Rohl C A, Chakrabartty A, Baldwin R L
Department of Biochemistry, Stanford University, California 94305, USA.
Protein Sci. 1996 Dec;5(12):2623-37. doi: 10.1002/pro.5560051225.
The helix propagation and N-cap propensities of the amino acids have been measured in alanine-based peptides in 40 volume percent trifluoroethanol (40% TFE) to determine if this helix-stabilizing solvent uniformly affects all amino acids. The propensities in 40% TFE are compared with revised values of the helix parameters of alanine-based peptides in water. Revision of the propensities in water is the result of redefining the capping statistical weights and evaluating the helix nucleation constant with N-capping explicitly included in the helix-coil model. The propagation propensities of all amino acids increase in 40% TFE relative to water, but the increases are highly variable. In water, all beta-branched and beta-substituted amino acids are helix breakers. In 40% TFE, the propagation propensities of the nonpolar amino acids increase greatly, leaving charged and neutral polar, beta-substituted amino acids as helix breakers. Glycine and proline are strong helix breakers in both solvents. Free energy differences for helix propagation (delta delta G) between alanine and other nonpolar amino acids are twice as large in water as predicted from side-chain conformational entropies, but delta delta G values in 40% TFE are close to those predicted from side-chain entropies. This dependence of delta delta G on the solvent points to a specific role of water in determining the relative helix propensities of the nonpolar amino acids. The N-cap propensities converge toward a common value in 40% TFE, suggesting that differential solvation by water contributes to the diversity of N-cap values shown by the amino acids.
在含40%(体积分数)三氟乙醇(40% TFE)的丙氨酸基肽中测量了氨基酸的螺旋延伸和N端封端倾向,以确定这种螺旋稳定溶剂是否对所有氨基酸产生均匀影响。将40% TFE中的倾向与水中丙氨酸基肽螺旋参数的修订值进行比较。水中倾向的修订是重新定义封端统计权重并在螺旋-线团模型中明确纳入N端封端来评估螺旋成核常数的结果。相对于水,所有氨基酸在40% TFE中的延伸倾向均增加,但增加幅度差异很大。在水中,所有β分支和β取代氨基酸都是螺旋破坏者。在40% TFE中,非极性氨基酸的延伸倾向大幅增加,使带电荷和中性极性的β取代氨基酸成为螺旋破坏者。甘氨酸和脯氨酸在两种溶剂中都是强螺旋破坏者。丙氨酸与其他非极性氨基酸之间螺旋延伸的自由能差(ΔΔG)在水中是根据侧链构象熵预测值的两倍,但在40% TFE中的ΔΔG值接近根据侧链熵预测的值。这种ΔΔG对溶剂的依赖性表明水在决定非极性氨基酸相对螺旋倾向方面具有特定作用。氨基酸的N端封端倾向在40% TFE中趋向于一个共同值,这表明水的差异溶剂化作用导致了氨基酸所表现出的N端封端值的多样性。