Interview with Prof. Kevin A. Schug

Significance of the Topic

Advances in trace analysis of bioactive compounds and comprehensive evaluation of environmental impacts are critical in both clinical diagnostics and environmental monitoring. High performance mass spectrometry coupled with innovative sample preparation methods enables researchers to detect compounds at ultra-low concentrations while maintaining robust throughput and reliability.

Aim and Overview of the Study

This work stems from a long term collaboration between the University of Texas at Arlington and Shimadzu that began in 2007 and formally established the Shimadzu Center for Advanced Analytical Chemistry in 2012. The primary objectives are to develop ultra sensitive methods for quantifying estrogens in biological fluids including plasma and cerebrospinal fluid and to conduct the most extensive academic study to date on potential impacts of unconventional natural gas and oil extraction on groundwater quality.

Methodology and Instrumentation

The research employs a combination of:

• Trap and elute liquid chromatography tandem mass spectrometry using restricted access media (CoSense) and Shimadzu triple quadrupole MS for trace estrogen quantification.
• Liquid chromatography ion trap time of flight MS (LCMS-ITTOF) for fundamental ionization studies.
• Gas chromatography MS and headspace GC-FID/BID, ICP-OES, TOC/TN analysis for comprehensive water quality assessment.

Sample preparation was optimized by replacing traditional liquid-liquid extraction with on-line restricted access media trapping for high throughput and low detection limits down to parts per trillion.

Main Results and Discussion

In clinical applications, the team achieved ultra-sensitive detection of endogenous estrogens in plasma and cerebrospinal fluid at low ppt levels and characterized trapping efficiency on restricted access media. In environmental studies, over 800 groundwater samples collected near unconventional drilling sites were analyzed. Initial findings revealed indirect impacts on water quality in North Texas. Ongoing survey and time-course studies aim to elucidate pre-drilling, during drilling, and post-drilling contaminant dynamics. A hybrid targeted and untargeted workflow enhances the scope of analyte detection and strengthens data reliability.

Benefits and Practical Applications of the Method

Key advantages include:

• High sensitivity and selectivity for trace compounds in complex matrices.
• Improved sample throughput via on-line sample preparation.
• Comprehensive environmental monitoring using a suite of orthogonal techniques.
• Training opportunities for students in cutting edge analytical methods.

These methods support clinical research on traumatic brain injury treatment and inform stakeholders about potential environmental risks from modern gas and oil extraction.

Future Trends and Applications

Future directions involve further instrument innovations driven by collaborative feedback, expansion of restricted access media methods to new biomarker classes, integration of high resolution untargeted screening, and application of these workflows to broader environmental and clinical studies. Continued academic industry partnerships will foster development of specialized instruments and solutions.

Conclusion

The sustained partnership between U T Arlington and Shimadzu has yielded pioneering methods in trace bioanalysis and the largest academic investigation of groundwater impacts from unconventional drilling. Leveraging diverse high performance instrumentation and flexible sample preparation approaches, the collaboration delivers novel insights, practical analytical workflows, and exceptional training for the next generation of analytical scientists.

References

• Beinhauer J Liangqiao B Fan H Sebela M Kukula M Barrera JA Schug KA Bulk derivatization and cation exchange restricted access media based trap and elute liquid chromatography mass spectrometry method for determination of trace estrogens in serum Anal Chim Acta 2015 858 74-81
• Schug KA Sawicki I Carlton DD Fan H McNair HM Nimmo JP Kroll P Smuts J Walsh P Harrison D A Vacuum Ultraviolet Detector for Gas Chromatography Anal Chem 2014 86 8329-8335
• Papouskova B Fan H Lemr K Schug KA Aspects of Trapping Efficiency And Matrix Effects in Development of a Restricted Access Media Based Trap and Elute Liquid Chromatography Mass Spectrometry Method J Sep Sci 2014 37 2192-2199
• Fan H Papouskova B Lemr K Wigginton JG Schug KA Bulk Derivatization and Direct Injection of Human Cerebrospinal Fluid for Trace Level Quantification of Endogenous Estrogens Using Trap and Elute LC MS MS J Sep Sci 2014 37 2010-2017
• Barnes JS Schug KA Oxidative Degradation of Quercetin with Hydrogen Peroxide Using Continuous Flow Kinetic Electrospray Ion Trap Time of Flight Mass Spectrometry J Agric Food Chem 2014 62 4322-4331
• Nguyen HP Chandel NS DeBerardinis RJ Schug KA Hydrophilic interaction liquid chromatography tandem mass spectrometry to detect and quantify dicarboxyethyl glutathione a metabolic biomarker of fumarate hydratase deficient cancer cell J Sep Sci 2013 36 3303-3309
• Fontenot BE Hunt LR Hildenbrand ZL Carlton DD Oka H Walton JL Hopkins D Osorio A Bjorndal B Hu Q Schug KA An evaluation of water quality in private drinking water wells near natural gas extraction sites in the Barnett Shale Formation Environ Sci Technol 2013 47 10032-10040
• Barnes JS Foss FW Jr Schug KA Thermally Accelerated Oxidative Degradation of Quercetin Using Continuous Flow Kinetic Electrospray Ion Trap Time of Flight Mass Spectrometry J Am Soc Mass Spectrom 2013 24 1513-1522
• Yang SH Wang EH Gurak JA Bhawal S Deshmukh R Wijeratne AB Edwards BL Foss FW Jr Schug KA Affinity Mesh Screen Materials for Selective Extraction and Analysis of Antibiotics using Transmission Mode Desorption Electrospray Ionization Mass Spectrometry Langmuir 2013 29 8046-8053
• Tedmon L Barnes JS Nguyen HP Schug KA Differentiating Isobaric Steroid Hormone Metabolites Using Multi Stage Tandem Mass Spectrometry J Am Soc Mass Spectrom 2013 24 399-409