IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2024-09-27 DOI: 10.1021/acs.est.4c04392

Qian Xiao, Zhe Yang, Wanbin Li, Bo Wei, Hao Guo, Shuili Yu, Qimao Gan, Wenyu Liu, Chuyang Y. Tang

{"title":"Iron Nanoparticles-Confined Graphene Oxide Membranes Coupled with Sulfite-Based Advanced Reduction Processes for Highly Efficient and Stable Removal of Bromate","authors":"Qian Xiao, Zhe Yang, Wanbin Li, Bo Wei, Hao Guo, Shuili Yu, Qimao Gan, Wenyu Liu, Chuyang Y. Tang","doi":"10.1021/acs.est.4c04392","DOIUrl":"https://doi.org/10.1021/acs.est.4c04392","url":null,"abstract":"Advanced reduction processes (ARPs) are promising for pollutant removal in drinking water treatment. In this study, we demonstrated highly efficient reduction of bromate, a harmful disinfection byproduct, by coupling ARPs with an iron nanoparticles-intercalated graphene oxide (GO@FeNPs) catalytic membrane. In the presence of 1.0 mM sulfite (S(IV)), the GO@FeNPs membrane/S(IV) system achieved nearly complete removal of 80 μg/L bromate in 3 min. The first-order reaction rate constant for bromate removal in this system was 420 ± 42 min–1, up to 5 orders of magnitude faster than previously reported ARPs. The GO@FeNPs catalytic membrane may offer potential advantages of nanoconfinement and facilitated electron shuttling in addition to the high surface area of the fine FeNPs, leading to the remarkable ARP performance. The GO@FeNPs membrane showed excellent stability, maintaining >97.0% bromate removal over 20 cycles of repeated runs. The membrane can also be applied for fast catalytic reduction of other oxyanions, showing >98.0% removal of nitrate and chlorate. This work may present a viable option for utilizing high-performance reductive catalytic membranes for water decontamination.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":9.028,"publicationDate":"2024-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142325694","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

Proton vs Electron: The Dual Role of Redox-Inactive Metal Ions in Permanganate Oxidation Kinetics 质子与电子：氧化还原不活跃的金属离子在高锰酸盐氧化动力学中的双重作用

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2024-09-27 DOI: 10.1021/acs.est.4c06557

Mengfan Luo, Heng Zhang, Jianhua Guo, Jia Zhao, Can Feng, Jialong Yin, Chang Xu, Ye Du, Yang Liu, Chuan-Shu He, Bo Lai

{"title":"Proton vs Electron: The Dual Role of Redox-Inactive Metal Ions in Permanganate Oxidation Kinetics","authors":"Mengfan Luo, Heng Zhang, Jianhua Guo, Jia Zhao, Can Feng, Jialong Yin, Chang Xu, Ye Du, Yang Liu, Chuan-Shu He, Bo Lai","doi":"10.1021/acs.est.4c06557","DOIUrl":"https://doi.org/10.1021/acs.est.4c06557","url":null,"abstract":"Redox-inactive metal-ion-driven modulation of the oxidation behavior of high-valent metal–oxo complex has garnered significant interest in biological and chemical synthesis; however, their role in permanganate (Mn(VII)) oxidation for the removal of organic pollutants has been largely neglected. Here, we uncover the impact of six metal ions (i.e., Ca2+, Mg2+, Ni2+, Zn2+, Al3+, and Sc3+) presenting in water environments on Mn(VII) activity. These ions uniformly boost the electron and oxygen transfer capabilities of Mn(VII) while impeding proton transfer, as evidenced by electrochemical tests, thioanisole probe analysis, and the kinetic isotope effect. The observed effects are intricately linked to the Lewis acidity of the metal ions. Further mechanistic insights reveal that Mn(VII) can interact with metal ions without direct reduction. Such interactions modify the electronic configuration of Mn(VII) and create an acidic microenvironment, thus increasing its electrophilicity and the energy barrier for the abstraction of proton from organic substrates. More importantly, the efficacy of Mn(VII) in removing phenolic pollutants is regulated by these ions through changing the driving force for proton and electron transfer, i.e., facilitated at pH > 4.5 and inhibited at lower pH. The contribution of active Mn intermediates is also discussed to reveal the oxidative mechanism of the metal ion/Mn(VII) system. These findings not only facilitate the rational design of Mn(VII) oxidation conditions in the presence of metal ions for water decontamination but also offer an alternative paradigm for enhancing electrophilic oxidation.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":9.028,"publicationDate":"2024-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142325696","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

Resolving Atmospheric Oxygenated Organic Molecules in Urban Beijing Using Online Ultrahigh-Resolution Chemical Ionization Mass Spectrometry 利用在线超高分辨率化学电离质谱法解析北京城区大气中的含氧有机分子

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2024-09-27 DOI: 10.1021/acs.est.4c04214

Yi Yuan, Xin Chen, Runlong Cai, Xiaoxiao Li, Yuyang Li, Rujing Yin, Dandan Li, Chao Yan, Yongchun Liu, Kebin He, Markku Kulmala, Jingkun Jiang

{"title":"Resolving Atmospheric Oxygenated Organic Molecules in Urban Beijing Using Online Ultrahigh-Resolution Chemical Ionization Mass Spectrometry","authors":"Yi Yuan, Xin Chen, Runlong Cai, Xiaoxiao Li, Yuyang Li, Rujing Yin, Dandan Li, Chao Yan, Yongchun Liu, Kebin He, Markku Kulmala, Jingkun Jiang","doi":"10.1021/acs.est.4c04214","DOIUrl":"https://doi.org/10.1021/acs.est.4c04214","url":null,"abstract":"Gaseous oxygenated organic molecules (OOMs) are crucial precursors of atmospheric organic aerosols. OOMs in urban atmospheres have complex compositions, posing challenges to understanding their formation, evolution, and influences. In this study, we identify 2403 atmospheric gaseous OOMs in urban Beijing using online nitrate-based chemical ionization Orbitrap mass spectrometry based on one-year atmospheric measurements. We find that OOMs in urban atmospheres can be identified with higher accuracy and wider coverage, compared to previously used online mass spectrometry. With optimized OOM resolving capabilities, previous knowledge of OOMs in urban atmospheres can be expanded. First, clear homologous and oxygen-addition characteristics of the OOMs are revealed. Second, OOMs with lower concentrations or higher masses are identified and characterized with high confidence, e.g., OOMs with masses above 350 Da. In particular, dimers of OOMs (e.g., C20H32O8–15N2), crucial species for organic nucleation, are identified. During four seasons, nitrogen-containing OOMs dominate the total concentration of OOMs, and OOMs are mainly from aromatic and aliphatic oxidation. Additionally, radicals with similar composition as OOMs, intermediates for OOM formation, are identified with clear diurnal variation, e.g., CnH2n–5O6 radicals (n = 8–10) and CmH2m–4NO9 radicals (m = 9–10), peak during the daytime and nighttime, respectively, previously having scarce measurement evidence in urban atmospheres.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":9.028,"publicationDate":"2024-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142325693","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

Diverse Effects of SO2-Induced Pt–O–SO3 on the Catalytic Oxidation of C3H6 and C3H8 二氧化硫诱导的 Pt-O-SO3 对 C3H6 和 C3H8 催化氧化的不同影响

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2024-09-26 DOI: 10.1021/acs.est.4c04946

Baojian Zhang, Yuan Yang, Juan Zheng, Dijierui Zhang, Wei Chen, Weidong Yuan, Xiaoping Chen, Rui Liu, Bosheng Chen, Liangwei Li, Limin Shi, Jinlong Wang, Zhu Luo, Yanbing Guo

{"title":"Diverse Effects of SO2-Induced Pt–O–SO3 on the Catalytic Oxidation of C3H6 and C3H8","authors":"Baojian Zhang, Yuan Yang, Juan Zheng, Dijierui Zhang, Wei Chen, Weidong Yuan, Xiaoping Chen, Rui Liu, Bosheng Chen, Liangwei Li, Limin Shi, Jinlong Wang, Zhu Luo, Yanbing Guo","doi":"10.1021/acs.est.4c04946","DOIUrl":"https://doi.org/10.1021/acs.est.4c04946","url":null,"abstract":"The effects of sulfur dioxide (SO2) in the catalytic purification of short-chain hydrocarbons are still controversial, and the exact role of SO2 on adsorption and reaction pathways during the catalytic oxidation of different volatile organic compounds (VOCs) remains unclear. Herein, a three-dimensional ordered macroporous Ce0.8Zr0.2O2 supported Pt nanoparticle monolithic catalyst (Pt/OM CZO) was synthesized to investigate these effects. Our findings uncover the diverse effects of SO2: Upon SO2 treatment, the coupling between the S 3p and Pt 5d orbitals promotes the Pt–O–SO3 structure in situ formed on the catalyst surface. The propene (C3H6) molecule readily binds with the oxygen atom in Pt–O–SO3, resulting in the accumulation of acetone and carbon deposition, thereby hindering C3H6 oxidation. Conversely, a cleaved oxygen atom within the Pt–O–SO3 structure enhances propane (C3H8) adsorption and activates the C–H bond, facilitating C3H8 oxidation. These insights are pivotal for advancing the frontier of sulfur-tolerant catalysts, addressing both economic and environmental challenges.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":9.028,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142321631","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

Natural Organic Matter Enhances Natural Transformation of Extracellular Antibiotic Resistance Genes in Sunlit Water 天然有机物增强了阳光照射下水体外抗生素耐药性基因的自然转化

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2024-09-26 DOI: 10.1021/acs.est.4c08211

Qian-He Liu, Li Yuan, Zheng-Hao Li, Kenneth Mei Yee Leung, Guo-Ping Sheng

{"title":"Natural Organic Matter Enhances Natural Transformation of Extracellular Antibiotic Resistance Genes in Sunlit Water","authors":"Qian-He Liu, Li Yuan, Zheng-Hao Li, Kenneth Mei Yee Leung, Guo-Ping Sheng","doi":"10.1021/acs.est.4c08211","DOIUrl":"https://doi.org/10.1021/acs.est.4c08211","url":null,"abstract":"Antibiotic resistance genes (ARGs) as emerging environmental contaminants exacerbate the risk of spreading antibiotic resistance. Natural organic matter (NOM) is ubiquitous in aquatic environments and plays a crucial role in biogeochemical cycles. However, its impact on the dissemination of extracellular antibiotic resistance genes (eARGs) under sunlight exposure remains elusive. This study reveals that environmentally relevant levels of NOM (0.1–20 mg/L) can significantly enhance the natural transformation frequency of the model bacterium Acinetobacter baylyi ADP1 by up to 7.6-fold under simulated sunlight. Similarly, this enhancement was consistently observed in natural water and wastewater systems. Further mechanism analysis revealed that reactive oxygen species (ROS) generated by NOM under sunlight irradiation, primarily singlet oxygen and hydroxyl radicals, play a crucial role in this process. These ROS induce intracellular oxidative stress and elevated cellular membrane permeability, thereby indirectly boosting ATP production and enhancing cell competence of extracellular DNA uptake and integration. Our findings highlight a previously underestimated role of natural factors in the dissemination of eARGs within aquatic ecosystems and deepen our understanding of the complex interplay between NOM, sunlight, and microbes in environmental water bodies. This underscores the importance of developing comprehensive strategies to mitigate the spread of antibiotic resistance in aquatic environments.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":9.028,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142321633","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

VUV Activated Fe(VI) by Promoting the Generation of Intermediate Valent Iron and Hydroxyl Radicals 紫外线通过促进生成中间价铁和羟基自由基活化铁(VI)

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2024-09-26 DOI: 10.1021/acs.est.4c05343

Lian Wu, Lu Wang, Yu-Lei Liu, Xiao-Na Zhao, Jun Ma

{"title":"VUV Activated Fe(VI) by Promoting the Generation of Intermediate Valent Iron and Hydroxyl Radicals","authors":"Lian Wu, Lu Wang, Yu-Lei Liu, Xiao-Na Zhao, Jun Ma","doi":"10.1021/acs.est.4c05343","DOIUrl":"https://doi.org/10.1021/acs.est.4c05343","url":null,"abstract":"In this study, vacuum ultraviolet (VUV) was first proposed to activate ferrate (Fe(VI)) for degrading micropollutants (e.g., carbamazepine (CBZ)). Results indicated that VUV/Fe(VI) could significantly facilitate the CBZ degradation, and the removal efficiencies of VUV/Fe(VI) were 30.9–83.4% higher than those of Fe(VI) at pH = 7.0–9.0. Correspondingly, the degradation rate constants of VUV/Fe(VI) were 2.3–36.0-fold faster than those of Fe(VI). Free radical quenching and probe experiments revealed that the dominant active species of VUV/Fe(VI) were •OH and Fe(V)/Fe(IV), whose contribution ratios were 43.3 to 48.6% and 48.2 to 46.6%, respectively, at pH = 7.0–9.0. VUV combined with Fe(VI) not only effectively mitigated the weak oxidizing ability of Fe(VI) under alkaline conditions (especially pH = 9.0) but also attenuated the deteriorating effect of background constituents on Fe(VI). In different real waters (tap water, river water, WWTPs effluent), VUV/Fe(VI) retained a remarkably enhanced effect on CBZ degradation compared to Fe(VI). Moreover, VUV/Fe(VI) exhibited outstanding performance in the debasement of CBZ and sulfamethoxazole (SMX), as well as six other micropollutants, displaying broad-spectrum capability in degrading micropollutants. Overall, this study developed a novel oxidation process that was efficient and energy-saving for the rapid removal of micropollutants.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":9.028,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142321573","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

Reduced CO2 Release from Arctic Soils Due to CO2 Binding to Calcium Forming Aragonite 由于二氧化碳与钙形成的文石结合，北极土壤中的二氧化碳释放量减少

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2024-09-26 DOI: 10.1021/acs.est.4c07496

Peter Stimmler, Martin Obst, Johannes Lehmann, Mathias Stein, Kerstin Hockmann, Mathias Goeckede, Joerg Schaller

{"title":"Reduced CO2 Release from Arctic Soils Due to CO2 Binding to Calcium Forming Aragonite","authors":"Peter Stimmler, Martin Obst, Johannes Lehmann, Mathias Stein, Kerstin Hockmann, Mathias Goeckede, Joerg Schaller","doi":"10.1021/acs.est.4c07496","DOIUrl":"https://doi.org/10.1021/acs.est.4c07496","url":null,"abstract":"Arctic soils are the largest pool of organic carbon compared with other soils globally and serve as a main source for greenhouse gases, especially in the course of the predicted future temperature increase. With increasing temperatures, substantial thawing of the permafrost layer of soils is expected, altering the availability of calcium in those soils, with an increase by ∼5 mg Ca g–1 DW predicted for Alaska. Here we show for two representative soils in Alaska (initially Ca-poor or Ca-rich) that this increase in Ca availability will lead to decreases in CO2 release by 50% and 57%. It is already well-known that the cation bridging of Ca ions to organic carbon renders this carbon unavailable for microbial respiration and that Ca is altering the transformation of Corg by microbes. Here we show that the decrease of the soil CO2 release may be also due to enhanced aragonite formation (by 300% for Ca-poor and 90–200% for Ca-rich soils), as revealed by synchrotron-based scanning transmission X-ray microscopy. We therefore call upon field experiments for validation of this process and inclusion of this process in global and local carbon budget models.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":9.028,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142321575","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

Development and Evaluation of Aquatic and Terrestrial Food Web Bioaccumulation Models for Per- and Polyfluoroalkyl Substances 全氟和多氟烷基物质水生和陆生食物网生物累积模型的开发与评估

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2024-09-26 DOI: 10.1021/acs.est.4c02134

Barry C. Kelly, Jennifer M. Sun, Mandy R. R. McDougall, Elsie M. Sunderland, Frank A. P. C. Gobas

{"title":"Development and Evaluation of Aquatic and Terrestrial Food Web Bioaccumulation Models for Per- and Polyfluoroalkyl Substances","authors":"Barry C. Kelly, Jennifer M. Sun, Mandy R. R. McDougall, Elsie M. Sunderland, Frank A. P. C. Gobas","doi":"10.1021/acs.est.4c02134","DOIUrl":"https://doi.org/10.1021/acs.est.4c02134","url":null,"abstract":"There is a need for reliable models to predict the food web bioaccumulation and assess ecological and human health risks of per- and polyfluoroalkyl substances (PFAS). This present study presents (i) the development of novel mechanistic aquatic and terrestrial food web bioaccumulation models for PFAS and (ii) an evaluation of model performance using available laboratory and field data. Model predictions of laboratory-measured bioconcentration factors and field-based bioaccumulation factors of PFAS in fish were in good agreement with observed data as measured by the mean model bias (MB), representing systematic over- or under-estimation and the standard deviation of the MB, representing general uncertainty. The models provide a mechanistic framework for evaluating the combined effect of simultaneously occurring uptake and elimination processes and indicate food web-specific magnification of PFAS, with the highest degree of biomagnification occurring in food webs composed of air-breathing wildlife. Albumin-water, structural protein–water, membrane-water distribution coefficients, and renal clearance rate are among the most important model parameters. With further development and testing, these models may be useful for future PFAS screening and risk assessment initiatives and advance bioaccumulation studies of PFAS by providing a mechanistic framework for PFAS bioaccumulation.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":9.028,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142325925","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

The Overlooked Role of Humin in Dark Hydroxyl Radical Production during Oxygenation 被忽视的 Humin 在氧合过程中产生暗羟基自由基方面的作用

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2024-09-26 DOI: 10.1021/acs.est.4c06101

Handan Zhang, Liping Li, Xinhui Liu, Linshuai Duan, Xin Zhang, Lu Dong, Xiqin Liu, Pengcheng Li, Bohan Li, Mengzhu Xue, Guohui Xia

{"title":"The Overlooked Role of Humin in Dark Hydroxyl Radical Production during Oxygenation","authors":"Handan Zhang, Liping Li, Xinhui Liu, Linshuai Duan, Xin Zhang, Lu Dong, Xiqin Liu, Pengcheng Li, Bohan Li, Mengzhu Xue, Guohui Xia","doi":"10.1021/acs.est.4c06101","DOIUrl":"https://doi.org/10.1021/acs.est.4c06101","url":null,"abstract":"Humin, endowed with abundant redox functional groups, can be reduced anaerobically under dark. When reduced humin encounters O2, the possibility of ·OH formation arises. However, the exploration of ·OH generation mediated by humin has not been comprehensively conducted. The study found that O2 oxidized the reduced humin, generating 8.61 μmol/g of ·OH. After isolating humin using the methyl isobutyl ketone (MIBK) method, the lipid component was identified as the primary contributor to ·OH generation. Subsequent polar separation revealed that the lipid fraction extracted from the ethanol–water mixture with a volume ratio of 7:3 (LFEW7:3) played the most significant role in ·OH production. Further characterization confirmed that the simultaneous presence of aromatic C═C and C═O were the predominant features contributing to the ·OH generation. The ·OH generation experiments with humin-pyridine analogue compound demonstrated that polycyclic pyridine N (≥3 rings) played a significant role in promoting the ·OH generation. Most importantly, the study compared the ·OH production by humin and homologous humic acid, indicating that ·OH generated by humin was higher than that of humic acid. Overall, these affirmative findings manifested the overlooked role of humin in ·OH production and offered valuable insights into the mechanism of ·OH generation by humin in the dark.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":9.028,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142321572","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

Comparative Evaluation of Mediated Electrochemical Reduction and Chemical Redox Titration for Quantifying the Electron Accepting Capacities of Soils and Redox-Active Soil Constituents 比较评估介导电化学还原法和化学氧化还原滴定法量化土壤和具有氧化还原作用的土壤成分的电子接受能力

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2024-09-26 DOI: 10.1021/acs.est.4c06514

Juan C. Rincón-Rodríguez, Paula A. Cárdenas-Hernández, Jimmy Murillo-Gelvez, Dominic M. Di Toro, Herbert E. Allen, Richard F. Carbonaro, Pei C. Chiu

{"title":"Comparative Evaluation of Mediated Electrochemical Reduction and Chemical Redox Titration for Quantifying the Electron Accepting Capacities of Soils and Redox-Active Soil Constituents","authors":"Juan C. Rincón-Rodríguez, Paula A. Cárdenas-Hernández, Jimmy Murillo-Gelvez, Dominic M. Di Toro, Herbert E. Allen, Richard F. Carbonaro, Pei C. Chiu","doi":"10.1021/acs.est.4c06514","DOIUrl":"https://doi.org/10.1021/acs.est.4c06514","url":null,"abstract":"The electron accepting capacity (EAC) of soil plays a pivotal role in the biogeochemical cycling of nutrients and transformation of redox-labile contaminants. Prior EAC studies of soils and soil constituents utilized different methods, reductants, and mediators, making cross-study comparison difficult. This study was conducted to quantify and compare the EACs of two soil constituents (hematite and Leonardite humic acid) and 12 soils of diverse composition, using chemical redox titration (CRT) with dithionite as the reductant and mediated electrochemical reduction (MER) with diquat as the mediator. The EACs of hematite and humic acid measured by CRT (EACCRT) and MER (EACMER) are similar and close to the theoretical/reported values. For soils, EACCRT and EACMER increased with iron and organic carbon (TOC) contents, suggesting iron and carbon were the main contributors to soil EAC. EACCRT > EACMER for all soils, and their difference (ΔEAC = EACCRT – EACMER) increased with TOC, presumably due to the longer contact time in CRT and thus more complete reduction of carbonaceous redox moieties. We propose an equation that relates EACCRT to EACMER (ΔEAC = 1796fTOC + 32) and another that predicts EACCRT from dithionite-reducible Fe and TOC (EACCRT = 2705 μmol e–/g C × fTOC + 17907 μmol e–/g Fe × fFedithionite-reducible). Our results suggest that at least 10−15% of soil organic carbon contributed to EACCRT.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":9.028,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142321632","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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