Towards kinetic control of coordination self-assembly: a case study of a Pd3L6 double-walled triangle to predict the outcomes by a reaction network model
Towards kinetic control of coordination self-assembly: a case study of a Pd3L6 double-walled triangle to predict the outcomes by a reaction network model
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协调自组装的动力学控制：以 Pd3L6 双壁三角形为例，通过反应网络模型预测结果
DOI：
10.1039/d0cp04623j
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发表时间：
2020
影响因子：
3.3
通讯作者：
Hiraoka Shuichi
中科院分区：
文献类型：
--
作者：
Takahashi Satoshi;Tateishi Tomoki;Sasaki Yuya;Sato Hirofumi;Hiraoka Shuichi
对[Pd3L6]6+双壁三角形（DWT）配合物的自组装过程（NASAP）进行了数值分析。利用化学反应网络和从十八维参数空间中的数值搜索获得的反应速率常数的参数集，以获得与实验对应物（自组装过程的定量分析，QASAP）的数据的良好拟合，精细计算导致每个分子物种的详细时间演化。基于这些线索的分析揭示了占主导地位的自组装途径和分子间和分子内反应之间的平衡，并根据动力学控制下的初始化学计量比预测反应结果。
Numerical analysis of self-assembly process (NASAP) was performed for a [Pd3L6]6+ double-walled triangle (DWT) complex. With a chemical reaction network and a parameter set of the reaction rate constants obtained from a numerical search in an eighteen-dimensional parameter space to obtain a good fit to the data from the experimental counterpart (quantitative analysis of self-assembly process, QASAP), a refined calculation resulted in a detailed time evolution of each molecular species. Analysis based on those clues revealed dominant self-assembly pathways and a balance between inter- and intramolecular reactions, and enabled prediction of the reaction outcomes depending on the initial stoichiometric ratio under kinetic control.