH₄⁺-N by the Pretreatment/O₃/Mn-Fe-CM system were 51.1%, 67.9% and 65.71%, respectively. Macromolecular organic compounds such as aromatic proteins and soluble microbial products (SMPs) were also effectively removed. The working time of the membrane was about twice that in the Pretreatment/CM system without the in situ ozone oxidation, which was measured by the change in transmembrane pressure, proving that membrane fouling was significantly reduced. Finally, based on the SEM, AFM and other characterization results, it was concluded that the main mitigation mechanisms of membrane fouling in the Pretreatment/O₃/Mn-Fe-CM system was as follows: (1) pretreatment could remove part of DOC and SUVA to reduce their subsequent entrapment on a membrane surface; (2) a certain amount of shear force generated by O₃ aeration can reduce the adhesion of pollutants; (3) the loaded MnFeO_X with a higher catalytic ability produced a smoother active layer on the surface of the ceramic membrane, which was conducive in reducing the contact among Mn-Fe-CM, O₃ and pollutants, thus increasing the proportion of reversible pollution and further reducing the adhesion of pollutants; (4) Mn-Fe-CM catalyzed O₃ to produce ·OH to degrade the pollutants adsorbed on the membrane surface into smaller molecular organic matter, which enabled them pass through the membrane pores, reducing their accumulation on the membrane surface. Full article

The mature landfill leachate (MLL) is characterized by a large number of fulvic acids and humic acids, which is refractory organic matter and can be cleaned by ozone oxidation. However, the poor property of mass transfer prohibits the widespread use of ozone oxidation in actual leachate treatment. Meanwhile, some combined processes are adopted to treat the mature landfill leachate, which places catalytic ozonation before the membrane bioreactor (MBR) process to enhance the biodegradability of MLL. Thus, this research is conducted to investigate the practicability of applying nano-Fe₃O₄ loaded cow-dung ash (Fe₃O₄@CDA) and biological post-treatment with MBR for the effective removal of pollutants from MLL and puts forward the variation of organics in leachate between catalytic ozonation and MBR. The addition of catalytic ozonation not only improved the removal of hazardous organics but also enhanced the biodegradability of the leachate and favored the subsequent MBR process. Chemical oxygen demand (COD) removal in the catalytic ozonation step was optimized, and 53% removal was obtained at pH = 7, catalyst dosage = 1.0 g/L, and O₃ dosage = 3.0 g/L. After the MBR process, COD in effluent stabilized in the range of 57.85–65.38 mg/L, and the variation range of the ammonia nitrogen (NH₃-N) concentration was 5.98–10.24 mg/L. The catalytic ozonation-MBR integrated process showed strong feasibility in dealing with the biologically pre-treated leachate. Full article

Over the years, the persistent occurrence of superfluous endocrine-disrupting compounds (EDCs) (sub µg L⁻¹) in water has led to serious health disorders in human and aquatic lives, as well as undermined the water quality. At present, there are no generally accepted regulatory discharge limits for the EDCs to avert their possible negative impacts. Moreover, the conventional treatment processes have reportedly failed to remove the persistent EDC pollutants, and this has led researchers to develop alternative treatment methods. Comprehensive information on the recent advances in the existing novel treatment processes and their peculiar limitations is still lacking. In this regard, the various treatment methods for the removal of EDCs are critically studied and reported in this paper. Initially, the occurrences of the EDCs and their attributed effects on humans, aquatic life, and wildlife are systematically reviewed, as well as the applied treatments. The most noticeable advances in the treatment methods include adsorption, catalytic degradation, ozonation, membrane separation, and advanced oxidation processes (AOP), as well as hybrid processes. The recent advances in the treatment technologies available for the elimination of EDCs from various water resources alongside with their associated drawbacks are discussed critically. Besides, the application of hybrid adsorption–membrane treatment using several novel nano-precursors is carefully reviewed. The operating factors influencing the EDCs’ remediations via adsorption is also briefly examined. Interestingly, research findings have indicated that some of the contemporary techniques could achieve more than 99% EDCs removal. Full article

In this study, powdered activated carbon (PAC) was added to replace the silica in a cementitious microfiltration membrane (CM) to solve the problems of the low mechanical strength and short lifetime of CMs. The carbon-cementitious microfiltration membrane (CCM) was fabricated by the dry pressing method and cured at room temperature. The bending strength of CCM was 12.69 MPa, which was about three times more than that of CM. The average pore size was 0.129 μm, and was reduced by about 80% compared to that of CM. The addition of PAC did not reduce the degradation efficiency of membrane catalytic ozonation. Because of the strong alkaline buffering ability of CCM, the CCM–ozone coupling process could eliminate the effect of the pH value of the solution. The strong alkaline environment inside the membrane pores effectively accelerated the ozone decomposition and produced oxidizing radicals, which accelerated the reaction rate and improved the utilization rate of ozone. The CCM–catalytic ozonation reaction of organic compounds occurred within the pores and membrane surface, resulting in the pH of the solution belonging to the neutral range. The addition of PAC accelerated the mass transfer and made the pollutants and oxidant react in the membrane pores and on the membrane surface. The reuse experiments of the CCM–ozone coupling process for removing nitrobenzene demonstrated that CCM has good catalytic activity and reuse stability. It broadens the application scope of CCM in the field of drinking water and provides theoretical support for the practical application of CCM. Full article

In this study, a low-cost cementitious microfiltration membrane (CM) with a catalytic ozone oxidation function for the removal of organic pollutants was fabricated by using cementitious and C-10 μm silica powders at a certain silica–cementitious particle ratio (s/c). The effect of the s/c on the pore size distribution and mechanical strength of the membrane was investigated. The membrane pore size showed a bimodal distribution, and the higher the s/c, the closer the second peak was to the accumulated average particle size of silica. The increase in the s/c led to a decrease in the bending strength of the membrane. The cross-sectional morphology by SEM and crystal structure by XRD of CMs confirmed that a calcium silicate hydrate gel was generated around the silica powder to improve the mechanical strength of the CM. Considering the bending strength and pore size distribution of CMs, s/c = 0.5 was selected as the optimal membrane fabrication condition. The FT-IR results characterizing the surface functional groups of CMs were rich in surface hydroxyl groups with the ability to catalyze ozone oxidation for organic pollutant removal. Six small molecule organic pollutants were selected as model compounds for the efficiency experiments via a CM–ozone coupling process to prove the catalytic property of the CM. The CM has an alkaline buffering effect and can stabilize the initial pH of the solution in the catalytic ozonation process. The reuse experiments of the CM–ozone coupling process demonstrated the broad spectrum of the CM catalytic performance and self-cleaning properties. The results of this study provide the basis and experimental support to expand the practical application of CMs. Full article

Catalytic membrane ozonation is a hybrid process that combines membrane filtration and catalytic ozonation. The membrane deposited with an appropriate solid material acts as catalyst. As a consequence, the catalytic membrane contactor can act simultaneously as contactor (i.e., improving the transfer/dissolution of gaseous ozone into the liquid phase), as well as reactor (i.e., oxidizing the organic compounds). It can be used in water and wastewater treatment limiting the disadvantages of membrane filtration (i.e., lower removal rates of emerging contaminants or fouling occurrence) and ozonation (i.e., selective oxidation, low mineralization rates, or bromate (BrO₃⁻) formation). The catalytic membrane ozonation process can enhance the removal of micropollutants and bacteria, inhibit or decrease the BrO₃⁻ formation and additionally, restrict the membrane fouling (i.e., the major/common problem of membranes’ use). Nevertheless, the higher operational cost is the main drawback of these processes. Full article

Membrane filtration has been widely used in water and wastewater treatment. However, this process is not very effective for the removal of refractory organic compounds (e.g., of pharmaceutical origin). Coupling membrane filtration with ozonation (or other Advanced Oxidation Methods) can enhance the degradation of these compounds and, subsequently, the incidence of membrane fouling (i.e., the major problem of membrane uses) would be also limited. Ozonation is an efficient oxidative process, although ozone is considered to be a rather selective oxidant agent and sometimes it presents quite low mineralization rates. An improvement of this advanced oxidation process is catalytic ozonation, which can decrease the by-product formation via the acceleration of hydroxyl radicals production. The hydroxyl radicals are unselective oxidative species, presenting high reaction constants with organic compounds. An efficient way to couple membrane filtration with catalytic ozonation is the deposition of an appropriate solid catalyst onto the membrane surface. However, it must be noted that only metal oxides have been used as catalysts in this process, while the membrane material can be of either polymeric or ceramic origin. The relevant studies regarding the application of polymeric membranes are rather scarce, because only a few polymeric materials can be ozone-resistant and the deposition of metal oxides on their surface presents several difficulties (e.g., affinity etc.). The respective literature about catalytic membrane ozonation is quite limited; however, some studies have been performed concerning membrane fouling and the degradation of micropollutants, which will be presented in this review. From the relevant results it seems that this hybrid process can be an efficient technology both for the reduction of fouling occurrence as well as of enhancement of micropollutant removal, when compared to the application of single filtration or ozonation. Full article

The present study evaluates micropollutant degradation from water by catalytic ozonation in a pilot scale unit comprising of a hydrophobic membrane for ozone dilution and a column filled with granules of the catalyst. The catalysts examined are alumina, calcite, dolomite, goethite, pearlite, polyethylene terephthalate (PET) and zeolite. Experimental results revealed zeolite as the most effective material achieving complete degradation of benzotriazole and carbamazepine, as well as 70% degradation of atrazine and about 50% of p-chlorobenzoic acid (p-CBA). The rest of the catalysts tested presented a moderate performance in micropollutant removal, reaching 30%–50% for atrazine, 25%–35% for p-CBA, more than 90% for benzotriazole and complete degradation of carbamazepine. Adsorption capacity of all materials examined did not exceed 5%. Full article