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Widespread Emissions of Polychlorinated Biphenyls from Building Materials in Vermont Schools 佛蒙特州学校建筑材料广泛排放多氯联苯
IF 9.028 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2026-02-03 DOI: 10.1021/acs.est.5c10939
Jason B. X. Hua, Rachel F. Marek, Michael P. Jones, Trevor D. Erb, Sarah C. Owen, Keri C. Hornbuckle
In collaboration with Vermont state and school officials, we conducted a research study to measure emissions of polychlorinated biphenyls (PCBs) from room surfaces in Vermont schools. Our study, the largest of its kind, investigated the sources of airborne PCBs in indoor school environments. Using simultaneous deployment of air samplers and emission samplers, we measured airborne PCBs in 16 schools and 98 school rooms constructed prior to 1980. There was a wide range in PCB air concentrations (1.7–5700 ng m–3, n = 159) and surface emissions (33–830,000 ng m–2 d–1, n = 182) across different schools as well as between rooms in the same school. We found that emissions of PCB congeners from walls, floors, ceiling and wall expansion joint caulking, and spray insulation explain the airborne PCB congener concentrations in many rooms. Our emission samplers identified three distinct types of building materials with emissions exceeding 30,000 ng m–2 d–1 including expansion joint sealant (up to 480,000 ng m–2 d–1), glass block windows (up to 30,000 ng m–2 d–1), and fireproof coating on steel columns (up to 830,000 ng m–2 d–1). Consequently, school staff have an estimated excess lifetime cancer risk from both dioxin-like and nondioxin-like PCBs that ranges from 1.3 × 10–8 to 1.7 × 10–4 for central tendency exposure, and 2.8 × 10–8 to 3.8 × 10–4 for reasonable maximum exposure (State of Vermont’s target cancer risk = 1 × 10–6). Although production has been banned for decades, our study illustrates that PCBs continue to pose an exposure risk to occupants due to their long history of use in building materials. Our findings underscore the risks associated with the historic presence of PCB-containing building materials, offering critical insights for community efforts aimed at reducing exposure among children and school staff in thousands of schools across the country.
我们与佛蒙特州和学校官员合作,进行了一项研究,测量佛蒙特州学校房间表面多氯联苯(PCBs)的排放量。我们的研究是同类研究中规模最大的,调查了室内学校环境中空气中多氯联苯的来源。通过同时部署空气采样器和排放采样器,我们测量了16所学校和98间1980年以前建造的教室中空气中的多氯联苯。不同学校之间以及同一学校的不同房间之间,PCB空气浓度(1.7-5700 ng m-3, n = 159)和地表排放(33-830,000 ng m-2 d-1, n = 182)的差异很大。我们发现,从墙壁、地板、天花板和墙壁的伸缩缝嵌缝以及喷雾绝缘中排放的PCB同系物解释了许多房间中空气中PCB同系物的浓度。我们的排放样本确定了三种不同类型的建筑材料,其排放量超过30,000 ng m-2 d-1,包括伸缩缝密封胶(高达480,000 ng m-2 d-1),玻璃块窗户(高达30,000 ng m-2 d-1)和钢柱防火涂层(高达830,000 ng m-2 d-1)。因此,学校工作人员对二恶英样多氯联苯和非二恶英样多氯联苯的过量终生癌症风险估计为:集中倾向暴露在1.3 × 10-8至1.7 × 10-4之间,合理最大暴露在2.8 × 10-8至3.8 × 10-4之间(佛蒙特州的目标癌症风险= 1 × 10-6)。虽然生产已经被禁止了几十年,但我们的研究表明,由于多氯联苯在建筑材料中的长期使用,它继续对居住者构成暴露风险。我们的研究结果强调了与含多氯联苯建筑材料的历史存在相关的风险,为旨在减少全国数千所学校的儿童和学校员工接触多氯联苯的社区努力提供了重要见解。
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引用次数: 0
Exposure to Quaternary Ammonium Compounds (QACs) in Assisted Living Facilities: Implications for Older Adults 在辅助生活设施中暴露于季铵化合物(QACs):对老年人的影响
IF 9.028 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2026-02-03 DOI: 10.1021/acs.est.5c05821
Minghao Kong, Tret Burdette, Raghu Sanath Kumar, Claire Dempsey, Parinya Panuwet, Amina Salamova
Quaternary ammonium compounds (QACs) are commonly used in disinfecting and personal care products for their antimicrobial, surfactant, and preservative properties. This study provides the first comprehensive assessment of QACs in assisted living facilities through the analysis of 19 QACs from three different QAC subgroups in indoor dust and air samples collected from three assisted living facilities in Indiana, United States (US), as well as in wristbands worn by the residents and staff of these facilities. The medians of the total QAC concentrations (∑QAC, the sum of 19 QAC concentrations) were 151,000 ng/g in dust, 3.17 ng/m3 in air, and 2,290 ng/g in wristbands. Benzylalkyldimethylammonium compounds (BACs) were the most abundant QAC group in all three matrices and contributed 58–87% to the ∑QAC concentrations. The QAC distribution patterns found in dust, air, and wristbands were similar to those reported for disinfecting products, suggesting these products could be an important indoor source in assisted living. QAC concentrations in wristbands worn by staff during their work shift were significantly higher than those in wristbands worn by residents (p < 0.05). In addition, the levels found in dust from assisted living were several times higher than those previously reported in US residential households. Concentrations of C12-, C14-, and C16-BACs in dust, air, and wristbands significantly and positively correlated, suggesting common sources in the indoor environment. Estimated daily intake (EDI) of QACs suggests that accidental dust ingestion is the predominant exposure route, accounting for approximately 62% of the total QAC intake. The elevated QAC concentrations in assisted living facilities are of concern for the residents and staff of these facilities because of the potential health risks associated with exposure to these chemicals, such as respiratory effects.
季铵化合物(QACs)因其抗菌、表面活性剂和防腐性能而常用于消毒和个人护理产品中。本研究通过分析从美国印第安纳州三家辅助生活设施收集的室内灰尘和空气样本以及这些设施的居民和工作人员佩戴的腕带中来自三个不同QAC亚组的19个QAC,首次对辅助生活设施中的QAC进行了全面评估。总QAC浓度中位数(∑QAC, 19个QAC浓度之和)分别为:粉尘151,000 ng/g,空气3.17 ng/m3,腕带2,290 ng/g。苯烷基二甲基铵化合物(BACs)是3种基质中最丰富的QAC基团,对∑QAC浓度的贡献为58 ~ 87%。在灰尘、空气和腕带中发现的QAC分布模式与报道的消毒产品相似,表明这些产品可能是辅助生活中重要的室内来源。工作人员当班佩戴的腕带中QAC浓度显著高于居民佩戴的腕带(p < 0.05)。此外,在辅助生活中发现的粉尘水平比之前报道的美国住宅家庭高出几倍。粉尘、空气和手环中C12-、C14-和C16-BACs浓度呈显著正相关,提示室内环境中存在共同来源。QAC的估计每日摄入量(EDI)表明,意外粉尘摄入是主要的暴露途径,约占QAC总摄入量的62%。辅助生活设施中质量空气污染物浓度的升高引起了这些设施的居民和工作人员的关注,因为接触这些化学品会带来潜在的健康风险,例如呼吸影响。
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引用次数: 0
3D-Engineered Electroactive Biosensors for Rapid and Sensitive Detection of Environmental Contaminants 3d工程电活性生物传感器快速和敏感的检测环境污染物
IF 9.028 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2026-02-03 DOI: 10.1021/acs.est.5c15345
Xingyu Wang,Xiao-Li Liu,Yixuan Wang,Meng-Jie Luo,Meng Liu,Dong-Feng Liu,Zhixiang She,Yang Mu
The growing concern about water pollution has intensified the demand for rapid and sensitive pollutant monitoring. Electroactive biosensors (e-biosensors) hold significant potential in detecting toxic pollutants through bioelectrical signal responses but are constrained by inefficient electron and mass transport within conventional biofilm-based architectures. Here, we address both limitations by developing a 3D-engineered e-biosensor with a synergistically optimized material composition and geometric architecture. A novel electroactive living material was fabricated by incorporating Ca2+-doped PEDOT:PSS to enhance microbial extracellular electron transport. The living material was then engineered into a grid-structure e-biosensor by extrusion-based 3D bioprinting, significantly improving analyte mass transport to the sensing cells. This dual optimization resulted in the 3D-engineered e-biosensor exhibiting a 6.3-fold increase in baseline current, a 1.9-fold improvement in signal-to-noise ratio, and an extended operational stability (>140 h) relative to conventional biofilm-based counterparts. Moreover, the 3D-engineered e-biosensors demonstrated a rapid response (<20 min) to various toxic pollutants, including Cr(VI) and nitrobenzene. Additionally, we constructed a portable device integrating the 3D-engineered e-biosensors and successfully validated its effectiveness and reproducibility for pollution monitoring in real waters. This work establishes a new paradigm for e-biosensor engineering by integrating materials science and digital biomanufacturing, offering an innovative solution for water pollution monitoring.
人们对水污染的日益关注加剧了对快速、灵敏的污染物监测的需求。电活性生物传感器(e-biosensors)在通过生物电信号响应检测有毒污染物方面具有巨大的潜力,但在传统的基于生物膜的结构中受到低效的电子和质量传输的限制。在这里,我们通过开发具有协同优化材料组成和几何结构的3d工程电子生物传感器来解决这两个限制。通过掺入Ca2+掺杂的PEDOT:PSS制备了一种新型的电活性生物材料,以增强微生物的细胞外电子传递。然后,通过基于挤压的3D生物打印技术,将活性材料设计成网格结构的电子生物传感器,显著改善了分析物向传感细胞的传输。这种双重优化导致3d工程电子生物传感器的基线电流增加了6.3倍,信噪比提高了1.9倍,并且与传统的基于生物膜的同类产品相比,工作稳定性(>140小时)得到了延长。此外,3d工程的电子生物传感器对各种有毒污染物(包括Cr(VI)和硝基苯)表现出快速反应(<20分钟)。此外,我们构建了一个集成3d工程电子生物传感器的便携式设备,并成功验证了其在真实水域污染监测中的有效性和可重复性。本研究将材料科学与数字生物制造相结合,建立了电子生物传感器工程的新范式,为水污染监测提供了创新的解决方案。
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引用次数: 0
Vegetation-Mediated Carbon Inputs and Erosion Protection Shape Soil Carbon Dynamics across Aridity Thresholds 植被介导的碳输入和侵蚀保护影响干旱阈值土壤碳动态
IF 9.028 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2026-02-03 DOI: 10.1021/acs.est.5c07643
Yuntao Wu, Josep Peñuelas, Jalaid Naersige, Jie Luo, Heng Ge, Xingming Zhang, Pengfei Chang, Ping Li, Lingli Liu
Intensified aridity beyond a critical threshold could disrupt vegetation, microbial, and soil processes, reshaping the mechanisms controlling soil carbon (C) storage in drylands. However, the aridity threshold at which the transition occurs and how the controls over different soil C fractions shift remain unclear. Here, we conducted a 2400 km transect survey across 45 sites spanning a broad aridity gradient in temperate grasslands of China. We identified a pronounced shift in the dominant drivers of soil C storage at an aridity threshold of 0.749. Below this threshold, complex vegetation structures enhanced soil C by promoting microbial activity and mineral abundance, which stimulated the accumulation of both POM and MAOM, with a stronger effect on POM. Above the threshold, fine roots dominated soil biochemical processes, sustaining microbial activity and mineral formation that indirectly stabilized SOC, particularly via MAOM. Across the entire aridity gradient, vegetation structure mediated surface soil susceptibility to wind erosion with complex structures providing effective protection, while simpler structures offered limited buffering. These findings highlight the dual role of vegetation-mediated C input and wind erosion protection in sustaining soil stocks in drylands, underscoring the need to account for canopy and root structure when species are selected for dryland restoration.
超过临界阈值的干旱加剧可能破坏植被、微生物和土壤过程,重塑控制旱地土壤碳(C)储存的机制。然而,发生转变的干旱阈值以及对不同土壤C组分的控制如何转变仍不清楚。在此,我们在中国温带草原的45个地点进行了2400公里的样带调查,跨越了广阔的干旱梯度。我们发现,在干旱阈值为0.749时,土壤C储存的主要驱动因素发生了明显的变化。在此阈值以下,复杂植被结构通过促进微生物活性和矿物质丰度来提高土壤C,从而刺激POM和MAOM的积累,且对POM的影响更强。高于阈值,细根主导土壤生化过程,维持微生物活动和矿物质形成,间接稳定有机碳,特别是通过MAOM。在整个干旱梯度中,植被结构调节了表层土壤对风蚀的敏感性,复杂的结构提供了有效的保护,而简单的结构提供了有限的缓冲。这些发现强调了植被介导的碳输入和风蚀保护在维持旱地土壤储量方面的双重作用,强调了在选择物种进行旱地恢复时需要考虑冠层和根系结构。
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引用次数: 0
Temporal Trends of Per- and Polyfluoroalkyl Substances (PFASs) in Tibetan Plateau Sediment Cores (1952–2020): Tracking Global Emission History and Industrial Transformation in PFAS Production 青藏高原沉积物岩心中全氟和多氟烷基物质(PFASs)的时间趋势(1952-2020):追踪全球排放历史和PFAS生产的产业转型
IF 9.028 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2026-02-03 DOI: 10.1021/acs.est.5c11161
Tengfei Cui, Yu Chen, Qianchen Fu, Xinyi Chen, Wei Luo, Yiyao Pan, Yifan Chen, Yali Shi, Ruiqiang Yang, Qinghua Zhang, Guibin Jiang
The Tibetan Plateau (TP), a critical sentinel for tracking long-range atmospheric transport (LRAT) of anthropogenic pollutants, provides indispensable archives for evaluating historical pollutant dynamics in pristine ecosystems. This study investigated temporal variations of 26 per- and polyfluoroalkyl substances (PFASs) in four alpine lake sediment cores across the TP spanning 1952–2020. Total PFAS concentrations ranged from 43.7 to 1428 pg g–1 of dw. Linear regression of log-transformed PFAS concentration revealed a significant elevation-dependent trend across the studied lakes (R2 = 0.58, p < 0.01) after excluding the lower-altitude, more human-impacted Qinghai Lake (3190 m), supporting mountain cold-trapping of these pollutants in high-altitude environments. Ranwu Lake demonstrated a unique PFAS profile dominated by perfluorobutanoic acid (PFBA), which contributed 48% of total PFASs on average, reflecting the predominant influence of glacier meltwater input pathways. The deposition flux exhibited an overall increasing trend, with fluctuations between 7.62 and 258 pg cm–2 a–1 during the studied period. Following a phase of relative stability or slight decline in the 1980s–1990s, all lakes showed a pronounced and sustained rise after 2000. Notably, the doubling time of short-chain PFBA (C4) flux in these lakes was estimated to be 7.4–15.6 years since the post-2000 period. Compositional analysis revealed a global shift from long-chain to short-chain PFASs in TP lake sediments, as reflected by declining PFOS (C8) and rapidly increasing levels of PFBA. The sedimentary record reveals temporal PFAS trends that closely track the historical evolution of global and regional PFAS emissions. Our findings provide crucial insights into the long-term trends of PFAS pollution in high-altitude ecosystems, contributing to global PFAS management efforts by assessing the effectiveness of regulations and the environmental impacts of industrial relocations.
青藏高原是人类活动污染物远距离大气输送的重要哨站,为评价原始生态系统污染物的历史动态提供了不可或缺的资料。研究了1952-2020年青藏高原4个高寒湖泊沉积物岩心中26种全氟烷基和多氟烷基物质(PFASs)的时间变化规律。总PFAS浓度范围为43.7 ~ 1428 pg g-1 / dw。在排除海拔较低、受人类活动影响较大的青海湖(3190 m)后,对数转换后的PFAS浓度线性回归显示,各湖泊之间存在显著的海拔依赖趋势(R2 = 0.58, p < 0.01),这支持了这些污染物在高海拔环境中的高山冷捕。然武湖呈现出以全氟丁酸(PFBA)为主的独特PFAS特征,平均占总PFAS的48%,反映了冰川融水输入途径的主导作用。沉积通量总体呈增加趋势,波动幅度在7.62 ~ 258 pg cm-2 a-1之间。在经历了80 - 90年代的相对稳定或轻微下降之后,所有湖泊在2000年之后都呈现出明显和持续的上升。值得注意的是,自2000年后,这些湖泊的短链PFBA (C4)通量增加了一倍的时间估计为7.4-15.6年。全氟辛烷磺酸(PFOS)呈下降趋势,全氟辛烷磺酸(PFBA)呈快速上升趋势。沉积记录揭示了PFAS的时间趋势,与全球和区域PFAS排放的历史演变密切相关。我们的研究结果为了解高海拔生态系统中PFAS污染的长期趋势提供了重要见解,通过评估法规的有效性和工业搬迁的环境影响,为全球PFAS管理工作做出了贡献。
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引用次数: 0
Recovered Calcium-Based Phosphorus Products from Synthetic Swine Wastewater: Fate and Behavior in Soils 从猪合成废水中回收的钙基磷产品:在土壤中的命运和行为
IF 9.028 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2026-02-02 DOI: 10.1021/acs.est.5c05565
Kasuni H. H. Gamage,Ganga M. Hettiarachchi,Evan Heronemus,Prathap Parameswaran
The increasing demand for phosphorus (P) sources and concerns about surface water quality raise the need to explore safe and efficient secondary P fertilizer sources. This study evaluated the effectiveness of a Ca-based recovered nutrient product (RNP) from synthetic swine wastewater using an innovative anaerobic membrane bioreactor (AnMBR) technology. This study aimed to characterize and compare the dissolution, transformations, and potential bioavailability of P in RNP with conventional P fertilizers (monoammonium phosphate; MAP, triple superphosphate; TSP) in selected soils over time by using short-term laboratory incubation studies in Petri dishes. Soil samples sectioned from the point of application were assessed for pH, total P, resin-extractable P, and selected samples by using X-ray absorption near-edge structure spectroscopy. The RNP treatment showed that over 90%, 70%, and 80% of added P remained in the center section in calcareous, neutral, and acid soils, respectively, where the potential plant-available P was greater than the control in all soils and similar to the MAP treatment only in acid soil after 5 weeks of incubation. The hydroxyapatite-like species dominated P speciation in both RNP and RNP-added soils, leading to less solubility. These results underscore the potential of Ca-based RNP as a P source for tested soils, and process modifications could yield a series of viable secondary P sources for agriculture.
随着对磷源需求的增加和对地表水水质的关注,迫切需要探索安全高效的二次磷肥来源。本研究利用创新的厌氧膜生物反应器(AnMBR)技术,评估了从合成猪废水中提取ca基回收营养物(RNP)的有效性。本研究旨在通过在培养皿中进行短期实验室培养研究,表征和比较RNP中P与常规P肥料(磷酸一铵、MAP、三重过磷酸磷、TSP)在选定土壤中的溶解、转化和潜在的生物利用度。利用x射线吸收近边结构光谱学对土壤样品的pH值、总磷、树脂可提取磷进行了评估。RNP处理表明,在钙质、中性和酸性土壤中,添加磷分别超过90%、70%和80%停留在中心剖面,培养5周后,所有土壤的潜在植物有效磷都大于对照,仅在酸性土壤中与MAP处理相似。在RNP和添加RNP的土壤中,类羟基磷灰石形态占主导地位,导致溶解度降低。这些结果强调了基于ca的RNP作为测试土壤磷源的潜力,并且工艺修改可以为农业产生一系列可行的二次磷源。
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引用次数: 0
Impact of Outdoor Environmental Exposome on Depressive Symptoms Among Children Aged 9–14 in China 室外环境暴露对中国9-14岁儿童抑郁症状的影响
IF 9.028 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2026-02-02 DOI: 10.1021/acs.est.5c10618
Yaqi Wang,Di Shi,Jiajia Dang,Jieyu Liu,Yunfei Liu,Ziyue Chen,Jianhui Guo,Xinyao Lian,Yihang Zhang,Xinxin Wang,Jieyun Song,Yanhui Dong,Jing Li,Yi Song
To assess associations between multiple environmental factors and depressive symptoms (DS) among children and adolescents, we conducted a school-based longitudinal study among 1,418 Chinese students aged 9–14 years, with baseline and follow-up surveys conducted from 2022 to 2023. Twenty outdoor environmental exposures from three domains, air pollutants, meteorological conditions, and geographical features were assessed. DS was measured using the Center for Epidemiologic Studies Depression Scale. An exposome-wide association study was used to explore associations and identify important environmental exposures related to DS, followed by eXtreme Gradient Boosting to rank their relative importance. Composite scores for three environmental domains were constructed to assess their joint impacts on DS. Exposure to PM2.5, PM10, temperature, wind speed, artificial light at night, and building density were significantly associated with increased odds of DS, while higher relative humidity, and higher greenness indicators (Normalized Difference Vegetation Index [NDVI], forest-shrub-grass coverage, and cropland coverage) were inversely associated. Among all exposures, building density showed the greatest contribution in the model ranking. Considering the joint impacts, unfavorable environmental profiles across all three domains were significantly associated with higher odds of DS, particularly among children with abnormal weight or higher metabolic risk. Importantly, population attributable fraction analysis indicates that improving environmental profiles could theoretically reduce 14.22–29.41% of DS cases, with geographical factors showing the largest theoretical contribution. These findings underscore the importance of incorporating environmental considerations into mental health strategies and support urban design and air quality improvements as tailored interventions for vulnerable populations to reduce the burden of DS.
为了评估多种环境因素与儿童和青少年抑郁症状(DS)之间的关联,我们对1418名9-14岁的中国学生进行了一项基于学校的纵向研究,并在2022年至2023年期间进行了基线和随访调查。从空气污染物、气象条件和地理特征三个领域评估了20个室外环境暴露。使用流行病学研究中心抑郁量表测量DS。一项暴露范围关联研究用于探索关联并确定与DS相关的重要环境暴露,然后使用极端梯度增强对其相对重要性进行排序。构建了三个环境域的综合得分来评估它们对DS的共同影响。暴露于PM2.5、PM10、温度、风速、夜间人造光和建筑密度与DS几率增加呈显著相关,而较高的相对湿度和较高的绿化指标(归一化植被指数[NDVI]、森林-灌木-草地覆盖度和农田覆盖度)呈负相关。在所有暴露中,建筑密度对模型排名的贡献最大。考虑到联合影响,所有三个领域的不利环境特征与DS的高几率显著相关,特别是在体重异常或代谢风险较高的儿童中。重要的是,人口归因分数分析表明,改善环境状况理论上可以减少14.22-29.41%的DS病例,其中地理因素的理论贡献最大。这些发现强调了将环境因素纳入心理健康战略的重要性,并支持将城市设计和空气质量改善作为针对弱势群体的量身定制的干预措施,以减轻DS的负担。
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引用次数: 0
Oxygen-Independent Mineralization of Acetaldehyde by a Cyclodextrin-Anchored WO3 Photocatalyst under Visible Light. 可见光下环糊精锚定WO3光催化剂对乙醛的不依赖氧矿化。
IF 11.3 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2026-02-02 DOI: 10.1021/acs.est.5c14689
Woojung Jeon, Seunghyun Weon, Ye He, Wonyong Choi

Photocatalytic degradation of volatile organic compounds (VOCs) using visible light has been widely investigated, but its practical implementation remains constrained by several limiting factors. Here, we prepared carboxymethyl-β-cyclodextrin (CMCD)-anchored WO3 that enabled visible-light-driven mineralization of acetaldehyde even under O2-free conditions. Anchoring CMCD on WO3 facilitated interfacial charge separation, enhancing the photocatalytic performance. Spectroscopic and electrochemical analyses revealed that loading CMCD on WO3 induced the formation of a charge-transfer complex via C-O-W bonding and extended the charge carrier lifetime by trapping electrons in CMCD. CMCD/WO3 sustained OH generation under visible light (λ > 420 nm) and fully mineralized acetaldehyde even in the absence of O2. It also produced dioxygen from water oxidation in O2-free conditions, supplying O2 needed to fully mineralize VOCs to CO2, and it enabled an unconventional three-electron reduction of O2 to OH. CMCD/WO3 exhibited a visible light degradation efficiency comparable to that of Pt-loaded WO3. In particular, CMCD/WO3 exhibited a higher carbon mass balance for acetaldehyde degradation than Pt/WO3, and this value remained nearly unchanged under both oxygen-rich and oxygen-free conditions. CMCD/WO3 also demonstrated long-term stability across repeated photocatalytic cycles with no decomposition of the CMCD structure. These findings highlight a supramolecular design strategy for developing an unconventional visible-light-active photocatalyst for indoor air purification, especially in enclosed or oxygen-depleted environments where conventional photocatalysts fail to operate.

利用可见光光催化降解挥发性有机化合物(VOCs)已经得到了广泛的研究,但其实际应用仍受到一些限制因素的制约。在这里,我们制备了羧甲基-β-环糊精(CMCD)锚定的WO3,即使在无o2的条件下也能实现可见光驱动的乙醛矿化。在WO3上锚定CMCD有利于界面电荷分离,提高了光催化性能。光谱和电化学分析表明,将CMCD加载到WO3上,通过C-O-W键形成电荷转移配合物,并通过捕获CMCD中的电子来延长载流子寿命。CMCD/WO3在可见光(λ > 420 nm)下持续生成•OH,即使在没有O2的情况下也能完全矿化乙醛。它还可以在无O2条件下通过水氧化产生二氧,提供将VOCs完全矿化为CO2所需的O2,并使O2以非常规的三电子还原为•OH。CMCD/WO3的可见光降解效率与pt负载WO3相当。特别是,CMCD/WO3在乙醛降解中表现出比Pt/WO3更高的碳质量平衡,并且在富氧和无氧条件下该值几乎保持不变。CMCD/WO3在重复光催化循环中也表现出长期稳定性,而CMCD结构不会被分解。这些发现强调了一种超分子设计策略,用于开发一种非传统的可见光活性光催化剂,用于室内空气净化,特别是在封闭或缺氧的环境中,传统的光催化剂无法起作用。
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引用次数: 0
Novel Bifunctional Enzyme AntO Catalyzes Antimonite Oxidation and H2O2 Decomposition in Environmental Antimony Detoxification 新型双功能酶AntO在环境锑解毒中催化锑矿氧化和H2O2分解
IF 9.028 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2026-02-02 DOI: 10.1021/acs.est.5c12342
Xiong Luo,Yan Lan,Ming Gao,Mingzhu Xu,Shuhao Liu,Shixue Zheng,Mingshun Li
Microbial oxidation of environmental antimonite (Sb(III)) to antimonate (Sb(V)) is a key antimony (Sb) detoxification mechanism. Comamonas testosteroni JL40 oxidizes Sb(III) to Sb(V) under oxic conditions via an uncharacterized mechanism. A redox-related enzyme identified via differential proteomics was designated AntO. The antO transcription was significantly upregulated upon addition of Sb(III). AntO is predicted to be a catalase-like heme-binding peroxidase, similar to the uncharacterized SrpA. Phylogenetic analysis indicates that AntO represents a novel Sb(III) oxidase or catalase. In E. coli AW3110(Δars), AntO confers Sb(III) resistance and oxidation activity and is induced by Sb(III) and H2O2. Further analysis confirms that antO mediates Sb(III) oxidation and H2O2 decomposition in JL40. Purified AntO catalyzes Sb(III) oxidation (with NADP+ as an electron acceptor) and H2O2 decomposition in vitro. Molecular docking shows that these reactions occur in distinct AntO structural domains. In summary, AntO has dual roles: Sb(III) oxidation for detoxification and H2O2 decomposition. This study identifies AntO as a novel environmental Sb(III) oxidase that facilitates Sb(III) detoxification, alleviates Sb(III)-induced oxidative stress, and advances understanding of microbial contributions to antimony biogeochemical cycling.
微生物氧化环境锑矿(Sb(III))生成锑酸盐(Sb(V))是锑(Sb)解毒的关键机制。睾酮单胞菌JL40在氧化条件下通过未知的机制将Sb(III)氧化为Sb(V)。通过差异蛋白质组学鉴定的氧化还原相关酶被命名为AntO。添加Sb(III)后,antO转录显著上调。预测AntO是一种类似过氧化氢酶的血红素结合过氧化物酶,类似于未表征的SrpA。系统发育分析表明,AntO是一种新的Sb(III)氧化酶或过氧化氢酶。在大肠杆菌AW3110(Δars)中,AntO具有Sb(III)抗性和氧化活性,并由Sb(III)和H2O2诱导。进一步分析证实antO介导了JL40中Sb(III)的氧化和H2O2的分解。纯化的AntO在体外催化Sb(III)氧化(以NADP+为电子受体)和H2O2分解。分子对接表明,这些反应发生在不同的AntO结构域。综上所述,AntO具有双重作用:氧化Sb(III)解毒和分解H2O2。本研究发现AntO是一种新的环境Sb(III)氧化酶,可以促进Sb(III)解毒,减轻Sb(III)诱导的氧化应激,并进一步了解微生物对锑生物地球化学循环的贡献。
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引用次数: 0
Biotransformation of Atmospheric-Aged Metal-Sulfide Nanosheets in Respiratory Tract Fluids Potentiates Ferroptosis toward Alveolar Macrophages 大气老化金属硫化物纳米片在呼吸道液体中的生物转化增强了对肺泡巨噬细胞的铁下垂
IF 9.028 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2026-02-02 DOI: 10.1021/acs.est.5c13859
Wei Zou,Yishuang Chang,Jiahui Wang,Xingli Zhang,Caixia Jin,Jiawei Wang,Guoqing Zhang,Shaohu Ouyang,Zhiguo Cao,Qixing Zhou
The widespread application and unavoidable atmospheric release of transitional metal dichalcogenides (TMDCs) pose significant inhalation-related health risks. During respiration, atmospheric aging of nanoparticles occurs first; nonetheless, the hazard of air-aged TMDCs and the effect of postbiotransformation in the microenvironment following inhalation remain unclear. By mimicking atmospheric conditions and respiratory media, we discovered that air-aged molybdenum disulfide (A-MoS2) and tungsten disulfide (A-WS2) underwent biotransformation in artificial nasal fluids and Gamble’s solution, increasing the hydrophobicity and roughness of the nanosheets. The oxidized products (31.7% in A-MoS2 and 44.5% in A-WS2) were partially converted to sulfidation-state species via thiol-mediated reduction. Both biotransformed and air-aged TMDCs were localized to macrophage lysosomes at approximate concentrations, whereas the lysosomal membrane damage and ferrous ion (Fe2+) release were more significant for biotransformed forms. Transcriptome and lipidomics analyses indicated that ferroprotein degradation and ferroportin1 inhibition also facilitated Fe2+ overload, along with glutathione peroxidase 4 inhibition, lipid acylation, and phospholipid biosynthesis activation, worsening lipid peroxidation (154.3–225.6%). Shapley Additive Explanations substantiated the reduction of oxidized species, 1T-phase stabilization, and increased hydrophobicity as major contributors to ferroptosis aggravation of biotransformed TMDCs. Our findings highlight the necessity of incorporating biotransformation into risk assessment, rather than merely relying on the versions of nanomaterials following environmental processes as the testing endpoints.
过渡金属二硫化物(TMDCs)的广泛应用和不可避免的大气释放构成了与吸入有关的重大健康风险。在呼吸过程中,纳米粒子首先发生大气老化;然而,空气老化TMDCs的危害和吸入后微环境中生物转化的影响尚不清楚。通过模拟大气条件和呼吸介质,我们发现空气老化的二硫化钼(A-MoS2)和二硫化钨(A-WS2)在人工鼻液和甘伯溶液中发生生物转化,增加了纳米片的疏水性和粗糙度。氧化产物(在A-MoS2中为31.7%,在A-WS2中为44.5%)通过硫醇介导的还原部分转化为硫化态物质。生物转化和空气老化的TMDCs都以近似的浓度定位于巨噬细胞溶酶体,而生物转化形式的溶酶体膜损伤和铁离子(Fe2+)释放更为显著。转录组学和脂质组学分析表明,铁蛋白降解和铁portin1抑制也促进了铁离子过载,以及谷胱甘肽过氧化物酶4抑制、脂质酰化和磷脂生物合成激活,加剧了脂质过氧化(154.3-225.6%)。Shapley加性解释证实了氧化态的减少、1t相的稳定和疏水性的增加是生物转化TMDCs铁中毒加重的主要原因。我们的发现强调了将生物转化纳入风险评估的必要性,而不是仅仅依靠纳米材料在环境过程中的版本作为测试终点。
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