Single photon ionization of methyl isocyanide and the subsequent unimolecular decomposition of its cation experiment and theory

International audienceMethyl isocyanide, CH3NC, is a key compound in astrochemistry and astrobiology. A combined theoretical and experimental investigation of the single photon ionization of gas phase methyl isocyanide and its fragmentation pathways is presented. Vacuum ultraviolet (VUV) synchrotron radiation based experiments are used to measure the threshold photoelectron photoion coincidence (TPEPICO) spectra between 10.6 and 15.5 eV. This allowed us to experimentally determine the adiabatic ionization energy (AIE) and fragment ion appearance energies (AE) of gas-phase methyl isocyanide. Its AIE has been measured with a precision never achieved before. It is found to be AIEexp = 11.263 ± 0.005 eV. We observe a vibrational progression upon ionization corresponding to the population of vibrational levels of the ground state of the methyl isocyanide cation. In addition, four fragment ion appearance energies (AEs) were measured to be AE (m/z 40) = 12.80 ± 0.05 eV, AE (m/z 39) = 13.70 ± 0.05, AE (m/z 15) = 13.90 ± 0.05 eV, AE (m/z 14) 13.85 ± 0.05 eV, respectively. In order to interpret the experimental data, we performed state-of-the-art computations using the explicitly correlated coupled cluster approach. We also considered the zero-point vibrational energy (ZPVE), core-valence (CV) and scalar relativistic (SR) effects. The results of theoretical calculations of the AIE and AEs are in excellent agreement with the experimental findings allowing for assignment of the fragmentations to the loss of neutral H, H2, CN and HCN upon ionization of CH3NC. The computations show that in addition to the obvious bond breakings, some of the corresponding ionic fragments result from rearrangements - upon photon absorption - either before or after electron ejection

CO-17: Polymorphismes du gène de la t-cadhérine (CDH13), adiponectinémie et indice de stéatose hépatique dans DESIR

National audienceIntroduction Le Fatty Liver Index (FLI), indice de stéatose hépatique, prédit la survenue du diabète de type 2 à 9 ans dans l'étude D.E.S.I.R. L'adiponectine est une adipocytokine insulino-sensibilisatrice inversement associée à la stéatose hépatique. Nous avons montré que les polymorphismes du gène de la t-cadhérine (CDH13), récepteur des formes actives de l'adiponectine, sont associés au diabète de type 2 et à l'adiponectinémie. Le but de notre étude est d'approfondir les relations entre variations génétiques de CDH13 et le FLI. Patients et Méthodes Quatre polymorphismes de CDH13 (rs11646213, rs12051272, rs3865188, rs4783244) ont été génotypés dans la cohorte issue de la population générale, D.E.S.I.R. Nous avons sélectionné les sujets consommant des doses d'alcool < 30 g/jour pour les hommes et < 20 g/jour pour les femmes (n = 3 650). Les concentrations initiales d'adiponectine ont été dosées chez des sujets devenus hyperglycémiques à 3 ans et des témoins normoglycémiques appariés pour le sexe, l'âge et l'indice de masse corporelle (IMC) (N = 400). Nous avons réparti le FLI en deux classes en fonction du seuil discriminant pour la survenue du diabète de type 2 dans D.E.S.I.R. (< 70 et ≥ 70). Les relations entre polymorphismes et FLI ont été estimées par régression logistique, avec ajustement sur les facteurs confondants (sexe, âge, IMC, consommation d'alcool). Résultats Dans D.E.S.I.R., le FLI est inversement corrélé à la concentration d'adiponectine (p < 0,0001). Les 4 polymorphismes sont associés au FLI. Le risque d'avoir un FLI ≥ 70, à l'entrée et à la fin de l'étude, est diminué chez les porteurs de l'allèle mineur du rs3865188 (début : OR = 0,72 [95 % IC 0,57-0,92] ; fin : OR = 0,75 [0,61-0,92]) et du rs4783244 (début : OR = 0,74 [0,58-0,95] ; fin : OR = 0,77 [0,62-0,94]). Ce risque est augmenté en début d'étude pour les porteurs de l'allèle mineur du rs12051272 (OR = 5,55 [1,19-26,0]) et en fin d'étude pour les porteurs de l'allèle mineur du rs11646213 (OR = 1,22 [1-1,49]). Les résultats restent significatifs après ajustement sur l'HbA1c. Conclusions Les polymorphismes de CDH13, associés au diabète de type 2, sont également associés au FLI dans la population française. Cette association pourrait s'expliquer par des variations d'adiponectinémie et suggérer un lien de causalit

T-cadherin gene variants are associated with type 2 diabetes and the Fatty Liver Index in the French population

International audienceAimAdiponectin is an adipocyte-secreted protein associated with insulin sensitivity. T-cadherin is a receptor for high and medium molecular weight adiponectin. In GWAS, T-cadherin gene (CDH13) polymorphisms are associated with circulating adiponectin levels. This study investigated the associations between genetic variants of CDH13 and type 2 diabetes (T2D), and its related parameters, in a Caucasian population.MethodsTwo polymorphisms of CDH13 (rs11646213 and rs3865188) were genotyped in two French cohorts, a general population from the D.E.S.I.R. study (n = 5212) and people with T2D in the DIABHYCAR study (n = 3123). Baseline adiponectin levels were measured in D.E.S.I.R. participants who were normoglycaemic at baseline, but hyperglycaemic after 3 years (n = 230), and in controls who remained normoglycaemic (n = 226) throughout.ResultsIn a cross-sectional analysis, CDH13 genotype distributions differed between those with and without T2D, with T2D odds ratios (OR) of 1.11 (95% CI: 1.04–1.18; P = 0.001) and 0.92 (95% CI: 0.87–0.98; P = 0.01) for rs11646213 and rs3865188, respectively. The rs11646213 variant, associated with a higher OR for T2D, was also associated with higher BMI (P = 0.03) and HbA1c (P = 0.006), and lower plasma adiponectin levels (P = 0.03) in the D.E.S.I.R. participants. Conversely, the rs3865188 variant, associated with a lower OR for T2D, was also associated with lower BMI (P = 0.03), HbA1c (P = 0.02) and Fatty Liver Index (FLI; P ≤ 0.01), and higher plasma adiponectin levels (P = 0.002). Associations with HbA1c, FLI and adiponectin levels persisted after adjusting for BMI.ConclusionCDH13 polymorphisms are associated with prevalent T2D in this French population study. The association may be mediated through effects on BMI and/or plasma adiponectin

VUV photoionization and dissociative photoionization of the prebiotic molecule acetyl cyanide: Theory and experiment

International audienceThe present combined theoretical and experimental investigation concerns the single photoionization of gas-phase acetyl cyanide and the fragmentation pathways of the resulting cation. Acetyl cyanide (AC) is inspired from both the chemistry of cyanoacetylene and the Strecker reaction which are thought to be at the origin of medium sized prebiotic molecules in the interstellar medium. AC can be formed by reaction from cyanoacetylene and water but also from acetaldehyde and HCN or the corresponding radicals. In view of the interpretation of vacuum ultraviolet (VUV) experimental data obtained using synchrotron radiation, we explored the ground potential energy surface (PES) of acetyl cyanide and of its cation using standard and recently implemented explicitly correlated methodologies. Our PES covers the regions of tautomerism (between keto and enol forms) and of the lowest fragmentation channels. This allowed us to deduce accurate thermochemical data for this astrobiologically relevant molecule. Unimolecular decomposition of the AC cation turns out to be very complex. The implications for the evolution of prebiotic molecules under VUV irradiation are discussed

VUV photoionization and dissociative photoionization spectroscopy of the interstellar molecule aminoacetonitrile: Theory and experiment

International audienceAminoacetonitrile (AAN) is a key compound in astrochemistry and astrobiology. We present a combined theoretical and experimental investigation concerning the single photoionization of gas-phase AAN and the fragmentation pathways of the resulting cation. At present, we measured photoelectron photoion coincidence (PEPICO) spectra in the 9.8–13.6 eV energy regime using synchrotron radiation as exciting light source. In order to interpret the VUV experimental data obtained, we explored the ground potential energy surface (PES) of AAN and of its cation using standard and explicitly correlated quantum chemical methodologies. This allowed us to deduce accurate thermochemical data for this molecule. We also determined, for the first time, the adiabatic ionization energy of AAN to lie at AIE = (10.085 ± 0.03) eV. The unimolecular decomposition pathways of the resulting AAN+ parent cation are also investigated. The appearance energies of five fragments are determined for the first time, with 30 meV accuracy. Interestingly, our work shows the possibility of the formation of both HCN and HNC isomeric forms. The implications for the evolution of prebiotic molecules under VUV irradiation are briefly discussed

Vitamin D deficiency, vitamin D receptor gene polymorphisms and cardiovascular risk factors in Caribbean patients with type 2 diabetes.

International audienceAIM: The prevalence of diabetes in the French West Indies is three times higher than in mainland France. We aimed to assess the associations between vitamin D deficiency, vitamin D receptor (VDR) gene polymorphisms and cardiovascular risk factors in Caribbean patients with type 2 diabetes (T2D). METHODS: In this cross-sectional study of 277 patients, 25-hydroxyvitamin D was measured by radioimmunoassay. FokI, BsmI, ApaI and TaqI single nucleotide polymorphisms (SNPs) of the VDR gene were genotyped. Analysis of covariance and logistic regression were performed. RESULTS: The study included 76 patients of Indian descent and 201 patients of African descent. The prevalence of vitamin D deficiency (<20 ng/mL) was 42.6%. When patients were classified into groups with (G1) and without (G2) vitamin D deficiency, there were no significant differences in age, systolic blood pressure, low-density lipoprotein cholesterol and HbA(1c), although body mass index was significantly higher in G1. Vitamin D deficiency was significantly associated with increased diastolic blood pressure and triglyceride levels, and reduced high-density lipoprotein cholesterol (P<0.05). Prevalence of vitamin D deficiency was decreased in patients carrying the f allele of FokI (OR: 0.52; P=0.02) and the aa genotype of ApaI (OR: 0.46; P=0.05). BsmI and TaqI SNPs were not associated with vitamin D deficiency. CONCLUSION: The rate of vitamin D deficiency was high in our T2D patients, and was associated with the VDR gene FokI and ApaI polymorphisms and cardiovascular risk profile. Measurements of vitamin D may help to detect T2D patients with cardiovascular risk, and VDR polymorphisms might explain why vitamin D deficiency is so frequently seen in some T2D patients

Catalase Activity, Allelic Variations In The Catalase Gene And Risk Of Kidney Complications In Patients With Type 1 Diabetes

Aims/hypothesis: Oxidative stress is involved in the pathogenesis of diabetic nephropathy. The antioxidant enzyme catalase plays a key role in redox regulation in the kidney. We investigated associations of catalase gene (CAT) polymorphisms and plasma catalase activity with diabetic nephropathy in type 1 diabetic patients. Methods: We genotyped nine single nucleotide polymorphisms (SNPs) in the CAT region in participants from the Survival Genetic Nephropathy (SURGENE) (340 French participants, 10 year follow-up) and the Génétique de la Néphropathie Diabétique (GENEDIAB) (444 Belgian and French participants, 8 year follow-up) study cohorts. Replication was performed in a Brazilian cross-sectional cohort (n = 451). Baseline plasma catalase activity was measured in SURGENE (n = 120) and GENEDIAB (n = 391) participants. Results: The A allele of rs7947841 was associated with the prevalence of incipient (OR 2.79, 95% CI 1.21, 6.24, p = 0.01) and established or advanced nephropathy (OR 5.72, 95% CI 1.62, 22.03, p = 0.007), and with the incidence of renal events, which were defined as new cases of microalbuminuria or progression to a more severe stage of nephropathy during follow-up (HR 1.82, 95% CI 1.13, 2.81, p = 0.01) in SURGENE participants. The same risk allele was associated with incipient nephropathy (OR 3.13, 95% CI 1.42, 7.24, p = 0.004) and with the incidence of end-stage renal disease (ESRD) (HR 2.11, 95% CI 1.23, 3.60, p = 0.008) in GENEDIAB participants. In both cohorts, the risk allele was associated with lower catalase activity. Associations with incipient and established or advanced nephropathy were confirmed in the replication cohort. Conclusions/interpretation: CAT variants were associated with the prevalence and incidence of diabetic nephropathy and ESRD in type 1 diabetic patients. 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