Elemental speciation analysis of metals, phosphorus and sulfur: Exploring environmental and biological samples.

摘要

There has been much attention in element specific characterization of metal and metalloid containing species within both environmental and biological systems, over the past few decades. In speciation analysis, an area of research that deals with the detection, identification, and determination of metals, metalloids and their different chemical forms, there have been huge advancements. These advancements are due mainly to instrument technology developments, and new innovative method developments. Hyphenated techniques, based on using ICPMS are among the fastest growing research and application areas in atomic spectroscopy. The combination of ICPMS with high resolution separation techniques presents a unique analytical tool that is able to provide qualitative and quantitative information on species at ultra low levels in complex matrices. Elements such as phosphorus, sulfur, and metals are known to be important atoms in a wide variety of molecules of environmental and biological interest ranging from small molecules to large macromolecules such as proteins. The goal of this dissertation is to characterize phosphorus, sulfur, and metal detection by ICPMS combined with other mass spectroscopy techniques to provide important new information for identifying phosphorus, sulfur, and metal-containing species from low to high molecular weight (MW) from a wide range of sample types. For low MW species the use of elemental and molecular MS techniques were used to demonstrate the viability and enhanced detection capabilities of phosphorus for low MW species (qualitative and quantitative) and illustrated by using organophosphorous fire retardants as samples. For high MW species ICPMS and ITMS in tandem were used for identifying phosphopeptides. Cap-LC-ICP-MS was used for a screening tool for metals in CSF. The simultaneous determination of sulfur in thio-arsenical-containing Rat Urine using HPLC-ICPMS shows, the simultaneous detection of arsenic and sulfur comprised a first report combining arsenicals and their thiolated derivatives.