环境科学与技术最新文献_第10页

Temporospatial Confined Catalytic Membranes with Controlled Diffusion-Reaction for Ultrafast Water Purification. 时空限制催化膜控制扩散反应用于超快水净化。

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2025-07-30 DOI: 10.1021/acs.est.5c04008

Na Lu,Haibo Lin,Jianqiang Wang,Qiu Han,Fu Liu,Chuyang Y Tang

{"title":"Temporospatial Confined Catalytic Membranes with Controlled Diffusion-Reaction for Ultrafast Water Purification.","authors":"Na Lu,Haibo Lin,Jianqiang Wang,Qiu Han,Fu Liu,Chuyang Y Tang","doi":"10.1021/acs.est.5c04008","DOIUrl":"https://doi.org/10.1021/acs.est.5c04008","url":null,"abstract":"Catalytic membrane is an appealing technology for eliminating refractory organic pollutants in comparison to conventional advanced oxidation methods. However, the application of this technology is constrained by the trade-off between membrane permeability and reactivity. Herein, we prepared a tubular macroporous catalytic membrane (MCM), which activated peroxymonosulfate to produce dominant singlet oxygen (1O2) and hydroxyl radicals (•OH) in the macropore channel (∼130 nm). The optimized MCM membrane demonstrated catalytic filtration performance far beyond the state-of-the-art, achieving >99% degradation of antibiotics, dyes, and phenolic compounds while simultaneously exhibiting ultrafast permeance (645.3 L m-2 h-1 bar-1). For the first time, we reveal the spatial distribution of shorter-lived •OH and long-lived 1O2 in the macropore channel via a diffusion-reaction kinetic model, which provides fundamental insights into how these two reactive oxygen species work synergistically to offer opportunities for breaking the permeability-reactivity trade-off. Furthermore, the MCM achieved robust and stable removal of total organic carbon for a real high-salinity wastewater, verifying its practical potential for treating refractory organics.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"1 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-07-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144737415","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

Biomimetic Dual-Iron-Site Single-Atom Nanozymes for N2-Selective Electrocatalytic Denitrification. 用于n2选择性电催化脱氮的仿生双铁原位单原子纳米酶。

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2025-07-30 DOI: 10.1021/acs.est.5c04948

Wanchao Song,Guoshuai Liu,Hua Zou,Yuan Yao,Shijie You

{"title":"Biomimetic Dual-Iron-Site Single-Atom Nanozymes for N2-Selective Electrocatalytic Denitrification.","authors":"Wanchao Song,Guoshuai Liu,Hua Zou,Yuan Yao,Shijie You","doi":"10.1021/acs.est.5c04948","DOIUrl":"https://doi.org/10.1021/acs.est.5c04948","url":null,"abstract":"Electrocatalytic denitrification (ECDN) for the reduction of NO3- to N2 offers an effective and environmentally benign method for removing nitrogen from wastewater, but challenges remain for poor N2 selectivity. To address this issue, this study reports a dual-iron-site single-atom nanozyme (SAN, FePc@FeNOC) electrocatalyst, resembling the natural cytochrome c-dependent nitric oxide reductase (cNOR). The FePc@FeNOC electrocatalyst exhibits a NO3- removal efficiency as high as 96.1%, accounting for N2 selectivity of 93.3% and Faradaic efficiency of 82.8% at a reaction time of 10 h. The theoretical results reveal that the potential-determining step of ECDN to N2 is more thermodynamically favorable than that to NH3 by FePc@FeNOC, as indicated by the lower free energy barrier for *NO to *N2O2 (0.82 eV) compared with that for *NO to *NOH (0.87 eV). The *N2O2 intermediate demonstrates enhanced charge separation compared with *NOH. The charge redistribution strengthens the electrostatic coupling between FePc@FeNOC and *N2O2, which not only stabilizes the intermediate structure but also creates a thermodynamic driving force for N2 formation. We further demonstrate that the superior N2-selectivity (90%) of FePc@FeNOC can offer a promising electrocatalyst for removing nitrogen from realistic photovoltaic wastewater with a low energy consumption of 9.8 kWh kgN2-1. This work provides a proof-in-concept demonstration of mimicking cNOR toward the sustainable treatment of nitrate-contaminated wastewater.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"142 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-07-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144747852","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

Bird-Inspired Time-Domain Analysis: High-Robustness Intelligent Sensing of Hypochlorite Aerosols. 鸟类启发的时域分析：次氯酸盐气溶胶的高鲁棒性智能感知。

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2025-07-30 DOI: 10.1021/acs.est.5c03485

Xinyi Yang,Cheng Chen,Dongling Wang,Xueting Yan,Lichun Zhang,Yang Feng,Yi Lv

{"title":"Bird-Inspired Time-Domain Analysis: High-Robustness Intelligent Sensing of Hypochlorite Aerosols.","authors":"Xinyi Yang,Cheng Chen,Dongling Wang,Xueting Yan,Lichun Zhang,Yang Feng,Yi Lv","doi":"10.1021/acs.est.5c03485","DOIUrl":"https://doi.org/10.1021/acs.est.5c03485","url":null,"abstract":"The increasing demand for highly reliable sensors capable of anti-interference and sensitive detection of aerosol-associated hypochlorite (ClO-) drives progress in luminescence-based sensing technologies. Inspired by collective behavioral patterns in bird flocks, we developed a \"bird-like flock\" time-domain sensing method through the utilization of functional long afterglow nanomaterials (AGNPs) for ClO- detection. Particularly, by translating avian aggregation-separation-alignment behaviors into an algorithmic framework, we presented a new sensing mode based on simplifying time decay curves into interpretable temporal metrics. In light of dual-emission AGNPs with impressive luminescence performance, ClO--stimulated responsiveness, and derived metrics, our approach accurately distinguished ClO- concentrations down to 95 nM, resulting from the well-refined six temporal parameters. Furthermore, by integrating a portable aerosol generation device via pneumatic atomization and an aerosol-enriched hydrogel sensing matrix, we demonstrated that this time-domain analysis method maintained superior detection accuracy, outperforming traditional methods that often falter with complex water samples. This advancement paves the way for high-contrast sensing while enabling deeper exploration of atmospheric targets. Inspired by the dynamic evolution of avian flock behavior patterns, we developed a high-fidelity analytical method based on time-resolved long-afterglow spectral partitioning for qualitative and quantitative investigation of hypochlorite (ClO-) in atmospheric aerosols.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"65 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-07-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144748080","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

Eugenol-Loaded Nanocarriers Exert Particle-Specific Adverse Effects on Daphnia magna Populations. 载丁香酚的纳米载体对大水蚤种群产生颗粒特异性不利影响。

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2025-07-30 DOI: 10.1021/acs.est.5c03624

Bregje W Brinkmann,Lan Dupuis,Sam Houdijk,Pelle Wattel,Cástor Salgado,Andrea Brunelli,José F Fernández,Willie J G M Peijnenburg,Martina G Vijver

{"title":"Eugenol-Loaded Nanocarriers Exert Particle-Specific Adverse Effects on Daphnia magna Populations.","authors":"Bregje W Brinkmann,Lan Dupuis,Sam Houdijk,Pelle Wattel,Cástor Salgado,Andrea Brunelli,José F Fernández,Willie J G M Peijnenburg,Martina G Vijver","doi":"10.1021/acs.est.5c03624","DOIUrl":"https://doi.org/10.1021/acs.est.5c03624","url":null,"abstract":"Nanocarriers provide promising prospects for the transition to more sustainable agrochemical practices. However, the unique release dynamics of their loaded chemicals raise concerns about potential adverse effects on nontarget organisms. To address this, we compared the toxicity of bentonite and sepiolite nanocarriers loaded with the anesthetic/antibacterial chemical eugenol to the toxicity of pure eugenol. Daphnia magna was exposed to loaded nanocarriers, pure eugenol, and bare nanocarriers. In acute immobilization tests, a 50% effect concentration (EC50) of 0.14 ± 0.01 mg eugenol L-1 was derived for pure eugenol. Loading eugenol onto bentonite and sepiolite nanocarriers mitigated this acute toxicity, as indicated by respective EC50 values of 0.48 ± 0.02 and 0.57 ± 0.07 mg eugenol L-1. In 12-day toxicity tests, similar concentrations of eugenol were released from both nanocarriers. For the first day of exposure, this temporarily reduced the swimming speed of the daphnids. Moreover, in contrast to sepiolite nanocarriers, bentonite nanocarriers induced marked decreases in population growth. This reveals that nanocarriers exert particle-specific adverse effects on daphnid populations that cannot be predicted based on the toxicity of their individual constituents. We therefore plead to assess nontarget effects of the complete nanocarrier system, including the carrier and its loading, before allowing these products on the market.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"68 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-07-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144737417","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

Maternal PM2.5 Exposure and Cardiac Developmental Abnormalities in Fetuses and Neonates: Progressive Activation of the Complement and Coagulation Cascade. 母体PM2.5暴露与胎儿和新生儿心脏发育异常：补体和凝血级联的渐进激活。

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2025-07-30 DOI: 10.1021/acs.est.4c11407

Yuqiong Guo,Sican Niu,Yingying Zhang,Wei Yan,Shaoyang Ji,Li Ma,Guangke Li,Nan Sang

{"title":"Maternal PM2.5 Exposure and Cardiac Developmental Abnormalities in Fetuses and Neonates: Progressive Activation of the Complement and Coagulation Cascade.","authors":"Yuqiong Guo,Sican Niu,Yingying Zhang,Wei Yan,Shaoyang Ji,Li Ma,Guangke Li,Nan Sang","doi":"10.1021/acs.est.4c11407","DOIUrl":"https://doi.org/10.1021/acs.est.4c11407","url":null,"abstract":"Emerging studies indicate a positive correlation between maternal PM2.5 exposure and an increased risk of congenital heart diseases (CHDs). However, the developmental origins in fetal and neonatal offspring, as well as the underlying mechanisms, remain elusive. To bridge this gap, we established an animal model of maternal PM2.5 exposure and confirmed its adverse effects on cardiac function and structure in neonates, primarily left ventricular systolic and diastolic dysfunction and myocardial hypertrophy in both male and female offspring, characterized by thick ventricular walls and narrowed ventricular chambers at embryonic (E) day 18.5. Then, combining transcriptional profiling and immunohistochemical analyses, we found that the upregulation of myosin-related genes was a key mediator in these myocardial contraction abnormalities. Importantly, using time-series transcriptome analysis across critical windows of cardiac development (E10.5, E14.5, and E18.5), we uncovered that the complement and coagulation cascade signaling pathways were progressively activated, triggering cellular inflammation and lysis and upregulating myosin genes, which ultimately contributed to compensatory cardiac hypertrophy and cardiac dysfunction. This work provides a comprehensive perspective for local governments and clinicians to control and prevent CHD burden in polluted areas.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"142 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-07-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144748084","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

Enhanced Thin-Film Composite Nanofiltration Membranes via Substrate Pore Structure Engineering: Performance and Mechanistic Insights. 基于基板孔结构工程的增强薄膜复合纳滤膜：性能和机理研究。

IF 11.3 1区环境科学与生态学

环境科学与技术 Pub Date : 2025-07-29 Epub Date: 2025-07-17 DOI: 10.1021/acs.est.5c06050

Xiao-Gang Jin, Hoei Ying Lim, Qian Wang, Rui Jia, Xiao-Hua Ma, Zhen-Liang Xu, Chuyang Y Tang

{"title":"Enhanced Thin-Film Composite Nanofiltration Membranes via Substrate Pore Structure Engineering: Performance and Mechanistic Insights.","authors":"Xiao-Gang Jin, Hoei Ying Lim, Qian Wang, Rui Jia, Xiao-Hua Ma, Zhen-Liang Xu, Chuyang Y Tang","doi":"10.1021/acs.est.5c06050","DOIUrl":"10.1021/acs.est.5c06050","url":null,"abstract":"Substrate pore size is a key factor influencing the structure and performance of polyamide thin-film composite (TFC) membranes, yet its constitutive relationship and mechanism remain unclear. In this study, we systematically elucidate its critical influence on the selective layer, separation performance, and kinetics of water molecule transport of TFC membranes by employing a combination of experimental investigations and molecular dynamics (MD) simulations. The experimental results revealed the formation of a thinner and less cross-linked polyamide layer on the substrate with larger pore size, leading to a high water permeance of 35.4 L m-2 h-1 bar-1. In contrast, the smaller-pore-size substrate promoted the formation of a polyamide layer with more uniformly distributed pore size, resulting in better solute/solute selectivity (erythromycin/NaCl selectivity = 426). MD simulations confirmed the significant influence of substrate pore size on mass transfer in the TFC membrane. This study offers both fundamental insights and a methodological framework for the targeted design of high-performance TFC nanofiltration membranes by substrate pore size optimization.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":" ","pages":"15538-15546"},"PeriodicalIF":11.3,"publicationDate":"2025-07-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144657864","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

Unveiling Chemical Gradients in the Fertosphere: A Paradigm Shift to Enhance Fertilizer Efficiency and Decrease the Environmental Impact of Overfertilisation. 揭示铁圈中的化学梯度：提高肥料效率和减少过度施肥对环境影响的范式转变。

IF 11.3 1区环境科学与生态学

环境科学与技术 Pub Date : 2025-07-29 Epub Date: 2025-07-17 DOI: 10.1021/acs.est.5c04757

Enzo Lombi, Casey L Doolette, Rodrigo Coqui da Silva, Brigid A McKenna, Peter M Kopittke

{"title":"Unveiling Chemical Gradients in the Fertosphere: A Paradigm Shift to Enhance Fertilizer Efficiency and Decrease the Environmental Impact of Overfertilisation.","authors":"Enzo Lombi, Casey L Doolette, Rodrigo Coqui da Silva, Brigid A McKenna, Peter M Kopittke","doi":"10.1021/acs.est.5c04757","DOIUrl":"10.1021/acs.est.5c04757","url":null,"abstract":"The need to increase food production means that fertilizers will continue to play a key role in farming systems. However, current formulation and practices are increasingly being scrutinized due to the low efficiency of applied nutrients with negative economic and environmental consequences. Enhance nutrient use efficiency requires a comprehensive understanding of soil-fertilizer interactions. Here, we contend that this knowledge has been generated by 'bulk' soil approaches that, while providing useful information, oversimplify these interactions by neglecting the strong chemical gradients occurring in the soils around fertilizers (i.e., in the fertosphere). Progress in non-destructive, in situ, and spatially resolved analytical techniques now allow a paradigm shift in the investigation of fertilizer chemistry in soil. For instance, mapping of diffusive gradients in thin films (DGT) allows for nutrient availability to be quantified in 2D. Complementing DGT information with imaging X-ray absorption near-edge structure (XANES-imaging) provides an avenue to understand how chemical speciation along chemical gradients in the fertosphere controls nutrient availability. This information is essential to improve agronomic practices and for the development of novel fertilizers. This is particularly important in developing fertilizers from recycled materials and return nutrient cycles within, or at least closer to, their planetary boundaries.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":" ","pages":"14853-14861"},"PeriodicalIF":11.3,"publicationDate":"2025-07-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144657867","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

A New Climate Impact of Wildfire Chars: Suppression of Biogenic Methane Production Over Repeated Redox Cycles. 野火燃烧对气候的新影响：在重复氧化还原循环中抑制生物源甲烷的产生

IF 11.3 1区环境科学与生态学

环境科学与技术 Pub Date : 2025-07-29 DOI: 10.1021/acs.est.5c05709

Jiwon Choi, Danhui Xin, Pei C Chiu

{"title":"A New Climate Impact of Wildfire Chars: Suppression of Biogenic Methane Production Over Repeated Redox Cycles.","authors":"Jiwon Choi, Danhui Xin, Pei C Chiu","doi":"10.1021/acs.est.5c05709","DOIUrl":"https://doi.org/10.1021/acs.est.5c05709","url":null,"abstract":"The warming climate has increased the frequency and intensity of wildfires, which can further exacerbate climate change. Here we report the suppression of biogenic methane (CH4) by wildfire chars, a previously unrecognized, potentially beneficial impact of wildfires on global climate. We hypothesized that char derived from wildfires possess an electron storage capacity (ESC) that can support char-respiring microbes, enabling them to outcompete methanogens. A total of 18 chars from fires that occurred between March and October 2023 were collected from across the U.S. All chars possessed sizable ESC, from 0.54 to 2.85 mmol e-/g in the EH range of -0.36 to +0.81 V. Without char, singly 13C-labeled acetate (13CH312COO-) was converted by a wastewater culture into equimolar 13CH4 and 12CO2. In the presence of an air-oxidized char, 13CO2 was produced at the expense of 13CH4, as anaerobic char respirers outcompeted acetoclastic methanogens. Char electron contents measured before and after acetate degradation showed that, electrons that would otherwise end up in CH4 were deposited into char instead. On average, 28.4 ± 2.2% of the wildfire chars' ESC was utilized to divert electrons away from CH4. Aeration of microbially utilized chars restored the chars' capacity to suppress CH4, confirming the redox-reversible nature of ESC. These results improve our understanding of, and ability to assess, the full climate impacts of wildfires and deforestation. This study provides the first significant data set of wildfire char ESC, and the first quantitative demonstration of CH4 suppression by wildfire chars.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":" ","pages":""},"PeriodicalIF":11.3,"publicationDate":"2025-07-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144740632","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

IF 10.8 1区环境科学与生态学

环境科学与技术 Pub Date : 2025-07-29

Joanke van Dijk, Anežka Sharma, Bernd Nowack, Zhanyun Wang and Martin Scheringer*,

引用次数: 0

IF 10.8 1区环境科学与生态学

环境科学与技术 Pub Date : 2025-07-29

Jiaying Hou, Ying Zhu, Yuanji Shi, Limin Lin, Fangang Meng, Meiying Xu, Linyan Yang, Bing-Jie Ni and Xueming Chen*,

引用次数: 0