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Consumer products are important reservoirs and sources of organophosphate tri-esters and di-esters: Characteristics, mass inventory, and implication for waste management 消费品是有机磷三酯和二酯的重要储存库和来源:特征、质量库存和对废物管理的影响
2区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2024-04-18 DOI: 10.1016/j.jes.2024.04.008
Jie Zhou , Chan Liang , Jinyun Li , Jiayi Gu , Amina Salamova , Liangying Liu

Numerous studies documented the occurrence of organophosphate tri-esters (tri-OPEs) and di-esters (di-OPEs) in the environment. Little information is available on their occurrence in waste consumer products, reservoirs and sources of these chemicals. This study collected and analyzed 92 waste consumer products manufactured from diverse polymers, including polyurethane foam (PUF), polystyrene (PS), acrylonitrile butadiene styrene (ABS), polypropylene (PP), and polyethylene (PE) to obtain information on the occurrence and profiles of 16 tri-OPEs and 10 di-OPEs. Total concentrations of di-OPEs (18−370,000 ng/ g, median 1,700 ng/g) were one order of magnitude lower than those of tri-OPEs (94−4,500,000 ng/g, median 5,400 ng/g). The concentrations of both tri- and di-OPEs in products made of PUF, PS, and ABS were orders of magnitude higher than those made of PP and PE. The compositional patterns of OPEs varied among different polymer types but were generally dominated by bisphenol A bis(diphenyl phosphate), triphenyl phosphate, tris(1-chloro-2-propyl) phosphate, di-phenyl phosphate (DPHP), and bis (2-ethylhexyl) phosphate. Two industrially applied di-OPEs (di-n-butyl phosphate and DPHP) exhibited higher levels than their respective tri-OPEs, contrary to their production volumes. Some non-industrially applied chlorinated di-OPEs were also detected, with concentrations up to 97,000 ng/g. These findings suggest that degradation of tri-OPEs during the manufacturing and use of products is an important source of di-OPEs. The mass inventories of tri-OPEs and di-OPEs in consumer products were estimated at 3,100 and 750 tons/year, respectively. This study highlights the importance of consumer products as emission sources of a broad suite of OPEs.

大量研究记录了环境中有机磷三酯(三-OPEs)和二酯(二-OPEs)的存在。关于它们在废弃消费品中的出现、这些化学品的储藏和来源的信息却很少。本研究收集并分析了 92 种由不同聚合物(包括聚氨酯泡沫 (PUF)、聚苯乙烯 (PS)、丙烯腈-丁二烯-苯乙烯 (ABS)、聚丙烯 (PP) 和聚乙烯 (PE))制造的废弃消费品,以获得有关 16 种三元 OPE 和 10 种二元 OPE 的存在和概况的信息。二OPE的总浓度(18-370,000 纳克/克,中位数为 1,700 纳克/克)比三OPE(94-4,500,000 纳克/克,中位数为 5,400 纳克/克)低一个数量级。PUF、PS 和 ABS 制成的产品中三-OPE 和二-OPE 的浓度都比 PP 和 PE 制成的产品高几个数量级。不同类型聚合物的 OPE 组成模式各不相同,但一般以双酚 A 双(二苯基磷酸酯)、磷酸三苯酯、磷酸三(1-氯-2-丙基)酯、磷酸二苯酯(DPHP)和磷酸二(2-乙基己基)酯为主。两种工业应用的二-OPE(磷酸二正丁酯和 DPHP)的含量高于其各自的三-OPE,这与它们的产量相反。还检测到一些非工业应用的氯化二-OPE,浓度高达 97,000 纳克/克。这些发现表明,产品在生产和使用过程中降解的三-OPE 是二-OPE 的一个重要来源。据估计,消费品中三-OPEs 和二-OPEs 的总库存量分别为每年 3,100 吨和 750 吨。这项研究强调了消费品作为各种 OPE 排放源的重要性。
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引用次数: 0
Current research status on the distribution and transport of micro(nano)plastics in hyporheic zones and groundwater 微(纳)塑料在水下带和地下水中的分布和迁移研究现状
2区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2024-04-17 DOI: 10.1016/j.jes.2024.03.042
Dongming Zhang , Qiqing Chen , Ting Xu , Daqiang Yin

Micro(nano)plastics, as an emerging environmental pollutant, are gradually discovered in hyporheic zones and groundwater worldwide. Recent studies have focused on the origin and spatial/temporal distribution of micro(nano)plastics in regional groundwater, together with the influence of their properties and effects of environmental factors on their transport. However, the transport of micro(nano)plastics in the whole hyporheic zone-groundwater system and the behavior of co-existing substances still lack a complete theoretical interpretation. To provide systematic theoretical support for that, this review summarizes the current pollution status of micro(nano)plastics in the hyporheic zone-groundwater system, provides a comprehensive introduction of their sources and fate, and classifies the transport mechanisms into mechanical transport, physicochemical transport and biological processes assisted transport from the perspectives of mechanical stress, physicochemical reactions, and bioturbation, respectively. Ultimately, this review proposes to advance the understanding of the multi-dimensional hydrosphere transport of micro(nano)plastics centered on groundwater, the microorganisms-mediated synergistic transformation and co-transport involving the intertidal circulation. Overall, this review systematically dissects the presence and transport cycles of micro(nano)plastics within the hyporheic zone-groundwater system and proposes prospects for future studies based on the limitations of current studies.

微(纳米)塑料作为一种新出现的环境污染物,逐渐在世界各地的底流区和地下水中被发现。近期研究的重点是区域地下水中微(纳米)塑料的来源和时空分布,以及微(纳米)塑料的特性和环境因素对其迁移的影响。然而,微(纳)塑料在整个水文带-地下水系统中的迁移以及共存物质的行为仍然缺乏完整的理论解释。为了提供系统的理论支持,本综述总结了微(纳)塑料在透水带-地下水系统中的污染现状,全面介绍了微(纳)塑料的来源和归宿,并分别从机械应力、物理化学反应和生物扰动的角度将其迁移机制分为机械迁移、物理化学迁移和生物过程辅助迁移。最终,本综述提出了以地下水为中心的微(纳)塑料多维水圈迁移、微生物介导的协同转化以及涉及潮间带循环的协同迁移的认识。总之,本综述系统地剖析了微(纳米)塑料在透水带-地下水系统中的存在和迁移循环,并根据当前研究的局限性提出了未来研究的展望。
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引用次数: 0
High potential in synergizing the reduction of dissolved organic carbon concentration and carbon dioxide emissions for submerged-vegetation-covered river networks 水下植被覆盖的河流网络在协同降低溶解有机碳浓度和二氧化碳排放量方面潜力巨大
2区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2024-04-16 DOI: 10.1016/j.jes.2024.04.007
Qingqian Li , Ruixia Liu , Zhangmu Jing , Yanjie Wei , Shengqiang Tu , Huibin Yu , Hongjie Gao , Peng Yuan

Various technologies and projects have been explored and developed for the synergetic control of environmental pollution and carbon emissions in aquatic ecosystems. Planting submerged vegetation in shallow waters was also expected to achieve this purpose. However, the magnitude and mechanism of carbon dioxide (CO2) emission affected by submerged vegetation is not clear enough in complex aquatic ecosystems. This study investigated the influences of submerged plants on CO2 emission, ecosystem metabolism features, and microbial community traits based on observations in river networks on the Changjiang River Delta. The results showed that CO2 emission from planted waters accounted for 73% of unplanted waters. Meanwhile, planted waters had higher dissolved organic carbon removal capacity in overlying water and higher potential of carbon sequestration in sediment at the same time. These distinctions between the two habitats were attributed to (1) improved CO2 and bicarbonate consumption in water columns via enhancing photosynthesis and (2) inhibited CO2 production by reconstructing the benthic microbial community. Additional eco-advantages were found in planted sediments, such as a high potential of methane oxidation and xenobiotics biodegradation and a low risk of becoming black and odorous. In brief, submerged vegetation is beneficial in promoting pollution removal and carbon retention synchronously. This study advances our understanding of the feedback between aquatic metabolism and CO2 emission.

为了协同控制水生生态系统的环境污染和碳排放,人们探索和开发了各种技术和项目。在浅水区种植沉水植被也有望实现这一目的。然而,在复杂的水生生态系统中,沉水植被对二氧化碳(CO2)排放的影响程度和机制还不够明确。本研究基于对长江三角洲河网的观测,研究了沉水植物对二氧化碳排放、生态系统代谢特征和微生物群落性状的影响。结果表明,种植水域的二氧化碳排放量占未种植水域的 73%。同时,种植水域上覆水体的溶解有机碳去除能力较强,沉积物固碳潜力较大。这两种生境之间的差异归因于:(1)通过提高光合作用改善了水体中二氧化碳和碳酸氢盐的消耗;(2)通过重建底栖微生物群落抑制了二氧化碳的产生。在种植的沉积物中还发现了其他生态优势,如甲烷氧化和异种生物降解潜力大,变黑和发臭的风险低。简而言之,沉水植被有利于同步促进污染清除和碳保留。这项研究加深了我们对水生新陈代谢与二氧化碳排放之间的反馈作用的理解。
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引用次数: 0
Research progress on secondary formation, photosensitive reaction mechanism and human health effects of chromophoric brown carbon 发色棕碳的二次形成、光敏反应机理及对人体健康影响的研究进展
2区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2024-04-14 DOI: 10.1016/j.jes.2024.04.003
Baihang Chen , Jiangyao Chen , Guiying Li , Taicheng An

Brown carbon (BrC) has attracted widespread attention because of its strong absorption of solar radiation in the ultraviolet-visible wavelength range, which causes adverse impacts on human health. Originally, BrC was a physically defined class of substances. However, current research has gradually shifted towards the identification of its chemical groups, because its light-absorbing capability, chemical properties and health effects mainly depend on the chemical composition of its chromophores. Therefore, this review mainly focuses on the chemical understanding of BrC based on chromophores, and the secondary formation mechanism of chromophores, photosensitized reactions, and human health effects of BrC were detailly summarized. Firstly, BrC chromophores are divided into five categories: nitrogen-heterocycles, nitrogen-chain, aromatic species, oligomers and sulfur-containing organic compounds. Different chromophore precursor species exhibit variations, and their formation mechanisms are also distinct. Secondly, BrC can trigger the production of secondary organic aerosol (SOA) precursors or cause SOA growth because BrC is an important component of light-absorbing particles formed during incomplete combustion of biomass and fossil fuels, potentially exerting adverse effects on human health. Finally, developing sufficiently separated methods for BrC and refining algorithms and machine learning can lead to a more effective understanding of the chemical composition of chromophores, thus enabling better evaluation of the atmospheric effects and health impacts of BrC. In all, this review provides new insights into the categories of BrC chromophores and new advance in secondary formation mechanisms, photosensitized reactions, and human health effects on the basis of chemical structures.

棕碳(BrC)之所以引起广泛关注,是因为它对紫外线-可见光波长范围内的太阳辐射有很强的吸收能力,从而对人类健康造成不利影响。最初,棕碳是一类物理定义的物质。然而,由于 BrC 的光吸收能力、化学性质和对健康的影响主要取决于其发色团的化学组成,目前的研究已逐渐转向对其化学基团的识别。因此,本综述主要侧重于基于发色团对 BrC 的化学认识,并详细总结了 BrC 发色团的二次形成机理、光敏反应以及对人体健康的影响。首先,BrC 发色团分为五类:氮杂环、氮链、芳香族、低聚物和含硫有机化合物。不同的发色团前体种类各不相同,其形成机制也各不相同。其次,由于溴化碳是生物质和化石燃料不完全燃烧过程中形成的光吸收颗粒的重要组成部分,溴化碳可引发二次有机气溶胶(SOA)前体的产生或导致 SOA 的增长,从而可能对人类健康产生不利影响。最后,针对 BrC 开发充分分离的方法并改进算法和机器学习,可以更有效地了解发色团的化学成分,从而更好地评估 BrC 对大气的影响和对健康的影响。总之,本综述对 BrC 发色团的分类提供了新的见解,并在化学结构的基础上,在二次形成机制、光敏反应和人类健康影响方面取得了新的进展。
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引用次数: 0
Efficient activation of peroxymonosulfate for catalytic degradation of organic pollutants by simultaneously using low-level cobalt ions and calcium carbonate micro-particles 同时使用低浓度钴离子和碳酸钙微粒高效活化过一硫酸盐以催化降解有机污染物
2区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2024-04-13 DOI: 10.1016/j.jes.2024.04.004
Yu Zhou , Xiaobo Wang , Nan Wang , Shuangshuang Huang , Lihua Zhu

An efficient catalytic system was developed to remove various organic pollutants by simultaneously using low-level cobalt ions, calcium carbonate micro-particles and peroxymonosulfate (PMS). A simple base-induced precipitation was used to successfully loaded Co-centered reactive sites onto the surface of CaCO3 microparticles. Under optimal conditions at 25 °C, 10 mg/L methylene blue (MB) could be completely degraded within 10 min with 480 µg/L Co2+, 0.4 g/L CaCO3 microparticles (or 0.4 g/L Co@CaCO3) and 0.1 g/L PMS. The MB degradation followed the pseudo first order kinetics with a rate constant of 0.583 min−1, being 8.3, 11.5 and 53.0 times that by using Co-OH (0.07 min−1), Co2+ (0.044 min−1) and CaCO3 (0.011 min−1) as the catalyst, respectively. It was confirmed that there was a synergistic effect in the catalytic activity between Co species and the CaCO3 particles but the major contributor was the highly dispersed Co species. When Co2+-containing simulated electroplating wastewater was used as the Co2+ source, not only the added MB was also completely degraded within 5 min in this catalytic system, but also the coexisting heavy metal ions were substantially removed. The presently developed method was applied to simultaneously treat organic wastewater and heavy metals wastewater. The present method was also successfully used to efficiently degrade other organic pollutants including bisphenol A, sulfamethoxazole, rhodamine B, tetrabromobisphenol A, ofloxacin and benzoic acid. A catalytic mechanism was proposed for the PMS activation by Co@CaCO3. The surface of CaCO3 particles favors the adsorption of Co2+. More importantly, the surface of CaCO3 particles provides plentiful surface -OH and -CO32+, and these surface groups complex with Co2+ to produce more catalytically active species such as surface [CoOH], resulting in rapid Co2+/Co3+ cycling and electron transfer. These interactions cause the observed synergistic effect between Co species and CaCO3 particles in PMS activation. Due to good cycle stability, strong anti-interference ability and wide universality, the new method will have broad application prospects.

通过同时使用低浓度钴离子、碳酸钙微粒和过一硫酸盐(PMS),开发了一种高效的催化系统来去除各种有机污染物。利用简单的碱诱导沉淀法成功地将钴中心反应位点负载到 CaCO3 微颗粒表面。在 25 °C 的最佳条件下,480 µg/L Co2+、0.4 g/L CaCO3 微颗粒(或 0.4 g/L Co@CaCO3)和 0.1 g/L PMS 可在 10 分钟内完全降解 10 mg/L 亚甲基蓝(MB)。甲基溴降解遵循伪一阶动力学,速率常数为 0.583 min-1,分别是使用 Co-OH(0.07 min-1)、Co2+(0.044 min-1)和 CaCO3(0.011 min-1)作为催化剂时的 8.3、11.5 和 53.0 倍。研究证实,Co 物种和 CaCO3 粒子之间在催化活性方面存在协同效应,但主要贡献者是高度分散的 Co 物种。当使用含 Co2+ 的模拟电镀废水作为 Co2+ 源时,在该催化体系中,不仅添加的甲基溴在 5 分钟内被完全降解,而且共存的重金属离子也被大量去除。目前开发的方法可同时处理有机废水和重金属废水。该方法还成功地用于高效降解其他有机污染物,包括双酚 A、磺胺甲噁唑、罗丹明 B、四溴双酚 A、氧氟沙星和苯甲酸。提出了 Co@CaCO3 活化 PMS 的催化机理。CaCO3 颗粒表面有利于 Co2+ 的吸附。更重要的是,CaCO3 颗粒的表面提供了大量的表面 -OH 和 -CO32+,这些表面基团与 Co2+ 复合,产生催化活性更强的物种,如表面 [CoOH]-,导致 Co2+/Co3+ 快速循环和电子转移。这些相互作用导致在 PMS 活化过程中观察到 Co 物种与 CaCO3 颗粒之间的协同效应。由于新方法具有良好的循环稳定性、较强的抗干扰能力和广泛的通用性,因此将具有广阔的应用前景。
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引用次数: 0
Correlation of volatile organic chemical exposure with uric acid metabolism among US population: A cross-sectional study from NHANES program 美国人口中挥发性有机化学物暴露与尿酸代谢的相关性:一项来自 NHANES 计划的横断面研究
IF 5.9 2区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2024-04-11 DOI: 10.1016/j.jes.2024.04.002
Yiyi Wang , Zichao Jiang , Jing Lei , Ziliang Tan , Yijie Wu , Yihe Hu , Junxiao Yang , Mingqing Li , Ting Lei , Long Hua

Volatile organic chemicals (VOC) have been identified as hazardous pollutants impairing human health. While whether the VOC exposure was associated with hyperuricemia is yet clarified. All the data was acquired from 6 survey cycles of the National Health and Nutrition Examination Survey (NHANES) program (2005–2006, 2011–2012, 2013–2014, 2015–2016, 2017–2018, 2017–2020). Hyperuricemia was defined as a serum uric acid (SUA) concentration exceeding 7 mg/mL in men or 6 mg/mL in women. Three quantile logistic regression models with varied covariates were developed to analyze the correlation between hyperuricemia and volatile organic chemical metabolites (VOCs) in urine, and three quantile linear regression models were used for examining the correlation between VOCs and SUA. N-acetyl-S-(2-carboxyethyl)-l-cysteine (CEMA), N-acetyl-S-(3,4-dihydroxybutyl)-l-cysteine (DHBM), and phenylglyoxylic acid (PHGA) were identified to associated positively with increased hyperuricemia risk and uric acid level. Meanwhile, the weighted quantile sum (WQS) model suggested a positive association between VOCs exposure and hyperuricemia. These data indicate that VOC exposure potentially increases hyperuricemia risk, necessitating policies to mitigate VOC exposure.

挥发性有机化学物质(VOC)已被确定为损害人类健康的有害污染物。虽然挥发性有机化合物的暴露是否与高尿酸血症有关尚不明确。所有数据均来自美国国家健康与营养调查(NHANES)计划的6个调查周期(2005-2006年、2011-2012年、2013-2014年、2015-2016年、2017-2018年、2017-2020年)。高尿酸血症的定义是男性血清尿酸(SUA)浓度超过 7 毫克/毫升,女性超过 6 毫克/毫升。为分析高尿酸血症与尿液中挥发性有机化学代谢物(VOCs)之间的相关性,建立了三个具有不同协变量的量子逻辑回归模型,并使用三个量子线性回归模型来检验 VOCs 与 SUA 之间的相关性。结果发现,N-乙酰基-S-(2-羧乙基)-l-半胱氨酸(CEMA)、N-乙酰基-S-(3,4-二羟基丁基)-l-半胱氨酸(DHBM)和苯乙酸(PHGA)与高尿酸血症风险增加和尿酸水平呈正相关。同时,加权量化总和(WQS)模型表明,VOCs 暴露与高尿酸血症之间存在正相关。这些数据表明,接触挥发性有机化合物可能会增加高尿酸血症的风险,因此有必要制定政策来减少挥发性有机化合物的接触。
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引用次数: 0
The influence mechanism of environmental factors on DGT adsorbing sulfonamides and the migration between water and sediment 环境因素对DGT吸附磺胺类药物及在水和沉积物之间迁移的影响机制
2区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2024-04-08 DOI: 10.1016/j.jes.2024.03.056
Peng Zhang , Jingfeng Yan , Hao Ji , Linke Ge , Yanying Li

Obtaining the sulfonamides (SAs) concentrations in the water body and sediment bulk was a prerequisite to reveal their transport and partitioning behavior in sediment-water environments and accurately assess their ecological risk. In the present study, the influences of multifactor interactions on the performance of o-DGTs with XAD-18 binding gels were analyzed by central combination experiments and response surfaces analysis, in which the target compounds were 9 SAs. The results indicated that dissolved organic matter (DOM), pH, and suspended particulate matter (SS) had significant effects on the o-DGT sampling, whereas this o-DGT was independent of the ionic strength (IS). Concentning the composite influence of the four factors, the interaction between DOM and SS posed the most significant effect on all 9 SAs compounds. Subsequently, an o-DGT and DIFS model was applied to explore the SAs migration between the water-sediments interface. The difference between desorption rate (kb) and adsorption rates (kf) values suggested that the kinetics of SAs was dominated by adsorption. Moreover, the short-term sediment-water partitioning of SAs was clarified on the basis of distribution coefficient (Kdl) for the labile SAs, among which the sulfadiazine (SDZ) had the largest labile pool. The ability of sediments to release SAs to the liquid phase as a sink was determined by response time (Tc). Among the 9 SAs, the long-term release of soseulfamethoxypyridazine (SMP) from the solid phase of sediments would have a potential risk to the aquatic environment, to which more attention should be paid in the future.

要揭示磺胺类药物(SAs)在沉积物-水环境中的迁移和分配行为,并准确评估其生态风险,就必须获得水体和沉积物中磺胺类药物(SAs)的浓度。本研究以 9 种 SAs 为目标化合物,通过中心组合实验和响应面分析,分析了多因素相互作用对邻位 DGTs 与 XAD-18 结合凝胶性能的影响。结果表明,溶解有机物(DOM)、pH 值和悬浮颗粒物(SS)对 o-DGT 采样有显著影响,而该 o-DGT 与离子强度(IS)无关。综合四个因素的影响,DOM 和 SS 之间的交互作用对所有 9 种 SAs 化合物的影响最为显著。随后,应用 o-DGT 和 DIFS 模型探讨了 SAs 在水-沉积物界面之间的迁移。解吸速率(kb)和吸附速率(kf)之间的差异表明,SAs 的动力学以吸附为主。此外,根据易溶 SAs 的分布系数(Kdl),阐明了 SAs 的短期沉积物-水分配,其中磺胺嘧啶(SDZ)的易溶池最大。根据响应时间(Tc)确定了沉积物向液相释放 SAs 的能力。在这 9 种 SAs 中,磺胺甲氧哒嗪(SMP)从沉积物固相中的长期释放将对水生环境造成潜在风险,今后应对此给予更多关注。
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引用次数: 0
Efficiency and mechanism of controlling phosphorus release from sediment using a biological aluminum-based P-inactivation agent 使用铝基生物磷灭活剂控制沉积物磷释放的效率和机制
2区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2024-04-06 DOI: 10.1016/j.jes.2024.03.053
Changxiong Chen , Fei Li , Chunhua Shen , Xueping Tang , Mazhan Zhuang , Zhenming Zhou , Denghong Wang

Eutrophication is a significant challenge for surface water, with sediment phosphorus (P) release being a key contributor. Although biological aluminum-based P-inactivation agent (BA-PIA) has shown effectiveness in controlling P release from sediment, the efficiency and mechanism by BA-PIA capping is still not fully understood. This study explored the efficiency and mechanism of using BA-PIA capping controlling P release from sediment. The main mechanisms controlling P release from sediment via BA-PIA capping involved transforming mobile and less stable fractions into stable ones, passivating DGT-labile P and establishing a 13 mm 'P static layer' within the sediment. Additionally, BA-PIA's impact on Fe redox processes significantly influenced P release from the sediment. After BA-PIA capping, notable reductions were observed in total P, soluble reactive P (SRP), and diffusive gradient in thin-films (DGT)-measured labile P (DGT-labile P) concentration in the overlying water, with reduction rates of 95.6%, 92.7%, and 96.5%, respectively. After BA-PIA capping, the diffusion flux of SRP across the sediment-water interface and the apparent P diffusion flux decreased by 91.3% and 97.8%, respectively. Additionally, BA-PIA capping led to reduced concentrations of SRP, DGT-labile P, and DGT-measured labile Fe(II) in the sediment interstitial water. Notably, BA-PIA capping significantly reduced P content and facilitated transformation in the 0∼30 mm sediment layers but not in the 30∼45 mm and 45∼60 mm sediment layers for NaOH-extractable inorganic P and HCl-extracted P. These findings offer a theoretical basis and technical support for the practical application of BA-PIA capping to control P release from sediment.

富营养化是地表水面临的一个重大挑战,而沉积物中磷(P)的释放是其中的一个关键因素。虽然生物铝基磷灭活剂(BA-PIA)在控制沉积物中磷的释放方面显示出了有效性,但人们对 BA-PIA 封盖的效率和机理仍不完全了解。本研究探讨了使用 BA-PIA 封盖控制沉积物中 P 释放的效率和机理。通过 BA-PIA 封层控制沉积物中 P 释放的主要机制包括将流动性和稳定性较差的馏分转化为稳定的馏分、钝化 DGT 标记的 P 以及在沉积物中建立一个 13 毫米的 "P 静态层"。此外,BA-PIA 对铁氧化还原过程的影响也极大地影响了沉积物中 P 的释放。BA-PIA 封盖后,上覆水中的总磷、可溶性活性磷(SRP)和薄层中的扩散梯度(DGT)测量的可溶性磷(DGT-可溶性磷)浓度明显降低,降低率分别为 95.6%、92.7% 和 96.5%。BA-PIA 封盖后,SRP 在沉积物-水界面上的扩散通量和表观 P 扩散通量分别降低了 91.3% 和 97.8%。此外,BA-PIA 封盖还降低了沉积物间隙水中的 SRP、DGT 标记的 P 和 DGT 测量的标记铁(II)的浓度。值得注意的是,对于 NaOH 萃取的无机磷和 HCl 萃取的磷而言,BA-PIA 封盖显著降低了 0∼30 毫米沉积层中的磷含量并促进了其转化,但在 30∼45 毫米和 45∼60 毫米沉积层中却没有这种效果。
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引用次数: 0
Nighttime reactions of a series of unsaturated alcohols with NO3•: Kinetics, products and mechanisms study 一系列不饱和醇与 NO3- 的夜间反应:动力学、产物和机理研究
2区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2024-04-06 DOI: 10.1016/j.jes.2024.03.043
Yanyong Xu , Shengrui Tong , Weiran Li , Meifang Chen , Lin Hu , Hailiang Zhang , Sufan Wang , Maofa Ge

Unsaturated alcohols are a class of Biogenic volatile organic compounds (BVOCs) emitted in large quantities by plants when damaged or under adverse environmental conditions, and studies on their atmospheric degradation at night are still lacking. We used chamber experiments to study the gas-phase reactions of three unsaturated alcohols, E-2-penten-1-ol, Z-2-hexen-1-ol and Z-3-hepten-1-ol, with NO3 radicals (NO3•) during the night. The rate constants of these reactions were (11.7 ± 1.76) × 10−13, (8.55 ± 1.33) × 10−13 and (6.08 ± 0.47) × 10−13 cm3/(molecule·s) at 298K and 760 Torr, respectively. In contrast, the reaction rate of similar substances with ozone was about 10−18 cm3/(molecule·s), which indicates that the reaction with NO3• is the main oxidation pathway for unsaturated alcohols at night. Small molecule aldehydes and ketones were the main gas-phase organic products of the reaction of three aldehydes and ketones with NO3•, and the total small molecule aldehydes and ketones yields can reach between 45%-60%. They mainly originate from the breakage of alkoxy radicals, and different breakage sites determine different product distributions. In addition, the SOA yields of the three unsaturated alcohols with NO3• were 7.1% ± 1.0%, 12.5% ± 1.9% and 30.0% ± 4.5%, respectively, which were much higher than those of similarly structured substances with O3 or OH radicals (•OH). The results of high-resolution mass spectrometry shows that the main components of Secondary organic aerosol (SOA) of the three unsaturated alcohols are dimeric compounds containing several nitrate groups, which are formed through the polymerization of oxyalkyl radicals.

不饱和醇类是一类生物挥发性有机化合物(BVOCs),当植物受到破坏或在不利环境条件下会大量释放,目前还缺乏对其在夜间大气中降解的研究。我们利用室内实验研究了三种不饱和醇(E-2-戊烯-1-醇、Z-2-己烯-1-醇和 Z-3-庚烯-1-醇)与 NO3 自由基(NO3-)在夜间的气相反应。在 298K 和 760 Torr 下,这些反应的速率常数分别为 (11.7 ± 1.76) × 10-13、(8.55 ± 1.33) × 10-13 和 (6.08 ± 0.47) × 10-13 cm3/(分子-s)。相比之下,同类物质与臭氧的反应速率约为 10-18 cm3/(分子-s),这表明与 NO3- 的反应是夜间不饱和醇的主要氧化途径。小分子醛酮是三种醛酮与 NO3- 反应的主要气相有机产物,小分子醛酮的总产率可达 45%-60% 之间。它们主要来源于烷氧基自由基的断裂,不同的断裂位点决定了不同的产物分布。此外,含有 NO3- 的三种不饱和醇的 SOA 产率分别为 7.1% ± 1.0%、12.5% ± 1.9% 和 30.0% ± 4.5%,远高于含有 O3 或 OH 自由基(-OH)的同类结构物质。高分辨率质谱分析结果表明,这三种不饱和醇的二次有机气溶胶(SOA)的主要成分是含有多个硝酸基团的二聚化合物,它们是由氧烷基自由基聚合而成的。
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引用次数: 0
Humic-like components in dissolved organic matter inhibit cadmium sequestration by sediment 溶解有机物中的类腐殖质成分抑制沉积物对镉的固碳作用
2区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2024-04-06 DOI: 10.1016/j.jes.2024.03.055
Bolin Li , Zhongwu Li , Jia Chen , Changsheng Jin , Weicheng Cao , Bo Peng

China's lakes are plagued by cadmium (Cd) pollution. Dissolved organic matter (DOM) significantly regulates Cd(II) transport properties at the sediment-water interface. Understanding the effects of different DOM components on the transportation properties of Cd(II) at the sediment-water interface is essential. In this study, typical DOM from different sources was selected to study Cd(II) mobility at the sediment-water interface. Results showed that terrestrial-derived DOM (fulvic acids, FA) and autochthonous-derived DOM (α-amylase, B1) inhibit Cd(II) sequestration by sediments (42.5% and 5.8%, respectively), while anthropogenic-derived DOM (sodium dodecyl benzene sulfonate, SDBS) increased the Cd(II) adsorption capacity by sediments by 2.8%. Fluorescence quenching coupling with parallel factor analysis (EEM-PARAFAC) was used to characterize different DOM components. The results showed that FA contains three kinds of components (C1, C3: protein-like components, C2: humic-like components); SDBS contains two kinds of components (C1, C2: protein-like components); B1 contains three kinds of components (C1, C2: protein-like components, C3: humic-like components).Three complex reaction models were used to characterize the ability of Cd(II) complex with DOM, and it was found that the humic-like component could hardly be complex with Cd(II). Accordingly, humic-like components compete for Cd(II) adsorption sites on the sediment surface and inhibit Cd(II) adsorption from sediments. Fourier transform infrared spectroscopy (FTIR) of the sediment surface before and after Cd(II) addition was analyzed and proved the competitive adsorption theory. This study provides a better understanding of the Cd(II) mobilization behavior at the sediment-water interface and indicates that the input of humic-like DOM will increase the bioavailability of Cd.

中国的湖泊深受镉(Cd)污染的困扰。溶解有机物(DOM)对镉(II)在沉积物-水界面的迁移特性有重要影响。了解不同溶解有机物成分对镉(II)在沉积物-水界面迁移特性的影响至关重要。本研究选择了不同来源的典型 DOM 来研究镉(II)在沉积物-水界面的迁移性。结果表明,陆生来源的 DOM(富里酸,FA)和自生来源的 DOM(α-淀粉酶,B1)会抑制沉积物对 Cd(II)的固着(分别为 42.5% 和 5.8%),而人为来源的 DOM(十二烷基苯磺酸钠,SDBS)会增加沉积物对 Cd(II)的吸附能力,增幅为 2.8%。荧光淬灭耦合平行因子分析(EEM-PARAFAC)用于描述不同 DOM 成分的特征。结果表明,FA含有3种成分(C1、C3:类蛋白成分,C2:腐殖质成分);SDBS含有2种成分(C1、C2:类蛋白成分);B1含有3种成分(C1、C2:类蛋白成分,C3:腐殖质成分)。因此,类腐殖质成分会竞争沉积物表面的镉(II)吸附位点,抑制沉积物对镉(II)的吸附。对添加 Cd(II) 前后沉积物表面的傅立叶变换红外光谱(FTIR)进行了分析,证明了竞争吸附理论。这项研究有助于更好地理解镉(II)在沉积物-水界面的迁移行为,并表明腐殖质类 DOM 的加入会增加镉的生物利用率。
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引用次数: 0
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Journal of Environmental Sciences-china
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