城郊与城镇河流中溶解性有机质与重金属的相关性

溶解性有机质(dissolved organic matter,DOM)在水体环境中广泛存在,对重金属在水环境中的环境行为有重要影响.本研究为探讨DOM与重金属的相关性,以宁波市城郊流域樟溪和城镇流域芦江为例,利用三维荧光技术分析不同城镇化梯度下河流水体溶解性有机质(DOM)的结构组成特征,分析DOM各项参数与重金属之间的相关性.结果表明,城镇化程度较高的河流水体具有较高的DOC、有色溶解性有机质(CDOM)和荧光溶解性有机质(FDOM)浓度;城郊流域与城镇流域水体中DOM均含有4个荧光峰,类富里酸荧光峰A和C以及类蛋白荧光峰B和T,且城镇流域水体荧光峰B和T的强度显著高于城郊流域,DOM腐殖化程度与芳香性也具有同样的趋势;城镇流域水体中重金属As、Cu和Mn浓度显著高于城郊流域.DOM与重金属的相关性结果表明,城镇河流中DOM与Cu、Cr、Mn、As、Zn和Pb都存在显著的正相关关系,而城郊河流中DOM只与Mn、Pb和Cu呈显著正相关,与其它重金属相关性不明显.总之,城镇化水平影响河流水体中CDOM的浓度和性质,而CDOM浓度和性质与重金属的行为密切相关.     

水环境中有机污染物与溶解性有机质相互作用研究

溶解性有机质(DOM)是水环境中重要的有机组分,主要通过氢键、范德华力、疏水作用等多种作用吸附结合有机污染物,影响有机污染物的迁移转化等环境行为,同时DOM对水环境中有机污染物的吸附作用还受DOM和有机污染物的性质等诸多因素的影响。     

乌梁素海沉积物溶解性有机质荧光光谱特性

采用三维荧光光谱技术(3DEEM)研究了乌梁素海沉积物溶解性有机质的结构组成特征.结果表明,乌梁素海沉积物溶解性有机质出现了6种荧光峰,分别代表类蛋白荧光物质和类富里酸荧光物质,且不同湖区沉积物溶解性有机质结构组成具有一定差异性.乌梁素海沉积物DOM的荧光指数处于1.74~1.96之间,及其DOM来源具有陆源和内源的双重特性,其中陆源主要来自西部河套灌区农田退水输入,内源主要来自芦苇等大型挺水植物死亡腐烂分解.因此,控制河套灌区农田退水排入以及抑制芦苇等挺水植物大量生长是保护乌梁素海生态环境和控制其富营养化的有效措施.     

水环境中溶解性有机物溯源分析及分子结构表征概述

溶解性有机物(DOM)是地球上最大的碳基化合物反应性储层之一,涉及各种生物地化反应并且在污染物溶解度、毒性、生物利用度、流变性和分布中发挥重要作用。本文介绍了当前用于表征水环境中DOM的策略和工具,探讨了当前研究在技术限制(预处理过程复杂、仪器分辨率低、数据处理困)、结构复杂性、结构多变性等方面存在的诸多局限性。分析认为:已有研究主要侧重于溯源分析和分子结构特征解析,未来研究应该在不同的结构层面和角度开展,加强多学科融合、数据库创建、对照实验和协同工作。     

湖泊草、藻来源溶解性有机质及其微生物降解的差异

太湖生态类型多样,存在着水环境差异比较显著的草、藻型湖区,其水体中溶解性有机质(DOM)的来源及组分特征也存在较大差异.为了检验草、藻来源的DOM组分特征及其微生物降解机制的差异性,分别选取太湖藻型湖区的蓝藻水华及草型湖区的优势水生植物马来眼子菜进行室内细菌降解实验.结果表明,浮游植物及沉水植物的细菌降解都能快速释放营养盐和有机质,而且释放的DOM均以极具活性的类蛋白荧光组分为主.草源和藻源DOM在组分构成上存在显著差异,藻源DOM以类色氨酸组分为主,而草源DOM荧光物质则基本上以类酪氨酸组分C3为主,草、藻来源DOM的荧光组分差异与野外调查结果相似.经过细菌的降解利用,草、藻来源的DOM类蛋白荧光强度都迅速减弱,藻源性溶解物质相对容易被细菌降解利用,在2 d之内就能降解约70%,而草源性DOM的降解速率则较低,通常降解转化周期则为更长时间.     

三峡库区消落带土壤溶解性有机质溯源:基于氮/碳比值的线性双端元源负荷分析

土壤溶解性有机质(soil DOM)作为陆地系统天然有机质的重要组成部分,以其活跃的生物地球化学性质,在污染物的环境行为中扮演着极其重要的作用.而了解其来源和结构组成是进一步明确其"结构-反应活性"的关键和前提.本文以三峡库区消落带土壤DOM为研究对象,基于传统氮/碳比值(N/C)及衍生的双端元源负荷模型,讨论该溯源方法在分子水平上的合理性;同时采用光漂白试验,进一步讨论各样本反应活性与其源负荷的相关性.结果表明,N/C值和双端元线性混合模型值均表明土壤DOM具有"陆源"和"内源"的双重特性——这与其他高级分析技术溯源结果基本一致.这种传统溯源分析结果在分子水平上具有合理性,但仅仅反映DOM结构和来源在特定面相上的信息,只能证明库区土壤DOM属于"混合型来源",却无法提供分辨率更高的特定组分来源信息.另外,N/C元素比值及源负荷分别和光漂白动力学过程极显著相关,因此可作为较方便的指标,快速简单判断DOM的光化学反应活性.但在关注DOM本身生物地球化学的研究工作中,仍建议使用多重方法的比较分析,以便于提高单一解析方法的分辨率.     

垃圾填埋场地下水溶解性有机物光谱特征

垃圾填埋为我国垃圾处理的最主要途径,填埋过程中渗滤液的泄漏将导致附近地下水污染.地下水中溶解性有机物(DOM)能示踪外来污染物的来源、形态和迁移转化过程,其组成、结构和分布的差异具有重要的环境指示意义.联合现代光谱技术及多元统计分析方法,研究了不同运行年限填埋场地下水中DOM来源、组成和分子结构特征,探究了不同年限地下水DOM动力学演化规律.结果表明,填埋场地下水DOM以微生物来源为主,其次为自生陆源.填埋前期阶段其微生物来源DOM较多,而在填埋后期微生物来源DOM减弱.填埋年限较短的填埋场地下水DOM主要为一些新生成腐殖化程度较低的易降解类色氨酸和类酪氨酸,其促进微生物活性,且各点位差异性较大,应提高预警措施.填埋时间相对较长的填埋场地下水有机质腐殖化率高,难降解的大分子物质累积,微生物活性减弱,填埋垃圾趋向稳定对地下水影响减弱.     

春灌背景下黄河上游清水河流域DOM的空间分布规律

运用三维荧光光谱技术结合紫外-可见吸收光谱表征技术,以及各种分析统计方法,对清水河流域水体中溶解性有机质（DOM）的空间分布、光谱特征及污染来源进行了解析,以期为黄河流域水环境治理及污染溯源提供较为可靠的信息.结果表明清水河流域春灌季水质指标空间差异性较大.DOM中类蛋白质物质浓度高于类腐殖质物质浓度,自生源特征强于陆源特征,且新生成的DOM占比较大,即DOM主要来源于水体微生物活动和细菌降解代谢的产物.PARAFAC解析得到6个主成分,包括4个类蛋白质组分（C1、C2、C3、C5）和2个类腐殖质组分（C4、C6）,其中类蛋白质组分的空间差异性大于类腐殖质组分,受水库水和污水处理厂排水等水体内源影响较大.PCA分析得到4个主成分,组分C5、氟离子、组分C2和HIX可分别作为该4个主成分的描述性指标.     

溶解性有机质的光谱特征及其对土壤吸附β-HCH的影响

通过考察4种不同来源的溶解性有机质(Dissoived Organic Matter,DOM)的紫外-可见光谱和三维荧光光谱特征,分析DOM的组分及结构,研究它们对β-HCH在土壤中的吸附影响.结果表明,不同来源的DOM具有不同的组成结构,对β-HCH在土壤中的吸附有不同影响.光谱特征分析结果显示,DOM芳香性和疏水性强弱顺序为:营养土A土淤泥B土.研究显示,在去除DOM条件下,土壤对β-HCH吸附量增加,即内源DOM的存在均抑制了土壤对β-HCH的吸附能力,吸附能力与内源DOM组分的亲疏水性有关.外源DOM均能促进土壤对β-HCH的吸附能力,但来源不同,促进土壤吸附β-HCH的能力不同,其吸附能力的强弱排序为:淤泥DOM营养土DOMB土DOM,这是由各土壤DOM的不同组分及不同的疏水性导致的.     

鄱阳湖沉积物溶解性有机质光谱特征

目前针对鄱阳湖流域沉积物溶解性有机质(DOM)光谱特征的研究仍较少,因此基于紫外-可见光谱和三维荧光光谱技术,并结合平行因子分析法(PARAFAC),对鄱阳湖沉积物中DOM的物质组成和来源特征进行了解析.结果表明,鄱阳湖沉积物DOM的腐殖化程度较高,是陆源输入和藻类、浮游生物等内源产生的混合型,且以陆源输入为主.与碟形湖区相比,通江水域沉积物DOM的有色溶解性有机质浓度更高、 DOM粒径更大且芳香性及腐殖化程度更高.通过PARAFAC共解析出3个类腐殖质组分(C1、 C2、 C4)和1个类蛋白组分(C3).与碟形湖相比,腐殖质组分均表现为通江水域更高,其中C1组分在两区域的占比均为所有组分中最高,前者为42%,后者为46%.空间分布上,4个组分荧光强度总体上呈现东高西低的趋势,高值主要分布在都昌和南矶湿地水域附近,分析主要与丰水期水位上涨、大量植物被淹死亡和人类活动有关.主成分分析结果表明,湖区不同沉积物DOM荧光组分差异较小,但以碟形湖区沉积物DOM腐殖化程度略高.     

海水溶解有机质分离富集方法的发展与比较

溶解有机质（dissolved organic matter,DOM）在海洋生物地球化学循环中扮演着重要的角色。了解海洋DOM的化学组成和化学性质是理解海洋碳、氮等重要生源要素环境行为的必要前提。近年来快速发展的分析技术为解析DOM分子组成与结构提供了新的机遇,与多数陆地淡水DOM相比,海水DOM不仅具有浓度低、化学成分复杂的特征,而且伴随着很高的无机盐含量。光谱技术如紫外-可见光谱和三维荧光光谱可对过滤后的海水进行直接测定,但对质谱和核磁技术而言,只有对海水DOM进行分离和富集后才能满足高分辨率分析的要求。本文对常用的海水DOM分离富集方法,包括固相萃取（SPE）、反渗透电渗析（RO/ED）和超滤（UF）进行了综述,讨论了每种方法的优缺点,并对未来海水DOM的分析发展做了展望。     

长期不同水分调控对污染场地土壤溶解性有机质含量及其结构特征的影响

为了考察不同水分调控下污染场地中土壤有机质和溶解性有机质（DOM）的演变过程,以2种冶炼厂重金属污染土壤为研究对象,通过恒温恒湿培养实验观察不同水分调控下土壤有机质和DOM的含量变化,并采用紫外-可见光谱和荧光光谱分析了土壤DOM的光谱特征.结果表明,水分调控180 d后,2种重金属污染土壤中有机质和DOM含量呈不同程度降低趋势,且随着水分含量增加,其降幅明显增加,最大降幅分别为33.28%和89.35%.水分调控过程中,土壤DOM中类蛋白物质最易发生降解,导致类富里酸和类腐殖酸的占比相应提高;随着水分含量增加,土壤DOM的芳香性提高,腐殖化程度升高,分子聚合度和分子量增大,最终导致DOM稳定性增强,上述结果有助于揭示水分诱导过程中DOM的变化对污染场地中重金属环境行为的影响.     

Improving biodegradation potential of domestic wastewater by manipulating the size distribution of organic matter

Carbon source is a critical constraint on nutrient removal in domestic wastewater treatment. However, the functions of particulate organic matter (POM) and some organics with high molecular weight (HMW) are overlooked in the conventional process, as they cannot be directly assimilated into cells during microbial metabolism. This further aggravates the problem of carbon source shortage and thus affects the effluent quality. Therefore, to better characterize organic matter (OM) based MW distribution, microfiltration/ultrafiltration/nanofiltration (MF/UF/NF) membranes were used in parallel to fractionate OM, which obtained seven fractions. Hydrolysis acidification (HA) was adopted to manipulate the MW distribution of dissolved organic matter (DOM) and further explore the correlation between molecular size and biodegradability. Results showed that HA pretreatment of wastewater not only promoted transformation from POM to DOM, but also boosted biodegradability. After 8 hr of HA, the concentration of dissolved organic carbon (DOC) increased by 65%, from the initial value of 20.25 to 33.48 mg/L, and the biodegradability index (BOD5 (biochemical oxygen demand)/SCOD (soluble chemical oxygen demand)) increased from 0.52 to 0.74. Using MW distribution analysis and composition optimization, a new understanding on the characteristics of organics in wastewater was obtained, which is of importance to solving low C/N wastewater treatment in engineering practice.     

Prediction of DOM removal of low specific UV absorbance surface waters using HPSEC combined with peak fitting

High performance size exclusion chromatography (HPSEC) is used in water quality research primarily to determine the molecular weight distribution of the dissolved organic matter (DOM), but by applying peak fitting to the chromatogram, this technique can also be used as a tool to model and predict DOM removal. Six low specific UV absorbance (SUVA) source waters were treated using coagulation with alum and both the source and treated water samples were analysed using HPSEC. By comparing the molecular weight profiles of the source and treated waters, it was established that several DOM components were not effectively removed by alum coagulation even after high dosage alum treatment. A peak-fitting technique was applied based on the concept of linking the character (molecular weight profile) of the recalcitrant organics in the treated water with those of the source water. This was then applied to predict DOM treatability by determining the areas of the peaks which were assigned to removable organics from the source water molecular weight profile after peak fitting, and this technique quantified the removable and non-removable organics. The prediction was compared with the actual dissolved organic carbon (DOC) removal determined from jar testing and showed good agreement, with variance between 2% and 10%. This confirmed that this prediction approach, which was originally developed for high SUVA waters, can also be applied successfully to predict DOC removal in low SUVA waters.     

Understanding the risks of mercury sulfide nanoparticles in the environment: Formation, presence, and environmental behaviors

Mercury (Hg) could be microbially methylated to the bioaccumulative neurotoxin methylmercury (MeHg), raising health concerns. Understanding the methylation of various Hg species is thus critical in predicting the MeHg risk. Among the known Hg species, mercury sulfide (HgS) is the largest Hg reservoir in the lithosphere and has long been considered to be highly inert. However, with advances in the analytical methods of nanoparticles, HgS nanoparticles (HgS NPs) have recently been detected in various environmental matrices or organisms. Furthermore, pioneering laboratory studies have reported the high bioavailability of HgS NPs. The formation, presence, and transformation (e.g., methylation) of HgS NPs are intricately related to several environmental factors, especially dissolved organic matter (DOM). The complexity of the behavior of HgS NPs and the heterogeneity of DOM prevent us from comprehensively understanding and predicting the risk of HgS NPs. To reveal the role of HgS NPs in Hg biogeochemical cycling, research needs should focus on the following aspects: the formation pathways, the presence, and the environmental behaviors of HgS NPs impacted by the dominant influential factor of DOM. We thus summarized the latest progress in these aspects and proposed future research priorities, e.g., developing the detection techniques of HgS NPs and probing HgS NPs in various matrices, further exploring the interactions between DOM and HgS NPs. Besides, as most of the previous studies were conducted in laboratories, our current knowledge should be further refreshed through field observations, which would help to gain better insights into predicting the Hg risks in natural environment.     

Environmental fate and behavior of silver nanoparticles in natural estuarine systems

Silver nanoparticles (AgNPs) are widely used in many consumer products, whereas their environmental behaviors in natural aquatic systems remain unknown, especially in natural brackish media. Therefore, it is urgent to investigate the environmental fate of AgNPs in natural brackish waters. Here, we investigated the stability of citrate-coated AgNPs in natural brackish water collected from 6 different sites with distinct salinities in the Xinglinwan Reservoir, located in Xiamen City, southeast China. The obtained results showed that AgNP colloids remained stable in low-salinity waters, which was mainly determined by the effects of dissolved organic matter (DOM) promoting the stability of the nanoparticles. However, the environmental fate of AgNPs in high-salinity waters was dominated by the salinity or ionic strength, especially the free ion concentrations of Cl^?, SO₄^2?, or S^2?, resulting in rapid sedimentation and dissolution. In addition, both DOM and salinity contributed to the environmental behavior of AgNPs in moderate-salinity waters, ultimately resulting in either colloidal stability or sedimentation. Overall, these results may reveal that AgNPs remain relatively stable for a long period in low-salinity natural waters, and that the stability might gradually decrease as AgNPs are transferred from freshwaters through brackish waters and eventually end up in seawater along the bay. Our findings also further indicate that the toxicity and potential risks of AgNPs may present more serious threats to the environment and organisms in natural freshwaters than in natural estuarine systems or seawater.     

Characterization of dissolved organic matter as N-nitrosamine precursors based on hydrophobicity, molecular weight and fluorescence

It is very important to identify the dominant precursors for N-nitrosamine formation from bulk organic matter, to enhance the understanding of N-nitrosamine formation pathways in water treatment plants and allow the development of practical treatment technologies. In this study, dissolved organic matter (DOM) from two source waters was fractionated with XAD resins and ultra- filtration membranes. The N-nitrosamine formation potential (FP) (ng of N-nitrosamines formed per mg of dissolved organic carbon (DOC)) from raw water and each fraction were measured and correlated with the fluorescence excitation-emission matrix (EEM), molecular weight (MW) and other assays. The results showed that the hydrophilic fraction had N-nitrosamine FP 1.3 to 3.5 times higher than the hydrophobic fraction from both source waters. The DOM fraction with low MW was the dominant fraction in these two source waters and contributed more precursors for N-nitrosamine formation than the larger MW fraction. The EEM spectra indicated there were notable amounts of soluble microbial products (SMPs) and aromatic proteins in the two studied rivers, which probably originated from wastewater discharge. The SMPs tended to be more closely correlated with N-nitrosodimethylamine formation potential than the other DOM components. Higher N-nitrosamine FP were also related to fractions with lower DOC/DON ratios and lower SUVA 254 values.     

水环境中天然溶解有机质分子量的研究现状及意义

溶解有机质存在于所有的水环境中,它是组成不均匀、结构复杂和分子量分布很宽的有机化合物混合体。本文综述了测量溶解有机质分子量的主要方法,各种方法的原理和优缺点,其中详细介绍了高效体积排阻色谱法的原理,平均分子量和分散系数的计算,以及分子量的校正;同时介绍了可能影响分子量分布的主要地球化学因素,以及天然水中溶解有机质的分子量分布的特征。     

施用污泥堆肥及其水溶性有机物对土壤中荧蒽解吸-淋滤的影响

以荧蒽（Fluoranthene）为多环芳烃（PAHs）的代表,通过序批试验及土柱淋洗试验研究了污泥堆肥及污泥堆肥水溶性有机物（DOM）对污染土壤中荧葸解吸和淋滤的影响．施用污泥堆肥实验结果表明,污泥堆肥施入土壤后的短时间内由于带入和产生的DOM而表现出促进土壤中荧蒽的解吸与淋滤,但随着DOM的降解,该作用逐渐消失．污泥堆肥充分腐熟后（腐熟堆肥）因DOM少而稳定的腐殖质等固相有机质含量相对较多,而表现出施用腐熟堆肥后土壤更易对荧葸吸持．单独施用污泥堆肥DOM后的试验,也进一步表明了污泥堆肥DOM的存在确实能促进土壤中荧蒽的迁移,且在相同DOM浓度下,腐熟堆肥DOM对土壤中荧蒽的解吸和淋滤的促进作用明显高于初始堆肥DOM处理,原因在于腐熟堆肥DOM中大分子组分和疏水性组分的含量比初始堆肥的DOM要多．因此,堆肥施用对土壤多环芳烃环境行为或活性的影响是堆肥施人土壤后固相有机质含量及性质和溶解性有机质的含量及性质等综合影响的结果．