Determination of Lead Elemental Concentration and Isotopic Ratios in Coal Ash and Coal Fly Ash Reference Materials Using Isotope Dilution Thermal Ionization Mass Spectrometry

利用同位素稀释热电离质谱法测定煤灰和煤粉灰参考物质中铅元素浓度和同位素比值

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Abstract

The rapid expansion of coal-fired power plants around the world has produced a huge volume of toxic elements associated with combustion residues such as coal fly ash (CFA) and coal ash (CA), which pose great threats to the global environment. It is therefore crucial for environmental science to monitor the migration and emission pathway of toxic elements such as CFA and CA. Lead isotopes have proved to be powerful tracers capable of dealing with this issue. Unfortunately, up to now, few high precision lead isotope data of CFA and CA certified reference materials (CRMs) determined by using the double spike technique have been reported. Hence, to facilitate the application of lead isotopes in environmental science, it is indispensable and urgent to determine a suite of high precision Pb isotope ratios and Pb elemental contents for CFA and CA CRMs. Here, we measured lead isotope ratios from four CFA and CA CRMs using thermal ionization mass spectrometry (TIMS) combined with the (204)Pb-(207)Pb double spike method. Lead isotope ratios values of CRMs (GBW11124, GBW08401, GBW11125d, and JCFA-1) covered wide variation ranges from 17.993 to 19.228 for (206)Pb/(204)Pb, from 15.513 to 15.675 for (207)Pb/(204)Pb, and from 38.184 to 39.067 for (208)Pb/(204)Pb. Lead isotope ratios of these CRMs, except for GBW11124, show good external reproducibility (2 RSD, n = 8), which is better than 0.05% for (206)Pb/(204)Pb and (207)Pb/(204)Pb, 0.07% for (208)Pb/(204)Pb, 0.04% for (206)Pb/(207)Pb, and 0.05% for (208)Pb/(206)Pb. The Pb concentrations of these CRMs were determined using (207)Pb single spike method. The reproducibility (1 RSD, n = 4) of Pb elemental content was <0.60%. This indicates the distribution of Pb elements in these CRMs is homogeneous. With the exception of GBW11124, the suite of CRMs can be used for determining CFA and CA matrix composition for quality control of Pb isotope analyses.

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