Lu Yiyang, Qiu Tian, Bloom Brian P, Subotnik Joseph E, Waldeck David H
Chemistry Department, University of Pittsburgh, Pittsburgh, Pennsylvania 15260, United States.
Departments of Chemistry, University of Pennsylvania, Philadelphia, Pennsylvania 19104, United States.
J Phys Chem C Nanomater Interfaces. 2023 Jul 13;127(29):14155-14162. doi: 10.1021/acs.jpcc.3c01159. eCollection 2023 Jul 27.
This work uses magneto-electrochemical quartz crystal microbalance methods to study the enantiospecific adsorption of chiral molecules onto a ferromagnetic substrate. The effects of solution conditions, pH, and solvent isotope composition indicate that the kinetics of the enantiomeric adsorption depend strongly on the charge state and geometry of the adsorbate, whereas no thermodynamic contributions to enantiospecificity are found. Density functional theory calculations reveal that an interplay between the adsorbate and solvent molecules is important for defining the observed enantiospecific preference with an applied magnetic field; however, it remains unclear if intermolecular vibrational couplings contribute to the phenomenon.
这项工作采用磁电化学石英晶体微天平方法，研究手性分子在铁磁基底上的对映体特异性吸附。溶液条件、pH值和溶剂同位素组成的影响表明，对映体吸附的动力学强烈依赖于吸附质的电荷状态和几何结构，而未发现对对映体特异性有热力学贡献。密度泛函理论计算表明，吸附质与溶剂分子之间的相互作用对于在施加磁场时确定观察到的对映体特异性偏好很重要；然而，分子间振动耦合是否导致该现象仍不清楚。
