Towards speciation of organically bound tritium and deuterium: Quantification of non-exchangeable forms in carbohydrate molecules. (April 2018)

• Record Type: Journal Article
• Authors: Péron, O.; Fourré, E.; Pastor, L.; Gégout, C.; Reeves, B.; Lethi, H.H.; Rousseau, G.; Baglan, N.; Landesman, C.; Siclet, F.; Montavon, G.
• Is Part Of: Chemosphere. Volume 196(2018)
• Page Start: 120
• Page End: 128
• Publication Date: 2018-04
• Subjects: Organically bound tritium -- Hydrogen isotopic exchange -- Buried tritium -- Fraction of exchangeable hydrogen; Pollution -- Periodicals; Pollution -- Physiological effect -- Periodicals; Environmental sciences -- Periodicals; Atmospheric chemistry -- Periodicals; 551.511
• DOI: 10.1016/j.chemosphere.2017.12.136
• Languages: English
• ISSNs: 0045-6535

Abstract

Abstract: An original methodology to quantitatively explore exchangeability of hydrogen isotopes in carbohydrate molecules is proposed. To access the speciation of organically bound hydrogen isotopes, isotopic exchanges were carried out under a soft path regime in the vapor phase at 20 °C with set (D, T/H) vapor pressure ratios. When steady states were reached, the fraction of exchangeable hydrogen of microcrystalline cellulose, alpha-cellulose and wheat grains were obtained and ranged from 13 to 31% (versus a theoretical value of 30%). In cellulose, and more specifically in microcrystalline cellulose, the molecular hydrogen bonds as well as the different conformations of the network seemed to decrease the hydroxyl groups of glucose units available for isotopic exchange. On the contrary, the assumed enzymatic hydrolysis of the constitutive molecules of wheat starch into low-molecular weight carbohydrate molecules enhanced the exchangeable pool. An average value of the activity between non-exchangeable organically bound tritium (NE-OBT) and non-exchangeable organically bound hydrogen was calculated for wheat grains, ( T H ) NE = 0.55 ± 0.03 Bq.g −1 of hydrogen atoms. Highlights: A methodology by equilibration under a soft path regime for determining the fraction of exchangeable hydrogen (α) is proposed. α of microcrystalline cellulose, alpha-cellulose and wheat grains ranged from 13 to 31% (versus αtheo. = 30% Hydrogen atoms buried in cellulose. A first level of speciation of organically bound tritium achieved by the calculation.