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Water · 2022 ·Vol. 14 ·期 7 ·1044 · IF 3.53

Construction of Novel Electro-Fenton Systems by Magnetically Decorating Zero-Valent Iron onto RuO2-IrO2/Ti Electrode for Highly Efficient Pharmaceutical Wastewater Treatment

Miao Deng,Keming Wu,Tao Yang,Deyou Yu,Gaojie Liu,Shuai Gong,Dongni Sun,Michal Petru

The Electro-Fenton (E-Fenton) technique has shown great potential in wastewater treatment, while the sustainable and continuing supply of Fe2+remains challenging. Herein, we demonstrate the construction of a novel E-Fenton system by magnetically decorating zero-valent iron (ZVI) onto a RuO2-IrO2/Ti (ZVI-RuO2-IrO2/Ti) electrode for high-efficient treatment of pharmaceutical wastewater, which is considerably refractory and harmful to conventional biological processes. By using ZVI as a durable source of Fe(II) irons, 78.69% of COD and 76.40% of TOC may be rapidly removed by the developed ZVI-RuO2-IrO2/Ti electrode, while the ZVI-RuO2-IrO2/Ti electrode using ZVI only reduces 35.64% of COD under optimized conditions at initial COD and TOC values of 5500 mg/L and 4300 mg/L, respectively. Moreover, the increase in BOD5/COD from 0.21 to 0.52 highlights the enhanced biodegradability of the treated effluent. The analysis of a simultaneously formed precipitation on electrodes suggests that the coagulation process dominated by Fe3+/Fe2+also plays a non-negligible role in pharmaceutical wastewater treatment. In addition, the monitoring of the evolution of nitrogen elements and the formation of by-products in the E-Fenton process verifies its great capacity toward those organic pollutants found in pharmaceutical wastewater. Our study offers a practical solution for enhancing the performance of E-Fenton systems, and effectively treating refractory pharmaceutical wastewater.Keywords:electro-oxidation;zero-valent iron;pharmaceutical wastewater;E-Fenton process

研究领域: 环境科学 · 化学工程
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JOURNAL OF SOLID STATE CHEMISTRY · 2024 · IF 3.2

Efficient palladium ion adsorption and catalyst preparation from pharmaceutical wastewater using amino-functionalized Ti3C2

Dancheng Zhu,Yonghui Lin,Changhui Chen,Hao Xu,Jiabin Shen,Jun Qiao,Chao Shen

This paper reports the recovery and reuse of Pd ions from pharmaceutical wastewater using amino-modified Ti 3 C 2 . Ti 3 C 2 –NH 2 was synthesized by modifying (3-aminopropyl)triethoxysilane and the successful substitution of some surface functional groups of Ti 3 C 2 ; the decrease in material thickness was verified by characterization. This study revealed that the presence of amino groups significantly enhanced the Pd(II) adsorption capacity of Ti 3 C 2 . The effects of the adsorbent material, adsorbent dosage, pH, initial concentration of Pd ions, presence of competing cations, and contact time on the adsorption performance were investigated. The maximum adsorption capacity of 20 mg of Ti 3 C 2 –NH 2 was 986.65 mg/g in 100 ml of a Pd-ion solution with an initial concentration of 200 mg/l at pH 3. A pseudo-second-order kinetic model fitted well with the experimentally obtained rate data, indicating that the main mode of Pd-ion removal by Ti 3 C 2 –NH 2 was via chemical reduction. Finally, the catalyst exhibited excellent performances during the photocatalytic and Suzuki coupling reactions with yields of 81 % and 95 %, respectively. The results demonstrated that Ti 3 C 2 –NH 2 is an excellent material for adsorbing Pd ions and can effectively recycle these ions from pharmaceutical wastewater.

研究领域: 环境科学 · 材料科学 · 化学工程
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Environmental Science-Water Research & Technology · 2019 ·Vol. 5 ·期 4 ·672-683 · IF 4.195

Tertiary treatment of secondary effluent using ultrafiltration for wastewater reuse: correlating membrane fouling with rejection of effluent organic matter and hydrophobic pharmaceuticals

Fangshu Qu,Hao Wang,Junguo He,Gongduan Fan,Zhihui Pan,Jiayu Tian,Hongwei Rong,Guibai Li,Huarong Yu

Permeability loss and the low retention efficiency of soluble organics significantly restrict the application of ultrafiltration (UF) for water reclamation. In this work, the tertiary treatment of secondary effluent using UF was investigated under a variety of transmembrane pressures (TMPs) (20–150 kPa) to obtain more insight into fouling by effluent organic matter (EfOM) and its impact on organic rejection, particularly for hydrophobic pharmaceuticals represented by carbamazepine and naproxen. The flux decline and the reversible fouling during secondary effluent filtration were substantially aggravated with increasing TMP, whereas the irreversible fouling was generally reduced, as attributed to restriction of EfOM adhesion to the membrane surface by the fouling layer. The fouling process was successively dominated by pore blocking and cake layer filtration, and the shift in the dominant mechanism was accelerated under higher TMPs. The rejection of EfOM was improved in the presence of a fouling layer, which acted as a secondary filtration medium, particularly at higher TMPs. The maximum rejection of hydrophobic pharmaceuticals by UF was observed in a moderate TMP range (40–60 kPa), probably due to a trade-off between increased fouling layer retention and reduced rejection due to increased wall shear and aggravated cake-enhanced concentration polarization with increasing TMP. The results would encourage the strategy of utilizing the fouling layer for irreversible-fouling restriction and better rejection of hydrophobic PhACs.

CAS / MDL: 501-53-1
研究领域: 环境科学 · 水处理工程
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SEPARATION AND PURIFICATION TECHNOLOGY · 2021 · IF 7.312

High-hydrophilic and antifouling reverse osmosis membrane prepared based an unconventional radiation method for pharmaceutical plant effluent treatment

Chao Liu,Yongqiang Guo,Yi Zhou,Bo Yang,Ke Xiao,Hua-Zhang Zhao

Membrane fouling is the vulnerable point of polyamide (PA) reverse osmosis (RO) membranes in industrial wastewater treatment (especially pharmaceutical plant effluent). The deposition and adsorption of foulants on the PA layer greatly reduce the permeability selectivity of the membrane and increase maintenance costs. In this work, a simple irradiation strategy was used to graft hydrophilic polymers on the membrane surface without any catalysts and initiators, and an excellent hydrophilic and antifouling modified RO membrane was developed. The successful introduction of Poly(vinyl alcohol)   (PVA) onto RO membrane surface was confirmed through systematic surface characterization (13C NMR, ATR-FTIR, XPS, SEM, and AFM). The membrane M−2 with a PVA modifier concentration of 1.0% has   remarkable hydrophilic properties (water contact angle of 24.93°) and excellent separation efficiency (salt rejection up to 99.4%). The antifouling property of the modified membrane is significantly enhanced due to the synergistic effect of the hydrophilic component and the roughness. In the bovine serum albumin (BSA) antifouling tests, the irreversible flux decline rate (DRir) of membrane M−2 was as low as   1.7% and the flux recovery ratio (FRR) values increased from 87.6% to 98.3% compared to pristine membrane.   Importantly, the membrane modified with PVA shows a high foulant removal efficiency (COD > 99.5%) in the actual pharmaceutical plant effluent treatment, and the performance is stable after continuous operation for 28 days. The proposed simple co-grafting strategy also opens up new possibilities for the optimization or modification of other membranes (e.g., nanofiltration and ultrafiltration). Simultaneously, the prepared modified membrane has stable performance, simple and efficient method, and can also be applied in desalination and other industrial wastewater treatment fields.

研究领域: 环境科学 · 材料科学 · 化学工程
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APPLIED SURFACE SCIENCE · 2023 · IF 6.7

Highly efficient removal of salicylic acid from pharmaceutical wastewater using a flexible composite nanofiber membrane modified with UiO-66(Hf) MOFs

Jing Wang,Yakun Teng,Shushu Jia,Wenyan Li,Tianyi Yang,Ya Cheng,Hao Zhang,Xiang Li,Lijuan Li,Ce Wang

The successful development of a cost-effective and efficient adsorbent is crucial for the optimal treatment of pharmaceutical sewage. In this study, a UiO-66(Hf)–NH 2 nanocrystal modified composite nanofiber membrane (HfPNFM) was synthesized through electrospinning and solvothermal techniques, for the removal of salicylic acid (SA). The in-situ growth of UiO-66(Hf)–NH 2 on the nanofibers led to a significant increase in the specific surface area of the composite nanofiber membrane. Furthermore, HfPNFM demonstrated exceptional flexibility and reusability, with the removal efficiency of SA still at 96.85 % even after ten cycles. The adsorption process of SA onto HfPNFM was well described by the pseudo-second-order kinetic model and Langmuir isotherm model, with a maximum adsorption capacity of 128.21 mg/g. In dynamic adsorption experiments, HfPNFM effectively removed 100 % of SA at a concentration of 50 mg/L. The chemical oxygen demand (COD) concentration of SA was reduced from 165.89 mg/L to 41.47 mg/L by two layers of HfPNFM filtration, below the standard for pharmaceutical wastewater discharge (GB: 21904-2008). X-ray photoelectron spectroscopy (XPS) revealed that electrostatic interactions, π-π interactions, hydrogen bond interactions, and metal complexation interactions between SA and HfPNFM were responsible for the adsorption. This highly effective composite nanofiber membrane has promising potential for pharmaceutical wastewater treatment.

CAS / MDL: 10312-55-7 13499-05-3
研究领域: 环境科学 · 材料科学
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Efficient treatment of high-concentration pharmaceutical wastewater with high-salinity by chemical synthesis coupling with evaporation: From lab-scale to pilot-scale

Mushi Li,Xi Wang,Mingyu Ma,Juan Wu,Yang Chen,Jinbao Ou,Xinyue Chen,Qianying Zhou,Wenjing Sang,Shihong Xu,Li Cai,Dengxin Li

This study focused on the treatment of high-concentration pharmaceutical wastewater with high-salinity by pretreatment of chemical synthesis coupling with evaporation. Via chemical synthesis, this pretreatment process was developed to remove the organic matter that inhibited evaporation of wastewater, resulting in improved evaporation efficiency. Lab-scale results demonstrated that under the optimum conditions (∼pH 9, 2 mL/L demulsifier, 98 mM/L H 2 O 2 , 3 h of aeration time, 80 °C, 500 mg/L PAC, and 20 mg/L PAM), 54.9 % of COD was successfully removed by single pretreatment and 98.6 % after coupling with evaporation. Compared to the 80.1 % COD removal efficiency of direct evaporation of 100 mL with 30 min, the pretreatment process coupling with evaporation demonstrated superior performance and halved the evaporation time. A pilot-scale chemical synthesis pretreatment (120 t/d) was further developed to treat pharmaceutical wastewater of both high COD concentrations and high salinity. Under the optimal conditions determined in the lab-scale experiments, the pilot-scale achieved a COD removal efficiency of 49 % with a single pretreatment and 95.8 % after coupling with mechanical vapor recompression (MVR). Additionally, the obtained salt appeared visually clean and white compared to that obtained from the treated wastewater without pretreatment. Furthermore, to elucidate the possible mechanisms driving the efficient removal of COD, GC–MS was performed on the wastewater before and after pretreatment, and the resulting products from pretreatment in pilot-scale applications were further determined by both FTIR and GC–MS. It was proposed that the aldol condensation reaction increased the formation of carbon chains to macromolecular compounds might be the possible mechanism. This study gives insights into the future application of low-investment and low-cost technology in the treatment of high-concentration pharmaceutical wastewater with high salinity in industry.

研究领域: 环境工程 · 化工技术 · 废水处理
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SEPARATION AND PURIFICATION TECHNOLOGY · 2022 · IF 9.136

Hydrogen generation from photocatalytic treatment of wastewater containing pharmaceuticals and personal care products by Oxygen-doped crystalline carbon nitride

Yingfei Wang,Junhui Zhou,Fengliang Wang,Yi Xie,Shengwei Liu,Zhimin Ao,Chuanhao Li

Degrading organic pollutants while generating hydrogen from water splitting is an ideal application of photocatalysis. Herein, we presented an efficient photocatalyst, oxygen-doped crystalline carbon nitride, to power the degradation of various kinds of pharmaceuticals and personal care products and the simultaneous hydrogen production. The highest efficiency was achieved in treating the simulated wastewater containing naproxen (NPX), with the H 2 evolution rate of 819.1 µmol/g/h and the NPX degradation efficiency of 92 % upon visible light irradiation. Experimental and computational results suggested that the doped oxygen atoms thermodynamically favored the generation of hydroxyl peroxide for pollutant degradation and lowered the energy barrier of H 2 O reduction to produce hydrogen fuel. Most importantly, the catalysts functioned well in the natural aquatic environment including sea water, sewage water, river water, and well water. This study provides fundamental insights into photocatalytic water treatment with simultaneous hydrogen production, indicating an energy-recovering approach for wastewater treatment.

研究领域: 环境科学 · 材料科学 · 化学工程
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JOURNAL OF HAZARDOUS MATERIALS · 2021 · IF 10.588

Residual β-lactam antibiotics and ecotoxicity to Vibrio fischeri, Daphnia magna of pharmaceutical wastewater in the treatment process

Yaru Hu,Dandan Lei,Da Wu,Jing Xia,Wang Zhou,Changzheng Cui

The discharge of pharmaceutical wastewater introduces numerous pollutants into the environment, and their pollution level reduction has aroused extensive concern. This study investigated the variation in residual antibiotics and ecotoxicity to two nutritional-level model organisms in the pharmaceutical wastewater treatment process (PWTP). The wastewater in the equalization tank contained massive organic matters (2.9–18.7 times higher than the permissible values in GB21903-2008) and antibiotics (310.88 μg/L), posing extremely toxic effects to Vibrio fischeri ( V. fischeri ) and Daphnia magna ( D. magna ) . The biological anaerobic/aerobic treatment units contributed the most to the reduction of antibiotics and the ecotoxicity to both organisms, with the removal rates of 72% and > 90%, respectively. The ecotoxicity of pharmaceutical wastewater was strongly and positively correlated with the residual antibiotics, amoxicillin, cephalexin, ammonia nitrogen, and total phosphorus ( P  < 0.05). However, the detected amounts of amoxicillin and cephalexin were approximately 10 5 times lower than the predicted no-effect concentrations of amoxicillin and cephalexin to V. fischeri and D. magna in freshwater, which implied the joint ecotoxicity posed by multicomponent mixtures, such as the residual antibiotics and organic toxic substances, rather than the specific residual antibiotics. This study provides a better understanding of the variations and residual levels of pollutants in PWTPs , including their ecotoxicity risk to the aquatic environment, highlighting the need to optimize pharmaceutical wastewater treatment technologies .

CAS / MDL: 75-05-8 67-56-1
研究领域: 环境科学 · 毒理学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2024 · IF 8.1

Stability optimization of iron-based catalysts: Application of Cr-enriched alloy steel catalyst in ozonation pharmaceutical wastewater

Siqi Xiao,Luming Ma,Wenhui An,Pengfei Shen

Catalytic ozonation for advanced treatment of industrial wastewater has proved to be effective, and the stability of the catalyst is crucial for the long-term application of the ozonation process in practical engineering. In this study, the electrochemical characteristics of four iron (Fe) shavings: alloy steels (38CrMoAl and 40Cr) and carbon steels (A3 and 45#) were investigated, and a new citric acid-optimized H 2 O 2 modification method was proposed. The low open circuit potential (OCP) of carbon steels indicated that they were more likely to be oxidized therefore required shorter modification times. The higher the OCP of alloy steels, the higher H 2 O 2 concentration was required to enhance modification efficiency. By adding citric acid, the rapid modification of alloy steel was achieved, and the catalysts exhibited lower passivation current (I p ), indicating a lower rate of substrate loss and a longer lifetime of alloy steel catalysts. Furthermore, chromium (Cr) enrichment occurred in the oxide layer of alloy steel catalysts. The Cr/Fe (atomic ratio) in oxide layer for 38CrMoAl and 40Cr increased from 0.018 to 0.040 and from 0.010 to 0.037, respectively. The presence of CrOOH and Cr 2 O 3 within the oxide layer reinforced the layer’s overall structural integrity and enhanced its protection for the internal substrate, making the catalysts more resistant to adapt to high-salinity wastewater. Through laboratory tests, it was found that among the four catalysts, 38CrMoAl showed the highest stability and good catalytic activity with low Fe loss concentration. Therefore, the pilot-scale application effect of 38CrMoAl catalyst was evaluated. In the advanced treatment of pharmaceutical wastewater, chemical oxygen demand (COD) and total organic carbon (TOC) removals were 56.3% and 32.4%, respectively. These results showed that the stability of catalyst can be improved by optimizing the selection of steel, and the introduction of citric acid achieved Cr enrichment effect and amplified the potential stability advantage of alloy steel. The research provides guidance on raw material selection for catalyst preparation to different industries' wastewater treatment, especially in high-salinity wastewater ozonation treatment, which can realize the long-term stable application of catalyst.

研究领域: 环境科学 · 材料科学
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CHEMICAL ENGINEERING JOURNAL · 2018 · IF 6.735

Direct Z-scheme 2D/2D MnIn2S4/g-C3N4 architectures with highly efficient photocatalytic activities towards treatment of pharmaceutical wastewater and hydrogen evolution

Wei Chen,Zhi-Cai He,Guo-Bo Huang,Cheng-Lin Wu,Wu-Fei Chen,Xiao-Heng Liu

Semiconductor photocatalysis has been regarded as an environmentally friendly technology in wastewater treatment and energy production. Here, a series of direct Z-scheme MnIn 2 S 4 /g-C 3 N 4 (MnISCN) photocatalysts without electron mediators were fabricated by a simple hydrothermal route on the basis of in-situ loading of MnIn 2 S 4 (MnIS) nanoflakes on the surface of g-C 3 N 4 (CN) nanosheets. Photocatalytic performances evaluated under visible light irradiation revealed these Z-scheme heterostructured photocatalysts exhibited higher photocatalytic activities than single-component samples. The effect of weight ratio between MnIn 2 S 4 nanoflakes and mesoporous CN nanosheets on photocatalytic activity towards treatment of pharmaceutical wastewater was optimized to achieve highly efficient photocatalytic activities for both degradation of pharmaceutical wastewater and hydrogen generation compared with alone MnIS nanoflakes and isolated mesoporous CN nanosheets. The significant enhancement in photocatalytic activity could be primarily ascribed to the construction of Z-scheme MnISCN architectures, which effectively accelerated the transfer and separation of photogenerated charge carriers via tight interface contacts built among these two components. The recycling experiments for pharmaceutical wastewater treatment revealed the excellent stability of MnISCN nanocomposites. The advantages of highly efficient photocatalytic activity and excellent stability endowed a promising potential for MnISCN nanocomposites to apply in photocatalytic fields.

研究领域: 材料科学 · 环境科学 · 能源科学
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JOURNAL OF HAZARDOUS MATERIALS · 2017 · IF 6.065

One-step in situ hydrothermal fabrication of octahedral CdS/SnIn4S8 nano-heterojunction for highly efficient photocatalytic treatment of nitrophenol and real pharmaceutical wastewater

Fang Deng,Fei Zhong,Lina Zhao,Xubiao Luo,Shenglian Luo,Dionysios D. Dionysiou

Octahedral CdS/SnIn 4 S 8 nano-heterojunctions were fabricated by a facile and simple one-step in situ hydrothermal method, and the molar ratio of CdS to SnIn 4 S 8 was optimized. The optimal (0.5:1)CdS/SnIn 4 S 8 heterojunctions exhibit the highest visible-light photocatalytic activity with 97.1% degradation efficiency of 2-nitrophenol in 120   min, which is much higher than those of individual CdS and SnIn 4 S 8 . The enhanced photocatalytic performance could be attributed to the effective separation and transfer of photogenerated charges originating from the well-matched band gap structures. Of special significance is that (0.5:1)CdS/SnIn 4 S 8 can effectively mineralize 2-nitrophenol and real pharmaceutical wastewater. Moreover, CdS/SnIn 4 S 8 nano-heterojunctions show excellent reusability in five cycles due to the stable surface composition and chemical valence state.

CAS / MDL: 88-75-5
研究领域: 材料科学 · 环境科学
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BMC Research Notes · 2025 ·Vol. 18 ·期 1 ·1-11 · IF 1.7

Preparation of geopolymer membranes using clay and some industrial wastes to remove the organic load of pharmaceutical wastewater

Hammal Abdulrazzaq

The importance of geopolymeric materials has increased in recent years due to their high effectiveness in water treatment by multiple techniques such as adsorption and filtration. Therefore, research has increased related to the preparation of geopolymers from different raw materials. In this research geopolymeric membranes were prepared from Syrian clay by calcinted it at 600˚C for 120 min, then it was mixed with an activated alkaline solution (NaOH + Na 2 SiO 3 : SiO 2 /Na 2 O = 1.3). The effect of adding quantities of chamotte waste, ceramics waste, and glass waste on the properties of the geopolymeric membrane was studied. The porosity decreased significantly due to waste additions, the decrease in porosity led to a decrease in water flow, while the compressive strength of the membranes increased with the effect of waste addition. The prepared membranes were used to remove organic pollutants from pharmaceutical wastewater in two stages, the first stage was absorbed by the prepared membrane powder, and the second stage was filtration by the prepared membrane. The tests showed good efficiency in removing organic pollutants, and the results of the bacteriological tests indicated good effectiveness of the prepared membranes in removing bacterial contamination from the treated water sample. Graphical

研究领域: 材料科学 · 环境工程 · 水处理技术
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