Publications (48)145.66 Total impact
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Article: A new validated analytical method for the determination of tributyltin in water samples at the quantification level set by the European Union.
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ABSTRACT: According to recent directives of the European Union (EU), limits of quantification (LOQ) for the determination of tributyltin (TBT) in surface waters should be ca. 60pg/L (ppq). This put very stringent requirements on analytical methodologies; definitely when they have to be applied in a routine environment. Stir bar sorptive extraction (SBSE), followed by thermal desorption (TD) and capillary gas chromatography-triple quadrupole mass spectrometry (GC-MS/MS) can provide accurate and precise data at the 2ng/L level (ppt). For lower concentrations, matrix and reagent interferences together with contamination may provide too high TBT values. A two-dimensional heart-cut GC method was developed to fractionate TBT from interferences. The GC-GC-MS/MS method shows excellent linearity in the range 50pg/L-4ng/L, good repeatability (RSD<20% at 200pg/L), and a limit of detection of 11pg/L. The method performance is demonstrated with representative samples i.e. harbor water and waste water samples.Journal of chromatography. A 07/2012; 1261:151-7. · 4.19 Impact Factor -
Article: Full evaporation dynamic headspace in combination with selectable one-dimensional/two-dimensional gas chromatography-mass spectrometry for the determination of suspected fragrance allergens in cosmetic products.
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ABSTRACT: Suspected fragrance allergens were determined in cosmetic products using a combination of full evaporation-dynamic headspace (FEDHS) with selectable one-dimensional/two-dimensional GC-MS. The full evaporation dynamic headspace approach allows the non-discriminating extraction and injection of both apolar and polar fragrance compounds, without contamination of the analytical system by high molecular weight non-volatile matrix compounds. The method can be applied to all classes of cosmetic samples, including water containing matrices such as shower gels or body creams. In combination with selectable (1)D/(2)D GC-MS, consisting of a dedicated heart-cutting GC-MS configuration using capillary flow technology (CFT) and low thermal mass GC (LTM-GC), a highly flexible and easy-to-use analytical solution is offered. Depending on the complexity of the perfume fraction, analyses can be performed in one-dimensional GC-MS mode or in heart-cutting two-dimensional GC-MS mode, without the need of hardware reconfiguration. The two-dimensional mode with independent temperature control of the first and second dimension column is especially useful to confirm the presence of detected allergen compounds when mass spectral deconvolution is not possible.Journal of chromatography. A 02/2012; 1255:207-15. · 4.19 Impact Factor -
Article: Profiling and characterizing skin ceramides using reversed-phase liquid chromatography-quadrupole time-of-flight mass spectrometry.
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ABSTRACT: An LC-MS based method for the profiling and characterization of ceramide species in the upper layer of human skin is described. Ceramide samples, collected by tape stripping of human skin, were analyzed by reversed-phase liquid chromatography coupled to high-resolution quadrupole time-of-flight mass spectrometry operated in both positive and negative electrospray ionization mode. All known classes of ceramides could be measured in a repeatable manner. Furthermore, the data set showed several undiscovered ceramides, including a class with four hydroxyl functionalities in its sphingoid base. High-resolution MS/MS fragmentation spectra revealed that each identified ceramide species is composed of several skeletal isomers due to variation in carbon length of the respective sphingoid bases and fatty acyl building blocks. The resulting variety in skeletal isomers has not been previously demonstrated. It is estimated that over 1000 unique ceramide structures could be elucidated in human stratum corneum. Ceramide species with an even and odd number of carbon atoms in both chains were detected in all ceramide classes. Acid hydrolysis of the ceramides, followed by LC-MS analysis of the end-products, confirmed the observed distribution of both sphingoid bases and fatty acyl groups in skin ceramides. The study resulted in an accurate mass retention time library for targeted profiling of skin ceramides. It is furthermore demonstrated that targeted data processing results in an improved repeatability versus untargeted data processing (72.92% versus 62.12% of species display an RSD < 15%).Analytical Chemistry 11/2011; 84(1):403-11. · 5.86 Impact Factor -
Article: In-vial pyrolysis (PyroVial) with pre- and post-sample treatment combined with different chromatographic techniques.
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ABSTRACT: A new generic pyrolysis unit (PyroVial) is presented. Pyrolysis is carried out in a 2 mL autosampler vial placed in a XYZ robot for automated pyrolysis as well as for pre- and post-pyrolysis treatment of the sample. Analysis of the volatiles is performed by headspace analysis while the semi- and non-volatiles are extracted from the pyrolysate with an organic solvent. The features of the PyroVial are such that all chromatographic techniques can be applied. The pyrolysis unit is discussed in terms of its technical features and its performance is illustrated with applications including conventional pyrolysis, in situ and post-pyrolysis derivatization, reaction pyrolysis and catalytic cracking.Journal of chromatography. A 11/2011; 1218(46):8303-12. · 4.19 Impact Factor -
Article: Evaluation of ionic liquid stationary phases for one dimensional gas chromatography-mass spectrometry and comprehensive two dimensional gas chromatographic analyses of fatty acids in marine biota.
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ABSTRACT: Ionic liquid stationary phases were tested for one dimensional gas chromatography-mass spectrometry (GC-MS) and comprehensive two dimensional gas chromatography (GC×GC) of fatty acid methyl esters from algae. In comparison with polyethylene glycol and cyanopropyl substituted polar stationary phases, ionic liquid stationary phases SLB-IL 82 and SLB-IL 100 showed comparable resolution, but lower column bleeding with MS detection, resulting in better sensitivity. The selectivity and polarity of the ionic liquid phases are similar to a highly polar biscyanopropyl-silicone phase (e.g. HP-88). In GC×GC, using an apolar polydimethyl siloxane×polar ionic liquid column combination, an excellent group-type separation of fatty acids with different carbon numbers and number of unsaturations was obtained, providing information that is complementary to GC-MS identification.Journal of chromatography. A 03/2011; 1218(20):3056-63. · 4.19 Impact Factor -
Article: Evaluation of automated sample preparation, retention time locked gas chromatography-mass spectrometry and data analysis methods for the metabolomic study of Arabidopsis species.
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ABSTRACT: In this paper, automated sample preparation, retention time locked gas chromatography-mass spectrometry (GC-MS) and data analysis methods for the metabolomics study were evaluated. A miniaturized and automated derivatisation method using sequential oximation and silylation was applied to a polar extract of 4 types (2 types×2 ages) of Arabidopsis thaliana, a popular model organism often used in plant sciences and genetics. Automation of the derivatisation process offers excellent repeatability, and the time between sample preparation and analysis was short and constant, reducing artifact formation. Retention time locked (RTL) gas chromatography-mass spectrometry was used, resulting in reproducible retention times and GC-MS profiles. Two approaches were used for data analysis. XCMS followed by principal component analysis (approach 1) and AMDIS deconvolution combined with a commercially available program (Mass Profiler Professional) followed by principal component analysis (approach 2) were compared. Several features that were up- or down-regulated in the different types were detected.Journal of chromatography. A 01/2011; 1218(21):3247-54. · 4.19 Impact Factor -
Article: The utility of sulfonate salts in drug development.
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ABSTRACT: The issue of controlling genotoxic impurities in novel active pharmaceutical ingredients (APIs) is a significant challenge. Much of the current regulatory concern, has been focused on the formation and control of genotoxic sulfonate esters. This is linked with the withdrawal of Viracept (Nefinavir mesilate) from European markets in mid-2007, over concerns about elevated levels of ethyl methanesulfonate (EMS). This issue has resulted in calls from European regulators to assess risk mitigation strategies for all marketed products employing a sulfonic acid counter-ion to ensure that the sulfonate esters that could be potentially formed are controlled to threshold of toxicological concern (TTC)-based limits. This has even led to calls to avoid sulfonic acids as salt counter-ions. However, sulfonic acid salts possess a range of properties that are useful to both synthetic and formulation chemists. Whilst sulfonate salts are not a universal panacea to some of the problems of salt formation they do offer significant advantages as alternatives to other salt forming moieties under certain circumstances. This review thus sets out to define some of the advantages provided through utilization of sulfonic acids, explaining the importance of their retention as part of a thorough salt selection process.Journal of Pharmaceutical Sciences 07/2010; 99(7):2948-61. · 3.06 Impact Factor -
Article: Analysis of bacterial fatty acids by flow modulated comprehensive two-dimensional gas chromatography with parallel flame ionization detector/mass spectrometry.
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ABSTRACT: Comprehensive two-dimensional gas chromatography (GCxGC) offers an interesting tool for profiling bacterial fatty acids. Flow modulated GCxGC using a commercially available system was evaluated, different parameters such as column flows and modulation time were optimized. The method was tested on bacterial fatty acid methyl esters (BAMEs) from Stenotrophomonas maltophilia LMG 958(T) by using parallel flame ionization detector (FID)/mass spectrometry (MS). The results are compared to data obtained using a thermal modulated GCxGC system. The data show that flow modulated GCxGC-FID/MS method can be applied in a routine environment and offers interesting perspectives for chemotaxonomy of bacteria.Journal of chromatography. A 04/2010; · 4.19 Impact Factor -
Article: A Detailed Study of Sulfonate Ester Formation and Solvolysis Reaction Rates and Application toward Establishing Sulfonate Ester Control in Pharmaceutical Manufacturing Processes
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ABSTRACT: Sulfonate esters of lower alcohols possess the capacity to react with DNA and cause mutagenic events, which in turn may be cancer inducing. Consequently, the control of residues of such substances in products that may be ingested by man (in food or pharmaceuticals) is of importance to both pharmaceutical producers and to regulatory agencies. Given that a detailed study of sulfonate ester reaction dynamics (mechanism, rates, and equilibria) has not been published to date, a detailed kinetic and mechanistic study was undertaken and is reported herein as a follow-up to our earlier communication in this journal. The study definitively demonstrates that sulfonate esters cannot form even at trace level if any acid present is neutralized with even the slightest excess of base. A key conclusion from this work is that the high level of regulatory concern over the potential presence of sulfonate esters in API sulfonate salts is largely unwarranted and that sulfonate salts should not be shunned by innovator pharmaceutical firms as a potential API form. Other key findings are that (1) an extreme set of conditions are needed to promote sulfonate ester formation, requiring both sulfonic acid and alcohol to be present in high concentrations with little or no water present; (2) sulfonate ester formation rates are exclusively dependent upon concentrations of sulfonate anion and protonated alcohol present in solution; and (3) acids that are weaker than sulfonic acids (including phosphoric acid) are ineffective in protonating alcohol to catalyze measurable sulfonate ester even when a high concentration of sulfonate anion is present and water is absent. Implications of the mechanistic and kinetic findings are discussed under various situations where sulfonic acids and their salts are typically used in active pharmaceutical ingredient (API) processing, and kinetic models are presented that should be of value to process development scientists in designing appropriate controls in situations where risk for sulfonate ester formation does exist.03/2010; -
Article: Comprehensive blood plasma lipidomics by liquid chromatography/quadrupole time-of-flight mass spectrometry.
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ABSTRACT: A lipidomics strategy, combining high resolution reversed-phase liquid chromatography (RPLC) with high resolution quadrupole time-of-flight mass spectrometry (QqTOF), is described. The method has carefully been assessed in both a qualitative and a quantitative fashion utilizing human blood plasma. The inherent low technical variability associated with the lipidomics method allows to measure 65% of the features with an intensity RSD value below 10%. Blood plasma lipid spike-in experiments demonstrate that relative concentration differences smaller than 25% can readily be revealed by means of a t-test. Utilizing an advanced identification strategy, it is shown that the detected features mainly originate from (lyso-)phospholipids, sphingolipids, mono-, di- and triacylglycerols and cholesterol esters. The high resolution offered by the up-front RPLC step further allows to discriminate various isomeric species associated with the different lipid classes. The added value of utilizing a Jetstream electrospray ionization (ESI) source over a regular ESI source in lipidomics is for the first time demonstrated. In addition, the application of ultra high performance LC (UHPLC) up to 1200bar to extend the peak capacity or increase productivity is discussed.Journal of chromatography. A 02/2010; 1217(25):4087-99. · 4.19 Impact Factor -
Article: Analysis of potential genotoxic impurities in pharmaceuticals by two-dimensional gas chromatography with Deans switching and independent column temperature control using a low-thermal-mass oven module.
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ABSTRACT: The analysis of potential genotoxic impurities (PGIs) in active pharmaceutical ingredients (APIs) is a challenging task. The target limit of detection for a PGI in an API is typically 1 ppm (1 microg/g API). This is about 500 times lower than for classical impurity analysis. Consequently, analytical methods for trace analysis, mostly in combination with MS detection, need to be applied for the qualitative and quantitative determination of these impurities. A two-dimensional capillary GC method is presented that can be used for the determination of some target PGIs. A concentrated solution of the API sample is directly introduced in the GC-MS system, using an apolar column for first-dimension separation. The fraction (heart-cut) containing the PGIs is transferred to a second capillary column, installed in a low-thermal-mass oven (LTM). The LTM focuses the heart-cut(s) and allows independent temperature-programmed analysis with a polar second-dimension column. The API, solvent, and derivatization agents are not introduced in the second column or in the MS detector, avoiding contamination, column degradation, and target analyte peak detection/integration issues. The performance of this set-up is illustrated by the analysis of some Michael-reactive acceptor PGIs and haloalcohols in carbamazepine as test matrix. Excellent reproducibility (<10% RSD) at the low parts per million level and low detection limits (<1 ppm) were obtained.Analytical and Bioanalytical Chemistry 12/2009; 396(3):1291-300. · 3.78 Impact Factor -
Article: Study on the migration of bisphenol-A from baby bottles by stir bar sorptive extraction-thermal desorption-capillary GC-MS.
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ABSTRACT: Migration of bisphenol-A (BPA), the principal monomer of polycarbonate (PC) baby bottles, was investigated using an aqueous migration simulant. BPA was determined in 200 mL water samples using stir bar sorptive extraction (SBSE) after in situ derivatization with acetic acid anhydride followed by thermal desorption (TD)-capillary GC-MS. The concentration of BPA was calculated using the deuterated internal standard d6-BPA. Calibration for BPA was shown to be linear in a concentration range from 1 ng/L to 10 microg/L with a correlation coefficient >0.99. The LOD for BPA (as acetate) was 0.12 ng/L and LOQ 0.40 ng/L (ppt). PC bottles were heated in a water bath and in a microwave oven at four different temperatures (37, 53, 65, and 85 degrees C). The higher the temperature, the more the BPA was released, and after a few heating cycles, the released concentrations became constant. At normal use, i.e. at 37 degrees C, concentrations are ca. 10 ng/L. No significant difference was noted between water bath and microwave heating illustrating that migration of BPA is mainly temperature dependent.Journal of Separation Science 10/2009; 32(21):3829-36. · 2.73 Impact Factor -
Article: Gas chromatography of 209 polychlorinated biphenyl congeners on an extremely efficient nonselective capillary column.
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ABSTRACT: The gas chromatographic-mass spectrometric (GC-MS) separation of all 209 polychlorinated biphenyl (PCB) congeners was studied on an extremely efficient 80 m x 0.1mm i.d. capillary column coated with a 0.1 microm film of poly(5%-phenyl methyl)siloxane stationary phase. The quality of the separation and the number of resolved and coeluting peaks were compared to predictions according to the statistical overlap theory (SOT) and to literature data on PCB separations obtained by one-dimensional and comprehensive two-dimensional GC (GC x GC) and GC-MS. Mass spectral and chemometric deconvolution procedures were used to resolve overlapping peaks. On the highly efficient column, 195 PCB congeners were resolved in 96 min separation time using spectral and chemometric deconvolution. This number is comparable to the best separations described in GC x GC-MS mode. The novel method was developed for spectral deconvolution of overlapped PCB congeners which was verified determining the most toxic, dioxin-like PCBs both in the model mixture of 209 PCBs as well as in the Aroclor 1242 and Aroclor 1254 formulations.Journal of chromatography. A 09/2009; 1216(32):6043-62. · 4.19 Impact Factor -
Article: The acetonitrile shortage: is reversed HILIC with water an alternative for the analysis of highly polar ionizable solutes?
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ABSTRACT: In hydrophilic interaction chromatography (HILIC), best results are obtained with high concentrations of ACN. In the framework of green chromatography and the present shortage and very high price of this hazardous solvent, reversing the stationary phase to apolar and the mobile phase to aqueous can be of interest for several applications. The features of the aqueous RP technique called per aqueous LC (PALC) are illustrated with the analysis of catecholamines, nucleobases, acids, and amino acids. The ca. three-fold higher viscosity of water compared to ACN has consequences on the shape of the Van Deemter plot. For dopamine (N = 26.450 on a 25 cm x 4.6 mm id, 5 microm bare silica column), a reduced plate height of 1.9 at an u(opt) of 0.3 mm/s was calculated. The plate number, however, strongly depends on pH and ionic strength. As in RP separations, retention is shortened by adding an organic modifier. In the framework of green chromatography, the biodegradable ethanol was used. On the other hand, retention increased by lengthening the carbon chain of ion-pair reagents supporting the RP mechanism as well.Journal of Separation Science 06/2009; 32(12):2001-7. · 2.73 Impact Factor -
Article: Mechanism and Processing Parameters Affecting the Formation of Methyl Methanesulfonate from Methanol and Methanesulfonic Acid: An Illustrative Example for Sulfonate Ester Impurity Formation
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ABSTRACT: Sulfonate salts offer useful modification of physicochemical properties of active pharmaceutical ingredients (APIs) containing basic groups, but there are regulatory concerns over the presence of sulfonate esters as potential genotoxic impurities (PGIs). Whilst sulfonate esters could theoretically result from interaction between sulfonic acids and alcohols, literature on their formation is sparse. GC−MS analysis of reactions of methanesulfonic acid (MSA) and isotopically labeled methanol (18O-label) confirm methanol C−O bond cleavage in the formation of the methyl methanesulfonate (MMS), consistent with reversal of well-established mechanisms for solvolysis of sulfonate esters. Studies of reaction profiles quantify methyl methanesulfonate formation under a range of conditions relevant to API processing. Maximum conversion to MMS in reaction mixtures was 0.35%, determined by analytical methods developed specifically for reaction mixture analysis. Sulfonate ester formation is dramatically reduced at lower temperatures, in the presence of small amounts of water, or when acid is partially neutralized by substoichiometric amounts of the weak base, 2,6-lutidine, used to mimic conversion of a basic API to a salt in pharmaceutical manufacture. In the presence of a slight excess of base, ester formation was not detected. These findings, particularly those involving an excess of base, are compelling and provide a scientific understanding to allow for the design of processing conditions to minimize and control sulfonate ester formation.05/2009; -
Article: Features of a micro-gas chromatograph equipped with enrichment device and microchip plasma emission detection (muPED) for air monitoring.
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ABSTRACT: A field portable gas chromatograph (GC) was constructed allowing the enrichment of organic solutes from air samples on a miniaturized chemical trap and the subsequent gas chromatographic analysis on a resistively heated capillary column. The heart of the system is an integrated chip-based plasma emission detector (muPED). As a non-selective detector, the sensitivity is similar to that of a flame ionization detector (FID). The detector shows good selectivity for phosphorus, sulfur and chlorine-containing compounds with relative selectivities of ca. 5 x 10(5) gP gC(-1), 50 gS gC(-1) and 10(2) gCl gC(-1). The lifetime of the plasma chip under air monitoring conditions exceeded 3000 analyses.Lab on a Chip 12/2008; 8(11):1819-28. · 5.67 Impact Factor -
Article: Determination of arylamines and aminopyridines in pharmaceutical products using in-situ derivatization and liquid chromatography-mass spectrometry.
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ABSTRACT: Arylamines and aminopyridines form a class of potentially genotoxic impurities (PGIs) that can be present at trace levels in active pharmaceutical ingredients (APIs). A generic method was developed that allows the analysis of a selected set of these solutes at sub-ppm level relative to the drug substance. A highly concentrated solution of the pharmaceutical compound is analyzed by LC-MS using a single quadrupole mass spectrometer in the selected ion monitoring (SIM) mode. Since a number of target compounds show little or no retention in the reversed-phase LC setup, a fast and simple derivatization procedure using hexylchloroformate was applied. The amide derivatives of the PGI result in a higher molecular weight (more specific ion for SIM) and better chromatographic behavior. The methodology, consisting of a dual run on respectively a non-derivatized and a derivatized sample, was validated and applied to a selection of pharmaceutical substances. The method was found to be sufficiently sensitive and robust and is applicable in a QA/QC environment.Journal of chromatography. A 10/2008; 1216(16):3563-70. · 4.19 Impact Factor -
Article: Chemotaxonomy of bacteria by comprehensive GC and GC-MS in electron impact and chemical ionisation mode.
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ABSTRACT: The analysis of the cellular lipidic fraction of bacteria is described. After hydrolysis and methylation, the fatty acid methyl esters (FAMEs) are determined by 1-D GC using the Sherlock MIDI bacteria identification system, by comprehensive GC (GC x GC) and by GC-MS in electron impact (EI) and positive chemical ionisation (PCI) mode. With GC x GC, the enhanced selectivity and group type separation provides a more complete elucidation of the fatty acids in microorganisms. GC-EI-MS and GC-PCI-MS were helpful for confirmation. The bacteria selected in this study are Brevundimonas diminuta, Chryseobacterium gleum and Stenotrophomonas maltophilia.Journal of Separation Science 10/2008; 31(19):3395-403. · 2.73 Impact Factor -
Article: Development and validation of an automated static headspace gas chromatography-mass spectrometry (SHS-GC-MS) method for monitoring the formation of ethyl methane sulfonate from ethanol and methane sulfonic acid.
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ABSTRACT: An automated sample preparation and analysis procedure was developed to monitor the formation of ethyl methane sulfonate from reaction mixtures containing ethanol and methane sulfonic acid. The system is based on a liquid handling robot combined with a static headspace module. The formed ethyl methane sulfonate is analysed after derivatisation with pentafluorothiophenol using static headspace-gas chromatography-mass spectrometry (SHS-GC-MS). Using the automated reaction-derivatisation-headspace GC-MS system, the formation of ethyl methane sulfonate can be monitored in different reaction mixtures under different reaction conditions, including temperature, water content and pH. Excellent linearity, repeatability and robustness were obtained, allowing the system to be used in kinetic studies.Journal of Pharmaceutical and Biomedical Analysis 10/2008; 48(5):1339-44. · 2.97 Impact Factor -
Article: Creating a fatty acid methyl ester database for lipid profiling in a single drop of human blood using high resolution capillary gas chromatography and mass spectrometry.
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ABSTRACT: Capillary gas chromatography (CGC) in combination with mass spectrometry (MS) was optimized for the separation and detection of the fatty acids occurring in the lipid fraction of blood. A fingertip blood sample (ca. 50 microL) was transesterified into the methyl esters and analyzed on a 100 m x 0.25 mm ID column coated with a biscyanopropyl polysiloxane (HP-88) stationary phase. The method was retention time locked. Programmed temperature vaporization injection (PTV) in the solvent venting mode was applied to minimize the sample size, while maintaining high sensitivity. The total analysis time was ca. 60 min. Retention times and both electron impact (EI) and positive chemical ionization (PCI) mass spectrometry were combined to elucidate the fatty acids according to alkyl chain, degree of unsaturation and position of the double bonds. Using extracted ion chromatograms about 100 fatty acids and related compounds were detected in blood samples and most of them were identified. This work resulted in a very large fatty acid methyl esters database, containing retention time and mass spectral information that will be applied to metabolomic studies.Journal of Chromatography 10/2008; 1211(1-2):120-8. · 4.53 Impact Factor
Top co-authors
Top Journals
Institutions
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2011
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Chinese Academy of Sciences
Beijing, Beijing Shi, China
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1995–2011
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Research Institute for Chromatography
Kortrijk, VLG, Belgium
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2010
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GlaxoSmithKline plc.
London, ENG, United Kingdom
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2005–2010
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Ghent University
- Department of Organic Chemistry
Gent, VLG, Belgium -
Università degli Studi di Torino
- Dipartimento di Scienza e Tecnologia del Farmaco
Torino, Piedmont, Italy
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2009
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Slovak University of Technology in Bratislava
- Institute of Analytical Chemistry
Bratislava, Bratislavsky Kraj, Slovakia
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