环境科学与技术Pub Date : 2024-12-17DOI: 10.1021/acs.est.4c07838
Jiadong Peng, Senhao Lu, Chii Shang, Ran Yin
{"title":"Modeling ClO2–NOM Reactions for Predicting Byproduct Formation and Micropollutant Degradation in Surface Water","authors":"Jiadong Peng, Senhao Lu, Chii Shang, Ran Yin","doi":"10.1021/acs.est.4c07838","DOIUrl":"https://doi.org/10.1021/acs.est.4c07838","url":null,"abstract":"Chlorine dioxide (ClO<sub>2</sub>) is a promising alternative disinfectant/oxidant to free chlorine in drinking water treatment, while it reacts with natural organic matter (NOM) to form free chlorine, chlorite ions (ClO<sub>2</sub><sup>–</sup>), and chlorate ions (ClO<sub>3</sub><sup>–</sup>) as byproducts. Predicting the ClO<sub>2</sub> consumption and the formation of these byproducts using a kinetic model helps to balance the trade-off between disinfection/oxidation efficiency and byproduct formation. This study establishes a summative equation to describe the reaction between ClO<sub>2</sub> and ClO<sub>2</sub>-reactive moieties in the NOM (CRNOM). The average molar yields of ClO<sub>2</sub><sup>–</sup>, free chlorine, Cl<sup>–</sup>, and ClO<sub>3</sub><sup>–</sup> from the reactions between ClO<sub>2</sub> and nine NOM isolates are determined to be 0.576 ± 0.017, 0.258 ± 0.022, 0.141 ± 0.010, and 0.039 ± 0.002 per consumed ClO<sub>2</sub>, respectively. The bimolecular rate constants of CRNOM toward ClO<sub>2</sub> (<i>k</i><sub>CRNOM-ClO<sub>2</sub></sub>) are comparable among nine NOM isolates (683 ± 57 M<sup>–1</sup>·s<sup>–1</sup> at pH 7.0). The CRNOM concentrations and <i>k</i><sub>CRNOM-ClO<sub>2</sub></sub> increase by 2-fold and 1.3-fold, respectively, as pH increases from 6.0 to 9.0, while pH barely affects the molar yields of inorganic products. A kinetic model is established and enables the accurate prediction of ClO<sub>2</sub><sup>–</sup> and ClO<sub>3</sub><sup>–</sup> formation and ofloxacin degradation during ClO<sub>2</sub> oxidation in surface water.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"41 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2024-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142841404","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}
{"title":"Cross-Generational Exposure to Low-Density Polyethylene Microplastics Induced Hyperactive Responses in <i>Eisenia fetida</i> Offsprings.","authors":"Yuanyuan Zhao, Huiting Jia, Hui Deng, Chengjun Ge, Haibin Luo, Ying Zhang","doi":"10.1021/acs.est.4c05208","DOIUrl":"10.1021/acs.est.4c05208","url":null,"abstract":"<p><p>The extensive application of plastic products in daily human life has led to the accumulation of microplastics (MPs) in agricultural soil. However, little is known about the cross-generational toxicity of MPs on terrestrial invertebrates. In this study, two-generational <i>Eisenia fetida</i> was exposed to low-density polyethylene (LDPE, 0-5%, w/w) for 98 days to reveal the cross-generational toxicity and the underlying mechanisms. Results showed that LDPE-MPs not only perpetrated deleterious effects on the development, hatchability, and fecundity of the F0 generation but also stimulated the antioxidant defense activity, inhibited lipid peroxidation, and disordered neurotransmission in F1 generation individuals. The susceptibility of the epidermal-intestinal barrier to LDPE-MPs was dose-dependent. According to the transcriptomic analysis, the cross-generational earthworms confirmed significant perturbances in the cell cycle, neural activity-related pathways, and amino acid metabolism pathways (<i>p</i> < 0.05). Nevertheless, the metabolomic profile of F1 generation individuals exhibited significant hyperactive responses in glutathione metabolism and alanine, aspartate, and glutamate metabolism (<i>p</i> < 0.05). This study provides a comprehensive knowledge of LDPE-MPs toxicity on cross-generational earthworms and highlights the hyperactive responses in the antioxidant defense performance of the offsprings. Our findings also underscore the necessity for long-term investigations in assessing the adverse impacts of emerging pollutants.</p>","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":" ","pages":"21918-21929"},"PeriodicalIF":10.8,"publicationDate":"2024-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142646263","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}
环境科学与技术Pub Date : 2024-12-17DOI: 10.1021/acs.est.4c07276
Feng-He Li, Zi-Han Liang, Hong Sun, Qiang Tang, Han-Qing Yu
{"title":"Engineering Programmable Electroactive Living Materials for Highly Efficient Uranium Capture and Accumulation","authors":"Feng-He Li, Zi-Han Liang, Hong Sun, Qiang Tang, Han-Qing Yu","doi":"10.1021/acs.est.4c07276","DOIUrl":"https://doi.org/10.1021/acs.est.4c07276","url":null,"abstract":"Uranium is the primary fuel for nuclear energy, critical for sustainable, carbon-neutral energy transitions. However, limited terrestrial resources and environmental risks from uranium contamination require innovative immobilization and recovery solutions. In this work, we present a novel uranium recovery method using programmable electroactive living materials (ELMs). Utilizing <i>Shewanella oneidensis</i>, this approach leverages the intrinsic extracellular electron transfer capability of exoelectrogenic species, combining their adaptability and programmability with the robustness of engineered multicellular systems. These exoelectrogenic cells were endowed to selectively capture and enhance U(VI) reduction by expressing uranyl-binding proteins, coupled with a reconfigured transmembrane Mtr electron nanoconduit. By incorporating biofilm-promoting circuits, we improved cell-to-cell interactions and biofilm formation, enabling the stable assembly of ELMs with robust structural integrity. The ELMs demonstrated superior electrogenic activity, achieving a 3.30-fold increase in current density and a 3.15-fold increase in voltage output compared to controls in microbial electrochemical and fuel cells. When applied for uranium recovery, the ELMs exhibited robust U(VI) capture, reduction, and accumulation capabilities, with a maximum capacity of 808.42 μmol/g. This work not only provides a versatile and environmentally friendly solution for uranium recovery, but also highlights the potential of ELMs in sustainable environmental and energy technologies.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"19 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2024-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142832860","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}
环境科学与技术Pub Date : 2024-12-17Epub Date: 2024-12-04DOI: 10.1021/acs.est.4c06267
Florian Schunck, Bernhard Kodritsch, Martin Krauss, Wibke Busch, Andreas Focks
{"title":"Integrating Time-Resolved <i>nrf2</i> Gene-Expression Data into a Full GUTS Model as a Proxy for Toxicodynamic Damage in Zebrafish Embryo.","authors":"Florian Schunck, Bernhard Kodritsch, Martin Krauss, Wibke Busch, Andreas Focks","doi":"10.1021/acs.est.4c06267","DOIUrl":"10.1021/acs.est.4c06267","url":null,"abstract":"<p><p>The immense production of the chemical industry requires an improved predictive risk assessment that can handle constantly evolving challenges while reducing the dependency of risk assessment on animal testing. Integrating omics data into mechanistic models offers a promising solution by linking cellular processes triggered after chemical exposure with observed effects in the organism. With the emerging availability of time-resolved RNA data, the goal of integrating gene expression data into mechanistic models can be approached. We propose a biologically anchored TKTD model, which describes key processes that link the gene expression level of the stress regulator <i>nrf2</i> to detoxification and lethality by associating toxicodynamic damage with <i>nrf2</i> expression. Fitting such a model to complex data sets consisting of multiple endpoints required the combination of methods from molecular biology, mechanistic dynamic systems modeling, and Bayesian inference. In this study, we successfully integrate time-resolved gene expression data into TKTD models and thus provide a method for assessing the influence of molecular markers on survival. This novel method was used to test whether <i>nrf2</i> can be applied to predict lethality in zebrafish embryos. With the presented approach, we outline a method to successfully approach the goal of a predictive risk assessment based on molecular data.</p>","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":" ","pages":"21942-21953"},"PeriodicalIF":10.8,"publicationDate":"2024-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142778705","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}
环境科学与技术Pub Date : 2024-12-17DOI: 10.1021/acs.est.4c05660
Shahin Ahmed Sujon, Anna Fabiszak, Janice Brahney, Kyle J. Moor
{"title":"Wavelength Sensitive Plastic Photodissolution: Elucidating Quantum Yield Trends for Solar Activation Spectra","authors":"Shahin Ahmed Sujon, Anna Fabiszak, Janice Brahney, Kyle J. Moor","doi":"10.1021/acs.est.4c05660","DOIUrl":"https://doi.org/10.1021/acs.est.4c05660","url":null,"abstract":"Plastic photodissolution into dissolved organic carbon (DOC) is a key proposed loss pathway for plastic in aquatic environments. However, the specific solar excitation wavelengths that drive photodissolution remain unknown, limiting our ability to model and predict photodissolution rates in natural aquatic environments. To better understand the impact of solar excitation wavelength on plastic photodissolution rates, we measured the wavelength sensitivity of photodissolution for a variety of transparent and semitransparent commercial and postconsumer plastic films with wide-spanning polymer chemistries. We irradiated plastic films using custom-built light-emitting diode (LED) photoreactors that emit light in the range of 275 to 445 nm and found that plastics exhibit a strong wavelength sensitivity, producing the highest DOC release rates for short wavelength ultraviolet (UV) light. We additionally calculated photodissolution quantum yield trends for transparent plastic films and then calculated photodissolution activation spectra. We found that solar UV light between 300–350 nm is responsible for most of the plastic photodissolution for all plastic compositions and predicted plastic photodissolution rates within water columns. Results advance our ability to model plastic photodissolution in natural aquatic environments.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"12 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2024-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142832858","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}
{"title":"Photoreforming of Plastic Waste to Sustainable Fuels and Chemicals: Waste to Energy","authors":"Shuai Yue, Zhiyong Zhao, Tao Zhang, Fei Li, Pengfei Wang, Sihui Zhan","doi":"10.1021/acs.est.4c06688","DOIUrl":"https://doi.org/10.1021/acs.est.4c06688","url":null,"abstract":"The extensive accumulation of plastic waste has given rise to severe environmental pollution issues. Contemporary conventional recycling methods, such as incineration and landfilling, contribute significantly to pollutant emissions and carbon footprints, against the principles of sustainable development. Leveraging renewable solar energy to transform plastics into high-value chemicals and green fuels offers a more promising and sustainable approach to managing plastic waste resources. This comprehensive review centers on the recent advancements in plastic photoreforming, categorizing them based on the types of end products. Particular emphasis is placed on the evolving research landscape surrounding the conversion of plastics into high-value chemicals through photoreforming, as well as the economic considerations for large-scale photoreforming production. The analysis conducted here reveals key pathways and emerging trends that are poised to shape the trajectory of enhanced photoconversion, ultimately influencing the realization of a carbon-neutral future.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"247 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2024-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142832859","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}
环境科学与技术Pub Date : 2024-12-17DOI: 10.1021/acs.est.4c08009
Xiuxiu Yao, Wendi Huo, Yuchen Wang, Dongfang Xia, Yan Chen, Yuhua Tang, Huayong Tang, Wenjiang Yang, Yu Liu, Jingquan Xue, Qing Yuan, Xueyun Gao, Kai Cao
{"title":"Environmental Low-Dose Radiation Activates Th1 Immunity through the Mitochondria-STING Pathway","authors":"Xiuxiu Yao, Wendi Huo, Yuchen Wang, Dongfang Xia, Yan Chen, Yuhua Tang, Huayong Tang, Wenjiang Yang, Yu Liu, Jingquan Xue, Qing Yuan, Xueyun Gao, Kai Cao","doi":"10.1021/acs.est.4c08009","DOIUrl":"https://doi.org/10.1021/acs.est.4c08009","url":null,"abstract":"The presence of low-dose radiation (LDR) in the environment has become more prevalent. However, the effect of LDR exposure on the immune system remains elusive. Here, we interestingly found that LDR specifically elevated the percentage of CD4<sup>+</sup>IFNγ<sup>+</sup> Th1 splenocytes, both in vitro and in vivo, without affecting the percentage of CD8<sup>+</sup>IFNγ<sup>+</sup> Tc1 cells and regulatory T cells. A similar phenomenon was found in T cells from peripheral blood. Mechanistically, we found that LDR can induce mitochondrial damage, which stimulated the STING signaling pathway, leading to the enhanced expression of T-bet, the master transcriptional factor of Th1-cell differentiation. The specific STING signal inhibitor can abrogate the effect of LDR on Th1 differentiation, confirming the central role of the STING pathway. To further validate the immunoregulatory role of LDR, we exposed mice with whole body LDR and evaluated if LDR could protect mice against triple-negative breast cancer through enhanced antitumor immunity. As expected, LDR significantly delayed tumor development and promoted cell death. Meanwhile, LDR resulted in increased tumor-infiltrating Th1 cells, while the proportion of Tc1 and Treg cells remained unchanged. Furthermore, the infiltration of antitumor macrophages was also increased. In summary, we revealed that environmental LDR could specifically regulate Th1 T-cell activities, providing critical information for the potential application of LDR in both clinical and nonclinical settings.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"201 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2024-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142841408","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}
环境科学与技术Pub Date : 2024-12-17DOI: 10.1021/acs.est.4c12812
Julie B. Zimmerman, Susan Richardson, Fernando Rosario-Ortiz, David Waite
{"title":"The 2023 Environmental Science & Technology Best Paper Awards","authors":"Julie B. Zimmerman, Susan Richardson, Fernando Rosario-Ortiz, David Waite","doi":"10.1021/acs.est.4c12812","DOIUrl":"https://doi.org/10.1021/acs.est.4c12812","url":null,"abstract":"This article has not yet been cited by other publications.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"20 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2024-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142832781","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}
环境科学与技术Pub Date : 2024-12-17DOI: 10.1021/acs.est.4c10227
Yuhan Xu, Tianzhu Wang, Zaiming Chen, Yungui Li, Dan Huang, Fangjie Guo, Meizhen Wang
{"title":"Hydrolysis of p-Phenylenediamine Antioxidants: The Reaction Mechanism, Prediction Model, and Potential Impact on Aquatic Toxicity","authors":"Yuhan Xu, Tianzhu Wang, Zaiming Chen, Yungui Li, Dan Huang, Fangjie Guo, Meizhen Wang","doi":"10.1021/acs.est.4c10227","DOIUrl":"https://doi.org/10.1021/acs.est.4c10227","url":null,"abstract":"While <i>p</i>-phenylenediamine antioxidants (PPDs) pose potential risks to aquatic ecosystems, their environmental persistence and transformation remain ambiguous due to the undefined nature of PPD C–N bond hydrolysis. Here, we investigated the hydrolysis patterns of PPDs by analyzing their hydrolysis half-lives, hydrolysis products around neutral pH (pH 6.0–7.7), and the role of atoms within the C–N bonds in PPDs. Hydrolysis preferentially targets the aromatic secondary amine N with the strongest proton affinity and the C atom of C–N with the highest nucleophilic-attack reactivity. The hydrolysis half-life (<i>t</i><sub>1/2</sub>) shortens when the maximum proton affinity of N increases. These results are supported by theoretical calculations, demonstrating a hydrolysis reaction propelled by proton transfer from water to N and complemented by aromatic nucleophilic substitution of N in C–N by water hydroxyl. With the experimental results and the atom reactivity-based predictive model, the <i>t</i><sub>1/2</sub> around neutral pH for 60 PPDs (monitored in environment, commercially available, or under investigation) is determined, showing variations ranging from 2.2 h to 47 days. The model prediction of primary C–N hydrolysis is confirmed through typical PPDs. With the elucidated mechanism and developed model, this research provides new insights into PPD hydrolysis, underscoring its significance in delineating environmental impacts.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"4 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2024-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142832861","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}
环境科学与技术Pub Date : 2024-12-17DOI: 10.1021/acs.est.4c1281210.1021/acs.est.4c12812
Julie B. Zimmerman*, Susan Richardson, Fernando Rosario-Ortiz and David Waite,
{"title":"The 2023 Environmental Science & Technology Best Paper Awards","authors":"Julie B. Zimmerman*, Susan Richardson, Fernando Rosario-Ortiz and David Waite, ","doi":"10.1021/acs.est.4c1281210.1021/acs.est.4c12812","DOIUrl":"https://doi.org/10.1021/acs.est.4c12812https://doi.org/10.1021/acs.est.4c12812","url":null,"abstract":"","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"58 50","pages":"21905–21907 21905–21907"},"PeriodicalIF":10.8,"publicationDate":"2024-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142850201","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}