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1.
鲁宗杰  邓娅敏  杜尧  沈帅  马腾 《地球科学》2017,42(5):771-782
水体中溶解性有机质(dissolved organic matter, DOM)是含水层中砷释放的主控因素之一.江汉平原河湖众多、沟渠广布,地表水体与浅层地下水的交互作用使得DOM的组分特征及其强度有显著差异.为查明江汉平原地下水中溶解性有机质在砷迁移转化过程中的作用,对江汉平原地表水和浅层地下水进行三维荧光光谱分析,使用平行因子分析法提取水体中有机质的分子组成、功能特点和荧光特征,并分析各组分相对含量与地下水中砷与铁的关联.江汉平原水体中DOM包括3种主要组分,组分C1、C2为类腐殖质,C2是生物降解过程中产生的小分子,C3为类蛋白物质.地下水DOM以类腐殖质组分C1、C2为主,地表水以类蛋白类物质C3和小分子腐殖质C2为主.高砷地下水中DOM以陆源为主,主要通过两种途径促进As的迁移转化:(1) DOM的腐殖质组分充当微生物群落的电子运输工具,促进微生物作用下的有机质氧化和铁氧化物的还原,并伴随As的释放及大量溶解性有机碳(dissolved organic carbon, DOC)和HCO3-的产生;(2) As以铁等金属阳离子为桥接物与腐殖质结合,通过形成As-Fe-DOM络合物,导致地下水中砷的迁移.   相似文献   

2.
洱海沉积物间隙水中溶解有机质的地球化学特性   总被引:11,自引:0,他引:11       下载免费PDF全文
对洱海沉积物间隙水中溶解有机质(DOM)含量、紫外可见吸收、荧光以及分子量等的垂直分布特征进行了研究。结果表明,DOC含量在沉积物水界面明显富集,随后急剧下降,6cm处达到最小值,随后呈上升趋势。DOC与吸光度值、荧光发射光谱强度之间具有一定的线性相关关系。DOM的E3/E4值范围在1~6之间,绝大多数在1~35之间。表征DOM中腐殖质来源的指标荧光指数值处于148~159之间,说明DOM以陆源输入为主。此外,洱海沉积物间隙水DOM分子量分布呈多峰分布模式,重均分子量(Mw)值在1462~1953Da之间,数均分子量(Mn)值在547~900Da之间,多分散性系数ρ值在202~305之间。随着沉积深度增大,Mw和Mn有略微的增大趋势,但变化不大。沉积物的氧化还原条件、微生物活动以及铁、锰氧化物等在沉积剖面的差异是控制间隙水中DOM各种地球化学特性的主要因素。  相似文献   

3.
冯琳  徐建中  翟立翔 《冰川冻土》2021,43(3):874-884
冰尘是冰川消融区表面黑色或棕色的球状聚合体,是冰川表面微生物的主要聚集区,同时含有丰富的溶解性有机质(dissolved organic matter, DOM),在冰川物质能量平衡、生物地球化学循环特别是碳循环中发挥着重要作用。在冰川消融期,受环境条件和微生物活动水平等方面的影响,冰川表面DOM的含量是动态变化的。为了研究冰尘中DOM的演化过程,于2017年7月在青藏高原东北部典型大陆性冰川老虎沟12号冰川消融区表面开展了为期18天的冰尘原位培养实验。结果显示:培养初期(第0~6天),冰尘水样中溶解性有机碳(DOC)浓度从13.41 mg?L-1显著降低到4.47 mg?L-1,培养后期(第6~18天),增加至6.71 mg?L-1;用特征紫外吸光度SUVA254分析培养期间“光-生物”演化过程对DOC吸光性的影响,结果表明:SUVA254的值先显著降低后显著升高,表明长时间的光照和微生物作用导致DOC浓度增加的同时,具有光吸收作用的化合物含量也显著增加。利用傅立叶离子回旋共振质谱分析DOM的分子组分发现,整个培养过程中(第0~18天),DOM中多肽类和脂类分子含量明显减少,不饱和烃类、芳烃类以及多环芳烃类化合物含量增加。分析第0天,第6天,第9天和第18天四个培养时段特有DOM分子组成的变化发现,“光-生物”演化过程使得冰尘中DOM的组成不断由脂类和多肽类向不饱和烃类、芳烃类以及多环芳烃类化合物转化。  相似文献   

4.
四川盆地卤水分布及开发前景展望   总被引:12,自引:4,他引:8  
四川盆地卤水分布广泛 ,自震旦系至白垩系各层系均有分布。卤水具低孔渗、高承压、品质优和气水同产等特点。卤水分高浓卤水、淡卤水和中浓卤水三类 ,均不同程度的含有Br-、I-、K+ 、B3 + 、Li+ 、Sr2 + 、Rb+ 等有益组分 ,皆为国家紧缺或紧俏物质 ,其含量多数可达工业品位 ,构成优质化工原料水 ,经济价值极高 ,开发利用前景广阔。  相似文献   

5.
地质流体自然类型与成矿流体类型   总被引:16,自引:2,他引:16  
水是地球上特征的地质流体 ,大部分矿床是在水热流体参与下形成的 ,但并不是所有流体都参与成矿。根据水的主要存在环境把水分为地质流体和成矿流体类型。各种环境广泛存在的水所构成的地质流体 ,又可细分为大气降水、盆地建造水、海水、岩浆水和变质水各种类型。研究认为成矿流体的形成主要与地质作用有关 ,是地质流体在特定环境特定演化阶段形成的特征产物。成矿流体则可划分为高温硅钾卤水、中温碳酸盐卤水及低温硫酸盐卤水。高温硅钾卤水中硅钾组分含量与温度、盐度成正相关关系 ,并且其中富含F-、B2 O3组分。这些特征与成矿作用中的高温钾化、硅化、萤石化及电气石化蚀变及热水沉积特征是一致的 ,高温成矿流体在演化过程中依次可以演变为中温或低温成矿流体。中温成矿流体以碳酸盐型流体为主 ,以富含Mn2 +,Fe2 +,Mg2 +的碳酸盐化合物为特征。低温成矿流体一般为硫酸盐型卤水 ,主要是Ba2 +,Sr2 +,Ca2 +的硫酸盐化合物 ,在海陆相各环境中广泛存在。大洋底部成矿流体是特殊环境下的地质流体类型 ,具有更广泛的温度区间 ,可以是从高温到中低温的系列流体类型 ,并且具有特殊地球化学组成。一般形成高温硅钾卤水与岩浆作用或变质作用有关 ,由于充分的水岩交代作用 ,可以获得较高的温度及足够的溶质组分 ;  相似文献   

6.
本研究通过测定有色溶解有机物(CDOM)的吸收光谱、荧光可溶性有机质(FDOM)的激发-发射-矩阵三维荧光光谱(excitation-emission-matrix spectra,EEMs)和稳定碳同位素组成(δ13C),系统探讨了长江口夏季水体可溶性有机质(DOM)的组成、来源、空间分布及河口混合行为等.研究结果表明,可溶性有机碳(DOC)浓度整体呈现由陆到海逐渐降低的趋势,表征有色溶解有机物含量水平的吸收系数a(355)与盐度呈负相关关系,指示可溶性有机质中荧光组分在河口的分布主要受稀释作用调控.利用EEMs并结合平行因子分析(PARAFAC)鉴定出代表陆源有机质的类腐殖质的荧光组分C2和C3,以及代表原地生产力的类蛋白质荧光组分C1和C4.由近岸到外海,表征海洋藻类生产力的C1组分在水体荧光有机质中所占比例增高,陆源信号则呈现逐渐降低趋势,与此相对应,外海水可溶性有机质具有高的光谱斜率S275–295/S350–400比值和重碳同位素组成.基于盐度vs.可溶性有机碳浓度、盐度vs.δ13C值的河流-海洋双端元混合模型,发现长江口最大混浊带存在可溶性有机碳的移除过程,且表现为以物理稀释作用为主的缺失性非保守混合行为.研究成果揭示了水动力条件是控制长江口-东海陆架系统可溶性有机质组成和空间分布的关键因素.  相似文献   

7.
马卡迪卡迪盐湖区为一现代干盐湖,盐湖以湖相碎屑沉积为主,在东侧的苏阿干盐湖赋存有高矿化孔隙卤水,通过对盐湖卤水系统的采样分析及综合研究,卤水主要化学组分为Na+和Cl-,其次为CO3^-2、HCO3^-,SO4^-2、K^+,矿化度平均为257.96g/L,卤水水化学类型为碳酸盐型;卤水组分与矿化度呈明显的正相关,表明卤水还未达到饱和阶段;受湖区构造及补给来源的影响,卤水的富集区位于研究区的西北部,同时也是矿化度最高的地区;KCl的含量在0.39%~0.99%之间,平均在0.65%,已超过液体钾盐矿的最低工业品位,分布面积约690km2,具有一定找矿前景。  相似文献   

8.
为探究溶解性有机质(DOM)不同相对分子质量组分对药物和个人护理品(PPCPs)类污染物吸附过程的影响,以卡马西平(CBZ)为目标污染物,以石英砂代表无机矿物,用商用腐殖酸(HA)制备DOM并进行超滤分级,然后开展吸附实验,并采用荧光光谱和红外光谱表征等手段,研究了DOM不同分子质量组分对石英砂吸附CBZ的影响及机制。结果表明,以3 000和10 000的超滤膜进行分级后的不同相对分子质量HA结构有明显差别,大分子质量HA中苯环等疏水性结构以及羟基的含量较多,芳香构造化程度高,多为分子量较高、稳定性较好的疏水性有机物,但中、小分子质量HA结构差异不大,含有更多羰基、羧基等含氧官能团,主要是一些分子质量较小的亲水物质; DOM不同分子质量组分对CBZ在石英砂上的吸附有明显影响,其中大分子质量组分促进吸附,而中、小分子质量组分抑制吸附,原因在于大分子质量组分可疏水结合于矿物表面,增加介质表面的活性吸附位点,同时其芳香性或脂肪性结构可与CBZ的疏水基团发生疏水作用共吸附或累积吸附于介质表面,从而促进CBZ的吸附;而中、小分子质量DOM的极性官能团可与CBZ酰胺部分通过极性作用结合,对CBZ分子有增溶作用,从而抑制吸附。  相似文献   

9.
薄膜吸附制样-波长色散X射线荧光光谱法测定卤水中的溴   总被引:2,自引:2,他引:0  
溴主要以离子形式分布在地壳水圈的溴化物型卤水、卤化物硫酸盐型卤水中,目前应用波长色散X射线荧光光谱(WDXRF)测定卤水中的溴,主要采用粉末载体压片法前处理待检样品,制样工作量大,制样均匀性和制样过程中的污染都会影响准确度,方法实用性不强。本文借助薄膜吸附前处理卤水样品,通过优化筛选薄膜材料及卤水取样量,确定移取50μL卤水样品滴于Ф=40 mm的3#层析滤纸的圆心位置,自然晾干后高压压平来前处理待检样品,采用人工配制标准样品校正溴的标准曲线,用WDXRF测定溴的含量。钾钠钙镁氯和硫酸根等共存离子的影响可以忽略,方法检出限(3σ)为0.95 mg/L,精密度(RSD,n=11)不大于0.8%,加标回收率为99.4%~101.2%。本方法操作简便,不需要使用化学试剂,解决了现行卤水中溴的分析方法流程复杂、分析成本高的问题。  相似文献   

10.
柴达木盆地西部卤水特征及成因探讨   总被引:15,自引:0,他引:15  
柴达木盆地自中生代末-新生代初以来,四周山体不断抬升,形成"高山深盆"的沉积环境,为盆地带来了大量盐类物质,再加上新近纪干旱封闭的气候环境,使得其西部沉积了广阔而厚层的岩盐.在对柴达木盆地西部新近系、第四系地层出露盐矿点实地考察的过程中,采集、分析了18件卤水样品的水化学组成.结果表明,卤水矿化度高,油田卤水富B3 、Li 、Sr2 和Br-等有益组分,其前缘第四纪形成的盐湖也有大量K 资源分布.通过离子含量及水化学特征系数,查明了卤水的水化学类型主要为氯化物型和硫酸镁亚型,地表浅层卤水富Mg2 、SO24-贫Ca2 ,而油田卤水富Ca2 ,贫Mg2 、SO24-.反映了油田卤水具有深部CaCl2型水体的特征,这种富Ca2 的卤水可能与白云岩化作用使卤水中的Ca2 增加而Mg2 减少,以及硫酸盐的还原作用使SO24-减少有关;地表浅层卤水接近青海湖湖水蒸发线,说明盆地卤水主要是由大气降水汇聚蒸发形成.通过卤水氢氧同位素的分析,发现卤水明显偏离于大气降水线,发生了明显的"氧同位素正漂移"现象,且卤水演化趋势线和当地大气降水线的交点与周围山体前缘的盐泉水的氢氧同位素值相近,地表浅层卤水主要分布在大气降水线附近,而油田卤水集中分布在变质水的范围内.说明地表浅层卤水主要是由大气降水汇聚而形成的;而深部油田卤水推测基本上来源于冰雪融水或雨水补给,这些冰雪融水或雨水沿着断裂带下渗,在迁移的途中发生了变质作用和深部地热水体掺杂作用,形成了深部油田卤水.  相似文献   

11.
Two organic rich sediments, an oxic muddy sand and a silty mud containing sulphate reducing and methane producing metabolic zones, were sampled from Loch Duich, a fjord type estuary in the N.W. coast of Scotland. Dissolved organic carbon (DOC), as measured by dry combustion and UV absorption, remained constant (8.3–15.8 mg C/l) with depth in the oxic pore waters at a concentration at least twice that of the overlying seawater. DOC in the anoxic pore waters increased linearly with depth from 13.6 at the surface to 55.9–70.5 mg C/l at 80cm. Most of the DOC was present in the high molecular weight (HMW) fraction as separated by ultrafiltration; the low molecular weight (LMW) fraction remained constant (10.0 mg C/l) in both oxic and anoxic pore waters. Spectroscopic data showed the ‘humic’ fraction of the HMW dissolved organic matter was mainly fulvic acid, a small proportion (approx 1%) of humic acid, and a third fraction, possibly melanoidins, which increased relative to fulvic acid with depth. These data confirm the pathway of humification (NissenBaum et al, 1971; nissenbaum and Kaplan, 1972) where HMW organic matter accumulates in pore waters as condensation products of LMW organic substances.  相似文献   

12.
The dominant phosphorus compound classes were characterized in marine samples using a new, high recovery method for isolating and concentrating bulk dissolved organic matter (DOM) called combined electrodialysis + reverse osmosis (ED/RO). In contrast to earlier studies that use ultrafiltration (UF) to recover only the high molecular weight DOM, ED/RO is capable of isolating both low molecular weight (LMW) and high molecular weight (HMW) DOM. Samples were collected from a broad range of marine environments: along a transect incorporating coastal and offshore waters off the Southeastern United States, in Effingham Inlet, a Pacific fjord located on Vancouver Island, British Columbia and in the Amundsen Sea, Antarctica. Results from phosphorus nuclear magnetic resonance (31P NMR) analysis reveal a similar abundance of P compound classes among samples, phosphate esters (80–85%), phosphonates (5–10%) and polyphosphates (8–13%). These samples contain significantly higher proportions of polyphosphate P and P esters and lower proportions of phosphonates than measured in previous studies using the UF method. The much higher levels of polyphosphate detected in our samples suggests that polyphosphate is present mainly in the LMW dissolved matter fraction. Polyphosphates in dissolved matter may be present as (or derived from) dissolved nucleotides or organismal polyphosphate bodies, or both. Low molecular weight P esters are possibly composed of phosphoamino acids and small carbohydrates, like simple sugar phosphates and/or dissolved nucleotides. Phosphonates in DOM are more prevalent as HMW phosphonate compounds, which suggests that LMW phosphonates are more readily utilized in marine ecosystems. Overall, the investigation of DOM across a size spectrum that includes both the HMW and the LMW fractions reveals a new picture of phosphorus distribution, cycling and bioavailability.  相似文献   

13.
We present a new stable isotope mass balance method for measuring the enhanced aqueous solubility of specific organic compounds in the presence of natural dissolved organic matter (DOM). It involves interfacing a standard dissolved organic carbon (DOC) analyzer with a stable isotope ratio monitoring system, is applicable to a wide range of model organic compounds and can be tuned to provide maximum precision for a given range of compound solubility and initial natural DOC concentration. Using 13C-labeled styrene as a model compound, we applied the method to investigate the reactivity of Dismal Swamp DOM as a function of season, nominal molecular size and chemical composition as determined using Fourier Transform Infrared Spectroscopy (FTIR). The solubility enhancement of styrene ranged from 23% to 118% relative to deionized water, while DOC-normalized enhancements varied from about 0.04 to 0.35 μM styrene/μM DOC as a function of season and nominal molecular weight. Statistical analysis of FTIR spectra reveals a strong positive correlation between the styrene concentration and the carboxyl content of the natural DOM. Reactivity differences between high molecular weight (HMW), low molecular weight (LMW) and total DOM samples are consistent with potential variations in their higher order structures.  相似文献   

14.
Here we report on the temporal changes in the composition of dissolved organic carbon (DOC) collected in the tidal freshwater region of the lower Mississippi River. Lignin-phenols, bulk stable carbon isotopes, compound-specific isotope analyses (CSIA) and 13C nuclear magnetic resonance (NMR) spectrometry were used to examine the composition of high molecular weight dissolved organic matter (HMW DOM) at one station in the lower river over 6 different flow regimes in 1998 and 1999. It was estimated that the annual input of DOC delivered to the Gulf of Mexico from the Mississippi River was of 3.1 × 10−3 Pg, which represents 1.2% of the total global input of DOC from rivers to the ocean. Average DOC and HMW DOC were 489 ±163 and 115 ± 47 μM, respectively. 13C-NMR spectra revealed considerably more aliphatic structures than aromatic carbons in HMW DOC. Lignin phenols were significantly 13C-depleted with respect to bulk HMW DOM indicating that C4 grass inputs to the HMW DOM were not significant. It is speculated that C4 organic matter in the river is not being converted (via microbial decay) to HMW DOM as readily as C3 organic matter is, because of the association of C4 organic matter with finer sediments. The predominantly aliphatic 13C NMR signature of HMW DOM suggests that autochthonous production in the river may be more important as a source of DOC than previously thought. Increases in nutrient loading and decreases in the suspended load (because of dams) in the Mississippi River, as well as other large rivers around the world, has resulted in significant changes in the sources and overall cycling of riverine DOC.  相似文献   

15.
In this work, we use Fourier transform infrared spectroscopy (FTIR) and nuclear magnetic resonance spectroscopy (13C NMR) data to quantify the changes of major chemical compound classes (carboxylic acid, amide, ester, aliphatic, aromatic and carbohydrate) in high molecular weight (HMW, >1 kDa) dissolved organic matter (DOM) isolated along a transect through the Elizabeth River/Chesapeake Bay system to the coastal Atlantic Ocean off Virginia, USA. Results show that carboxylic acids and aromatic compounds are lost along the transect, while HMW DOC becomes enriched in carbohydrate moieties that could have a mid-transect source, perhaps the intensive red tide bloom (Choclodinium polykrikoides) which occurred during our sampling period. Taking the second derivative of the FTIR spectra resolved three pools of de-protonated carboxylic acids at our Dismal Swamp site (used to represent terrestrial organic matter in this area): one carboxylic acid pool, complexed with iron, seems to be lost between the Dismal Swamp and river sites; the second appears biogeochemically active throughout the riverine transect, disappearing in the coastal ocean sample; the third seems refractory, with the potential to be transported to and to accumulate within the open ocean. Five-member ring esters (γ-lactones) were the major ester form in the Dismal Swamp; aliphatic and acetate esters were the dominant esters in the estuary/marine DOM. No amide groups were detectable in Dismal Swamp DOM; secondary amides were present at the estuarine/marine sites. Coupling FTIR with 13C NMR provides new insights into the biogeochemical roles of carboxylic acid, amide and ester compounds in aquatic ecosystems.  相似文献   

16.
In the present study, we explored the use of various optical parameters to detect differences in the composition of the dissolved organic matter (DOM) in a set of lakes that are all located on the Canadian Precambrian Shield, but within which Cu and Ni speciation predictions were previously shown to diverge from measured values in some lakes but not in others. Water samples were collected with in situ diffusion samplers in 2007 (N = 18 lakes) and 2008 (N = 8 lakes). Significant differences in DOM quality were identified between the sampling regions (Rouyn-Noranda, Québec and Sudbury, Ontario) and among lakes, based on dissolved organic carbon concentrations ([DOC]), specific UV absorbance (SUVA254), fluorescence indices (FI), and excitation–emission matrix (EEM) fluorescence measurements. Parallel factor analysis (PARAFAC) of the EEM spectra revealed four components, two of which (C3, oxidized quinone fluorophore of allochthonous origin, and C4, tryptophan-like protein fluorescence of autochthonous origin) showed the greatest inter-regional variation. The inter-lake differences in DOM quality were consistent with the regional watershed characteristics as determined from satellite imagery (e.g., watershed-to-lake surface area ratios and relative percentages of surface water, rock outcrops vegetative cover and urban development). Source apportionment plots, built upon PARAFAC components ratios calculated for our lakes, were used to discriminate among DOM sources and to compare them to sources identified in the literature. These results have implications for other areas of research, such as quantifying lake-to-lake variations in the influence of organic matter on the speciation of trace elements in natural aquatic environments.  相似文献   

17.
The environmental dynamics of dissolved organic matter (DOM) were characterized for a shallow, subtropical, seagrass-dominated estuarine bay, namely Florida Bay, USA. Large spatial and seasonal variations in DOM quantity and quality were assessed using dissolved organic C (DOC) measurements and spectrophotometric properties including excitation emission matrix (EEM) fluorescence with parallel factor analysis (PARAFAC). Surface water samples were collected monthly for 2 years across the bay. DOM characteristics were statistically different across the bay, and the bay was spatially characterized into four basins based on chemical characteristics of DOM as determined by EEM-PARAFAC. Differences between zones were explained based on hydrology, geomorphology, and primary productivity of the local seagrass community. In addition, potential disturbance effects from a very active hurricane season were identified. Although the overall seasonal patterns of DOM variations were not significantly affected on a bay-wide scale by this disturbance, enhanced freshwater delivery and associated P and DOM inputs (both quantity and quality) were suggested as potential drivers for the appearance of algal blooms in high impact areas. The application of EEM-PARAFAC proved to be ideally suited for studies requiring high sample throughput methods to assess spatial and temporal ecological drivers and to determine disturbance-induced impacts in aquatic ecosystems.  相似文献   

18.
Properties of fluorescent dissolved organic matter in the Gironde Estuary   总被引:5,自引:0,他引:5  
The isolation, characterization and study of the properties of aquatic dissolved organic matter (DOM) still represent a challenge because of the heterogeneity, complexity and low concentration of organic material in natural waters. Based on its ability to interact with contaminants and thus to modify their transport and bioavailability, DOM is of interest for environmental purposes. The objective of this work was to better characterize DOM in the Gironde Estuary (southwestern France). The estuary represents an exchange zone between the continent and the Atlantic Ocean and conditions the transfer of organic and inorganic substances from the continental to the oceanic environment. Several samples were collected along the estuary during three cruises in 2002 and 2006. They were analysed using excitation–emission matrix (EEM) spectroscopy, a sensitive technique that allows direct analysis of water samples. Fluorescent DOM and dissolved organic carbon (DOC) did not behave conservatively in this estuarine system, i.e. the organic material did not undergo simple dilution from the upstream to the downstream part of the estuary. A seasonal variability in DOC content was pointed out, whereas few seasonal variations in DOM fluorescence were observed. DOM sources and processing in the estuary were further evaluated by determining two fluorescence indices – the humification index (HIX) and the index of recent autochthonous contribution (BIX). By applying these indices, the relative degree of humification (HIX) and autotrophic productivity (BIX) could be assessed. Based on the fluorescence and DOC results, the estuary was divided into three zones depending on salinity (S) and characterized by specific DOM: (i) A turbid zone of low salinity (S < 5) and high suspended particulate matter concentration with increase in the intensities of the α′ and α fluorophores, characteristic of humic-like compounds. (ii) A mid-estuarine zone (5 < S < 25) characterized by low autotrophic productivity and containing strongly degraded organic material, as shown by the low values of BIX and high values of HIX. (iii) A higher salinity area (S > 25) characterized by increased autotrophic productivity and a marked marine influence, and associated with high and low values of BIX and HIX, respectively. The HIX and BIX indices were shown as useful tools for readily defining and classifying DOM characteristics in estuarine waters.  相似文献   

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