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Parameterization of adsorption onto minerals by Extended Triple Layer Model
Applied Geochemistry ( IF 3.1 ) Pub Date : 2021-08-31 , DOI: 10.1016/j.apgeochem.2021.105087
Keisuke Fukushi 1 , Akihiro Okuyama 2 , Natsumi Takeda 2 , Shigeyori Kosugi 3
Affiliation  

Adsorption is the most important geochemical process that regulates trace element concentrations in natural water. The behavior of solutes adsorbed onto mineral surfaces depends on conditions in the solution, including pH, ionic strength, and concentrations of competing components. Surface complexation modeling (SCM) is the commonly accepted way to model the effect of variable solution conditions on adsorption. Extended Triple Layer Model (ETLM) is a SCM for ion adsorption to minerals developed by Prof. Sverjensky group. It considers adsorption reaction on mineral surfaces that contain one type of amphoteric surface hydroxyl, in combination with a triple layer model for the electrostatic interaction. The amphoteric surface hydroxyl represents an average of the actual surface sites. The ETLM implements the site occupancy standard states for the activities of surface species, which enables the direct comparison of the adsorption constants. ETLM has the minimum complexity required to realistically represent adsorption processes with the least number of parameters. The ETLM can provide predictions of adsorption behavior and surface speciation that are consistent with independent spectroscopic observations. Nowadays, ETLM can be used in many conventional geochemical codes. Practical application of ETLM in geochemical modeling will require an expansion of the inter-consistent database for the adsorption of various solutes on minerals. This review describes the theoretical background and conventions needed to estimate inter-consistent ETLM parameters. We review the surface charge characteristics of minerals in general, the experimental acquisition of their surface charges, the theory and conventions associated with the modeling of surface charges in the ETLM, and the procedure used to parameterize them. The acquisition of adequate adsorption data, the theory needed to model solute adsorption, and the procedure for parameterizing adsorption are then described. Finally, we introduce the features of a newly developed program, ETL(MIN)2, that facilitates the application of the ETLM, including model parameterization.



中文翻译:

通过扩展三层模型对矿物吸附进行参数化

吸附是调节天然水中微量元素浓度的最重要的地球化学过程。吸附在矿物表面的溶质的行为取决于溶液中的条件,包括 pH 值、离子强度和竞争成分的浓度。表面络合建模 (SCM) 是模拟可变溶液条件对吸附的影响的普遍接受的方法。扩展三层模型 (ETLM) 是 Sverjensky 教授团队开发的用于离子吸附到矿物的 SCM。它考虑了在含有一种两性表面羟基的矿物表面上的吸附反应,并结合了静电相互作用的三层模型。两性表面羟基代表实际表面位点的平均值。ETLM 实现了表面物种活动的场地占用标准状态,这使得吸附常数的直接比较成为可能。ETLM 具有以最少的参数实际表示吸附过程所需的最低复杂性。ETLM 可以提供与独立光谱观察一致的吸附行为和表面形态的预测。如今,ETLM 可用于许多常规地球化学代码。ETLM 在地球化学建模中的实际应用将需要扩展用于矿物上各种溶质吸附的一致性数据库。这篇综述描述了估计相互一致的 ETLM 参数所需的理论背景和约定。我们总体上回顾了矿物的表面电荷特征,表面电荷的实验获取,与 ETLM 中表面电荷建模相关的理论和约定,以及用于参数化它们的程序。然后描述了获得足够的吸附数据、模拟溶质吸附所需的理论以及参数化吸附的程序。最后,我们介绍一个新开发的程序 ETL(MIN) 的特点2,这有利于 ETLM 的应用,包括模型参数化。

更新日期:2021-09-07
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