Characterization of Pu concentration and its isotopic composition in soils of Gansu in northwestern China

The total ^239+240Pu activities and ²⁴⁰Pu/²³⁹Pu atom ratios in surface soil samples (0–5 cm) in the Kumtag Desert in western Gansu Province, and in a soil core sample in Lanzhou were investigated using a sector-field ICP-MS. In the surface soil samples, ^239+240Pu activities in fine particles (<150 μm) were 1.3–2.1 times of those in coarse particles (150 μm–1 mm) which ranged from 0.005 to 0.157 mBq/g. Atom ratios of ²⁴⁰Pu/²³⁹Pu in the surface soils ranged from 0.168 to 0.192 with a mean of 0.182 ± 0.008. The mean ratio was similar to the typical global fallout value although the Kumtag Desert was believed to have received close-in fallout derived from Chinese nuclear weapons tests mainly conducted in the 1970s. Furthermore, the mean ²⁴⁰Pu/²³⁹Pu atom ratio observed in the soil core sample in Lanzhou was similar to the typical global fallout value. In the soil core sample, ^239+240Pu activities in the various layers ranged from 0.012 to 0.23 mBq/g, and the inventory of ^239+240Pu (32.4 Bq/m², 0–23 cm) was slightly lower than that expected from global fallout (42 Bq/m²) at the same latitude. Rapid downward migration of Pu isotopes was observed in Lanzhou soil core sample layers. The contribution of the 10-cm deep top layers of surface soils to total inventory was only 17%, while the contribution of deeper layers (10–23 cm) was as high as 83%. The ^239+240Pu activity levels and ²⁴⁰Pu/²³⁹Pu atom ratios in soils in Gansu Province, China are similar to those in atmospheric deposition samples collected in the spring in recent years in Japan.     

A rapid isotope ratio analysis protocol for nuclear solid materials using nano-second laser-ablation time-of-flight ICP-MS

The analysis of the isotopic composition of nuclear or non-nuclear solid materials is performed in a variety of fields, e.g., for quality assurance in the production of nuclear fuels, as signatures in forensics, nuclear safeguards, and non-proliferation control, in material characterization, geology, and archeology. We have investigated the capability of laser ablation (New Wave Research, 213 nm) coupled to time-of-flight (TOF) ICP-MS (GBC OptiMass 8000) as a rapid analytical protocol for multi-isotope screening of nuclear and non-nuclear solid samples. This includes natural and non-natural isotopic compositions for elements including Cu, Zr, Mo, Cd, In, Ba, Ta, W, Re, Pt, Pb, and U, in pure metals, alloys, and glasses. Without correcting for mass bias (mass fractionation), an overall precision and accuracy of about 4% (1σ) can be achieved by minimizing the deposited laser power and thus fractionation (mass removal based on thermal properties). The precision and accuracy in combination with literally no or minimized sample preparation enables a rapid isotope screening of solid samples that is of particular interest to support nuclear forensic and safeguard analysis.     

湖南长沙地区大气降水中稳定同位素特征变化

根据2010年1月~2011年2月长沙地区日降水中δD、δ18O资料,分析了该地区天气尺度下降水中δD、δ18O变化特征。结果表明:在天气尺度下长沙地区大气降水中δ18O与降水量、水汽压、温度及相对湿度之间存在显著的负相关关系,表明该地区降水中δ18O的变化具有显著的降水量效应、湿度效应及反温度效应。长沙地区的大气降水线为:δD=8.38δ18O+173〖WTBZ〗,该方程与GNIP（Globe Network of Isotopes in Precipitation）提供的长沙在月尺度下所得到的大气水线方程的斜率和截距相近,但斜率和截距都比GMWL(Globe Meteoric Water Line)偏大,说明该地区具有湿润多雨的气候特点。研究结果对揭示东亚季风区稳定同位素变化特征以及古气候的解释具有重要意义     

An alternative approach to reconstructing organic matter accumulation with contrasting watershed disturbance histories from lake sediments

A number of proxies, including carbon to nitrogen ratio (C:N) and stable isotopes (delta(13)C and delta(15)N), have been used to reconstruct organic matter (OM) profiles from lake sediments and these proxies individually or in combination cannot clearly discriminate different sources. Here we present an alternative approach to elucidate this problem from lake sediments as a function of watershed scale land use changes. Stable isotope signatures of defined OM sources from the study watersheds, Shawnigan Lake (SHL) and Elk Lake (ELL), were compared with sedimentary proxy records. Results from this study reveal that terrestrial inputs and catchment soil coinciding with the watershed disturbances histories probably contributed in recent trophic enrichment in SHL. In contrast, cultural eutrophication in ELL was partially a result of input from catchment soil (agricultural activities) with significant input from lake primary production as well. Results were consistent in both IsoSource (IsoSource version 1.2 is a Visual Basic program used for source separation, (http://www.epa.gov/wed/pages/models/isosource/isosource.htm) and discriminant analysis (statistical classification technique).     

Temporal changes in the distribution, methylation, and bioaccumulation of newly deposited mercury in an aquatic ecosystem

Our objective was to examine how the behavior of atmospheric mercury (Hg) deposited to boreal lake mesocosms changed over time. We added inorganic Hg enriched in a different stable isotope in each of two years, which allowed us to differentiate between Hg added in the first and second year. Although inorganic Hg and methylmercury (MeHg) continued to accumulate in sediments throughout the experiment, the availability of MeHg to the food web declined within one year. This decrease was detected in periphyton, zooplankton, and water mites, but not in gomphid larvae, amphipods, or fish. We suggest that reductions in atmospheric Hg deposition should lead to decreases in MeHg concentrations in biota, but that changes will be more easily detected in short-lived pelagic species than long-lived species associated with benthic food webs.     

改进沉淀法在溶解性无机碳稳定同位素测定中的应用研究

水体中溶解性无机碳(Dissolved inorganic carbon, DIC)的稳定碳同位素比值(δ¹³C_DIC)是揭示碳循环过程的重要技术指标。DIC的分离和富集是测定δ¹³C_DIC的基础,也是影响δ¹³C_DIC测定准确度的主要过程之一。沉淀法和气体法均为常用的DIC分离和富集方法。相比于气体法,沉淀法操作流程简单,适用性较强,在δ¹³C_DIC测定过程中具有广阔的应用前景。然而,基于沉淀法的DIC分离和富集过程中常存在碳稳定同位素分馏问题。为此,本研究在综合气体法和沉淀法优缺点的基础上,以超声时间,水浴温度和氮气吹扫速率为自变量,以δ¹³C_DIC的理论值与实测值之间绝对误差的最小化为目标,采用响应面法对传统NaOH-BaCl₂沉淀法进行了改进。基于改进沉淀法测定的δ¹³C_DIC理论值与实测值之间的...     

海相沉积岩铁同位素体系及其古环境指示

铁(Fe)作为主要造岩元素及生命必需元素,广泛参与地球表层圈层所涉及的物理、化学和生物作用,在调节海洋初级生产力和驱动海洋生物地球化学循环过程扮演重要角色.Fe同位素作为较早开发的非传统稳定同位素体系,目前已成为示踪生物地球化学循环过程及古海洋环境演变的有效手段.本文在对全球海洋Fe循环和表生地质过程Fe同位素分馏机理...     

南京春季北郊地区大气PM2.5中主要化学组分及碳同位素特征

PM_(2.5)是大气的重要污染物之一,其成分复杂,为研究PM_(2.5)的污染特征及来源,于2016年3月采集南京北郊地区大气中的PM_(2.5),利用Dinoex ICS-3000和ICS-2000型离子色谱和DRI Model 2001A热/光碳分析仪分别测定了PM_(2.5)中的阴阳离子和碳质组分,利用元素分析仪-同位素质谱仪测定大气PM_(2.5)中的总碳同位素(δ~(13)CTC)组成特征.结果表明,2016年3月期间南京北郊地区PM_(2.5)污染严重,平均浓度达(106.16±48.70)μg·m~(-3),且88%观测天中存在明显的二次有机污染,SOC平均浓度为(3.58±2.78)μg·m~(-3),且在晴天条件下高浓度的二次有机碳(SOC)与紫外线作用下的O_3具有较强的相关性.大气PM_(2.5)中δ~(13)CTC值范围是-26.56‰~-23.75‰,平均值为(-25.47‰±0.63‰),结合化学组分的三相聚类分析结果可知,大气PM_(2.5)主要来源于燃煤过程、机动车排放,此外还受地质源和生物质燃烧源的影响.     

碳同位素解析厌氧产酸过程挥发性有机酸来源

针对厌氧产酸条件下挥发性有机酸（VFAs）来源不明确及定向合成无依据的问题,基于同位素示踪技术对VFAs来源与合成比例进行研究.构建完全的厌氧产酸体系,采用牛血清蛋白、植物油和稳定同位素型葡萄糖（碳13丰度99%）作为反应底物,利用碳同位素示踪原理,定量分析VFAs的来源及其比例.结果表明：碳水化合物（碳13丰度99%）主要贡献偶数型短链脂肪酸的生成,其中对乙酸（HAc）和丁酸（HBu）的贡献率分别为77%和86%;而蛋白质（碳12）主要贡献奇数型短链脂肪酸的生成,其中对丙酸（HPr）和戊酸（HVa）的贡献率分别为85%和99%.通过改变发酵底物中碳水化合物和蛋白质比例,可以有效调节水解液中奇数型与偶数型短链脂肪酸的浓度和比例,为后期微生物合成高品质聚羟基脂肪酸酯（PHA）提供物质基础.     

北极楚科奇海、白令海上空大气气溶胶铅浓度及同位素研究

北极楚科奇海大气气溶胶中铅浓度为 0 1 7～ 0 96ng·m-3,平均值为 0 4 6± 0 2 7ng·m-3.气溶胶铅同位素地球化学示踪和铅的富集因子计算 ,揭示北极楚科奇海和白令海上空大气中的铅可能主要由两个端元组分混合而成 ,这两个端元一是来自北美如美国和加拿大具高同位素比值的工业释放铅 ,另一个是源于俄罗斯及其远东如立陶宛、乌克兰、阿塞拜疆、哈萨克斯坦、蒙古和亚洲如日本、韩国、中国和越南 .铅的总沉降通量计算表明 ,北极楚科奇海和白令海铅的入海通量平均值为 0 0 2mg·m-2 ·a-1 ,与南太平洋相当 ,略低于北印度洋和南大西洋 ,大大低于波罗的海、北海、地中海等近岸海域