O.I. Panasenko, I.V. Melnik, T.O. Samura, R.A. Scherbna, V.V. Parchenko, I.M. Keitlyn, V.A. Salionov, A.S. Gotsulya, V.A. Safonov, A.A. Kremzer, N.A. Postol, V.P. Buryak, S.N. Kulish

Zaporozhye State Medical University

GAS CHROMATOGRAPHY IN ANALYTICAL TOXICOLOGY

In analytical toxicology gas chromatography (GS) has a number of advantages over other widely used techniques such as HPLC and immunoassay. Firstly , GC has a range of sensitive detectors, such as the "universal" flame ionization detector (FID) and the selective nitrogen-phosphorus detector (NPD), electron capture detection (ECD) and mass spectrometry (MS) detectors, which can be used in parallel. Secondly, stable, high efficiency ( capillary) GC columns are now widely available. Thirdly, GC is easy to interface with techniques giving direct information about compound identity such as electron-ionization MS (EI-MS) and Fourier-transform infrared spectrometer (FTIR) {2,10]. A compendium of GC terms and techniques is available [3].

With GC, as with HPLC, qualitative and quantitative information can often be obtained in the same analysis provided that appropriate calibration and QC(quality control) procedures are followed. Temperature programming in GC is analogous to gradient elution in HPLC, but is much simpler to perform and permits the analysis of compounds of different volatilities in one analysis. Moreover the return to starting conditions is easy and the interdependence of Mr (relative molecular mass), retention time and column temperature is valuable in aiding peak assignment is STA(systematic toxicological analysis). In addition, GC retention data are reproducible between different days columns, instruments, operators, centres and so on (see Box 1).

Box 1. Advantage of GC in analytical toxicology

-Can inject aqueous in some applications such as ethanol although headspace almost as easy and applicable to wide range of volatiles.

-Easy to use SPME(solid phase microextraction)/ thermal desorption.

-Range of stable, efficient Capilary Columns.

-Sensitive universel flame ionization detector(FID) and selective nitrogen-phosphorus detector, evaporative light detector, mass spectrometry (NPD, ECD, MS) detectors.-Qualitative and quantitative:

a) wide-bore capillary columns used with injection liners facilitate quantitative work

b) Inter-dependence of elution time column temperature, and Mr. valuable in qualitative work.

-Retention data reproducible between days/columns/ operators laboratories/countries.

-Temperature programming and interfacing to MS or FTYR easy-need few column types because of high resolving power especially with GC -MS. Can generate EI (electron ionization) spectra from GC-MS.

-Can generate EI ( electron ionization ) spectra from GC-MS

-Principal peak index valuable in compound identification. Can be used for a wide range of gases and solvents. Disadvantage of GC include the requirement what the analyte or a derivative should be volatile and stable at the temperature required for the analysis(in practice below 400C or so).

In additions, substances with highly polar or ionizable functional groups may give poor performance (broad, tailing peaks), and some form of sample preparation is normally need ( see Box 2). Moreover, same compounds their may be thermally labile and the decomposition products may interfere in the analysis. Thus, in addition to the choice of the sample preparation procedure, the column and the chromatographic and detection conditions, due consideration must be given to other factors including sample collection and storage , choice of internal standard and quality assurance. This being said , GC remaining the method of choice for gases and other volatiles such as ethanol and inhalational anaesthetics. GC is also widely used in the analysis of other compounds, in STA , and as an interface to MS, an especial advantage here being that EI spectra can be obtained.

Box 2. Limitations of GC in analytical toxicology need experienced operators, pure gas supplies, consumables, support from instrument manufacturer.

-Septum injection-need frequent maintenance.

-Sequential analysis-need auto injectors.

- Usually need same form of sample pretreatment.

-Cannot adjust selectivity by modifying eluent.

- Cannot analyze very polar/high Mr compounds, although can sometimes derivatize.

-Cannot analyze carbon monoxide directly by FID.

-There is always the possibility of interference from co eluting compounds.

Typically a GC system consists of a gas to the column as well as gases, such as compressed air and hydrogen, to the detector, a sample injection system, an analytical column, and a detector with associated data acquisition/processing. The injector, column and detector ovens are normally being maintained at a higher temperature than the maximum temperatur by the column oven to minimize the risk of frantionation or condensation of sample components in the detector. A similar consideration applies to the injector oven in isothermal operation same detectors, such as the ECD require an additional "make-up" gas flow in order to give optimum performance.

Gas chromatographs are usually purchased as a single unit, with gas supplies and data capture being separate. Increasingly instrument control is from a personal computer that also provides data capture facilities. Although commercially, supplied cylinders are a conventional source of the gases needed in GC operation, alternatives are available for air (sample compressor), hydrogen (electrolytic hydrogen generator ) and nitrogen ( nitrogen generator based on molecular sieve). Flowever, regular monitoring and maintenance, and the use of appropriate filter to remove hydrocarbons, oxygen and moisture are mandatory. filters should always be used with gas from cylinders.

The refinement of capillary column technology and the introduction of "bench-top" GC-MS systems have led to renewed appreciation of the value of GC in analytical toxicology. In developing GC methods, knowledge of the Mr and structure of the compound of interest is important even if a published method is to be followed. Information on any co-formulated or co-administered may sometimes be able to give details of assay methods, current literature and potential internal standards for particular compounds.

The role of capillary GC in STA has been discussed extensively [5,8], and more recently has been compared with HPLC-DAD, HPLC-MS and other techniques [4,9]

Packed column GC retention data for many drugs ans other poisons on a range of stationary phases of differing polarities are highly correlated [7] due to the inter-relationship between Mr, volutility and retention that is dominant in GC.

GC offers advantages over spectrophotometric methods for carbon monoxide analysis especially if badly decomposed postmortem blood or tissues are to be analyzed [6]. Flowever, because the sensitivity for carbon monoxide by FYD is very poor, either TCD or analyte reduction with hydrogen on a heated Ni catalyst to produce methane before FID have had to be used. This latter procedure introduces an additional step, and requires non-standard apparatus. With the development of the helium discharge ionization detector it is possible to measure carbon monoxide directly with good sensitivity. Helium is generally used as the carrier gas and as the ionized species. Sample manipulation, assay calibration, calculation of % COHb, and so on, are the same as with the use of TCD [6].

Blood cyanide concentrations have measured by GC-NPD using acetonitrile as internal standard after addition of phosphoric acid to the sample in a headspace vial[1].

Assay calibration was be addition of potassium cyanide solution to alkalinized human blood.

The earliest GC-FID method for the measurement of blood ethanol involved simple dilution og the sample (hole blood, plasma or urine) (50 ml) with internal standard solution (0,16 gl-1 agueous propanol, 500 ml) followed by vortex-mixing (10 s) and direct injection of the resulting mixture onto a column packed with a molecular sieve such a Chromosorb. Other volatiles such as methanol, 2-propanol and acetone, were resolved and could be measured if required-Modified cardon black materials can also be used.

Nowadays, static headspace sampling combined with temperature-programmed GC on a PDMS (polydimethylsiloxane)can be used to screen for not only ethanol, methanol and 2-propanol, but also for a wide range of other volatile compounds in biological fluids.

SUMMARY

There is no doubt that GC is the system of choice for the analysis of solvents and other volatiles, in STA, and as an interface with MS. The high efficiency and stability of modern capillary columns together with other features of GC, such as the ease of temperature programming and the reproducibility of retention data, are features that other chromatographic systems cannot match. The drawbacks of GC are the need for dedicated instruments, experienced operators and appropriate laboratory infrastructure. There is also the requirement to perform solvent extraction or same similar method of sample preparation and the restriction on the Mr of analytes to those that are stable and volatile,either derivatized or derivatized at the oven temperature required for the analysis ( in practice up to Mr 750 or so ). The great advantages of LC, especially when combined with MS, are that these letter restrictions are minimized. But all is not necessarily straightforward even with LC and LC-MS.

REFERENCES

1.            Calafat A.M., stasfile S.B., RAPD quantitation of cyanide in whole blood by automated head space gas chromatography. I. Chromatogr., 2002.-val.772.-pp131-137

2.            Grod R.L. and Barry E.F. Modern Practice of Gas Chromatography, 5 thedn. Wiley-Intencience, New York, 2004.-364 p.

3.            Hinshaw I.V. A compendium of GC terms and techniques. LC GC North America, 2002.-val.20.-pp.1034-1040.

4.            Maurer H.H. Position of chromatographic teachniques in screening for detection of drugs os poisons in clinical and forensic toxicology and/or doping control. Clin.Chem.Lab.Med., 2004.-val.42.-pp. 1310-1324.

5.            Maurer H.H. Systematic toxicological analysis of drugs and their metabolites by gas chromatography-nass spectrometry. I.Chromatogr. 1992.-val.580.-pp. 3-41.

6.            Mayes R.W. ACP Broadsheet № 142: November 1993. Measurement of carbon monoxide and cyanide in blood. I.CLIN.Pathal., 1993.-val.47-pp 982-988.

7.            Moffat A.C., Stead A.H., Smalldon K.W. Optiomum use of paper, thin-layer and gas-liqued chromutography for the identification of basic drugs. Gas-liquid chromatography.I. Chromatogr., 1974.-vol.90.-pp.19-33.

8.            Peters F.T. Schaefer S., staack R.F., Kraemer T., Maurer H.H. Screening for and validated quantification of amhetamines and amphetamine-and piperazine-derived designes drug in human blood plasma by gas chromatography mass spectrometry. I. Mass Spectrom., 2003.-val.38.-pp.659-676.

9.            Polettini A. Systematic toxicological analysis of drugs and paisons in biosamples by hyphenated chramotographic and spectroseopic techiques.I. Chromatogr., 1999.-val.733.-pp 47-63

10.        Rood D. The Thoubleshooting and Maintenance Guide for Gas chromatographers, 4th edn., Wiley, New York, 2006.-576 p.