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Evaluation of slow-pyrolysis process effect on adsorption characteristics of cow bone for Ni ion removal from Ni-contaminated aqueous solutions 全文
2022
Saffari, Mahboub | Moazallahi, Masomeh
The optimization of nickel ion (Ni2+) removal in aqueous solutions with various factors (initial Ni concentration, solution pH, adsorbent dosage, contact time), as affected by raw cow bone (RBO) and its biochar (bone char: BC; produced by pyrolysis processes at 500 °C and a residence time of 4 hours) as adsorbents was investigated by a three-level Box–Behnken model (BBM) under response surface methodology (RSM). A total of 29 experimental runs were set for each adsorbent, and the experimental data were fitted to the empirical model. To understand the Ni2+ adsorption processes better, the properties of RBO and BC were characterized using Fe-SEM, FT-IR, BET, XRD, and CHNS elemental analysis techniques. The BC characteristics showed that pyrolysis increased the specific surface area (by 100 times) and phosphate functional groups, but decreased the carbonate functional groups, and yielded a more irregular and rougher morphological surface compared to RBO. Based on BC's superior ion exchange mechanisms and physical electrostatic adsorption compared to RBO, the removal efficiency of Ni2+ by BC was higher in aqueous solutions. The numerical optimization of BBM revealed that the optimum removal by BC (82.56%) was obtained at an initial Ni2+ concentration of 30.79 mg L−1, pH of 6.99, adsorbent dose of 4.87 g L−1, and contact time of 57.82 min, with the desirability of "1". BC can be effectively used for Ni removal from Ni-contaminated aqueous solutions; still, the application of modification methods (e.g., physical and chemical activation) may be necessary to help remove more Ni2+ by BC.
显示更多 [+] 显示较少 [-]Reactivity and fate of secondary alkane sulfonates (SAS) in marine sediments 全文
Baena Nogueras, Rosa María | Rojas Ojeda, Patricia | Sanz, José Luis | González Mazo, Eduardo | Lara Martín, Pablo Antonio | Química Física
This research is focused on secondary alkane sulfonates (SAS), anionic surfactants widely used in household applications that access aquatic environments mainly via sewage discharges.We studied their sorption capacity and anaerobic degradation in marine sediments, providing the first data available on this topic. SAS partition coefficients increased towards those homologues having longer alkyl chains(from up to 141 L kg 1 for C14 to up to 1753 L kg 1 for C17), which were those less susceptible to undergo biodegradation. Overall, SAS removal percentages reached up to 98% after 166 days of incubation using anoxic sediments. The degradation pathway consisted on the formation of sulfocarboxylic acids after an initial fumarate attack of the alkyl chain and successive b-oxidations. This is the first study showing that SAS can be degraded in absence of oxygen, so this new information should be taken into account for future environmental risk assessments on these chemicals.
显示更多 [+] 显示较少 [-]Fate of nanoplastics in the environment: Implication of the cigarette butts 全文
2021
El Hadri, Hind | Lisa, Jesus Maza | Gigault, Julien | Reynaud, Stephanie | Grassl, Bruno | Institut des sciences analytiques et de physico-chimie pour l'environnement et les materiaux (IPREM) ; Université de Pau et des Pays de l'Adour (UPPA)-Institut de Chimie - CNRS Chimie (INC-CNRS)-Centre National de la Recherche Scientifique (CNRS) | Géosciences Rennes (GR) ; Université de Rennes (UR)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Observatoire des sciences de l'environnement de Rennes (OSERen) ; Université de Rennes (UR)-Institut national des sciences de l'Univers (INSU - CNRS)-Université de Rennes 2 (UR2)-Centre National de la Recherche Scientifique (CNRS)-Institut National de Recherche pour l’Agriculture, l’Alimentation et l’Environnement (INRAE)-Institut national des sciences de l'Univers (INSU - CNRS)-Université de Rennes 2 (UR2)-Centre National de la Recherche Scientifique (CNRS)-Institut National de Recherche pour l’Agriculture, l’Alimentation et l’Environnement (INRAE) | Agence Nationale de la Recherche | ANR-16-IDEX-0002,E2S,E2S(2016)
International audience | Fate, transport and accumulation of nanoplastics have attracted considerable attention in the past few years. While actual researches have been focused on nanoplastics dispersed or aggregated in different environmental system, no study have been focused on the possibility that nanoplastics are co-transported with other natural or anthropogenic materials. Therefore, the large quantity of debris released in the environment, such as cigarette butts (CGB), could be part of the nanoplastics fate and behavior. Here we show the considerable sorption capacities of cigarette filters for nanoplastics. To address this topic, we chose polystyrene-based nanoplastics with similar state of charge (according to the physico-chemical characteristic of the zeta potential −45 to −40 mV) but with different sizes (50–800 nm) and morphologies. A kinetic approach to sorption in fresh water (pH = 8.05; 179.5 μS cm−1) at room temperature was carried out by means of the flow field flow analysis method (AF4) to determine the partition coefficients and water sampling rates between nanoplastics and cigarette butts. Using different models of, more or less environmentally relevant, nanoplastics (NPTs) and adequate analytical strategies, we found partition coefficients between the NPTs and CGBs ranged from 102 to 104 in freshwater conditions. We demonstrated that the physical features of the NPTs (size and morphology) have an influence on the sorption behaviour. Asymmetrical shaped NPTs with broader size distribution seems to be mostly retained in the CGBs after longer equilibration time. This result shows the importance of the NPTs features on the mechanisms governing their transfer and fate in the environment through environmental matrices, especially when other materials are involved. We anticipate our work to be a starting point for investigating the co-transport of NPTs with other materials present in the environment (natural and anthropogenic).
显示更多 [+] 显示较少 [-]Trace element distribution in marine microplastics using laser ablation-ICPMS 全文
2020
El Hadri, Hind | Gigault, Julien | Mounicou, Sandra | Grassl, Bruno | Reynaud, Stephanie | Institut des sciences analytiques et de physico-chimie pour l'environnement et les materiaux (IPREM) ; Université de Pau et des Pays de l'Adour (UPPA)-Institut de Chimie - CNRS Chimie (INC-CNRS)-Centre National de la Recherche Scientifique (CNRS) | Géosciences Rennes (GR) ; Université de Rennes (UR)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Observatoire des sciences de l'environnement de Rennes (OSERen) ; Université de Rennes (UR)-Institut national des sciences de l'Univers (INSU - CNRS)-Université de Rennes 2 (UR2)-Centre National de la Recherche Scientifique (CNRS)-Institut National de Recherche pour l’Agriculture, l’Alimentation et l’Environnement (INRAE)-Institut national des sciences de l'Univers (INSU - CNRS)-Université de Rennes 2 (UR2)-Centre National de la Recherche Scientifique (CNRS)-Institut National de Recherche pour l’Agriculture, l’Alimentation et l’Environnement (INRAE) | Nouvelle-Aquitaine Region | ANR-17-CE34-0008,PEPSEA,Nanoparticules de plastiques dans l'environnement: source, impact et prédiction(2017)
Trace element distribution in marine microplastics using laser ablation-ICPMS 全文
2020
El Hadri, Hind | Gigault, Julien | Mounicou, Sandra | Grassl, Bruno | Reynaud, Stephanie | Institut des sciences analytiques et de physico-chimie pour l'environnement et les materiaux (IPREM) ; Université de Pau et des Pays de l'Adour (UPPA)-Institut de Chimie - CNRS Chimie (INC-CNRS)-Centre National de la Recherche Scientifique (CNRS) | Géosciences Rennes (GR) ; Université de Rennes (UR)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Observatoire des sciences de l'environnement de Rennes (OSERen) ; Université de Rennes (UR)-Institut national des sciences de l'Univers (INSU - CNRS)-Université de Rennes 2 (UR2)-Centre National de la Recherche Scientifique (CNRS)-Institut National de Recherche pour l’Agriculture, l’Alimentation et l’Environnement (INRAE)-Institut national des sciences de l'Univers (INSU - CNRS)-Université de Rennes 2 (UR2)-Centre National de la Recherche Scientifique (CNRS)-Institut National de Recherche pour l’Agriculture, l’Alimentation et l’Environnement (INRAE) | Nouvelle-Aquitaine Region | ANR-17-CE34-0008,PEPSEA,Nanoparticules de plastiques dans l'environnement: source, impact et prédiction(2017)
International audience | Due to the dramatic quantity of plastic debris released into our environment, one of the biggest challenges of the next decades is to trace and quantify microplastics (MPs) in our environments, especially to better evaluate their capacity to transport other contaminants such as trace metals. In this study, trace elements (Fe, Cu, Zn, As, Cd, Sn, Sb, Pb, and U) were analyzed in the microplastic subsurface (200 μm) using laser ablation inductively coupled plasma mass spectrometry (LA-ICP-MS). Microplastics subjected to the marine environment were collected on beaches (Guadeloupe) exposed to the north Atlantic gyre. We established a strategy to discriminate sorbed contaminants from additives based on the metal concentration profiles in MP subsurface using qualitative and quantitative approaches. A spatiotemporal correlation of the sorption pattern was proposed to compare MPs in terms of relative exposure time and time-weighted average concentrations in the exposure media.
显示更多 [+] 显示较少 [-]Trace element distribution in marine microplastics using laser ablation-ICP-MS 全文
2020
El Hadri, Hind | Gigault, Julien | Mounicou, Sandra | Grassl, Bruno | Reynaud, Stéphanie
Due to the dramatic quantity of plastic debris released into our environment, one of the biggest challenges of the next decades is to trace and quantify microplastics (MPs) in our environments, especially to better evaluate their capacity to transport other contaminants such as trace metals. In this study, trace elements (Fe, Cu, Zn, As, Cd, Sn, Sb, Pb, and U) were analyzed in the microplastic subsurface (200 μm) using laser ablation inductively coupled plasma mass spectrometry (LA-ICP-MS). Microplastics subjected to the marine environment were collected on beaches (Guadeloupe) exposed to the north Atlantic gyre. We established a strategy to discriminate sorbed contaminants from additives based on the metal concentration profiles in MP subsurface using qualitative and quantitative approaches. A spatiotemporal correlation of the sorption pattern was proposed to compare MPs in terms of relative exposure time and time-weighted average concentrations in the exposure media.
显示更多 [+] 显示较少 [-]Effect of salinity on the fate of pesticides in irrigated systems: a first overview 全文
2023
Khouni, Mariem | Hammecker, Claude | Grünberger, Olivier | Chaabane, Hanène | Institut National Agronomique de Tunisie (INAT) | Laboratoire d'étude des Interactions Sol - Agrosystème - Hydrosystème (UMR LISAH) ; Institut de Recherche pour le Développement (IRD)-Institut National de Recherche pour l’Agriculture, l’Alimentation et l’Environnement (INRAE)-Institut Agro Montpellier ; Institut national d'enseignement supérieur pour l'agriculture, l'alimentation et l'environnement (Institut Agro)-Institut national d'enseignement supérieur pour l'agriculture, l'alimentation et l'environnement (Institut Agro) | PROJET PRIMA ALTOS
International audience | This review investigates the impact of salinity on the fate of the active compounds of pesticides in a cultivated environment. Due to the over-exploitation of water resources and intensification of agriculture, salinity outbreaks are being observed more often in cultivated fields under pesticide treatments. Nevertheless, there is a poor understanding of the incidence of varying water salt loads on the behavior of pesticides’ active ingredients in soil and water bodies. The present review established that water salinity can affect the diffusion of pesticides’ active ingredients through numerous processes. Firstly, by increasing the vapor pressure and decreasing the solubility of the compounds, which is known as the salting-out effect, salinity can change the colligative properties of water towards molecules and the modification of exchange capacity and sorption onto the chemicals. It has also been established that the osmotic stress induced by salinity could inhibit the biodegradation process by reducing the activity of sensitive microorganisms. Moreover, soil properties like dissolved organic matter, organic carbon,clay content, and soil texture control the fate and availability of chemicals in different processes of persistence in water and soil matrix. In the same line, salinity promotes the formation of different complexes, such as between humic acid and the studied active compounds. Furthermore, salinity can modify the water flux due to soil clogging because of the coagulation and dispersion of clay particle cycles, especially when the change in salinity ranges is severe.
显示更多 [+] 显示较少 [-]Trace element distribution in marine microplastics using laser ablation-ICPMS 全文
2020
El Hadri, Hind | Gigault, Julien | Mounicou, Sandra | Grassl, Bruno | Reynaud, Stephanie
International audience | Due to the dramatic quantity of plastic debris released into our environment, one of the biggest challenges of the next decades is to trace and quantify microplastics (MPs) in our environments, especially to better evaluate their capacity to transport other contaminants such as trace metals. In this study, trace elements (Fe, Cu, Zn, As, Cd, Sn, Sb, Pb, and U) were analyzed in the microplastic subsurface (200 μm) using laser ablation inductively coupled plasma mass spectrometry (LA-ICP-MS). Microplastics subjected to the marine environment were collected on beaches (Guadeloupe) exposed to the north Atlantic gyre. We established a strategy to discriminate sorbed contaminants from additives based on the metal concentration profiles in MP subsurface using qualitative and quantitative approaches. A spatiotemporal correlation of the sorption pattern was proposed to compare MPs in terms of relative exposure time and time-weighted average concentrations in the exposure media.
显示更多 [+] 显示较少 [-]Effect of varying pH and co-existing microcystin-LR on time- and concentration-dependent cadmium sorption by goethite-modified biochar derived from distillers’ grains 全文
2022
Zhao, Yu | Li, Jieming
Cadmium (Cd) is one dangerous and widespread heavy metal that of great environmental concern. To cost-efficiently adsorb aqueous Cd under influence of various factors, this study succeeded in fabricating goethite-modified biochar (GBC) derived from distillers’ grains (DGs) for Cd sorption of different concentrations (10–100 mg L⁻¹) at pH of 3, 6 and 8 with and without microcystin-LR (MC-LR). Sorption kinetics and isotherms data revealed that Cd sorption capacity of GBC and unmodified BC increased as pH elevated from 3 to 6 but stabilized when pH further elevated to 8. Pseudo-second-order and Langmuir models more accurately fitted to sorption data for both BCs, implying monolayer chemisorption of Cd onto BCs. GBC exhibited more robust sorption for each Cd concentration than unmodified BC, with the maximum sorption capacity of around 28 mg g⁻¹ at neutral and weak alkaline pH. Notably, goethite-modification obviously increased bulk polarity, specific surface area, porosity and surface oxygenic group abundance of BC, thus strongly enhancing Cd sorption by creating more sorption sites mainly via pore-filling, electrostatic attraction, and also via complexation and cation exchange. Co-existing MC-LR of 100 μg L⁻¹ did not obviously affect Cd sorption by both BCs for most Cd levels at each pH, mostly because sorption mechanisms diverged between MC-LR and Cd to largely avoid their competition for sorption sties. Thus, goethite could modify DG-BC as promising and cost-efficient sorbent for Cd even with co-existing MC-LR, especially at neutral and weak alkaline pH that common in the nature. This study was greatly implicated in modifying and applying DG-BC for Cd immobilization in MC-LR laden waters with various pH circumstances.
显示更多 [+] 显示较少 [-]Distribution of florfenicol and norfloxacin in ice during water freezing process: Dual effects by fluorine substituents 全文
2022
Sun, Heyang | Chen, Tianyi | Zhang, Liwen | Dong, Deming | Li, Yanchun | Guo, Zhiyong
Distribution in ice is regarded as one of important transport modes for pollutants in seasonal freeze-up waters in cold regions. However, the distribution characteristics and mechanisms of fluorinated antibiotics as emerging contaminants during the water freezing process remain unclear. Here, florfenicol and norfloxacin were selected as model fluorinated antibiotics to investigate their ice-water distribution. Effects of antibiotic molecular structure on the distribution were explored through comparative studies with their non-fluorinated structural analogs. Results showed that phase changes during the ice growth process redistributed the antibiotics, with antibiotic concentrations in water 3.0–6.4 times higher than those in ice. The solute-rich boundary layer with a concentration gradient was presented at the ice-water interface and controlled by constitutional supercooling during the freezing process. The ice-water distribution coefficient (KIW) values of antibiotics increased by 34.8%–38.0% with a doubling of the cooling area. The solute distribution coefficient (Kbₛ) values of antibiotics at −20 °C were 65.6%–70.3% higher than at −10 °C. The KIW and Kbₛ values of all antibiotics were negatively correlated with their water solubilities. The fluorine substituents influenced the binding energies between antibiotics and ice, resulting in a 1.1-fold increase in the binding energy of norfloxacin on the ice surface relative to its structural analog pipemidic acid. The results provide a new insight into the transport behaviors of fluorinated pharmaceuticals in ice-water systems.
显示更多 [+] 显示较少 [-]Impact of catalytic hydrothermal treatment and Ca/Al-modified hydrochar on lability, sorption, and speciation of phosphorus in swine manure: Microscopic and spectroscopic investigations 全文
2022
He, Xinyue | Zhang, Tao | Niu, Yingqi | Xue, Qing | Ali, Esmat F. | Shaheen, Sabry M. | Tsang, Daniel C.W. | Rinklebe, Jörg
The effects of catalytic hydrothermal (HT) pretreatment on animal manure followed by the addition of hydrochar on the nutrients recovery have not yet been investigated using a combination of chemical, microscopic, and spectroscopic techniques. Therefore, a catalytic HT process was employed to pretreat swine manure without additives (manure-HT) and with H₂O₂ addition (manure-HT- H₂O₂) to improve the conversion efficiency of labile or organic phosphorus (P) to inorganic phase. Then, a Ca–Al layered double hydroxide hydrochar (Ca/Al LDH@HC) derived from corn cob biomass was synthesized and applied to enhance P sorption. Scanning electron microscopy (SEM), and three-dimensional excitation emission matrix (3D-EEM), X-ray photoelectron spectroscopy (XPS), P k-edge X-ray absorption near edge structure (XANES), were used to elucidate the mechanisms of P release and capture. The H₂O₂ assisted HT treatment significantly enhanced the release of inorganic P (251.4 mg/L) as compared to the untreated manure (57.2 mg/L). The 3D-EEM analysis indicated that the labile or organic P was transformed and solubilized efficiently along with the deconstruction of manure components after the H₂O₂ assisted HT pretreatment. Application of Ca/Al LDH@HC improved the removal efficiency of P from the derived P-rich HT liquid. This sorption process was conformed to the pseudo-second-order model, suggesting that chemisorption was the primary mechanism. The results of SEM and P k-edge XANES exhibited that Ca, as the dominated metal component, could act as a reaction site for the formation of phosphate precipitation. These results provide critical findings about recovering P from manure waste, which is useful for biowastes management and nutrients utilization, and mitigating unintended P loss and potential environmental risks.
显示更多 [+] 显示较少 [-]Enhanced removal of per- and polyfluoroalkyl substances in complex matrices by polyDADMAC-coated regenerable granular activated carbon 全文
2022
Ramos, Pia | Singh Kalra, Shashank | Johnson, Nicholas W. | Khor, Chia Miang | Borthakur, Annesh | Cranmer, Brian | Dooley, Gregory | Mohanty, Sanjay K. | Jassby, David | Blotevogel, Jens | Mahendra, Shaily
Granular activated carbon (GAC) has been used to remove per- and polyfluoroalkyl substances (PFASs) from industrial or AFFF-impacted waters, but its effectiveness can be low because adsorption of short-chained PFASs is ineffective and its sites are exhausted rapidly by co-contaminants. To increase adsorption of anionic PFASs on GAC by electrostatic attractions, we modified GAC's surface with the cationic polymer poly diallyldimethylammonium chloride (polyDADMAC) and tested its capacity in complex water matrices containing dissolved salts and humic acid. Amending with concentrations of polyDADMAC as low as 0.00025% enhanced GAC's adsorption capacity for PFASs, even in the presence of competing ions. This suggests that electrostatic interactions with polyDADMAC's quaternary ammonium functional groups helped bind organic and inorganic ions as well as the headgroup of short-chain PFASs, allowing more overall PFAS removal by GAC. Evaluating the effect of polymer dose is important because excessive addition can block pores and reduce overall PFAS removal rather than increase it. To decrease the waste associated with this adsorption strategy by making the adsorbent viable for more than one saturation cycle, a regeneration method is proposed which uses low-power ultrasound to enhance the desorption of PFASs from the polyDADMAC-GAC with minimum disruption to the adsorbent's structure. Re-modification with the polymer after sonication resulted in a negligible decrease in the sorbent's capacity over four saturation rounds. These results support consideration of polyDADMAC-modified GAC as an effective regenerable adsorbent for ex-situ concentration step of both short and long-chain PFASs from real waters with high concentrations of competing ions and low PFAS loads.
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