Basiuk V A, Khil'chevskaya E G
Instituto de Ciencias Nucleares, Universidad Nacional Autonoma de Mexico, Mexico, D.F.
Orig Life Evol Biosph. 1995 Aug;25(4):375-93. doi: 10.1007/BF01581776.
To describe quantitatively the adsorption of prebiotically important compounds of low molecular weight (amino acids, short linear peptides, cyclic dipeptides, the Krebs's cycle and other carboxylic acids, nucleosides and related phosphates) on silica surface from diluted neutral aqueous solutions, equilibrium constants (K) and free energies (-delta G) of adsorption were determined from the retention values measured by means of high-performance liquid chromatography on a silica gel column and from the isotherms measured under static conditions. For most carboxylic acids (including amino acids and linear peptides) -delta G values were negative and K < 1, thus showing very weak adsorption. Cyclic dipeptides (2,5-piperazinediones) exhibited higher adsorbability; -delta G > 0 and K > 1 were found for most of them. Influence of the structure of alpha-substituent on the adsorbability is analyzed. A linear dependence of -delta G on the number of aliphatic carbon atoms in a sorbate molecule was found for the series of aliphatic bifunctional amino acids, related dipeptides and 2,5-piperazinediones, as well as for the row from glycine to triglycyl glycine. The adsorption of nucleosides and their phosphates is characterized by much higher K and -delta G values (of the order of 10(2) and 10(4), respectively). The adsorption data available from our work and literature are summarized and discussed with implications to the Bernal's hypothesis on the roles of solid surfaces in the prebiotic formation of biopolymers from monomeric 'building blocks'.
为了定量描述低分子量的对益生元具有重要意义的化合物(氨基酸、短线性肽、环二肽、三羧酸循环及其他羧酸、核苷和相关磷酸盐)在硅胶表面从稀释的中性水溶液中的吸附情况,通过在硅胶柱上用高效液相色谱法测量保留值以及在静态条件下测量等温线,确定了吸附的平衡常数(K)和自由能(-ΔG)。对于大多数羧酸(包括氨基酸和线性肽),-ΔG值为负且K<1,因此显示出非常弱的吸附。环二肽(2,5-哌嗪二酮)表现出更高的吸附性;大多数环二肽的-ΔG>0且K>1。分析了α-取代基结构对吸附性的影响。对于一系列脂肪族双功能氨基酸、相关二肽和2,5-哌嗪二酮,以及从甘氨酸到三甘氨酰甘氨酸的序列,发现-ΔG与被吸附物分子中脂肪族碳原子数呈线性关系。核苷及其磷酸盐的吸附特征是具有高得多的K和-ΔG值(分别约为10²和10⁴)。总结并讨论了我们的工作以及文献中可得的吸附数据,并探讨了其对伯纳尔关于固体表面在由单体“构件”进行益生元生物聚合物形成过程中作用的假设的影响。