Pretreatment of lignocellulosic biomass is crucial yet challenging for sustainable energy production. This study focuses on enhancing enzymatic accessibility of cellulose in oil palm empty fruit bunches by optimizing pretreatment parameters to improve glucose and ethanol yields while reducing fermentation inhibitors. It evaluates the impact of maleic acid concentrations on biorefinery processes. High maleic acid concentrations (>25% w/w) may allow reuse and offer benefits over lower concentrations, such as enhanced delignification and increased sugar yield under milder conditions. Biomass undergoes pretreatment, enzymatic saccharification, and fermentation using Saccharomyces cerevisiae F118. Pretreatment with 75% maleic acid (w/w) for 60 min at 180 °C effectively removes lignin and hemicellulose, increasing cellulose accessibility but results in 74.8% crystallinity, hindering saccharification. A 50% maleic acid pretreatment yielded higher glucose (77.1%). Optimal ethanol production is achieved with 1% maleic acid pretreatment. However, the ethanol yield is negatively impacted by residual maleic acid on the solid matrix.
{"title":"Maleic Acid-Butanol Pretreatment to Enhance Cellulose Accessibility for Enzymatic Hydrolysis and Ethanol Production from Oil Palm Empty Fruit Bunch.","authors":"Annaëlle Postiaux, Filemon Jalu Nusantara Putra, Prihardi Kahar, Aurore Richel, Chiaki Ogino","doi":"10.1021/acsenvironau.4c00045","DOIUrl":"10.1021/acsenvironau.4c00045","url":null,"abstract":"<p><p>Pretreatment of lignocellulosic biomass is crucial yet challenging for sustainable energy production. This study focuses on enhancing enzymatic accessibility of cellulose in oil palm empty fruit bunches by optimizing pretreatment parameters to improve glucose and ethanol yields while reducing fermentation inhibitors. It evaluates the impact of maleic acid concentrations on biorefinery processes. High maleic acid concentrations (>25% w/w) may allow reuse and offer benefits over lower concentrations, such as enhanced delignification and increased sugar yield under milder conditions. Biomass undergoes pretreatment, enzymatic saccharification, and fermentation using <i>Saccharomyces cerevisiae</i> F118. Pretreatment with 75% maleic acid (w/w) for 60 min at 180 °C effectively removes lignin and hemicellulose, increasing cellulose accessibility but results in 74.8% crystallinity, hindering saccharification. A 50% maleic acid pretreatment yielded higher glucose (77.1%). Optimal ethanol production is achieved with 1% maleic acid pretreatment. However, the ethanol yield is negatively impacted by residual maleic acid on the solid matrix.</p>","PeriodicalId":29801,"journal":{"name":"ACS Environmental Au","volume":"5 1","pages":"76-85"},"PeriodicalIF":6.7,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11741055/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143012749","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}
Pretreatment of lignocellulosic biomass is crucial yet challenging for sustainable energy production. This study focuses on enhancing enzymatic accessibility of cellulose in oil palm empty fruit bunches by optimizing pretreatment parameters to improve glucose and ethanol yields while reducing fermentation inhibitors. It evaluates the impact of maleic acid concentrations on biorefinery processes. High maleic acid concentrations (>25% w/w) may allow reuse and offer benefits over lower concentrations, such as enhanced delignification and increased sugar yield under milder conditions. Biomass undergoes pretreatment, enzymatic saccharification, and fermentation using Saccharomyces cerevisiae F118. Pretreatment with 75% maleic acid (w/w) for 60 min at 180 °C effectively removes lignin and hemicellulose, increasing cellulose accessibility but results in 74.8% crystallinity, hindering saccharification. A 50% maleic acid pretreatment yielded higher glucose (77.1%). Optimal ethanol production is achieved with 1% maleic acid pretreatment. However, the ethanol yield is negatively impacted by residual maleic acid on the solid matrix.
{"title":"Maleic Acid-Butanol Pretreatment to Enhance Cellulose Accessibility for Enzymatic Hydrolysis and Ethanol Production from Oil Palm Empty Fruit Bunch","authors":"Annaëlle Postiaux*, Filemon Jalu Nusantara Putra, Prihardi Kahar, Aurore Richel and Chiaki Ogino, ","doi":"10.1021/acsenvironau.4c0004510.1021/acsenvironau.4c00045","DOIUrl":"https://doi.org/10.1021/acsenvironau.4c00045https://doi.org/10.1021/acsenvironau.4c00045","url":null,"abstract":"<p >Pretreatment of lignocellulosic biomass is crucial yet challenging for sustainable energy production. This study focuses on enhancing enzymatic accessibility of cellulose in oil palm empty fruit bunches by optimizing pretreatment parameters to improve glucose and ethanol yields while reducing fermentation inhibitors. It evaluates the impact of maleic acid concentrations on biorefinery processes. High maleic acid concentrations (>25% w/w) may allow reuse and offer benefits over lower concentrations, such as enhanced delignification and increased sugar yield under milder conditions. Biomass undergoes pretreatment, enzymatic saccharification, and fermentation using <i>Saccharomyces cerevisiae</i> F118. Pretreatment with 75% maleic acid (w/w) for 60 min at 180 °C effectively removes lignin and hemicellulose, increasing cellulose accessibility but results in 74.8% crystallinity, hindering saccharification. A 50% maleic acid pretreatment yielded higher glucose (77.1%). Optimal ethanol production is achieved with 1% maleic acid pretreatment. However, the ethanol yield is negatively impacted by residual maleic acid on the solid matrix.</p>","PeriodicalId":29801,"journal":{"name":"ACS Environmental Au","volume":"5 1","pages":"76–85 76–85"},"PeriodicalIF":6.7,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsenvironau.4c00045","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143091591","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}
Pub Date : 2024-11-20DOI: 10.1021/acsenvironau.4c0006110.1021/acsenvironau.4c00061
Ming Yong, Yang Yang, Liangliang Sun, Meng Tang, Zhuyuan Wang, Chao Xing, Jingwei Hou, Min Zheng, Ting Fong May Chui, Zhikao Li* and Zhe Yang*,
The global transition to clean energy technologies has escalated the demand for lithium (Li), a critical component in rechargeable Li-ion batteries, highlighting the urgent need for efficient and sustainable Li+ extraction methods. Nanofiltration (NF)-based separations have emerged as a promising solution, offering selective separation capabilities that could advance resource extraction and recovery. However, an NF-based lithium extraction process differs significantly from conventional water treatment, necessitating a paradigm shift in membrane materials design, performance evaluation metrics, and process optimization. In this review, we first explore the state-of-the-art strategies for NF membrane modifications. Machine learning was employed to identify key parameters influencing Li+ extraction efficiency, enabling the rational design of high-performance membranes. We then delve into the evolution of performance evaluation metrics, transitioning from the traditional permeance-selectivity trade-off to a more relevant focus on Li+ purity and recovery balance. A system-scale analysis considering specific energy consumption, flux distribution uniformity, and system-scale Li+ recovery and purity is presented. The review also examines process integration and synergistic combinations of NF with emerging technologies, such as capacitive deionization. Techno-economic and lifecycle assessments are also discussed to provide insights into the economic viability and environmental sustainability of NF-based Li+ extraction. Finally, we highlight future research directions to bridge the gap between fundamental research and practical applications, aiming to accelerate the development of sustainable and cost-effective Li+ extraction methods.
{"title":"Nanofiltration Membranes for Efficient Lithium Extraction from Salt-Lake Brine: A Critical Review","authors":"Ming Yong, Yang Yang, Liangliang Sun, Meng Tang, Zhuyuan Wang, Chao Xing, Jingwei Hou, Min Zheng, Ting Fong May Chui, Zhikao Li* and Zhe Yang*, ","doi":"10.1021/acsenvironau.4c0006110.1021/acsenvironau.4c00061","DOIUrl":"https://doi.org/10.1021/acsenvironau.4c00061https://doi.org/10.1021/acsenvironau.4c00061","url":null,"abstract":"<p >The global transition to clean energy technologies has escalated the demand for lithium (Li), a critical component in rechargeable Li-ion batteries, highlighting the urgent need for efficient and sustainable Li<sup>+</sup> extraction methods. Nanofiltration (NF)-based separations have emerged as a promising solution, offering selective separation capabilities that could advance resource extraction and recovery. However, an NF-based lithium extraction process differs significantly from conventional water treatment, necessitating a paradigm shift in membrane materials design, performance evaluation metrics, and process optimization. In this review, we first explore the state-of-the-art strategies for NF membrane modifications. Machine learning was employed to identify key parameters influencing Li<sup>+</sup> extraction efficiency, enabling the rational design of high-performance membranes. We then delve into the evolution of performance evaluation metrics, transitioning from the traditional permeance-selectivity trade-off to a more relevant focus on Li<sup>+</sup> purity and recovery balance. A system-scale analysis considering specific energy consumption, flux distribution uniformity, and system-scale Li<sup>+</sup> recovery and purity is presented. The review also examines process integration and synergistic combinations of NF with emerging technologies, such as capacitive deionization. Techno-economic and lifecycle assessments are also discussed to provide insights into the economic viability and environmental sustainability of NF-based Li<sup>+</sup> extraction. Finally, we highlight future research directions to bridge the gap between fundamental research and practical applications, aiming to accelerate the development of sustainable and cost-effective Li<sup>+</sup> extraction methods.</p>","PeriodicalId":29801,"journal":{"name":"ACS Environmental Au","volume":"5 1","pages":"12–34 12–34"},"PeriodicalIF":6.7,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsenvironau.4c00061","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143091695","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}
Pub Date : 2024-11-20eCollection Date: 2025-01-15DOI: 10.1021/acsenvironau.4c00061
Ming Yong, Yang Yang, Liangliang Sun, Meng Tang, Zhuyuan Wang, Chao Xing, Jingwei Hou, Min Zheng, Ting Fong May Chui, Zhikao Li, Zhe Yang
The global transition to clean energy technologies has escalated the demand for lithium (Li), a critical component in rechargeable Li-ion batteries, highlighting the urgent need for efficient and sustainable Li+ extraction methods. Nanofiltration (NF)-based separations have emerged as a promising solution, offering selective separation capabilities that could advance resource extraction and recovery. However, an NF-based lithium extraction process differs significantly from conventional water treatment, necessitating a paradigm shift in membrane materials design, performance evaluation metrics, and process optimization. In this review, we first explore the state-of-the-art strategies for NF membrane modifications. Machine learning was employed to identify key parameters influencing Li+ extraction efficiency, enabling the rational design of high-performance membranes. We then delve into the evolution of performance evaluation metrics, transitioning from the traditional permeance-selectivity trade-off to a more relevant focus on Li+ purity and recovery balance. A system-scale analysis considering specific energy consumption, flux distribution uniformity, and system-scale Li+ recovery and purity is presented. The review also examines process integration and synergistic combinations of NF with emerging technologies, such as capacitive deionization. Techno-economic and lifecycle assessments are also discussed to provide insights into the economic viability and environmental sustainability of NF-based Li+ extraction. Finally, we highlight future research directions to bridge the gap between fundamental research and practical applications, aiming to accelerate the development of sustainable and cost-effective Li+ extraction methods.
{"title":"Nanofiltration Membranes for Efficient Lithium Extraction from Salt-Lake Brine: A Critical Review.","authors":"Ming Yong, Yang Yang, Liangliang Sun, Meng Tang, Zhuyuan Wang, Chao Xing, Jingwei Hou, Min Zheng, Ting Fong May Chui, Zhikao Li, Zhe Yang","doi":"10.1021/acsenvironau.4c00061","DOIUrl":"10.1021/acsenvironau.4c00061","url":null,"abstract":"<p><p>The global transition to clean energy technologies has escalated the demand for lithium (Li), a critical component in rechargeable Li-ion batteries, highlighting the urgent need for efficient and sustainable Li<sup>+</sup> extraction methods. Nanofiltration (NF)-based separations have emerged as a promising solution, offering selective separation capabilities that could advance resource extraction and recovery. However, an NF-based lithium extraction process differs significantly from conventional water treatment, necessitating a paradigm shift in membrane materials design, performance evaluation metrics, and process optimization. In this review, we first explore the state-of-the-art strategies for NF membrane modifications. Machine learning was employed to identify key parameters influencing Li<sup>+</sup> extraction efficiency, enabling the rational design of high-performance membranes. We then delve into the evolution of performance evaluation metrics, transitioning from the traditional permeance-selectivity trade-off to a more relevant focus on Li<sup>+</sup> purity and recovery balance. A system-scale analysis considering specific energy consumption, flux distribution uniformity, and system-scale Li<sup>+</sup> recovery and purity is presented. The review also examines process integration and synergistic combinations of NF with emerging technologies, such as capacitive deionization. Techno-economic and lifecycle assessments are also discussed to provide insights into the economic viability and environmental sustainability of NF-based Li<sup>+</sup> extraction. Finally, we highlight future research directions to bridge the gap between fundamental research and practical applications, aiming to accelerate the development of sustainable and cost-effective Li<sup>+</sup> extraction methods.</p>","PeriodicalId":29801,"journal":{"name":"ACS Environmental Au","volume":"5 1","pages":"12-34"},"PeriodicalIF":6.7,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11740921/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143012777","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}
Pub Date : 2024-11-13DOI: 10.1021/acsenvironau.4c0008010.1021/acsenvironau.4c00080
Fan Wang, Zifeng Lu, Guangxing Lin, Gregory R. Carmichael and Meng Gao*,
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–2. 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 PM2.5 and O3 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.
{"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 and Meng Gao*, ","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}
Pub Date : 2024-11-13eCollection Date: 2025-01-15DOI: 10.1021/acsenvironau.4c00080
Fan Wang, Zifeng Lu, Guangxing Lin, Gregory R Carmichael, Meng Gao
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-2. 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 PM2.5 and O3 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.
棕色碳(BrC)是一种重要的吸光性碳质气溶胶,但对其对区域气候和空气质量的影响尚缺乏认识,这主要是由于对区域气象化学耦合模式的无知。此外,在以前的勘探中对其排放的假设可能会在估计中造成很大的不确定性。在这里,我们在WRF-Chem模型中实现了一个BrC模块,该模块考虑了源依赖性吸收,并避免了由排放强度假设引起的不确定性。据我们所知,我们第一次尝试在区域耦合模型中考虑BrC。利用该模型分析了BrC吸收对东亚地区辐射强迫、区域气候和空气质量的影响。我们发现,在高OC浓度地区,气溶胶吸收光学深度(AAOD)显著增加。BrC吸收最强烈的强迫发生在东南亚的秋季,其值可达到4 W m-2左右。大气吸收的增强改变了地表能量平衡,导致随后的地表温度、热通量、边界层高度和湍流交换率下降。这些气象变量的变化还改变了近地表弥散和光化学条件,导致PM2.5和O3浓度的变化。这些发现表明,BrC可能在特定的地区和时期发挥重要影响。稍后可以使用开发的模型实现更深入的理解。
{"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}
Pub Date : 2024-11-04DOI: 10.1021/acsenvironau.4c0003710.1021/acsenvironau.4c00037
Gauthier J.-P. Deblonde*,
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., Th4+ and UO22+), 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.
{"title":"Biogeochemistry of Actinides: Recent Progress and Perspective","authors":"Gauthier J.-P. Deblonde*, ","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}
Pub Date : 2024-11-04eCollection Date: 2024-11-20DOI: 10.1021/acsenvironau.4c00037
Gauthier J-P Deblonde
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., Th4+ and UO22+), 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.
{"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}
Pub Date : 2024-10-30eCollection Date: 2025-01-15DOI: 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
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.
{"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}
Pub Date : 2024-10-30DOI: 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,
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.
{"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 and Luís R. Ribeiro Rodrigues, ","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}