化学
吸附
生物物理学
拥挤
聚合物
氢键
疏水效应
分子动力学
分子结合
分子间力
分子
化学工程
化学物理
计算化学
有机化学
神经科学
工程类
生物
作者
Yue Wang,Chengli Xie,Yike Huang,Kai Zhou,Zhining Xia
标识
DOI:10.1021/acs.analchem.5c03729
摘要
Molecular crowding, as a crucial mechanism for regulating intermolecular interactions, has demonstrated significant application potential in materials science in recent years. This study proposes and systematically explores the enhancement effect and underlying mechanism of molecular crowding on the adsorption performance of paracetamol molecularly imprinted polymers (AMIP). By introducing glucose as a molecular crowding agent into the adsorption system of AMIP for paracetamol (APAP), the correlation between the physical parameters of the solution microenvironment and the adsorption capacity of AMIP was elucidated through nuclear magnetic resonance (NMR) transverse relaxation time and diffusion-ordered spectroscopy (DOSY) analyses. Experimental results reveal that the crowding effect emerges when the glucose concentration exceeds 10 g/L. At a glucose concentration of 500 g/L, the adsorption capacity of AMIP increases to 1.96 times that under nonmolecular crowding conditions. The primary mechanism originates from the compression of the solution's free volume by glucose through the excluded volume effect, significantly increasing the local effective concentration of APAP. Secondarily, glucose competitively binds a large number of water molecules, altering the polar microenvironment of water and weakening the hydrogen bonding between APAP and water, thereby facilitating the specific binding of APAP to AMIP. To validate the mechanism, adsorption studies on MIPs for four compounds with distinct polarities confirmed that molecular crowding enhances the adsorption capacities of both hydrophilic and hydrophobic compounds. This work provides a novel solution microenvironment strategy for optimizing MIP performance and expands the application potential of molecular crowding in the rational design of functional materials.
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