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Brown Carbon in East Asia: Seasonality, Sources, and Influences on Regional Climate and Air Quality. 东亚褐碳:季节性、来源及其对区域气候和空气质量的影响。
IF 6.7
ACS Environmental Au Pub Date : 2024-11-13 eCollection Date: 2025-01-15 DOI: 10.1021/acsenvironau.4c00080
Fan Wang, Zifeng Lu, Guangxing Lin, Gregory R Carmichael, Meng Gao
{"title":"Brown Carbon in East Asia: Seasonality, Sources, and Influences on Regional Climate and Air Quality.","authors":"Fan Wang, Zifeng Lu, Guangxing Lin, Gregory R Carmichael, Meng Gao","doi":"10.1021/acsenvironau.4c00080","DOIUrl":"https://doi.org/10.1021/acsenvironau.4c00080","url":null,"abstract":"<p><p>Brown carbon (BrC) has been recognized as an important light-absorbing carbonaceous aerosol, yet understanding of its influence on regional climate and air quality has been lacking, mainly due to the ignorance of regional coupled meteorology-chemistry models. Besides, assumptions about its emissions in previous explorations might cause large uncertainties in estimates. Here, we implemented a BrC module into the WRF-Chem model that considers source-dependent absorption and avoids uncertainties caused by assumptions about emission intensities. To our best knowledge, we made the first effort to consider BrC in a regional coupled model. We then applied the developed model to explore the impacts of BrC absorption on radiative forcing, regional climate, and air quality in East Asia. We found notable increases in aerosol absorption optical depth (AAOD) in areas with high OC concentrations. The most intense forcing of BrC absorption occurs in autumn over Southeast Asia, and values could reach around 4 W m<sup>-2</sup>. The intensified atmospheric absorption modified surface energy balance, resulting in subsequent declines in surface temperature, heat flux, boundary layer height, and turbulence exchanging rates. These changes in meteorological variables additionally modified near-surface dispersion and photochemical conditions, leading to changes of PM<sub>2.5</sub> and O<sub>3</sub> concentrations. These findings indicate that BrC could exert important influence in specific regions and time periods. A more in-depth understanding could be achieved later with the developed model.</p>","PeriodicalId":29801,"journal":{"name":"ACS Environmental Au","volume":"5 1","pages":"128-137"},"PeriodicalIF":6.7,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11741057/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143012125","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}
引用次数: 0
Brown Carbon in East Asia: Seasonality, Sources, and Influences on Regional Climate and Air Quality 东亚褐碳:季节性、来源及其对区域气候和空气质量的影响
IF 6.7
ACS Environmental Au Pub Date : 2024-11-13 DOI: 10.1021/acsenvironau.4c0008010.1021/acsenvironau.4c00080
Fan Wang, Zifeng Lu, Guangxing Lin, Gregory R. Carmichael and Meng Gao*, 
{"title":"Brown Carbon in East Asia: Seasonality, Sources, and Influences on Regional Climate and Air Quality","authors":"Fan Wang,&nbsp;Zifeng Lu,&nbsp;Guangxing Lin,&nbsp;Gregory R. Carmichael and Meng Gao*,&nbsp;","doi":"10.1021/acsenvironau.4c0008010.1021/acsenvironau.4c00080","DOIUrl":"https://doi.org/10.1021/acsenvironau.4c00080https://doi.org/10.1021/acsenvironau.4c00080","url":null,"abstract":"<p >Brown carbon (BrC) has been recognized as an important light-absorbing carbonaceous aerosol, yet understanding of its influence on regional climate and air quality has been lacking, mainly due to the ignorance of regional coupled meteorology-chemistry models. Besides, assumptions about its emissions in previous explorations might cause large uncertainties in estimates. Here, we implemented a BrC module into the WRF-Chem model that considers source-dependent absorption and avoids uncertainties caused by assumptions about emission intensities. To our best knowledge, we made the first effort to consider BrC in a regional coupled model. We then applied the developed model to explore the impacts of BrC absorption on radiative forcing, regional climate, and air quality in East Asia. We found notable increases in aerosol absorption optical depth (AAOD) in areas with high OC concentrations. The most intense forcing of BrC absorption occurs in autumn over Southeast Asia, and values could reach around 4 W m<sup>–2</sup>. The intensified atmospheric absorption modified surface energy balance, resulting in subsequent declines in surface temperature, heat flux, boundary layer height, and turbulence exchanging rates. These changes in meteorological variables additionally modified near-surface dispersion and photochemical conditions, leading to changes of PM<sub>2.5</sub> and O<sub>3</sub> concentrations. These findings indicate that BrC could exert important influence in specific regions and time periods. A more in-depth understanding could be achieved later with the developed model.</p>","PeriodicalId":29801,"journal":{"name":"ACS Environmental Au","volume":"5 1","pages":"128–137 128–137"},"PeriodicalIF":6.7,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsenvironau.4c00080","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143091526","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}
引用次数: 0
Biogeochemistry of Actinides: Recent Progress and Perspective 锕系元素的生物地球化学:最新进展与展望
IF 6.7
ACS Environmental Au Pub Date : 2024-11-04 DOI: 10.1021/acsenvironau.4c0003710.1021/acsenvironau.4c00037
Gauthier J.-P. Deblonde*, 
{"title":"Biogeochemistry of Actinides: Recent Progress and Perspective","authors":"Gauthier J.-P. Deblonde*,&nbsp;","doi":"10.1021/acsenvironau.4c0003710.1021/acsenvironau.4c00037","DOIUrl":"https://doi.org/10.1021/acsenvironau.4c00037https://doi.org/10.1021/acsenvironau.4c00037","url":null,"abstract":"<p >Actinides are elements that are often feared because of their radioactive nature and potentially devastating consequences to humans and the environment if not managed properly. As such, their chemical interactions with the biosphere and geochemical environment, i.e., their “biogeochemistry,” must be studied and understood in detail. In this Review, a summary of the past discoveries and recent advances in the field of actinide biogeochemistry is provided with a particular emphasis on actinides other than thorium and uranium (i.e., actinium, neptunium, plutonium, americium, curium, berkelium, and californium) as they originate from anthropogenic activities and can be mobile in the environment. The nuclear properties of actinide isotopes found in the environment and used in research are reviewed with historical context. Then, the coordination chemistry properties of actinide ions are contrasted with those of common metal ions naturally present in the environment. The typical chelators that can impact the biogeochemistry of actinides are then reviewed. Then, the role of metalloproteins in the biogeochemistry of actinides is put into perspective since recent advances in the field may have ramifications in radiochemistry and for the long-term management of nuclear waste. Metalloproteins are ubiquitous ligands in nature but, as discussed in this Review, they have largely been overlooked for actinide chemistry, especially when compared to traditional environmental chelators. Without discounting the importance of abundant and natural actinide ions (i.e., Th<sup>4+</sup> and UO<sub>2</sub><sup>2+</sup>), the main focus of this review is on trivalent actinides because of their prevalence in the fields of nuclear fuel cycles, radioactive waste management, heavy element research, and, more recently, nuclear medicine. Additionally, trivalent actinides share chemical similarities with the rare earth elements, and recent breakthroughs in the field of lanthanide-binding chelators may spill into the field of actinide biogeochemistry, as discussed hereafter.</p>","PeriodicalId":29801,"journal":{"name":"ACS Environmental Au","volume":"4 6","pages":"292–306 292–306"},"PeriodicalIF":6.7,"publicationDate":"2024-11-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsenvironau.4c00037","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142671338","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}
引用次数: 0
Biogeochemistry of Actinides: Recent Progress and Perspective. 锕系元素的生物地球化学:最新进展与展望》。
IF 6.7
ACS Environmental Au Pub Date : 2024-11-04 eCollection Date: 2024-11-20 DOI: 10.1021/acsenvironau.4c00037
Gauthier J-P Deblonde
{"title":"Biogeochemistry of Actinides: Recent Progress and Perspective.","authors":"Gauthier J-P Deblonde","doi":"10.1021/acsenvironau.4c00037","DOIUrl":"10.1021/acsenvironau.4c00037","url":null,"abstract":"<p><p>Actinides are elements that are often feared because of their radioactive nature and potentially devastating consequences to humans and the environment if not managed properly. As such, their chemical interactions with the biosphere and geochemical environment, i.e., their \"biogeochemistry,\" must be studied and understood in detail. In this Review, a summary of the past discoveries and recent advances in the field of actinide biogeochemistry is provided with a particular emphasis on actinides other than thorium and uranium (i.e., actinium, neptunium, plutonium, americium, curium, berkelium, and californium) as they originate from anthropogenic activities and can be mobile in the environment. The nuclear properties of actinide isotopes found in the environment and used in research are reviewed with historical context. Then, the coordination chemistry properties of actinide ions are contrasted with those of common metal ions naturally present in the environment. The typical chelators that can impact the biogeochemistry of actinides are then reviewed. Then, the role of metalloproteins in the biogeochemistry of actinides is put into perspective since recent advances in the field may have ramifications in radiochemistry and for the long-term management of nuclear waste. Metalloproteins are ubiquitous ligands in nature but, as discussed in this Review, they have largely been overlooked for actinide chemistry, especially when compared to traditional environmental chelators. Without discounting the importance of abundant and natural actinide ions (i.e., Th<sup>4+</sup> and UO<sub>2</sub> <sup>2+</sup>), the main focus of this review is on trivalent actinides because of their prevalence in the fields of nuclear fuel cycles, radioactive waste management, heavy element research, and, more recently, nuclear medicine. Additionally, trivalent actinides share chemical similarities with the rare earth elements, and recent breakthroughs in the field of lanthanide-binding chelators may spill into the field of actinide biogeochemistry, as discussed hereafter.</p>","PeriodicalId":29801,"journal":{"name":"ACS Environmental Au","volume":"4 6","pages":"292-306"},"PeriodicalIF":6.7,"publicationDate":"2024-11-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11583103/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142711028","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}
引用次数: 0
Systematic Review and Spatiotemporal Assessment of Mercury Concentration in Fish from the Tapajós River Basin: Implications for Environmental and Human Health. Tapajós河流域鱼类汞浓度的系统评价和时空评价:对环境和人类健康的影响。
IF 6.7
ACS Environmental Au Pub Date : 2024-10-30 eCollection Date: 2025-01-15 DOI: 10.1021/acsenvironau.4c00053
Karen L Auzier Guimarães, Sarah J do Nascimento Andrade, Ahieska A Liscano-Carreño, Ricardo B de Oliveira, Luís R Ribeiro Rodrigues
{"title":"Systematic Review and Spatiotemporal Assessment of Mercury Concentration in Fish from the Tapajós River Basin: Implications for Environmental and Human Health.","authors":"Karen L Auzier Guimarães, Sarah J do Nascimento Andrade, Ahieska A Liscano-Carreño, Ricardo B de Oliveira, Luís R Ribeiro Rodrigues","doi":"10.1021/acsenvironau.4c00053","DOIUrl":"10.1021/acsenvironau.4c00053","url":null,"abstract":"<p><p>This study reviews the literature on mercury (Hg) pollution in the Tapajós River basin from 1992 to 2022, focusing on the bioaccumulation in fish and the associated health risks to humans via ingesting contaminated species. Variability in Hg bioaccumulation was analyzed from both spatial (sub-basins) and ecological (trophic levels) perspectives. Mercury concentrations in fish muscle tissue and spatial differences in Hg levels were analyzed using nonparametric Kruskal-Wallis ANOVA and mapped with Inverse Distance Weighting. Additionally, a risk assessment of mercury contamination was conducted using the Target Hazard Quotient (THQ) and Maximum Safe Consuming Quantity (MSCQ) indices. Results indicate that Hg contamination is pervasive across the basin, with piscivorous fish showing the highest Hg levels, particularly in the middle Tapajós, upper Tapajs óand Teles Pires sub-basins, identified as contamination hotspots. Piscivorous species exhibited high Target Hazard Quotients (THQ), suggesting health risks for local consumers. The MSCQ values indicated that 75% of the fish species analyzed should be consumed in quantities lower than the current consumption daily average to avoid health risks.</p>","PeriodicalId":29801,"journal":{"name":"ACS Environmental Au","volume":"5 1","pages":"86-100"},"PeriodicalIF":6.7,"publicationDate":"2024-10-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11741060/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143012808","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}
引用次数: 0
Systematic Review and Spatiotemporal Assessment of Mercury Concentration in Fish from the Tapajós River Basin: Implications for Environmental and Human Health Tapajós河流域鱼类汞浓度的系统评价和时空评价:对环境和人类健康的影响
IF 6.7
ACS Environmental Au Pub Date : 2024-10-30 DOI: 10.1021/acsenvironau.4c0005310.1021/acsenvironau.4c00053
Karen L. Auzier Guimarães*, Sarah J. do Nascimento Andrade, Ahieska A. Liscano-Carreño, Ricardo B. de Oliveira and Luís R. Ribeiro Rodrigues, 
{"title":"Systematic Review and Spatiotemporal Assessment of Mercury Concentration in Fish from the Tapajós River Basin: Implications for Environmental and Human Health","authors":"Karen L. Auzier Guimarães*,&nbsp;Sarah J. do Nascimento Andrade,&nbsp;Ahieska A. Liscano-Carreño,&nbsp;Ricardo B. de Oliveira and Luís R. Ribeiro Rodrigues,&nbsp;","doi":"10.1021/acsenvironau.4c0005310.1021/acsenvironau.4c00053","DOIUrl":"https://doi.org/10.1021/acsenvironau.4c00053https://doi.org/10.1021/acsenvironau.4c00053","url":null,"abstract":"<p >This study reviews the literature on mercury (Hg) pollution in the Tapajós River basin from 1992 to 2022, focusing on the bioaccumulation in fish and the associated health risks to humans via ingesting contaminated species. Variability in Hg bioaccumulation was analyzed from both spatial (sub-basins) and ecological (trophic levels) perspectives. Mercury concentrations in fish muscle tissue and spatial differences in Hg levels were analyzed using nonparametric Kruskal–Wallis ANOVA and mapped with Inverse Distance Weighting. Additionally, a risk assessment of mercury contamination was conducted using the Target Hazard Quotient (THQ) and Maximum Safe Consuming Quantity (MSCQ) indices. Results indicate that Hg contamination is pervasive across the basin, with piscivorous fish showing the highest Hg levels, particularly in the middle Tapajós, upper Tapajs óand Teles Pires sub-basins, identified as contamination hotspots. Piscivorous species exhibited high Target Hazard Quotients (THQ), suggesting health risks for local consumers. The MSCQ values indicated that 75% of the fish species analyzed should be consumed in quantities lower than the current consumption daily average to avoid health risks.</p>","PeriodicalId":29801,"journal":{"name":"ACS Environmental Au","volume":"5 1","pages":"86–100 86–100"},"PeriodicalIF":6.7,"publicationDate":"2024-10-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsenvironau.4c00053","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143091880","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}
引用次数: 0
Graphene Membrane for Water-Related Environmental Application: A Comprehensive Review and Perspectives. 石墨烯膜在水环境中的应用综述与展望
IF 6.7
ACS Environmental Au Pub Date : 2024-10-16 eCollection Date: 2025-01-15 DOI: 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}
引用次数: 0
Graphene Membrane for Water-Related Environmental Application: A Comprehensive Review and Perspectives 石墨烯膜在水环境中的应用综述与展望
IF 6.7
ACS Environmental Au Pub Date : 2024-10-16 DOI: 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,&nbsp;Ohchan Kwon,&nbsp;Jeong Pil Kim,&nbsp;Ju Yeon Kim,&nbsp;Jiwon Kim,&nbsp;Yonghwi Cho and Dae Woo Kim*,&nbsp;","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}
引用次数: 0
Advancing Microbial Electrochemical H2O2 Synthesis by Tailoring the Surface Chemistry of Stereolithography-Derived 3D Pyrolytic Carbon Electrodes 通过调整立体光刻三维热解碳电极的表面化学性质推进微生物电化学 H2O2 合成
IF 6.7
ACS Environmental Au Pub Date : 2024-10-15 DOI: 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,&nbsp;Babak Rezaei,&nbsp;Stephan Sylvest Keller and Yifeng Zhang*,&nbsp;","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}
引用次数: 0
Advancing Microbial Electrochemical H2O2 Synthesis by Tailoring the Surface Chemistry of Stereolithography-Derived 3D Pyrolytic Carbon Electrodes. 通过调整立体光刻三维热解碳电极的表面化学性质推进微生物电化学 H2O2 合成。
IF 6.7
ACS Environmental Au Pub Date : 2024-10-15 eCollection Date: 2024-11-20 DOI: 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}
引用次数: 0
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