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Characterization and biodegradability assessment of water-soluble fraction of oily sludge using stir bar sorptive extraction and GCxGC-TOF MS
2022
Chand, Priyankar | Dutta, Suryendu | Mukherji, Suparna
Percolation of water through oily sludge during storage and handling of the sludge can cause soil and groundwater contamination. In this study, oily sludge from a refinery was equilibrated with water to obtain the water-soluble fraction (WSF) of oily sludge. The WSF had dissolved organic carbon (DOC) of 166 mg/L. Human cell line-based toxicity assay revealed IC₅₀ of 41 mg/L indicating its toxic nature. The predominant compounds in WSF of oily sludge included isomers of methyl, dimethyl and trimethyl quinolines and naphthalenes along with phenol derivatives and other polynuclear aromatic hydrocarbons (PAHs). Biodegradation of WSF of oily sludge was studied using a consortium of Rhodococcus ruber, Bacillus sp. and Bacillus cereus isolated from the refinery sludge. The consortium of the three strains resulted in 70% degradation over 15 days with a first-order degradation rate of 0.161 day⁻¹. Further analysis of the WSF was performed using the stir-bar sorptive extraction (SBSE) followed by GCxGC-TOF MS employing a PDMS Twister. The GCxGC analysis showed that Bacillus cereus was capable of degrading the quinoline, phenol and naphthalene derivatives in WSF of oily sludge at a faster rate compared to pyridine and benzoquinoline derivatives. Quinoline, phenol, biphenyl, naphthalene, pyridine and benzoquinolines derivatives in the WSF of oily sludge were reduced by 87%, 92%, 88%, 77%, 40% and 62%, respectively with respect to the controls. The WSF of oily sludge contained, n-alkanes, ranging from n-C12 to n-C18 which were removed within 2 days of biodegradation.
Show more [+] Less [-]Polyethylenimine-grafted nitrogen-doping magnetic biochar for efficient Cr(VI) decontamination: Insights into synthesis and adsorption mechanisms
2022
Qu, Jianhua | Zhang, Xiubo | Bi, Fuxuan | Wang, Siqi | Zhang, Xinmiao | Tao, Yue | Wang, Yifan | Zhao, Jiang | Zhang, Ying
Herein, polyethylenimine (PEI)-grafted nitrogen (N)-doping magnetic biochar (PEIMW@MNBCBM) was synthesized, and characterization results showed that the microwave-assisted PEI grafting and ball milling-assisted N doping introduced abundant amino, pyridine N and pyrrole N structures onto biochar, which possessed high affinity to Cr(VI) in the anion form. The as-prepared PEIMW@MNBCBM displayed pH-dependence adsorption performance and high tolerance to co-existing ions with maximum uptake capacity of Cr(VI) identified as 183.02 mg/g. Furthermore, PEIMW@MNBCBM could bind Cr(VI) through electrostatic attraction, complexion, precipitation, reduction and pore filling. Especially, effective reduction of Cr(VI) was ascribed to cooperative electron transfer of partial oxygen-containing functional groups, intramolecular pyridine/pyrrole N, protonated amino and Fe²⁺ on the adsorbent, while oxygen-containing and amino functional groups from N-doping biochar and PEI synergistically complexed Cr(III) via providing lone pair electrons to form coordinate bonds. Furthermore, the stable precipitation was formed between Fe³⁺ and Cr(III). Additionally, the Cr(VI) elimination efficiency could maintain 95.83% even after four adsorption-desorption cycles, suggesting PEIMW@MNBCBM as a high-performance adsorbent for Cr(VI) contaminated water remediation.
Show more [+] Less [-]Hexachloroethane dechlorination in sulfide-containing aqueous solutions catalyzed by nitrogen-doped carbon materials
2021
Liu, Na | Hu, Qing | Wang, Chao | Tong, Lizhi | Weng, Chih-Huang | Ding, Longzhen
This study demonstrated that nitrogen-doped carbon materials (NCMs) could effectively catalyze the chlorine elimination process in hexachloroethane (HCA) declorination in sulfide-containing environments for the first time. The kₒbₛ values of HCA dechlorination by sulfide in the presence of 10 mg/L NCMs were higher than that of no mediator at pH 7.3 by one or two orders of magnitude. The catalytic capabilities of NCMs on HCA dechlorination were evident in common ranges of natural pH (5.3–8.9) and it could be accelerated by the increase of pH but be suppressed by the presence of dissolved humic acid. Moreover, NCMs exhibited much better catalytic capability on HCA dechlorination compared to the carbon materials, mainly owing to the combined contributions of pyridine N, including enhanced nucleophilic attack to HCA molecule by generating newborn C–S–S and activation of HCA molecule by elongating C–Cl bonds. The functions of pyridine N in micron-sized NCMs with mesopores were better than in nano-sized NCMs on HCA dechlorination. These findings displayed the potential of NCMs, when released into sulfide-containing environments, may significantly increase the dechlorination of chlorinated aliphatic hydrocarbons.
Show more [+] Less [-]Catalytic upgrade for pyrolysis of food waste in a bubbling fluidized-bed reactor
2021
Ly, Hoang Vu | Tran, Quoc Khanh | Kim, Seung-Soo | Kim, Jinsoo | Choi, Suk Soon | Oh, Changho
Biofuel production via pyrolysis has received increasing interest as a promising solution for utilization of now wasted food residue. In this study, the fast pyrolysis of mixed food waste (MFW) was performed in a bubbling fluidized-bed reactor. This was done under different operating conditions (reaction temperatures and carrier gas flow rate) that influence product distribution and bio-oil composition. The highest liquid yield (49.05 wt%) was observed at a pyrolysis temperature of 475 °C. It was also found that the quality of pyrolysis bio-oils (POs) could be improved using catalysts. The catalytic fast pyrolysis of MFW was studied to upgrade the pyrolysis vapor, using dolomite, red mud, and HZSM-5. The higher heating values (HHVs) of the catalytic pyrolysis bio-oils (CPOs) ranged between 30.47 and 35.69 MJ/kg, which are higher than the HHVs of non-catalytic pyrolysis bio-oils (27.69–31.58 MJ/kg). The major components of the bio-oils were fatty acids, N-containing compounds, and derivatives of phenol. The selectivity for bio-oil components varied depending on the catalysts. In the presence of the catalysts, the oxygen was removed from oxygenates via moisture, CO₂, and CO. The CPOs contained aliphatic hydrocarbons, polycyclic aromatic compounds (such as naphthalene), pyridine derivatives, and light oxygenates (cyclic alkenes and ketones).
Show more [+] Less [-]Degradation of 17β-estradiol by Novosphingobium sp. ES2-1 in aqueous solution contaminated with tetracyclines
2020
Li, Shunyao | Liu, Juan | Sun, Kai | Yang, Zhiyao | Ling, Wanting
17β-estradiol (E2) often coexists with tetracyclines (TCs) in wastewater lagoons at intensive breeding farms, threatening the quality of surrounding water bodies. Microbial degradation is vital in E2 removal, but it is unclear how TCs affect E2 biodegradation. This primary study investigated the mechanisms of E2 degradation by Novosphingobium sp. ES2-1 in the presence of TCs and assessed the removal efficiency of E2 by strain ES2-1 in natural waters containing TCs. E2 biodegradation was unaffected at TCs concentrations below 0.1 mg L⁻¹ yet significantly inhibited at TCs above 10 mg L⁻¹. As elevation of TCs, E2 biodegradation rate constant decreased, and the biodegradation kinetics equation gradually deviated from the pseudo-first-order dynamics model. Importantly, the presence of TCs, especially at high-level concentrations, significantly hindered E2 ring-opening process but promoted the condensation of some phenolic ring-opening products with NH₃, thereby increasing the abundance of pyridine derivatives, which were difficult to decompose over time. Additionally, strain ES2-1 could remove 52.1–100% of nature estrogens in TCs-contaminated natural waters within 7 d. Results revealed the mechanisms of TCs in E2 biodegradation and the performance of a functional strain in estrogen removal in realistic TCs-contaminated aqueous solution.
Show more [+] Less [-]Electrochemical oxidation of ceftazidime with graphite/CNT-Ce/PbO2–Ce anode: Parameter optimization, toxicity analysis and degradation pathway
2020
Duan, Pingzhou | Gao, Shiheng | Lei, Jiawei | Li, Xiang | Hu, Xiang
In this work, the electrochemical degradation of antibiotic ceftazidime has been studied using a novel rare earth metal Ce and carbon nanotubes codoped PbO₂ electrode. A competitively high oxygen evolution potential (2.4 V) and enhanced catalytic surface area were obtained, evidence by LSV and CV electrochemical characterization. The G/CNT-Ce/PbO₂–Ce electrode possessed a more compact structure and a smaller grain size than the other PbO₂ and Ce–PbO₂ electrodes, exhibiting a prolonged service lifetime, evidence by accelerated lifespan test and recycling degradation experiment. As electrolysis time reached 120 min, the removal efficiency of ceftazidime and TOC arrived at 100.0% and 54.2% respectively in 0.05 M Na₂SO₄ solution containing 50 mg⋅L⁻¹ ceftazidime. The effect of applied current density, pH value, initial ceftazidime concentration and chloride contents on the degradation performance were systematically evaluated. The results demonstrated that electrochemical oxidation of ceftazidime over the G/CNT-Ce/PbO₂–Ce electrode was highly effective, and the mineralization rate was greatly improved, compared with pristine PbO₂ electrode. Considering the toxicity was increased after 30 min electrolysis, the intermediates were quantitatively investigated through HPLC-MS, GC-MS and IC technology. According to the identified products, a reaction mechanism has been proposed and pyridine and aminothiazole were detected with concentration from approximately 1 to 3 mg⋅L⁻¹, which were regarded as toxic byproducts during electrooxidation. Further electrocatalyzing by ring cleavage reaction and complete mineralization to CO₂, NO₃⁻ and NH₄⁺ was proposed, which demonstrated the G/CNT-Ce/PbO₂–Ce electrode exhibited high efficiency for ceftazidime removal in mild conditions.
Show more [+] Less [-]Thiacloprid affects trophic interaction between gammarids and mayflies
2012
Englert, D. | Bundschuh, M. | Schulz, R.
Neonicotinoid insecticides like thiacloprid enter agricultural surface waters, where they may affect predator–prey-interactions, which are of central importance for ecosystems as well as the functions these systems provide. The effects of field relevant thiacloprid concentrations on the leaf consumption of Gammarus fossarum (Amphipoda) were assessed over 96 h (n = 13–17) in conjunction with its predation on Baetis rhodani (Ephemeroptera) nymphs. The predation by Gammarus increased significantly at 0.50–1.00 μg/L. Simultaneously, its leaf consumption decreased with increasing thiacloprid concentration. As a consequence of the increased predation at 1.00 μg/L, gammarids' dry weight rose significantly by 15% compared to the control. At 4.00 μg/L, the reduced leaf consumption was not compensated by an increase in predation causing a significantly reduced dry weight of Gammarus (∼20%). These results may finally suggest that thiacloprid adversely affects trophic interactions, potentially translating into alterations in ecosystem functions, like leaf litter breakdown and aquatic-terrestrial subsidies.
Show more [+] Less [-]Leaching of hydrophobic Cu and Zn from discarded marine antifouling paint residues: Evidence for transchelation of metal pyrithiones
2009
Holmes, Luke | Turner, Andrew
Leaching of Cu and Zn from a composite of discarded antifouling paint residues ([Cu] = 288 mg g−1; [Zn] = 96 mg g−1) into natural sea water has been studied over a period of 75 h. Total Cu and Zn were released according to a pseudo first-order reaction, with rate constants on the order of 0.3 and 2.5 (mg L−1)−1 h−1, respectively, and final concentrations equivalent to the dissolution of about 8 and 2% of respective concentrations in the composite. Time-distributions of hydrophobic metals, determined by solid phase extraction-methanol elution, were more complex. Net release of hydrophobic Cu was greater in the absence of light than under a sequence of light–dark cycles; however, hydrophobic Zn release was not detected under the former conditions but contributed up to 50% of total aqueous Zn when light was present. These observations are interpreted in terms of the relative thermodynamic and photolytic stabilities of biocidal pyrithione complexes. Hydrophobic Cu and Zn leached from antifouling paint particles into sea water appear to be pyrithione complexes.
Show more [+] Less [-]Mechanism of biochar functional groups in the catalytic reduction of tetrachloroethylene by sulfides
2022
Yang, Yadong | Piao, Yunxian | Wang, Ruofan | Su, Yaoming | Qiu, Jinrong | Liu, Na
In recent years, biochar has become of considerable interest for environmental applications, it can be used as a catalyst for sulfides reduction of perchloroethylene, but the crucial role of biochar properties played in catalyzing dechlorination remained ambiguous investigation. To pinpoint the critical functional groups, the modified biochars were respectively produced by HNO₃, KOH and H₂O₂ with similar dimensional structures but different functional groups. Combined with the adsorption and catalytic results of different biochars, the acid-modified biochar had the best catalytic performance (99.9% removal) due to the outstanding specific surface area and ample functional groups. According to characterization and DFT results, carboxyl and pyridine nitrogen exhibited a positive correlation with the catalytic rate, indicating that their contribution to catalytic performance. Customizing biochar with specific functional groups removed depth demonstrated that the carboxyl was essential component. Further, alkaline condition was conducive to catalytic reduction, while tetrachloroethylene cannot be reduced under acidic conditions, because HS⁻ and S²⁻ mainly existed in alkaline environment and the sulfur-containing nucleophilic structure formed with biochar was more stable under this condition. Overall, this study opens new perspectives for in situ remediation by biochar in chlorinated olefin polluted anoxic environment and promotes our insight of modifying for biochar catalyst design.
Show more [+] Less [-]Peat burning – An important source of pyridines in the earth atmosphere
2020
Kosyakov, Dmitry S. | Ul’yanovskii, Nikolay V. | Latkin, Tomas B. | Pokryshkin, Sergey A. | Berzhonskis, Valeria R. | Polyakova, Olga V. | Lebedev, Albert T.
Studies of the chemical composition of atmospheric aerosols, rain water and snow in various regions of the globe quite often show the presence of pyridine and a number of its low mass derivatives. Nevertheless, the sources of those compounds in the environment have not yet been established and definitely require elucidation, supported by reliable experimental results. In the present work the chemical composition of peat combustion products as one of the important sources of atmospheric aerosol emission is studied by two-dimensional gas chromatography – high-resolution mass spectrometry with a focus on the detection of pyridine derivatives. Twenty-five compounds of this class were reliably identified and quantified in laboratory experiments on peat burning. Among them 3-hydroxypyridine predominates, while the rest analytes are mostly represented by alkyl derivatives: pyridine, 2-methylpyridine, 3-methylpyridine, 2,5-dimethylpyridine, 2,6-dimethylpyridine, 2-ethylpyridine, lutidines (in order of decreasing concentration). The distribution of these combustion products coincides with that obtained earlier in environmental studies carried out in Arctic, Central Russia and France. The experiments on peat thermal decomposition by pyrolysis GC-MS demonstrated that the maximum concentrations as well as the number of detected analytes were found under conditions of oxygen lack and a temperature of about 500 °C, i.e. characteristic conditions of peat wildfires. The observed levels of pyridines’ emission recalculated on the peat dry weight exceeded 200 mg kg⁻¹. Considering hundreds of millions tons of peat burning in megafires over 20,000 tons of pyridines penetrate the Earth atmosphere annually. The obtained results allow concluding that peat burning may be the major and still underestimated source of pyridine and lower alkylpyridines in the Earth atmosphere.
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