Center for Intelligent Chemical Instrumentation (CICI)

Department of Chemistry, Clippinger Laboratories, Ohio University, Athens, OH 45701-2979

April 28, 2008
 

Introduction

Analytical chemistry is a discipline that has realized great benefits from the growth in power and availability of laboratory computers. The decade of the 1980's produced a generation of general-purpose laboratory microcomputers that could be used routinely for the control of chemical instrumentation and the analysis of data arising from chemical measurements. The combination of computational and control capabilities offered by these computer systems has made possible the development of a variety of automated analytical instruments for use in dedicated monitoring scenarios such as patient monitoring in hospitals, process monitoring and control in the chemical industry, and environmental monitoring.

For the 1990's and beyond, the focus of research in combining computational and instrumental methods is turning to the development of "intelligent" chemical instrumentation. The term, "intelligent instrument", refers to a new generation of analytical instrument with advanced capabilities for data interpretation, self-optimization, and decision-making. Building upon these concepts, researchers at CICI are conducting basic research in the development of new methods and instrumentation for a variety of chemical analyses. Work is currently underway in each of the areas of electrochemistry, spectroscopy, and chromatography.

CICI presently has a core working group in forensic analysis specializing in mass and ion mobility spectrometry.  CICI members administer a wide range of instruments including an isotope ratio mass spectrometer and several different ion trap mass analyzers.  Coupled with chemometrics techniques, standard methods such as gas chromatography/mass spectrometry can reach new levels of discrimination ability.

 

Faculty’s Areas of Expertise

 

Hao Chen, Assistant Professor of Chemistry & Biochemistry
*Fundamental study of gas-phase ion chemistry

*Novel application to bioanalytical chemistry using ambient mass spectrometry

*Ambient ion thermal dissociation in proteomics

*Protein footprinting using fast photolytic oxidation of protein (FPOP) method with various oxidants

Peter de B. Harrington, Professor of Chemistry & Biochemistry
* Intelligent chemical instrument design
* Biological and forensic analysis using ion and differential mobility spectrometries
* New methods for chromatographic fingerprinting
* Forensic and biomaterial characterization by mass spectrometry

Glen P. Jackson, Assistant Professor of Chemistry & Biochemistry
* Fast GC-ECD and Fast GC-MS of explosives
* Fast tandem mass spectrometry using custom-programmed ion traps
* LC-MS of ceramides, cholesterols, and fatty acids
* Mass spectrometry instrumentation and novel approaches to tandem mass spectrometry

* Isotope ratio mass spectrometry

Opportunities for Graduate Students

CICI offers a unique environment for students who are interested in working with instrumentation, computers, and software.  There is a large demand for doctoral students with expertise in chemometrics.  Chemometrics is emphasized throughout the OU analytical chemistry curriculum.  Chemometrics includes the topics of systematic design and statistical interpretation of experiments, signal processing, calibration, modeling, and machine intelligence.  A burgeoning area of research is adapting chemometric methods to be used in bioinformatic applications of proteomic and genomic experiments.   

Prospective graduate students interested in forensic science should consider exploring graduate work in analytical or bioanalytical chemistry with a forensic emphasis at Ohio University.  You will have the advantage of receiving financial aid in the form of teaching or research assistantships and a full tuition waiver. Most graduate programs in forensic science do not have assistantships and are not research based degrees.  Our program provides the strong scientific and research background lab directors are looking for. 

As you work towards a PhD, you can take classes in forensic chemistry, DNA typing, and toxicology as well as taking traditional graduate coursework in analytical chemistry, biochemistry, and chemometrics.  In addition, you will work closely with a member of our faculty performing research in one of several areas in forensic science including remote sensing, DNA typing, toxicology, explosives analysis, and hazardous materials detection.  Researchers in our department have received major funding for forensic based projects from the National Institute of Justice, the US Army, and various counter-terrorism agencies. 


CICI and Homeland Security

The Ohio University Center for Intelligent Chemical Instrumentation has a history of research related to Homeland Security that spans a decade.  The US Army has sponsored Prof. Harrington’s research which was focused on chemical weapons detection.  Prof. Harrington’s group has worked on real-time modeling and compression methods of ion mobility spectrometry (IMS) data.  He is currently funded by the Army for wavelet compression of IMS spectra acquire from an unmanned aerial vehicle (UAV) that is used for remote detection of chemical weapons.   Prof. Harrington has worked on biological weapons detection and developed advanced algorithms for pattern recognition of microbes with mass spectrometry (MS).  He presently has a microbiology lab with a BioSafety Level 2 capability for analysis of microbes by IMS and MS.  Prof. Peter Harrington is also working with detection of food-borne pathogens and there is concern of a biological attack on the national food supply using pathogenic organisms. Prof. Peter Harrington is a pioneer in the area of real-time chemometric modeling of sensor data.

Prof. Glen Jackson’s group is working on rapid methods of explosives detection with fast-GC/fast-MS.  He also is developing low cost miniaturized mass spectrometers using novel ion filters.  Prof. Hao Chen is developing new methods for selectively sampling drugs and explosives for mass spectrometric detection.

Intelligent instrumentation is of paramount importance for Homeland Security because analytical instrumentation that is field employed cannot require operators with sophisticated knowledge in analytical chemistry.  Some sensors may not have an operator, but may be stand alone monitors or propelled in robotic vehicles (e.g., the IMS detector in the UAV).  These smart instruments must encode analytical knowledge so that they display an alarm or perform a required action when a target analyte is detected.  Consider IMS that is used in virtually every US airport for detecting explosive residues on hand-luggage and has been recently been installed in the Pentagon.  The IMS instruments have a green light that illuminates if no explosives are detected and a red light for detection.  Therefore, the algorithms embedded in the instrument must make the accurate decision that a spectroscopic signature attributed to an explosive occurs amidst a large range of potential interfering compounds. 

 
Selected Publication List of CICI Members Related to Forensic/Analytical Chemistry

Chen

Chen, H.; Eberlin, L.S.; Cooks, R.G.  Neutral Fragment Mass Spectra via Ambient Thermal Dissociation of Peptide/Protein Ions.  J. Am. Chem. Soc. 2007, 129, 5880-5886.

Chen, H.; Ouyang, Z.; Cooks, R.G. Thermal Production and Reactions of Organic Ions at Atmospheric Pressure.  Angew. Chem. Int. Ed., 2006, 3656-3660.

Cooks, R.G.; Chen, H.; Eberlin, M.N.; Zheng, X.; Tao, W.A. Polar Acetalization and Transacetalization in the Gas Phase: The Eberlin Reaction. Chem. Rev. 2006, 106, 188-211.

Chen, H.; Cotte-Rodriguez, I.; Cooks, R.G. cis-Diol Functional Group Recognition by Reactive Desorption Electrospray Ionization. Chem. Commun. 2006, 597-599.

Chen, H.; Justes, D.R.; Cooks, R.G. Proton Affinities of N-Heterocyclic Carbene Super Bases. Org. Lett. 2005, 7, 3949-3952.

Harrington

Chen, P.; Harrington, P. B. Discriminant analysis of fused positive and negative ion mobility spectra using multivariate self-modeling mixture analysis and neural networks. Applied Spectroscopy 2008, 62, 133-141.

 

Chen, P.; Lu, Y.; Harrington, P. B. Biomarker profiling and reproducibility study of MALDI-MS measurements of Escherichia coli by analysis of variance-principal component analysis. Analytical Chemistry 2008, 80, 1474-1481.

 

O'Donnell, R. M.; Sun, X. B.; Harrington, P. D. Pharmaceutical applications of ion mobility spectrometry. Trac-Trends in Analytical Chemistry 2008, 27, 44-53.

 

Lu, Y.; Harrington, P. B. Forensic application of gas chromatography - Differential mobility spectrometry with two-way classification of ignitable liquids from fire debris. Analytical Chemistry 2007, 79, 6752-6759.

 

Rearden, P.; Harrington, P. B.; Karnes, J. J.; Bunker, C. E. Fuzzy rule-building expert system classification of fuel using solid-phase microextraction two-way gas chromatography differential mobility spectrometric data. Analytical Chemistry 2007, 79, 1485-1491.

 

Zhang, Z. Y.; Wang, Y. M.; Fan, G. Q.; Harrington, P. D. B. A comparative study of multilayer perceptron neural networks for the identification of rhubarb samples. Phytochemical Analysis 2007, 18, 109-114.

 

P.B. Harrington; Laurent, C.; Levinson, D. F.; Markey, P. L. S. P. Bootstrap Classification and Point-Based Feature Selection from Age-Staged Mouse Cerebellum Tissues of Matrix Assisted Laser Desorption/Ionization Mass Spectra using a Fuzzy Rule-Building Expert System. Analytica Chimica Acta 2007, 599, 219-231.  

 

Rearden, P.; Harrington, P. B.  Detection of VOCs Using Gas Chromatography-Differential Mobility Spectrometry (GC-DMS).  LabPlus International 2006, 20(1), 20-24.

Bota, G. M.; Harrington, P .B.  Direct Detection of Trimethylamine in Meat Food Products Using Ion Mobility Spectrometry. Talanta 2006, 68(3), 629-635.

Fox, R. V.; Ball, R. D.; Harrington, P. B.; Rollins, H. W.; Wai, C. M.  Holmium Nitrate Complexation with Tri-n-butyl Phosphate in Supercritical Carbon Dioxide.  Journal of Supercritical Fluids 2005, 36(2), 137-144.

Zhang, Z. Y.; Chen, G.; Harrington, P. B.  Detection of Trace Organic Compounds by Using Ion Mobility Spectrometry and SIMPLISMA.  Spectroscopy and Spectral Analysis 2005, 25(9), 1530-1533.

Laurent, C.; Levinson, D. F.; Schwartz, S. A.;  Harrington, P. B.; Markey, S. P.;  Caprioli, R. M.; Levitt, P.  Direct Profiling of the Cerebellum by MALDI MS: A Methodological Study in Postnatal and Adult Mouse.  Journal of Neuroscience Research 2005, 81(5), 613-621.

Zhang, Z.; Harrington, P. B.  Recent Studies on Artificial Neural Networks and Their Application.  Current Topics in Analytical Chemistry 2005, 5, 24-41.

Ochoa, M.L.; Harrington, P. B.  Immunomagnetic Isolation of Enterohemorrhagic Escherichia coli O157:H7 from Ground Beef and Identification by Matrix-Assisted Laser Desorption/Ionization Time-of-Flight Mass Spectrometry and Database Searches.  Analytical Chemistry 2005, 77, 5258-5267.

Rainsberg, M. R.; Harrington, P. B.  Thermal Desorption Solid-Phase Microextraction Inlet for Differential Mobility Spectrometry.  Applied Spectroscopy 2005, 59, 754-762.

Rearden, P.; Harrington, P. B.  Rapid Screening of Precursor and Degradation Products of Chemical Warfare Agents in Soil by Solid-Phase Microextraction Ion Mobility Spectrometry (SPME-IMS).  Analytica Chimica Acta 2005, 545, 13-20.

Harrington, P. B.; Vieira, N. E.; Espinoza, J.; Nien, J. K.; Romero, R.; Yergey, A. L.  Analysis of Variance-Principal Component Analysis:  A Soft Tool for Proteomic Discovery.  Analytica Chimica Acta 2005, 544, 118-127.

Cao, L.; Harrington, P. B.; Liu, J.  SIMPLISMA and ALS Applied to Two-dimensional Nonlinear Wavelet Compressed Ion Mobility Spectra of Chemical Warfare Agent Simulants.  Analytical Chemistry 2005, 77(8), 2575-2586.

Ochoa, M. L.; Harrington, P .B.  Chemometric Studies for the Characterization and Differentiation of Microorganisms Using in Situ Derivatization and Thermal Desorption Ion Mobility Spectrometry.  Analytical Chemistry 2005, 77, 854-863.

Cui, X. J.; Zhang, Z. Y.; Harrington, P. B.; Ren, Y. L.  Quality control of the powder pharmaceutical samples of metronidazole based on near infrared reflectance spectra with temperature-constrained cascade correlation neural networks.  Chemical Journal of Chinese Universities 2004, 25(7), 1251-1253.

Cui, X. J.; Zhang, Z. Y.; Ren, Y. L.; Harrington, P. B.  Quality control of the powder pharmaceutical samples of sulfaguanidine by using NIR reflectance spectrometry and temperature-constrained cascade correlation networks.  Talanta 2004, 64(4), 943-948.

Fox, R. V.; Ball, R. D.; Harrington, P. B.; Rollins, H. W.; Jolley, J. J.; Wai, C. M.  Praseodymium Nitrate and Neodymium Nitrate Complexation with Organophosphorus Reagents in Supercritical Carbon Dioxide Solvent.  Journal of Supercritical Fluids 2004, 31, 273-286.

Zhang, Z.; Wang, D.; Harrington, P. B.; Voorhees, K. J.; Rees, J.  Forward Selection Radial Basis Function Networks Applied to Bacterial Classification Based on MALDI-TOF-MS.  Talanta 2004, 63, 527-532.

Cao, L.; Harrington, P. B.  Two-dimensional Nonlinear Wavelet Compression (NLWC) of Ion Mobility Spectra of Chemical Warfare Agent Simulants.  Analytical Chemistry 2004, 76, 2859-2868.

Ochoa, M.; Harrington, P. B.  Detection of Methamphetamine in the Presence of Nicotine Using In Situ Chemical Derivatization and Ion Mobility Spectrometry.  Analytical Chemistry 2004, 76, 985-991.

Cao, L.; Harrington, P. B.; Harden, C. S.; McHugh, V. M.; Thomas, M. A.  Nonlinear Wavelet Compression of Ion Mobility Spectra from Ion Mobility Spectrometers Mounted in an Unmanned Aerial Vehicle.  Analytical Chemistry 2004, 76, 1069-1077.

Jackson

Jackson, G. P.; Hyland, J. J.; Laskay, U. A. Energetics and efficiencies of collision-induced dissociation achieved during the mass acquisition scan in a quadrupole ion trap. Rapid Communications in Mass Spectrometry 2005, 19, 3555-3563.

 

Collin, O. L.; Niegel, C.; DeRhodes, K. E.; McCord, B. R.; Jackson, G. P. Fast gas chromatography of explosive compounds using a pulsed-discharge electron capture detector. Journal of Forensic Sciences 2006, 51, 815-818.

 

Collin, O. L.; Beier, M.; Jackson, G. P. Dynamic collision-induced dissociation of peptides in a quadrupole ion trap mass spectrometer. Analytical Chemistry 2007, 79, 5468-5473.

 

Laskay, Ü. A.; Hyland, J. J.; Jackson, G. P. Dynamic collision-induced dissociation (DCID) in a quadrupole ion trap using a two-frequency excitation waveform: I. Effects of excitation frequency and phase angle. Journal of the American Society for Mass Spectrometry 2007, 18, 749-761.

 

Laskay, Ü. A.; Collin, O. L.; Hyland, J. J.; Nichol, B.; Jackson, G. P.; Pasilis, S. P.; Duckworth, D. C. Dynamic Collision-Induced Dissociation (DCID) in a quadrupole ion trap using a two-frequency excitation waveform: II. Effects of frequency spacing and scan rate. Journal of the American Society for Mass Spectrometry 2007, 18, 2017-2025.