Development of the Sequential Binding Model and Application for Anticooperative Protein Adsorption onto Charged Dendrimers
Development of the Sequential Binding Model and Application for Anticooperative Protein Adsorption onto Charged Dendrimers
复制标题
顺序结合模型的发展及其在带电树枝状聚合物上抗协同蛋白质吸附的应用
DOI：
10.1021/acs.langmuir.2c00173
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发表时间：
2022
期刊：
影响因子：
3.9
通讯作者：
Xiao Xu
中科院分区：
文献类型：
--
作者：
Xiao Xu
Langmuir结合模型提供了表征吸附过程的最简单和优雅的方法之一。尽管其广泛的应用，已经花费了巨大的努力，以进一步整合复杂的标准朗缪尔等温线，以纳入广泛的结合动力学与配体和受体之间的异质性和协同效应。在这里，我们使用统计力学作为一个方便的理论框架来描绘几个吸附过程的朗缪尔描述。对于具有大分子粘合剂双组分混合物的系统，我们推导出了两组序贯结合等温线，作为原始序贯模型的重要扩展，具有更多应用，包括非相同粘合剂系统。通过朗缪尔平衡与玻尔兹曼平衡的比较，第一次朗缪尔类模型中定义的结合自由能可以与模拟进行有意义的比较。在一个实际的例子中的溶菌酶蛋白质和带电的树枝状聚合物之间的吸附，我们已经证明了如何该系统的量热数据可以解释上述的结合模型，与吸附过程的准确描述，包括合作效应和树枝状聚合物的异质性。使用计算机模拟作为基准，我们还揭示并讨论了所提出的结合模型的优点和局限性。整个分析作为一个起点，扩展标准的朗缪尔模型，以访问更复杂的绑定过程。
The Langmuir binding model provides one of the simplest and elegant methods for characterizing an adsorption process. Despite its wide-ranging applications, enormous effort has been spent to further integrate complexity onto the standard Langmuir isotherm to incorporate a wide breadth of binding kinetics with the heterogeneity and cooperative effect among ligands and receptors. Here, we use statistical mechanics as a convenient theoretical framework to depict several adsorption processes on a Langmuir-like description. With regard to the system with a two-component mixture of macromolecular binders, we have derived the two-group sequential binding isotherm as an important extension of the original sequential model with more applications, including systems of non-identical binders. Via comparison of the Langmuir equilibrium with the Boltzmann equilibrium, for the first time the binding free energy defined in the Langmuir-like models can be meaningfully compared with simulations. In a practical example of the adsorption between the lysozyme protein and charged dendrimer, we have demonstrated how the calorimetry data of this system could be interpreted by the binding models described above, with an accurate description of the adsorption process, including the cooperative effect and dendrimer heterogeneity. Using the computer simulation as a benchmark, we also reveal and discuss the strengths and limitations of the proposed binding models. The entire analysis serves as a starting point for extending the standard Langmuir model to access more complicated binding processes.