Probing Ionophore Selectivity in Argon-Tagged Hydrated Alkali Metal Ion-Crown Ether Systems

被引:46
作者
Rodriguez, Jason D. [1 ]
Lisy, James M. [1 ]
机构
[1] Univ Illinois, Dept Chem, Urbana, IL 61801 USA
基金
美国国家科学基金会;
关键词
EFFECTIVE CORE POTENTIALS; GAS-PHASE CONFORMATIONS; INFRARED-SPECTROSCOPY; AB-INITIO; CLUSTER IONS; MOLECULAR CALCULATIONS; CYCLIC POLYETHERS; INTERNAL ENERGY; COMPLEXES; CATIONS;
D O I
10.1021/ja107383c
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Crown ethers are an important family of compounds that are closely related to naturally occurring ionophores. Thus, crown ethers are useful in modeling the size-selective behavior of ionophores. Using a combination of infrared predissociation spectroscopy and density functional theory calculations, we have investigated M(+)(18-crown-6 ether)(H(2)O)(1-4) Ar complexes, where M = Li, Na, K, Rb and Cs in the gas phase. The argon-tagging technique was used to lower the internal energies (effective temperatures similar to 100 K), yielding well-resolved spectra in the OH stretching region for systems containing up to three waters. Spectral changes were monitored as both the size of the ion and degree of hydration were varied. While there is not a particular spectroscopic signature of gas-phase selectivity reported in this work, the unique role that K(+) plays in the systems studied, as a "bridge" between the smaller and larger alkali metal ions, is consistent with the well-known special affinity for K(+) by 18-crown-6 ether in the aqueous phase.
引用
收藏
页码:11136 / 11146
页数:11
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