Faculty of Chemistry, Adam Mickiewicz University, Uniwersytetu Poznańskiego 8, 61 614 Poznań, Poland.
Centre for Advanced Technologies, Adam Mickiewicz University, Uniwersytetu Poznańskiego 10, 61 614 Poznań, Poland.
J Org Chem. 2021 May 7;86(9):6433-6448. doi: 10.1021/acs.joc.1c00279. Epub 2021 Apr 28.
We have proven the usability and versatility of chiral triphenylacetic acid esters, compounds of high structural diversity, as chirality-sensing stereodynamic probes and as molecular tectons in crystal engineering. The low energy barrier to stereoisomer interconversion has been exploited to sense the chirality of an alkyl substituent in the esters. The structural information are cascaded from the permanently chiral alcohol (inducer) to the stereodynamic chromophoric probe through cooperative interactions. The ECD spectra of triphenylacetic acid esters are highly sensitive to very small structural differences in the inducer core. The tendencies to maximize the C-H···O hydrogen bonds, van der Waals interactions, and London dispersion forces determine the way of packing molecules in the crystal lattice. The phenyl embraces of trityl groups allowed, to some extent, the control of molecular organization in the crystal. However, the spectrum of possible molecular arrangements is very broad and depends on the type of substituent, the optical purity of the sample, and the presence of a second trityl group in the proximity. Racemates crystallize as the solid solution of enantiomers, where the trityl group acts as a protecting group for the stereogenic center. Therefore, the absolute configuration of the inducer is irrelevant to the packing mode of molecules in the crystal.
我们已经证明了手性三苯乙酸酯作为手性感应动态探针和晶体工程中分子构筑基元的可用性和多功能性,这些化合物具有高度的结构多样性。通过立体异构相互转化的低能垒,手性三苯乙酸酯可以用于感应酯中烷基取代基的手性。通过协同相互作用,从永久手性醇(诱导剂)到动态立体发色团传递结构信息。三苯乙酸酯的 ECD 光谱对手性诱导剂核中非常小的结构差异非常敏感。最大程度地形成 C-H···O 氢键、范德华相互作用和伦敦色散力的趋势决定了分子在晶格中的堆积方式。三苯甲基基团的苯基包围在一定程度上允许控制晶体中分子的组织。然而,可能的分子排列的范围非常广泛,这取决于取代基的类型、样品的光学纯度以及在附近是否存在第二个三苯甲基基团。外消旋体结晶为对映异构体的固溶体,其中三苯甲基基团作为立体中心的保护基团。因此,诱导剂的绝对构型与晶体中分子的堆积模式无关。