Time; Gas Chromatography-Mass Spectrometry/methods; Analytes; Comprehensive two-dimensional gas chromatography; Gaschromatography-mass spectrometry; GC×GC; Modeling approach; Retention time; Retention time prediction; Space occupation; Time of flight mass spectrometry; Top down approaches; Analytical Chemistry
Abstract :
[en] In this contribution, we describe a novel modeling approach to predicting retention times (tr) in comprehensive two-dimensional gas chromatography coupled to time-of-flight mass spectrometry (GC × GC-ToF-MS) with a particular emphasis on the second-dimension (2D) retention time predictions (2tr). This approach is referred to as a "top-down" approach in that it breaks down the complete GC × GC separation into two independent one-dimensional gas chromatography separations (1D-GC). In this regard, both dimensions, that is, first dimension (1D) and second dimension (2D) are treated separately, and the cryogenic modulator is simply considered as a second consecutive injection device. Separate 1D-GC tr predictions are performed on both dimensions using the same flow rate as the one deployed in the conventional GC × GC system. The separate tr predictions are then combined to account for the two-dimensional separation. This model was applied to 24 analytes from 2 standard mixtures (Grob Test Mix and Fragrance Materials Test Mix) and assessed across 9 GC × GC chromatographic conditions. The experimental and predicted chromatographic retention space occupations were assessed by using the convex hull approach defined by the Delaunay triangulation. The predicted percentage of space occupation corresponded favorably with the experimental values. Furthermore, the top-down approach enabled an accurate prediction of the 2tr of all investigated analytes, providing an average 2tr modeling error of 0.26 ± 0.01 s.
Disciplines :
Chemistry
Author, co-author :
Gaida, Meriem ; Université de Liège - ULiège > Molecular Systems (MolSys)
Franchina, Flavio ; Université de Liège - ULiège > Département de chimie (sciences) > Chimie analytique, organique et biologique ; Department of Chemistry, Pharmaceutical, and Agricultural Sciences, University of Ferrara, via L. Borsari 46, 44121Ferrara, Italy
Stefanuto, Pierre-Hugues ; Université de Liège - ULiège > Département de chimie (sciences) > Chimie analytique, organique et biologique
Focant, Jean-François ; Université de Liège - ULiège > Département de chimie (sciences) > Chimie analytique, organique et biologique
Language :
English
Title :
Top-Down Approach to Retention Time Prediction in Comprehensive Two-Dimensional Gas Chromatography-Mass Spectrometry.
Liu, Z.; Phillips, J. B. Comprehensive two-dimensional gas chromatography using an on-column thermal modulator interface. J. Chromatogr. Sci. 1991, 29, 227-231, 10.1093/chromsci/29.6.227
Di Giovanni, N.; Meuwis, M. A.; Louis, E.; Focant, J. F. Untargeted Serum Metabolic Profiling by Comprehensive Two-Dimensional Gas Chromatography-High-Resolution Time-of-Flight Mass Spectrometry. J. Proteome Res. 2020, 19, 1013-1028, 10.1021/acs.jproteome.9b00535
Stefanuto, P. H.; Perrault, K. A.; Stadler, S.; Pesesse, R.; LeBlanc, H. N.; Forbes, S. L.; Focant, J. F. GC × GC-TOFMS and supervised multivariate approaches to study human cadaveric decomposition olfactive signatures. Anal. Bioanal. Chem. 2015, 407, 4767-4778, 10.1007/s00216-015-8683-5
Zou, Y.; Gaida, M.; Franchina, F. A.; Stefanuto, P. H.; Focant, J. Distinguishing between Decaffeinated and Regular Coffee by HS-SPME-GC×GC-TOFMS, Chemometrics, and Machine Learning. Molecules 2022, 27, 1806, 10.3390/molecules27061806
Prebihalo, S. E.; Berrier, K. L.; Freye, C. E.; Bahaghighat, H. D.; Moore, N. R.; Pinkerton, D. K.; Synovec, R. E. Multidimensional Gas Chromatography: Advances in Instrumentation, Chemometrics, and Applications. Anal. Chem. 2018, 90, 505-532, 10.1021/acs.analchem.7b04226
Harynuk, J.; Górecki, T. Experimental variables in GC×GC: A complex interplay. Am. Lab. 2007, 39, 36-39
Dorman, F. L.; Schettler, P. D.; English, C. M.; Patwardhan, D. V. Predicting gas chromatographic separation and stationary-phase selectivity using computer modeling. Anal. Chem. 2002, 74, 2133-2138, 10.1021/ac0110496
Lu, X.; Kong, H.; Li, H.; Ma, C.; Tian, J.; Xu, G. Resolution prediction and optimization of temperature programme in comprehensive two-dimensional gas chromatography. J. Chromatogr. A 2005, 1086, 175-184, 10.1016/j.chroma.2005.05.105
Dorman, F. L.; Schettler, P. D.; Vogt, L. A.; Cochran, J. W. Using computer modeling to predict and optimize separations for comprehensive two-dimensional gas chromatography. J. Chromatogr. A 2008, 1186, 196-201, 10.1016/j.chroma.2007.12.039
McGinitie, T. M.; Harynuk, J. J. Prediction of retention times in comprehensive two-dimensional gas chromatography using thermodynamic models. J. Chromatogr. A 2012, 1255, 184-189, 10.1016/j.chroma.2012.02.023
Zhu, S.; He, S.; Worton, D. R.; Goldstein, A. H. Predictions of comprehensive two-dimensional gas chromatography separations from isothermal data. J. Chromatogr. A 2012, 1233, 147-151, 10.1016/j.chroma.2012.02.032
Barcaru, A.; Anroedh-Sampat, A.; Janssen, H. G.; Vivó-Truyols, G. Retention time prediction in temperature-programmed, comprehensive two-dimensional gas chromatography: Modeling and error assessment. J. Chromatogr. A 2014, 1368, 190-198, 10.1016/j.chroma.2014.09.055
Silva, A. C. A.; Ebrahimi-Najafadabi, H.; McGinitie, T. M.; Casilli, A.; Pereira, H. M. G.; Aquino Neto, F. R.; Harynuk, J. J. Thermodynamic-based retention time predictions of endogenous steroids in comprehensive two-dimensional gas chromatography. Anal. Bioanal. Chem. 2015, 407, 4091-4099, 10.1007/s00216-015-8627-0
Burel, A.; Vaccaro, M.; Cartigny, Y.; Tisse, S.; Coquerel, G.; Cardinael, P. Retention modeling and retention time prediction in gas chromatography and flow-modulation comprehensive two-dimensional gas chromatography: The contribution of pressure on solute partition. J. Chromatogr. A 2017, 1485, 101-119, 10.1016/j.chroma.2017.01.011
Jaramillo, R.; Dorman, F. L. Retention time prediction in thermally modulated comprehensive two-dimensional gas chromatography: Correcting second dimension retention time modeling error. J. Chromatogr. A 2018, 1581-1582, 116-124, 10.1016/j.chroma.2018.10.054
Jaramillo, R.; Dorman, F. L. Retention time prediction of hydrocarbons in cryogenically modulated comprehensive two-dimensional gas chromatography: A method development and translation application. J. Chromatogr. A 2020, 1612, 460696, 10.1016/j.chroma.2019.460696
Stevenson, K. A. J. M.; Blumberg, L. M.; Harynuk, J. J. Thermodynamics-based retention maps to guide column choices for comprehensive multi-dimensional gas chromatography. Anal. Chim. Acta 2019, 1086, 133-141, 10.1016/j.aca.2019.08.011
McGinitie, T. M.; Ebrahimi-Najafabadi, H.; Harynuk, J. J. Rapid determination of thermodynamic parameters from one-dimensional programmed-temperature gas chromatography for use in retention time prediction in comprehensive multidimensional chromatography. J. Chromatogr. A 2014, 1325, 204-212, 10.1016/j.chroma.2013.12.008
Blumberg, L. M. Distribution-centric 3-parameter thermodynamic models of partition gas chromatography. J. Chromatogr. A 2017, 1491, 159-170, 10.1016/j.chroma.2017.02.047
Thewalim, Y.; Aldaeus, F.; Colmsjö, A. Retention time prediction of compounds in Grob standard mixture for apolar capillary columns in temperature-programmed gas chromatography. Anal. Bioanal. Chem. 2009, 393, 327-334, 10.1007/s00216-008-2295-2
González, F. R. Application of capillary gas chromatography to studies on solvation thermodynamics. J. Chromatogr. A 2004, 1037, 233-253, 10.1016/j.chroma.2003.11.024
Snijders, H.; Janssen, H. G.; Cramers, C. Optimization of temperature-programmed gas chromatographic separations I. Prediction of retention times and peak widths from retention indices. J. Chromatogr. A 1995, 718, 339-355, 10.1016/0021-9673(95)00692-3
Clarke, E. C. W.; Glew, D. N. Evaluation of thermodynamic functions from equilibrium constants. Trans. Faraday Soc. 1966, 62, 539, 10.1039/tf9666200539
Beens, J.; Tijssen, R.; Blomberg, J. Prediction of comprehensive two-dimensional gas chromatographic separations. J. Chromatogr. A 1998, 822, 233-251, 10.1016/s0021-9673(98)00649-9
Pesesse, R.; Stefanuto, P. H.; Schleich, F.; Louis, R.; Focant, J. F. Multimodal chemometric approach for the analysis of human exhaled breath in lung cancer patients by TD-GC × GC-TOFMS. J. Chromatogr. B: Anal. Technol. Biomed. Life Sci. 2019, 1114-1115, 146-153, 10.1016/j.jchromb.2019.01.029
Schleich, F. N.; Zanella, D.; Stefanuto, P. H.; Bessonov, K.; Smolinska, A.; Dallinga, J. W.; Henket, M.; Paulus, V.; Guissard, F.; Graff, S.; Moermans, C.; Wouters, E. F. M.; Van Steen, K.; van Schooten, F. J.; Focant, J. F.; Louis, R. Exhaled volatile organic compounds are able to discriminate between neutrophilic and eosinophilic asthma. Am. J. Respir. Crit. Care Med. 2019, 200, 444-453, 10.1164/rccm.201811-2210oc
Gaida, M.; Franchina, F. A.; Stefanuto, P. H.; Focant, J. F. Modeling approaches for temperature-programmed gas chromatographic retention times under vacuum outlet conditions. J. Chromatogr. A 2021, 1651, 462300, 10.1016/j.chroma.2021.462300
Blumberg, L. M. Temperature-Programmed Gas Chromatography; 1 st ed.; Wiley-VCH: Weinheim, 2010.
Nahir, T. M.; Morales, K. M. Constant holdup times in gas chromatography by programming of column temperature and inlet pressure. Anal. Chem. 2000, 72, 4667-4670, 10.1021/ac0004153
Weggler, B. A.; Dubois, L. M.; Gawlitta, N.; Gröger, T.; Moncur, J.; Mondello, L.; Reichenbach, S.; Tranchida, P.; Zhao, Z.; Zimmermann, R.; Zoccali, M.; Focant, J. F. A unique data analysis framework and open source benchmark data set for the analysis of comprehensive two-dimensional gas chromatography software. J. Chromatogr. A 2021, 1635, 461721, 10.1016/j.chroma.2020.461721
Vezzani, S.; Moretti, P.; Castello, G. Automatic prediction of retention times in multi-linear programmed temperature analyses. J. Chromatogr. A 1997, 767, 115-125, 10.1016/s0021-9673(96)01043-6
Vezzani, S.; Moretti, P.; Mazzi, M.; Castello, G. Prediction of retention times in linear gradient temperature and pressure programmed analysis on capillary columns. J. Chromatogr. A 2004, 1055, 151-158, 10.1016/j.chroma.2004.09.038
de Zeeuw, J. Impact of GC Parameters on The Separation: Column temperature. Sep. Sci. 2014, 6, 8-13
Lee, D. T.; Lin, A. K. Generalized delaunay triangulation for planar graphs. Discrete Comput. Geom. 1986, 1, 201-217, 10.1007/bf02187695
Semard, G.; Peulon-Agasse, V.; Bruchet, A.; Bouillon, J. P.; Cardinaël, P. Convex hull: A new method to determine the separation space used and to optimize operating conditions for comprehensive two-dimensional gas chromatography. J. Chromatogr. A 2010, 1217, 5449-5454, 10.1016/j.chroma.2010.06.048