Studies on Lead Isotope Analysis and Composition in Soils and Near-surface Atmospheric Aerosols of the Ruoergai High Altitude Plateau, and Lead Sources Identification
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摘要: 若尔盖高原牧场处于中国偏远洁净高海拔地区，大气沉降是污染物主要来源途径之一。由于季风的影响，污染源的辨析较为困难。本文通过多点大气气溶胶不同季节同时采样方式，利用热电离固体同位素质谱仪可有效校正质谱分析中同位素分馏效应的优点，对若尔盖地区土壤和大气气溶胶的铅同位素比值进行精确分析，并结合季风特征对该地区污染物的来源进行解析。结果表明：土壤的 208Pb/204Pb比值变化范围为38.79059±0.00194~38.94461±0.00135，206Pb/207Pb为1.18551±0.00002~1.19362±0.00002；大气气溶胶的208Pb/204Pb比值变化范围为37.49571±0.00117~38.48980±0.00105，206Pb/207Pb为1.12894±0.00001~1.16734±0.00001。该地区土壤铅同位素的特征是放射成因铅高，来自于自身天然存在的岩石矿物，与大气污染关系不大；大气气溶胶的铅同位素组成与土壤差异较大，显示为多元混合模式，受到了天然物质和人类活动来源的混合影响，机动车尾气及来自北部（兰州）和西北部（青海、新疆、哈萨克斯坦、俄罗斯）的大气远程运移是若尔盖大气气溶胶及污染物质的主要来源。Abstract: The Ruoergai highland pasture is located in the remote, high altitude area of China. Atmospheric transport and precipitation is one of the major routes of pollutants to this area, but pollution source identification is difficult due to the monsoon. Atmospheric aerosol samples were taken in different seasons at multiple sites in Ruoergai. High precision Pb isotope analysis for soils and atmospheric aerosols was performed by using Thermal Ionization Mass Spectrometry (TIMS), which has the advantage of effectively removing the isotope fractionation effect in mass analysis. The sources of the aerosols were analyzed in association with the characteristics of the monsoon. The range of 208Pb/204Pb ratio is 38.79059±0.00194-38.94461±0.00135 and 206Pb/207Pb 1.18551±0.00002-1.19362±0.00002, 208Pb/204Pb in the atmo-spheric aerosol is 37.49571±0.00117-38.48980±0.00105 and 206Pb/207Pb 1.12894±0.00001-1.16734±0.00001. The Pb isotopic composition of soil in Ruoergai is characterized by high radiogenic Pb, mainly from local rock and minerals. The Pb isotopic composition of aerosols differs from that of soil, showing a multiple mode of mixing of natural and anthropogenic sources. Automobile exhaust gas and long-range atmospheric transport mainly from the north (Lanzou) and northwest (Qinghai, Xinjiang, Kazakhstan and Russia) are possible sources of aerosols and pollutants.
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图 3 若尔盖与中国西部(青海大气气溶胶和矿石，新疆矿石)、中亚(哈萨克斯坦矿石)、俄罗斯大气气溶胶和矿石、印度大气气溶胶样品中208Pb/207Pb和206Pb/207Pb比值的比较
Figure 3.
表 1 若尔盖地区土壤、大气气溶胶铅同位素组成(原子数比)及与兰州、成都比较
Table 1. Composition of lead isotope ratio (atomic ratio) of soil and aerosol in Ruoergai and data comparison with Lanzhou and Chengdu
样品类型 采样地点 采样季节 208Pb/204Pb 207Pb/204Pb 206Pb/204Pb 208Pb/207Pb 206Pb/207Pb 表层土壤 若尔盖 秋 38.79059±0.00194 15.65379±0.00073 18.55763±0.00080 2.478032±0.000028 1.18551±0.00002 表层土壤 若尔盖 秋 38.94461±0.00135 15.66181±0.00045 18.69384±0.00055 2.486597±0.000018 1.19362±0.00002 表层土壤 若尔盖 秋 38.83947±0.00139 15.64258±0.00046 18.60041±0.00067 2.482932±0.000019 1.18908±0.00003 表层土壤 若尔盖 秋 38.88189±0.00224 15.65591±0.00057 18.66972±0.00107 2.483530±0.000027 1.19255±0.00004 平均值 若尔盖 秋 38.86414±0.00173 15.65352±0.00055 18.63041±0.00077 2.482773±0.000023 1.19020±0.00003 汽车尾气 若尔盖 秋 37.34677±0.00225 15.55149±0.00085 17.4529±0.00094 2.401491±0.000034 1.12236±0.00005 大气 若尔盖 夏 37.77733±0.00357 15.57383±0.00122 18.00227±0.00138 2.419284±0.000018 1.15589±0.00002 大气 若尔盖 秋 37.49571±0.00117 15.49868±0.00046 17.49700±0.00046 2.425693±0.000051 1.12894±0.00001 大气 若尔盖 夏 37.76873±0.00263 15.57417±0.00099 17.99150±0.00110 2.425088±0.000039 1.15522±0.00002 大气 若尔盖 夏 37.78468±0.00211 15.57632±0.00089 18.01242±0.00097 2.425777±0.000033 1.15641±0.00001 大气 若尔盖 秋 38.48980±0.00105 15.64171±0.00039 18.25889±0.00042 2.460716±0.000015 1.16734±0.00001 大气 若尔盖 秋 38.38435±0.00099 15.63828±0.00038 18.23290±0.00042 2.454512±0.000014 1.16592±0.00001 平均值 若尔盖 - 37.95010±0.00192 15.58383±0.00072 17.99916±0.00079 2.435178±0.000028 1.15495±0.00001 大气 成都 夏 38.45013±0.00151 15.64558±0.00058 18.27440±0.00054 2.457571±0.000022 1.16803±0.00002 大气 成都 夏 38.44478±0.00147 15.63987±0.00037 18.25394±0.00059 2.458127±0.000018 1.16720±0.00003 大气 成都 夏 38.44479±0.00154 15.64533±0.00047 18.25746±0.00064 2.457269±0.000020 1.16694±0.00003 大气 成都 夏 38.50391±0.00143 15.65974±0.00040 18.31912±0.00072 2.458783±0.000018 1.16985±0.00005 大气 成都 夏 38.48133±0.00229 15.65578±0.00081 18.29963±0.00110 2.457963±0.000032 1.16891±0.00006 大气 成都 秋 38.46083±0.00288 15.64490±0.00092 18.31102±0.00121 2.458362±0.000039 1.17042±0.00006 大气 成都 秋 38.47638±0.00159 15.64845±0.00055 18.31136±0.00060 2.458798±0.000022 1.17019±0.00001 平均值 成都 - 38.46602±0.00182 15.64852±0.00059 18.28956±0.00077 2.458125±0.000025 1.16879±0.00004 大气 兰州 夏 37.56235±0.00305 15.50344±0.00049 17.52090±0.00142 2.422840±0.000036 1.13011±0.00008 大气 兰州 夏 36.68900±0.00172 15.48831±0.00077 16.93649±0.00082 2.368819±0.000029 1.09350±0.00002 大气 兰州 夏 37.57728±0.00127 15.50712±0.00048 17.52217±0.00051 2.423228±0.000019 1.12995±0.00001 大气 兰州 秋 37.33754±0.00086 15.47206±0.00036 17.31269±0.00036 2.413224±0.000014 1.11896±0.00001 大气 兰州 秋 37.73698±0.00133 15.53288±0.00050 17.71074±0.00060 2.429490±0.000020 1.14020±0.00001 大气 兰州 秋 37.50364±0.00107 15.50118±0.00035 17.50012±0.00047 2.419405±0.000015 1.12890±0.00001 平均值 兰州 - 37.40113±0.00155 15.50083±0.00049 17.41719±0.00070 2.412834±0.000022 1.12361±0.00002 
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