Detection and binding interactions of pharmaceutical contaminants using quartz crystal microbalance – Role of adsorbate structure and surface functional group on adsorption
Detection and binding interactions of pharmaceutical contaminants using quartz crystal microbalance – Role of adsorbate structure and surface functional group on adsorption
复制标题
使用石英晶体微天平检测药物污染物和结合相互作用 – 吸附物结构和表面官能团对吸附的作用
DOI：
10.1016/j.chemosphere.2022.137075
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发表时间：
2022
期刊：
影响因子：
8.8
通讯作者：
Subir, Mahamud
中科院分区：
文献类型：
--
作者：
Olaniyan, Philomena Oluwatosin;Nadim, Md-Masuduzzaman;Subir, Mahamud
摘要假设新出现的污染物(ECs)可以与水环境中颗粒有机物和微塑料的软固体/水界面相互作用，但作用程度如何？假设可以用石英晶体微天平(QCM)这一灵敏的重量分析工具来检测EC的吸附，并且可以测量它们对不同官能团的底物的吸附能和吸附容量。这反过来又揭示了特定与非特定的交互。实验用气相色谱检测和测量了氨氯地平和卡马西平在丁基、羧基、胺和苯基功能化自组装单分子膜上的吸附，绘制了疏水效应、氢键能力和π−相互作用图。比较了这两种表面的吸附自由能(ΔG和S)和最大界面浓度(Cmax)。用紫外-可见吸收光谱对CBZ和AMP的氢键相互作用的可能性进行了溶致变色研究。结果氨氯地平和卡马西平在丁基/水界面上吸附，ΔG和S分别为−35.8±1.1和−3 7.7±0.1kJ/m ol。非特异性相互作用允许在疏水/水界面上有更大范围的cmax。CBZ不与苯基表面结合。AMP和CBZ表现出氢键，并表现出对胺和羧基自组装膜的倾向。界面化学环境和吸附产物的结构性质对EC的吸附有重要影响。
Abstract Hypothesis Emerging contaminants (ECs) can interact with soft solid/aqueous interfaces of particulate organic matter and microplastics in the aquatic environment but to what extent? It is hypothesized that EC adsorption can be detected using quartz crystal microbalance (QCM), a sensitive gravimetric tool, and their adsorption energetics and uptake capacity can be measured for various substrates of distinct functional group. This in turn reveals the specific vs. nonspecific interactions. Experiments QCM has been used to detect and measure the adsorption of selected pharmaceuticals, amlodipine (AMP) and carbamazepine (CBZ), onto butyl, carboxyl, amine, and phenyl functionalized self-assembled monolayers (SAMs), mapping out the hydrophobic effect, H-bonding capability, and π− interactions. Adsorption free energy (Δ G a d s) and maximum interfacial concentration (c max) for these surfaces are compared. Solvatochromic studies to elucidate the likelihood of H-bonding interactions for CBZ and AMP have been conducted using UV–Vis absorption spectroscopy. Findings Amlodipine and carbamazepine adsorb onto butyl/aqueous interface with respective Δ G a d s values of− 35.8±1.1 and− 37.7±0.1 kJ/mol. Nonspecific interaction allows a greater extent of c max on the hydrophobic/aqueous interface. CBZ does not bind to the phenyl surface. AMP and CBZ exhibit H-bonding and show proclivity for the amine and carboxyl SAMs. Interfacial chemical environment and adsorbate structural properties play a significant role on EC adsorption.