Department of Chemistry, University at Buffalo, The State University of New York, NY 14260-3000, USA.
Analyst. 2011 Feb 21;136(4):749-55. doi: 10.1039/c0an00707b. Epub 2010 Dec 6.
The creation of tetracycline (TC) responsive molecularly imprinted xerogels (MIXs) was investigated using electronic absorbance, liquid chromatography-ion-trap mass spectrometry (LC-ITMS), and first-principles theory. Experimental results show that the template molecule converts to its epimer, 4-epitetracycline (ETC), during the imprinting process. Additionally, end capping of the MIX surface silanols transforms TC into anhydrotetracycline (ATC) and 4-epianhydrotetracycline (EATC). Hence, despite aiming to imprint for a single analyte (TC), one simultaneously imprints for up to four analogs (TC, ETC, EATC and ATC) within a MIX. Binding studies using LC-MS showed the binding of the prepared xerogels with the four analogs. In some formulations, preferential uptake of ETC, EATC and ATC relative to the template molecule (TC) was observed. Computations of the interaction energies between silane monomers and the four analogs reveal that ETC, EATC and ATC have higher interaction energies and are more likely to be imprinted in comparison to TC.
使用电子吸收光谱法、液相色谱-离子阱质谱（LC-ITMS）和第一性原理理论研究了四环素（TC）响应性分子印迹干凝胶（MIX）的制备。实验结果表明，模板分子在印迹过程中转化为其表异构四环素（ETC）。此外，MIX 表面硅醇的端封端将 TC 转化为脱水四环素（ATC）和 4-表脱水四环素（EATC）。因此，尽管旨在印迹单一分析物（TC），但在 MIX 中同时印迹多达四种类似物（TC、ETC、EATC 和 ATC）。使用 LC-MS 进行的结合研究表明，制备的干凝胶与四种类似物结合。在某些配方中，与模板分子（TC）相比，观察到 ETC、EATC 和 ATC 的优先吸收。计算硅烷单体与四种类似物之间的相互作用能表明，ETC、EATC 和 ATC 具有更高的相互作用能，并且与 TC 相比更有可能被印迹。
