Binyu Xiao, Gehui Wang, Zheng Li, Rongjie Li, Chenlong Liang, Haoyang Wang, Si Zhang, Can Wu, Rui Li, Fan Zhang, Renjian Zhang, Yunfei Wu, Lei Zhang
To better understand the sources and formation mechanisms of atmospheric brown carbon (BrC) in China haze, an intensive field observation was conducted in the North China Plain (NCP) during the 2023 winter. Our results showed that compared to that (28%) in dry haze, the contribution of secondary formation to BrC was significantly enhanced during humid haze, accounting for 46% of BrC production with the aqueous-phase reaction as the dominant formation pathway. The strong correlations between light absorption at λ365nm and water-soluble organic nitrogen compounds, particularly imidazoles (IMs), indicated a key role of nitrogen-containing organic compounds in the aqueous-phase BrC formation process. In the humid haze, IMs are largely produced by liquid-phase reactions of carbonyls with amines and free ammonia (NH3(aq)), which accounted for 57% of the total IMs in the humid haze events. Amines produced IMs more efficiently and less pH dependent than NH3(aq), with alkyl IMs and oxidized IMs being their products, respectively. Both types of BrC increased with increasing levels of amines and NH3(aq) during humid haze, suggesting their enhancing roles in BrC formation in China haze, which should be accounted for by models for better simulating the physicochemical characteristics and climate effects of atmospheric BrC.
{"title":"High Contribution of Secondary Formation to Brown Carbon in China Humid Haze: Enhancing Role of Ammonia and Amines","authors":"Binyu Xiao, Gehui Wang, Zheng Li, Rongjie Li, Chenlong Liang, Haoyang Wang, Si Zhang, Can Wu, Rui Li, Fan Zhang, Renjian Zhang, Yunfei Wu, Lei Zhang","doi":"10.1021/acs.est.5c13436","DOIUrl":"https://doi.org/10.1021/acs.est.5c13436","url":null,"abstract":"To better understand the sources and formation mechanisms of atmospheric brown carbon (BrC) in China haze, an intensive field observation was conducted in the North China Plain (NCP) during the 2023 winter. Our results showed that compared to that (28%) in dry haze, the contribution of secondary formation to BrC was significantly enhanced during humid haze, accounting for 46% of BrC production with the aqueous-phase reaction as the dominant formation pathway. The strong correlations between light absorption at λ<sub>365nm</sub> and water-soluble organic nitrogen compounds, particularly imidazoles (IMs), indicated a key role of nitrogen-containing organic compounds in the aqueous-phase BrC formation process. In the humid haze, IMs are largely produced by liquid-phase reactions of carbonyls with amines and free ammonia (NH<sub>3</sub>(aq)), which accounted for 57% of the total IMs in the humid haze events. Amines produced IMs more efficiently and less pH dependent than NH<sub>3</sub>(aq), with alkyl IMs and oxidized IMs being their products, respectively. Both types of BrC increased with increasing levels of amines and NH<sub>3</sub>(aq) during humid haze, suggesting their enhancing roles in BrC formation in China haze, which should be accounted for by models for better simulating the physicochemical characteristics and climate effects of atmospheric BrC.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"28 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-12-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145732207","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}
Noah Lim, Alessandro Del Ponte, Lina Ang, Wei Jie Seow
Using a nationally representative quota sample of 10,618 participants from 1372 localities from the ten most populous countries in the world (Bangladesh, Brazil, China, India, Indonesia, Mexico, Nigeria, Pakistan, Russia, and the United States), we assessed the association between fine particulate matter (PM2.5) exposure and air quality knowledge (AQ-IQ). Additionally, we evaluated which demographics are more vulnerable to PM2.5 exposure amid a low AQ-IQ. PM2.5 concentrations were estimated based on satellite observations and data from ground monitoring stations, while AQ-IQ was measured using ten items pertaining to general knowledge, knowledge specific to the air quality index, and knowledge of best practices about air quality. Annual average PM2.5 levels in these countries varied significantly, ranging from 7.58 μg/m3 in the US to 78.00 μg/m3 in Bangladesh. We found that AQ-IQ is the highest in Mexico and China and the lowest in Bangladesh and Nigeria. Moreover, women, as well as people who live in rural areas, are single, lack a college education, are politically conservative, and currently smoke know less about air quality (p < 0.05). Overall, the findings indicate that people who are most exposed to air pollution are significantly less knowledgeable about air quality.
{"title":"Global Populations Vulnerable to Air Pollution Know Less about Air Quality","authors":"Noah Lim, Alessandro Del Ponte, Lina Ang, Wei Jie Seow","doi":"10.1021/acs.est.5c07862","DOIUrl":"https://doi.org/10.1021/acs.est.5c07862","url":null,"abstract":"Using a nationally representative quota sample of 10,618 participants from 1372 localities from the ten most populous countries in the world (Bangladesh, Brazil, China, India, Indonesia, Mexico, Nigeria, Pakistan, Russia, and the United States), we assessed the association between fine particulate matter (PM<sub>2.5</sub>) exposure and air quality knowledge (AQ-IQ). Additionally, we evaluated which demographics are more vulnerable to PM<sub>2.5</sub> exposure amid a low AQ-IQ. PM<sub>2.5</sub> concentrations were estimated based on satellite observations and data from ground monitoring stations, while AQ-IQ was measured using ten items pertaining to general knowledge, knowledge specific to the air quality index, and knowledge of best practices about air quality. Annual average PM<sub>2.5</sub> levels in these countries varied significantly, ranging from 7.58 μg/m<sup>3</sup> in the US to 78.00 μg/m<sup>3</sup> in Bangladesh. We found that AQ-IQ is the highest in Mexico and China and the lowest in Bangladesh and Nigeria. Moreover, women, as well as people who live in rural areas, are single, lack a college education, are politically conservative, and currently smoke know less about air quality (<i>p</i> < 0.05). Overall, the findings indicate that people who are most exposed to air pollution are significantly less knowledgeable about air quality.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"15 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145732628","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}
Qiong Zhang, Jiayou Ge, Fengjie Liu, Shabaz Mohammed, Kedong Yin, Rosalind E. M. Rickaby
Metalloproteins, which can bind with one or more metals, are the basis of many important biological processes in a marine environment. The metalloproteome data for phytoplankton are limited, hindering our understanding of trace metal requirements and their biological function in these primary producers. Here, we conducted a semiquantitative analysis of metal requirements using a protein modeling approach across several phytoplankton species, including the chlorophytes Ostreococcus tauri and Chlamydomonas reinhardtii, the haptophyte Geophyracapsa huxleyi, and the cyanobacterium Synechocystis. Our results show strong alignment between trace metal requirements inferred from the proteome and those measured by ICP-MS, with the metalloproteome providing deeper insights into the biological roles of each metal compared with ICP-MS, which indicates only cellular metal abundance. Among all metalloproteins, those containing Mg are the most abundant in all phytoplankton studied here. Among the trace elements, Zn, Fe, and Mn are the most abundant cofactors found in phytoplankton proteins. The cyanobacterium has a much higher percentage of Fe in its expressed proteome compared to the eukaryotes studied here, agreeing with findings from previous comparative genomic studies that trace element requirements are different in prokaryotic and eukaryotic phytoplankton. Using G. huxleyi strains from distinct oceanic environments, we further demonstrated that their metalloproteome can be used to identify limiting metals and understand the strategies that phytoplankton use to adapt to specific environments. These findings enhance our understanding of the interactions between biota and their metal environments.
{"title":"Unlocking Phytoplankton Metallomes with Comparative Analysis of Metal Quotas, Quantitative Proteomics, and Inferred Metalloproteomes","authors":"Qiong Zhang, Jiayou Ge, Fengjie Liu, Shabaz Mohammed, Kedong Yin, Rosalind E. M. Rickaby","doi":"10.1021/acs.est.5c11233","DOIUrl":"https://doi.org/10.1021/acs.est.5c11233","url":null,"abstract":"Metalloproteins, which can bind with one or more metals, are the basis of many important biological processes in a marine environment. The metalloproteome data for phytoplankton are limited, hindering our understanding of trace metal requirements and their biological function in these primary producers. Here, we conducted a semiquantitative analysis of metal requirements using a protein modeling approach across several phytoplankton species, including the chlorophytes <i>Ostreococcus tauri</i> and <i>Chlamydomonas reinhardtii</i>, the haptophyte <i>Geophyracapsa huxleyi</i>, and the cyanobacterium <i>Synechocystis</i>. Our results show strong alignment between trace metal requirements inferred from the proteome and those measured by ICP-MS, with the metalloproteome providing deeper insights into the biological roles of each metal compared with ICP-MS, which indicates only cellular metal abundance. Among all metalloproteins, those containing Mg are the most abundant in all phytoplankton studied here. Among the trace elements, Zn, Fe, and Mn are the most abundant cofactors found in phytoplankton proteins. The cyanobacterium has a much higher percentage of Fe in its expressed proteome compared to the eukaryotes studied here, agreeing with findings from previous comparative genomic studies that trace element requirements are different in prokaryotic and eukaryotic phytoplankton. Using <i>G. huxleyi</i> strains from distinct oceanic environments, we further demonstrated that their metalloproteome can be used to identify limiting metals and understand the strategies that phytoplankton use to adapt to specific environments. These findings enhance our understanding of the interactions between biota and their metal environments.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"36 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145728921","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}
Heterogeneous catalytic ozonation (HCO) is widely used for degrading organic contaminants in wastewater, yet its efficiency is severely compromised in high-salinity environments due to the quenching of hydroxyl radicals (HO•) by common background anions. Herein, we report the rational evolution from single-atom to diatomic Co catalysts (Co-DAC), which precisely regulate the adsorption configuration of O3 and switch the dominant reactive oxygen species from nonselective HO• to highly selective Co(IV)═O species. In contrast to the end-on O3 adsorption on an isolated single-atom site, the adjacent dual Co atoms favor a bridge-like O3 adsorption configuration with a more symmetric charge distribution, which facilitates homolytic O-O bond cleavage and thus promotes Co(IV)═O formation. Consequently, the Co-DAC/O3 system exhibits exceptional resistance to high salinity (100 mM Cl-) and achieves a record-high mass activity (0.90 mmol g-1 min-1) of oxalic acid removal. As a proof of concept, a carbon nanotube-supported Co-DAC membrane is equipped in a flow-through reactor to intensify convective mass transfer, yielding a 162-fold increase in the decontamination rate over a conventional batch configuration. This work not only advances the mechanistic understanding of O3 activation on diatomic sites but also provides a scalable solution for treating refractory organic pollutants in high-salinity wastewater.
{"title":"Selective Generation of Co(IV)-Oxo Species in Catalytic Ozonation Process for Effective Decontamination of High-Salinity Wastewater.","authors":"Yinhao Dai,Hongyu Dong,Fuqiang Liu,Chenyang Gao,Wei Chen,Xuelu Wang,Deyong Yang,Xiaoguang Duan,Xiaohong Guan","doi":"10.1021/acs.est.5c12008","DOIUrl":"https://doi.org/10.1021/acs.est.5c12008","url":null,"abstract":"Heterogeneous catalytic ozonation (HCO) is widely used for degrading organic contaminants in wastewater, yet its efficiency is severely compromised in high-salinity environments due to the quenching of hydroxyl radicals (HO•) by common background anions. Herein, we report the rational evolution from single-atom to diatomic Co catalysts (Co-DAC), which precisely regulate the adsorption configuration of O3 and switch the dominant reactive oxygen species from nonselective HO• to highly selective Co(IV)═O species. In contrast to the end-on O3 adsorption on an isolated single-atom site, the adjacent dual Co atoms favor a bridge-like O3 adsorption configuration with a more symmetric charge distribution, which facilitates homolytic O-O bond cleavage and thus promotes Co(IV)═O formation. Consequently, the Co-DAC/O3 system exhibits exceptional resistance to high salinity (100 mM Cl-) and achieves a record-high mass activity (0.90 mmol g-1 min-1) of oxalic acid removal. As a proof of concept, a carbon nanotube-supported Co-DAC membrane is equipped in a flow-through reactor to intensify convective mass transfer, yielding a 162-fold increase in the decontamination rate over a conventional batch configuration. This work not only advances the mechanistic understanding of O3 activation on diatomic sites but also provides a scalable solution for treating refractory organic pollutants in high-salinity wastewater.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"150 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145728420","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}
China’s 2060 carbon neutrality target is critical for mitigating air pollution and safeguarding public health. However, the potential variations in the expected benefits across different carbon neutrality strategies and the associated distributional impacts remain unclear. Here, we established three representative technological pathways toward carbon neutrality, and investigated their multifaceted health benefits in terms of improved ambient and indoor air quality in China. We found that, relative to a no-carbon-neutrality baseline, a high solar and wind scenario yields the largest reductions in ambient and additional indoor PM2.5 concentration (6.0 and 7.0 μg m–3) and averts 1.5 (1.2–1.8) million premature deaths in 2060; this almost quadruples avoided deaths under a high biomass energy scenario and doubles that under a high carbon capture and storage scenario. After subtraction of costs, the net benefits of the high solar and wind scenario are up to 5.9 times those of other scenarios, and are the highest across provinces with varying income levels. However, the high solar and wind scenario imposes 2–3 times the costs on low-income provinces compared to other scenarios, suggesting that distributional policies, such as interprovincial financial transfer from higher- to low-income provinces, could be implemented for a more stable transition.
{"title":"Different Carbon Neutrality Strategies Induce Substantially Divergent Health Benefits and Distributional Impacts in China","authors":"Da Gao, Chenfei Qu, Bin Zhao, Shuxiao Wang, Xiaodan Huang, Yisheng Sun, Yueqi Jiang, Zhongfeng Xu, Xiaocong Wang, Yicong He, Jiewen Shen, Dejia Yin, Haotian Zheng, Hongrong Shi, Zhe Jiang, Xiao-Wen Zeng, Yun Zhu, Biwu Chu, Hong He, Xiliang Zhang, Da Zhang","doi":"10.1021/acs.est.5c12120","DOIUrl":"https://doi.org/10.1021/acs.est.5c12120","url":null,"abstract":"China’s 2060 carbon neutrality target is critical for mitigating air pollution and safeguarding public health. However, the potential variations in the expected benefits across different carbon neutrality strategies and the associated distributional impacts remain unclear. Here, we established three representative technological pathways toward carbon neutrality, and investigated their multifaceted health benefits in terms of improved ambient and indoor air quality in China. We found that, relative to a no-carbon-neutrality baseline, a high solar and wind scenario yields the largest reductions in ambient and additional indoor PM<sub>2.5</sub> concentration (6.0 and 7.0 μg m<sup>–3</sup>) and averts 1.5 (1.2–1.8) million premature deaths in 2060; this almost quadruples avoided deaths under a high biomass energy scenario and doubles that under a high carbon capture and storage scenario. After subtraction of costs, the net benefits of the high solar and wind scenario are up to 5.9 times those of other scenarios, and are the highest across provinces with varying income levels. However, the high solar and wind scenario imposes 2–3 times the costs on low-income provinces compared to other scenarios, suggesting that distributional policies, such as interprovincial financial transfer from higher- to low-income provinces, could be implemented for a more stable transition.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"101 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145728916","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}
Although the importance of transgenerational effects and multiple stressors in ecotoxicology is well-established, transgenerational interactions between toxicants and natural stressors remain largely unexplored, yet are critical for advancing ecological risk assessment. In this study, we exposed the water flea Daphnia magna to a heat spike (25 °C vs 32 °C) followed by exposure to chlorpyrifos at an environmentally relevant concentration (0.5 μg/L) across the parental and grand-offspring generations using a full-factorial design. In both generations, chlorpyrifos reduced survival and acute heat tolerance, which, as expected, were further magnified by the preceding heat spike. Notably, parental exposure to chlorpyrifos decreased the sensitivity of grand-offspring to the toxicant, and more strikingly, offset the synergistic interaction between the heat spike and chlorpyrifos. Both the increased toxicity of the pesticide after exposure to the heat spike and the mitigating impact of the transgenerational effects on this synergism could be explained by changes in acetylcholinesterase activity and hemoglobin concentration. These findings underscore the critical role of transgenerational effects in ecotoxicology, including their potential to shape toxicant–warming interactions. Our results emphasize the necessity of incorporating transgenerational effects and multistressor scenarios into ecological risk assessments of toxicants in the context of global warming.
虽然跨代效应和多重压力源在生态毒理学中的重要性已经确立，但毒物和自然压力源之间的跨代相互作用在很大程度上仍未被探索，但对推进生态风险评估至关重要。在本研究中，我们采用全因子设计，将大水蚤暴露于高温峰值（25°C vs 32°C），然后在亲代和后代中暴露于环境相关浓度（0.5 μg/L）的毒死蜱。在这两代中，毒死蜱降低了存活率和急性耐热性，正如预期的那样，这被之前的高温峰值进一步放大了。值得注意的是，亲代接触毒死蜱降低了后代对毒物的敏感性，更引人注目的是，抵消了高温峰值和毒死蜱之间的协同相互作用。暴露于高温峰后农药毒性的增加和跨代效应对这种协同作用的缓解作用都可以用乙酰胆碱酯酶活性和血红蛋白浓度的变化来解释。这些发现强调了跨代效应在生态毒理学中的关键作用，包括它们形成毒物-变暖相互作用的潜力。我们的研究结果强调了将跨代效应和多应激情景纳入全球变暖背景下毒物生态风险评估的必要性。
{"title":"Adaptive Transgenerational Effects Offset the Increased Toxicity of the Pesticide Chlorpyrifos under Heat Stress","authors":"Shandong Meng, Xiaowei Jin, Wei Xiong, Robby Stoks, Aibin Zhan","doi":"10.1021/acs.est.5c09369","DOIUrl":"https://doi.org/10.1021/acs.est.5c09369","url":null,"abstract":"Although the importance of transgenerational effects and multiple stressors in ecotoxicology is well-established, transgenerational interactions between toxicants and natural stressors remain largely unexplored, yet are critical for advancing ecological risk assessment. In this study, we exposed the water flea <i>Daphnia magna</i> to a heat spike (25 °C vs 32 °C) followed by exposure to chlorpyrifos at an environmentally relevant concentration (0.5 μg/L) across the parental and grand-offspring generations using a full-factorial design. In both generations, chlorpyrifos reduced survival and acute heat tolerance, which, as expected, were further magnified by the preceding heat spike. Notably, parental exposure to chlorpyrifos decreased the sensitivity of grand-offspring to the toxicant, and more strikingly, offset the synergistic interaction between the heat spike and chlorpyrifos. Both the increased toxicity of the pesticide after exposure to the heat spike and the mitigating impact of the transgenerational effects on this synergism could be explained by changes in acetylcholinesterase activity and hemoglobin concentration. These findings underscore the critical role of transgenerational effects in ecotoxicology, including their potential to shape toxicant–warming interactions. Our results emphasize the necessity of incorporating transgenerational effects and multistressor scenarios into ecological risk assessments of toxicants in the context of global warming.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"19 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145732209","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}
Jonas K. LaPier, Yu-Jung Liu, Jacob F. King, Théotime Béguerie, Ange Nzihou, William A. Mitch
Both legacy (e.g., polybrominated diphenyl ethers; PBDEs) and emerging (e.g., hexabromobenzene) flame retardants frequently feature brominated aromatic motifs, which are associated with persistent and bioaccumulative properties. While activated carbon has been used to treat brominated aromatics, it is a passive sorbent and does not degrade them. Using model bromobenzenes, this study illustrates debromination of brominated aromatics sorbed to activated carbon when the carbon is fashioned into cathodes and treated at a −1.3 V/SHE applied potential. Debromination rates fit a quantitative structure–activity relationship (QSAR), increasing with increasing free energy changes (ΔG) for a two-electron transfer to the brominated aromatic. Half-lives ranged from ∼4 min for hexabromobenzene to ∼15 d for bromobenzene, although the debromination half-life for bromobenzene decreased to ∼50 h at −1.8 V/SHE. The QSAR for bromobenzene debromination was also predictive for debromination of two PBDEs (BDE-99 and BDE-47), indicating that the QSAR was broadly applicable across brominated aromatic structures. Debromination released bromide to the catholyte, while lower-order brominated aromatic intermediates remained sorbed to the cathode. Debromination rates roughly correlated with the conductivity of the black carbon. The strong sorption capacity of carbon-based cathodes permits sequestration of brominated aromatics from contaminated waters within short hydraulic residence times, while an electric potential can be periodically applied to debrominate contaminants sequestered on the carbon.
{"title":"Electrochemical Debromination of Brominated Aromatic Flame Retardants Using Activated Carbon-Based Cathodes","authors":"Jonas K. LaPier, Yu-Jung Liu, Jacob F. King, Théotime Béguerie, Ange Nzihou, William A. Mitch","doi":"10.1021/acs.est.5c03324","DOIUrl":"https://doi.org/10.1021/acs.est.5c03324","url":null,"abstract":"Both legacy (e.g., polybrominated diphenyl ethers; PBDEs) and emerging (e.g., hexabromobenzene) flame retardants frequently feature brominated aromatic motifs, which are associated with persistent and bioaccumulative properties. While activated carbon has been used to treat brominated aromatics, it is a passive sorbent and does not degrade them. Using model bromobenzenes, this study illustrates debromination of brominated aromatics sorbed to activated carbon when the carbon is fashioned into cathodes and treated at a −1.3 V/SHE applied potential. Debromination rates fit a quantitative structure–activity relationship (QSAR), increasing with increasing free energy changes (Δ<i>G</i>) for a two-electron transfer to the brominated aromatic. Half-lives ranged from ∼4 min for hexabromobenzene to ∼15 d for bromobenzene, although the debromination half-life for bromobenzene decreased to ∼50 h at −1.8 V/SHE. The QSAR for bromobenzene debromination was also predictive for debromination of two PBDEs (BDE-99 and BDE-47), indicating that the QSAR was broadly applicable across brominated aromatic structures. Debromination released bromide to the catholyte, while lower-order brominated aromatic intermediates remained sorbed to the cathode. Debromination rates roughly correlated with the conductivity of the black carbon. The strong sorption capacity of carbon-based cathodes permits sequestration of brominated aromatics from contaminated waters within short hydraulic residence times, while an electric potential can be periodically applied to debrominate contaminants sequestered on the carbon.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"11 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145728851","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}
Pengcheng Zhao, Peihua Wang, Nan Zhang, Tze Hau Lam, Huanhuan Wang, Jiquan Liu, Yuguo Li
Particles such as allergens and pathogens can invade indoor environments via human activities, affecting occupant health and indoor microbiota. However, the particle transmission dynamics and distribution patterns remain underexplored. In this study, Lactobacillus strains were applied as tracers to the palms and shirtfronts of adults in four families, whereafter they were dispersed into the residential environments overnight through routine activities. The target genes of the tracers were detected in over 80% of the extracted surface samples. While touch events and contamination were both concentrated on specific surfaces, frequent touching did not correspond to high contamination. Instead, contamination levels were affected by a combination of factors, including the sequence of surface touches and the promptness of handwashing. Additionally, resuspension redistributed tracers more uniformly across surfaces, with tracer concentrations on air-conditioning filters being twice the median value for all environmental samples. Accordingly, we established a physical model that predicts tracer distribution considering surface touch and resuspension. Based on the modeling results, hand-seeded and shirt-seeded contaminants were reduced more effectively through prompt handwashing and shirt changing upon entering home than by cleaning multiple surfaces at a later time. These findings provide insights into the dynamic processes underlying indoor infection, hygiene, and microbiota.
{"title":"Experimental Tracing and Modeling of Exogenous Microbe Dynamics in Home Environments","authors":"Pengcheng Zhao, Peihua Wang, Nan Zhang, Tze Hau Lam, Huanhuan Wang, Jiquan Liu, Yuguo Li","doi":"10.1021/acs.est.5c06069","DOIUrl":"https://doi.org/10.1021/acs.est.5c06069","url":null,"abstract":"Particles such as allergens and pathogens can invade indoor environments via human activities, affecting occupant health and indoor microbiota. However, the particle transmission dynamics and distribution patterns remain underexplored. In this study, <i>Lactobacillus</i> strains were applied as tracers to the palms and shirtfronts of adults in four families, whereafter they were dispersed into the residential environments overnight through routine activities. The target genes of the tracers were detected in over 80% of the extracted surface samples. While touch events and contamination were both concentrated on specific surfaces, frequent touching did not correspond to high contamination. Instead, contamination levels were affected by a combination of factors, including the sequence of surface touches and the promptness of handwashing. Additionally, resuspension redistributed tracers more uniformly across surfaces, with tracer concentrations on air-conditioning filters being twice the median value for all environmental samples. Accordingly, we established a physical model that predicts tracer distribution considering surface touch and resuspension. Based on the modeling results, hand-seeded and shirt-seeded contaminants were reduced more effectively through prompt handwashing and shirt changing upon entering home than by cleaning multiple surfaces at a later time. These findings provide insights into the dynamic processes underlying indoor infection, hygiene, and microbiota.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"16 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145728908","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}
Haoquan Zhang, Haiyan Yu, Zhan Wang, Yue Qing, Minyuan Han, Jin Ye, Le Han
The ammonia recovery from wastewater via a concentration-driven membrane stripping process is highly promising yet constrained by the trade-off issue between ammonia permeability and antiwettability of hydrophobic gas-permeable membranes (GPMs). We designated a tailored hierarchical-porous GPM (HGPM) via a facile fabrication method to address the above issue and established its transfer model, clearly illustrating the ammonia diffusion across the distinct layers. Molecular diffusion across the finger-like layer of HGPMs was responsible for a superior overall mass transfer coefficient of 3.3 × 10–5 m/s. Meanwhile, its nanoscale pores in the top-skin and sponge-like layers conferred commendable wetting resistance against neighboring alkaline or acidic liquids, with the liquid entrance pressure measured at 182 kPa. The hierarchy of HGPMs together achieved the best-ever balance between ammonia permeability and antiwettability (both increased up to ∼150–200% of the commercial GPMs), significantly breaking the upper bound limit. Dealing with the real wastewater from anaerobic digestate, HGPMs demonstrated a robust ammonia recovery flux of 75–80 g N/m2 h over 50 h, 3 times higher than that of the commercial GPMs. This work sheds light on the effective recovery of volatile valuable compounds from complex wastewater, with the as-tailored membrane of great upscalability holding great potential toward a future circular society.
{"title":"Hierarchical-Porous Gas-Permeable Membrane toward Efficient and Robust Ammonia Recovery","authors":"Haoquan Zhang, Haiyan Yu, Zhan Wang, Yue Qing, Minyuan Han, Jin Ye, Le Han","doi":"10.1021/acs.est.5c10757","DOIUrl":"https://doi.org/10.1021/acs.est.5c10757","url":null,"abstract":"The ammonia recovery from wastewater via a concentration-driven membrane stripping process is highly promising yet constrained by the trade-off issue between ammonia permeability and antiwettability of hydrophobic gas-permeable membranes (GPMs). We designated a tailored hierarchical-porous GPM (HGPM) via a facile fabrication method to address the above issue and established its transfer model, clearly illustrating the ammonia diffusion across the distinct layers. Molecular diffusion across the finger-like layer of HGPMs was responsible for a superior overall mass transfer coefficient of 3.3 × 10<sup>–5</sup> m/s. Meanwhile, its nanoscale pores in the top-skin and sponge-like layers conferred commendable wetting resistance against neighboring alkaline or acidic liquids, with the liquid entrance pressure measured at 182 kPa. The hierarchy of HGPMs together achieved the best-ever balance between ammonia permeability and antiwettability (both increased up to ∼150–200% of the commercial GPMs), significantly breaking the upper bound limit. Dealing with the real wastewater from anaerobic digestate, HGPMs demonstrated a robust ammonia recovery flux of 75–80 g N/m<sup>2</sup> h over 50 h, 3 times higher than that of the commercial GPMs. This work sheds light on the effective recovery of volatile valuable compounds from complex wastewater, with the as-tailored membrane of great upscalability holding great potential toward a future circular society.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"22 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145728909","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}
Lili Wang, Xiaonan Lu, Yao Yao, Xing Liu, Tida Ge, Yu Luo, Hanzhong Jia, Lukas Van Zwieten, Georg Guggenberger
The widespread contamination of paddy soils with microplastics (MPs) has the potential to significantly influence the global carbon (C) cycle. While there are reports of MPs affecting methane (CH4) emissions from paddy soil, the mechanisms, especially associated with the aging of different types of MPs, remain unknown. To address this paucity in knowledge and better understand and quantify the role of MPs and aged MPs on CH4 emissions, we conducted a microcosm experiment using paddy soil amended with pristine and aged polyethylene (PE) and polylactic acid (PLA). Our results showed that MPs inhibited CH4 emissions with pristine PLA lowering cumulative CH4 emissions from 6.80 to 4.90 μM/g soil over a 50 day incubation, while pristine PE was less effective by lowering emissions to 5.50 μM/g soil (P < 0.05). Interestingly, aging of PE increased the efficacy of CH4 mitigation, while aging of PLA lowered its efficacy. Mechanistic analyses revealed that aged PE, in contrast to pristine PE, decreased the ratio of methanogenesis to CH4 oxidation gene abundance. In comparison, the aging of PLA confers its role as an electron shuttle, facilitating the transfer of electrons from Geobacteraceae to nitrates and iron minerals, thereby competing with the methanogenic process for electrons and substrates, and thus inhibiting methanogenesis. Our study provides key evidence with supporting mechanisms showing that aging of MPs influences the emissions of CH4 from paddy soils, with the results having importance in national greenhouse gas inventories and their abatement.
{"title":"Mechanisms Associated with Lower Methane Emissions from Paddy Soil by Aged Polylactic Acid Microplastics","authors":"Lili Wang, Xiaonan Lu, Yao Yao, Xing Liu, Tida Ge, Yu Luo, Hanzhong Jia, Lukas Van Zwieten, Georg Guggenberger","doi":"10.1021/acs.est.5c11590","DOIUrl":"https://doi.org/10.1021/acs.est.5c11590","url":null,"abstract":"The widespread contamination of paddy soils with microplastics (MPs) has the potential to significantly influence the global carbon (C) cycle. While there are reports of MPs affecting methane (CH<sub>4</sub>) emissions from paddy soil, the mechanisms, especially associated with the aging of different types of MPs, remain unknown. To address this paucity in knowledge and better understand and quantify the role of MPs and aged MPs on CH<sub>4</sub> emissions, we conducted a microcosm experiment using paddy soil amended with pristine and aged polyethylene (PE) and polylactic acid (PLA). Our results showed that MPs inhibited CH<sub>4</sub> emissions with pristine PLA lowering cumulative CH<sub>4</sub> emissions from 6.80 to 4.90 μM/g soil over a 50 day incubation, while pristine PE was less effective by lowering emissions to 5.50 μM/g soil (<i>P</i> < 0.05). Interestingly, aging of PE increased the efficacy of CH<sub>4</sub> mitigation, while aging of PLA lowered its efficacy. Mechanistic analyses revealed that aged PE, in contrast to pristine PE, decreased the ratio of methanogenesis to CH<sub>4</sub> oxidation gene abundance. In comparison, the aging of PLA confers its role as an electron shuttle, facilitating the transfer of electrons from <i>Geobacteraceae</i> to nitrates and iron minerals, thereby competing with the methanogenic process for electrons and substrates, and thus inhibiting methanogenesis. Our study provides key evidence with supporting mechanisms showing that aging of MPs influences the emissions of CH<sub>4</sub> from paddy soils, with the results having importance in national greenhouse gas inventories and their abatement.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"14611 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145732210","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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