利用铅同位素方法量化不同端元源对南京土壤和长江下游悬浮物铅富集的影响

环境中铅污染及其地球化学行为关系到生态环境安全和人类健康.利用地球化学同位素方法研究长江下游典型地区土壤和河流悬浮物中铅富集特征和成因,量化不同端元源对铅富集的影响,对于环境科学发展以及铅污染治理具有重要促进意义.结果表明,南京城区表层土壤和长江下游悬浮物中的铅相对于当地背景土壤呈现出富集特征.土壤和悬浮物的铅同位素相对于自然端元具有较高的206Pb/207Pb和较低的208Pb/206Pb比值,为受到了人为铅输入影响的缘故.铅同位素地球化学端元识别模型估算表明,南京市区土壤中的铅有18%~56%(平均35%)来自人为端元源,而长江下游悬浮物样品中铅的人为端元源贡献率为22%~46%(平均32%).     

长江源区降水氢氧稳定同位素特征及水汽来源

基于长江源区冬克玛底流域2014年5～10月连续采集的73个降水同位素数据,结合相关气象资料,分析了降水中δD、δ~(18)O及氘盈余(d-excess)变化特征,讨论了δ~(18)O与气温、降水量的关系,利用HYSPLIT模型追踪流域降水的水汽来源并估算不同水汽来源对降水量的贡献比例.结果表明:研究区降水中δ~(18)O和δD变化范围分别为-26.5‰～1.9‰和-195.2‰～34.0‰,且δ~(18)O和δD值随时间变化波动较大,与不同来源水汽输送有直接的关系;区域降水线的斜率和截距均大于全球大气降水线,与青藏高原北侧地区的降水线相近;不同降水类型中的δ~(18)O和δD的关系差异显著,主要与水汽来源和形成降水时的气象条件有关;由于受局地蒸发水汽及水汽输送过程影响,流域大气降水d-excess值整体上相对偏大;研究区的降水同位素存在显著的降水量效应,但不存在温度效应,表明降水量对大气降水中稳定同位素含量的控制作用更强;水汽来源轨迹表明,研究区大气降水水汽来源主要有西南季风携带的海洋性水汽、局地蒸发水汽及西风输送水汽,对降水量的贡献比例分别为43%、36%和21%.该研究结果有助于进一步了解长江源头区冬克玛底流域的大气环流特征及水循环过程.     

闪电河流域“三水”氢氧同位素特征及水体转换分析

通过采集闪电河流域2020年2月至2022年2月的降水与2021年的丰(8月)和枯(10月)水期的地表水和地下水,运用稳定同位素技术,对流域“三水”的氢氧稳定同位素进行时空变化分析,探讨水体同位素与环境因子的关系,结合HYSPLIT模型追踪大气水汽来源,利用端元混合模型揭示水体转换关系.结果发现,当地降水线的斜率和截距均小于当地大气降水线,水汽主要来自西风水汽、极地气团和东亚季风环流,降水同位素有显著的温度效应;时间上,地表水与地下水同位素在季节变化上均表现出枯水期较丰水期更富集,地表水与地下水d-excess值均低于全球平均值,显现出当地强烈的蒸发作用;空间上,地表水δ¹⁸O值丰枯季节在空间上具有相同的变化特征,呈现上游至下游逐渐富集,地下水δ¹⁸O高值区空间分布不均,地下水δ¹⁸O值随埋深的增加更加贫化;地下水水线斜率最高在丰水期为7.87,与当地大气降水线和地表水水线斜率十分接近,表明丰水期“三水”存在复杂的水力联系.研究区在丰水期地表水主要接受降水的补给,其次是接受地下水的径流补给.研究结果有助于明确闪电河流域同...     

岩溶流域地表水和地下水硝酸盐来源定量识别

选取岩溶地区花溪河流域典型农业区为研究对象,运用δ¹⁵N-NO₃^-,δ¹⁸O-NO₃^-和δ¹⁸O-H₂O同位素示踪技术和水化学分析方法,阐明了研究区地表水和地下水中硝酸盐的分布特征,并揭示其来源和形成过程,基于R语言下运行的贝叶斯模型（stable isotope analysis in R）,对研究区水体中各种硝酸盐来源的贡献比例进行了定量识别.结果显示：受碳酸岩盐风化的控制,流域内地表水和地下水的水化学类型以HCO₃-Ca型为主,硝酸盐在研究区水体中的空间分布特征受土地利用类型影响明显;在研究区水体硝酸盐形成过程中,硝化作用起主导作用,水体中的硝酸盐来源主要有化肥、降雨中的氨盐、土壤有机氮、粪便和污水,与地表水相比,地下水中硝酸盐受粪便和污水的影响较大;基于SIAR源解析模型分析,大气沉降、化肥、土壤有机氮和粪便污水对研究区地表水硝酸盐的贡献比例分别为3.97%、26.87%、36.80%和32.37%,对地下水硝酸盐的贡献比例分别为2.83%、13.96%、21.03%和62.18%.     

城镇生活污水处理厂出水硝酸盐浓度及同位素组成的影响因素

城镇生活污水是地表水硝酸盐(NO^-₃)的重要来源,但其NO^-₃浓度和同位素组成(δ¹⁵N-NO^-₃和δ¹⁸O-NO^-₃)仍不明确,特别是污水处理工艺对出水NO^-₃浓度、δ¹⁵N-NO^-₃和δ¹⁸O-NO^-₃影响仍不清楚.选择焦作市污水处理厂作为研究载体,每隔8 h收集污水厂进水、二沉池出水以及总排口出水样品,连续收集3 d,分析NH⁺₄浓度、 NO^-₃浓度以及δ¹⁵N-NO^-₃和δ¹⁸O-NO^-     

青海湖沙柳河流域不同时期地表水与地下水的相互作用

氢氧稳定同位素技术是研究地表水和地下水相互作用的有效手段。依据青海湖沙柳河流域2018年消融期、多雨期和冰冻期所收集的降水、河水和地下水样品中对氢氧同位素组成(δD、δ18O)的测定结果,识别和量化不同时期高山草原带和高山草甸带地表水和地下水间的补给关系和比例,其目的旨在明确高寒内陆河流域地表水和地下水δD和δ18O受降水影响的时空差异。结果表明:青海湖沙柳河流域地表水和地下水δD和δ18O值受降水响应存在时空差异性,δD和δ18O值在消融期受降水影响最强,冰冻期最弱;在高山草甸带δD和δ18O值受降水的影响强于高山草原带。消融期的高山草甸带、高山草原带和冰冻期的高山草原带地表水补给地下水的比例分别为80.65%、93.36%和89.44%;多雨期的高山草甸带、高山草原带和冰冻期的高山草甸带地下水补给地表水的比例分别为44.50%、74.85%和88.58%。研究结果可为该流域水资源优化配置和管理提供科学依据。     

Trophodynamics and distribution of silver in a Patagonia mountain lake

Silver (Ag) ions are among the most toxic metallic ions to aquatic biota. In southern Argentina, fish from Patagonian lakes have liver Ag concentrations [Ag] among the highest ever reported globally. Silver concentration in phytoplankton from Lake Moreno (1.82 ± 3.00 μg g⁻¹ dry weight, DW) was found to be significantly higher than [Ag] in zooplankton (0.25 ± 0.13 μg g⁻¹). Values in snails and decapods (0.60 ± 0.28 μg g⁻¹ and 0.47 ± 0.03 μg g⁻¹ respectively), were higher than in insect larvae (0.28 ± 0.39 μg g⁻¹ for Trichoptera). We examined trophic transfer of Ag in the biota using stable nitrogen and carbon isotopes ratios (δ¹⁵N and δ¹³C respectively). Silver concentrations in the biota of Lake Moreno were not associated with any particular C source, as assessed by δ¹³C. Hepatic [Ag] significantly increased with trophic position, as measured by δ¹⁵N, within the brook trout sample set. Biodilution of Ag was observed between primary producers and small forage fish when whole body [Ag] was analyzed. Nevertheless, when considering whole food web biomagnification and hepatic [Ag] of top predator fish, a significant positive regression was found between [Ag] and trophic position, as measured by δ¹⁵N. The importance of species-specific and tissue-specific considerations to obtain more information on Ag trophodynamics than that usually presented in the literature is shown. To the best of our knowledge, this is the first study in assessing Ag trophodynamics and tissue-specific biomagnification in a whole freshwater food web.     

The emergence of stable isotopes in environmental and forensic geochemistry studies: a review

In the past decade, environmental forensics has emerged as a discipline directed toward determining parties liable for causing spills of contaminants into the environment. Such investigations, while geared toward determining the guilty parties in order to recover costs of the cleanup and remediation, require various questions to be addressed. These include determination of the nature of the product; Where did it come from?; Extent of weathering, if any; How long has it been there?; and Is it degrading naturally? Traditionally, these studies have been addressed through utilization of techniques such as gas chromatography (GC) and gas chromatography–mass spectrometry (GCMS). However, in recent years, stable isotopes, primarily determined through the use of combined gas chromatography–isotope ratio mass spectrometry (GCIRMS), have emerged as an equally important tool in environmental forensics. For relatively low molecular, volatile compounds such as MTBE, BTEX, or chlorinated solvents, the isotopes, primarily carbon and hydrogen, have been used extensively for evaluating the onset of natural attenuation. For larger molecules such as PCBs or PAHs, in which the effects of biodegradation on the isotope composition of these molecules is minimal, the isotopic fingerprints of the individual compounds can be used for correlation purposes. In this paper, a brief introduction to isotope geochemistry will be given, followed by a review of applications of stable isotopes to a variety of environmental problems. While the review may not necessarily be exhaustive, it will provide a comprehensive overview of areas where isotopes have been used and potential applications for the future. Most of the review is concerned with carbon and hydrogen isotopes, although a brief overview of the emerging area of chlorine isotopes will also be discussed.     

Analytical model for site-specific isotope fractionation in 13C during sorption: determination by isotopic 13C NMR spectrometry with vanillin as model compound

The aim of this study was to conceive a reactive transport model capable of providing quantitative site-specific enrichment factors for fractionation in ¹³C isotopic content during sorption. As test compound the model treats vanillin, for which the ¹³C isotopic content at natural abundance at each of the 8 carbon positions can be measured by quantitative ¹³C nuclear magnetic resonance spectrometry. This technique determines the isotope ratios with a resolution better than ±1‰ (0.1%) at each carbon position. Site-specific isotope fractionations were recorded in chromatography column experiments with silica RP-18 as stationary phase. The one dimensional reactive transport model accounted for the sorption/desorption behavior of 8 individual ¹³C-isotopomers and one ¹²C-isotopomer of vanillin and reproduced satisfactorily the bulk (average over the whole compound) fractionation observed during elution. After model calibration, the enrichment factors were fitted for each carbon site where a significant fractionation was recorded. To show the interest of such a transport model for environmental studies, the model, extended to three dimensions, was exploited to simulate reactive transport in an aquifer. These results show that significant ¹³C isotope fractionation is expected for 4 out of 8 ¹³C-isotopomers in vanillin, and illustrate that bulk isotope ratios measured by conventional compound specific isotope analysis and mass spectrometry would hardly document significant isotope fractionations in vanillin. It is concluded that modeling of site-specific isotope ratios in molecules is a priori feasible and may help to quantify unknown processes in the environment.     

Nitrate Concentrations in Springs Flowing into the Lower Flint River Basin,Georgia U.S.A.1

Allums, Stephanie E., Stephen P. Opsahl, Stephen W. Golladay, David W. Hicks, and L. Mike Conner, 2012. Nitrate Concentrations in Springs Flowing Into the Lower Flint River Basin, Georgia U.S.A. Journal of the American Water Resources Association (JAWRA) 48(3): 423-438. DOI: 10.1111/j.1752-1688.2011.00624.x Abstract: Analysis of long-term data from (2001-2009) in four springs that discharge from the Upper Floridan aquifer into the Flint River (southwestern Georgia, United States) indicate aquifer and surface-water susceptibility to nutrient loading. Nitrate-N concentrations ranged from 1.74 to 3.30 mg/l, and exceeded historical levels reported for the Upper Floridan aquifer (0.26-1.52 mg/l). Statistical analyses suggest increasing nitrate-N concentration in groundwater discharging at the springs (n = 146 over eight years) and that nitrate-N concentration is influenced by a dynamic interaction between depth to groundwater (an indicator of regional hydrologic conditions) and land use. A one-time synoptic survey of 10 springs (6 springs in addition to the 4 previously mentioned) using stable isotopes generated δ¹⁵N-NO₃⁻ values (4.8-8.4‰ for rural springs and 7.7-13.4‰ for developed/urban springs) suggesting mixed sources (i.e., fertilizer, animal waste, and soil organic nitrogen) of nitrate-N to rural springs and predominantly animal/human waste to urban springs. These analyses indicate a direct relation between nitrate-N loading since the 1940s and intensification of agricultural and urban land use. This study demonstrates the importance of evaluating long-term impacts of land use on water quality in groundwater springs and in determining how rapidly these changes occur.