The “forever chemicals”, per- and polyfluoroalkyl substances (PFAS), have become a threat to public health and environment because of their toxicity and bioaccumulation. Addressing this critical issue, we develop a state-of-the-art nanocomposite adsorbent by covalently grafting amine functional groups onto graphene oxide (GO) surfaces and making them magnetic with iron-oxide (Fe3O4) nanoparticles. This process results in the creation of magnetic amine-functionalized graphene oxide (MAGO). The efficiency of MAGO is evaluated in the adsorptive removal of perfluorooctanoic acid (PFOA), perfluorooctane sulfonate (PFOS), perfluorohexane sulfonate (PFHxS), and perfluorobutane sulfonate (PFBS) as model long-chain and short-chain PFAS under different experimental conditions. Our findings reveal that MAGO achieves remarkable removal rates—exceeding 95% for long-chain PFAS and 85% for short-chain PFAS within just 30 minutes—demonstrating not only rapid kinetics but also a resilience across pH levels from 4 to 7. These results are indicative of the synergistic effects of GO and amine groups, harnessing both electrostatic and hydrophobic interactions to adsorb PFAS molecules. MAGO not only shows potent pollutant removal but also has impressive regeneration capabilities. Moreover, we demonstrate a novel liquid phase extraction method for PFAS detection, utilizing a colored methylene blue-PFAS complex for spectrophotometric analysis.
{"title":"Magnetic amino-functionalized graphene oxide nanocomposite for PFAS removal from water†","authors":"Shokouh Mahpishanian, Muchu Zhou and Reza Foudazi","doi":"10.1039/D4VA00171K","DOIUrl":"10.1039/D4VA00171K","url":null,"abstract":"<p >The “forever chemicals”, per- and polyfluoroalkyl substances (PFAS), have become a threat to public health and environment because of their toxicity and bioaccumulation. Addressing this critical issue, we develop a state-of-the-art nanocomposite adsorbent by covalently grafting amine functional groups onto graphene oxide (GO) surfaces and making them magnetic with iron-oxide (Fe<small><sub>3</sub></small>O<small><sub>4</sub></small>) nanoparticles. This process results in the creation of magnetic amine-functionalized graphene oxide (MAGO). The efficiency of MAGO is evaluated in the adsorptive removal of perfluorooctanoic acid (PFOA), perfluorooctane sulfonate (PFOS), perfluorohexane sulfonate (PFHxS), and perfluorobutane sulfonate (PFBS) as model long-chain and short-chain PFAS under different experimental conditions. Our findings reveal that MAGO achieves remarkable removal rates—exceeding 95% for long-chain PFAS and 85% for short-chain PFAS within just 30 minutes—demonstrating not only rapid kinetics but also a resilience across pH levels from 4 to 7. These results are indicative of the synergistic effects of GO and amine groups, harnessing both electrostatic and hydrophobic interactions to adsorb PFAS molecules. MAGO not only shows potent pollutant removal but also has impressive regeneration capabilities. Moreover, we demonstrate a novel liquid phase extraction method for PFAS detection, utilizing a colored methylene blue-PFAS complex for spectrophotometric analysis.</p>","PeriodicalId":72941,"journal":{"name":"Environmental science. Advances","volume":" 12","pages":" 1698-1713"},"PeriodicalIF":3.5,"publicationDate":"2024-08-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/va/d4va00171k?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142208554","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Sofina Begum, Nicole Prince, Lidia Mínguez-Alarcón, Yulu Chen, Djøra I. Soeteman, Vrushali Fangal, Mengna Huang, Craig Wheelock, Kevin Mendez, Augusto A. Litonjua, Scott T. Weiss, Jessica Lasky-Su and Rachel S. Kelly
Per- and polyfluoroalkyl substances (PFAS) are a group of synthetic, highly fluorinated aliphatic compounds, commonly utilised in a wide variety of consumer products with diverse applications. Since the genesis of these compounds, a growing body of evidence has demonstrated adverse health effects associated with PFAS exposure. In a racially diverse cohort of 459 pregnant mothers, demographically weighted towards minority representation (black 44.4%, white 38.4%, other 17.2%), across three major populous cities of the US, PFAS profiling was performed. Nine distinct PFAS species were quantified using mass spectrometry in plasma samples collected during the third trimester. Multivariable logistic and linear regression analyses were conducted to interrogate the associations of PFAS with gestational and birth outcomes: gestational diabetes, preeclampsia, gestational age at delivery, low birth weight, birth weight-, birth length- and head circumference-for-gestational-age. Detectable levels for eight out of nine profiled PFAS species were found in the plasma of pregnant mothers with a median range of 0.1–2.70 ng ml−1. Using a mixtures approach, we observe that increased quantile-based g-computation (Qg-comp) “total” PFAS levels were associated with increased newborn birth-weight-for-gestational-age (β 1.28; 95% CI 1.07–1.52; FDR p 0.006). In study centre-stratified analyses, we observed a similar trend in Boston pregnant mothers, with Qg-comp total PFAS associated with higher newborn birth-weight-for-gestational-age (β 1.39; 95% CI 1.01–1.92, FDR p 0.05). We additionally found elevated PFUA concentrations were associated with longer gestational terms in San Diego pregnant mothers (β 0.60; 95% CI 0.18–1.02, FDR p 0.05). In this multi-city study, we detected lower levels of PFAS than in many previous US environmental studies, concordant with current US trends indicating environmental PFAS levels are falling, and we note geographical variation in the associations between PFAS levels and birth outcomes.
全氟烷基和多氟烷基物质(PFAS)是一组人工合成的高氟脂肪族化合物,通常用于各种用途广泛的消费品中。自这些化合物问世以来,越来越多的证据表明,接触 PFAS 会对健康造成不良影响。在美国三个主要人口城市的 459 名不同种族的怀孕母亲中,进行了全氟辛烷磺酸分析,人口统计学上以少数族裔代表为主(黑人 44.4%、白人 38.4%、其他 17.2%)。在怀孕三个月期间采集的血浆样本中,使用质谱法对九种不同的 PFAS 进行了量化。通过多变量逻辑分析和线性回归分析,研究了 PFAS 与妊娠和分娩结局的关系:妊娠糖尿病、子痫前期、胎龄、低出生体重、出生体重、出生身长和胎龄头围。在怀孕母亲的血浆中发现了九种全氟辛烷磺酸中的八种,其可检测水平的中位数范围为 0.1-2.70 纳克毫升-1。通过使用混合物方法,我们发现基于量子化 g 计算(Qg-comp)的 "总 "PFAS 水平的增加与新生儿出生体重-妊娠年龄的增加有关(β 1.28;95% CI 1.07-1.52;FDR p 0.006)。在研究中心的分层分析中,我们在波士顿的孕妇中观察到了类似的趋势,Qg-omp 总 PFAS 与较高的新生儿出生体重-胎龄相关(β 1.39;95% CI 1.01-1.92;FDR p 0.05)。我们还发现,PFUA 浓度升高与圣地亚哥孕妇的妊娠期延长有关(β 0.60;95% CI 0.18-1.02,FDR p 0.05)。在这项多城市研究中,我们检测到的全氟辛烷磺酸水平低于之前的许多美国环境研究,这与当前美国环境中全氟辛烷磺酸水平正在下降的趋势一致。
{"title":"Pregnancy complications and birth outcomes following low-level exposure to per- and polyfluoroalkyl substances in the vitamin D antenatal asthma reduction trial†","authors":"Sofina Begum, Nicole Prince, Lidia Mínguez-Alarcón, Yulu Chen, Djøra I. Soeteman, Vrushali Fangal, Mengna Huang, Craig Wheelock, Kevin Mendez, Augusto A. Litonjua, Scott T. Weiss, Jessica Lasky-Su and Rachel S. Kelly","doi":"10.1039/D4VA00001C","DOIUrl":"10.1039/D4VA00001C","url":null,"abstract":"<p >Per- and polyfluoroalkyl substances (PFAS) are a group of synthetic, highly fluorinated aliphatic compounds, commonly utilised in a wide variety of consumer products with diverse applications. Since the genesis of these compounds, a growing body of evidence has demonstrated adverse health effects associated with PFAS exposure. In a racially diverse cohort of 459 pregnant mothers, demographically weighted towards minority representation (black 44.4%, white 38.4%, other 17.2%), across three major populous cities of the US, PFAS profiling was performed. Nine distinct PFAS species were quantified using mass spectrometry in plasma samples collected during the third trimester. Multivariable logistic and linear regression analyses were conducted to interrogate the associations of PFAS with gestational and birth outcomes: gestational diabetes, preeclampsia, gestational age at delivery, low birth weight, birth weight-, birth length- and head circumference-for-gestational-age. Detectable levels for eight out of nine profiled PFAS species were found in the plasma of pregnant mothers with a median range of 0.1–2.70 ng ml<small><sup>−1</sup></small>. Using a mixtures approach, we observe that increased quantile-based g-computation (Qg-comp) “total” PFAS levels were associated with increased newborn birth-weight-for-gestational-age (<em>β</em> 1.28; 95% CI 1.07–1.52; FDR <em>p</em> 0.006). In study centre-stratified analyses, we observed a similar trend in Boston pregnant mothers, with Qg-comp total PFAS associated with higher newborn birth-weight-for-gestational-age (<em>β</em> 1.39; 95% CI 1.01–1.92, FDR <em>p</em> 0.05). We additionally found elevated PFUA concentrations were associated with longer gestational terms in San Diego pregnant mothers (<em>β</em> 0.60; 95% CI 0.18–1.02, FDR <em>p</em> 0.05). In this multi-city study, we detected lower levels of PFAS than in many previous US environmental studies, concordant with current US trends indicating environmental PFAS levels are falling, and we note geographical variation in the associations between PFAS levels and birth outcomes.</p>","PeriodicalId":72941,"journal":{"name":"Environmental science. Advances","volume":" 10","pages":" 1426-1437"},"PeriodicalIF":3.5,"publicationDate":"2024-08-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11328948/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142001473","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Fluorotelomer (FT) alcohols (FTOHs) belong to the subclass of per- and polyfluoroalkyl substances (PFAS) and are used as building blocks of FT-based side chain fluorinated polymers (SCFPs), which are applied to consumer products to provide hydro- and oleophobic characteristics. FTOHs are consistently detected in consumer products, indicating FTOHs as major degradation products of FT-based SCFPs. Literature on FTOHs indicates that much is known about the release of FTOHs during the production, throughout the lifetime, and at the end-of-life of consumer products. This Perspective combines information from FTOHs in consumer products with sufficient knowledge on FTOH volatility, partitioning to the gas phase, and transformation to perfluorocarboxylates (PFCAs) to understand the extent of FTOH release to the environment. In the indoor environment, FTOHs are released in textile factories to the air during the production of consumer products, indicating a potential inhalation risk for the workers. Meanwhile, indoor air FTOH levels at residential sites are estimated to pose low inhalation risk to humans based on studies of 8:2 FTOH, which is known to undergo human metabolism to perfluorooctanoate (PFOA). Release of FTOHs from FT-based SCFP-applied consumer products to the indoor environment throughout the lifetime of the products is known, as well as release to the outdoor environment through washing, weathering, or drying. At the end-of-life of consumer products, FTOHs are released to air from landfills and can be detected in biosolids. Future policies need to not only account for FTOH presence in consumer products, but also the known FTOH volatility, partitioning to the gas phase, and transformation to PFCAs.
{"title":"Chemical transformation, exposure assessment, and policy implications of fluorotelomer alcohol partitioning from consumer products to the indoor and outdoor environment—from production to end-of-life","authors":"Ivan A. Titaley","doi":"10.1039/D4VA00019F","DOIUrl":"10.1039/D4VA00019F","url":null,"abstract":"<p >Fluorotelomer (FT) alcohols (FTOHs) belong to the subclass of per- and polyfluoroalkyl substances (PFAS) and are used as building blocks of FT-based side chain fluorinated polymers (SCFPs), which are applied to consumer products to provide hydro- and oleophobic characteristics. FTOHs are consistently detected in consumer products, indicating FTOHs as major degradation products of FT-based SCFPs. Literature on FTOHs indicates that much is known about the release of FTOHs during the production, throughout the lifetime, and at the end-of-life of consumer products. This Perspective combines information from FTOHs in consumer products with sufficient knowledge on FTOH volatility, partitioning to the gas phase, and transformation to perfluorocarboxylates (PFCAs) to understand the extent of FTOH release to the environment. In the indoor environment, FTOHs are released in textile factories to the air during the production of consumer products, indicating a potential inhalation risk for the workers. Meanwhile, indoor air FTOH levels at residential sites are estimated to pose low inhalation risk to humans based on studies of 8:2 FTOH, which is known to undergo human metabolism to perfluorooctanoate (PFOA). Release of FTOHs from FT-based SCFP-applied consumer products to the indoor environment throughout the lifetime of the products is known, as well as release to the outdoor environment through washing, weathering, or drying. At the end-of-life of consumer products, FTOHs are released to air from landfills and can be detected in biosolids. Future policies need to not only account for FTOH presence in consumer products, but also the known FTOH volatility, partitioning to the gas phase, and transformation to PFCAs.</p>","PeriodicalId":72941,"journal":{"name":"Environmental science. Advances","volume":" 10","pages":" 1364-1384"},"PeriodicalIF":3.5,"publicationDate":"2024-08-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/va/d4va00019f?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141933899","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Alex T. Ford, Mark F. Fitzsimons and Crispin Halsall
The North East coast of England experienced a mass mortality event in late 2021 affecting millions of crabs and lobsters. The die-off coincided with the redevelopment of one of the UK's flagship ports, prompting local scientists to suggest the remobilization of dredged industrial contaminants as a cause. A multi-agency investigation found no definitive causal factor; however, re-evaluation of data by consultants drew a different conclusion, linking the industrial compound pyridine to the crustacean deaths. Authors of an unpublished study subsequently claimed that their data demonstrated pyridine to be exceptionally toxic and that their modeling explained the coastal distribution of washups. These data were presented to a cross-party Environmental, Fisheries and Rural Affairs (EFRA) committee in the UK parliament and led to the commissioning of an independent panel to review the data. This panel was also unable to identify a definitive cause, but found that a major role for pyridine was ‘very unlikely’. Unfortunately, the debate has been highly politicised, with misleading information aired by the two leading political parties. Here, several members of that independent review panel refute the pyridine link to the mass mortality, based on both reported data and the known chemistry and behaviour of this molecule, and highlight where the science has been misrepresented by the media.
{"title":"Why there is no evidence that pyridine killed the English crabs†","authors":"Alex T. Ford, Mark F. Fitzsimons and Crispin Halsall","doi":"10.1039/D4VA00006D","DOIUrl":"10.1039/D4VA00006D","url":null,"abstract":"<p >The North East coast of England experienced a mass mortality event in late 2021 affecting millions of crabs and lobsters. The die-off coincided with the redevelopment of one of the UK's flagship ports, prompting local scientists to suggest the remobilization of dredged industrial contaminants as a cause. A multi-agency investigation found no definitive causal factor; however, re-evaluation of data by consultants drew a different conclusion, linking the industrial compound pyridine to the crustacean deaths. Authors of an unpublished study subsequently claimed that their data demonstrated pyridine to be exceptionally toxic and that their modeling explained the coastal distribution of washups. These data were presented to a cross-party Environmental, Fisheries and Rural Affairs (EFRA) committee in the UK parliament and led to the commissioning of an independent panel to review the data. This panel was also unable to identify a definitive cause, but found that a major role for pyridine was ‘very unlikely’. Unfortunately, the debate has been highly politicised, with misleading information aired by the two leading political parties. Here, several members of that independent review panel refute the pyridine link to the mass mortality, based on both reported data and the known chemistry and behaviour of this molecule, and highlight where the science has been misrepresented by the media.</p>","PeriodicalId":72941,"journal":{"name":"Environmental science. Advances","volume":" 10","pages":" 1385-1391"},"PeriodicalIF":3.5,"publicationDate":"2024-08-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/va/d4va00006d?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141933964","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The European Union and governments of various economies in the world are currently developing supply chain legislation for businesses, aiming to protect the environment and human rights in supply chains. These laws regulate firms active on home markets in these countries, but in terms of environmental and human rights risks also apply to global supply chains. Legislative initiatives assume that firms have the ability to influence many suppliers and their conditions of production abroad. Illustrated by the urgent case of garment production exported to Europe, we conclude that current import–export relations could limit the scope and impact of such supply chain legislation. If patterns as visible in the garment sector hold more broadly, policymakers that are ambitious about the impact of supply chain legislation on environment and human rights face a policy trilemma: they must sacrifice one out of three current design features of such legislation: designing legislation unilaterally for their home markets, letting regulation apply to supply chains across the world, or giving firms the ability to freely choose their suppliers. We discuss the different combinations of design options that could advance sustainability in supply chains.
{"title":"Advancing sustainability through supply chain legislation? A policy trilemma","authors":"Luc Fransen, Martin Curley and Anne Lally","doi":"10.1039/D4VA00048J","DOIUrl":"10.1039/D4VA00048J","url":null,"abstract":"<p >The European Union and governments of various economies in the world are currently developing supply chain legislation for businesses, aiming to protect the environment and human rights in supply chains. These laws regulate firms active on home markets in these countries, but in terms of environmental and human rights risks also apply to global supply chains. Legislative initiatives assume that firms have the ability to influence many suppliers and their conditions of production abroad. Illustrated by the urgent case of garment production exported to Europe, we conclude that current import–export relations could limit the scope and impact of such supply chain legislation. If patterns as visible in the garment sector hold more broadly, policymakers that are ambitious about the impact of supply chain legislation on environment and human rights face a policy trilemma: they must sacrifice one out of three current design features of such legislation: designing legislation unilaterally for their home markets, letting regulation apply to supply chains across the world, or giving firms the ability to freely choose their suppliers. We discuss the different combinations of design options that could advance sustainability in supply chains.</p>","PeriodicalId":72941,"journal":{"name":"Environmental science. Advances","volume":" 9","pages":" 1317-1328"},"PeriodicalIF":3.5,"publicationDate":"2024-08-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/va/d4va00048j?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141883643","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Angelo Ferlazzo, Antonino Gulino and Giovanni Neri
Modified yttria- and scandia-doped zirconium oxides were exploited for the development of an effective electrochemical sensor for the simultaneous detection of dihydroxy benzene (DHB) isomers, i.e. hydroquinone (HQ), catechol (CC) and resorcinol (RS). A morphological, microstructural and electrochemical characterization, by scanning electron microscopy (SEM), infrared spectroscopy (FT-IR), X-ray diffraction (XRD), electrical impedance spectroscopy (EIS), cyclic voltammetry (CV), and square wave voltammetry (SWV), of pure zirconium oxide, zirconium oxide doped with 8% yttria and zirconium oxide doped with 10% scandium (ZrO2, ZrO28Y, and ZrO210Sc, respectively), were carried out. Modified electrochemical sensors were fabricated by using a screen-printed carbon electrode (SPCE). Electrochemical analysis conducted in phosphate buffer solution (0.01 M PBS; pH = 7.4) showed the great ability of the ZrO210Sc/SPCE sensor to detect simultaneously DHB isomers with high sensitivity. SWV analysis performed with this sensor showed the lowest limits of detection (LODs) among all sensors tested, with values of 0.92, 0.69, and 5.61 nM, for hydroquinone (HQ), catechol (CC), and resorcinol (RS), respectively. In addition, the sensor shows good repeatability and simultaneous detection capability for all DHB isomers. This sensor also showed excellent results for the detection of HQ, CC, and RS in tap and mineral water samples, with good recoveries (90–116%).
{"title":"Scandia-doped zirconia for the electrochemical detection of hazardous dihydroxybenzene (DHB) isomers in water†","authors":"Angelo Ferlazzo, Antonino Gulino and Giovanni Neri","doi":"10.1039/D4VA00126E","DOIUrl":"10.1039/D4VA00126E","url":null,"abstract":"<p >Modified yttria- and scandia-doped zirconium oxides were exploited for the development of an effective electrochemical sensor for the simultaneous detection of dihydroxy benzene (DHB) isomers, <em>i.e.</em> hydroquinone (HQ), catechol (CC) and resorcinol (RS). A morphological, microstructural and electrochemical characterization, by scanning electron microscopy (SEM), infrared spectroscopy (FT-IR), X-ray diffraction (XRD), electrical impedance spectroscopy (EIS), cyclic voltammetry (CV), and square wave voltammetry (SWV), of pure zirconium oxide, zirconium oxide doped with 8% yttria and zirconium oxide doped with 10% scandium (ZrO<small><sub>2</sub></small>, ZrO<small><sub>2</sub></small>8Y, and ZrO<small><sub>2</sub></small>10Sc, respectively), were carried out. Modified electrochemical sensors were fabricated by using a screen-printed carbon electrode (SPCE). Electrochemical analysis conducted in phosphate buffer solution (0.01 M PBS; pH = 7.4) showed the great ability of the ZrO<small><sub>2</sub></small>10Sc/SPCE sensor to detect simultaneously DHB isomers with high sensitivity. SWV analysis performed with this sensor showed the lowest limits of detection (LODs) among all sensors tested, with values of 0.92, 0.69, and 5.61 nM, for hydroquinone (HQ), catechol (CC), and resorcinol (RS), respectively. In addition, the sensor shows good repeatability and simultaneous detection capability for all DHB isomers. This sensor also showed excellent results for the detection of HQ, CC, and RS in tap and mineral water samples, with good recoveries (90–116%).</p>","PeriodicalId":72941,"journal":{"name":"Environmental science. Advances","volume":" 10","pages":" 1392-1399"},"PeriodicalIF":3.5,"publicationDate":"2024-07-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/va/d4va00126e?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141866160","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Dissolved oxygen (DO) is an important variable for rivers, which controls many biogeochemical processes within rivers and the survival of aquatic species. Therefore, accurate forecasting of DO is of great importance. This study proposes two models, including AR-RBF by leveraging the additive regression (AR) of radial basis function (RBF) neural networks and MLP-RF by stacking multilayer perceptron (MLP) and random forest (RF), for the prediction of daily DO with multiple forecast horizons (1 day ahead to 15 days ahead) in the Mississippi River using a long-term observed dataset from the Baton Rouge station. Two input scenarios were considered: scenario A includes mean water temperature and a certain number of preceding DO values and scenario B comprises solely the aforementioned number of preceding DO values while entirely disregarding exogenous variables. The AR-RBF and stacked MLP-RF models excel in short-term forecasting and offer sufficiently accurate predictions for medium-term horizons of up to 15 days. For instance, in 3 day ahead predictions, the root mean square error (RMSE) amounts to 0.28 mg L−1, with the mean absolute percentage error (MAPE) hovering around 2.5% in the worst-case scenario. Similarly, for 15 day ahead forecasts, RMSE remains below 0.93 mg L−1, with MAPE not exceeding 8.2%, even under the worst-case scenario. Both models effectively capture the extreme values and the fluctuations of DO. However, as the forecasting horizon is extended, both models experience a decrease in accuracy, which is particularly evident for scenario B when the average water temperature is not included in the input variables. When examining longer forecasting horizons in the study, AR-RBF demonstrates a more restrained bias as compared to the stacked MLP-RF model. The consistently robust performance of the models, in comparison to prior research on DO levels in US rivers, underscores their potential as more effective tools for predicting such an essential water quality parameter.
{"title":"Dissolved oxygen forecasting in the Mississippi River: advanced ensemble machine learning models","authors":"Francesco Granata, Senlin Zhu and Fabio Di Nunno","doi":"10.1039/D4VA00119B","DOIUrl":"10.1039/D4VA00119B","url":null,"abstract":"<p >Dissolved oxygen (DO) is an important variable for rivers, which controls many biogeochemical processes within rivers and the survival of aquatic species. Therefore, accurate forecasting of DO is of great importance. This study proposes two models, including AR-RBF by leveraging the additive regression (AR) of radial basis function (RBF) neural networks and MLP-RF by stacking multilayer perceptron (MLP) and random forest (RF), for the prediction of daily DO with multiple forecast horizons (1 day ahead to 15 days ahead) in the Mississippi River using a long-term observed dataset from the Baton Rouge station. Two input scenarios were considered: scenario A includes mean water temperature and a certain number of preceding DO values and scenario B comprises solely the aforementioned number of preceding DO values while entirely disregarding exogenous variables. The AR-RBF and stacked MLP-RF models excel in short-term forecasting and offer sufficiently accurate predictions for medium-term horizons of up to 15 days. For instance, in 3 day ahead predictions, the root mean square error (RMSE) amounts to 0.28 mg L<small><sup>−1</sup></small>, with the mean absolute percentage error (MAPE) hovering around 2.5% in the worst-case scenario. Similarly, for 15 day ahead forecasts, RMSE remains below 0.93 mg L<small><sup>−1</sup></small>, with MAPE not exceeding 8.2%, even under the worst-case scenario. Both models effectively capture the extreme values and the fluctuations of DO. However, as the forecasting horizon is extended, both models experience a decrease in accuracy, which is particularly evident for scenario B when the average water temperature is not included in the input variables. When examining longer forecasting horizons in the study, AR-RBF demonstrates a more restrained bias as compared to the stacked MLP-RF model. The consistently robust performance of the models, in comparison to prior research on DO levels in US rivers, underscores their potential as more effective tools for predicting such an essential water quality parameter.</p>","PeriodicalId":72941,"journal":{"name":"Environmental science. Advances","volume":" 11","pages":" 1537-1551"},"PeriodicalIF":3.5,"publicationDate":"2024-07-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/va/d4va00119b?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141866161","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Rashmi Ira, Vikas Sharma, Shrawan Kumar, Mira Koul, Lalita Sharma, Aditi Halder and Tulika Prakash
The world's increasing dependency on fossil fuels has become a significant energy and environmental concern as they contribute 83% of the global energy supply and produce large amounts of carbon dioxide. Biohythane, a blend of biomethane (5–10%) and biohydrogen (50–60%), is emerging as a promising and environmentally friendly alternative fuel derived from organic wastes and offers a sustainable solution. The existing methods of biohythane production suffer from major limitations of being cost- and labor-intensive due to adopting bulk substrate pretreatment to enhance biohythane yield thereby limiting their industrial applications. In this study, we have developed a synthetic microbial consortium (E(C2)Tx) for anaerobic digestion by combining various organic wastes and subjecting them to heat pre-treatment and acclimatization to enrich biohydrogen producers and methanogens, respectively. Raw cow dung was anaerobically digested as the substrate with E(C2)Tx and this resulted in the production of biohythane with 3% biohydrogen and 36% biomethane. The consortia designing strategy avoided any bulk substrate pretreatment and only included the pretreatment of the inoculum which is used in four times less volume than the substrate. A 16S rRNA gene based metagenomic analysis revealed that the CD samples treated with E(C2)Tx were enriched in cellulolytic and hydrogen-producing Firmicutes, along with methylotrophic and hydrogenotrophic methanogens. The developed technology offers promising commercial benefits by requiring less energy for biohythane production. In addition, it offers environmental advantages by providing an efficient CD waste management alternative and reducing climatic impact by lowering greenhouse gas emissions associated with fossil fuel burning. Using a waste complementarity approach for consortia designing aligns with the principles of circular economy and presents a sustainable, scalable energy solution. The developed method can support the growing energy market by increasing biohythane yield and lowering its production cost.
由于化石燃料占全球能源供应的 83%,并产生大量二氧化碳,世界对化石燃料的依赖性日益增加,已成为一个重大的能源和环境问题。生物乙烷是生物甲烷(5-10%)和生物氢(50-60%)的混合物,正在成为一种从有机废物中提炼出来的前景广阔的环保型替代燃料,并提供了一种可持续的解决方案。现有的生物乙烷生产方法由于采用大量基质预处理来提高生物乙烷产量,因此存在成本高和劳动密集型的主要局限性,从而限制了其工业应用。在这项研究中,我们开发了一种合成微生物联合体(E(C2)Tx),通过将各种有机废物结合在一起,并对其进行热预处理和适应性处理,以分别富集生物产氢菌和甲烷菌,从而实现厌氧消化。生牛粪作为底物与 E(C2)Tx 一起进行厌氧消化,产生了含 3% 生物氢和 36% 生物甲烷的生物沼气。联合体设计策略避免了对大量底物的预处理,只包括对接种物的预处理,而接种物的使用量是底物的四倍。基于 16S rRNA 基因的元基因组分析表明,经 E(C2)Tx 处理的 CD 样品富含纤维素分解菌和产氢菌,以及甲养甲烷菌和氢养甲烷菌。由于生物乙烷生产所需的能源较少,所开发的技术具有良好的商业效益。此外,该技术还具有环境优势,它提供了一种高效的 CD 废物管理替代方法,并通过降低与化石燃料燃烧相关的温室气体排放来减少对气候的影响。使用废物互补法进行联合体设计符合循环经济原则,并提供了一种可持续、可扩展的能源解决方案。所开发的方法可以提高生物乙烷的产量并降低其生产成本,从而支持不断增长的能源市场。
{"title":"Production of biohythane from cow dung using novel microbial synthetic consortia designed by heat-treated and acclimatized combined wastes†","authors":"Rashmi Ira, Vikas Sharma, Shrawan Kumar, Mira Koul, Lalita Sharma, Aditi Halder and Tulika Prakash","doi":"10.1039/D4VA00107A","DOIUrl":"10.1039/D4VA00107A","url":null,"abstract":"<p >The world's increasing dependency on fossil fuels has become a significant energy and environmental concern as they contribute 83% of the global energy supply and produce large amounts of carbon dioxide. Biohythane, a blend of biomethane (5–10%) and biohydrogen (50–60%), is emerging as a promising and environmentally friendly alternative fuel derived from organic wastes and offers a sustainable solution. The existing methods of biohythane production suffer from major limitations of being cost- and labor-intensive due to adopting bulk substrate pretreatment to enhance biohythane yield thereby limiting their industrial applications. In this study, we have developed a synthetic microbial consortium (E(C2)Tx) for anaerobic digestion by combining various organic wastes and subjecting them to heat pre-treatment and acclimatization to enrich biohydrogen producers and methanogens, respectively. Raw cow dung was anaerobically digested as the substrate with E(C2)Tx and this resulted in the production of biohythane with 3% biohydrogen and 36% biomethane. The consortia designing strategy avoided any bulk substrate pretreatment and only included the pretreatment of the inoculum which is used in four times less volume than the substrate. A 16S rRNA gene based metagenomic analysis revealed that the CD samples treated with E(C2)Tx were enriched in cellulolytic and hydrogen-producing <em>Firmicutes</em>, along with methylotrophic and hydrogenotrophic methanogens. The developed technology offers promising commercial benefits by requiring less energy for biohythane production. In addition, it offers environmental advantages by providing an efficient CD waste management alternative and reducing climatic impact by lowering greenhouse gas emissions associated with fossil fuel burning. Using a waste complementarity approach for consortia designing aligns with the principles of circular economy and presents a sustainable, scalable energy solution. The developed method can support the growing energy market by increasing biohythane yield and lowering its production cost.</p>","PeriodicalId":72941,"journal":{"name":"Environmental science. Advances","volume":" 9","pages":" 1289-1308"},"PeriodicalIF":3.5,"publicationDate":"2024-07-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/va/d4va00107a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141866053","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Venu Sreekala Smitha, Parola Athulya, Kazhuthoottil Kochu Jayasooryan and Thoppil Ramakrishnan Resmi
The injected tracer technique using nanoparticles has evoked a lot of research interest in hydrogeological research as it encompasses a broad spectrum of applications in water resource management. The present work deals with developing carbon dot embedded silica-based nanocomposites using a microwave-assisted co-polycondensation method. The synthesized carbon dot-embedded silica nanocomposites have been characterized for their structural and functional characteristics using UV-visible spectroscopy, photoluminescence spectroscopy (PL), lifetime analysis, Raman spectroscopy, Scanning Electron Microscopy (SEM), Transmission Electron Microscopy (TEM), Fourier Transform Infrared spectroscopy (FTIR) and X-ray Diffractometry (XRD). The results obtained showed that carbon dots having a size of less than 5 nm had been successfully embedded into the silica structure, and the nanocomposite as such shows interesting optical properties. Laboratory scale column experimental studies were further conducted to ascertain the applications of the synthesized carbon dot-embedded silica nanocomposite for hydrological studies. Experiments were performed by varying the filling materials (sand/soil) in the column during which different concentrations of the nanotracer were injected under the continuous flow of water at a constant flow rate of 5 ml min−1 followed by monitoring the detection of carbon dots for a definite time. The developed nanocomposite was found to exhibit satisfactory results in terms of the detection and recovery of carbon dots when injected as a tracer in an experimental hydrological study. About 99% of the nano tracer could be regained when ∼0.5 g of the CD-SiO2 nanotracer is injected into the column and the detection was much faster with a peak detection time of 6 minutes. The better traceability and retention of the original optical properties of the developed tracer under different experimental conditions could be attributed to the optimal size of the nanocomposite system. Thus, the current challenges faced in groundwater flow analysis such as huge time consumption/expenses can be resolved to a significant extent considering the better traceability of the developed nanotracer.
{"title":"Fluorescent carbon dot embedded silica nanocomposites as tracers for hydrogeological investigations: a sustainable approach†","authors":"Venu Sreekala Smitha, Parola Athulya, Kazhuthoottil Kochu Jayasooryan and Thoppil Ramakrishnan Resmi","doi":"10.1039/D4VA00156G","DOIUrl":"10.1039/D4VA00156G","url":null,"abstract":"<p >The injected tracer technique using nanoparticles has evoked a lot of research interest in hydrogeological research as it encompasses a broad spectrum of applications in water resource management. The present work deals with developing carbon dot embedded silica-based nanocomposites using a microwave-assisted co-polycondensation method. The synthesized carbon dot-embedded silica nanocomposites have been characterized for their structural and functional characteristics using UV-visible spectroscopy, photoluminescence spectroscopy (PL), lifetime analysis, Raman spectroscopy, Scanning Electron Microscopy (SEM), Transmission Electron Microscopy (TEM), Fourier Transform Infrared spectroscopy (FTIR) and X-ray Diffractometry (XRD). The results obtained showed that carbon dots having a size of less than 5 nm had been successfully embedded into the silica structure, and the nanocomposite as such shows interesting optical properties. Laboratory scale column experimental studies were further conducted to ascertain the applications of the synthesized carbon dot-embedded silica nanocomposite for hydrological studies. Experiments were performed by varying the filling materials (sand/soil) in the column during which different concentrations of the nanotracer were injected under the continuous flow of water at a constant flow rate of 5 ml min<small><sup>−1</sup></small> followed by monitoring the detection of carbon dots for a definite time. The developed nanocomposite was found to exhibit satisfactory results in terms of the detection and recovery of carbon dots when injected as a tracer in an experimental hydrological study. About 99% of the nano tracer could be regained when ∼0.5 g of the CD-SiO<small><sub>2</sub></small> nanotracer is injected into the column and the detection was much faster with a peak detection time of 6 minutes. The better traceability and retention of the original optical properties of the developed tracer under different experimental conditions could be attributed to the optimal size of the nanocomposite system. Thus, the current challenges faced in groundwater flow analysis such as huge time consumption/expenses can be resolved to a significant extent considering the better traceability of the developed nanotracer.</p>","PeriodicalId":72941,"journal":{"name":"Environmental science. Advances","volume":" 10","pages":" 1400-1412"},"PeriodicalIF":3.5,"publicationDate":"2024-07-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/va/d4va00156g?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141866052","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Sandali Panagoda, Pengyi Yuan, Vladimir Pavlovic, John Barber and Younggy Kim
Ammonia recovery from food waste (including its liquid digestate) is highly emphasized in wastewater treatment and management. Among various membrane-based separation technologies, bipolar membrane electrodialysis (BMED) without anion exchange membranes (AEMs) is an attractive candidate for selective ammonia separation with reduced scaling problems. In this study, a bench-scale BMED stack was built using 5 pairs of cation exchange membranes (CEMs) and bipolar membranes (BPMs). A simulated food liquid digestate was treated using a lab-scale BMED stack to examine the ammonia separation with 3 different intermembrane distances (0.82, 1.64, and 2.46 mm). The highest electric current and ammonia separation were obtained for the intermembrane distance of 1.64 mm, while the BMED stack with 3 spacer gaskets (2.46 mm) still showed comparable separation performance without significant decreases in electric current or ammonia recovery. The residual Ca2+ and Mg2+ in the cleaning-in-place (CIP) solutions indicated that there were no noticeable scaling problems during the BMED operation. Finally, the pH polarization between the base and feed cells was found to minimize the ammonia back-diffusion even with the highly accumulated ammonia concentration (>11 000 mgN L−1) in the base cell. With the relatively low energy requirement (1.24–6.78 kW h kgN−1), BMED lacking AEMs with wide intermembrane distances was confirmed to be a sustainable candidate for ammonia recovery from wastewater with high levels of ammonia.
{"title":"Enhancing ammonia recovery through pH polarization in bipolar membrane electrodialysis†","authors":"Sandali Panagoda, Pengyi Yuan, Vladimir Pavlovic, John Barber and Younggy Kim","doi":"10.1039/D4VA00082J","DOIUrl":"10.1039/D4VA00082J","url":null,"abstract":"<p >Ammonia recovery from food waste (including its liquid digestate) is highly emphasized in wastewater treatment and management. Among various membrane-based separation technologies, bipolar membrane electrodialysis (BMED) without anion exchange membranes (AEMs) is an attractive candidate for selective ammonia separation with reduced scaling problems. In this study, a bench-scale BMED stack was built using 5 pairs of cation exchange membranes (CEMs) and bipolar membranes (BPMs). A simulated food liquid digestate was treated using a lab-scale BMED stack to examine the ammonia separation with 3 different intermembrane distances (0.82, 1.64, and 2.46 mm). The highest electric current and ammonia separation were obtained for the intermembrane distance of 1.64 mm, while the BMED stack with 3 spacer gaskets (2.46 mm) still showed comparable separation performance without significant decreases in electric current or ammonia recovery. The residual Ca<small><sup>2+</sup></small> and Mg<small><sup>2+</sup></small> in the cleaning-in-place (CIP) solutions indicated that there were no noticeable scaling problems during the BMED operation. Finally, the pH polarization between the base and feed cells was found to minimize the ammonia back-diffusion even with the highly accumulated ammonia concentration (>11 000 mg<small><sub>N</sub></small> L<small><sup>−1</sup></small>) in the base cell. With the relatively low energy requirement (1.24–6.78 kW h kg<small><sub>N</sub></small><small><sup>−1</sup></small>), BMED lacking AEMs with wide intermembrane distances was confirmed to be a sustainable candidate for ammonia recovery from wastewater with high levels of ammonia.</p>","PeriodicalId":72941,"journal":{"name":"Environmental science. Advances","volume":" 9","pages":" 1309-1316"},"PeriodicalIF":3.5,"publicationDate":"2024-07-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/va/d4va00082j?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141781966","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}