高精度铅同位素比值MC-ICP-MS测试方法及岩石标样铅同位素组成

卢山松, 童喜润, 谭娟娟, 邱啸飞, 杨红梅. 2023. 高精度铅同位素比值MC-ICP-MS测试方法及岩石标样铅同位素组成. 地质通报, 42(9): 1516-1530. doi: 10.12097/j.issn.1671-2552.2023.09.008
引用本文: 卢山松, 童喜润, 谭娟娟, 邱啸飞, 杨红梅. 2023. 高精度铅同位素比值MC-ICP-MS测试方法及岩石标样铅同位素组成. 地质通报, 42(9): 1516-1530. doi: 10.12097/j.issn.1671-2552.2023.09.008
LU Shansong, TONG Xirun, TAN Juanjuan, QIU Xiaofei, YANG Hongmei. 2023. High-precision analysis of Pb isotope ratios using MC-ICP-MS and the Pb isotope compositions of rock standard samples. Geological Bulletin of China, 42(9): 1516-1530. doi: 10.12097/j.issn.1671-2552.2023.09.008
Citation: LU Shansong, TONG Xirun, TAN Juanjuan, QIU Xiaofei, YANG Hongmei. 2023. High-precision analysis of Pb isotope ratios using MC-ICP-MS and the Pb isotope compositions of rock standard samples. Geological Bulletin of China, 42(9): 1516-1530. doi: 10.12097/j.issn.1671-2552.2023.09.008

高精度铅同位素比值MC-ICP-MS测试方法及岩石标样铅同位素组成

  • 基金项目:
    国家自然科学基金项目《北大别始太古代基底岩系的组成、地球化学特征及其对早期地壳演化的制约》(批准号:42272229)、国家自然科学基金青年基金项目《MC-ICP-MS高效准确测定Pb同位素标准参考物质绝对比值的分析方法研究》(批准号:42003017)、原国土资源部公益性行业专项《同位素地质样品分析方法行业标准(DZ/T0184.1~22—1997)修订》(编号:201411075)、古生物与地质环境演化湖北省重点实验室开放研究基金项目《鄂西神农架群碎屑锆石年龄特征及其对扬子北缘演化的制约》(编号:PEL-202205)、中国地质调查局花岗岩成岩成矿地质研究中心开放基金项目《磷灰石矿物包裹体微区原位Sr同位素组成精确测定及其对扬子克拉通太古宙花岗岩成因的制约》(编号:PM202302)
详细信息
    作者简介: 卢山松(1986-),男,硕士,高级工程师,从事同位素分析测试和地球化学示踪研究。E-mail: lushansong@mail.cgs.gov.cn
  • 中图分类号: P597+.3;P58

High-precision analysis of Pb isotope ratios using MC-ICP-MS and the Pb isotope compositions of rock standard samples

  • 利用多接收电感耦合等离子体质谱仪(Neptune plus)建立了高精度铅同位素比值MC-ICP-MS测试方法。建立该方法的过程中,重点评估了加入的Tl标准溶液对铅同位素比值测试结果的影响,并最终确定Tl标准溶液的浓度为25 ng/mL,同时样品溶液Pb的浓度应该大于25 ng/mL(即Pb/Tl浓度比应大于1)。利用该方法对铅同位素标准物质SRM 981进行了长期监控(2020年7月—2021年6月),测试结果为:206Pb/204Pb=16.9415±0.0010、207Pb/204Pb=15.4985±0.0009、208Pb/204Pb=36.7204±0.0023,与统计的文献报道值一致。长期监控的全流程空白均小于0.25 ng,能满足地质样品高精度铅同位素比值测试的需要。同时运用该方法,对4个元素含量标样(BCR-2、AGV-2、BHVO-2和BIR-1a)进行了铅同位素比值测试,测试结果与文献报道的测试结果和精度一致,表明建立的方法是准确、可靠的。

  • 加载中
  • 图 1  标准物质SRM 981(不同浓度Tl标准溶液及不同Pb/Tl值)铅同位素比值测试结果

    Figure 1. 

    图 2  标准物质SRM 981铅同位素比值长期测试结果(2020年7月—2021年6月)

    Figure 2. 

    表 1  样品的化学分离流程

    Table 1.  Chemical procedure for lead separation

    步骤 用量 备注
    6 mol/L HCl和超纯水交替淋洗 每次各10 mL,3次 清洗树脂
    1mol/L HBr+2 mol/L HCl 2 mL 平衡树脂
    1mol/L HBr+2 mol/L HCl 4 mL 上样
    0.3 mol/L HBr 8 mL,2次 淋洗杂质
    0.5 mol/L HCl 3mL 转换体系
    6 mol/L HCl 7 mL 解吸Pb
    下载: 导出CSV

    表 2  MC-ICP-MS的仪器参数设置

    Table 2.  MC-ICP-MS operation conditions

    名称 具体描述
    仪器型号 Thermo Fisher Scientific,Neptune plus
    高频发生器功率 约1200 W
    冷却气 16 L/min
    辅助气 0.8 L/min
    样品气 约1 L/min
    分辨率 低分辨
    Ni锥(标准采样锥+H截取锥)
    接收器法拉第杯;L3(202Hg),L2(203Tl),L1(204Pb),C(205Tl),H1(206Pb),H2(207Pb),H3(208Pb)
    灵敏度 208Pb: 10~12 V(Pb标准溶液的浓度为200 ng/mL)
    下载: 导出CSV

    表 3  标准物质SRM 981(不同浓度Tl标准溶液及不同Pb/Tl值)铅同位素比值测试结果

    Table 3.  Pb isotope ratios of SRM 981 with different concentrations of Tl standard solution and Pb/Tl ratio

    Tl/(ng·mL-1) Pb/(ng·mL-1) Pb/Tl 206Pb/204Pb 207Pb/204Pb 208Pb/204Pb
    15 300 20 16.9418 0.0002 15.4992 0.0003 36.7229 0.0008
    30 300 10 16.9416 0.0002 15.4991 0.0005 36.7227 0.0010
    60 300 5 16.9408 0.0003 15.4984 0.0003 36.7208 0.0010
    150 300 2 16.9398 0.0002 15.4976 0.0002 36.7190 0.0006
    300 300 1 16.9379 0.0003 15.4958 0.0003 36.7146 0.0006
    10 200 20 16.9410 0.0003 15.4988 0.0003 36.7210 0.0012
    20 200 10 16.9417 0.0005 15.4990 0.0004 36.7221 0.0011
    40 200 5 16.9406 0.0003 15.4981 0.0002 36.7196 0.0010
    100 200 2 16.9405 0.0004 15.4981 0.0005 36.7204 0.0010
    200 200 1 16.9400 0.0005 15.4977 0.0004 36.7192 0.0011
    400 200 0.5 16.9341 0.0005 15.4918 0.0005 36.7054 0.0012
    5 100 20 16.9427 0.0006 15.5006 0.0006 36.7261 0.0019
    10 100 10 16.9414 0.0007 15.4993 0.0007 36.7217 0.0010
    20 100 5 16.9412 0.0002 15.4991 0.0003 36.7218 0.0006
    50 100 2 16.9404 0.0005 15.4979 0.0004 36.7206 0.0008
    100 100 1 16.9386 0.0009 15.4963 0.0007 36.7160 0.0016
    200 100 0.5 16.9337 0.0008 15.4915 0.0006 36.7050 0.0017
    500 100 0.2 16.9204 0.0016 15.4789 0.0015 36.6751 0.0035
    2.5 50 20 16.9419 0.0010 15.4996 0.0015 36.7242 0.0046
    5 50 10 16.9425 0.0006 15.5003 0.0006 36.7269 0.0014
    10 50 5 16.9416 0.0005 15.4993 0.0005 36.7229 0.0017
    25 50 2 16.9405 0.0006 15.4980 0.0006 36.7191 0.0014
    50 50 1 16.9386 0.0008 15.4962 0.0007 36.7155 0.0016
    100 50 0.5 16.9351 0.0008 15.4930 0.0007 36.7075 0.0020
    250 50 0.2 16.9231 0.0015 15.4816 0.0016 36.6813 0.0033
    500 50 0.1 16.9012 0.0029 15.4614 0.0027 36.6330 0.0060
    1 20 20 16.9417 0.0033 15.5003 0.0035 36.7267 0.0098
    2 20 10 16.9428 0.0024 15.5009 0.0023 36.7263 0.0071
    4 20 5 16.9422 0.0030 15.4998 0.0030 36.7245 0.0079
    10 20 2 16.9376 0.0011 15.4950 0.0011 36.7139 0.0030
    20 20 1 16.9371 0.0025 15.4949 0.0024 36.7122 0.0056
    40 20 0.5 16.9341 0.0032 15.4923 0.0028 36.7048 0.0067
    100 20 0.2 16.9233 0.0035 15.4813 0.0035 36.6816 0.0084
    200 20 0.1 16.9028 0.0035 15.4630 0.0029 36.6369 0.0073
    0.5 10 20 16.9357 0.0014 15.4980 0.0047 36.7209 0.0137
    1 10 10 16.9434 0.0049 15.5034 0.0048 36.7363 0.0128
    2 10 5 16.9374 0.0021 15.4970 0.0022 36.7164 0.0067
    5 10 2 16.9394 0.0005 15.4957 0.0010 36.7185 0.0011
    10 10 1 16.9329 0.0045 15.4906 0.0045 36.7033 0.0113
    20 10 0.5 16.9354 0.0008 15.4943 0.0008 36.7112 0.0023
    50 10 0.2 16.9214 0.0037 15.4793 0.0032 36.6783 0.0087
    100 10 0.1 16.9108 0.0049 15.4694 0.0046 36.6518 0.0099
    0.25 5 20 16.9370 0.0089 15.4921 0.0087 36.7070 0.0234
    0.5 5 10 16.9544 0.0105 15.5105 0.0108 36.7508 0.0286
    1 5 5 16.9376 0.0052 15.4940 0.0049 36.7079 0.0118
    2.5 5 2 16.9410 0.0060 15.4976 0.0059 36.7197 0.0125
    5 5 1 16.9408 0.0048 15.4966 0.0040 36.7155 0.0093
    10 5 0.5 16.9340 0.0100 15.4913 0.0094 36.7043 0.0222
    25 5 0.2 16.9211 0.0038 15.4786 0.0032 36.6769 0.0074
    50 5 0.1 16.9150 0.0069 15.4737 0.0068 36.6591 0.0162
    Tl/(ng·mL-1) Pb/(ng·mL-1) Pb/Tl 208Pb/206Pb 207Pb/206Pb 204Pb/206Pb
    15 300 20 2.16757 0.00003 0.914848 0.000008 0.059025 0.000001
    30 300 10 2.16762 0.00002 0.914873 0.000004 0.059026 0.000001
    60 300 5 2.16758 0.00003 0.914858 0.000003 0.059029 0.000001
    150 300 2 2.16760 0.00002 0.914865 0.000007 0.059032 0.000001
    300 300 1 2.16760 0.00002 0.914861 0.000001 0.059039 0.000001
    10 200 20 2.16754 0.00005 0.914855 0.000005 0.059028 0.000001
    20 200 10 2.16756 0.00002 0.914852 0.000007 0.059026 0.000002
    40 200 5 2.16753 0.00002 0.914849 0.000007 0.059030 0.000001
    100 200 2 2.16761 0.00002 0.914858 0.000007 0.059030 0.000002
    200 200 1 2.16761 0.00002 0.914860 0.000005 0.059032 0.000002
    400 200 0.5 2.16757 0.00002 0.914847 0.000004 0.059052 0.000002
    5 100 20 2.16757 0.00001 0.914860 0.000008 0.059023 0.000002
    10 100 10 2.16763 0.00006 0.914854 0.000015 0.059027 0.000003
    20 100 5 2.16761 0.00003 0.914866 0.000007 0.059028 0.000001
    50 100 2 2.16763 0.00005 0.914863 0.000009 0.059031 0.000002
    100 100 1 2.16763 0.00002 0.914855 0.000007 0.059037 0.000003
    200 100 0.5 2.16758 0.00002 0.914843 0.000006 0.059054 0.000003
    500 100 0.2 2.16751 0.00001 0.914824 0.000009 0.059100 0.000006
    2.5 50 20 2.16751 0.00009 0.914837 0.000017 0.059025 0.000004
    5 50 10 2.16773 0.00002 0.914875 0.000005 0.059023 0.000002
    10 50 5 2.16759 0.00004 0.914876 0.000010 0.059026 0.000002
    25 50 2 2.16757 0.00004 0.914841 0.000010 0.059030 0.000002
    50 50 1 2.16759 0.00003 0.914856 0.000013 0.059037 0.000003
    100 50 0.5 2.16758 0.00003 0.914850 0.000009 0.059049 0.000003
    250 50 0.2 2.16752 0.00001 0.914827 0.000009 0.059091 0.000005
    500 50 0.1 2.16745 0.00002 0.914795 0.000016 0.059167 0.000010
    1 20 20 2.16779 0.00016 0.914909 0.000035 0.059026 0.000011
    2 20 10 2.16763 0.00012 0.914871 0.000037 0.059022 0.000008
    4 20 5 2.16766 0.00008 0.914857 0.000016 0.059024 0.000010
    10 20 2 2.16764 0.00006 0.914846 0.000019 0.059040 0.000004
    20 20 1 2.16758 0.00004 0.914873 0.000026 0.059042 0.000009
    40 20 0.5 2.16757 0.00002 0.914851 0.000021 0.059053 0.000011
    100 20 0.2 2.16751 0.00002 0.914806 0.000013 0.059090 0.000012
    200 20 0.1 2.16745 0.00003 0.914794 0.000016 0.059162 0.000012
    0.5 10 20 2.16756 0.00034 0.914829 0.000087 0.059047 0.000005
    1 10 10 2.16792 0.00022 0.914894 0.000047 0.059020 0.000017
    2 10 5 2.16789 0.00015 0.914916 0.000035 0.059041 0.000007
    5 10 2 2.16757 0.00007 0.914849 0.000020 0.059034 0.000002
    10 10 1 2.16757 0.00007 0.914904 0.000024 0.059057 0.000016
    20 10 0.5 2.16758 0.00002 0.914892 0.000023 0.059048 0.000003
    50 10 0.2 2.16755 0.00006 0.914799 0.000029 0.059097 0.000013
    100 10 0.1 2.16746 0.00004 0.914762 0.000019 0.059134 0.000017
    0.25 5 20 2.16709 0.00081 0.914668 0.000179 0.059043 0.000031
    0.5 5 10 2.16775 0.00037 0.914836 0.000097 0.058982 0.000037
    1 5 5 2.16724 0.00023 0.914781 0.000053 0.059041 0.000018
    2.5 5 2 2.16755 0.00015 0.914834 0.000045 0.059029 0.000021
    5 5 1 2.16746 0.00008 0.914793 0.000019 0.059029 0.000017
    10 5 0.5 2.16749 0.00009 0.914806 0.000042 0.059053 0.000035
    25 5 0.2 2.16731 0.00003 0.914729 0.000039 0.059098 0.000013
    50 5 0.1 2.16729 0.00005 0.914801 0.000051 0.059120 0.000024
    下载: 导出CSV

    表 4  不同实验室标准物质SRM 981铅同位素比值测试结果比对

    Table 4.  Comparison of Pb isotope ratios of SRM 981 with different methods in different laboratories

    数据来源 测试方法 测试仪器 206Pb/204Pb 207Pb/204Pb 208Pb/204Pb 207Pb/206Pb 208Pb/206Pb
    推荐值 16.9371 15.4913 36.7213 0.91464 0.00033 2.1681 0.0008
    何学贤等,2005 Tl内标 MC-ICP-MS 16.9402 0.0007 15.4966 0.0030 36.7155 0.0012 0.91478 0.00018 2.1674 0.0004
    Taylor et al., 2015 长期统计结果 16.9412 15.4988 36.7233
    Yuan et al., 2016 长期统计结果 16.9406 0.0003 15.4957 0.0002 36.7184 0.0007
    Galer et al., 1998 三稀释剂 TIMS 16.9405 0.0015 15.4963 0.0016 36.7219 0.0044 0.91475 0.00004 2.16771 0.00010
    Thirlwall, 2002 双稀释剂 TIMS 16.9408 0.0021 15.4980 0.0025 36.7220 0.0080 0.91483 0.00007 2.16767 0.00041
    Thirlwall, 2002 双稀释剂 MC-ICP-MS 16.9417 0.0029 15.4996 0.0031 36.7240 0.0080 0.91488 0.00008 2.16770 0.00024
    Kuritani et al., 2003 双稀释剂 TIMS 16.9414 0.0028 15.4992 0.0029 36.7230 0.0075 0.91487 0.00005 2.16765 0.00018
    Bake et al., 2004 双稀释剂 MC-ICP-MS 16.9416 0.0013 15.5000 0.0015 36.7262 0.0031 0.91491 0.00004 2.16781 0.00012
    Amelin et al., 2006 双稀释剂 TIMS 16.9408 0.0012 15.4987 0.0011 36.7278 0.0029 0.91483 0.00005 2.16741 0.00016
    Makishima et al., 2007 双稀释剂 MC-ICP-MS 16.9417 0.0024 15.4988 0.0025 36.7196 0.0066 0.91483 0.00005 2.16741 0.00016
    Makishima et al., 2010 双稀释剂 MC-ICP-MS 16.9415 0.0030 15.4991 0.0034 36.7233 0.0077 0.91486 0.00005 2.16766 0.00019
    Hoernle et al., 2011 双稀释剂 TIMS 16.9416 0.0024 15.4998 0.0024 36.7231 0.0063 0.91490 0.00005 2.16763 0.00019
    刘希君等, 2013 双稀释剂 TIMS 16.9408 0.0034 15.4953 0.0046 36.7178 0.0100
    本文 Tl内标 MC-ICP-MS 16.9415 0.0010 15.4985 0.0009 36.7204 0.0023 0.914829 0.000023 2.16749 0.00008
    测试平均值 16.9411 0.0010 15.4981 0.0032 36.7220 0.0068 0.914844 0.000102 2.16761 0.00029
    下载: 导出CSV

    表 5  2020年7月—2021年6月标准物质SRM 981铅同位素比值测试结果

    Table 5.  Pb isotope ratios of reference material SRM 981 from July 2020 to June 2021

    序号 206Pb/204Pb 207Pb/204Pb 208Pb/204Pb 208Pb/206Pb 207Pb/206Pb
    1 16.9406 0.0005 15.4979 0.0004 36.7192 0.0015 2.16752 0.00003 0.914839 0.000007
    2 16.9405 0.0002 15.4979 0.0003 36.7191 0.0010 2.16753 0.00002 0.914841 0.000009
    3 16.9412 0.0004 15.4985 0.0004 36.7207 0.0011 2.16755 0.00002 0.914847 0.000006
    4 16.9415 0.0002 15.4990 0.0002 36.7226 0.0007 2.16760 0.00002 0.914852 0.000007
    5 16.9411 0.0004 15.4985 0.0004 36.7210 0.0011 2.16754 0.00002 0.914831 0.000005
    6 16.9406 0.0002 15.4979 0.0003 36.7197 0.0007 2.16755 0.00002 0.914844 0.000005
    7 16.9402 0.0004 15.4974 0.0004 36.7175 0.0013 2.16750 0.00003 0.914836 0.000007
    8 16.9413 0.0002 15.4987 0.0002 36.7215 0.0005 2.16758 0.00002 0.914849 0.000008
    9 16.9415 0.0003 15.4987 0.0003 36.7213 0.0008 2.16752 0.00003 0.914829 0.000006
    10 16.9412 0.0004 15.4984 0.0003 36.7200 0.0009 2.16747 0.00001 0.914832 0.000004
    11 16.9412 0.0004 15.4982 0.0003 36.7195 0.0009 2.16747 0.00001 0.914825 0.000007
    12 16.9409 0.0002 15.4979 0.0002 36.7181 0.0007 2.16746 0.00003 0.914824 0.000005
    13 16.9408 0.0003 15.4977 0.0002 36.7187 0.0006 2.16747 0.00001 0.914818 0.000007
    14 16.9407 0.0004 15.4980 0.0003 36.7188 0.0009 2.16749 0.00003 0.914834 0.000007
    15 16.9411 0.0003 15.4983 0.0003 36.7196 0.0006 2.16749 0.00002 0.914829 0.000004
    16 16.9420 0.0004 15.4992 0.0004 36.7221 0.0011 2.16752 0.00003 0.914842 0.000006
    17 16.9422 0.0004 15.4993 0.0003 36.7220 0.0006 2.16751 0.00002 0.914841 0.000008
    18 16.9419 0.0004 15.4991 0.0003 36.7218 0.0010 2.16750 0.00002 0.914831 0.000009
    19 16.9423 0.0002 15.4992 0.0003 36.7222 0.0009 2.16749 0.00002 0.914839 0.000003
    20 16.9410 0.0004 15.4982 0.0004 36.7195 0.0009 2.16751 0.00002 0.914834 0.000006
    21 16.9419 0.0004 15.4985 0.0003 36.7213 0.0011 2.16745 0.00004 0.914814 0.000013
    22 16.9423 0.0001 15.4992 0.0003 36.7214 0.0008 2.16749 0.00002 0.914839 0.000004
    23 16.9412 0.0002 15.4984 0.0002 36.7200 0.0007 2.16749 0.00002 0.914834 0.000003
    24 16.9409 0.0005 15.4980 0.0005 36.7189 0.0013 2.16747 0.00002 0.914828 0.000004
    25 16.9408 0.0003 15.4979 0.0003 36.7186 0.0006 2.16750 0.00002 0.914830 0.000006
    26 16.9410 0.0003 15.4982 0.0004 36.7194 0.0011 2.16752 0.00002 0.914836 0.000010
    27 16.9409 0.0004 15.4980 0.0004 36.7191 0.0008 2.16747 0.00001 0.914826 0.000006
    28 16.9406 0.0003 15.4979 0.0003 36.7188 0.0008 2.16750 0.00003 0.914829 0.000005
    29 16.9408 0.0002 15.4980 0.0002 36.7193 0.0004 2.16749 0.00001 0.914836 0.000003
    30 16.9415 0.0005 15.4987 0.0004 36.7204 0.0006 2.16753 0.00001 0.914844 0.000005
    31 16.9419 0.0002 15.4991 0.0002 36.7221 0.0007 2.16751 0.00001 0.914836 0.000005
    32 16.9420 0.0005 15.4985 0.0002 36.7200 0.0006 2.16747 0.00001 0.914830 0.000007
    33 16.9419 0.0005 15.4993 0.0005 36.7223 0.0013 2.16755 0.00002 0.914849 0.000005
    34 16.9419 0.0003 15.4991 0.0003 36.7217 0.0010 2.16751 0.00002 0.914839 0.000006
    35 16.9417 0.0003 15.4990 0.0003 36.7218 0.0006 2.16755 0.00002 0.914848 0.000006
    36 16.9415 0.0003 15.4991 0.0002 36.7217 0.0006 2.16753 0.00001 0.914854 0.000003
    37 16.9417 0.0004 15.4989 0.0003 36.7213 0.0009 2.16752 0.00002 0.914839 0.000004
    38 16.9414 0.0003 15.4986 0.0003 36.7204 0.0008 2.16748 0.00002 0.914838 0.000009
    39 16.9418 0.0003 15.4990 0.0003 36.7213 0.0007 2.16749 0.00002 0.914832 0.000005
    40 16.9418 0.0004 15.4989 0.0005 36.7216 0.0012 2.16752 0.00002 0.914834 0.000005
    41 16.9424 0.0003 15.4997 0.0002 36.7232 0.0005 2.16752 0.00001 0.914851 0.000004
    42 16.9417 0.0003 15.4988 0.0004 36.7214 0.0009 2.16751 0.00003 0.914833 0.000007
    43 16.9417 0.0003 15.4987 0.0003 36.7203 0.0007 2.16745 0.00002 0.914826 0.000003
    44 16.9421 0.0004 15.4991 0.0004 36.7212 0.0013 2.16747 0.00004 0.914821 0.000008
    45 16.9424 0.0004 15.4993 0.0004 36.7225 0.0011 2.16749 0.00002 0.914821 0.000009
    46 16.9420 0.0004 15.4987 0.0004 36.7209 0.0012 2.16747 0.00002 0.914826 0.000006
    47 16.9424 0.0004 15.4990 0.0003 36.7218 0.0009 2.16748 0.00002 0.914814 0.000005
    48 16.9419 0.0003 15.4987 0.0003 36.7210 0.0008 2.16749 0.00002 0.914814 0.000008
    49 16.9422 0.0004 15.4992 0.0004 36.7223 0.0009 2.16750 0.00002 0.914823 0.000007
    50 16.9416 0.0001 15.4985 0.0002 36.7213 0.0003 2.16750 0.00002 0.914825 0.000004
    51 16.9419 0.0004 15.4989 0.0005 36.7220 0.0011 2.16754 0.00002 0.914829 0.000007
    52 16.9421 0.0003 15.4992 0.0003 36.7224 0.0009 2.16752 0.00003 0.914828 0.000009
    53 16.9419 0.0004 15.4989 0.0005 36.7215 0.0009 2.16749 0.00002 0.914832 0.000009
    54 16.9413 0.0004 15.4984 0.0004 36.7196 0.0010 2.16746 0.00002 0.914825 0.000006
    55 16.9411 0.0002 15.4981 0.0001 36.7189 0.0006 2.16744 0.00001 0.914822 0.000006
    56 16.9414 0.0006 15.4981 0.0004 36.7192 0.0012 2.16742 0.00002 0.914815 0.000003
    57 16.9414 0.0003 15.4983 0.0004 36.7189 0.0011 2.16744 0.00002 0.914826 0.000007
    58 16.9412 0.0003 15.4985 0.0002 36.7214 0.0008 2.16759 0.00001 0.914841 0.000005
    59 16.9412 0.0003 15.4983 0.0003 36.7204 0.0010 2.16754 0.00003 0.914831 0.000009
    60 16.9415 0.0002 15.4989 0.0003 36.7212 0.0008 2.16751 0.00003 0.914848 0.000006
    61 16.9416 0.0004 15.4986 0.0004 36.7203 0.0009 2.16746 0.00001 0.914828 0.000008
    62 16.9410 0.0003 15.4982 0.0004 36.7198 0.0011 2.16753 0.00002 0.914836 0.000002
    63 16.9417 0.0002 15.4988 0.0002 36.7218 0.0005 2.16753 0.00003 0.914836 0.000010
    64 16.9416 0.0003 15.4989 0.0003 36.7215 0.0005 2.16752 0.00001 0.914845 0.000004
    65 16.9411 0.0003 15.4985 0.0003 36.7212 0.0006 2.16757 0.00002 0.914841 0.000007
    66 16.9416 0.0003 15.4987 0.0003 36.7210 0.0008 2.16751 0.00002 0.914835 0.000007
    67 16.9414 0.0003 15.4987 0.0003 36.7207 0.0007 2.16749 0.00001 0.914829 0.000004
    68 16.9414 0.0003 15.4984 0.0003 36.7195 0.0010 2.16749 0.00003 0.914835 0.000010
    69 16.9410 0.0001 15.4981 0.0002 36.7203 0.0002 2.16749 0.00002 0.914819 0.000004
    70 16.9412 0.0007 15.4980 0.0004 36.7195 0.0011 2.16748 0.00002 0.914838 0.000006
    71 16.9418 0.0005 15.4987 0.0004 36.7202 0.0010 2.16749 0.00002 0.914827 0.000010
    72 16.9413 0.0004 15.4985 0.0004 36.7209 0.0011 2.16752 0.00002 0.914840 0.000007
    73 16.9409 0.0002 15.4982 0.0002 36.7192 0.0006 2.16747 0.00001 0.914839 0.000004
    74 16.9408 0.0001 15.4981 0.0002 36.7187 0.0007 2.16744 0.00002 0.914824 0.000005
    75 16.9420 0.0004 15.4990 0.0004 36.7209 0.0012 2.16745 0.00002 0.914823 0.000005
    76 16.9411 0.0003 15.4982 0.0002 36.7188 0.0007 2.16742 0.00002 0.914820 0.000007
    77 16.9418 0.0005 15.4989 0.0004 36.7206 0.0009 2.16745 0.00004 0.914829 0.000010
    78 16.9411 0.0002 15.4982 0.0003 36.7187 0.0008 2.16742 0.00002 0.914834 0.000006
    79 16.9424 0.0004 15.4992 0.0003 36.7219 0.0008 2.16745 0.00002 0.914819 0.000014
    80 16.9422 0.0002 15.4989 0.0003 36.7211 0.0007 2.16742 0.00003 0.914812 0.000013
    81 16.9416 0.0002 15.4983 0.0002 36.7202 0.0005 2.16744 0.00003 0.914797 0.000008
    82 16.9422 0.0004 15.4991 0.0004 36.7210 0.0011 2.16743 0.00002 0.914822 0.000006
    83 16.9421 0.0002 15.4989 0.0002 36.7207 0.0007 2.16743 0.00002 0.914823 0.000003
    84 16.9419 0.0004 15.4985 0.0003 36.7197 0.0009 2.16738 0.00002 0.914803 0.000005
    85 16.9413 0.0002 15.4979 0.0002 36.7188 0.0006 2.16740 0.00003 0.914802 0.000007
    86 16.9420 0.0002 15.4987 0.0002 36.7207 0.0006 2.16744 0.00002 0.914808 0.000009
    87 16.9414 0.0007 15.4980 0.0004 36.7193 0.0014 2.16743 0.00003 0.914815 0.000011
    88 16.9418 0.0004 15.4986 0.0003 36.7207 0.0010 2.16743 0.00002 0.914813 0.000008
    89 16.9411 0.0003 15.4982 0.0003 36.7193 0.0005 2.16745 0.00001 0.914825 0.000007
    90 16.9418 0.0003 15.4986 0.0003 36.7201 0.0008 2.16744 0.00002 0.914817 0.000007
    91 16.9415 0.0003 15.4983 0.0002 36.7200 0.0009 2.16747 0.00003 0.914837 0.000006
    92 16.9422 0.0002 15.4991 0.0002 36.7211 0.0008 2.16741 0.00002 0.914815 0.000004
    93 16.9421 0.0002 15.4986 0.0002 36.7206 0.0002 2.16743 0.00001 0.914800 0.000003
    94 16.9424 0.0004 15.4988 0.0003 36.7214 0.0011 2.16746 0.00002 0.914804 0.000005
    95 16.9413 0.0005 15.4983 0.0004 36.7194 0.0011 2.16745 0.00003 0.914822 0.000006
    96 16.9413 0.0003 15.4984 0.0001 36.7190 0.0006 2.16744 0.00001 0.914824 0.000002
    97 16.9414 0.0004 15.4985 0.0003 36.7198 0.0009 2.16748 0.00002 0.914833 0.000009
    98 16.9413 0.0003 15.4981 0.0003 36.7193 0.0009 2.16745 0.00002 0.914817 0.000006
    99 16.9418 0.0004 15.4987 0.0003 36.7209 0.0007 2.16749 0.00002 0.914817 0.000004
    100 16.9420 0.0003 15.4990 0.0004 36.7218 0.0010 2.16754 0.00002 0.914837 0.000007
    101 16.9415 0.0002 15.4984 0.0002 36.7202 0.0005 2.16746 0.00001 0.914829 0.000004
    102 16.9416 0.0003 15.4986 0.0003 36.7206 0.0009 2.16749 0.00001 0.914825 0.000005
    103 16.9417 0.0003 15.4987 0.0003 36.7211 0.0008 2.16746 0.00001 0.914818 0.000005
    104 16.9412 0.0004 15.4980 0.0004 36.7195 0.0013 2.16749 0.00003 0.914828 0.000007
    105 16.9414 0.0002 15.4986 0.0003 36.7196 0.0003 2.16749 0.00002 0.914828 0.000007
    106 16.9412 0.0003 15.4980 0.0004 36.7189 0.0009 2.16743 0.00002 0.914811 0.000005
    107 16.9414 0.0003 15.4984 0.0001 36.7201 0.0001 2.16744 0.00002 0.914810 0.000003
    108 16.9413 0.0005 15.4980 0.0004 36.7191 0.0012 2.16742 0.00001 0.914816 0.000007
    109 16.9409 0.0002 15.4977 0.0002 36.7188 0.0006 2.16747 0.00002 0.914817 0.000004
    110 16.9406 0.0002 15.4982 0.0001 36.7196 0.0006 2.16756 0.00003 0.914849 0.000006
    111 16.9414 0.0003 15.4984 0.0003 36.7204 0.0009 2.16750 0.00001 0.914837 0.000004
    112 16.9411 0.0001 15.4981 0.0002 36.7193 0.0006 2.16749 0.00002 0.914832 0.000006
    113 16.9410 0.0003 15.4984 0.0002 36.7202 0.0009 2.16753 0.00004 0.914843 0.000008
    114 16.9408 0.0003 15.4982 0.0003 36.7196 0.0008 2.16753 0.00001 0.914838 0.000004
    115 16.9411 0.0002 15.4984 0.0003 36.7205 0.0010 2.16752 0.00003 0.914839 0.000007
    116 16.9407 0.0003 15.4981 0.0003 36.7197 0.0009 2.16752 0.00002 0.914832 0.000003
    117 16.9410 0.0005 15.4983 0.0005 36.7195 0.0013 2.16750 0.00002 0.914843 0.000005
    118 16.9406 0.0005 15.4981 0.0005 36.7189 0.0011 2.16749 0.00001 0.914832 0.000005
    119 16.9416 0.0004 15.4988 0.0004 36.7202 0.0013 2.16747 0.00003 0.914836 0.000005
    120 16.9414 0.0003 15.4988 0.0004 36.7202 0.0009 2.16748 0.00003 0.914838 0.000007
    121 16.9411 0.0004 15.4984 0.0005 36.7198 0.0012 2.16748 0.00002 0.914838 0.000008
    平均值 16.9415 0.0010 15.4985 0.0009 36.7204 0.0023 2.16749 0.00008 0.914829 0.000023
    下载: 导出CSV

    表 6  2020年7月—2021年11月全流程空白的测试结果

    Table 6.  Blank results from July 2020 to November 2021

    序号 稀释剂称重/g 208Pb/206Pb 全流程空白/ng
    1 0.01951 1025 0.16
    2 0.01950 1049 0.12
    3 0.01894 1038 0.13
    4 0.01772 1049 0.18
    5 0.01825 957 0.25
    6 0.01831 982 0.21
    7 0.01757 971 0.22
    8 0.01545 948 0.22
    9 0.01917 1042 0.13
    10 0.01816 955 0.25
    11 0.01865 1034 0.13
    下载: 导出CSV

    表 7  元素含量标样BCR-2铅同位素比值测试结果及比对

    Table 7.  Comparison of Pb isotope ratios of BCR-2 in different laboratories

    数据来源 测试方法 测试仪器 206Pb/204Pb 207Pb/204Pb 208Pb/204Pb 测试次数
    Woodhead et al., 2000 双稀释剂 TIMS 18.750 0.011 15.615 0.003 38.691 0.021 4
    Collerson et al., 2002 Tl内标 MC-ICP-MS 18.765 0.011 15.628 0.005 38.752 0.022 3
    Li et al., 2003 Tl内标 MC-ICP-MS 18.757 0.012 15.624 0.009 38.723 0.018 11
    Bake et al., 2004 双稀释剂 MC-ICP-MS 18.760 0.010 15.621 0.008 38.731 0.028 8
    Weis et al., 2006 Tl内标 MC-ICP-MS 18.7529 0.0195 15.6249 0.0040 38.7237 0.0405 11
    刘希君等, 2013 双稀释剂 TIMS 18.752 0.011 15.619 0.005 38.723 0.020 \
    李世珍等, 2015 Tl内标 MC-ICP-MS 18.7574 0.0053 15.6234 0.0035 38.7305 0.0125 \
    测试平均值 18.757 0.009 15.624 0.006 38.725 0.025
    本文 Tl内标 MC-ICP-MS 18.7618 0.0060 15.6270 0.0014 38.7383 0.0110 18
    下载: 导出CSV

    表 8  元素含量标样AGV-2铅同位素比值测试结果及比对

    Table 8.  Comparison of Pb isotope ratios of AGV-2 in different laboratories

    数据来源 测试方法 测试仪器 206Pb/204Pb 207Pb/204Pb 208Pb/204Pb 测试次数
    Woodhead et al., 2000 双稀释剂 TIMS 18.864 0.007 15.609 0.006 38.511 0.020 4
    Li et al., 2003 Tl内标 MC-ICP-MS 18.879 0.011 15.618 0.008 38.547 0.017 2
    Bake et al., 2004 双稀释剂 MC-ICP-MS 18.873 0.005 15.621 0.003 38.552 0.010 5
    Weis et al., 2006 Tl内标 MC-ICP-MS 18.8688 0.0063 15.6173 0.0071 38.5443 0.0135 7
    刘希君等, 2013 双稀释剂 TIMS 18.870 0.006 15.619 0.003 38.546 0.012 \
    李世珍等, 2015 Tl内标 MC-ICP-MS 18.866 0.001 15.621 0.001 38.530 0.002 \
    测试平均值 18.870 0.011 15.618 0.009 38.538 0.031
    本文 Tl内标 MC-ICP-MS 18.8725 0.0050 15.6201 0.0012 38.5445 0.0045 14
    下载: 导出CSV

    表 9  元素含量标样BHVO-2铅同位素比值测试结果及比对

    Table 9.  Comparison of Pb isotope ratios of BHVO-2 in different laboratories

    数据来源 测试方法 测试仪器 206Pb/204Pb 207Pb/204Pb 208Pb/204Pb 测试次数
    Woodhead et al., 2000 双稀释剂 TIMS 18.640 0.010 15.538 0.009 38.228 0.026 4
    Collerson et al., 2002 Tl内标 MC-ICP-MS 18.679 0.002 15.562 0.002 38.285 0.004 2
    Li et al., 2003 Tl内标 MC-ICP-MS 18.687 0.024 15.558 0.019 38.294 0.060 4
    Bake et al., 2004 双稀释剂 MC-ICP-MS 18.649 0.019 15.540 0.015 38.249 0.022 5
    Weis et al., 2006 Tl内标 MC-ICP-MS 18.6474 0.0242 15.5334 0.0094 38.2367 0.0182 5
    测试平均值 18.660 0.042 15.546 0.026 38.259 0.059
    本文 Tl内标 MC-ICP-MS 18.6470 0.0078 15.5420 0.0087 38.2522 0.0143 3
    下载: 导出CSV

    表 10  元素含量标样BIR-1a铅同位素比值测试结果及比对

    Table 10.  Comparison of Pb isotope ratios of BIR-1a in different laboratories

    数据来源 测试方法 测试仪器 206Pb/204Pb 207Pb/204Pb 208Pb/204Pb 测试次数
    Li et al., 2003 Tl内标 MC-ICP-MS 18.8471 0.0004 15.6407 0.0012 38.4493 0.0022 3
    Bake et al., 2004 双稀释剂 MC-ICP-MS 18.851 0.005 15.662 0.001 38.501 0.006 3
    测试平均值 18.849 0.006 15.651 0.030 38.475 0.073
    本文 Tl内标 MC-ICP-MS 18.8511 0.0084 15.6597 0.0011 38.4918 0.0075 4
    下载: 导出CSV
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出版历程
收稿日期:  2022-01-10
修回日期:  2022-06-10
刊出日期:  2023-09-15

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