Department of Chemistry, University of Nebraska-Lincoln, Lincoln, Nebraska, United States of America.
Department of Chemistry and Biochemistry, University of Toledo, Toledo, Ohio, United States of America.
PLoS One. 2019 Feb 28;14(2):e0204194. doi: 10.1371/journal.pone.0204194. eCollection 2019.
The high affinity (KD ~ 10-15 M) of biotin for avidin and streptavidin is the essential component in a multitude of bioassays with many experiments using biotin modifications to invoke coupling. Equilibration times suggested for these assays assume that the association rate constant (kon) is approximately diffusion limited (109 M-1s-1) but recent single molecule and surface binding studies indicate that they are slower than expected (105 to 107 M-1s-1). In this study, we asked whether these reactions in solution are diffusion controlled, which reaction model and thermodynamic cycle describes the complex formation, and if there are any functional differences between avidin and streptavidin. We have studied the biotin association by two stopped-flow methodologies using labeled and unlabeled probes: I) fluorescent probes attached to biotin and biocytin; and II) unlabeled biotin and HABA, 2-(4'-hydroxyazobenzene)-benzoic acid. Both native avidin and streptavidin are homo-tetrameric and the association data show no cooperativity between the binding sites. The kon values of streptavidin are faster than avidin but slower than expected for a diffusion limited reaction in both complexes. Moreover, the Arrhenius plots of the kon values revealed strong temperature dependence with large activation energies (6-15 kcal/mol) that do not correspond to a diffusion limited process (3-4 kcal/mol). Accordingly, we propose a simple reaction model with a single transition state for non-immobilized reactants whose forward thermodynamic parameters complete the thermodynamic cycle, in agreement with previously reported studies. Our new understanding and description of the kinetics, thermodynamics, and spectroscopic parameters for these complexes will help to improve purification efficiencies, molecule detection, and drug screening assays or find new applications.
生物素与亲和素和链霉亲和素的高亲和力(KD~10-15 M)是许多生物测定中必不可少的组成部分,许多实验都使用生物素修饰来引发偶联。这些测定的平衡时间假设缔合速率常数(kon)近似为扩散限制(109 M-1s-1),但最近的单分子和表面结合研究表明,它们比预期的要慢(105 到 107 M-1s-1)。在这项研究中,我们询问这些溶液中的反应是否受扩散控制,哪种反应模型和热力学循环描述了复合物的形成,以及亲和素和链霉亲和素之间是否存在任何功能差异。我们使用标记和未标记的探针通过两种停流方法研究了生物素的缔合:I)荧光探针连接到生物素和生物胞嘧啶上;和 II)未标记的生物素和 HABA,2-(4'-羟基偶氮苯)-苯甲酸。天然亲和素和链霉亲和素都是同四聚体,结合数据显示结合位点之间没有协同作用。链霉亲和素的 kon 值比亲和素快,但在两种复合物中,都比扩散限制反应预期的要慢。此外,kon 值的 Arrhenius 图显示出强烈的温度依赖性,活化能很大(6-15 kcal/mol),与扩散限制过程(3-4 kcal/mol)不对应。因此,我们提出了一种简单的反应模型,其中非固定化反应物具有单一过渡态,其正向热力学参数完成热力学循环,与之前报道的研究一致。我们对这些复合物的动力学、热力学和光谱参数的新理解和描述将有助于提高纯化效率、分子检测、药物筛选测定或寻找新的应用。