Abstract
Isotope dilution (ID) method has been widely applied to studies of elemental speciation and certification of the concentrations of geological reference materials. One of the key factors restricting the application of the ID method is the difficulty in identifying the optimal ratios of the isotope tracer (spike) to sample (S/N) and in estimating the error propagation. Here, using Se isotope as an example and employing a Monte Carlo method, we found that the optimal choice of spike and S/N are 77Sespike and 0.7, respectively. The S/N in the range from 0.1 to 4 can produce sufficiently low errors (< 0.4 %). Extending this method to other elements such as Cr, Fe, Ni, Sr, Cd and etc., their optimal spike and S/N were also presented. According to the optimized parameters of Se, we determined the Se concentrations of geological reference materials (GRMs) by thiol cotton fiber (TCF)-hydride generation ID-MC-ICP-MS. The relative standard deviation is < 5 %, and the detection limit is reduced to 0.1 ng/g. Most of the measured concentrations are consistent with those recommended by IGGE or reported previously. For some GRMs, discrepancies (e.g. 6.90 % for GSS-5) exist between our measurements and previous ones, which can be explained by the inhomogeneity of GRMs and/or the different digestion, purification and measurement methods among laboratories.
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References
Adriaens AG, Kelly WR, Adams FC (1993) Propagation of uncertainties in isotope dilution mass spectrometry using pulse counting detection. Anal Chem 65(5):660–663
Albarède F, Beard B (2004) Analytical methods for non-traditional isotopes. Rev Mineral Geochem 55:113–152
Amereih S, Meisel T, Barghouthi Z, Wegscheider W (2013) Determination of inorganic antimony species conversions during its speciation analysis in soil using isotope dilution techniques. J Anal Sci Methods Instrum 3(2):130–136
Baedecker PA, Rowe JJ, Steinnes E (1977) Application of epithermal neutron activation in multielement analysis of silicate rocks employing both coaxial Ge(Li) and low energy photon detector systems. J Radioanal Chem 40:115–146
Balaba RB, Smart RS (2012) Total arsenic and selenium analysis in Marcellus shale, high-salinity water, and hydrofracture flowback wastewater. Chemosphere 89:1437–1442
Belshaw NS, Freedman PA, O’Nions PK, Frank M, Guo Y (1998) A new variable dispersion double-focusing plasma mass spectrometer with performance illustrated for Pb isotopes. Int J Mass Spectrom 181(1–3):51–58
Beranoaguirre A, Pin C, Sanchez-Lorda ME, García MS, Gil IJI (2019) An evaluation of Rb-Sr isotope dilution analyses with a 86Sr-enriched tracer and Multiple Collection-ICP-MS. Int J Mass Spectrom 435:234–240
Cotta AB, Enzweiler J (2013) Determination of Cr, Cu, Ni, Sn, Sr and Zn mass fractions in geochemical reference materials by isotope dilution ICP-MS. Geostand Geoanal Res 37(1):35–50
de Jong J, Schoemann V, Lannuzel D, Tison JL, Mattielli N (2008) High-accuracy determination of iron in seawater by isotope dilution multiple collector inductively coupled plasma mass spectrometry (ID-MC-ICP-MS) using nitrilotriacetic acid chelating resin for pre-concentration and matrix separation. Anal Chim Acta 623(2):126–139
Dodson MH (1963) A theoretical study of the use of internal standards for precise isotopic analysis by the surface ionization technique: part I-General first-order algebraic solutions. J Sci Instrum 40(6):289–295
Ellis AS, Johnson TM, Herbel MJ, Bullen T (2003) Stable isotope fractionation of selenium by natural microbial consortia. Chem Geol 195:119–129
Fassett JD, Paulsen PJ (1989) Isotope dilution mass spectrometry for accurate elemental analysis. Anal Chem 61(10):643A–649A
Feng L, Wang J, Li H, Luo X, Li J (2017) A novel absolute quantitative imaging strategy of iron, copper and zinc in brain tissues by Isotope Dilution Laser Ablation ICP-MS. Anal Chim Acta 984:66–75
Fernandez DP, Gagnon AC, Adkins JF (2011) An isotope dilution ICP-MS method for the determination of Mg/Ca and Sr/Ca ratios in calcium carbonate. Geostand Geoanal Res 35(1):23–37
Fritsche J, Meisel T (2004) Determination of anthropogenic input of Ru, Rh, Pd, Re, Os, Ir and Pt in soils along Austrian motorways by isotope dilution ICP-MS. Sci Total Environ 325:145–154
García-Ruiz S, Petrov I, Vassileva E, Quétel CR (2011) Cadmium determination in natural waters at the limit imposed by European legislation by isotope dilution and TiO2 solid-phase extraction. Anal Bioanal Chem 401:2785–2792
Gardolinski PCFC, Packer AP, de Almeida CR, Giné MF (2002) Determination of Cd, Pb, Zn and Cu in sediment compartments by sequential extraction and isotope dilution inductively coupled plasma mass spectrometry (ID-ICP-MS). J Braz Chem Soc 13(3):375–381
Harte R, Newman G, Sargent M (2004) Achieving traceable chemical measurements: inter-laboratory evaluation of a simplified technique for isotope dilution mass spectrometry (IDMS). Part 1: methodology for high accuracy analysis of trace metals. Accred Qual Assur 9:33–38
Henrion A (1994) Reduction of systematic errors in quantitative analysis by isotope dilution mass spectrometry (IDMS): an iterative method. Fresenius’ J Anal Chem 350(12):657–658
Hoelzl R, Hoelzl C, Kotz L, Fabry L (1998) The optimal amount of isotopic spike solution for ultra-trace analysis by isotope dilution mass spectrometry. Accred Qual Assur 3(5):185–188
Huo D, Kingston HM, Larget B (2000) Application of isotope dilution in elemental speciation: speciated isotope dilution mass spectrometry (SIDMS). Compr Anal Chem 33:277–313
Inagaki K, Takatsu A, Nakama A, Eyama S, Yarita T, Okamoto K, Chiba K (2006) Determination of selenium in sediment by isotope-dilution inductively coupled plasma mass spectrometry with an octapole reaction cell. Anal Bioanal Chem 385:67–75
Inagaki K, Narukawa T, Yarita T, Takatsu A, Okamoto K, Chiba K (2007) Determination of cadmium in grains by isotope dilution ICP–MS and coprecipitation using sample constituents as carrier precipitants. Anal Bioanal Chem 389:691–696
John SG (2012) Optimizing sample and spike concentrations for isotopic analysis by double-spike ICPMS. J Anal At Spectrom 27(12):2123–2131
Kirchenbaur M, Heuser A, Bragagni A, Wombacher F (2018) Determination of In and Sn mass fractions in sixteen geological reference materials by isotope dilution MC-ICP-MS. Geostand Geoanal Res 42(3):361–377
Kleckner AE, Kakouros E, Stewart AR (2017) A practical method for the determination of total selenium in environmental samples using isotope dilution-hydride generation inductively coupled plasma-mass spectrometry. Limnol Oceanogr: Methods 15:363–371
Lam JC, Chan K, Yip Y, Tong W, Sin DW (2010) Accurate determination of lead in Chinese herbs using isotope dilution inductively coupled plasma mass spectrometry (ID-ICP-MS). Food Chem 121:552–560
Le Fèvre B, Pin C (2005) A straightforward separation scheme for concomitant Lu–Hf and Sm–Nd isotope ratio and isotope dilution analysis. Anal Chim Acta 543(1):209–221
Lee JM, Boyle EA, Echegoyen-Sanz Y, Fitzsimmons J, Zhang R, Kayser RA (2011) Analysis of trace metals (Cu, Cd, Pb, and Fe) in seawater using single batch nitrilotriacetate resin extraction and isotope dilution inductively coupled plasma mass spectrometry. Anal Chim Acta 686:93–101
Liu F, Zhu HL, Li X, Wang GQ, Zhang ZF (2017) Calcium isotopic fractionation and compositions of geochemical reference materials. Geostand Geoanal Res 41(4):675–688
Long LE (1966) Isotope dilution analysis of common and radiogenic strontium using 84Sr-enriched spike. Earth Planet Sci Lett 1(5):289–292
Maia SM, Pozebon D, Curtius AJ (2003) Determination of Cd, Hg, Pb and Tl in coal and coal fly ash slurries using electrothermal vaporization inductively coupled plasma mass spectrometry and isotopic dilution. J Anal At Spectrom 18(4):330–337
Makishima A, Kobayashi K, Nakamura E (2002) Determination of chromium, nickel, copper and zinc in milligram samples of geological materials using isotope dilution high resolution inductively coupled plasma-mass spectrometry. Geostand Geoanal Res 26(1):41–51
Obata H, Yoshida T, Ogawa H (2006) Determination of picomolar levels of platinum in estuarine waters: a comparison of cathodic stripping voltammetry and isotope dilution-inductively coupled plasma mass spectrometry. Anal Chim Acta 580:32–38
Qin H, Zhu J, Su H (2012) Selenium fractions in organic matter from Se-rich soils and weathered stone coal in selenosis areas of China. Chemosphere 86:626–633
Rapp I, Schlosser C, Rusiecka D, Gledhill M, Achterberg EP (2017) Automated preconcentration of Fe, Zn, Cu, Ni, Cd, Pb Co, and Mn in seawater with analysis using high-resolution sector field inductively coupled plasma mass spectrometry. Anal Chim Acta 976:1–13
Renedo M, Bustamante P, Tessier E, Pedrero Z, Cherel Y, Amouroux D (2017) Assessment of mercury speciation in feathers using species-specific isotope dilution analysis. Talanta 174:100–110
Reyes LH, Marchante-Gayón MJ, Alonso JIG, Sanz-Medel A (2006) Application of isotope dilution analysis for the evaluation of extraction conditions in the determination of total Selenium and selenomethionine in yeast-based nutritional supplements. J Agric Food Chem 54(5):1557–1563
Rouxel O, Ludden J, Carignan J, Marin L, Fouquet Y (2002) Natural variations of Se isotopic composition determined by hydride generation multiple collector inductively coupled plasma mass spectrometry. Geochim Cosmochim Acta 66:3191–3199
Rudge TJF, Reynolds BC, Bourdon B (2009) The double spike toolbox. Chem Geol 265(3–4):1–12
Sanzolone RF, Chao TT (1987) Determination of selenium in thirty-two geochemical reference materials by continuous—flow hydride generation atomic absorption spectrophotometry. Geostand Geoanal Res 11(1):81–85
Savard D, Bedard P, Barnes SJ (2009) selenium concentrations in twenty-six geological reference materials: new determinations and proposed values. Geostand Geoanal Res 33(2):249–259
Schaumlöffel D, Bierla K, Łobiński R (2007) Accurate determination of selenium in blood serum by isotope dilution analysis using inductively coupled plasma collision cell mass spectrometry with xenon as collision gas. J Anal At Spectrom 22(3):318–321
Siebert C, Nägler TF, Kramers JD (2001) Determination of molybdenum isotope fractionation by double-spike multicollector inductively coupled plasma mass spectrometry. Geochem Geophys Geosyst 2:1032
Stracke A, Scherer EE, Reynolds BC (2014) Application of isotope dilution in geochemistry Treatise on geochemistry, vol 15, 2nd edn. Elsevier, Amsterdam, pp 71–86
Sun Y, Zhou MF, Sun M (2001) Routine Os analysis by isotope dilution-inductively coupled plasma mass spectrometry: OsO4 in water solution gives high sensitivity. J Anal Atom Spectrom 16(4):345–349
Unceta N, Astorkia M, Abrego Z, Gómez-Caballero A, Goicolea MA, Barrio RJ (2016) A novel strategy for Cr(III) and Cr(VI) analysis in dietary supplements by speciated isotope dilution mass spectrometry. Talanta 154:255–262
Vieira MA, Ribeiro AS, Curtius AJ (2006) Determination of As, Ge, Hg, Pb, Sb, Se and Sn in coal slurries by CVG-ETV-ICP-MS using external or isotopic dilution calibration. Microchem J 82:127–136
Vogl J, Klingbeil P, Pritzkow W, Riebe G (2003) High accuracy measurements of Fe isotopes using hexapole collision cell MC-ICP-MS and isotope dilution for certification of reference materials. J Anal At Spectrom 18(9):1125–1132
Waight T, Baker J, Willigers B (2002) Rb isotope dilution analyses by MC-ICPMS using Zr to correct for mass fractionation: towards improved Rb–Sr geochronology? Chem Geol 186(1):99–116
Wang Z, Becker H (2014) Abundances of sulfur, selenium, tellurium, rhenium and platinum-group elements in eighteen reference materials by isotope dilution sector-field ICP-MS and negative TIMS. Geostand Geoanal Res 38(2):189–209
White WM, Albarède F, Telouk P (2000) High-precision analysis of Pb isotope ratios by multi- collector ICP-MS. Chem Geol 167(3–4):257–270
Yip Y, Chan K, Cheung P, Poon K, Shan W (2009) Analysis of non-fat soybean powder for the mass fractions of three elements: copper and zinc by isotope dilution ICP–MS and calcium by ICP–AES. Food Chem 112:1065–1071
Zhang N, Sun G, Ma H (2007) Determination of ultra-trace selenium in mineral samples by hydride generation atomic fluorescence spectrometry with pressurized-PTFE-vessel acid digestion. Miner Eng 20:1397–1400
Zhao Z, Zhao X, Jiang X, Zhao L, Zhang L (2019) Interference sources and elimination methods for the determination of selenium in soil and water sediment by atomic fluorescence spectrometry. Rock and Mineral Analysis 38(3):333–340 (in Chinese with English abstract)
Zhu XK, O’Nions RK, Guo Y, Belshaw NS, Rickard D (2000) Determination of natural Cu-isotope variation by plasma-source mass spectrometry: implications for use as geochemical tracers. Chem Geol 163(1–4):139–149
Zhu JM, Johnson TM, Clark SK, Zhu XK (2008a) High Precision Measurement of Selenium Isotopic Composition by Hydride Generation Multiple Collector Inductively Coupled Plasma Mass Spectrometry with a 74Se-77Se Double Spike. Chin J Anal Chem 36(10):1385–1390
Zhu JM, Wang N, Li S, Li L, Su H, Liu C (2008b) Distribution and transport of selenium in Yutangba, China: impact of human activities. Sci Total Environ 392(2–3):252–261
Zhu JM, Johnson TM, Finkelman RB, Zheng B, Sýkorová I, Pešek J (2012) The occurrence and origin of selenium minerals in Se-rich stone coals, spoils and their adjacent soils in Yutangba, China. Chem Geol 330–331:27–38
Zhu JM, Johnson TM, Clark SK, Zhu XK, Wang XL (2014) Selenium redox cycling during weathering of Se-rich shales: a selenium isotope study. Geochim Cosmochim Acta 126:228–249
Acknowledgements
This work was supported by Natural Science Foundation of China (No. U1612441, 41673017). We would like to thank Dr. Xiangli Wang at University of South Alabama for improving English and suggestions. The authors also thank Drs. Jing Wang and Li Zeng for assistance with Se isotope determination.
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Tan, D., Xu, W., Zhu, Z. et al. Optimizing the ratio of the spike to sample for isotope dilution analysis: a case study with selenium isotopes. Acta Geochim 39, 192–202 (2020). https://doi.org/10.1007/s11631-019-00390-6
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DOI: https://doi.org/10.1007/s11631-019-00390-6