IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2024-09-19 DOI: 10.1021/acs.est.4c07539

Haoxin Li, Ziyi Li, Xi Zhang, Wenjun Sun, Xiuwei Ao, Zifu Li

{"title":"Nitrate Enhanced Sulfamethoxazole Degradation by 222 nm Far-UVC Irradiation: Role of Reactive Nitrogen Species","authors":"Haoxin Li, Ziyi Li, Xi Zhang, Wenjun Sun, Xiuwei Ao, Zifu Li","doi":"10.1021/acs.est.4c07539","DOIUrl":"https://doi.org/10.1021/acs.est.4c07539","url":null,"abstract":"The application of 222 nm far-UVC irradiation for degrading organic micropollutants in water shows promise. Nitrate (NO3–), found in nearly all water bodies, can significantly impact the performance of 222 nm far-UVC-driven systems. This work was the first to investigate the effect of NO3– on sulfamethoxazole (SMX) photodegradation at 222 nm, finding that NO3– significantly enhances SMX degradation in different dissociated forms. Besides the hydroxyl radical (•OH), reactive nitrogen species (RNS) also played important roles in SMX degradation. With increasing NO3– concentration, the RNS contribution to SMX degradation decreased from 25.7 to 8.6% at pH 3 but increased from 1.5 to 24.7% at pH 7, since the deprotonated SMX with electron-rich groups reacted more easily with RNS. The transformation mechanisms of SMX involving isomerization, bond cleavage, hydroxylation, nitrosation, and nitration processes were proposed. 15N isotope labeling experiments showed that the RNS-induced nitrated products even became the major products of SMX in the 222 nm far-UVC/NO3– system at pH 7 and exhibited a higher toxicity than SMX itself. Further research is necessary to avoid or eliminate these toxic byproducts. This study provides valuable insights for guiding the utilization of 222 nm far-UVC for treating antibiotics in NO3–-containing water.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":9.028,"publicationDate":"2024-09-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142246160","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}

引用次数: 0

New Analytical Paradigm to Determine Concentration of Brown Carbon and Its Sample-by-Sample Mass Absorption Efficiency 确定棕碳浓度及其逐样质量吸收效率的新分析范例

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2024-09-19 DOI: 10.1021/acs.est.4c06831

Kezheng Liao, Yuk Ying Cheng, Sui Shing Yea, L.-W. Antony Chen, John H. Seinfeld, Jian Zhen Yu

{"title":"New Analytical Paradigm to Determine Concentration of Brown Carbon and Its Sample-by-Sample Mass Absorption Efficiency","authors":"Kezheng Liao, Yuk Ying Cheng, Sui Shing Yea, L.-W. Antony Chen, John H. Seinfeld, Jian Zhen Yu","doi":"10.1021/acs.est.4c06831","DOIUrl":"https://doi.org/10.1021/acs.est.4c06831","url":null,"abstract":"Brown carbon (BrC) has a substantial direct radiative effect, but current estimates of its impact on radiative balance are highly uncertain due to a lack of measurements of its light-absorbing properties, such as mass absorption efficiency (MAE). Here, we present a new analytical paradigm based on a Bayesian inference (BI) model that takes multiwavelength aethalometer measurements and total carbon data to resolve the concentrations of black carbon and BrC, and MAEs of BrC on a sample-by-sample basis. Hourly MAEs, unattainable in previous studies, can now be calculated, enabling the first-time observation of the darkening-bleaching dynamics of BrC in response to photochemical transformation. We demonstrate the application of this BI model to analyze measurements collected over one year (2021–2022) in Hong Kong. Diel variations in MAE370 nm of BrC reveal a darkening-to-bleaching transition occurring between 8 and 10 O’clock when the solar irradiance ranges from 30 to 400 W m–2. Furthermore, we consistently observe an increase in MAE370 nm of BrC with nitrogen oxide concentrations, suggesting the enhanced formation of nitrogenous organics. This BI model-based data analysis would bring forth a breakthrough in amassing observation data of BrC and its MAEs in diverse ambient environments and with high time resolution.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":9.028,"publicationDate":"2024-09-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142246186","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}

引用次数: 0

Identification of Urban Carbon Emission Peaks through Tree-Ring 14C 通过树环 14C 确定城市碳排放峰值

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2024-09-18 DOI: 10.1021/acs.est.4c06041

Zhenchuan Niu, Weijian Zhou, Yunfei Huang, Sen Wang, Guiqian Zhang, Xue Feng, Xuefeng Lu, Mengni Lyu, Jocelyn C. Turnbull

{"title":"Identification of Urban Carbon Emission Peaks through Tree-Ring 14C","authors":"Zhenchuan Niu, Weijian Zhou, Yunfei Huang, Sen Wang, Guiqian Zhang, Xue Feng, Xuefeng Lu, Mengni Lyu, Jocelyn C. Turnbull","doi":"10.1021/acs.est.4c06041","DOIUrl":"https://doi.org/10.1021/acs.est.4c06041","url":null,"abstract":"Independent identification of carbon emission peaks determined from fuel inventories is a challenging goal. Because of the complete depletion of radiocarbon (14C) in fossil fuel sources, the measurement of atmospheric 14CO2 has proven to offer a means of achieving this goal. Here, we present a study identifying peak carbon emissions from two Chinese cities using urban tree-ring Δ14C time series during 2000–2019. After subtracting background atmospheric Δ14C from urban tree-ring Δ14C to isolate local Δ14C (Δ14Clocal), we find a minimum in 2010 (−51.1 ± 4.5‰) in Beijing and in 2013 in Xi’an (−52.5 ± 0.5‰). These levels correspond to an urban carbon emission peak in 2010 and in 2013 in the two respective cities. The urban carbon emission peaks are further identified by the declines of the mean absolute interannual rate of decrease of tree-ring Δ14C during a period, with the respective values of 3.6 and 6.4 ‰/yr after and before a turning point in Beijing and 3.0 and 6.0 ‰/yr after and before a turning point in Xi’an. This study provides an observation method to identify carbon emission peaks in basin cities.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":9.028,"publicationDate":"2024-09-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142236981","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}

引用次数: 0

Determining Marine Biodegradation Kinetics of Chemicals Discharged from Offshore Oil Platforms─Whole Mixture Testing at High Dilutions Increases Environmental Relevance 确定近海石油平台排放的化学品的海洋生物降解动力学--高稀释度下的全混合物测试提高了环境相关性

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2024-09-18 DOI: 10.1021/acs.est.4c05692

Mette T. Møller, Heidi Birch, Karina K. Sjøholm, Lars M. Skjolding, Hongyu Xie, Stefano Papazian, Philipp Mayer

{"title":"Determining Marine Biodegradation Kinetics of Chemicals Discharged from Offshore Oil Platforms─Whole Mixture Testing at High Dilutions Increases Environmental Relevance","authors":"Mette T. Møller, Heidi Birch, Karina K. Sjøholm, Lars M. Skjolding, Hongyu Xie, Stefano Papazian, Philipp Mayer","doi":"10.1021/acs.est.4c05692","DOIUrl":"https://doi.org/10.1021/acs.est.4c05692","url":null,"abstract":"Offshore oil platforms discharge enormous volumes of produced water that contain mixtures of petrochemicals and production chemicals. It is crucial to avoid the discharge of particularly those chemicals that are persistent in the marine environment. This study aims to (1) develop a biodegradation testing approach for discharged chemicals by native marine microorganism, (2) determine how dilution affects biodegradation, and (3) determine biodegradation kinetics for many discharged chemicals at low and noninhibitory concentrations. Produced water from an offshore oil platform was diluted in the ratio of 1:20, 1:60, and 1:200 in seawater from the same location and incubated for 60 days at 10 °C. Automated solid-phase microextraction GC-MS was used as a sensitive analytical technique, and chemical-specific primary degradation was determined based on peak area ratios between biotic test systems and abiotic controls. Biodegradation was inhibited at lower dilutions, consistent with ecotoxicity tests. Biodegradation kinetics were determined at the highest dilution for 139 chemicals (43 tentatively identified), and 6 chemicals were found persistent (half-life >60 days). Nontargeted analysis by liquid chromatography-high-resolution MS was demonstrated as a proof-of-principle for a comprehensive assessment. Biodegradation testing of chemicals in discharges provides the possibility to assess hundreds of chemicals at once and find the persistent ones.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":9.028,"publicationDate":"2024-09-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142236982","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}

引用次数: 0

Energy Recovery from Hexavalent Chromium Reduction for In Situ Electrocatalytic Hydrogen Peroxide Production 原位电催化过氧化氢生产中六价铬还原的能量回收

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2024-09-18 DOI: 10.1021/acs.est.4c03827

Huaijia Xin, Wei Zhang, Xiaofeng Zhang, Gong Zhang, Qinghua Ji, Huijuan Liu, Jiuhui Qu

{"title":"Energy Recovery from Hexavalent Chromium Reduction for In Situ Electrocatalytic Hydrogen Peroxide Production","authors":"Huaijia Xin, Wei Zhang, Xiaofeng Zhang, Gong Zhang, Qinghua Ji, Huijuan Liu, Jiuhui Qu","doi":"10.1021/acs.est.4c03827","DOIUrl":"https://doi.org/10.1021/acs.est.4c03827","url":null,"abstract":"Recovering chemical energy embedded in pollutants is significant in achieving carbon-neutral industrial wastewater treatment. Considering that industrial wastewater is usually treated in a decentralized manner, in situ utilization of chemical energy to achieve waste-to-treasure should be given priority. Herein, the chemical energy released by the electroreduction of Cr(VI) was used to enhance on-site H2O2 generation in a stacked flow-through electrochemical system. The driving force of water flow efficiently coupled O2 evolution with 2-e O2 reduction to facilitate H2O2 generation by transporting anode-produced O2 to the cathode. Meanwhile, the chemical energy released by Cr(VI) promoted O2 evolution and impeded H2 evolution by regulating the electrode potentials, accounting for the enhanced H2O2 generation. The system could completely reduce 10–100 ppm of Cr(VI), reaching the maximum H2O2 concentration of 2.41 mM. In particular, the H2O2 concentrations in the Cr(VI)-containing electrolyte were 10.6–88.1% higher than those in the Cr(VI) free electrolyte at 1.8–2.5 V. A 24-day continuous experiment demonstrated the high efficiency and stability of the system, achieving a 100% reduction efficiency for 100 ppm of Cr(VI) and producing ∼1.5 mM H2O2 at 1.8 V. This study presents a feasible strategy for Cr(VI) detoxification and synchronous on-site H2O2 generation, providing a new perspective for innovative Cr(VI) wastewater treatment toward resource utilization.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":9.028,"publicationDate":"2024-09-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142236934","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}

引用次数: 0

Diversity and Activity of Soil N2O-Reducing Bacteria Shaped by Urbanization 城市化影响土壤氧化亚氮还原菌的多样性和活性

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2024-09-18 DOI: 10.1021/acs.est.4c01750

Le-Yang Yang, Shun Li, Hua-Yuan Shangguan, Zhi-Hong Qiao, Xin-Rong Huang, Shu-Yi-Dan Zhou, Hu Li, Xiao-Xuan Su, Xin Sun, Yong-Guan Zhu, Xiao-Ru Yang

{"title":"Diversity and Activity of Soil N2O-Reducing Bacteria Shaped by Urbanization","authors":"Le-Yang Yang, Shun Li, Hua-Yuan Shangguan, Zhi-Hong Qiao, Xin-Rong Huang, Shu-Yi-Dan Zhou, Hu Li, Xiao-Xuan Su, Xin Sun, Yong-Guan Zhu, Xiao-Ru Yang","doi":"10.1021/acs.est.4c01750","DOIUrl":"https://doi.org/10.1021/acs.est.4c01750","url":null,"abstract":"Nitrous oxide (N2O) is a potent greenhouse gas with various production pathways. N2O reductase (N2OR) is the primary N2O sink, but the distribution of its gene clades, typically nosZI and atypically nosZII, along urbanization gradients remains poorly understood. Here we sampled soils from forests, parks, and farmland across eight provinces in eastern China, using high-throughput sequencing to distinguish between two N2O-reducing bacteria clades. A deterministic process mainly determined assemblies of the nosZI communities. Homogeneous selection drove nosZI deterministic processes, and both homogeneous and heterogeneous selection influenced nosZII. This suggests nosZII is more sensitive to environmental changes than nosZI, with significant changes in community structure over time or space. Ecosystems with stronger anthropogenic disturbance, such as urban areas, provide diverse ecological niches for N2O-reducing bacteria (especially nosZII) to adapt to environmental fluctuations. Structural equation modeling (SEM) and correlation analyses revealed that pH significantly influences the community composition of both N2O-reducing bacteria clades. This study underscores urbanization’s impact on N2O-reducing bacteria in urban soils, highlighting the importance of nosZII and survival strategies. It offers novel insights into the role of atypical denitrifiers among N2O-reducing bacteria, underscoring their potential ecological importance in mitigating N2O emissions from urban soils.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":9.028,"publicationDate":"2024-09-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142236931","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}

引用次数: 0

Multimedia and Full-Life-Cycle Monitoring Discloses the Dynamic Accumulation Rules of PFAS and Underestimated Foliar Uptake in Wheat near a Fluorochemical Industrial Park 多媒体和全生命周期监测揭示了氟化工工业园区附近小麦中 PFAS 的动态累积规律和被低估的叶面吸收量

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2024-09-18 DOI: 10.1021/acs.est.4c03525

Xin Chen, Dashan Xu, Yuehan Xiao, Mingjiang Zuo, Jian Zhou, Xiao Sun, Guoqiang Shan, Lingyan Zhu

{"title":"Multimedia and Full-Life-Cycle Monitoring Discloses the Dynamic Accumulation Rules of PFAS and Underestimated Foliar Uptake in Wheat near a Fluorochemical Industrial Park","authors":"Xin Chen, Dashan Xu, Yuehan Xiao, Mingjiang Zuo, Jian Zhou, Xiao Sun, Guoqiang Shan, Lingyan Zhu","doi":"10.1021/acs.est.4c03525","DOIUrl":"https://doi.org/10.1021/acs.est.4c03525","url":null,"abstract":"The escalating concern of perfluoroalkyl and polyfluoroalkyl substances (PFAS), particularly at contaminated sites, has prompted extensive investigations. In this study, samples of multimedia including air, rhizosphere soil, and tissues of wheat at various growing stages were collected near a mega fluorochemical industrial park in China. Perfluorooctanoic acid (PFOA) was predominant in both air and soil with a strong correlation, highlighting air deposition as an important source in the terrestrial system. PFAS concentrations in wheat decreased in the stem and ear but increased in the leaves as wheat matured. Specifically, perfluorobutanoic acid (PFBA) dominated in the aboveground tissues in the full-life-cycle, except that PFOA surpassed and became predominant in leaves during the filling and maturing stages, hinting at an airborne source. For all PFAS, both bioaccumulation factors and translocation factors (TFs) were inversely correlated with the carbon chain length during the full-life-cycle. The obtained TF values were considerably higher than those obtained from ambient sites reported previously, further suggesting an unneglectable foliar uptake from air, which was estimated to be 25% for PFOA. Moreover, spray irrigation remarkably enhanced the absorption of PFAS in wheat via foliar uptake relative to flood irrigation. The estimated daily intake of PFBA via wheat consumption and air inhalation was 0.50 μg/kg/day for local residents, at least one magnitude higher than the corresponding threshold, suggesting an alarmingly high exposure risk.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":9.028,"publicationDate":"2024-09-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142236933","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}

引用次数: 0

Inhibiting the Formation of Toxic HCN Induced by C3H6 Coexistence and Enhancing C3H6 Resistance of Cu-Zeolite in the NH3–SCR Reaction 在 NH3-SCR 反应中抑制 C3H6 共存诱发的有毒 HCN 生成并增强铜沸石的抗 C3H6 能力

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2024-09-18 DOI: 10.1021/acs.est.4c05571

Yu Sun, Tongliang Zhang, Wenqing Ding, Jingjing Liu, Diru Liu, Jinpeng Du, Zhi Liu, Xiaoyan Shi, Yunbo Yu, Peirong Chen, Yan Zhang, Wenpo Shan, Yulong Shan, Hong He

{"title":"Inhibiting the Formation of Toxic HCN Induced by C3H6 Coexistence and Enhancing C3H6 Resistance of Cu-Zeolite in the NH3–SCR Reaction","authors":"Yu Sun, Tongliang Zhang, Wenqing Ding, Jingjing Liu, Diru Liu, Jinpeng Du, Zhi Liu, Xiaoyan Shi, Yunbo Yu, Peirong Chen, Yan Zhang, Wenpo Shan, Yulong Shan, Hong He","doi":"10.1021/acs.est.4c05571","DOIUrl":"https://doi.org/10.1021/acs.est.4c05571","url":null,"abstract":"The presence of light hydrocarbons (HCs) in diesel exhaust, specifically C3H6, significantly affects the performance of the state-of-the-art Cu-SSZ-13 zeolite NH3–SCR catalysts. It also leads to the formation of highly toxic HCN, posing risks to the environment and human health. In this work, the highly toxic HCN formation is inhibited, and the C3H6 resistance of Cu-SSZ-13 is improved by secondary metal modification via doping with rare earth/transition metal elements. Upon introduction of C3H6, the activity of Cu-SSZ-13 significantly decreases at medium-high temperatures. This is primarily due to the competitive reaction between C3H6 and NH3, which compete for the NH3 reductant required in the NH3–SCR reaction, resulting in the production of HCN. The unfavorable effect is alleviated on the modified catalysts due to their enhanced oxidation capabilities toward C3H6 and the HCHO intermediate, facilitating the complete oxidation of C3H6 to COx. This inhibits the undesirable partial oxidation reaction between C3H6 and NH3, thereby improving the activity of Cu-SSZ-13 at medium to high temperatures and significantly reducing the formation of highly toxic HCN.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":9.028,"publicationDate":"2024-09-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142236940","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}

引用次数: 0

Carbonyl Compounds Regulate Atmospheric Oxidation Capacity and Particulate Sulfur Chemistry in the Coastal Atmosphere 羰基化合物调节沿海大气的氧化能力和颗粒硫化学性质

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2024-09-18 DOI: 10.1021/acs.est.4c03947

Min Zhao, Hengqing Shen, Ji Zhang, Yuhong Liu, Yue Sun, Xinfeng Wang, Can Dong, Yujiao Zhu, Hongyong Li, Ye Shan, Jiangshan Mu, Xuelian Zhong, Jinghao Tang, Mingzhi Guo, Wenxing Wang, Likun Xue

{"title":"Carbonyl Compounds Regulate Atmospheric Oxidation Capacity and Particulate Sulfur Chemistry in the Coastal Atmosphere","authors":"Min Zhao, Hengqing Shen, Ji Zhang, Yuhong Liu, Yue Sun, Xinfeng Wang, Can Dong, Yujiao Zhu, Hongyong Li, Ye Shan, Jiangshan Mu, Xuelian Zhong, Jinghao Tang, Mingzhi Guo, Wenxing Wang, Likun Xue","doi":"10.1021/acs.est.4c03947","DOIUrl":"https://doi.org/10.1021/acs.est.4c03947","url":null,"abstract":"Carbonyl compounds play a crucial role in the formation of ozone (O3) and secondary aerosols, with recent studies particularly highlighting formaldehyde (HCHO) as a significant contributor to the missing particulate sulfur. However, evaluations based on field observations are limited, especially in clean marine environments. Utilizing observation data from a coastal mountain site in May 2021 in Qingdao, northern China, we reveal the important regulating effect of carbonyls in atmospheric oxidation capacity and particulate sulfur chemistry using detailed chemical box models. Photolysis of gaseous carbonyls accounted for >90% and >60% of the primary sources of HO2 and RO2, respectively, contributing 38% of net O3 production. Notably, HCHO alone constituted 80% of the primary HO2 and 15% of net O3 production. Using a multiphase model with updated HCHO-related chemistry, we determine that HCHO chemistry can account for up to 30% of total particulate sulfur (the sum of hydroxymethanesulfonate and sulfate) and address more than one-third of the simulated sulfate gap. The emission-based multiphase model indicates that the HCHO-related pathway remains significant and can account for 20% of the particulate sulfur under clean marine conditions. These findings underscore the importance of carbonyls, particularly HCHO, in regulating the atmospheric oxidation capacity and particulate sulfur chemistry in the marine atmosphere, urging further laboratory studies on chemical kinetics and field measurements of particle-phase carbonyls.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":9.028,"publicationDate":"2024-09-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142236936","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}

引用次数: 0

Photoinduced Evolutions of Permafrost-Derived Carbon in Subarctic Thermokarst Pond Surface Waters 亚北极恒温池塘地表水中永久冻土衍生碳的光诱导演变

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2024-09-18 DOI: 10.1021/acs.est.4c05320

Tao Wang, Carmen Kalalian, Xinke Wang, Dandan Li, Sébastien Perrier, Jianmin Chen, Florent Domine, Liwu Zhang, Christian George

{"title":"Photoinduced Evolutions of Permafrost-Derived Carbon in Subarctic Thermokarst Pond Surface Waters","authors":"Tao Wang, Carmen Kalalian, Xinke Wang, Dandan Li, Sébastien Perrier, Jianmin Chen, Florent Domine, Liwu Zhang, Christian George","doi":"10.1021/acs.est.4c05320","DOIUrl":"https://doi.org/10.1021/acs.est.4c05320","url":null,"abstract":"In subarctic regions, rising temperature and permafrost thaw lead to the formation of thermokarst ponds, where organics from eroding permafrost accumulate. Despite its environmental significance, limited knowledge exists regarding the photosensitivity of permafrost-derived carbon in these ponds. In this study, laboratory experiments were conducted to explore the photochemical transformations of organic matter in surface water samples from thermokarst ponds from different environments in northern Quebec, Canada. One pond near Kuujjuarapik is characterized by the presence of a collapsing palsa and is therefore organically rich, while the other pond near Umiujaq is adjacent to a collapsing lithalsa and thus contains fewer organic matters. Photobleaching occurred in the Umiujaq sample upon irradiation, whereas the Kuujjuarapik sample exhibited an increase in light absorbance at wavelength related to aromatic functionalities, indicating different photochemical aging processes. Ultrahigh-resolution mass spectrometry analysis reveals that the Kuujjuarapik sample preferentially photoproduced highly unsaturated CHO compounds with great aromaticity, while the irradiated Umiujaq sample produced a higher proportion of CHON aromatics with reduced nitrogen functionalities. Overall, this study illustrates that the photochemical reactivity of thermokarst pond water varies with the source of organic matter. The observed differences in reactivity contribute to an improved understanding of the photochemical emission of volatile organic compounds discovered earlier. Further insights into the photoinduced evolutions in thermokarst ponds may require the classification of permafrost-derived carbon therein.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":9.028,"publicationDate":"2024-09-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142236938","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}

引用次数: 0

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