The advantages of high sensitivity, low detection, large dynamic range and multi-element/isotope capability for most elements in the periodic table have enabled inductively coupled plasma mass spectrometry (ICPMS) to become a popular technique for elemental analysis. However, there are challenges from sample loss, matrix effects, interferences, or contamination when applying this technique in various analysis. To explore methods for reducing these difficulties in ICPMS-based analysis, the first part of this thesis is focused on removing inorganic phosphate interferences for the determination of organophosphate nerve agent degradation products based on the detection of 31P+. Calcium chloride and ammonium hydroxide were chosen as the coagulant and for pH adjustment to remove inorganic phosphate interferences. Applications to apple juice and cola drink indicate that this method is suitable for enhancing the determination of organophosphate species in high inorganic phosphate matrices.
The growing interest in metals and their biological functions have promoted the utilization of ICPMS in the biological area for trace element determination and metal-containing speciation studies. The remaining focus of this dissertation is to investigate and characterize the metal-protein associations in various biological systems, which is referred as metallomics. To achieve overall screening and sufficient confidence in protein identifications, state-of-the-art metallomics techniques via two-dimensional chromatographic separations in combination with elemental and molecular mass spectrometries were utilized. Two biological systems were studied with different purposes and possible applications. Human cerebrospinal fluid (CSF) from healthy control patients and patients who suffered subarachnoid hemorrhage and its complication, cerebral vasospasm was screened at different metal detection points (Fe, Ni, Cu, Zn and Pb) for molecular distribution patterns and was investigated for possible markers. The identification and comparisons across the three types of CSF resulted in six protein families of possible biomarkers, which are now possible focus areas to study further for predicting, diagnosing and treating the hemorrhage to preclude the debilitating or deadly vasospasm. Bacteriophage lambda was investigated for possible phage-metal association at proteome level. Of a large number of metals, Mn, Fe, Co, Ni, Cu and Zn were observed to best associate with lambda phage sample from SEC-ICPMS screening. Further identification indicates that gpE, gpD and gpV have the highest likelihood of association with these transition metals to provide valuable information for lambda phage engineered technologies.