Quantitative structure-activity relationship modelling of the carcinogenic risk of nitroso compounds using regression analysis and the TOPS-MODE approach

Worldwide, legislative and governmental efforts are focusing on establishing simple screening tools for identifying those chemicals most likely to cause adverse effects without experimentally testing all chemicals of regulatory concern. This is because even the most basic biological testing of compounds of concern, apart from requiring a huge number of test animals, would be neither resource nor time effective. Thus, alternative approaches such as the one proposed here, quantitative structure-activity relationship (QSAR) modelling, are increasingly being used for identifying the potential health hazards and subsequent regulation of new industrial chemicals. This paper follows up on our earlier work that demonstrated the use of the TOPological Substructural MOlecular DEsign (TOPS-MODE) approach to QSAR modelling for predictions of the carcinogenic potency of nitroso compounds. The data set comprises 56 nitroso compounds which have been bio-assayed in female rats and administered by the oral water route. The QSAR model was able to account for about 81% of the variance in the experimental activity and exhibited good cross-validation statistics. A reasonable interpretation of the TOPS-MODE descriptors was achieved by means of bond contributions, which in turn afforded the recognition of structural alerts (SAs) regarding carcinogenicity. A comparison of the SAs obtained from different data sets showed that experimental factors, such as the sex and the oral administration route, exert a major influence on the carcinogenicity of nitroso compounds. The present and previous QSAR models combined together provide a reliable tool for estimating the carcinogenic potency of yet untested nitroso compounds and they should allow the identification of SAs, which can be used as the basis of prediction systems for the rodent carcinogenicity of these compounds.

[1]  Maykel Pérez González,et al.  The Prediction of Carcinogenicity from Molecular Structure , 2005 .

[2]  R. Benigni Structure-activity relationship studies of chemical mutagens and carcinogens: mechanistic investigations and prediction approaches. , 2005, Chemical reviews.

[3]  C. Michejda,et al.  Evidence for several demethylase enzymes in the oxidation of dimethylnitrosamine and phenylmethylnitrosamine by rat liver fractions. , 1979, Cancer research.

[4]  Hartmut Derendorf,et al.  How Important Are Gender Differences in Pharmacokinetics? , 2002, Clinical pharmacokinetics.

[5]  A. Sasco,et al.  The growing incidence of cancer: role of lifestyle and screening detection (Review). , 2007, International journal of oncology.

[6]  S. S. Singer Decomposition reactions of (hydroxyalkyl) nitrosoureas and related compounds: possible relationship to carcinogenicity. , 1985, Journal of medicinal chemistry.

[7]  W. H. Butler,et al.  N-methyl-N'-nitro-N-nitrosoguanidine-induced carcinogenesis: differential pattern of upper gastrointestinal tract tumours in Wistar rats after single or chronic oral doses. , 1993, Carcinogenesis.

[8]  A. Morales Helguera,et al.  TOPS-MODE versus DRAGON descriptors to predict permeability coefficients through low-density polyethylene. , 2003, Journal of computer-aided molecular design.

[9]  R. Boggia,et al.  Genetic algorithms as a strategy for feature selection , 1992 .

[10]  M. P. González,et al.  A topological substructural molecular design to predict soil sorption coefficients for pesticides , 2006, Molecular Diversity.

[11]  A. Tropsha,et al.  Beware of q2! , 2002, Journal of molecular graphics & modelling.

[12]  P. Goelzer,et al.  DNA adducts from N-nitrosodiethanolamine and related beta-oxidized nitrosamines in vivo: (32)P-postlabeling methods for glyoxal- and O(6)-hydroxyethyldeoxyguanosine adducts. , 2002, Chemical research in toxicology.

[13]  N. Dubrawsky Cancer statistics , 1989, CA: a cancer journal for clinicians.

[14]  Douglas M. Hawkins,et al.  The Problem of Overfitting , 2004, J. Chem. Inf. Model..

[15]  C. Thomas Gnewuch,et al.  A Critical Appraisal of the Evolution of N-Nitrosoureas as Anticancer Drugs. , 1997, Chemical reviews.

[16]  D. J. Reed,et al.  Active site specific inactivation of chymotrypsin by cyclohexyl isocyanate formed during degradation of the carcinostatic 1-(2-chloroethyl)-3-cyclohexyl-1-nitrosourea. , 1977, Biochemistry.

[17]  F. Clavel-Chapelon,et al.  Endogenous versus exogenous exposure to N-nitroso compounds and gastric cancer risk in the European Prospective Investigation into Cancer and Nutrition (EPIC-EURGAST) study. , 2006, Carcinogenesis.

[18]  K. Zwierz,et al.  Formation and metabolism of N-nitrosamines , 1998 .

[19]  Eugenio Uriarte,et al.  Stochastic-based descriptors studying peptides biological properties: modeling the bitter tasting threshold of dipeptides. , 2004, Bioorganic & medicinal chemistry.

[20]  E. Zeiger,et al.  Handbook of Carcinogenic Potency and Genotoxicity Databases , 1996 .

[21]  Romualdo Benigni,et al.  The Benigni / Bossa rulebase for mutagenicity and carcinogenicity - a module of Toxtree , 2008 .

[22]  Paola Gramatica,et al.  Statistically Validated QSARs, Based on Theoretical Descriptors, for Modeling Aquatic Toxicity of Organic Chemicals in Pimephales promelas (Fathead Minnow) , 2005, J. Chem. Inf. Model..

[23]  L. Gold,et al.  Supplement to the Carcinogenic Potency Database (CPDB): results of animal bioassays published in the general literature in 1993 to 1994 and by the National Toxicology Program in 1995 to 1996. , 1999, Environmental health perspectives.

[24]  T. Dragani,et al.  Libri Ricevuti: IARC Monographs on the Evaluation of Carcinogenic Risks to Humans , 1992 .

[25]  Feng Luan,et al.  Classification of the carcinogenicity of N-nitroso compounds based on support vector machines and linear discriminant analysis. , 2005, Chemical research in toxicology.

[26]  F. Berthou,et al.  Effect of the length of alkyl chain on the cytochrome P450 dependent metabolism of N-diakylnitrosamines. , 1996, Cancer letters.

[27]  H. Frankish 15 million new cancer cases per year by 2020, says WHO , 2003, The Lancet.

[28]  P. Choudhari,et al.  Application quantum and physico chemical molecular descriptors utilizing principal components to study mode of anticoagulant activity of pyridyl chromen-2-one derivatives. , 2009, Bioorganic & medicinal chemistry.

[29]  N. Takeichi,et al.  Effects of sex difference, gonadectomy, and estrogen on N-methyl-N-nitrosourea induced rat thyroid tumors. , 1990, Cancer research.

[30]  D. J. Reed,et al.  Inactivation of glutathione reductase by 2-chloroethyl nitrosourea-derived isocyanates. , 1978, Biochemical and biophysical research communications.

[31]  G. Eisenbrand,et al.  Urinary excretion of N-nitrosodiethanolamine administered orally to rats. , 1978, Cancer letters.

[32]  M. C. Archer,et al.  Structure-activity relationships in nitrosamine carcinogenesis. , 1976, British Journal of Cancer.

[33]  Romualdo Benigni,et al.  Mechanistic QSAR of aromatic amines: New models for discriminating between homocyclic mutagens and nonmutagens, and validation of models for carcinogens , 2007, Environmental and molecular mutagenesis.

[34]  Maykel Pérez González,et al.  Quantitative structure carcinogenicity relationship for detecting structural alerts in nitroso-compounds. , 2007, Toxicology and applied pharmacology.

[35]  K. Tew,et al.  Probes to study the effect of methyl nitrosourea on ADP-ribosylation and chromatin structure at the subunit level. , 1980, Chemico-biological interactions.

[36]  C. Goodall,et al.  Toxicity and oncogenicity of nitrosomethylaniline and nitrosomethylcyclohexylamine. , 1970, Toxicology and applied pharmacology.

[37]  Aliuska Morales Helguera,et al.  Quantitative structure carcinogenicity relationship for detecting structural alerts in nitroso-compounds: species: rat; sex: male; route of administration: water. , 2008, Toxicology and applied pharmacology.

[38]  M. A. Cabrera Pérez,et al.  Quantitative structure-carcinogenicity relationship for detecting structural alerts in nitroso compounds: species, rat; sex, female; route of administration, gavage. , 2008, Chemical research in toxicology.

[39]  William Lijinsky,et al.  Chemistry and Biology of N-Nitroso Compounds , 1992 .

[40]  Maria Helena de Aguiar Pereira e Pestana,et al.  Análise de Dados para Ciências Sociais: a Complementaridade do SPSS , 2008 .

[41]  Michael H. Abraham,et al.  Factors that influence tadpole narcosis. An LFER analysis , 1995 .

[42]  Milan Randić,et al.  Correlation of enthalphy of octanes with orthogonal connectivity indices , 1991 .

[43]  A. Jemal,et al.  Cancer Statistics, 2008 , 2008, CA: a cancer journal for clinicians.

[44]  E. Lethco,et al.  The fate of N-nitrosodiethanolamine after oral and topical administration to rats. , 1982, Food and chemical toxicology : an international journal published for the British Industrial Biological Research Association.

[45]  P. Goelzer,et al.  Microsome-mediated oxidation of N-nitrosodiethanolamine (NDELA), a bident carcinogen. , 2002, Chemical research in toxicology.

[46]  W. Prusoff,et al.  Measurement of carbamoylating activity of nitrosoureas and isocyanates by a novel high-pressure liquid chromatography assay. , 1986, Biochemical pharmacology.

[47]  Svante Wold,et al.  An assessment of the carcinogenicity of N-nitroso compounds by the SIMCA method of pattern recognition , 1981, J. Chem. Inf. Comput. Sci..

[48]  Roberto Todeschini,et al.  Handbook of Molecular Descriptors , 2002 .

[49]  G. L. Kedderis,et al.  Sex-dependent metabolism of xenobiotics. , 1998, Drug metabolism reviews.

[50]  Maykel Pérez González,et al.  Quantitative structure-carcinogenicity relationship for detecting structural alerts in nitroso compounds: species, rat; sex, female; route of administration, gavage. , 2008 .

[51]  Strategy for a future Chemicals Policy , 2001 .

[52]  Research on the Quantitative Structure-Carcinogenic Activity Relationship of N-Nitroso Compounds , 2005, 2005 IEEE Engineering in Medicine and Biology 27th Annual Conference.

[53]  W. Lijinsky Structure-activity relations in carcinogenesis by N-nitroso compounds , 2004, Cancer and Metastasis Reviews.

[54]  Maykel Pérez González,et al.  A topological sub-structural approach of the mutagenic activity in dental monomers. 1. Aromatic epoxides , 2004 .

[55]  M. Bartels,et al.  Differential adduction of proteins vs. deoxynucleosides by methyl methanesulfonate and 1-methyl-1-nitrosourea in vitro. , 2005, Rapid communications in mass spectrometry : RCM.

[56]  Jack A. Taylor,et al.  Avoided and avoidable risks of cancer. , 1997, Carcinogenesis.

[57]  K. Straif,et al.  Exposure to nitrosamines, carbon black, asbestos, and talc and mortality from stomach, lung, and laryngeal cancer in a cohort of rubber workers. , 2000, American journal of epidemiology.

[58]  Aliuska Morales Helguera,et al.  QSPR modelling with the topological substructural molecular design approach: beta-cyclodextrin complexation. , 2009, Journal of pharmaceutical sciences.

[59]  G. Eisenbrand,et al.  Urinary excretion of N-nitrosamines in rats and humans. , 1982, IARC scientific publications.

[60]  Douglas M. Hawkins,et al.  Assessing Model Fit by Cross-Validation , 2003, J. Chem. Inf. Comput. Sci..

[61]  K. Straif,et al.  Occupational exposure to NDMA and NMor in the European rubber industry. , 2007, Journal of environmental monitoring : JEM.

[62]  T. Shibuya,et al.  A review of the genotoxicity of 1-ethyl-1-nitrosourea. , 1993, Mutation research.

[63]  L. Keefer,et al.  Sex differences in the single-dose toxicokinetics of N-nitrosomethyl(2-hydroxyethyl)amine in the rat. , 1989, Cancer research.

[64]  Stephen Dunn Smiles , 1932 .

[65]  David Weininger,et al.  SMILES, a chemical language and information system. 1. Introduction to methodology and encoding rules , 1988, J. Chem. Inf. Comput. Sci..

[66]  W M Rand,et al.  Nitrosamine carcinogenicity: a quantitative Hansch-Taft structure-activity relationship. , 1978, Chemico-biological interactions.

[67]  C Helma,et al.  Data quality in predictive toxicology: reproducibility of rodent carcinogenicity experiments. , 2001, Environmental health perspectives.

[68]  James A. Platts,et al.  Estimation of Molecular Linear Free Energy Relation Descriptors Using a Group Contribution Approach , 1999, J. Chem. Inf. Comput. Sci..

[69]  E. Rogan,et al.  An investigation of the metabolism of N-nitroso-N-methylaniline by phenobarbital- and pyrazole-induced Sprague-Dawley rat liver and esophagus derived S-9. , 1987, Chemico-biological interactions.

[70]  Ramón García-Domenech,et al.  Antimicrobial Activity Characterization in a Heterogeneous Group of Compounds , 1998, J. Chem. Inf. Comput. Sci..