固-液界面电离/络合反应模型研究

The electrical and adsorption phenomena at solid-liquid reversible interfaces are the basic phenomena studied in the field of interfacial chemistry, and their natures are derived from the interfacial ionization/complexation reactions. Traditional interface ionization/complexation models were established upon solid-liquid systems without structural charges, and did not involve solid concentration effects. Therefore, they cannot correctly describe the interface electrical and adsorption properties of structurally charged systems. .This project aims to establish general ionization/complexation models which can be applied to both systems with and without structural charges, and to explore experimental methods for measuring model parameters, such as points of zero charge and intrinsic equilibrium constants of interfacial reactions. Emphasis will be placed on investigations of the effects of structural charges and solid concentrations on interface reactions. Experimental studies about the interface electrical and adsorption behavior will be conducted on various solid-liquid systems, single-component or multicomponent and single-site or multisite systems, consisting of structurally positively charged layered double hydroxides (LDHs) and organic-LDHs nanohybrids. Numerical simulation technique will be used to verify and optimize the models. The overall goal of this project is to enhance scientific understandings of the electrical and adsorption phenomena at solid-liquid interfaces.

固-液界面的电现象和吸附现象是界面物理化学研究的基本现象，其本质皆源于界面电离/络合反应。传统的界面电离/络合模型是以不带结构电荷的固-液体系为对象建立的，也未涉及固体浓度效应，因此不能正确地描述带结构电荷体系的界面电性能和吸附性能等。. 本课题拟构建普适型（带与不带结构电荷皆适用的）固-液界面电离/络合模型，探索模型参数（如零电荷点、界面反应特征平衡常数等）的实验测定方法，重点考察结构电荷和固体浓度对界面反应及电性能和吸附性能的影响；拟以带结构正电荷的层状双氢氧化物（LDHs）和有机-LDHs纳米杂化物为模型固体，实验研究不同（单组分或多组分、单表面位或多表面位）固-液体系的界面电性能和吸附性能，并结合数值模拟技术验证和优化理论模型。以期加深对固-液界面电现象和吸附现象的科学认识。

固-液界面的电现象和吸附现象是界面物理化学研究的基本现象，其本质皆源于界面电离/络合反应。传统的界面电离/络合模型是以不带结构电荷的固-液体系为对象建立的，不能正确地描述带结构电荷体系的界面电性能和吸附性能等。. 本研究构建了普适型（带与不带结构电荷皆适用的）固-液界面电离/络合模型，其中包含“静电-电负性”模型、“尺寸效应”模型、“动态键合平衡”模型、“特性离子效应”模型和“表面组分活度”模型等，将界面反应（吸附）特征平衡常数、电性能参数等与结构电荷密度、元素物理特性、组分比、特性吸附离子的基本物理参数和浓度、以及颗粒尺寸（表面曲率）和固体浓度等相关联，阐释了界面现象的基本特性，特别是结构电荷的影响。以(氢)氧化物、荷结构正电荷的层状双氢氧化物和荷结构负电荷的粘土等为模型固体，实验研究了固-液体系的界面反应、电性能和吸附性能等，并结合数值模拟技术对理论模型进行了验证，证明所建模型是合理的。本研究加深了对固-液界面电现象和吸附现象的科学认识。（已发表SCI收录论文30余篇）