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Responses of CO2 and CH4 in the alpine wetlands of the Tibetan Plateau to warming and nitrogen and phosphorus additions† 青藏高原高寒湿地的 CO₂ 和 CH₄ 对气候变暖和氮磷添加的响应
IF 4.3 3区 环境科学与生态学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-07-16 DOI: 10.1039/D4EM00174E
Wenbao Zhang, Huijuan Xin, Zongxing Li, Qiao Cui, Bin Xu, Biao Tang, Yaning Wang, Chong Xu and Jian Xue

Wetland ecosystems store large amounts of carbon, and CO2 and CH4 fluxes from this ecosystem receive the double impact of climate change and human activities. Nonetheless, research on how multi-gradient warming and nitrogen and phosphorus additions affect these wetland greenhouse gas emissions is still limited, particularly in alpine wetland ecosystems. Therefore, we conducted a field experiment on the Tibetan Plateau wetlands, investigating the effects of warming and nitrogen and phosphorus additions on the CO2 and CH4 fluxes in alpine wetlands. Results indicated that warming enhanced the CO2 absorption and CH4 emission in the alpine meadow ecosystem, possibly related to changes in plant growth and microbial activity induced by warming, while we noticed that the promotion of CO2 uptake weakened with the increase in the magnitude of warming, suggesting that there may be a temperature threshold beyond which the ecosystem's capacity for carbon sequestration may be reduced. Nitrogen addition increased CH4 emission, with the effect on CO2 absorption shifting from inhibition to enhancement as the amount of applied nitrogen or phosphorus increased. The interaction between warming and nitrogen and phosphorus additions further influenced CH4 emission, exhibiting a synergistic enhancement effect. This study deepens our understanding of the greenhouse gas responses of alpine wetland ecosystems to warming and nitrogen and phosphorus additions, which is significant for predicting and managing ecosystem carbon balance under global change.

湿地是全球重要的生态系统之一,储存着大量的碳。然而,气候变化和人类活动导致氮和磷等外源营养物质涌入湿地生态系统,可能对二氧化碳和甲烷通量产生深远影响。然而,关于多梯度变暖和氮磷添加如何影响这些湿地温室气体排放的研究仍然有限,尤其是在高山湿地生态系统中。因此,我们在青藏高原湿地开展了一项野外实验,研究增温和氮磷添加对高寒湿地二氧化碳和甲烷通量的影响。结果表明,升温增强了高寒草甸生态系统对CO2的吸收和CH4的排放,这可能与升温引起的植物生长和微生物活动的变化有关,同时我们注意到,升温对CO2吸收的促进作用随着升温幅度的增加而减弱,这表明可能存在一个温度阈值,超过该温度阈值,生态系统的固碳能力可能会降低。氮的添加增加了 CH4 的排放,随着施氮量或施磷量的增加,对 CO2 吸收的影响从抑制转为增强。气候变暖与氮和磷的添加之间的相互作用进一步影响了CH4的排放,表现出一种协同增强效应。这项研究加深了我们对高山湿地生态系统对气候变暖和氮磷添加的温室气体响应的理解,对预测和管理全球变化下的生态系统碳平衡具有重要意义。
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引用次数: 0
Distribution characteristics of soil microplastics and their impact on soil physicochemical properties in agricultural areas of the North China plain† 华北平原农业区土壤微塑料的分布特征及其对土壤理化性质的影响
IF 4.3 3区 环境科学与生态学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-07-15 DOI: 10.1039/D4EM00242C
Yuze Zhou, Ming Dou, Yan Zhang, Kaizi Ning and Yuxuan Li

Microplastic (MPs) pollution has become a global issue, with particular concern regarding MPs in soil. To determine the characteristics of MPs in agricultural production areas and their impact on soil physicochemical properties, soil samples were collected from different land use types in the North China Plain. Layered sampling was conducted and the soil physicochemical properties were determined. A novel image recognition method based on fluorescence staining was proposed for the batch analysis of MPs in the study area. Together with the results of the soil physicochemical properties, the impact of MPs on soil physicochemical properties was analyzed and evaluated. The results showed that the soil MPs abundance in this agricultural area was moderate to low compared to other agricultural areas, with a larger proportion of particle-type and fragment-type MPs smaller than 10 μm. The soil MPs were predominantly composed of polyvinyl chloride (PVC) and polypropylene (PP). MPs abundance was higher in farmland and forest land than in vegetable fields. The impact of MPs on soil physicochemical properties was mainly manifested in the changes in soil structure due to the different MPs characteristics. Apart from abundance, the type of MPs was found to be the main factor affecting soil bulk density, with particle size and shape influencing the soil aggregate structure. MPs may effect the pH values of sandy and loamy soils, primarily by altering the soil porosity and water holding capacity, but also by increasing the area and duration of contact between the soil medium and external water sources. This study revealed the MPs characteristics in agricultural areas as well as the pathways by which they can impact soil physicochemical properties.

微塑料(MPs)污染已成为一个全球性问题,其中土壤中的 MPs 尤为令人担忧。为了解农业生产区土壤中微塑料的特征及其对土壤理化性质的影响,研究人员从华北平原不同土地利用类型中采集了土壤样品。分层取样,测定土壤理化性质。提出了一种基于荧光染色的新型图像识别方法,用于批量分析研究区域的 MPs。结合土壤理化性质结果,分析评价了 MPs 对土壤理化性质的影响。结果表明,与其他农业区相比,该农业区土壤 MPs 丰度处于中等偏低的水平,其中小于 10 μm 的颗粒型和碎片型 MPs 占了相当大的比例。土壤中的 MPs 主要由聚氯乙烯(PVC)和聚丙烯(PP)组成。农田和林地中 MPs 的丰度高于菜地。MPs 对土壤理化性质的影响主要表现在不同 MPs 特性导致的土壤结构变化上。除丰度外,MPs 类型是影响土壤容重的主要因素,粒径和粒形对土壤团粒结构也有影响。多孔质微粒主要通过改变土壤孔隙度和持水能力,同时也通过增加土壤介质与外部水源的接触面积和接触时间,对砂质土壤和壤土的 pH 值产生重要影响。这项研究揭示了农业地区多孔介质的特点,以及它们影响土壤理化性质的途径。
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引用次数: 0
Biodegradability of unheated and laboratory heated dissolved organic matter† 未加热和实验室加热的溶解有机物的生物降解性
IF 4.3 3区 环境科学与生态学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-07-12 DOI: 10.1039/D3EM00383C
Saraf Islam Promi, Courtney M. Gardner and Amanda K. Hohner

Following wildfires, partially combusted biomass remains on the forest floor and erosion from the landscape can release dissolved pyrogenic organic matter (dPyOM) to surface waters. Therefore, post-fire alterations to dissolved organic matter (DOM) in aquatic systems may play a vital role in DOM stability and biogeochemical cycles. Dissolved PyOM biodegradation remains poorly understood and is expected to vary with combustion temperature and fuel source. In this study laboratory heating and leaching of forest floor materials (soil and litter) were used to compare the biodegradability of unheated, low (250 °C), and moderate (450 °C) temperature leachates. Inoculation experiments were performed with river microbes. Dissolved organic carbon (DOC) and nitrogen (DON), inorganic nitrogen, and DOM optical properties were monitored for 38 days. Inoculation experiments showed significantly greater DOC biodegradation of low and moderate temperature samples (64% and 71%, respectively) compared to unheated samples (32%). The greater DOC biodegradation may be explained by lower molecular weight DOM composition of heated leachates which was supported by higher initial E2/E3 ratios (absorbance at 250 nm/365 nm). Further, the observed decrease in the E2/E3 ratio after incubation suggests biodegradation of smaller compounds. This trend was greater for heated samples than unheated DOM. Specific ultraviolet absorbance increased after incubation, suggesting biodegradation of aliphatic compounds. Inoculated moderate temperature samples showed the greatest DON degradation (74%), followed by low temperature (58%) and unheated (51%) samples. Overall, results suggest that low and moderate temperature dPyOM was more biodegradable than unheated DOM, which may have implications for aquatic biogeochemical cycling, ecosystem function, and water quality in fire-impacted watersheds.

野火发生后,部分燃烧的生物质会残留在森林地面上,而地表的侵蚀会向地表水释放溶解热原有机物(dPyOM)。因此,火灾后水生系统中溶解有机物(DOM)的变化可能对 DOM 的稳定性和生物地球化学循环起着至关重要的作用。人们对溶解 PyOM 的生物降解仍然知之甚少,而且预计它会随燃烧温度和燃料来源的不同而变化。本研究采用实验室加热和浸出林地材料(土壤和垃圾)的方法,比较未加热、低温(250°C)和中温(450°C)浸出液的生物降解性。对河流微生物进行了接种实验。对溶解有机碳(DOC)、溶解有机氮(DON)、无机氮和 DOM 光学特性进行了长达 38 天的监测。接种实验表明,与未加热的样本(32%)相比,低温和中温样本的 DOC 生物降解率明显更高(分别为 64% 和 71%)。DOC 生物降解能力更强的原因可能是加热浸出液中的 DOM 分子重量较低,而较高的初始 E2/E3 比率(250 纳米/365 纳米吸光度)也证明了这一点。此外,培养后观察到的 E2/E3 比率下降表明,生物降解的是较小的化合物。与未加热的 DOM 相比,加热样品的这一趋势更为明显。特定紫外线吸光度在培养后增加,表明脂肪族化合物发生了生物降解。接种温度适中的样本显示出最大的 DON 降解率(74%),其次是低温样本(58%)和未加热样本(51%)。总之,研究结果表明,低温和中温 dPyOM 比未加热的 DOM 更容易生物降解,这可能会对受火灾影响流域的水生生物地球化学循环、生态系统功能和水质产生影响。
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引用次数: 0
Correction: Emerging pollutants in the Esmeraldas watershed in Ecuador: discharge and attenuation of emerging organic pollutants along the San Pedro–Guayllabamba–Esmeraldas rivers 更正:厄瓜多尔埃斯梅拉达斯流域新出现的污染物:圣佩德罗-瓜伊拉班巴-埃斯梅拉达斯河流沿岸新出现的有机污染物的排放和衰减。
IF 4.3 3区 环境科学与生态学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-07-12 DOI: 10.1039/D4EM90029D
A. Voloshenko-Rossin, G. Gasser, K. Cohen, J. Gun, L. Cumbal-Flores, W. Parra-Morales, F. Sarabia, F. Ojeda and O. Lev

Correction for ‘Emerging pollutants in the Esmeraldas watershed in Ecuador: discharge and attenuation of emerging organic pollutants along the San Pedro–Guayllabamba–Esmeraldas rivers’ by A. Voloshenko-Rossin et al., Environ. Sci.: Processes Impacts, 2015, 17, 41–53, https://doi.org/10.1039/C4EM00394B.

对 A. Voloshenko-Rossin 等人撰写的 "厄瓜多尔埃斯梅拉达斯流域新出现的污染物:圣佩德罗-瓜伊拉班巴-埃斯梅拉达斯河流沿岸新出现的有机污染物的排放和衰减 "的更正,Environ.Sci:Processes Impacts, 2015, 17, 41-53, https://doi.org/10.1039/C4EM00394B。
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引用次数: 0
Cu(ii) inhibited the transport of tetracycline in porous media: role of complexation† Cu(II)抑制了四环素在多孔介质中的迁移:络合作用
IF 4.3 3区 环境科学与生态学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-07-12 DOI: 10.1039/D4EM00210E
Chang Xu, Bo Gong, Shan Zhao, Xiao-Min Sun, Shu-Guang Wang and Chao Song

Tetracycline (TC) and Cu(II) coexist commonly in various waters, which may infiltrate into the subterranean environment through runoff and leaching, resulting in substantial ecological risks. However, the underlying mechanisms why Cu(II) affects the transport of TC in porous media remain to be further explored and supported by more evidence, especially the role of complexation. In this study, the transport of TC with coexisting Cu(II) was comprehensively explored with column experiments and density functional theory (DFT) calculation. At natural environmental concentrations, Cu(II) significantly inhibited the transport of TC in the quartz sand column. Cu(II) augmented the retention of TC in the column mainly via electrostatic force and complexation. The interaction between TC and TC–Cu complexes on the surface of SiO2 was investigated with first-principles calculations for the first time. There were strong van der Waals forces and coordination bonds on the surface of complexes and SiO2, leading to higher adsorption energy than that of TC and inhibiting its penetration. This study offers novel insights and theoretical framework for the transport of antibiotics in the presence of metal ions to better understand the fate of antibiotics in nature.

四环素(TC)和铜(II)通常共存于各种水体中,并可能通过径流和沥滤渗入地下环境,从而对生态环境造成严重危害。然而,Cu(II)为何会影响 TC 在多孔介质中的迁移,尤其是络合作用的作用,其深层机理仍有待进一步探索和证据支持。本研究通过柱实验和密度泛函理论(DFT)计算,全面探讨了共存 Cu(II)的三氯乙酸迁移问题。在自然环境浓度下,Cu(II) 明显抑制了 TC 在石英砂柱中的迁移。Cu(II)主要通过静电力和络合作用增强了TC在石英砂柱中的保留。通过第一原理计算,首次研究了二氧化硅表面上 TC 与 TC-Cu 复合物之间的相互作用。络合物和 SiO2 表面存在很强的范德华力和配位键,导致吸附能高于 TC 的吸附能,从而抑制了 TC 的渗透。这项研究为抗生素在金属离子存在下的迁移提供了新的见解和理论框架,有助于更好地理解抗生素在自然界中的命运。
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引用次数: 0
Effects of copper on chemical kinetics and brown carbon formation in the aqueous ˙OH oxidation of phenolic compounds† 铜对酚类化合物水溶液 ∙OH 氧化过程中的化学动力学和褐碳形成的影响
IF 4.3 3区 环境科学与生态学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-07-10 DOI: 10.1039/D4EM00191E
Junwei Yang, Tianye Zhou, Yuting Lyu, Beatrix Rosette Go Mabato, Jason Chun-Ho Lam, Chak K. Chan and Theodora Nah

Many phenolic compounds (PhCs) in biomass burning and fossil fuel combustion emissions can partition into atmospheric aqueous phases (e.g., cloud/fog water and aqueous aerosols) and undergo reactions to form secondary organic aerosols (SOAs) and brown carbon (BrC). Redox-active transition metals, particularly Fe and Cu, are ubiquitous species in atmospheric aqueous phases known to participate in Fenton/Fenton-like chemistry as a source of aqueous ˙OH. However, even though the concentrations of water-soluble Cu are close to those of water-soluble Fe in atmospheric aqueous phases in some areas, unlike Fe, the effects that Cu have on SOA and BrC formation in atmospheric aqueous phases have scarcely been studied and remain poorly understood. We investigated the effects of Cu(II) on PhC reaction rates and BrC formation during the aqueous oxidation of four PhCs (guaiacol, catechol, syringol, and vanillin) by ˙OH generated from Fenton-like chemistry under different pH conditions. While the PhCs reacted when both H2O2 and Cu(II) were present in the absence (i.e., dark oxidation) and presence (i.e., photooxidation) of light, the reaction rates were at least one order of magnitude higher during photooxidation. Higher PhC reaction rates were measured at higher pH during both dark oxidation and photooxidation as a result of higher ˙OH concentrations produced by Fenton-like chemistry. Only water-soluble BrC was formed during dark oxidation and photooxidation when Cu(II) was present. Mass absorption coefficients (103 to 104 cm2 g−1) comparable to those of biomass burning BrC were measured during dark oxidation and photooxidation when Cu(II) was present. Light absorption was enhanced at higher pH during dark oxidation and photooxidation, which indicated that higher quantities and/or more absorbing BrC chromophores were formed at higher pH. The effects that Cu(II) had on the PhC reaction rates and the composition of SOAs and BrC formed depended on the PhC base structure (i.e., benzenediol vs. methoxyphenol). Overall, these results show how aqueous reactions involving Cu(II), H2O2, and PhCs can be an efficient source of daytime and nighttime water-soluble BrC and SOAs, which can have significant implications for how the atmospheric fates of PhCs are modeled for areas with substantial concentrations of water-soluble Cu in highly to moderately acidic cloud/fog water and aqueous aerosols.

生物质燃烧和化石燃料燃烧排放物中的许多酚类化合物(PhCs)会进入大气水相并发生反应,形成二次有机气溶胶(SOA)和褐碳(BrC)。具有氧化还原活性的过渡金属(铁和铜)是大气水相中无处不在的物种,它们参与类似芬顿/芬顿的化学反应,成为 ∙OH 的来源。然而,尽管在某些地区大气水相中水溶性铜的浓度与水溶性铁的浓度接近,但与铁不同的是,铜对大气水相中 SOA 和 BrC 形成的影响却鲜有研究,人们对这一问题的了解仍然不够深入。我们研究了在不同 pH 值条件下,芬顿类化学反应产生的 ∙OH 对四种 PhC(愈创木酚、邻苯二酚、丁香酚和香草醛)的水氧化过程中,Cu(II)对 PhC 反应速率和 BrC 形成的影响。在没有光(即暗氧化)和有光(即光氧化)的情况下,当 H2O2 和 Cu(II)同时存在时,PhCs 都会发生反应,而在光氧化过程中,反应速率至少要高出一个数量级。在暗氧化和光氧化过程中,pH 值越高,PhC 反应速率越高,这是因为芬顿化学反应产生的 ∙OH 浓度越高。有 Cu(II)存在时,暗氧化和光氧化过程中只形成水溶性 BrC。在有 Cu(II)存在的暗氧化和光氧化过程中,测得的质量吸收系数(103 至 104 cm2 g-1)与生物质燃烧的 BrC 的质量吸收系数相当。在暗氧化和光氧化过程中,pH 值越高,光吸收越强,这表明 pH 值越高,形成的 BrC 发色团数量越多和/或吸收能力越强。Cu(II) 对 PhC 反应速率以及所形成的 SOA 和 BrC 成分的影响取决于 PhC 碱结构(即苯二酚与甲氧基苯酚)。总之,这些结果表明了涉及 Cu(II)、H2O2 和 PhCs 的水反应如何成为白天和夜间水溶性 BrC 和 SOA 的有效来源,这对如何模拟 PhCs 在高度至中度酸性云/雾水和水气溶胶中具有大量水溶性 Cu 的地区的大气命运具有重要意义。
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引用次数: 0
Outstanding Reviewers for Environmental Science: Processes & Impacts in 2023 环境科学》杰出评审员:2023 年的过程与影响。
IF 4.3 3区 环境科学与生态学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-07-10 DOI: 10.1039/D4EM90024C

We would like to take this opportunity to thank all of Environmental Science: Processes & Impacts’ reviewers for helping to preserve quality and integrity in chemical science literature. We would also like to highlight the Outstanding Reviewers for Environmental Science: Processes & Impacts in 2023.

我们想借此机会感谢《环境科学:过程与影响》的所有审稿人,感谢他们帮助保持化学科学文献的质量和完整性:过程与影响》的审稿人帮助维护化学科学文献的质量和完整性。我们还想特别表扬一下 2023 年《环境科学:过程与影响》的杰出审稿人:过程与影响》2023 年的杰出审稿人。
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引用次数: 0
Assessment of toxic effects of thallium on the earthworm Eisenia fetida using the biomarker response index† 利用生物标记反应指数评估铊对蚯蚓的毒性影响
IF 4.3 3区 环境科学与生态学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-07-09 DOI: 10.1039/D4EM00253A
Shuai Li, Zhifeng Wang, Nan Gao, Xiaoyu Niu, Benteng Zhu, Lusheng Xu and Weina Xue

Thallium (Tl), though not essential for biological systems, is widely used in industrial activities, resulting in soil pollution and adverse effects on soil biota. Systematic toxicological studies on Tl, especially concerning soil organisms, are relatively rare. This research evaluates the toxic effects of Tl on earthworms by measuring oxidative stress biomarkers, such as superoxide dismutase (SOD), catalase (CAT), glutathione S-transferase (GST), malondialdehyde (MDA), and 8-hydroxydeoxyguanosine (8-OHdG), and by assessing the expression of functional genes, such as heat shock protein 70 (Hsp70), metallothionein (MT), and annetocin (ANN). Additionally, this study employs the Biomarker Response Index (BRI) and two-way ANOVA to comprehensively assess the cumulative toxicity of Tl in earthworms. The findings indicate that Tl exposure significantly exacerbates oxidative stress and cellular damage in earthworms, particularly under conditions of high concentration and prolonged exposure. BRI results demonstrate a continuous decline in the physiological state of earthworms with increasing Tl concentration and exposure duration. Two-way ANOVA reveals significant dose-responsive increases in SOD and CAT activities, as well as in ANN gene expression. Apart from GST activity, other biomarkers significantly increased over time, and the changes in biomarkers such as SOD, CAT, MDA, and 8-OHdG were significantly influenced by dose and time. LSD post hoc tests show significant effects of dose, time, and their interactions on all biomarkers except for GST. These findings are valuable for gaining a deeper understanding of the ecological risks of Tl in soil environments and its potential threats to soil biota, aiding in the management of ecological risks associated with Tl-contaminated soils.

铊(Tl)虽然不是生物系统所必需的,但却被广泛用于工业活动,造成土壤污染并对土壤生物群产生不利影响。有关铊的系统毒理学研究,特别是有关土壤生物的研究,相对较少。本研究通过测量氧化应激生物标志物,如超氧化物歧化酶 (SOD)、过氧化氢酶 (CAT)、谷胱甘肽 S 转移酶 (GST)、丙二醛 (MDA) 和 8- 羟基脱氧鸟苷 (8-OHdG),以及评估功能基因的表达,如热休克蛋白 70 (Hsp70)、金属硫蛋白 (MT) 和蒽醌 (ANN),来评估 Tl 对蚯蚓的毒性影响。此外,本研究还采用了生物标记反应指数(BRI)和双向方差分析来全面评估蚯蚓体内碲的累积毒性。研究结果表明,碲暴露会显著加剧蚯蚓的氧化应激和细胞损伤,尤其是在高浓度和长时间暴露的条件下。BRI 结果表明,蚯蚓的生理状态随着 Tl 浓度和暴露时间的增加而持续下降。双向方差分析显示,SOD 和 CAT 活性以及 ANN 基因表达量都出现了显著的剂量反应性增加。除 GST 活性外,其他生物标志物也随时间的延长而显著增加,SOD、CAT、MDA 和 8-OHdG 等生物标志物的变化受剂量和时间的显著影响。LSD 事后检验表明,除 GST 外,剂量、时间及其相互作用对所有生物标志物都有明显影响。这些研究结果对于深入了解土壤环境中 Tl 的生态风险及其对土壤生物区系的潜在威胁非常有价值,有助于管理与 Tl 污染土壤相关的生态风险。
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引用次数: 0
Emerging investigator series: preferential adsorption and coprecipitation of permafrost organic matter with poorly crystalline iron minerals† 新晋研究人员系列:永久冻土有机物与弱结晶铁矿物的优先吸附和共沉淀作用
IF 4.3 3区 环境科学与生态学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-07-09 DOI: 10.1039/D4EM00241E
Eva Voggenreiter, Philippe Schmitt-Kopplin, Laurel ThomasArrigo, Casey Bryce, Andreas Kappler and Prachi Joshi

Future permafrost thaw will likely lead to substantial release of greenhouse gases due to thawing of previously unavailable organic carbon (OC). Accurate predictions of this release are limited by poor knowledge of the bioavailability of mobilized OC during thaw. Organic carbon bioavailability decreases due to adsorption to, or coprecipitation with, poorly crystalline ferric iron (Fe(III)) (oxyhydr)oxide minerals but the maximum binding extent and binding selectivity of permafrost OC to these minerals is unknown. We therefore utilized water-extractable organic matter (WEOM) from soils across a permafrost thaw gradient to quantify adsorption and coprecipitation processes with poorly crystalline Fe(III) (oxyhydr)oxides. We found that the maximum adsorption capacity of WEOM from intact and partly thawed permafrost soils was similar (204 and 226 mg C g−1 ferrihydrite, respectively) but decreased to 81 mg C g−1 ferrihydrite for WEOM from the fully thawed site. In comparison, coprecipitation of WEOM from intact and partly thawed soils with Fe immobilized up to 925 and 1532 mg C g−1 Fe respectively due to formation of precipitated Fe(III)–OC phases. Analysis of the OC composition before and after adsorption/coprecipitation revealed that high molecular weight, oxygen-rich, carboxylic- and aromatic-rich OC was preferentially bound to Fe(III) minerals relative to low molecular weight, aliphatic-rich compounds which may be more bioavailable. This selective binding effect was stronger after adsorption than coprecipitation. Our results suggest that OC binding by Fe(III) (oxyhydr)oxides sharply decreases under fully thawed conditions and that small, aliphatic OC molecules that may be readily bioavailable are less protected across all thaw stages.

由于以前不可利用的有机碳(OC)解冻,未来的永久冻土解冻可能会导致温室气体的大量释放。由于对解冻过程中移动的有机碳的生物利用率知之甚少,因此对这种释放的准确预测受到了限制。有机碳的生物利用率会因吸附或共沉淀在结晶度较低的氧化铁(Fe(III))矿物上而降低,但永久冻土有机碳与这些矿物的最大结合范围和结合选择性尚不清楚。因此,我们利用永冻土融化梯度土壤中的水提取有机物(WEOM)来量化与弱结晶氧化铁(III)的吸附和共沉淀过程。我们发现,完整土壤和部分融化的永久冻土中的 WEOM 的最大吸附容量相似(分别为 204 和 226 毫克 C g-1 铁水物),但完全融化土壤中的 WEOM 的吸附容量降至 81 毫克 C g-1 铁水物。相比之下,由于形成了沉淀的铁(III)-OC 相,完整和部分解冻土壤中的 WEOM 与固定铁的共沉淀分别高达 925 和 1532 毫克 C g-1 Fe。对吸附/共沉淀前后的 OC 成分分析表明,相对于生物利用率较高的低分子量、富含脂肪族的化合物,高分子量、富含氧、富含羧基和芳香族的 OC 会优先与铁(III)矿物结合。这种选择性结合效应在吸附后比共沉淀更强。我们的研究结果表明,在完全解冻的条件下,OC 与铁(III)(氧氢)氧化物的结合急剧下降,而在所有解冻阶段,可能容易被生物利用的小分子脂肪族 OC 的保护作用较弱。
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引用次数: 0
Porphyrin metabolism and carbon fixation response of Skeletonema costatum at different growth phases to mixed emerging PFASs at environmental concentrations† 不同生长阶段的 Skeletonema costatum 对环境浓度下新出现的混合 PFAS 的卟啉代谢和碳固定反应。
IF 4.3 3区 环境科学与生态学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-07-08 DOI: 10.1039/D4EM00137K
Xiaofeng Li, Yongzheng Ma, Ying Zhang, Xiaohan Zhang, Hongyu Li, Yueling Sun and Zhiguang Niu

Per- and polyfluoroalkyl substances (PFASs), especially as emerging compounds, have been widely detected in coastal seawater. However, the awareness of the interaction between PFASs at environmental concentrations and marine diatoms is still limited. In this study, Skeletonema costatum was exposed to three co-existing PFASs, namely hexafluoropropylene oxide dimer acid (HFPO-DA), 6 : 2 chlorinated polyfluorinated ether sulfonate (Cl-PFAES), and perfluoroethylcyclohexane sulfonate (PFECHS) (15–300 ng L−1 in total), for 14 days. In the 300 ng L−1 test group, the significant down-regulation of chlorophyllide a in porphyrin metabolism, light-harvesting capacity and carbon fixation were the main inhibitory mechanisms of photosynthesis by emerging PFASs at the 14th day compared to the 8th day, which indicated that they may have a shading effect on S. costatum. Additionally, mixed PFASs could also activate nicotinamide adenine dinucleotide phosphate (NADPH) oxidase by up-regulating gene gp91 and down-regulating genes CaM4 and NDPK2 to generate excessive ROS. This resulted in a decrease in the algal biomass, which would further weaken the primary productivity of S. costatum. Our findings illustrated that mixed emerging PFASs at environmental concentrations may interfere with the carbon balance of marine diatoms.

全氟烷基和多氟烷基物质(PFASs),尤其是新出现的化合物,已在沿海海水中被广泛检测到。然而,人们对环境浓度下 PFAS 与海洋硅藻之间相互作用的认识仍然有限。本研究将硅藻暴露于三种共存的 PFASs(即六氟环氧丙烷二聚酸(HFPO-DA)、6 : 2 氯化聚氟醚磺酸盐(Cl-PFAES)和全氟乙基环己烷磺酸盐(PFECHS),共计 15-300 ng L-1)中 14 天。在 300 ng L-1 试验组中,与第 8 天相比,第 14 天新出现的 PFASs 对光合作用的主要抑制机制是显著下调卟啉代谢中的叶绿素 a、光收集能力和碳固定能力,这表明它们可能对 S. costatum 具有遮光作用。此外,混合 PFAS 还能通过上调基因 gp91 和下调基因 CaM4 和 NDPK2 激活烟酰胺腺嘌呤二核苷酸磷酸(NADPH)氧化酶,产生过量的 ROS。这导致了藻类生物量的减少,从而进一步削弱了 S. costatum 的初级生产力。我们的研究结果表明,环境浓度下的混合新兴全氟辛烷磺酸可能会干扰海洋硅藻的碳平衡。
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Environmental Science: Processes & Impacts
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