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Adsorption, desorption, and surface-promoted hydrolysis of Glucose-1-phosphate in Aqueous Goethite (α-FeOOH) Suspensions

机译:针铁矿(α-FeO​​OH)悬浮液中1-磷酸葡萄糖的吸附,解吸和表面促进水解

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摘要

Adsorption, desorption, and precipitation reactions at environmental interfaces govern the fate of phosphorus in terrestrial and aquatic environments. Typically, a substantial part of the total pool of phosphorus consists of organophosphate, and in this study we have focused on the interactions between glucose-1-phosphate (G1P) and goethite (α-FeOOH) particles. The adsorption and surface-promoted hydrolysis reactions have been studied at room temperature as a function of pH, time, and total concentration of G1P by means of quantitative batch experiments in combination with infrared spectroscopy. A novel simultaneous infrared and potentiometric titration (SIPT) technique has also been used to study the rates and mechanisms of desorption of the surface complexes. The results have shown that G1P adsorption occurs over a wide pH interval and at pH values above the isoelectric point of goethite (IEP(goethite) = 9.4), indicating a comparatively strong interaction with the particle surfaces. As evidenced by IR spectroscopy, G1P formed pH-dependent surface complexes on goethite, and investigations of both adsorption and desorption processes were consistent with a model including three types of surface complexes. These complexes interact monodentately with surface Fe but differ in hydrogen bonding interactions via the auxiliary oxygens of the phosphate group. The apparent desorption rates were shown to be influenced by reaction pathways that include interconversion of surface species, which highlights the difficulty in determining the intrinsic desorption rates of individual surface complexes. Desorption results have also indicated that the molecular structures of surface complexes and the surface charge are two important determinants of G1P desorption rates. Finally, this study has shown that surface-promoted hydrolysis of G1P by goethite is base-catalyzed but that the extent of hydrolysis was small.
机译:环境界面的吸附,解吸和沉淀反应控制着陆地和水生环境中磷的命运。通常,磷总量中的很大一部分由有机磷酸酯组成,在本研究中,我们着重研究了葡萄糖-1-磷酸(G1P)与针铁矿(α-FeO​​OH)颗粒之间的相互作用。通过定量分批实验结合红外光谱技术,研究了室温下吸附和表面促进的水解反应与pH,时间和G1P总浓度的关系。新型同时红外和电位滴定(SIPT)技术也已用于研究表面复合物解吸的速率和机理。结果表明,G1P吸附发生在较宽的pH间隔内,且pH值高于针铁矿的等电点(IEP(goethite)= 9.4),表明与颗粒表面的相互作用较强。正如红外光谱所证明的那样,G1P在针铁矿上形成了pH依赖的表面配合物,吸附和解吸过程的研究均与包含三种类型的表面配合物的模型一致。这些络合物与表面Fe单齿相互作用,但通过磷酸基团的辅助氧在氢键相互作用上有所不同。已表明表观解吸速率受反应途径的影响,这些反应途径包括表面物种的相互转化,这突出说明了确定各个表面复合物的固有解吸速率的难度。解吸结果还表明,表面配合物的分子结构和表面电荷是G1P解吸速率的两个重要决定因素。最后,该研究表明,针铁矿表面促进的G1P水解是碱催化的,但水解程度很小。

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