Rigidity, conformation, and solvation of native and oxidized tannin macromolecules in water-ethanol solution

化学 小角X射线散射 溶剂化 单体 支化(高分子化学) 聚合物 溶解度 结晶学 聚合 溶剂 有机化学 散射 物理 光学
作者
D. Zanchi,Petr V. Konarev,Christophe Tribet,Alain Baron,Dmitri I. Svergun,Sylvain Guyot
出处
期刊:Journal of Chemical Physics [American Institute of Physics]
卷期号:130 (24) 被引量:39
标识
DOI:10.1063/1.3156020
摘要

We studied by light scattering and small angle x-rays scattering (SAXS) conformations and solvation of plant tannins (oligomers and polymers) in mixed water-ethanol solutions. Their structures are not simple linear chains but contain about 6% of branching. Ab initio reconstruction reveals that monomers within a branch are closely bound pairwise. The chains are rather rigid, with the Kuhn length b=13±3 nm, corresponding to about 35 linearly bound monomers. Contribution of solvation layer to SAXS intensity varies in a nonmonotonic way with ethanol content ϕA, which is an indication of amphipathic nature of tannin molecules. Best solvent composition ϕAB is a decreasing function of polymerization degree N, in agreement with increasing water solubility of tannins with N. Polymers longer than b present a power-law behavior I∼Q−d in the SAXS profile at high momentum transfer Q. The monotonic decrease in d with increasing ϕA (from 2.4 in water to 1.9 in ethanol) points that the tannins are more compact in water than in ethanol, presumably due to attractive intramolecular interactions in water. Tannins were then oxidized in controlled conditions similar to real biological or food systems. Oxidation does not produce any intermolecular condensation, but generates additional intramolecular links. Some oxidation products are insoluble in water rich solvent. For that reason, we identify these species as a fraction of natural tannins called “T1” in the notation of Zanchi et al. [Langmuir 23, 9949 (2007)]. Within the fraction left soluble after oxidation, conformations of polymeric tannins, despite their higher rigidity, remain sensitive to solvent composition.
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