Shenzhen Grubbs Institute, Department of Chemistry, Guangdong Provincial Key Laboratory of Catalysis and Academy for Advanced Interdisciplinary Studies, Southern University of Science and Technology, Xueyuan Blvd 1088, Shenzhen, 518055, China.
Department of Chemistry, University of Jyvaskyla, P.O. Box 35, FI-40014, Jyväskylä, Finland.
Nat Commun. 2020 Jun 2;11(1):2740. doi: 10.1038/s41467-020-16534-9.
Induced fit and conformational selection are two dominant binding mechanisms in biology. Although induced fit has been widely accepted by supramolecular chemists, conformational selection is rarely studied with synthetic systems. In the present research, we report a macrocyclic host whose binding mechanism is unambiguously assigned to conformational selection. The kinetic and thermodynamic aspects of this system are studied in great detail. It reveals that the kinetic equation commonly used for conformational selection is strictly followed here. In addition, two mathematical models are developed to determine the association constants of the same guest to the two host conformations. A "conformational selectivity factor" is defined to quantify the fidelity of conformational selection. Many details about the kinetic and thermodynamic aspects of conformational selection are revealed by this synthetic system. The conclusion and the mathematical models reported here should be helpful in understanding complex molecular recognition in both biological and synthetic systems.
诱导契合和构象选择是生物学中的两种主要结合机制。尽管诱导契合已被超分子化学家广泛接受，但构象选择在合成系统中很少被研究。在本研究中，我们报告了一种大环主体，其结合机制明确地被分配到构象选择。该系统的动力学和热力学方面得到了详细研究。结果表明，这里严格遵循了通常用于构象选择的动力学方程。此外，还开发了两个数学模型来确定同一客体与两种主体构象的结合常数。定义了一个“构象选择性因子”来量化构象选择的保真度。通过这个合成系统揭示了构象选择的动力学和热力学方面的许多细节。这里报告的结论和数学模型应该有助于理解生物和合成系统中复杂的分子识别。
