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Highly Efficient Removal of Cr(Vi) from Electroplating Wastewater by Ferrous/Ferric Hydroxide Complexes: From laboratory to Pilot-Scale Study

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SSRN 2022年

作者： Lin, Xiaoqing Xu, Longqian Zhao, Zhenyu Liu, Shanshan Zhang, Jiaming Wu, Deli State Key Laboratory of Pollution Control and Resources Reuse College of Environmental Science & Engineering Tongji University Shanghai200092 China Shanghai Institute of Pollution Control and Ecological Security Shanghai200092 China

Low electron transfer efficiency and cumbersome processes are widely known to negatively affect the application of iron-based materials in the treatment of electroplating wastewater. In this study, ferrous/ferric hydroxide complex (FHC) was successfully synthesized to greatly improve the efficiency of electron transfer for Cr(VI) removal;meanwhile, the effect of the anionic interlayer and the possible removal mechanism were well investigated. We revealed that sulfate interlayer can greatly promote Cr(VI) removal of FHC by 10.4% and 29.0% compared to chloride interlayer and carbonate interlayer, respectively. It was innovatively discovered that the inhibitory of complexing agents (in the order of EDTA > CA > NTA > TA > OA) was closely associated with the amount of -OH and/or -COOH. In comparison to dissolved Fe(II), almost no effect of the initial pH value was found due to the buffering effect of the surface -OH. These results were different from some previously reported Cr(VI) removal of Fe(II)-containing minerals. Based on the characterization and batch experiments, the electrostatic attraction of surface -OH to Cr(VI), accompanied by simultaneous reduction by surface structural Fe(II), was responsible for the rapid reaction within the first 2 min and then co-precipitation to the formation of CrOOH and FeCr 2 O 4 . The chemical cost (1.12 $ m -3 ) and the sludge yield (29.14 kg m -3 ) were reduced by 71.3% and 54.1%, respectively, in the pilot-scale experiments using the FHC process compared to the NaHSO 3 process. These findings provided new insight for utilizing the anionic interlayer to improve the activity of FHC to remediate Cr(VI)-containing electroplating wastewater. © 2022, The Authors. All rights reserved.

关键词： Iron compounds

Enhancing the Separation Performance of the Resulting Pa-Tfc Nanofiltration Membrane by Modulating Interfacial Polymerization with Nanobubbles: Regulation Technology and Mechanism

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SSRN 2022年

作者： Bai, Chengling Li, Ping Gao, Xuerui Li, Pan Gu, Zhengyang Yu, Shuili State Key Laboratory of Pollution Control and Resources Reuse College of Environmental Science and Engineering Tongji University Shanghai200092 China Shanghai Institute of Pollution Control and Ecological Security Shanghai200092 China

Due to the low flux and unsatisfactory selective separation performance, the wider application of the nanofiltration membranes in reclamation of wastewater is limited. Therefore, breaking through the permeation-selectivity trade-off of polyamide thin film composite (PA-TFC) nanofiltration membranes remains a challenging problem. Herein, a strategy for preparing PA TFC NF membranes with enhanced performance by using nanobubbles (NBs) to control PIP moleculars diffusion is first introduced. The negatively charged NBs are confined to the aqueous phase side after the initial nanofilm is formed, which reduces the further diffusion of PIP monomers to the reaction zone by electrostatic interaction;thus, then smoother, thinner, and looser PA layers, with enhanced permeabilities, are formed. The restricted diffusion of PIP monomers also makes more acyl chloride groups, which can be hydrolyzed into carboxyl groups, being left in the PA layer. Therefore, an enhanced negatively charged surface is achieved, which endows the membrane with a higher separation potential. Compared with the control PA-TFC membranes, the NB3-PA-TFC membrane increases the rejection rate of Na 2 SO 4 from 91.67% to 97.78%, the pure water flux from 16.6 L·m 2 ·h -1 ·bar -1 to 24.0 L·m 2 ·h -1 ·bar -1 , and the Cl - /SO 4 2- selective separation factor ( S ) from 35.17 to 135.58. This study develops a novel type of well-behaved NF membranes, which are suitable to be produced in industry, and it extends the application scope of nanobubble technology. © 2022, The Authors. All rights reserved.

关键词： Monomers

New Sight into the Enhanced Ozonation of Malodorous Compounds by Cu(Ii): Inhibiting the Formation of Free Radicals to Promote Ozone Utilization

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SSRN 2022年

作者： Lin, Xiaoqing Ma, Canming Wu, Deli State Key Laboratory of Pollution Control and Resources Reuse College of Environmental Science & Engineering Tongji University Shanghai200092 China Shanghai Institute of Pollution Control and Ecological Security Shanghai200092 China

Metal-enhanced ozonation can greatly improve the decay of organic matter;however, whether this method benefits the decay of malodorous compounds or not and the possible mechanism are not well understood. In this study, nine typical malodorous compounds were selected to reveal that Cu(II)-enhanced ozonation can greatly promote the decay of fatty amines because of the direct ozone oxidation, which was enhanced to promote ozone utilization. Moreover, trace Cu(II) can amplify the observed rate constants of dimethylamine and trimethylamine for 48.9% and 155.7%, respectively and Cu(II) dosage was the determining factor using response surface methodology to investigate the interactions between initial pH, Cu(II) dosage and ozone dosage. These results demonstrated that the formation of •OH and O2•– was inhibited rather than promoted, which was quite different from some previously reported Cu(II)-enhanced ozonation counterparts. Moreover, the enhanced effect of trace Cu(II) was exhibited in both single and complex malodorous compounds. The conversion pathway of nitrogen and sulfur elements was clarified, with the targeted mineralization of nitrogen of nitrogen-containing malodorous compounds into NO3-N and the odor characteristics of sulfur-containing malodorous compounds disappeared. These findings provided new insight for utilizing metal ions to enhance the direct ozone oxidation capacity of malodorous compounds. © 2022, The Authors. All rights reserved.

关键词： Ozone

Efficient Decomposition of Pfos by Hydrated Electrons: Performance, Mechanism and Carbon Emission Reduction

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SSRN 2022年

作者： Chu, Liquan Zhang, Chaojie Chen, Pei Zhou, Qi Zhou, Xuefei Zhang, Yalie State Key Laboratory of Pollution Control and Resources Reuse College of Environmental Science and Engineering Tongji University Shanghai200092 China Shanghai Institute of Pollution Control and Ecological Security Shanghai200092 China

Perfluorooctane sulfonate (PFOS) is a typical perfluorinated compound, and the presence of sulfonic groups makes it more difficult to decompose. In this study, ultraviolet photolysis of iodide (UV/KI) was conducted to generate hydrated electrons for PFOS decomposition, the key factors affecting the decomposition efficiency were investigated and the possible decomposition pathways were speculated. The results implied that the UV/KI system can effectively promote the decomposition and defluorination of PFOS. When the PFOS and KI concentrations were 0.03 mmol L-1 and 0.3 mmol L-1, the decomposition and defluorination efficiency of PFOS at pH 10 reached 99.5% and 94.8% after 12 hours of reaction, respectively. With the increase of KI concentration from 0.1 to 0.5 mmol L-1, the decomposition and defluorination efficiency of PFOS increased, but a further increase of KI will lead to a decrease in the performance. Weak and strong alkaline conditions were more favorable for PFOS decomposition than acid conditions. Compared with UV/Sulfite system, this system can be conducted under a lower concentration of hydrated electron source chemicals and a wider range of pH. Kinetic analysis implied that PFOS decomposition followed the pseudo-first-order model with a reaction rate constant of 1.004 h-1, which was higher than most PFOS decomposition processes. Intermediates analysis and mass balance indicated there were three decomposition pathways of PFOS: desulfonation, H/F exchange and C-C bond dissociation. The main products were harmless fluorine ions, formic acid and acetic acid, which suggested that the UV/KI system for PFOS decomposition is a relatively mild and green process. © 2022, The Authors. All rights reserved.

关键词： Rate constants

Coordination-Driven Synthesis of Mofs-Based Facilitated Transport Hybrid Membranes for Co2 Separation

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SSRN 2023年

作者： Li, Boyu Liu, Jiaxiang He, Xuanting Mao, Shun Tao, Wenquan Li, Zhuo Hong, Yuexian State Key Laboratory of Pollution Control and Resource Reuse College of Environment Science and Engineering Tongji University Shanghai200092 China Shanghai Institute of Pollution Control and Ecological Security Shanghai200092 China Key Laboratory for Polymeric Composite and Functional Materials Ministry of Education School of Chemistry State Key Laboratory of Optoelectronic Materials and Technologies Sun Yat-sen University Guangzhou510275 China Xi’an Jiaotong University China

MOFs-based facilitated transport hybrid membranes (FTHMs) have shown their great potential in CO2-selective gas separation. However, rational membrane fabrication by distributing evenly and introducing functional groups in MOFs-based facilitated transport hybrid membrane is crucial but challenging. We herein report a facile coordination-driven approach to realizing the integration of MOF onto a polymetric matrix by introducing the polyaniline (PANI) as a binder as well as a filler disperser through Cu(II)-N coordination interaction. The resulting facilitated membrane exhibited synergetic channels to process CO2 facilitated transport due to the CO2-philic nature of PANI and MOFs with low-density pore blockage observed. The even distribution of well-dispersed MOFs nanoparticles upon PANI is realized through coordination interaction between the metal center and amino and imine groups in PANI. Moreover, PANI is highly compatible with the polymetric matrix by forming hydrogen bonds, as verified by experimental characterization and molecular dynamics (MD) simulations. The resulting FTHMs exhibit a simultaneous enhancement of individual-gas permeance (676.6 GPU) and CO2/N2 ideal selectivity (28.3), as well as enhanced decomposition temperature up to 474°C and lasting sustainability over 72 days (1728 hours). The coordination-driven membrane fabrication paves a new and promising way for designing stable, uniform, and longevity FTHMs, thus offering a potential facile route to fabricate high-performance FTHMs for CO2/N2 separation. © 2023, The Authors. All rights reserved.

关键词： Molecular dynamics

Laruo3 Perovskites as Effective and Reusable Heterogeneous Catalysts to Activate Peroxymonosulfate for Carbamazepine Degradation

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SSRN 2022年

作者： Zhou, Xuefei Li, Jiacheng Guo, Huichao Zhang, Yalei Yang, Libin Chen, Jiabin State Key Laboratory of Pollution Control and Resources Reuse College of Environmental Science and Engineering Tongji University Shanghai200092 China Shanghai Institute of Pollution Control and Ecological Security Shanghai200092 China

Sulfate radical-based technologies have been frequently applied to degrade pharmaceutical and personal care products (PPCPs). Metal-based catalysts have shown great potential for activating persulfate (PS) and peroxymonosulfate (PMS) to degrade PPCPs. In this study, a Ru-based perovskite (ARuO3, A= La, Ba, Ce, Sr) was synthesized by the sol-gel method and used as a catalyst to activate PMS for the degradation of carbamazepine (CBZ). Results show that the A-site cations had a significant influence on the catalytic performance of perovskite, and the degradation efficiency of CBZ in descending order was: La > Ba > Sr > Ce. LaRuO3 was selected as the optimal catalyst for CBZ degradation. LaRuO3 could efficiently activate PMS to degrade CBZ in a neutral environment. The reaction rate constant had a positive linear correlation with the concentration of PMS in a range between 0.1mM and 0.5 mM. ESR analysis and radical quenching experiments confirmed the existence of 1O2, •OH, and SO4•- in the LaRuO3/PMS system, and SO4•- played the most significant role in decomposing CBZ. The recycling experiment and XPS spectrogram suggested good stability and reusability of LaRuO3. © 2022, The Authors. All rights reserved.

关键词： Lanthanum compounds

A Highly Efficient Method for Analysis Cefadroxil Antibiotic Hydrolysis Based on Electrochemical Fingerprints

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SSRN 2022年

作者： Zhu, Xiaoyu Zhang, Huirong Zhai, Yongxin Wang, Ying State Key Laboratory of Pollution Control and Resources Reuse College of Environmental Science and Engineering Tongji University Shanghai 200092 China Shanghai Institute of Pollution Control and Ecological Security Shanghai 200092 China

Understanding antibiotic hydrolysis rates are important for predicting their environmental persistence as biologically active contaminants. In this study, hydrolysis rates and Arrhenius constants were determined as a function of pH and temperature for cefadroxil antibiotics by the electrochemical method. Hydrolysis rate and half-life were studied as a function of temperature (5, 25, and 45°C), and pH (1, 3, 5, 7, 9, and 11). The antibiotics were hydrolyzed under ambient conditions (pH 7 and 25 °C);half-live was 11 d by electrochemical method. Base-catalyzed hydrolysis rates were significantly greater than acid-catalyzed and neutral pH hydrolysis rates. Hydrolysis rates increased 2.6- to 3.3-fold for a 10 °C increase in temperature. Meanwhile, the hydrolysis product was also determined by the electrochemical approach and the potential degradation pathway was proposed based on mass spectrometry results. The results of this research demonstrate that degradation of β-lactam antibiotics will likely occur over several weeks in most surface waters and over several days in more alkaline systems. Our research shows a new method that under typical environmental conditions (pH and temperature) β -lactam antibiotics are hydrolytically stable with a long half-life;they thus contribute to the ongoing assessment of their environmental fate. © 2022, The Authors. All rights reserved.

关键词： Antibiotics

Absorption and Transportation of Nano-Biochar by Plants: Implications for Environmental Fate and Food Chain Risk

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SSRN 2023年

作者： Li, Yuliang Ge, Chenhao Cheng, Cheng Wang, Xiaolei Si, Dunfeng Mu, Chunyi Wang, Min Li, Hongbo Zhou, Dongmei State Key Laboratory of Pollution Control and Resource Reuse School of the Environment Nanjing University Nanjing210023 China School of Applied Meteorology Nanjing University of Information Science & Technology Nanjing210044 China

Nano-biochar (N-BC) is an emerging nanomaterial with potential applications in various fields. Understanding its behavior in the environment and its interaction with plants is crucial for assessing its ecological implications and potential risks to the food chain. In this study, we investigated the absorption and transportation of N-BC by wheat and Chinese cabbage plants using microscopy techniques and stable isotope analysis. Our results revealed that N-BC particles were readily absorbed by the plants through their root systems and transported to the aboveground tissues. Scanning electron microscopy and transmission electron microscopy provided visual evidence of N-BC particles inside the plants, predominantly located in the xylem and cell walls of the cortical tissue. Stable isotope analysis confirmed the uptake and transportation of N-BC, with elevated isotopic values observed in the plant tissues exposed to 13C-N-BC. Our results demonstrated that around 50.2% - 52.4% of the absorbed N-BC by plants was accumulated in the roots of wheat and Chinese cabbage, and the remaining fraction was transferred to the shoots including steam (31.0% -32.1%) and leaf (16.5% - 17.6%). Importantly, we observed significant accumulation of N-BC in the edible parts of Chinese cabbage, raising concerns about its potential entry into the food chain and associated health risks. These findings highlight the need for further research to explore the specific pathways and modes of N-BC uptake and transport in plants. Monitoring the presence of N-BC in the environment and its potential impact on the food chain is crucial for ensuring food security and safeguarding human health. © 2023, The Authors. All rights reserved.

关键词： Health risks

Biochar-supported nano-scale zerovalent iron activated persulfate for remediation of aromatic hydrocarbon-contaminated soil:an in-situ pilot-scale study

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Biochar 2022年第1期4卷 122-133页

作者： Yu Zeng Tai Li Yingzhi Ding Guodong Fang Xiaolei Wang Bo Ye Liqiang Ge Juan Gao Yujun Wang Dongmei Zhou Key Laboratory of Soil Environment and Pollution Remediation Institute of Soil ScienceChinese Academy of SciencesNanjing 210008People’s Republic of China University of Chinese Academy of Sciences Beijing 100049People’s Republic of China School of Environmental and Safety Engineering Changzhou UniversityChangzhou 213164China School of Earth and Environment Anhui University of Science and TechnologyHuainan 232001People’s Republic of China Geological Survey of Jiangsu Province Nanjing 210018People’s Republic of China State Key Laboratory of Pollution Control and Resource Reuse School of the EnvironmentNanjing UniversityNanjing 210023People’s Republic of China

Biochar supported nano-scale zerovalent iron(nZVI/BC)for persulfate(PS)activation has been studied extensively for the degradation of pollutants on the lab scale,but it was rarely applied in practical soil remediation in the *** this research,we developed a facile ball-milling method for the mass production of nZVI/BC,which was successfully applied to activate persulfate for the remediation of organic polluted soil on an in-situ pilot ***-situ high-pressure injection device was developed to inject nZVI/BC suspension and PS solution into the soil with a depth of 0-70 *** removal efficiency of target pollutants such as 2-ethylnitrobenzene(ENB,1.47-1.56 mg/kg),biphenyl(BP,0.19-0.21 mg/kg),4-(methylsulfonyl)toluene(MST,0.32-0.43 mg/kg),and 4-phenylphenol(PP,1.70-2.46 mg/kg)at different soil depths was 99.7%,99.1%,99.9%and 99.7%,respectively,after 360 days of *** application of nZVI/BC significantly increased the degradation rates of contaminants by 11-322%,ascribed to its relatively higher efficiency of free radical generation than that of control *** addition,it was found that nZVI/BC-PS inhibited soil urease and sucrase enzyme activities by 1-61%within 55 days due to the oxidative stress for microbes induced by free radicals,while these inhibition effects disappeared with remediation time prolonged(>127 days).Our research provides a useful implementation case of remediation with nZVI/BC-PS activation and verifies its feasibility in practical contaminated soil remediation.

关键词： Persulfate Biochar Nanoscale zerovalent iron Pilot-scale Enzyme activities