Madeline E. Clough, Eduardo Ochoa Rivera, Rebecca L. Parham, Andrew P. Ault, Paul M. Zimmerman, Anne J. McNeil, Ambuj Tewari
Microplastics are an emerging pollutant of concern, with environmental observations recorded across the world. Identifying the type of microplastic is challenging due to spectral similarities among the most common polymers, necessitating methods that can confidently distinguish plastic identities. In practice, a researcher chooses the reference vibrational spectrum that is most like the unknown spectrum, where the likeness between the two spectra is expressed numerically as the hit quality index (HQI). Despite the widespread use of HQI thresholds in the literature, acceptance of a spectral label often lacks any associated confidence. To address this gap, we apply a machine-learning framework called conformal prediction to output a set of possible labels that contain the true identity of the unknown spectrum with a user-defined probability (e.g., 90%). Microplastic reference libraries of environmentally aged and pristine polymeric materials, as well as unknown environmental plastic spectra, were employed to illustrate the benefits of this approach when used with two similarity metrics to compute HQI. We present an adaptable workflow using our open-access code to ensure spectral matching confidence for the microplastic community, reducing manual inspection of spectral matches and enhancing the robustness of quantification in the field.
{"title":"Enhancing Confidence in Microplastic Spectral Identification via Conformal Prediction","authors":"Madeline E. Clough, Eduardo Ochoa Rivera, Rebecca L. Parham, Andrew P. Ault, Paul M. Zimmerman, Anne J. McNeil, Ambuj Tewari","doi":"10.1021/acs.est.4c05167","DOIUrl":"https://doi.org/10.1021/acs.est.4c05167","url":null,"abstract":"Microplastics are an emerging pollutant of concern, with environmental observations recorded across the world. Identifying the type of microplastic is challenging due to spectral similarities among the most common polymers, necessitating methods that can confidently distinguish plastic identities. In practice, a researcher chooses the reference vibrational spectrum that is most like the unknown spectrum, where the likeness between the two spectra is expressed numerically as the hit quality index (HQI). Despite the widespread use of HQI thresholds in the literature, acceptance of a spectral label often lacks any associated confidence. To address this gap, we apply a machine-learning framework called conformal prediction to output a set of possible labels that contain the true identity of the unknown spectrum with a user-defined probability (e.g., 90%). Microplastic reference libraries of environmentally aged and pristine polymeric materials, as well as unknown environmental plastic spectra, were employed to illustrate the benefits of this approach when used with two similarity metrics to compute HQI. We present an adaptable workflow using our open-access code to ensure spectral matching confidence for the microplastic community, reducing manual inspection of spectral matches and enhancing the robustness of quantification in the field.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"99 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2024-11-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142712980","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Junli Wang, Kunpeng Chen, Bosen Jin, Wonsik Woo, Michael Lum, Alexa Canchola, Yiwen Zhu, Yujie Men, Jinyong Liu, Ying-Hsuan Lin
Thermal treatment of perfluoroalkyl and polyfluoroalkyl substances (PFASs) presents a promising opportunity to halt the PFAS cycle. However, how co-occurring materials such as granular activated carbon (GAC) influence thermal decomposition products of PFASs, and underlying mechanisms remain unclear. We studied the pyrolysis of two potassium salts of perfluoroalkanesulfonates (PFSAs, CnF2n+1SO3K), perfluorobutanesulfonate (PFBS-K), and perfluorooctanesulfonate (PFOS-K), with or without GAC. PFBS-K is more stable than PFOS-K for pure standards, but when it is adsorbed onto GAC, its thermal stabilities and decomposition behaviors are similar. Temperatures and heating rates can significantly influence the decomposition mechanisms and products for pure standards, while these effects are less pronounced when PFSAs are adsorbed onto GAC. We further studied the underlying decomposition mechanisms. Pure standards of CnF2n+1SO3K can decompose directly in their condense phase by reactions: F(CF2)nSO3K → F(CF2)n-2CF═CF2 + KFSO3 or F(CF2)nSO3K → F(CF2)n- + K+ + SO3. GAC appears to facilitate breakage of the C-S bond to release SO2 at temperatures as low as 280 °C. GAC promotes fluorine mineralization through functional reactive sites. SiO2 is particularly important for the surface-mediated mineralization of PFASs into SiF4. These findings offer valuable insights into optimizing thermal treatment strategies for PFAS-contaminated waste.
{"title":"Pyrolysis of Two Perfluoroalkanesulfonates (PFSAs) and PFSA-Laden Granular Activated Carbon (GAC): Decomposition Mechanisms and the Role of GAC.","authors":"Junli Wang, Kunpeng Chen, Bosen Jin, Wonsik Woo, Michael Lum, Alexa Canchola, Yiwen Zhu, Yujie Men, Jinyong Liu, Ying-Hsuan Lin","doi":"10.1021/acs.est.4c06805","DOIUrl":"https://doi.org/10.1021/acs.est.4c06805","url":null,"abstract":"<p><p>Thermal treatment of perfluoroalkyl and polyfluoroalkyl substances (PFASs) presents a promising opportunity to halt the PFAS cycle. However, how co-occurring materials such as granular activated carbon (GAC) influence thermal decomposition products of PFASs, and underlying mechanisms remain unclear. We studied the pyrolysis of two potassium salts of perfluoroalkanesulfonates (PFSAs, C<sub>n</sub>F<sub>2n+1</sub>SO<sub>3</sub>K), perfluorobutanesulfonate (PFBS-K), and perfluorooctanesulfonate (PFOS-K), with or without GAC. PFBS-K is more stable than PFOS-K for pure standards, but when it is adsorbed onto GAC, its thermal stabilities and decomposition behaviors are similar. Temperatures and heating rates can significantly influence the decomposition mechanisms and products for pure standards, while these effects are less pronounced when PFSAs are adsorbed onto GAC. We further studied the underlying decomposition mechanisms. Pure standards of C<sub>n</sub>F<sub>2n+1</sub>SO<sub>3</sub>K can decompose directly in their condense phase by reactions: F(CF<sub>2</sub>)<sub>n</sub>SO<sub>3</sub>K → F(CF<sub>2</sub>)<sub>n-2</sub>CF═CF<sub>2</sub> + KFSO<sub>3</sub> or F(CF<sub>2</sub>)<sub>n</sub>SO<sub>3</sub>K → F(CF<sub>2</sub>)<sub>n</sub><sup>-</sup> + K<sup>+</sup> + SO<sub>3</sub>. GAC appears to facilitate breakage of the C-S bond to release SO<sub>2</sub> at temperatures as low as 280 °C. GAC promotes fluorine mineralization through functional reactive sites. SiO<sub>2</sub> is particularly important for the surface-mediated mineralization of PFASs into SiF<sub>4</sub>. These findings offer valuable insights into optimizing thermal treatment strategies for PFAS-contaminated waste.</p>","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":" ","pages":""},"PeriodicalIF":10.8,"publicationDate":"2024-11-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142724517","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yangzhao Sun, Roland Weber, Yang Chen, Shijing Lin, Liyuan Liu
Dr. Yangzhao Sun is a professorate senior engineer. He works currently as the director of Scientific Research Academy of Guangxi Environmental Protection. With decades of experience in chemical management, he has been actively engaged in the negotiations of Multilateral Environmental Agreements on POPs, mercury, plastic, etc., and conducted a great deal of policy research as well as international projects in these fields, including the Sino-Norwegian Cooperation Project on Capacity Building for Reducing Plastic and Microplastic Pollution (SINOPLAST). He has 15 monographs and more than 50 published papers in core journals at home and abroad. The authors thank the Sino-Norwegian Cooperation Project on Capacity Building for Reducing Plastic and Microplastic Pollution and the National Key Research and Development Program of China (2022YFC3902300) for supporting this study. This article references 15 other publications. This article has not yet been cited by other publications.
{"title":"How Will Consensus on Key Elements of the International Legally Binding Instrument on Plastic Pollution Be Reached by the End of 2024?","authors":"Yangzhao Sun, Roland Weber, Yang Chen, Shijing Lin, Liyuan Liu","doi":"10.1021/acs.est.4c11458","DOIUrl":"https://doi.org/10.1021/acs.est.4c11458","url":null,"abstract":"Dr. Yangzhao Sun is a professorate senior engineer. He works currently as the director of Scientific Research Academy of Guangxi Environmental Protection. With decades of experience in chemical management, he has been actively engaged in the negotiations of Multilateral Environmental Agreements on POPs, mercury, plastic, etc., and conducted a great deal of policy research as well as international projects in these fields, including the Sino-Norwegian Cooperation Project on Capacity Building for Reducing Plastic and Microplastic Pollution (SINOPLAST). He has 15 monographs and more than 50 published papers in core journals at home and abroad. The authors thank the Sino-Norwegian Cooperation Project on Capacity Building for Reducing Plastic and Microplastic Pollution and the National Key Research and Development Program of China (2022YFC3902300) for supporting this study. This article references 15 other publications. This article has not yet been cited by other publications.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"160 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2024-11-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142712988","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-26Epub Date: 2024-10-29DOI: 10.1021/acs.est.3c10948
Junhong Wu, Yin Zhong, Yirong Deng, Sen Yang, Heli Wang, Qian Yang, Dan Li, Jianzhong Song, Huanheng Zhang, Ping'an Peng
Combining organohalide-respiring bacteria with nanoscale zero-valent iron (nZVI) represents a promising approach for remediating chloroethene-contaminated aquifers. However, limited information is available regarding their synergistic dechlorinating ability for chloroethenes when nZVI is sulfidated (S-nZVI) under the organic electron donor-limited conditions typically found in deep aquifers. Herein, we developed a combined system utilizing a mixed culture containing Dehalococcoides (Dhc) and S-nZVI particles, which achieved sustainable dechlorination with repeated rounds of spiking with 110 μM perchloroethene (PCE). The relative abundance of Dhc considerably increased from 5.2 to 91.5% after five rounds of spiking with PCE, as evidenced by 16S rRNA gene amplicon sequencing. S-nZVI corrosion generated hydrogen as an electron donor for Dhc and other volatile fatty acid (VFA)-producing bacteria. Electron balance analysis indicated that 68.1% of electrons from Fe0 consumed in S-nZVI were involved in dechlorination, and 6.2, 1.1, and 3.2% were stored in formate, acetate, and other VFAs, respectively. The produced acetate possibly served as a carbon source for Dhc. Metagenomic analysis revealed that Desulfovibrio, Syntrophomonas, Clostridium, and Mesotoga were likely involved in VFA production. These findings provide valuable insights into the synergistic mechanisms of biotic and abiotic dechlorination, with important implications for sustainable remediation of electron donor-limited aquifers contaminated by chloroethenes.
{"title":"Sustainable Abiotic-Biotic Dechlorination of Perchloroethene with Sulfidated Nanoscale Zero-Valent Iron as Electron Donor Source.","authors":"Junhong Wu, Yin Zhong, Yirong Deng, Sen Yang, Heli Wang, Qian Yang, Dan Li, Jianzhong Song, Huanheng Zhang, Ping'an Peng","doi":"10.1021/acs.est.3c10948","DOIUrl":"10.1021/acs.est.3c10948","url":null,"abstract":"<p><p>Combining organohalide-respiring bacteria with nanoscale zero-valent iron (nZVI) represents a promising approach for remediating chloroethene-contaminated aquifers. However, limited information is available regarding their synergistic dechlorinating ability for chloroethenes when nZVI is sulfidated (S-nZVI) under the organic electron donor-limited conditions typically found in deep aquifers. Herein, we developed a combined system utilizing a mixed culture containing <i>Dehalococcoides</i> (<i>Dhc</i>) and S-nZVI particles, which achieved sustainable dechlorination with repeated rounds of spiking with 110 μM perchloroethene (PCE). The relative abundance of <i>Dhc</i> considerably increased from 5.2 to 91.5% after five rounds of spiking with PCE, as evidenced by 16S rRNA gene amplicon sequencing. S-nZVI corrosion generated hydrogen as an electron donor for <i>Dhc</i> and other volatile fatty acid (VFA)-producing bacteria. Electron balance analysis indicated that 68.1% of electrons from Fe<sup>0</sup> consumed in S-nZVI were involved in dechlorination, and 6.2, 1.1, and 3.2% were stored in formate, acetate, and other VFAs, respectively. The produced acetate possibly served as a carbon source for <i>Dhc</i>. Metagenomic analysis revealed that <i>Desulfovibrio</i>, <i>Syntrophomonas</i>, <i>Clostridium</i>, and <i>Mesotoga</i> were likely involved in VFA production. These findings provide valuable insights into the synergistic mechanisms of biotic and abiotic dechlorination, with important implications for sustainable remediation of electron donor-limited aquifers contaminated by chloroethenes.</p>","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":" ","pages":"20931-20941"},"PeriodicalIF":10.8,"publicationDate":"2024-11-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142520331","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Alana K Ayasse, Daniel H Cusworth, Katherine Howell, Kelly O'Neill, Bradley M Conrad, Matthew R Johnson, Joseph Heckler, Gregory P Asner, Riley Duren
Satellites are becoming a widely used measurement tool for methane detection and quantification. The landscape of satellite instruments with some methane point-source quantification capabilities is growing. Combining information across available sensor platforms could be pivotal for understanding trends and uncertainties in source-level emissions. However, to effectively combine information across sensors of varying performance levels, the probability of detection (POD) for all instruments must be well characterized, which is time-consuming and costly, especially for satellites. In August 2023, we timed methane-sensing aerial surveys from the Global Airborne Observatory (GAO) to overlap with observations from the NASA Earth Surface Mineral Dust Source Investigation (EMIT). We show how these coincident observations can be used to determine and verify the detection limits of EMIT and to develop and test a multisensor persistence framework. Under favorable conditions, the 90% POD at 3 for EMIT is 1060. We further derive a Bayesian model to infer probabilistically whether nondetected emissions were truly off, and we validate and show how this model can be used to assess the intermittency of emissions with GAO and EMIT. Time-averaged emission rates from persistent sources can be underestimated if POD is not characterized and if differences in POD across multisensor frameworks are not properly accounted for.
卫星正成为甲烷探测和定量的一种广泛使用的测量工具。具有一定甲烷点源量化能力的卫星仪器正在不断增加。综合利用现有传感器平台的信息对于了解源级排放的趋势和不确定性至关重要。然而，要有效地将不同性能水平的传感器之间的信息结合起来，必须对所有仪器的探测概率（POD）进行充分描述，这既费时又费钱，尤其是对卫星而言。2023 年 8 月，我们将全球机载观测站（GAO）的甲烷传感空中勘测与美国国家航空航天局（NASA）的地球表面矿物尘源调查（EMIT）的观测进行了时间上的重叠。我们展示了如何利用这些重合观测来确定和验证 EMIT 的探测极限，以及如何开发和测试多传感器持久性框架。在有利条件下，EMIT 的 90% POD at 3 为 1060。我们进一步推导出一个贝叶斯模型，从概率上推断未检测到的排放是否真正关闭，我们还验证并展示了该模型如何用于评估 GAO 和 EMIT 的排放间歇性。如果未对 POD 进行描述，也未适当考虑多传感器框架之间 POD 的差异，则可能会低估持久源的时间平均排放率。
{"title":"Probability of Detection and Multi-Sensor Persistence of Methane Emissions from Coincident Airborne and Satellite Observations.","authors":"Alana K Ayasse, Daniel H Cusworth, Katherine Howell, Kelly O'Neill, Bradley M Conrad, Matthew R Johnson, Joseph Heckler, Gregory P Asner, Riley Duren","doi":"10.1021/acs.est.4c06702","DOIUrl":"https://doi.org/10.1021/acs.est.4c06702","url":null,"abstract":"<p><p>Satellites are becoming a widely used measurement tool for methane detection and quantification. The landscape of satellite instruments with some methane point-source quantification capabilities is growing. Combining information across available sensor platforms could be pivotal for understanding trends and uncertainties in source-level emissions. However, to effectively combine information across sensors of varying performance levels, the probability of detection (POD) for all instruments must be well characterized, which is time-consuming and costly, especially for satellites. In August 2023, we timed methane-sensing aerial surveys from the Global Airborne Observatory (GAO) to overlap with observations from the NASA Earth Surface Mineral Dust Source Investigation (EMIT). We show how these coincident observations can be used to determine and verify the detection limits of EMIT and to develop and test a multisensor persistence framework. Under favorable conditions, the 90% POD at 3 for EMIT is 1060. We further derive a Bayesian model to infer probabilistically whether nondetected emissions were truly off, and we validate and show how this model can be used to assess the intermittency of emissions with GAO and EMIT. Time-averaged emission rates from persistent sources can be underestimated if POD is not characterized and if differences in POD across multisensor frameworks are not properly accounted for.</p>","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":" ","pages":""},"PeriodicalIF":10.8,"publicationDate":"2024-11-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142714785","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Stacey M. Trevathan-Tackett, Sebastian Kepfer-Rojas, Martino Malerba, Peter I. Macreadie, Ika Djukic, Junbin Zhao, Erica B. Young, Paul H. York, Shin-Cheng Yeh, Yanmei Xiong, Gidon Winters, Danielle Whitlock, Carolyn A. Weaver, Anne Watson, Inger Visby, Jacek Tylkowski, Allison Trethowan, Scott Tiegs, Ben Taylor, Jozef Szpikowski, Grażyna Szpikowska, Victoria L. Strickland, Normunds Stivrins, Ana I. Sousa, Sutinee Sinutok, Whitney A. Scheffel, Rui Santos, Jonathan Sanderman, Salvador Sánchez-Carrillo, Joan-Albert Sanchez-Cabeza, Krzysztof G. Rymer, Ana Carolina Ruiz-Fernandez, Bjorn J. M. Robroek, Tessa Roberts, Aurora M. Ricart, Laura K. Reynolds, Grzegorz Rachlewicz, Anchana Prathep, Andrew J. Pinsonneault, Elise Pendall, Richard Payne, Ilze Ozola, Cody Onufrock, Anne Ola, Steven F. Oberbauer, Aroloye O. Numbere, Alyssa B. Novak, Joanna Norkko, Alf Norkko, Thomas J. Mozdzer, Pam Morgan, Diana I. Montemayor, Charles W. Martin, Sparkle L. Malone, Maciej Major, Mikołaj Majewski, Carolyn J. Lundquist, Catherine E. Lovelock, Songlin Liu, Hsing-Juh Lin, Ana Lillebo, Jinquan Li, John S. Kominoski, Anzar Ahmad Khuroo, Jeffrey J. Kelleway, Kristin I. Jinks, Daniel Jerónimo, Christopher Janousek, Emma L. Jackson, Oscar Iribarne, Torrance Hanley, Maroof Hamid, Arjun Gupta, Rafael D. Guariento, Ieva Grudzinska, Anderson da Rocha Gripp, María A. González Sagrario, Laura M. Garrison, Karine Gagnon, Esperança Gacia, Marco Fusi, Lachlan Farrington, Jenny Farmer, Francisco de Assis Esteves, Mauricio Escapa, Monika Domańska, André T. C. Dias, Carmen B. de los Santos, Daniele Daffonchio, Paweł M. Czyryca, Rod M. Connolly, Alexander Cobb, Maria Chudzińska, Bart Christiaen, Peter Chifflard, Sara Castelar, Luciana S. Carneiro, José Gilberto Cardoso-Mohedano, Megan Camden, Adriano Caliman, Richard H. Bulmer, Jennifer Bowen, Christoffer Boström, Susana Bernal, John A. Berges, Juan C. Benavides, Savanna C. Barry, Juha M. Alatalo, Alia N. Al-Haj, Maria Fernanda Adame
Patchy global data on belowground litter decomposition dynamics limit our capacity to discern the drivers of carbon preservation and storage across inland and coastal wetlands. We performed a global, multiyear study in over 180 wetlands across 28 countries and 8 macroclimates using standardized litter as measures of “recalcitrant” (rooibos tea) and “labile” (green tea) organic matter (OM) decomposition. Freshwater wetlands and tidal marshes had the highest tea mass remaining, indicating a greater potential for carbon preservation in these ecosystems. Recalcitrant OM decomposition increased with elevated temperatures throughout the decay period, e.g., increase from 10 to 20 °C corresponded to a 1.46-fold increase in the recalcitrant OM decay rate constant. The effect of elevated temperature on labile OM breakdown was ecosystem-dependent, with tidally influenced wetlands showing limited effects of temperature compared with freshwater wetlands. Based on climatic projections, by 2050 wetland decay constants will increase by 1.8% for labile and 3.1% for recalcitrant OM. Our study highlights the potential for reduction in belowground OM in coastal and inland wetlands under increased warming, but the extent and direction of this effect at a large scale is dependent on ecosystem and OM characteristics. Understanding local versus global drivers is necessary to resolve ecosystem influences on carbon preservation in wetlands.
有关地下废弃物分解动态的全球零散数据限制了我们辨别内陆和沿海湿地碳保存和储存驱动因素的能力。我们在全球 28 个国家和 8 种宏观气候条件下的 180 多处湿地开展了一项为期多年的研究，使用标准化垃圾作为 "难分解"（罗布麻茶）和 "易分解"（绿茶）有机物（OM）分解的衡量标准。淡水湿地和潮汐沼泽的茶叶剩余质量最高，表明这些生态系统具有更大的碳保存潜力。在整个腐烂过程中，随着温度的升高，难分解有机物的分解量增加，例如，温度从 10 ℃ 升至 20 ℃，难分解有机物的腐烂速率常数增加了 1.46 倍。温度升高对可溶性 OM 分解的影响取决于生态系统，与淡水湿地相比，受潮汐影响的湿地受温度的影响有限。根据气候预测，到 2050 年，湿地可腐烂有机物的腐烂常数将增加 1.8%，难腐烂有机物的腐烂常数将增加 3.1%。我们的研究突出表明，在气候变暖的情况下，沿海和内陆湿地地下 OM 有可能减少，但这种影响在大范围内的程度和方向取决于生态系统和 OM 的特征。要解决生态系统对湿地碳保存的影响问题，就必须了解当地与全球的驱动因素。
{"title":"Climate Effects on Belowground Tea Litter Decomposition Depend on Ecosystem and Organic Matter Types in Global Wetlands","authors":"Stacey M. Trevathan-Tackett, Sebastian Kepfer-Rojas, Martino Malerba, Peter I. Macreadie, Ika Djukic, Junbin Zhao, Erica B. Young, Paul H. York, Shin-Cheng Yeh, Yanmei Xiong, Gidon Winters, Danielle Whitlock, Carolyn A. Weaver, Anne Watson, Inger Visby, Jacek Tylkowski, Allison Trethowan, Scott Tiegs, Ben Taylor, Jozef Szpikowski, Grażyna Szpikowska, Victoria L. Strickland, Normunds Stivrins, Ana I. Sousa, Sutinee Sinutok, Whitney A. Scheffel, Rui Santos, Jonathan Sanderman, Salvador Sánchez-Carrillo, Joan-Albert Sanchez-Cabeza, Krzysztof G. Rymer, Ana Carolina Ruiz-Fernandez, Bjorn J. M. Robroek, Tessa Roberts, Aurora M. Ricart, Laura K. Reynolds, Grzegorz Rachlewicz, Anchana Prathep, Andrew J. Pinsonneault, Elise Pendall, Richard Payne, Ilze Ozola, Cody Onufrock, Anne Ola, Steven F. Oberbauer, Aroloye O. Numbere, Alyssa B. Novak, Joanna Norkko, Alf Norkko, Thomas J. Mozdzer, Pam Morgan, Diana I. Montemayor, Charles W. Martin, Sparkle L. Malone, Maciej Major, Mikołaj Majewski, Carolyn J. Lundquist, Catherine E. Lovelock, Songlin Liu, Hsing-Juh Lin, Ana Lillebo, Jinquan Li, John S. Kominoski, Anzar Ahmad Khuroo, Jeffrey J. Kelleway, Kristin I. Jinks, Daniel Jerónimo, Christopher Janousek, Emma L. Jackson, Oscar Iribarne, Torrance Hanley, Maroof Hamid, Arjun Gupta, Rafael D. Guariento, Ieva Grudzinska, Anderson da Rocha Gripp, María A. González Sagrario, Laura M. Garrison, Karine Gagnon, Esperança Gacia, Marco Fusi, Lachlan Farrington, Jenny Farmer, Francisco de Assis Esteves, Mauricio Escapa, Monika Domańska, André T. C. Dias, Carmen B. de los Santos, Daniele Daffonchio, Paweł M. Czyryca, Rod M. Connolly, Alexander Cobb, Maria Chudzińska, Bart Christiaen, Peter Chifflard, Sara Castelar, Luciana S. Carneiro, José Gilberto Cardoso-Mohedano, Megan Camden, Adriano Caliman, Richard H. Bulmer, Jennifer Bowen, Christoffer Boström, Susana Bernal, John A. Berges, Juan C. Benavides, Savanna C. Barry, Juha M. Alatalo, Alia N. Al-Haj, Maria Fernanda Adame","doi":"10.1021/acs.est.4c02116","DOIUrl":"https://doi.org/10.1021/acs.est.4c02116","url":null,"abstract":"Patchy global data on belowground litter decomposition dynamics limit our capacity to discern the drivers of carbon preservation and storage across inland and coastal wetlands. We performed a global, multiyear study in over 180 wetlands across 28 countries and 8 macroclimates using standardized litter as measures of “recalcitrant” (rooibos tea) and “labile” (green tea) organic matter (OM) decomposition. Freshwater wetlands and tidal marshes had the highest tea mass remaining, indicating a greater potential for carbon preservation in these ecosystems. Recalcitrant OM decomposition increased with elevated temperatures throughout the decay period, e.g., increase from 10 to 20 °C corresponded to a 1.46-fold increase in the recalcitrant OM decay rate constant. The effect of elevated temperature on labile OM breakdown was ecosystem-dependent, with tidally influenced wetlands showing limited effects of temperature compared with freshwater wetlands. Based on climatic projections, by 2050 wetland decay constants will increase by 1.8% for labile and 3.1% for recalcitrant OM. Our study highlights the potential for reduction in belowground OM in coastal and inland wetlands under increased warming, but the extent and direction of this effect at a large scale is dependent on ecosystem and OM characteristics. Understanding local versus global drivers is necessary to resolve ecosystem influences on carbon preservation in wetlands.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"32 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2024-11-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142712987","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Tolga Ayeri, Yutong Guo, Peter J. T. M. van Puijenbroek, Nynke Hofstra, Ad M. J. Ragas, Maryna Strokal
Global mitigation strategies are needed to reduce the amount of microplastics reaching our oceans via rivers. However, what strategies will be most effective, and when and where to implement these strategies is unclear. We applied the global water quality model MARINA-Plastics, covering 10,226 sub-basins worldwide, to assess the effects of different emission reduction strategies on microplastic inputs to rivers worldwide over the period 2010–2100, taking time steps of 10 years. We applied four scenarios: three focused on wastewater treatment technologies, ranging from high to low technology improvement levels, and one combining high technology in wastewater treatment with source-oriented measures. The results show that the combined strategy of high wastewater treatment and source-oriented measures is expected to be the most effective for reducing future microplastics in rivers on a global scale. By 2100, this combined strategy is expected to result in a 68% microplastic reduction in global rivers compared to 2010. African rivers will be the main hotspots, receiving more than five times more microplastics in 2100 than in 2010. In 2100, wear from car tires is expected to be the dominant source of microplastics globally. Our insights support the implementation of the European Green Deal and the realization of Sustainable Development Goal 6 (clean water).
{"title":"Combined Effects of Treatment and Sewer Connections to Reduce Future Microplastic Emissions in Rivers","authors":"Tolga Ayeri, Yutong Guo, Peter J. T. M. van Puijenbroek, Nynke Hofstra, Ad M. J. Ragas, Maryna Strokal","doi":"10.1021/acs.est.4c07730","DOIUrl":"https://doi.org/10.1021/acs.est.4c07730","url":null,"abstract":"Global mitigation strategies are needed to reduce the amount of microplastics reaching our oceans via rivers. However, what strategies will be most effective, and when and where to implement these strategies is unclear. We applied the global water quality model MARINA-Plastics, covering 10,226 sub-basins worldwide, to assess the effects of different emission reduction strategies on microplastic inputs to rivers worldwide over the period 2010–2100, taking time steps of 10 years. We applied four scenarios: three focused on wastewater treatment technologies, ranging from high to low technology improvement levels, and one combining high technology in wastewater treatment with source-oriented measures. The results show that the combined strategy of high wastewater treatment and source-oriented measures is expected to be the most effective for reducing future microplastics in rivers on a global scale. By 2100, this combined strategy is expected to result in a 68% microplastic reduction in global rivers compared to 2010. African rivers will be the main hotspots, receiving more than five times more microplastics in 2100 than in 2010. In 2100, wear from car tires is expected to be the dominant source of microplastics globally. Our insights support the implementation of the European Green Deal and the realization of Sustainable Development Goal 6 (clean water).","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"185 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2024-11-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142696961","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Gaojie Chen, Lingling Xu, Shaocai Yu, Likun Xue, Ziyi Lin, Chen Yang, Xiaoting Ji, Xiaolong Fan, Yee Jun Tham, Haichao Wang, Youwei Hong, Mengren Li, John H. Seinfeld, Jinsheng Chen
Chlorine (Cl) radicals strongly affect atmospheric oxidation and the fate of pollutants. Despite several observations, the potential impacts of nitrogen chemistry associated with NO2 on Cl chemistry are poorly understood. Here, we provided direct field evidence that the nitrogen chemistry enhancements triggered by the increased NO2 drove daytime nitrate (NO3–) photolysis and nighttime NO3–N2O5 reactions, significantly promoting the increases in the concentrations of ClNO2 and Cl2 after the Chinese Spring Festival. The enhancement in the Cl chemistry facilitated the elevations of both O3 and atmospheric oxidation capacity during the winter daytime. Our findings highlighted the importance of nitrogen chemistry induced by the increased NO2 in enhanced Cl chemistry.
{"title":"Increasing Contribution of Chlorine Chemistry to Wintertime Ozone Formation Promoted by Enhanced Nitrogen Chemistry","authors":"Gaojie Chen, Lingling Xu, Shaocai Yu, Likun Xue, Ziyi Lin, Chen Yang, Xiaoting Ji, Xiaolong Fan, Yee Jun Tham, Haichao Wang, Youwei Hong, Mengren Li, John H. Seinfeld, Jinsheng Chen","doi":"10.1021/acs.est.4c09523","DOIUrl":"https://doi.org/10.1021/acs.est.4c09523","url":null,"abstract":"Chlorine (Cl) radicals strongly affect atmospheric oxidation and the fate of pollutants. Despite several observations, the potential impacts of nitrogen chemistry associated with NO<sub>2</sub> on Cl chemistry are poorly understood. Here, we provided direct field evidence that the nitrogen chemistry enhancements triggered by the increased NO<sub>2</sub> drove daytime nitrate (NO<sub>3</sub><sup>–</sup>) photolysis and nighttime NO<sub>3</sub>–N<sub>2</sub>O<sub>5</sub> reactions, significantly promoting the increases in the concentrations of ClNO<sub>2</sub> and Cl<sub>2</sub> after the Chinese Spring Festival. The enhancement in the Cl chemistry facilitated the elevations of both O<sub>3</sub> and atmospheric oxidation capacity during the winter daytime. Our findings highlighted the importance of nitrogen chemistry induced by the increased NO<sub>2</sub> in enhanced Cl chemistry.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"3 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2024-11-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142712986","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Ziqi Zhou, Shikha Garg, Christopher J. Miller, Qing-Long Fu, Andrew S. Kinsela, Timothy E. Payne, T. David Waite
Redox fluctuations within redox dynamic environments influence the redox state of natural organic matter (NOM) and its interaction with redox-active elements, such as iron. In this work, we investigate the changes in the molecular composition of NOM during redox fluctuations as well as the impact of these changes on the Fe-NOM interaction employing Suwannee River Dissolved Organic Matter (SRDOM) as a representative NOM. Characterization of SRDOM using X-ray photoelectron spectroscopy and Fourier transform infrared spectrometry showed that irreversible changes occurred following electrochemical reduction and reoxidation of SRDOM in air. Changes in the redox state of SRDOM impacted its interaction with iron with higher rates of Fe(III) reduction in the presence of reduced and reoxidized SRDOM than in the presence of the original SRDOM. The increased rate of Fe(III) reduction in the presence of reduced SRDOM was due to the formation of reduced organic moieties on SRDOM reduction. The Fe(II) oxidation rate also increased in the presence of reduced SRDOM due to the formation of redox-active moieties that were capable of oxidizing Fe(II). Overall, our study provides useful insights into the changes in SRDOM that may occur in redox dynamic environments and the associated impact of these changes on Fe transformations.
{"title":"Transformation of Natural Organic Matter in Simulated Abiotic Redox Dynamic Environments: Impact on Fe Cycling","authors":"Ziqi Zhou, Shikha Garg, Christopher J. Miller, Qing-Long Fu, Andrew S. Kinsela, Timothy E. Payne, T. David Waite","doi":"10.1021/acs.est.4c05517","DOIUrl":"https://doi.org/10.1021/acs.est.4c05517","url":null,"abstract":"Redox fluctuations within redox dynamic environments influence the redox state of natural organic matter (NOM) and its interaction with redox-active elements, such as iron. In this work, we investigate the changes in the molecular composition of NOM during redox fluctuations as well as the impact of these changes on the Fe-NOM interaction employing Suwannee River Dissolved Organic Matter (SRDOM) as a representative NOM. Characterization of SRDOM using X-ray photoelectron spectroscopy and Fourier transform infrared spectrometry showed that irreversible changes occurred following electrochemical reduction and reoxidation of SRDOM in air. Changes in the redox state of SRDOM impacted its interaction with iron with higher rates of Fe(III) reduction in the presence of reduced and reoxidized SRDOM than in the presence of the original SRDOM. The increased rate of Fe(III) reduction in the presence of reduced SRDOM was due to the formation of reduced organic moieties on SRDOM reduction. The Fe(II) oxidation rate also increased in the presence of reduced SRDOM due to the formation of redox-active moieties that were capable of oxidizing Fe(II). Overall, our study provides useful insights into the changes in SRDOM that may occur in redox dynamic environments and the associated impact of these changes on Fe transformations.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"19 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2024-11-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142712984","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Antibiotic resistance poses a significant threat to human health. While most studies focus on bacteria, interactions between antibiotics and other crucial microbial groups like protists remain uncertain. This study investigates how protists interact with antibiotics and examines how these interactions impact the fate of resistance genes. It reveals that amoebae exhibit high resistance to eight high-risk environmental antibiotics, accumulating significant quantities within their cells. Wild amoeboid strains from distant locations carry substantial antibiotic resistance genes (ARGs) and metal resistance genes (MRGs), with significant heterogeneity within a single species. Amoeboid symbionts and pathogens predominantly carry these genes. Paraburkholderia symbionts have reduced genomes and fewer resistance genes compared to free-living strains, while amoeba-endogenous Stenotrophomonas maltophilia does not exhibit a significantly reduced genome size. This suggests that the amoeboid hosts serve as a temporary medium facilitating its transmission. In summary, the study unveils that soil amoebae represent unexpected hotspots for antibiotics and resistance genes. Future research should assess the effects of antibiotics on often-overlooked protists and explore their role in spreading ARGs and MRGs in ecosystems. Incorporating protists into broader antibiotic resistance research is recommended, highlighting their significance within a One Health perspective.
{"title":"Soil Amoebae Are Unexpected Hotspots of Environmental Antibiotics and Antibiotic Resistance Genes","authors":"Yijing Shi, Minxi Liang, Jiaxiong Zeng, Zihe Wang, Lin Zhang, Zhili He, Mengyuan Li, Longfei Shu, Guangguo Ying","doi":"10.1021/acs.est.4c10455","DOIUrl":"https://doi.org/10.1021/acs.est.4c10455","url":null,"abstract":"Antibiotic resistance poses a significant threat to human health. While most studies focus on bacteria, interactions between antibiotics and other crucial microbial groups like protists remain uncertain. This study investigates how protists interact with antibiotics and examines how these interactions impact the fate of resistance genes. It reveals that amoebae exhibit high resistance to eight high-risk environmental antibiotics, accumulating significant quantities within their cells. Wild amoeboid strains from distant locations carry substantial antibiotic resistance genes (ARGs) and metal resistance genes (MRGs), with significant heterogeneity within a single species. Amoeboid symbionts and pathogens predominantly carry these genes. <i>Paraburkholderia</i> symbionts have reduced genomes and fewer resistance genes compared to free-living strains, while amoeba-endogenous <i>Stenotrophomonas maltophilia</i> does not exhibit a significantly reduced genome size. This suggests that the amoeboid hosts serve as a temporary medium facilitating its transmission. In summary, the study unveils that soil amoebae represent unexpected hotspots for antibiotics and resistance genes. Future research should assess the effects of antibiotics on often-overlooked protists and explore their role in spreading ARGs and MRGs in ecosystems. Incorporating protists into broader antibiotic resistance research is recommended, highlighting their significance within a One Health perspective.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"80 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2024-11-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142696962","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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