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A Physically Constrained Deep-Learning Fusion Method for Estimating Surface NO2 Concentration from Satellite and Ground Monitors 利用卫星和地面监测器估算地表 NO2 浓度的物理约束深度学习融合方法
IF 9.028 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-20 DOI: 10.1021/acs.est.4c07341
Jia Xing, Bok H. Baek, Siwei Li, Chi-Tsan Wang, Ge Song, Siqi Ma, Shuxin Zheng, Chang Liu, Daniel Tong, Jung-Hun Woo, Tie-Yan Liu, Joshua S. Fu
Accurate estimation of atmospheric chemical concentrations from multiple observations is crucial for assessing the health effects of air pollution. However, existing methods are limited by imbalanced samples from observations. Here, we introduce a novel deep-learning model-measurement fusion method (DeepMMF) constrained by physical laws inferred from a chemical transport model (CTM) to estimate NO2 concentrations over the Continental United States (CONUS). By pretraining with spatiotemporally complete CTM simulations, fine-tuning with satellite and ground measurements, and employing a novel optimization strategy for selecting proper prior emission, DeepMMF delivers improved NO2 estimates, showing greater consistency and daily variation alignment with observations (with NMB reduced from −0.3 to −0.1 compared to original CTM simulations). More importantly, DeepMMF effectively addressed the sample imbalance issue that causes overestimation (by over 100%) of downwind or rural concentrations in other methods. It achieves a higher R2 of 0.98 and a lower RMSE of 1.45 ppb compared to surface NO2 observations, overperforming other approaches, which show R2 values of 0.4–0.7 and RMSEs of 3–6 ppb. The method also offers a synergistic advantage by adjusting corresponding emissions, in agreement with changes (−10% to −20%) reported in the NEI between 2019 and 2020. Our results demonstrate the great potential of DeepMMF in data fusion to better support air pollution exposure estimation and forecasting.
通过多次观测准确估算大气中的化学物质浓度对于评估空气污染对健康的影响至关重要。然而,现有方法受到观测样本不平衡的限制。在此,我们介绍了一种新型的深度学习模型-测量融合方法(DeepMMF),该方法受化学传输模型(CTM)推断出的物理定律的约束,用于估算美国大陆(CONUS)上空的二氧化氮浓度。通过利用时空完整的 CTM 模拟进行预训练,利用卫星和地面测量数据进行微调,并采用新颖的优化策略选择适当的先验排放,DeepMMF 提供了更好的二氧化氮估计值,显示出与观测结果更高的一致性和日变化一致性(与原始 CTM 模拟相比,NMB 从-0.3 降至-0.1)。更重要的是,DeepMMF 有效地解决了样本不平衡问题,该问题会导致其他方法高估(超过 100%)下风向或农村地区的浓度。与地表二氧化氮观测值相比,它的 R2 值高达 0.98,RMSE 低至 1.45 ppb,优于其他 R2 值为 0.4-0.7 和 RMSE 为 3-6 ppb 的方法。该方法还通过调整相应的排放量提供了协同优势,这与 2019 年至 2020 年期间 NEI 报告的变化(-10% 至 -20%)一致。我们的研究结果证明了 DeepMMF 在数据融合方面的巨大潜力,可以更好地支持空气污染暴露估计和预测。
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引用次数: 0
Mechanistic Modeling of Pollutant Mass Redistribution (Sorption/Desorption) in Heterogeneous Systems Explaining Unexpected Slow Kinetics 异质系统中污染物质量再分布(吸附/解吸)的机理模型,解释意想不到的缓慢动力学过程
IF 9.028 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-20 DOI: 10.1021/acs.est.4c03176
Binlong Liu, Michael Finkel, Qiyue Qin, Wenxiao Shi, Peter Grathwohl
Redistribution of pollutants between different solid phases occurs frequently in field and laboratory settings. Examples include the input of urban particles carrying pollutants into soils or rivers with suspended particles or passive sampling. Since multiple mass transfer mechanisms are involved and natural particles typically are very heterogeneous, modeling of sorption/desorption kinetics is challenging. Here, we present a semi-analytical model formulated in the Laplace domain to simulate pollutant redistribution kinetics in heterogeneous systems. The model accounts for a coupled process governed by intraparticle and external boundary layer diffusion, and it considers the heterogeneity of various sorbents (e.g., geometric shape, size, sorption capacity coefficient, and solid and porous particles). The model is validated against data of two batch experiments: (i) the redistribution of phenanthrene in spherical polyethylene particles of different sizes and (ii) redistribution of anthracene-d10 and phenanthrene in a heterogeneous sediment suspension with polyethylene passive samplers. It allows to explain the temporary overshooting of concentrations in the aqueous phase due to different kinetic controls of various particles involved (fast desorption vs. slow sorption) as well as initial fast kinetics followed by surprising long tailing in batch experiments. The approach is very flexible and can be used for many different scenarios.
污染物在不同固相之间的再分布经常发生在现场和实验室环境中。例如,城市颗粒携带污染物进入土壤或河流的悬浮颗粒或被动采样。由于涉及多种传质机制,而且天然颗粒通常具有很强的异质性,因此吸附/解吸动力学建模具有挑战性。在此,我们提出了一个在拉普拉斯域中制定的半解析模型,用于模拟异质系统中的污染物再分布动力学。该模型考虑了颗粒内部和外部边界层扩散的耦合过程,并考虑了各种吸附剂的异质性(如几何形状、尺寸、吸附容量系数以及固体和多孔颗粒)。该模型根据两个批次实验的数据进行了验证:(i) 菲在不同尺寸的球形聚乙烯颗粒中的再分布;(ii) 蒽-d10 和菲在使用聚乙烯被动采样器的异质沉积悬浮液中的再分布。该方法可以解释水相中由于各种颗粒的动力学控制不同(快速解吸与慢速吸附)而导致的浓度暂时超调,以及批量实验中最初的快速动力学随后出现令人惊讶的长尾现象。这种方法非常灵活,可用于多种不同情况。
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引用次数: 0
Application of a Multispecies Pulse-Exposure Microalgal Bioassay to Assess Duration and Time-of-Day Influences on the Toxicity of Chemicals
IF 10.8 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-20 DOI: 10.1021/acs.est.4c0787510.1021/acs.est.4c07875
Sarah Stone*, Darren J. Koppel, Monique T. Binet, Dianne F. Jolley and Stuart L. Simpson*, 

Aquatic organisms may frequently be exposed to short-term discharges of contaminants, including those from pesticide use, stormwater runoff, or industrial effluents entering waterways. Here, a new microalgal multispecies flow cytometry-based bioassay is used to assess knowledge gaps in risk assessments posed by the short-term exposure of organisms to contaminants. The toxicities of atrazine, metolachlor, and copper were assessed using four exposure scenarios, a 72 h exposure (continuous), an 18 h pulse exposure, and two 3 h pulse exposures (light and dark conditions), that assessed chronotoxicity. The influence of duration on toxicity explored the utility of two expressions of chemical-exposure dose: pulse-exposure concentration (PeC) and time-weighted average concentrations (TACs). The three coexisting microalgae (Monoraphidium arcuatum, Nannochloropsis-like sp., and Pediastrum duplex) tolerated higher concentrations for shorter 3 and 18 h pulses compared to continuous 72 h exposures. Toxicity estimates calculated on a TAC basis were effective for predicting the toxicity of the pulses of atrazine, metolachlor, and copper. Fluorescence data collected using flow cytometry were linked to physiological diel changes for each species. Chronotoxicity was observed for copper with two species. While continuous contaminant exposures provide a conservative estimate of toxicity compared to pulses, the duration and time of exposure are critical factors to consider when assessing the toxicity of contaminants to microalgae.

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引用次数: 0
Improving the Chemical Utilization Efficiency of Pd Hydrodechlorination Catalysts through Hydrogen-Spillover Empowered Synergy between Pd and TiNiN Support 通过氢气溢出促进钯和 TiNiN 载体之间的协同作用提高钯加氢脱氯催化剂的化学利用效率
IF 9.028 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-20 DOI: 10.1021/acs.est.4c05860
Wenxuan Wang, Xiaoling Zhang, Wei Ran, Chunyan Ma, Jiefang Sun, Muyao Zhao, Wenxiao Pan, Jingfu Liu, Rui Liu, Guibin Jiang
The sustainable and affordable environmental application of Pd catalysis needs further improvement of Pd mass activity. Besides the well-recognized importance of physical utilization efficiency─the ratio of surface atoms forming reactant-accessible reactive sites─a lesser-known fact is that the congestion of these reactive sites, which we term as the chemical utilization efficiency, also influences the mass activity. Herein, by leveraging the 100% physical utilization efficiency of a fully exposed Pd cluster (Pdn) and the hydrogenation activity of TiNiN, we developed Pdn/TiNiN as a high physical and chemical utilization efficiency catalyst. During the catalytic hydrodechlorination of 4-chlorophenol and the subsequent hydrogenation of phenol, Pdn focuses on H2 dissociation and C–Cl cleavage, while TiNiN facilitates the subsequent hydrogenation of phenol into less toxic cyclohexanone via H-spillover. This synergy results in a 20–40-fold increase in the hydrodechlorination rate. The enhanced chemical utilization efficiency of Pd informs the design of Pdn/TiNiN microspheres for the conversion of halogenated organics from pharmaceutical wastewater and the design of a fixed-bed reactor to transfer trace amounts of 4-CP from river water. Ultimately, this approach decentralizes the use of Pd in environmental catalysis and reduction processes.
要实现钯催化的可持续和经济环保应用,就必须进一步提高钯的质量活性。除了公认的物理利用效率--形成反应物可进入反应位点的表面原子比例--的重要性之外,一个鲜为人知的事实是,这些反应位点的拥挤程度(我们称之为化学利用效率)也会影响质量活性。在此,我们利用完全暴露的 Pd 簇(Pdn)100% 的物理利用效率和 TiNiN 的氢化活性,开发出 Pdn/TiNiN 作为一种高物理和化学利用效率的催化剂。在催化 4-氯苯酚的加氢脱氯和随后的苯酚加氢过程中,Pdn 专注于 H2 解离和 C-Cl 裂解,而 TiNiN 则通过 H 溢出促进苯酚随后加氢成毒性较低的环己酮。这种协同作用使加氢脱氯速率提高了 20-40 倍。Pd 化学利用效率的提高为 Pdn/TiNiN 微球的设计提供了参考,该微球可用于转化制药废水中的卤代有机物,还可用于设计固定床反应器,从河水中转移微量的 4-CP。最终,这种方法将钯分散用于环境催化和还原过程。
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引用次数: 0
Exosomal miRNAs as Participators of Hexavalent Chromium-Induced Genotoxicity and Immunotoxicity: A Two-Stage Population Study 外泌体 miRNAs 是六价铬诱导的遗传毒性和免疫毒性的参与者:一项两阶段人群研究
IF 9.028 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-20 DOI: 10.1021/acs.est.4c06411
Shiyi Hong, Zekang Su, Yali Zhang, Guiping Hu, Qiaojian Zhang, Zhiqiang Ji, Li Wang, Shanfa Yu, Xiaojun Zhu, Fang Yuan, Guang Jia
Genotoxic and immunosuppressive characteristics are central to the carcinogenic profile of hexavalent chromium [Cr(VI)], with dysregulation of circulating exosomal miRNA potentially acting as oncogenes or tumor suppressors or participating in the carcinogenic landscape of heavy metals through immunomodulation. In this two-stage epidemiological investigation, we unveiled for the first time the perturbations of exosomal miRNAs among individuals exposed to Cr(VI), alongside their significant correlations with biomarkers of genetic injury (γ-H2AX positivity in circulating lymphocytes and the urinary 8-OHdG levels) and immunological indicators (immunosuppressive PD-1 expression), which was supported by validation in an external cohort. Employing a support vector machine model, we discerned that exosomal miRNAs, particularly miR-4467, miR-345-5p, miR-144-3p, and miR-206, exhibited a remarkable capacity to delineate the genetic damage stratum within the population with high precision, and the target genes predicted of these miRNAs further elucidated their intricate regulatory interplay with the effector biomarkers. Additionally, employing a Bayesian mediation framework, we observed the intermediary function of miR-4467 in the nexus between chromium exposure and the escalation of urinary 8-OHdG levels (mediation effect: 0.47, P < 0.05). Although our findings suggested a link between extracellular miRNAs and immunosuppressive biomarkers, this association did not achieve validation in the external cohort, possibly due to population heterogeneity. Collectively, this study advanced our understanding of the epigenetic orchestration of health hazards of Cr(VI) by exosomal miRNAs, shedding light on their expression signatures and their intricate interplay with Cr(VI)-induced genetic and immunological perturbations, thus providing novel perspectives on the toxic pathways of heavy metals.
基因毒性和免疫抑制特性是六价铬[Cr(VI)]致癌特征的核心,循环外泌体miRNA的失调可能充当致癌基因或肿瘤抑制因子,或通过免疫调节参与重金属的致癌过程。在这项分两个阶段进行的流行病学调查中,我们首次揭示了暴露于六价铬的个体的外泌体miRNA干扰,以及它们与遗传损伤生物标志物(循环淋巴细胞中的γ-H2AX阳性和尿液中的8-OHdG水平)和免疫指标(免疫抑制性PD-1表达)之间的显著相关性,并在外部队列中进行了验证。利用支持向量机模型,我们发现外泌体miRNA,尤其是miR-4467、miR-345-5p、miR-144-3p和miR-206,在高精度地划分人群中的遗传损伤层方面表现出卓越的能力,而这些miRNA预测的靶基因进一步阐明了它们与效应生物标志物之间错综复杂的调控相互作用。此外,利用贝叶斯中介框架,我们观察到 miR-4467 在铬暴露与尿 8-OHdG 水平上升之间的中介功能(中介效应:0.47,P < 0.05)。尽管我们的研究结果表明,细胞外 miRNA 与免疫抑制生物标志物之间存在联系,但这种联系并未在外部队列中得到验证,这可能是由于人群的异质性造成的。总之,这项研究加深了我们对细胞外 miRNA 在表观遗传学上协调六价铬对健康危害的理解,揭示了它们的表达特征及其与六价铬诱导的遗传和免疫学干扰之间错综复杂的相互作用,从而为重金属的毒性途径提供了新的视角。
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引用次数: 0
A Physically Constrained Deep-Learning Fusion Method for Estimating Surface NO2 Concentration from Satellite and Ground Monitors
IF 10.8 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-20 DOI: 10.1021/acs.est.4c0734110.1021/acs.est.4c07341
Jia Xing, Bok H. Baek*, Siwei Li*, Chi-Tsan Wang, Ge Song, Siqi Ma, Shuxin Zheng, Chang Liu, Daniel Tong, Jung-Hun Woo, Tie-Yan Liu and Joshua S. Fu, 

Accurate estimation of atmospheric chemical concentrations from multiple observations is crucial for assessing the health effects of air pollution. However, existing methods are limited by imbalanced samples from observations. Here, we introduce a novel deep-learning model-measurement fusion method (DeepMMF) constrained by physical laws inferred from a chemical transport model (CTM) to estimate NO2 concentrations over the Continental United States (CONUS). By pretraining with spatiotemporally complete CTM simulations, fine-tuning with satellite and ground measurements, and employing a novel optimization strategy for selecting proper prior emission, DeepMMF delivers improved NO2 estimates, showing greater consistency and daily variation alignment with observations (with NMB reduced from −0.3 to −0.1 compared to original CTM simulations). More importantly, DeepMMF effectively addressed the sample imbalance issue that causes overestimation (by over 100%) of downwind or rural concentrations in other methods. It achieves a higher R2 of 0.98 and a lower RMSE of 1.45 ppb compared to surface NO2 observations, overperforming other approaches, which show R2 values of 0.4–0.7 and RMSEs of 3–6 ppb. The method also offers a synergistic advantage by adjusting corresponding emissions, in agreement with changes (−10% to −20%) reported in the NEI between 2019 and 2020. Our results demonstrate the great potential of DeepMMF in data fusion to better support air pollution exposure estimation and forecasting.

This study introduces a novel physically constrained deep-learning fusion method for accurately estimating the atmospheric surface concentration to improve better exposure estimates for health assessment of air pollution.

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引用次数: 0
Bottom-Feeders Eat Their Fiber: Ingestion of Anthropogenic Microdebris by Antarctic Deep-Sea Invertebrates Depends on Feeding Ecology 底层食者吃纤维:南极深海无脊椎动物摄取人为微碎屑取决于摄食生态学
IF 9.028 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-20 DOI: 10.1021/acs.est.4c09487
Gabriel Stefanelli-Silva, Pâmela Friedemann, Beatriz Rocha de Moraes, Romulo Augusto Ando, Lúcia de Siqueira Campos, Mônica Angélica Varella Petti, Craig R. Smith, Paulo Yukio Gomes Sumida
Anthropogenic debris has been documented in Antarctica for the past 40 years. Upon breakdown, large pieces become microdebris, which reaches the seafloor through a variety of physical and biological processes. The Antarctic benthos, deeply reliant on sinking organic particles, is thus vulnerable to ingesting microdebris. By using benthic specimens sampled between 1986 and 2016 and deposited in biological collections, we provide the first record of microdebris in Southern Ocean deep-sea invertebrates. Specimens from 15 species (n = 169 organisms) had their gut content examined, with 13 species yielding microdebris in the shape of fibers (n = 85 fibers). The highest ingestion percentages were recorded in the sea cucumbers Heterocucumis steineni (100%), Molpadia violacea (83%) and Scotoplanes globosa (75%), and in the brittle star Amphioplus peregrinator (53%). Deposit- and suspension-feeding were the strategies which yielded the most fibers, accounting for 83.53% of particles. Seven fibers were identified as microplastics, composed of polyamide, polycarbonate, polyester, polyethylene terephthalate, polyisoprene and polysulfone. We also provide the earliest record of a microplastic in Antarctica, a polysulfone fiber ingested by a Boreomysis sp. mysid caught in 1986. The occurrence of fibers in the world’s most remote continental margin renews concerns of pollution in seemingly isolated regions.
过去 40 年来,南极洲一直有人为碎片的记录。大块碎片在分解后成为微碎片,通过各种物理和生物过程到达海底。南极底栖生物深深依赖于下沉的有机颗粒,因此很容易摄入微碎片。通过使用 1986 年至 2016 年间采样并保存在生物馆藏中的底栖标本,我们首次记录了南大洋深海无脊椎动物体内的微碎片。我们对 15 个物种(n = 169 个生物)的标本进行了肠道内容检查,其中 13 个物种发现了纤维状的微碎片(n = 85 纤维)。海参 Heterocucumis steineni(100%)、Molpadia violacea(83%)和 Scotoplanes globosa(75%)以及脆星 Amphioplus peregrinator(53%)的摄取率最高。沉积捕食和悬浮捕食是产生纤维最多的捕食方式,占颗粒的 83.53%。七种纤维被鉴定为微塑料,由聚酰胺、聚碳酸酯、聚酯、聚对苯二甲酸乙二酯、聚异戊二烯和聚砜组成。我们还提供了南极洲最早的微塑料记录,即 1986 年捕获的一条 Boreomysis sp.糠虾摄入的聚砜纤维。纤维出现在世界上最偏远的大陆边缘,再次引起了人们对看似与世隔绝地区的污染问题的关注。
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引用次数: 0
Exosomal miRNAs as Participators of Hexavalent Chromium-Induced Genotoxicity and Immunotoxicity: A Two-Stage Population Study
IF 10.8 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-20 DOI: 10.1021/acs.est.4c0641110.1021/acs.est.4c06411
Shiyi Hong, Zekang Su, Yali Zhang, Guiping Hu*, Qiaojian Zhang, Zhiqiang Ji, Li Wang, Shanfa Yu, Xiaojun Zhu, Fang Yuan and Guang Jia*, 

Genotoxic and immunosuppressive characteristics are central to the carcinogenic profile of hexavalent chromium [Cr(VI)], with dysregulation of circulating exosomal miRNA potentially acting as oncogenes or tumor suppressors or participating in the carcinogenic landscape of heavy metals through immunomodulation. In this two-stage epidemiological investigation, we unveiled for the first time the perturbations of exosomal miRNAs among individuals exposed to Cr(VI), alongside their significant correlations with biomarkers of genetic injury (γ-H2AX positivity in circulating lymphocytes and the urinary 8-OHdG levels) and immunological indicators (immunosuppressive PD-1 expression), which was supported by validation in an external cohort. Employing a support vector machine model, we discerned that exosomal miRNAs, particularly miR-4467, miR-345-5p, miR-144-3p, and miR-206, exhibited a remarkable capacity to delineate the genetic damage stratum within the population with high precision, and the target genes predicted of these miRNAs further elucidated their intricate regulatory interplay with the effector biomarkers. Additionally, employing a Bayesian mediation framework, we observed the intermediary function of miR-4467 in the nexus between chromium exposure and the escalation of urinary 8-OHdG levels (mediation effect: 0.47, P < 0.05). Although our findings suggested a link between extracellular miRNAs and immunosuppressive biomarkers, this association did not achieve validation in the external cohort, possibly due to population heterogeneity. Collectively, this study advanced our understanding of the epigenetic orchestration of health hazards of Cr(VI) by exosomal miRNAs, shedding light on their expression signatures and their intricate interplay with Cr(VI)-induced genetic and immunological perturbations, thus providing novel perspectives on the toxic pathways of heavy metals.

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引用次数: 0
Achieving Stable Partial Denitrification by Selective Inhibition of Nitrite Reductase with the Biosafe Aprotic Solvent DMSO 用生物安全改进型溶剂二甲基亚砜选择性抑制亚硝酸盐还原酶,实现稳定的部分反硝化作用
IF 9.028 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-19 DOI: 10.1021/acs.est.4c08731
Zhi-Bin Wang, Jinpeng Zhang, Qinshu Miao, Hai-Yan Cao, Fei Xiong, Taeho Lee, Amro El-Baz, Liangke Xie, Shou-Qing Ni
The recently proposed partial denitrification (PD), terminating nitrate reduction to nitrite, has been regarded as a promising alternative to nitrite supplying for anammox bacteria. The most important aspect of the PD process for engineering application is the stable and continuous supply of nitrite. However, the activity of nitrate reductase is often higher than that of nitrite reductase (NIR), making it difficult to accumulate nitrite during the denitrification process. Herein, a strategy for achieving efficient and stable partial denitrification using the biosafe additive dimethyl sulfoxide (DMSO) was constructed, and the mechanism of DMSO inhibiting NIR was analyzed. DMSO addition reduced the expression of NIR gene, and 1% DMSO addition can significantly inhibit NIR enzyme activity to achieve a stable PD process. When the DMSO concentration increased to 3.5%, the NIR enzyme activity was almost inhibited with the enzyme activity of only 0.95 mg nitrite/min. However, the addition of DMSO has almost no inhibitory effect on the nitrate reductase (NAR) enzyme. The affinity constant of DMSO with the NAR enzyme is −2.4 kcal/mol, while the affinity constant of DMSO with the NIR enzyme is as high as −3.1 kcal/mol. DMSO shows a higher affinity for NIR. Moreover, DMSO and nitrite occupy the same catalytic cavity in the NIR enzyme, which is the fundamental reason why DMSO selectively inhibits the NIR enzyme. This study provides a new idea for realizing efficient and stable partial denitrification function.
最近提出的部分反硝化(PD),即终止硝酸盐还原为亚硝酸盐的过程,被认为是向厌氧菌供应亚硝酸盐的一种很有前途的替代方法。在工程应用中,部分反硝化过程最重要的一点是亚硝酸盐的稳定和持续供应。然而,硝酸还原酶的活性往往高于亚硝酸还原酶(NIR)的活性,因此在反硝化过程中很难积累亚硝酸盐。本文构建了一种利用生物安全添加剂二甲基亚砜(DMSO)实现高效稳定部分反硝化的策略,并分析了DMSO抑制NIR的机理。DMSO的添加降低了NIR基因的表达,1%的DMSO添加量可显著抑制NIR酶的活性,从而实现稳定的部分脱氮过程。当二甲基亚砜浓度增加到 3.5%时,近红外酶活性几乎被抑制,酶活性仅为 0.95 毫克亚硝酸盐/分钟。然而,添加 DMSO 对硝酸还原酶(NAR)几乎没有抑制作用。二甲基亚砜与硝酸还原酶的亲和力常数为-2.4 kcal/mol,而二甲基亚砜与近红外酶的亲和力常数高达-3.1 kcal/mol。二甲基亚砜与近红外酶的亲和力更高。此外,二甲基亚砜和亚硝酸盐在近红外酶中占据相同的催化空腔,这是二甲基亚砜选择性抑制近红外酶的根本原因。这项研究为实现高效、稳定的部分脱硝功能提供了新思路。
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引用次数: 0
Impact of Pristine and Aged Tire Wear Particles on Ipomoea aquatica and Rhizospheric Microbial Communities: Insights from a Long-Term Exposure Study. 原始和老化轮胎磨损颗粒对水生红苕和根瘤微生物群落的影响:长期暴露研究的启示。
IF 10.8 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-19 DOI: 10.1021/acs.est.4c07188
Aurang Zeb, Weitao Liu, Nouman Ali, Ruiying Shi, Yuexing Zhao, Jianling Wang, Qi Wang, Sheharyar Khan, Abdul Mateen Baig, Jinzheng Liu, Amir Abdullah Khan, Yichen Ge, Xiang Li, Chuan Yin

Tire wear particles (TWPs), generated from tire abrasion, contribute significantly to environmental contamination. The toxicity of TWPs to organisms has raised significant concerns, yet their effects on terrestrial plants remain unclear. Here, we investigated the long-term impact of pristine and naturally aged TWPs on water spinach (Ipomoea aquatica) and its rhizospheric soil. The results indicated that natural aging reduced the toxicity of TWPs, as evidenced by decreased levels of polycyclic aromatic hydrocarbons (PAHs) in soil and TWPs themselves. Consequently, aged TWPs were found to enhance the plant growth and chlorophyll content, whereas pristine TWPs increased the plant stress. Furthermore, aged TWPs improved soil organic matter (SOM) and total organic carbon (TOC), thereby boosting the microbial enzymes involved in nitrogen cycling. Metabolomic analysis revealed that aged TWPs upregulated key pathways related to carbon and nitrogen metabolism, enhancing plant growth and stress responses. Additionally, rhizosphere bacterial diversity was higher under aged TWPs, favoring nutrient-cycling taxa such as Acidobacteriota and Nitrospirota. Pristine TWPs may lead to overproliferation of certain dominant species, thereby reducing microbial diversity in soil, which could ultimately compromise the soil health. These findings contribute to a deeper understanding of the mechanisms underlying TWP toxicity in plants and highlight the necessity for further research on the impact of aged TWPs across various plant species over different exposure durations for comprehensive risk assessment.

轮胎磨损产生的轮胎磨损颗粒(TWPs)是造成环境污染的重要原因。轮胎磨损颗粒对生物的毒性引起了人们的极大关注,但其对陆生植物的影响仍不清楚。在这里,我们研究了原始 TWPs 和自然老化 TWPs 对蕹菜(Ipomoea aquatica)及其根瘤土壤的长期影响。结果表明,自然老化可降低 TWPs 的毒性,土壤和 TWPs 本身中多环芳烃(PAHs)含量的降低就证明了这一点。因此,老化的 TWPs 能促进植物生长和叶绿素含量,而原始 TWPs 则会增加植物的压力。此外,老化的 TWPs 改善了土壤有机质(SOM)和总有机碳(TOC),从而促进了参与氮循环的微生物酶。代谢组分析表明,老化的 TWPs 上调了与碳和氮代谢相关的关键途径,增强了植物的生长和胁迫响应。此外,在老化的 TWPs 下,根瘤菌多样性更高,有利于养分循环类群,如酸性杆菌和硝化螺菌。纯净的 TWP 可能会导致某些优势物种过度繁殖,从而降低土壤中的微生物多样性,最终损害土壤健康。这些发现有助于加深对植物中 TWP 毒性机理的理解,并突出表明有必要进一步研究老化 TWP 在不同植物物种中不同接触持续时间的影响,以进行全面的风险评估。
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引用次数: 0
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环境科学与技术
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