ACS Environmental AuPub Date : 2024-10-16eCollection Date: 2025-01-15DOI: 10.1021/acsenvironau.4c00088
Junhyeok Kang, Ohchan Kwon, Jeong Pil Kim, Ju Yeon Kim, Jiwon Kim, Yonghwi Cho, Dae Woo Kim
{"title":"Graphene Membrane for Water-Related Environmental Application: A Comprehensive Review and Perspectives.","authors":"Junhyeok Kang, Ohchan Kwon, Jeong Pil Kim, Ju Yeon Kim, Jiwon Kim, Yonghwi Cho, Dae Woo Kim","doi":"10.1021/acsenvironau.4c00088","DOIUrl":"10.1021/acsenvironau.4c00088","url":null,"abstract":"<p><p>Graphene-based materials can be potentially utilized for separation membranes due to their unique structural properties such as precise molecular sieving by interlayer spacing or pore structure and excellent stability in harsh environmental conditions. Therefore, graphene-based membranes have been extensively demonstrated for various water treatment applications, including desalination, water extraction, and rare metal ion recovery. While most of the utilization has still been limited to the laboratory scale, emerging studies have dealt with scalable approaches to show commercial feasibility. This review summarizes the recent studies on diverse graphene membrane fabrications and their environmental applications related to water-containing conditions in addition to the molecular separation mechanism and critical factors related to graphene membrane performance. Additionally, we discuss future perspectives and challenges to provide insights into the practical applications of graphene-based membranes on the industrial scale.</p>","PeriodicalId":29801,"journal":{"name":"ACS Environmental Au","volume":"5 1","pages":"35-60"},"PeriodicalIF":6.7,"publicationDate":"2024-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11741062/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143012825","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}
ACS Environmental AuPub Date : 2024-10-16DOI: 10.1021/acsenvironau.4c0008810.1021/acsenvironau.4c00088
Junhyeok Kang, Ohchan Kwon, Jeong Pil Kim, Ju Yeon Kim, Jiwon Kim, Yonghwi Cho and Dae Woo Kim*,
{"title":"Graphene Membrane for Water-Related Environmental Application: A Comprehensive Review and Perspectives","authors":"Junhyeok Kang, Ohchan Kwon, Jeong Pil Kim, Ju Yeon Kim, Jiwon Kim, Yonghwi Cho and Dae Woo Kim*, ","doi":"10.1021/acsenvironau.4c0008810.1021/acsenvironau.4c00088","DOIUrl":"https://doi.org/10.1021/acsenvironau.4c00088https://doi.org/10.1021/acsenvironau.4c00088","url":null,"abstract":"<p >Graphene-based materials can be potentially utilized for separation membranes due to their unique structural properties such as precise molecular sieving by interlayer spacing or pore structure and excellent stability in harsh environmental conditions. Therefore, graphene-based membranes have been extensively demonstrated for various water treatment applications, including desalination, water extraction, and rare metal ion recovery. While most of the utilization has still been limited to the laboratory scale, emerging studies have dealt with scalable approaches to show commercial feasibility. This review summarizes the recent studies on diverse graphene membrane fabrications and their environmental applications related to water-containing conditions in addition to the molecular separation mechanism and critical factors related to graphene membrane performance. Additionally, we discuss future perspectives and challenges to provide insights into the practical applications of graphene-based membranes on the industrial scale.</p>","PeriodicalId":29801,"journal":{"name":"ACS Environmental Au","volume":"5 1","pages":"35–60 35–60"},"PeriodicalIF":6.7,"publicationDate":"2024-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsenvironau.4c00088","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143091751","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}
ACS Environmental AuPub Date : 2024-10-15DOI: 10.1021/acsenvironau.4c0006710.1021/acsenvironau.4c00067
Rusen Zou, Babak Rezaei, Stephan Sylvest Keller and Yifeng Zhang*,
{"title":"Advancing Microbial Electrochemical H2O2 Synthesis by Tailoring the Surface Chemistry of Stereolithography-Derived 3D Pyrolytic Carbon Electrodes","authors":"Rusen Zou, Babak Rezaei, Stephan Sylvest Keller and Yifeng Zhang*, ","doi":"10.1021/acsenvironau.4c0006710.1021/acsenvironau.4c00067","DOIUrl":"https://doi.org/10.1021/acsenvironau.4c00067https://doi.org/10.1021/acsenvironau.4c00067","url":null,"abstract":"<p >Microbial electrosynthesis of H<sub>2</sub>O<sub>2</sub> offers an economical and eco-friendly alternative to the costly and environmentally detrimental anthraquinone process. Three-dimensional (3D) electrodes fabricated through additive manufacturing demonstrate significant advantages over carbon electrodes with two-dimensional (2D) surfaces in microbial electrosynthesis of H<sub>2</sub>O<sub>2</sub>. Nevertheless, the presence of oxygen-containing free acidic groups on the prototype electrode surface imparts hydrophilic properties to the electrode, which affects the efficiency of the two-electron oxygen reduction reaction for H<sub>2</sub>O<sub>2</sub> generation. In this study, we elucidated that the efficiency of microbial H<sub>2</sub>O<sub>2</sub> synthesis is markedly enhanced by utilizing oxygen-free 3D electrodes produced via additive manufacturing techniques followed by surface modifications to eradicate oxygen-containing functional groups. These oxygen-free 3D electrodes exhibit superior hydrophobicity compared to traditional carbon electrodes with 2D surfaces and their 3D printed analogues. The oxygen-free 3D electrode is capable of generating up to 130.2 mg L<sup>–1</sup> of H<sub>2</sub>O<sub>2</sub> within a 6-h time frame, which is 2.4 to 13.6 times more effective than conventional electrodes (such as graphite plates) and pristine 3D printed electrodes. Additionally, the reusability of the oxygen-free 3D electrode underscores its practical viability for large-scale applications. Furthermore, this investigation explored the role of the oxygen-free 3D electrode in the bioelectro-Fenton process, affirming its efficacy as a tertiary treatment technology for the elimination of micropollutants. This dual functionality accentuates the versatility of the oxygen-free 3D electrode in facilitating both the synthesis of valuable chemicals and advancing environmental remediation. This research introduces an innovative electrode design that fosters efficient and sustainable H<sub>2</sub>O<sub>2</sub> synthesis while concurrently enabling subsequent environmental restoration.</p>","PeriodicalId":29801,"journal":{"name":"ACS Environmental Au","volume":"4 6","pages":"344–353 344–353"},"PeriodicalIF":6.7,"publicationDate":"2024-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsenvironau.4c00067","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142671843","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}
ACS Environmental AuPub Date : 2024-10-15eCollection Date: 2024-11-20DOI: 10.1021/acsenvironau.4c00067
Rusen Zou, Babak Rezaei, Stephan Sylvest Keller, Yifeng Zhang
{"title":"Advancing Microbial Electrochemical H<sub>2</sub>O<sub>2</sub> Synthesis by Tailoring the Surface Chemistry of Stereolithography-Derived 3D Pyrolytic Carbon Electrodes.","authors":"Rusen Zou, Babak Rezaei, Stephan Sylvest Keller, Yifeng Zhang","doi":"10.1021/acsenvironau.4c00067","DOIUrl":"10.1021/acsenvironau.4c00067","url":null,"abstract":"<p><p>Microbial electrosynthesis of H<sub>2</sub>O<sub>2</sub> offers an economical and eco-friendly alternative to the costly and environmentally detrimental anthraquinone process. Three-dimensional (3D) electrodes fabricated through additive manufacturing demonstrate significant advantages over carbon electrodes with two-dimensional (2D) surfaces in microbial electrosynthesis of H<sub>2</sub>O<sub>2</sub>. Nevertheless, the presence of oxygen-containing free acidic groups on the prototype electrode surface imparts hydrophilic properties to the electrode, which affects the efficiency of the two-electron oxygen reduction reaction for H<sub>2</sub>O<sub>2</sub> generation. In this study, we elucidated that the efficiency of microbial H<sub>2</sub>O<sub>2</sub> synthesis is markedly enhanced by utilizing oxygen-free 3D electrodes produced via additive manufacturing techniques followed by surface modifications to eradicate oxygen-containing functional groups. These oxygen-free 3D electrodes exhibit superior hydrophobicity compared to traditional carbon electrodes with 2D surfaces and their 3D printed analogues. The oxygen-free 3D electrode is capable of generating up to 130.2 mg L<sup>-1</sup> of H<sub>2</sub>O<sub>2</sub> within a 6-h time frame, which is 2.4 to 13.6 times more effective than conventional electrodes (such as graphite plates) and pristine 3D printed electrodes. Additionally, the reusability of the oxygen-free 3D electrode underscores its practical viability for large-scale applications. Furthermore, this investigation explored the role of the oxygen-free 3D electrode in the bioelectro-Fenton process, affirming its efficacy as a tertiary treatment technology for the elimination of micropollutants. This dual functionality accentuates the versatility of the oxygen-free 3D electrode in facilitating both the synthesis of valuable chemicals and advancing environmental remediation. This research introduces an innovative electrode design that fosters efficient and sustainable H<sub>2</sub>O<sub>2</sub> synthesis while concurrently enabling subsequent environmental restoration.</p>","PeriodicalId":29801,"journal":{"name":"ACS Environmental Au","volume":"4 6","pages":"344-353"},"PeriodicalIF":6.7,"publicationDate":"2024-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11583100/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142710965","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}
ACS Environmental AuPub Date : 2024-10-14eCollection Date: 2024-11-20DOI: 10.1021/acsenvironau.4c00076
Amthal Al-Gailani, Martin J Taylor, Muhammad Hashir Zaheer, Richard Barker
{"title":"Evaluation of Natural Organic Additives as Eco-friendly Inhibitors for Calcium and Magnesium Scale Formation in Water Systems.","authors":"Amthal Al-Gailani, Martin J Taylor, Muhammad Hashir Zaheer, Richard Barker","doi":"10.1021/acsenvironau.4c00076","DOIUrl":"10.1021/acsenvironau.4c00076","url":null,"abstract":"<p><p>Mineral scale formation reduces the heat transfer efficiency and clogs pipes and valves, increasing power consumption. To address the environmental concerns of conventional scale inhibitors, this paper explores biodegradable and eco-friendly alternatives. It examines the effects of organic additives on calcium (Ca) and magnesium (Mg) scaling in water vaporization. Batch experiments were conducted with potable water and various organic molecules (saponin, caffeine, tannic acid, dextran, citrus pectin, Ficoll 400, and Triton X-100). Saponin showed the highest calcium scale inhibition efficiency (60.9%) followed by caffeine (49.6%) and tannic acid (39.6%), while Ficoll 400, pectin, and Triton X-100 were less effective. For the magnesium scale, caffeine was the most effective (97.4%) followed by saponin (88.6%) and tannic acid (67.1%). Inhibition efficiencies for magnesium-containing scales were generally higher than those for calcium scales. Regarding the inhibition mechanisms, saponin, caffeine, dextran, and tannic acid adsorbed onto mineral crystal growth sites according to the Langmuir model, while pectin, Triton X-100, and Ficoll 400 formed complexes with Ca<sup>2+</sup> and Mg<sup>2+</sup> in solution. Needle-like aragonite was the predominant form of calcium carbonate (CaCO<sub>3</sub>) with the most additives, except tannic acid, which produced rhombohedral calcite, and caffeine, which promoted flower-like vaterite CaCO<sub>3</sub> crystallites. Saponin, caffeine, tannic acid, and dextran are effective, biodegradable, and environmentally friendly inhibitors for mineral scaling.</p>","PeriodicalId":29801,"journal":{"name":"ACS Environmental Au","volume":"4 6","pages":"354-365"},"PeriodicalIF":6.7,"publicationDate":"2024-10-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11583101/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142711136","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}
ACS Environmental AuPub Date : 2024-10-14DOI: 10.1021/acsenvironau.4c0007610.1021/acsenvironau.4c00076
Amthal Al-Gailani*, Martin J. Taylor, Muhammad Hashir Zaheer and Richard Barker,
{"title":"Evaluation of Natural Organic Additives as Eco-friendly Inhibitors for Calcium and Magnesium Scale Formation in Water Systems","authors":"Amthal Al-Gailani*, Martin J. Taylor, Muhammad Hashir Zaheer and Richard Barker, ","doi":"10.1021/acsenvironau.4c0007610.1021/acsenvironau.4c00076","DOIUrl":"https://doi.org/10.1021/acsenvironau.4c00076https://doi.org/10.1021/acsenvironau.4c00076","url":null,"abstract":"<p >Mineral scale formation reduces the heat transfer efficiency and clogs pipes and valves, increasing power consumption. To address the environmental concerns of conventional scale inhibitors, this paper explores biodegradable and eco-friendly alternatives. It examines the effects of organic additives on calcium (Ca) and magnesium (Mg) scaling in water vaporization. Batch experiments were conducted with potable water and various organic molecules (saponin, caffeine, tannic acid, dextran, citrus pectin, Ficoll 400, and Triton X-100). Saponin showed the highest calcium scale inhibition efficiency (60.9%) followed by caffeine (49.6%) and tannic acid (39.6%), while Ficoll 400, pectin, and Triton X-100 were less effective. For the magnesium scale, caffeine was the most effective (97.4%) followed by saponin (88.6%) and tannic acid (67.1%). Inhibition efficiencies for magnesium-containing scales were generally higher than those for calcium scales. Regarding the inhibition mechanisms, saponin, caffeine, dextran, and tannic acid adsorbed onto mineral crystal growth sites according to the Langmuir model, while pectin, Triton X-100, and Ficoll 400 formed complexes with Ca<sup>2+</sup> and Mg<sup>2+</sup> in solution. Needle-like aragonite was the predominant form of calcium carbonate (CaCO<sub>3</sub>) with the most additives, except tannic acid, which produced rhombohedral calcite, and caffeine, which promoted flower-like vaterite CaCO<sub>3</sub> crystallites. Saponin, caffeine, tannic acid, and dextran are effective, biodegradable, and environmentally friendly inhibitors for mineral scaling.</p>","PeriodicalId":29801,"journal":{"name":"ACS Environmental Au","volume":"4 6","pages":"354–365 354–365"},"PeriodicalIF":6.7,"publicationDate":"2024-10-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsenvironau.4c00076","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142671840","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}
ACS Environmental AuPub Date : 2024-09-30eCollection Date: 2024-11-20DOI: 10.1021/acsenvironau.4c00057
Shinyun Park, Xitong Liu, Tianshu Li, Joshua L Livingston, Jin Zhang, Tiezheng Tong
{"title":"Protein-Decorated Reverse Osmosis Membranes with High Gypsum Scaling Resistance.","authors":"Shinyun Park, Xitong Liu, Tianshu Li, Joshua L Livingston, Jin Zhang, Tiezheng Tong","doi":"10.1021/acsenvironau.4c00057","DOIUrl":"10.1021/acsenvironau.4c00057","url":null,"abstract":"<p><p>The global challenge of water scarcity has fueled significant interest in membrane desalination, particularly reverse osmosis (RO), for producing fresh water from various unconventional sources. However, mineral scaling remains a critical issue that compromises the membrane efficiency and lifespan. This study explores the use of naturally occurring proteins to develop scaling-resistant RO membranes through an eco-friendly modification method. We systematically evaluate three protein modification techniques, namely, polydopamine (PDA)-assisted coating, protein conditioning, and protein drying, for fabricating membranes resistant to gypsum scaling. Protein conditioning is found to be the most effective approach, resulting in protein-decorated membranes with an exceptional resistance to gypsum scaling. We also demonstrate that a hydrated protein layer is essential for optimal scaling resistance. To further understand the mechanism underlying the scaling resistance of protein-decorated membranes, five proteins (i.e., bovine serum albumin, casein, lactalbumin, lysozyme, and protamine) with distinct physicochemical properties are used to explore the key factors governing membrane scaling resistance. The results of dynamic RO experiments indicate that the molecular weight of proteins plays a crucial role, with higher molecular weights leading to higher membrane scaling resistance through steric effects. However, static experiments of bulk crystallization highlight the importance of electrostatic interactions, where proteins with more negative charge delay gypsum crystallization more effectively. These findings suggest the difference between gypsum scaling in the RO and gypsum crystallization in bulk solutions. Overall, this research offers a novel approach to developing resilient and sustainable RO membranes for the desalination of feedwater with high scaling potential while elucidating mechanistic insights on the mitigating effects of protein on gypsum scaling.</p>","PeriodicalId":29801,"journal":{"name":"ACS Environmental Au","volume":"4 6","pages":"333-343"},"PeriodicalIF":6.7,"publicationDate":"2024-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11583097/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142711138","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}
ACS Environmental AuPub Date : 2024-09-29DOI: 10.1021/acsenvironau.4c0005710.1021/acsenvironau.4c00057
Shinyun Park, Xitong Liu, Tianshu Li, Joshua L. Livingston, Jin Zhang and Tiezheng Tong*,
{"title":"Protein-Decorated Reverse Osmosis Membranes with High Gypsum Scaling Resistance","authors":"Shinyun Park, Xitong Liu, Tianshu Li, Joshua L. Livingston, Jin Zhang and Tiezheng Tong*, ","doi":"10.1021/acsenvironau.4c0005710.1021/acsenvironau.4c00057","DOIUrl":"https://doi.org/10.1021/acsenvironau.4c00057https://doi.org/10.1021/acsenvironau.4c00057","url":null,"abstract":"<p >The global challenge of water scarcity has fueled significant interest in membrane desalination, particularly reverse osmosis (RO), for producing fresh water from various unconventional sources. However, mineral scaling remains a critical issue that compromises the membrane efficiency and lifespan. This study explores the use of naturally occurring proteins to develop scaling-resistant RO membranes through an eco-friendly modification method. We systematically evaluate three protein modification techniques, namely, polydopamine (PDA)-assisted coating, protein conditioning, and protein drying, for fabricating membranes resistant to gypsum scaling. Protein conditioning is found to be the most effective approach, resulting in protein-decorated membranes with an exceptional resistance to gypsum scaling. We also demonstrate that a hydrated protein layer is essential for optimal scaling resistance. To further understand the mechanism underlying the scaling resistance of protein-decorated membranes, five proteins (i.e., bovine serum albumin, casein, lactalbumin, lysozyme, and protamine) with distinct physicochemical properties are used to explore the key factors governing membrane scaling resistance. The results of dynamic RO experiments indicate that the molecular weight of proteins plays a crucial role, with higher molecular weights leading to higher membrane scaling resistance through steric effects. However, static experiments of bulk crystallization highlight the importance of electrostatic interactions, where proteins with more negative charge delay gypsum crystallization more effectively. These findings suggest the difference between gypsum scaling in the RO and gypsum crystallization in bulk solutions. Overall, this research offers a novel approach to developing resilient and sustainable RO membranes for the desalination of feedwater with high scaling potential while elucidating mechanistic insights on the mitigating effects of protein on gypsum scaling.</p>","PeriodicalId":29801,"journal":{"name":"ACS Environmental Au","volume":"4 6","pages":"333–343 333–343"},"PeriodicalIF":6.7,"publicationDate":"2024-09-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsenvironau.4c00057","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142674032","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}
Daisy N. Grace, Matthew N. Newmeyer, Carsten Prasse
{"title":"Solid-Phase Reactivity-Directed Extraction (SPREx): An Alternative Approach for Simultaneous Extraction, Identification, and Prioritization of Toxic Electrophiles Produced in Water Treatment Applications","authors":"Daisy N. Grace, Matthew N. Newmeyer, Carsten Prasse","doi":"10.1021/acsenvironau.4c00025","DOIUrl":"https://doi.org/10.1021/acsenvironau.4c00025","url":null,"abstract":"Current strategies to assess water quality are ineffective at prioritizing the most toxic chemicals within a treated water sample. Although it is well known that oxidation byproducts (OBPs) from water treatment processes (e.g., chlorination and ozonation) are linked to adverse health outcomes such as skin diseases, reproductive toxicity, and various cancers, we are still unable to account for a large fraction of the toxicity drivers. Previous approaches utilize <i>in vitro</i> or <i>in vivo</i> assays to assess OBPs on an individual basis, which is too time- and resource-intensive considering the countless number of transformation byproducts of unknown toxicities that exist in treated waters. <i>In vitro</i> assays have also been developed to analyze the toxicity of OBPs in environmental mixtures, but these approaches do not provide identification information about the responsible toxicants. Furthermore, an additional challenge for OBP detection arises during the extraction and detection stages of analysis, as certain OBPs are typically lost using traditional extraction methods or are not detectable via liquid-chromatography–high-resolution mass spectrometry (LC-HRMS) without derivatization. To address these issues, we have developed the analytical assay <u><b>S</b></u>olid-<u><b>P</b></u>hase <u><b>R</b></u>eactivity-directed <u><b>Ex</b></u>traction (SPREx), which aims to provide an all-in-one evaluation for (i) <i>in chemico</i> toxicity screening, (ii) extraction, (iii) detection, and (iv) identification via LC-HRMS. The performance of SPREx was evaluated by testing different nucleophile probes for the capture and detection of 24 different carbonyl compounds, which serve as model electrophiles and are known OBPs that provide unique extraction and detection challenges. SPREx provided distinct advantages for extraction recoveries and was an effective screening tool for carbonyl detection and quantification in complex water matrices such as drinking water and wastewater.","PeriodicalId":29801,"journal":{"name":"ACS Environmental Au","volume":"6 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-09-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142253580","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Environmental AuPub Date : 2024-09-20DOI: 10.1021/acsenvironau.4c0002510.1021/acsenvironau.4c00025
Daisy N. Grace, Matthew N. Newmeyer and Carsten Prasse*,
{"title":"Solid-Phase Reactivity-Directed Extraction (SPREx): An Alternative Approach for Simultaneous Extraction, Identification, and Prioritization of Toxic Electrophiles Produced in Water Treatment Applications","authors":"Daisy N. Grace, Matthew N. Newmeyer and Carsten Prasse*, ","doi":"10.1021/acsenvironau.4c0002510.1021/acsenvironau.4c00025","DOIUrl":"https://doi.org/10.1021/acsenvironau.4c00025https://doi.org/10.1021/acsenvironau.4c00025","url":null,"abstract":"<p >Current strategies to assess water quality are ineffective at prioritizing the most toxic chemicals within a treated water sample. Although it is well known that oxidation byproducts (OBPs) from water treatment processes (e.g., chlorination and ozonation) are linked to adverse health outcomes such as skin diseases, reproductive toxicity, and various cancers, we are still unable to account for a large fraction of the toxicity drivers. Previous approaches utilize <i>in vitro</i> or <i>in vivo</i> assays to assess OBPs on an individual basis, which is too time- and resource-intensive considering the countless number of transformation byproducts of unknown toxicities that exist in treated waters. <i>In vitro</i> assays have also been developed to analyze the toxicity of OBPs in environmental mixtures, but these approaches do not provide identification information about the responsible toxicants. Furthermore, an additional challenge for OBP detection arises during the extraction and detection stages of analysis, as certain OBPs are typically lost using traditional extraction methods or are not detectable via liquid-chromatography–high-resolution mass spectrometry (LC-HRMS) without derivatization. To address these issues, we have developed the analytical assay <u><b>S</b></u>olid-<u><b>P</b></u>hase <u><b>R</b></u>eactivity-directed <u><b>Ex</b></u>traction (SPREx), which aims to provide an all-in-one evaluation for (i) <i>in chemico</i> toxicity screening, (ii) extraction, (iii) detection, and (iv) identification via LC-HRMS. The performance of SPREx was evaluated by testing different nucleophile probes for the capture and detection of 24 different carbonyl compounds, which serve as model electrophiles and are known OBPs that provide unique extraction and detection challenges. SPREx provided distinct advantages for extraction recoveries and was an effective screening tool for carbonyl detection and quantification in complex water matrices such as drinking water and wastewater.</p>","PeriodicalId":29801,"journal":{"name":"ACS Environmental Au","volume":"4 6","pages":"317–332 317–332"},"PeriodicalIF":6.7,"publicationDate":"2024-09-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsenvironau.4c00025","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142671932","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}