Ezenwafor Oluebube F, Liu Hao, Shimizu Ken D
Department of Chemistry and Biochemistry, University of South Carolina, Columbia, SC, 29205, USA.
Chemistry. 2025 Oct 1;31(55):e02034. doi: 10.1002/chem.202502034. Epub 2025 Jul 29.
A supramolecular protecting group (sPG) was developed that can selectively protect dicarboxylic acids, enabling the preferential esterification of monocarboxylic acids. The high selectivity (selectivity factor s = 72) was achieved through reversible hydrogen bonding and measured under synthetically relevant conditions. This strategy offers an efficient and dynamic alternative to traditional covalent protecting groups. To deepen understanding and optimize the performance of the supramolecular approach, a systems chemistry model was developed, which was validated by the good agreement with experimental results. The computational model was then used to explore parameter space and define selectivity-limiting factors. The insights gained from the model guided the optimization of reaction conditions and provided general principles for using supramolecular protecting groups (sPGs). This strategy is expected to have broad implications for the development of new synthetic tools for efficient and selective organic chemical transformations in the selective functionalization of complex molecules.
开发了一种超分子保护基团(sPG),它可以选择性地保护二元羧酸,从而实现一元羧酸的优先酯化。通过可逆氢键作用实现了高选择性(选择性因子s = 72),并在合成相关条件下进行了测量。该策略为传统的共价保护基团提供了一种高效且动态的替代方案。为了加深对超分子方法的理解并优化其性能,开发了一种系统化学模型,该模型通过与实验结果的良好吻合得到了验证。然后使用该计算模型探索参数空间并确定选择性限制因素。从模型中获得的见解指导了反应条件的优化,并为使用超分子保护基团(sPGs)提供了一般原则。预计该策略将对开发用于复杂分子选择性官能化中高效和选择性有机化学转化的新合成工具产生广泛影响。