Pub Date : 2024-11-19DOI: 10.1021/acs.est.4c0854410.1021/acs.est.4c08544
Yuemei Ye*, Ivan A. Titaley, Mitchell L. Kim-Fu, Ansel R. Moll, Jennifer A. Field and Morton A. Barlaz,
Per- and polyfluoroalkyl substances (PFAS) have been detected in plant fiber-based food packaging and most such packaging is disposed in landfills. The objective of this research was to evaluate the release of volatile PFAS to the gas-phase from PFAS-containing, single-use food packaging materials and from municipal solid waste (MSW) during anaerobic decomposition under simulated landfill conditions. After screening 46 materials for total F and 6:2 fluorotelomer alcohol (FTOH), packaging materials were classified as high or low F. High F materials included microwavable popcorn bags, natural plates, compostable bowls, biodegradable boxes, bagasse containers and eco-friendly plates, while the low F materials tested were paper plates, eco-friendly food trays and poly coated freezer paper. Summed PFAS release from the high F materials was 62–800 ng PFAS/g sample and 6:2 FTOH comprised 96.8–99.9% of the summed PFAS. The low F materials and MSW released 0.1–0.4 ng summed PFAS/g sample and 7:2-secondary (s) FTOH was the dominant volatile PFAS. PFAS were generally released early in the 123–285-day decomposition cycle, suggesting that some PFAS will be released prior to the installation of landfill gas collection systems. Nonetheless, PFAS have been reported in collected landfill gas, indicating that release occurs over many years.
This study demonstrates the release of volatile PFAS to the gas phase from PFAS-contaminated plant fiber-based food packaging under simulated landfill conditions.
{"title":"Release of Volatile Per- and Polyfluoroalkyl Substances from Plant Fiber-Based Food Packaging and Municipal Solid Waste to Gas under Simulated Landfill Conditions","authors":"Yuemei Ye*, Ivan A. Titaley, Mitchell L. Kim-Fu, Ansel R. Moll, Jennifer A. Field and Morton A. Barlaz, ","doi":"10.1021/acs.est.4c0854410.1021/acs.est.4c08544","DOIUrl":"https://doi.org/10.1021/acs.est.4c08544https://doi.org/10.1021/acs.est.4c08544","url":null,"abstract":"<p >Per- and polyfluoroalkyl substances (PFAS) have been detected in plant fiber-based food packaging and most such packaging is disposed in landfills. The objective of this research was to evaluate the release of volatile PFAS to the gas-phase from PFAS-containing, single-use food packaging materials and from municipal solid waste (MSW) during anaerobic decomposition under simulated landfill conditions. After screening 46 materials for total <i>F</i> and 6:2 fluorotelomer alcohol (FTOH), packaging materials were classified as high or low <i>F</i>. High <i>F</i> materials included microwavable popcorn bags, natural plates, compostable bowls, biodegradable boxes, bagasse containers and eco-friendly plates, while the low <i>F</i> materials tested were paper plates, eco-friendly food trays and poly coated freezer paper. Summed PFAS release from the high <i>F</i> materials was 62–800 ng PFAS/g sample and 6:2 FTOH comprised 96.8–99.9% of the summed PFAS. The low <i>F</i> materials and MSW released 0.1–0.4 ng summed PFAS/g sample and 7:2-secondary (s) FTOH was the dominant volatile PFAS. PFAS were generally released early in the 123–285-day decomposition cycle, suggesting that some PFAS will be released prior to the installation of landfill gas collection systems. Nonetheless, PFAS have been reported in collected landfill gas, indicating that release occurs over many years.</p><p >This study demonstrates the release of volatile PFAS to the gas phase from PFAS-contaminated plant fiber-based food packaging under simulated landfill conditions.</p>","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"58 48","pages":"21295–21304 21295–21304"},"PeriodicalIF":10.8,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acs.est.4c08544","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142761342","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yanping Liang, Yunfeng Yan, Lulu Shi, Mingyu Wang, Xianzheng Yuan, Shuguang Wang, Li Ye, Zhen Yan
Methanogenic archaea are known to play a crucial role in the biogeochemical cycling of arsenic (As); however, the molecular basis of As transformation mediated by methanogenic archaea remains poorly understood. Herein, the characterization of the redox transformation and methylation of As by Methanosarcina acetivorans, a model methanogenic archaeon, is reported. M. acetivorans was demonstrated to mediate As(V) reduction via a cytoplasmic As reductase (ArsC) in the exponential phase of methanogenic growth and to methylate As(III) via a cytoplasmic As(III) methyltransferase (ArsM) in the stationary phase. Characterization of the ArsC-catalyzed As(V) reduction and the ArsM-catalyzed As(III) methylation showed that a thioredoxin (Trx) encoded by MA4683 was preferentially utilized as a physiological electron donor for ArsC and ArsM, providing a redox link between methanogenesis and As transformation. The structures of ArsC and ArsM complexed with Trx were modeled using AlphaFold-Multimer. Site-directed mutagenesis of key cysteine residues at the interaction sites of the complexes indicated that the archaeal ArsC and ArsM employ evolutionarily distinct disulfide bonds for interacting with Trx compared to those used by bacterial ArsC or eukaryotic ArsM. The findings of this study present a major advance in our current understanding of the physiological roles and underlying mechanism of As transformation in methanogenic archaea.
{"title":"Molecular Basis of Thioredoxin-Dependent Arsenic Transformation in Methanogenic Archaea.","authors":"Yanping Liang, Yunfeng Yan, Lulu Shi, Mingyu Wang, Xianzheng Yuan, Shuguang Wang, Li Ye, Zhen Yan","doi":"10.1021/acs.est.4c06611","DOIUrl":"10.1021/acs.est.4c06611","url":null,"abstract":"<p><p>Methanogenic archaea are known to play a crucial role in the biogeochemical cycling of arsenic (As); however, the molecular basis of As transformation mediated by methanogenic archaea remains poorly understood. Herein, the characterization of the redox transformation and methylation of As by <i>Methanosarcina acetivorans</i>, a model methanogenic archaeon, is reported. <i>M. acetivorans</i> was demonstrated to mediate As(V) reduction via a cytoplasmic As reductase (ArsC) in the exponential phase of methanogenic growth and to methylate As(III) via a cytoplasmic As(III) methyltransferase (ArsM) in the stationary phase. Characterization of the ArsC-catalyzed As(V) reduction and the ArsM-catalyzed As(III) methylation showed that a thioredoxin (Trx) encoded by MA4683 was preferentially utilized as a physiological electron donor for ArsC and ArsM, providing a redox link between methanogenesis and As transformation. The structures of ArsC and ArsM complexed with Trx were modeled using AlphaFold-Multimer. Site-directed mutagenesis of key cysteine residues at the interaction sites of the complexes indicated that the archaeal ArsC and ArsM employ evolutionarily distinct disulfide bonds for interacting with Trx compared to those used by bacterial ArsC or eukaryotic ArsM. The findings of this study present a major advance in our current understanding of the physiological roles and underlying mechanism of As transformation in methanogenic archaea.</p>","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":" ","pages":""},"PeriodicalIF":10.8,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142666420","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 : 2024-11-19Epub Date: 2024-10-10DOI: 10.1021/acs.est.4c05605
Wenzhi Gu, Jing Hu, Lei Li, Mingqiu Hong, Chaohui Yang, Guoping Ren, Jie Ye, Shungui Zhou
Bio-nano hybrids (BNH), combining semiconductors and microorganisms, have shown great promise for effective solar-to-fuel energy conversion. However, the high-energy ultraviolet (UV) photons in the solar spectrum can cause severe photocorrosion of semiconductors and irreversible photodamage to microorganisms within BNH. Here, we developed an encapsulation strategy using natural luminogens with aggregation-induced emission characteristics (AIEgens) to construct a protective layer for BNH, effectively shielding them against high-energy UV photons. We incorporated natural berberine (BBR) into the BNH composed of Methanosarcina barkeri and polymeric carbon nitrides (CNx). The self-assembled BNH-BBR system displayed a 2.75-fold higher CH4 yield than BNH under simulated solar irradiation. Mechanism analysis revealed that BBR acted as a UV sunscreen for BNH by converting high-energy short wavelengths into low-energy long wavelengths, thereby reducing the accumulation of reactive oxygen species and alleviating the photocorrosion of CNx. Furthermore, BBR functioned as a photosynergist for BNH by regulating photoelectron production and utilization, enhancing the intracellular energy formation in M. barkeri for growth and metabolism. This work provides important insights into the effective and scalable conversion of CO2 into valuable biofuels with BNH under light illumination containing high-energy photons.
{"title":"Natural AIEgens as Ultraviolet Sunscreens and Photosynergists for Solar Fuel Production.","authors":"Wenzhi Gu, Jing Hu, Lei Li, Mingqiu Hong, Chaohui Yang, Guoping Ren, Jie Ye, Shungui Zhou","doi":"10.1021/acs.est.4c05605","DOIUrl":"10.1021/acs.est.4c05605","url":null,"abstract":"<p><p>Bio-nano hybrids (BNH), combining semiconductors and microorganisms, have shown great promise for effective solar-to-fuel energy conversion. However, the high-energy ultraviolet (UV) photons in the solar spectrum can cause severe photocorrosion of semiconductors and irreversible photodamage to microorganisms within BNH. Here, we developed an encapsulation strategy using natural luminogens with aggregation-induced emission characteristics (AIEgens) to construct a protective layer for BNH, effectively shielding them against high-energy UV photons. We incorporated natural berberine (BBR) into the BNH composed of <i>Methanosarcina barkeri</i> and polymeric carbon nitrides (CN<sub><i>x</i></sub>). The self-assembled BNH-BBR system displayed a 2.75-fold higher CH<sub>4</sub> yield than BNH under simulated solar irradiation. Mechanism analysis revealed that BBR acted as a UV sunscreen for BNH by converting high-energy short wavelengths into low-energy long wavelengths, thereby reducing the accumulation of reactive oxygen species and alleviating the photocorrosion of CN<sub><i>x</i></sub>. Furthermore, BBR functioned as a photosynergist for BNH by regulating photoelectron production and utilization, enhancing the intracellular energy formation in <i>M. barkeri</i> for growth and metabolism. This work provides important insights into the effective and scalable conversion of CO<sub>2</sub> into valuable biofuels with BNH under light illumination containing high-energy photons.</p>","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":" ","pages":"20434-20443"},"PeriodicalIF":10.8,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142398695","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 : 2024-11-19Epub Date: 2024-11-05DOI: 10.1021/acs.est.4c06471
Jinha Kim, Scott W Leonard, Mariann Inga Van Meter, Mitchell L Kim-Fu, Dunping Cao, Jennifer A Field, Kung-Hui Chu
The unpredictable biodegradation of fluorotelomer (FT)-based per- and polyfluoroalkyl substances (PFAS) causes complicated risk management of PFAS-impacted sites. Here, we have successfully used redundancy analysis to link FT-based precursor biodegradation to key microbes and genes of soil microbiomes shaped by different classes of carbon sources: alcohols (C2-C4), alkanes (C6 and C8), an aromatic compound (phenol), or a hydrocarbon surfactant (cocamidopropyl betaine [CPB]). All the enrichments defluorinated fluorotelomer alcohols (n:2 FtOH; n = 4, 6, 8) effectively and grew on 6:2 fluorotelomer sulfonate (6:2 FtS) as a sulfur source. The butanol-enriched culture showed the highest defluorination extent for FtOHs and 6:2 FtS due to the high microbial diversity and the abundance of desulfonating and defluorinating genes. The CPB-enriched culture accumulated more 5:3 fluorotelomer carboxylic acid, suggesting unique roles of Variovorax and Pseudomonas. Enhanced 6:2 FtOH defluorination was observed due to a synergism between two enrichments with different carbon source classes except for those with phenol- and CPB-enriched cultures. While the 6:2 fluorotelomer sulfonamidoalkyl betaine was not degraded, trace levels of 6:2 fluorotelomer sulfonamidoalkyl amines were detected. The identified species and genes involved in desulfonation, defluorination, and carbon source metabolism are promising biomarkers for assessing precursor degradation at the sites.
{"title":"Nexus of Soil Microbiomes, Genes, Classes of Carbon Substrates, and Biotransformation of Fluorotelomer-Based Precursors.","authors":"Jinha Kim, Scott W Leonard, Mariann Inga Van Meter, Mitchell L Kim-Fu, Dunping Cao, Jennifer A Field, Kung-Hui Chu","doi":"10.1021/acs.est.4c06471","DOIUrl":"10.1021/acs.est.4c06471","url":null,"abstract":"<p><p>The unpredictable biodegradation of fluorotelomer (FT)-based per- and polyfluoroalkyl substances (PFAS) causes complicated risk management of PFAS-impacted sites. Here, we have successfully used redundancy analysis to link FT-based precursor biodegradation to key microbes and genes of soil microbiomes shaped by different classes of carbon sources: alcohols (C2-C4), alkanes (C6 and C8), an aromatic compound (phenol), or a hydrocarbon surfactant (cocamidopropyl betaine [CPB]). All the enrichments defluorinated fluorotelomer alcohols (<i>n</i>:2 FtOH; <i>n</i> = 4, 6, 8) effectively and grew on 6:2 fluorotelomer sulfonate (6:2 FtS) as a sulfur source. The butanol-enriched culture showed the highest defluorination extent for FtOHs and 6:2 FtS due to the high microbial diversity and the abundance of desulfonating and defluorinating genes. The CPB-enriched culture accumulated more 5:3 fluorotelomer carboxylic acid, suggesting unique roles of <i>Variovorax</i> and <i>Pseudomonas</i>. Enhanced 6:2 FtOH defluorination was observed due to a synergism between two enrichments with different carbon source classes except for those with phenol- and CPB-enriched cultures. While the 6:2 fluorotelomer sulfonamidoalkyl betaine was not degraded, trace levels of 6:2 fluorotelomer sulfonamidoalkyl amines were detected. The identified species and genes involved in desulfonation, defluorination, and carbon source metabolism are promising biomarkers for assessing precursor degradation at the sites.</p>","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":" ","pages":"20553-20565"},"PeriodicalIF":10.8,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11580179/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142581311","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yuemei Ye, Ivan A. Titaley, Mitchell L. Kim-Fu, Ansel R. Moll, Jennifer A. Field, Morton A. Barlaz
Per- and polyfluoroalkyl substances (PFAS) have been detected in plant fiber-based food packaging and most such packaging is disposed in landfills. The objective of this research was to evaluate the release of volatile PFAS to the gas-phase from PFAS-containing, single-use food packaging materials and from municipal solid waste (MSW) during anaerobic decomposition under simulated landfill conditions. After screening 46 materials for total F and 6:2 fluorotelomer alcohol (FTOH), packaging materials were classified as high or low F. High F materials included microwavable popcorn bags, natural plates, compostable bowls, biodegradable boxes, bagasse containers and eco-friendly plates, while the low F materials tested were paper plates, eco-friendly food trays and poly coated freezer paper. Summed PFAS release from the high F materials was 62–800 ng PFAS/g sample and 6:2 FTOH comprised 96.8–99.9% of the summed PFAS. The low F materials and MSW released 0.1–0.4 ng summed PFAS/g sample and 7:2-secondary (s) FTOH was the dominant volatile PFAS. PFAS were generally released early in the 123–285-day decomposition cycle, suggesting that some PFAS will be released prior to the installation of landfill gas collection systems. Nonetheless, PFAS have been reported in collected landfill gas, indicating that release occurs over many years.
在以植物纤维为基础的食品包装中检测到了全氟和多氟烷基物质(PFAS),而大多数此类包装都被丢弃在垃圾填埋场。这项研究的目的是评估在模拟垃圾填埋场条件下,含全氟烷基化合物的一次性食品包装材料和城市固体废物(MSW)在厌氧分解过程中挥发性全氟烷基化合物向气相的释放情况。高 F 值材料包括微波炉爆米花袋、天然盘子、可堆肥碗、可生物降解盒、甘蔗渣容器和环保盘子,而低 F 值材料则包括纸盘、环保食品托盘和聚酯涂层冷冻纸。高 F 值材料释放的全氟辛烷磺酸总和为 62-800 纳克 PFAS/克样品,其中 6:2 FTOH 占全氟辛烷磺酸总和的 96.8-99.9%。低 F 值材料和 MSW 释放的全氟辛烷磺酸总和为 0.1-0.4 纳克/克样品,7:2-secondary (s) FTOH 是主要的挥发性全氟辛烷磺酸。PFAS 一般在 123-285 天分解周期的早期释放,这表明一些 PFAS 会在安装填埋气体收集系统之前释放。不过,据报告,在收集的垃圾填埋气中也存在全氟辛烷磺酸,这表明释放会持续多年。
{"title":"Release of Volatile Per- and Polyfluoroalkyl Substances from Plant Fiber-Based Food Packaging and Municipal Solid Waste to Gas under Simulated Landfill Conditions","authors":"Yuemei Ye, Ivan A. Titaley, Mitchell L. Kim-Fu, Ansel R. Moll, Jennifer A. Field, Morton A. Barlaz","doi":"10.1021/acs.est.4c08544","DOIUrl":"https://doi.org/10.1021/acs.est.4c08544","url":null,"abstract":"Per- and polyfluoroalkyl substances (PFAS) have been detected in plant fiber-based food packaging and most such packaging is disposed in landfills. The objective of this research was to evaluate the release of volatile PFAS to the gas-phase from PFAS-containing, single-use food packaging materials and from municipal solid waste (MSW) during anaerobic decomposition under simulated landfill conditions. After screening 46 materials for total <i>F</i> and 6:2 fluorotelomer alcohol (FTOH), packaging materials were classified as high or low <i>F</i>. High <i>F</i> materials included microwavable popcorn bags, natural plates, compostable bowls, biodegradable boxes, bagasse containers and eco-friendly plates, while the low <i>F</i> materials tested were paper plates, eco-friendly food trays and poly coated freezer paper. Summed PFAS release from the high <i>F</i> materials was 62–800 ng PFAS/g sample and 6:2 FTOH comprised 96.8–99.9% of the summed PFAS. The low <i>F</i> materials and MSW released 0.1–0.4 ng summed PFAS/g sample and 7:2-secondary (s) FTOH was the dominant volatile PFAS. PFAS were generally released early in the 123–285-day decomposition cycle, suggesting that some PFAS will be released prior to the installation of landfill gas collection systems. Nonetheless, PFAS have been reported in collected landfill gas, indicating that release occurs over many years.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"7 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142673057","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 : 2024-11-19Epub Date: 2024-11-01DOI: 10.1021/acs.est.4c06014
Yi Jiao, Yulan Zhang, Xiaoping Wang, Ianina Altshuler, Fengwu Zhou, Mingliang Fang, Riikka Rinnan, Jianmin Chen, Zimeng Wang
Permafrost is a crucial part of the Earth's cryosphere. These millennia-old frozen soils not only are significant carbon reservoirs but also store a variety of chemicals. Accelerated permafrost thaw due to global warming leads to profound consequences such as infrastructure damage, hydrological changes, and, notably, environmental concerns from the release of various chemicals. In this perspective, we metaphorically term long-preserved substances as "dormant chemicals" that experience an "awakening" during permafrost thaw. We begin by providing a comprehensive overview and categorization of these chemicals and their potential transformations, utilizing a combination of field observations, laboratory studies, and modeling approaches to assess their environmental impacts. Following this, we put forward several perspectives on how to enhance the scientific understanding of their ensuing environmental impacts in the context of climate change. Ultimately, we advocate for broader research engagement in permafrost exploration and emphasize the need for extensive environmental chemical studies. This will significantly enhance our understanding of the consequences of permafrost thaw and its broader impact on other ecosystems under rapid climate warming.
{"title":"Awakening: Potential Release of Dormant Chemicals from Thawing Permafrost Soils under Climate Change.","authors":"Yi Jiao, Yulan Zhang, Xiaoping Wang, Ianina Altshuler, Fengwu Zhou, Mingliang Fang, Riikka Rinnan, Jianmin Chen, Zimeng Wang","doi":"10.1021/acs.est.4c06014","DOIUrl":"10.1021/acs.est.4c06014","url":null,"abstract":"<p><p>Permafrost is a crucial part of the Earth's cryosphere. These millennia-old frozen soils not only are significant carbon reservoirs but also store a variety of chemicals. Accelerated permafrost thaw due to global warming leads to profound consequences such as infrastructure damage, hydrological changes, and, notably, environmental concerns from the release of various chemicals. In this perspective, we metaphorically term long-preserved substances as \"dormant chemicals\" that experience an \"awakening\" during permafrost thaw. We begin by providing a comprehensive overview and categorization of these chemicals and their potential transformations, utilizing a combination of field observations, laboratory studies, and modeling approaches to assess their environmental impacts. Following this, we put forward several perspectives on how to enhance the scientific understanding of their ensuing environmental impacts in the context of climate change. Ultimately, we advocate for broader research engagement in permafrost exploration and emphasize the need for extensive environmental chemical studies. This will significantly enhance our understanding of the consequences of permafrost thaw and its broader impact on other ecosystems under rapid climate warming.</p>","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":" ","pages":"20336-20344"},"PeriodicalIF":10.8,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142556540","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}
Microplastics (MPs) have become a global hotspot due to their widespread distribution in recent years. MPs frequently interact with dissolved organic matter (DOM) and microbes, thereby influencing the carbon fate of soils. However, the role of plant presence in regulating MPs-mediated changes in the DOM and microbial structure remains unclear. Here, we compared the mechanisms of soil response to 3 common nonbiodegradable MPs in the absence or presence of radish (Raphanus sativus L. var. radculus Pers) plants. Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR-MS) analysis revealed that MPs reduced the chemodiversity and biodiversity of dissolved organic matter (DOM). MPs enhanced the degradation of lignin-like compounds and reduced the DOM stability. Comparative analysis showed that MPs caused less disturbance to the microbial composition and metabolism in planted soil than in unplanted soil. In unplanted soil, MPs stimulated fermentation while upregulating photoautotrophic activity in planted soil, thereby enhancing system stability. The rhizosphere effect mitigated MPs-induced CO2 emissions. Overall, our study highlights the crucial role of rhizosphere effects in maintaining ecosystem stability under soil microbe-DOM-pollutant interactions, which provides a theoretical basis for predicting the resistance, resilience, and transitions of the ecosystem upon exposure to the anthropogenic carbon source.
近年来,微塑料(MPs)的广泛分布已成为全球热点。微塑料经常与溶解有机物(DOM)和微生物相互作用,从而影响土壤中碳的归宿。然而,植物的存在在调节 MPs 介导的 DOM 和微生物结构变化中的作用仍不清楚。在此,我们比较了在没有或有萝卜(Raphanus sativus L. var.傅立叶变换离子回旋共振质谱(FT-ICR-MS)分析表明,MPs 降低了溶解有机物(DOM)的化学多样性和生物多样性。MPs 增强了木质素类化合物的降解,降低了 DOM 的稳定性。比较分析表明,与未种植土壤相比,MPs 对种植土壤中微生物组成和新陈代谢的干扰较小。在未种植土壤中,MPs 刺激了发酵,而在种植土壤中则提高了光自养活性,从而增强了系统稳定性。根圈效应减轻了 MPs 引起的二氧化碳排放。总之,我们的研究强调了根圈效应在土壤微生物-DOM-污染物相互作用下维持生态系统稳定性的关键作用,这为预测生态系统暴露于人为碳源时的抵抗力、恢复力和过渡提供了理论依据。
{"title":"Planting Enhances Soil Resistance to Microplastics: Evidence from Carbon Emissions and Dissolved Organic Matter Stability","authors":"Qi Wang, Weitao Liu, Qixing Zhou, Shuting Wang, Fan Mo, Xinyi Wu, Jianling Wang, Ruiying Shi, Xiang Li, Chuan Yin, Yuebing Sun","doi":"10.1021/acs.est.4c07189","DOIUrl":"https://doi.org/10.1021/acs.est.4c07189","url":null,"abstract":"Microplastics (MPs) have become a global hotspot due to their widespread distribution in recent years. MPs frequently interact with dissolved organic matter (DOM) and microbes, thereby influencing the carbon fate of soils. However, the role of plant presence in regulating MPs-mediated changes in the DOM and microbial structure remains unclear. Here, we compared the mechanisms of soil response to 3 common nonbiodegradable MPs in the absence or presence of radish (<i>Raphanus sativus</i> L. var. <i>radculus Pers</i>) plants. Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR-MS) analysis revealed that MPs reduced the chemodiversity and biodiversity of dissolved organic matter (DOM). MPs enhanced the degradation of lignin-like compounds and reduced the DOM stability. Comparative analysis showed that MPs caused less disturbance to the microbial composition and metabolism in planted soil than in unplanted soil. In unplanted soil, MPs stimulated fermentation while upregulating photoautotrophic activity in planted soil, thereby enhancing system stability. The rhizosphere effect mitigated MPs-induced CO<sub>2</sub> emissions. Overall, our study highlights the crucial role of rhizosphere effects in maintaining ecosystem stability under soil microbe-DOM-pollutant interactions, which provides a theoretical basis for predicting the resistance, resilience, and transitions of the ecosystem upon exposure to the anthropogenic carbon source.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"70 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142673143","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 : 2024-11-19Epub Date: 2024-11-04DOI: 10.1021/acs.est.4c04755
Yue Li, Zhongming Lu, Xiangru Zhang, Qingfu Zhang, Huifu Xu, Jimmy C H Fung, Glen Daigger
Investing in nonpotable water reuse (NPWR) is essential for circular urban water management. Existing research lacks methods to determine the number and capacities of NPWR plants (i.e., degree of decentralization) for large-scale applications in existing cities. We developed a spatial optimization framework in which the degree of decentralization emerges from the collective decisions of urban districts regarding where to send wastewater for reclamation and where to source water for nonpotable uses. We modified the genetic algorithm to optimize collective decisions with objectives including minimizing freshwater withdrawal, electricity consumption, and the cost of NPWR plants. Optimization results suggest an optimal number from one to eight among Pareto optimal solutions, with two to three being most common in Hong Kong. The cost-effective solutions suggest locations of NPWR plants in Kowloon and Hong Kong Island where NPWR demand is significant, while the electricity use for freshwater and seawater is high. The city could save about 6% freshwater and 29.4% seawater while consuming 20.7% more electricity. Overall, our spatial optimization framework provides a holistic evaluation of the optimal degree of decentralization for NPWR at the water-energy-cost nexus on an urban scale. Our findings serve as a benchmark to explore more energy-conscious planning strategies in Hong Kong.
{"title":"Multiobjective Spatial Optimization Framework for Determining the Optimal Degree of Decentralization for Nonpotable Water Reuse in Existing Cities: A Case Study of Hong Kong.","authors":"Yue Li, Zhongming Lu, Xiangru Zhang, Qingfu Zhang, Huifu Xu, Jimmy C H Fung, Glen Daigger","doi":"10.1021/acs.est.4c04755","DOIUrl":"10.1021/acs.est.4c04755","url":null,"abstract":"<p><p>Investing in nonpotable water reuse (NPWR) is essential for circular urban water management. Existing research lacks methods to determine the number and capacities of NPWR plants (i.e., degree of decentralization) for large-scale applications in existing cities. We developed a spatial optimization framework in which the degree of decentralization emerges from the collective decisions of urban districts regarding where to send wastewater for reclamation and where to source water for nonpotable uses. We modified the genetic algorithm to optimize collective decisions with objectives including minimizing freshwater withdrawal, electricity consumption, and the cost of NPWR plants. Optimization results suggest an optimal number from one to eight among Pareto optimal solutions, with two to three being most common in Hong Kong. The cost-effective solutions suggest locations of NPWR plants in Kowloon and Hong Kong Island where NPWR demand is significant, while the electricity use for freshwater and seawater is high. The city could save about 6% freshwater and 29.4% seawater while consuming 20.7% more electricity. Overall, our spatial optimization framework provides a holistic evaluation of the optimal degree of decentralization for NPWR at the water-energy-cost nexus on an urban scale. Our findings serve as a benchmark to explore more energy-conscious planning strategies in Hong Kong.</p>","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":" ","pages":"20424-20433"},"PeriodicalIF":10.8,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142574847","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 : 2024-11-19Epub Date: 2024-11-05DOI: 10.1021/acs.est.4c05009
Bin Shui, Ming Xu, Xiaowei Luo
Accelerated vehicle retirement is recognized as crucial for managing fleet emissions effectively. However, the emergence of new energy vehicles introduces complexities in assessing their environmental impacts. This study developed a dynamic fleet-based life cycle assessment model to analyze the effects of four distinct scrappage strategies in China from 2021 to 2060. The results underscore the importance of a meticulously chosen retirement strategy that harmonizes fleet characteristics with advancements in vehicle technology to promote sustainable mobility. Accelerated retirement strategies are demonstrated to enhance vehicle sales and expedite the incorporation of new energy vehicles into the fleet. Although these policies reduce greenhouse gas and carbon monoxide emissions, they may exacerbate other air pollutants, necessitating vigilant management. Additionally, the temporal distribution of environmental impacts reveals the critical need for long-term assessments. By evaluating six negative externalities of emissions, the research indicates that targeted scrappage policies, which advocate for the retirement of older vehicles, could potentially generate economic benefits of 6.81 to 7.29 billion dollars in reduced losses. However, an overly aggressive scrappage policy could increase negative externalities, leading to additional costs ranging from 0.84 to 3.31 billion dollars. This study reveals the intricate long-term environmental consequences of scrappage strategies accompanying the rise of new energy vehicles and lays a methodological groundwork for ongoing research into the most effective retirement scheme.
{"title":"Wheels of Change: The Environmental Paradox of Accelerating Vehicle Retirement Program.","authors":"Bin Shui, Ming Xu, Xiaowei Luo","doi":"10.1021/acs.est.4c05009","DOIUrl":"10.1021/acs.est.4c05009","url":null,"abstract":"<p><p>Accelerated vehicle retirement is recognized as crucial for managing fleet emissions effectively. However, the emergence of new energy vehicles introduces complexities in assessing their environmental impacts. This study developed a dynamic fleet-based life cycle assessment model to analyze the effects of four distinct scrappage strategies in China from 2021 to 2060. The results underscore the importance of a meticulously chosen retirement strategy that harmonizes fleet characteristics with advancements in vehicle technology to promote sustainable mobility. Accelerated retirement strategies are demonstrated to enhance vehicle sales and expedite the incorporation of new energy vehicles into the fleet. Although these policies reduce greenhouse gas and carbon monoxide emissions, they may exacerbate other air pollutants, necessitating vigilant management. Additionally, the temporal distribution of environmental impacts reveals the critical need for long-term assessments. By evaluating six negative externalities of emissions, the research indicates that targeted scrappage policies, which advocate for the retirement of older vehicles, could potentially generate economic benefits of 6.81 to 7.29 billion dollars in reduced losses. However, an overly aggressive scrappage policy could increase negative externalities, leading to additional costs ranging from 0.84 to 3.31 billion dollars. This study reveals the intricate long-term environmental consequences of scrappage strategies accompanying the rise of new energy vehicles and lays a methodological groundwork for ongoing research into the most effective retirement scheme.</p>","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":" ","pages":"20412-20423"},"PeriodicalIF":10.8,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142574848","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 : 2024-11-19Epub Date: 2024-11-06DOI: 10.1021/acs.est.4c09301
Ting Liu, Zhuo Xiong, Shengnan Deng, Han Wu, Xianhong Wang, Yuhan Huang, Zizhen Ma, Yan Tan, Huawei Zhang
A collaborative COS conversion of Hg0 in natural gas on the nitrogen-doped and copper oxide-supported carbon aerogel (0.9PPD-Cu/CA), which is synthesized by the p-phenylenediamine sources and carbon source of sodium alginate, was proposed to overcome the easy deactivation of the catalyst, high reaction temperature, and limited lifespan. At 40 °C, the 0.9PPD-Cu/CA presented a 100% COS conversion efficiency in the presence of H2O; meanwhile, the N doping realized the enhancement of basic density, leading to an improved COS conversion, and the intermediates H2S in the reaction were wholly adsorbed, implying that 0.9PPD-Cu/CA was a bifunctional carbon material. Furthermore, the Hg0 addition achieved a synergistic performance as well as higher COS yield and a significant lifetime period, in which the sulfur immediate could have a high reactive activity for Hg0 and the sulfate proportion would be alleviated as well. Subsequently, the catalyst poisoning would be alleviated after the protection of the collaborative process by strengthening the electron transfer, consuming the sulfur-based products, and accelerating the cleavage of the H-S bond. Finally, the synergetic mechanism on COS and Hg0 on 0.9PPD-Cu/CA was concluded according to the experimental results and sample analysis. Additionally, the effects of space velocity and the regeneration performance were explored.
为了克服催化剂易失活、反应温度高、寿命有限等问题,提出了在对苯二胺为源、海藻酸钠为碳源合成的氮掺杂氧化铜支撑碳气凝胶(0.9PPD-Cu/CA)上协同转化天然气中的Hg0的方法。在 40 ℃ 时,0.9PPD-Cu/CA 在 H2O 存在下的 COS 转化率为 100%;同时,N 掺杂实现了碱密度的增强,从而提高了 COS 转化率,并且完全吸附了反应中间产物 H2S,这意味着 0.9PPD-Cu/CA 是一种双功能碳材料。此外,Hg0 的添加实现了协同增效,提高了 COS 收率并延长了使用寿命,其中硫立即对 Hg0 具有较高的反应活性,硫酸盐的比例也得到缓解。随后,通过加强电子传递、消耗硫基产物和加速 H-S 键的裂解,保护协同过程后催化剂中毒现象将得到缓解。最后,根据实验结果和样品分析,得出了 0.9PPD-Cu/CA 上 COS 和 Hg0 的协同机理。此外,还探讨了空间速度和再生性能的影响。
{"title":"Deep Removal of COS and Hg<sup>0</sup> by Carbon Aerogel in Natural Gas: Good Antipoisoning Properties as well as Synergy Effect at Low Temperatures on 0.9PPD-Cu/CA Adsorbent.","authors":"Ting Liu, Zhuo Xiong, Shengnan Deng, Han Wu, Xianhong Wang, Yuhan Huang, Zizhen Ma, Yan Tan, Huawei Zhang","doi":"10.1021/acs.est.4c09301","DOIUrl":"10.1021/acs.est.4c09301","url":null,"abstract":"<p><p>A collaborative COS conversion of Hg<sup>0</sup> in natural gas on the nitrogen-doped and copper oxide-supported carbon aerogel (0.9PPD-Cu/CA), which is synthesized by the <i>p</i>-phenylenediamine sources and carbon source of sodium alginate, was proposed to overcome the easy deactivation of the catalyst, high reaction temperature, and limited lifespan. At 40 °C, the 0.9PPD-Cu/CA presented a 100% COS conversion efficiency in the presence of H<sub>2</sub>O; meanwhile, the N doping realized the enhancement of basic density, leading to an improved COS conversion, and the intermediates H<sub>2</sub>S in the reaction were wholly adsorbed, implying that 0.9PPD-Cu/CA was a bifunctional carbon material. Furthermore, the Hg<sup>0</sup> addition achieved a synergistic performance as well as higher COS yield and a significant lifetime period, in which the sulfur immediate could have a high reactive activity for Hg<sup>0</sup> and the sulfate proportion would be alleviated as well. Subsequently, the catalyst poisoning would be alleviated after the protection of the collaborative process by strengthening the electron transfer, consuming the sulfur-based products, and accelerating the cleavage of the H-S bond. Finally, the synergetic mechanism on COS and Hg<sup>0</sup> on 0.9PPD-Cu/CA was concluded according to the experimental results and sample analysis. Additionally, the effects of space velocity and the regeneration performance were explored.</p>","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":" ","pages":"20598-20606"},"PeriodicalIF":10.8,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142581305","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}