电化学脱盐机理及相关研究进展

doi:10.11949/0438-1157.20230661

摘要/Abstract

摘要：

电化学脱盐技术通过可逆的电化学过程实现离子固定化，是一种很有前途的节能水处理技术。有关脱盐机理的研究有助于深入了解离子传输和去除特性，进而为材料和电池的设计提供理论支持。根据电化学基本原理，可以将电化学脱盐机理分为电吸附机理与电荷转移机理两大类，后者包括氧化还原活性导电聚合物、离子插入（或插层）反应、转化反应以及氧化还原活性电解质。先进表征技术（包括原位X射线技术、原位波谱技术以及其他技术）和计算机建模与仿真（包括分子动力学模拟、密度泛函理论、有限元分析）在机理分析中起到关键作用。

关键词: 电化学, 脱盐, 机理, 吸附, 电荷转移

Abstract:

Electrochemical desalination, which achieves ion immobilization through a reversible electrochemical process, is a promising energy-saving water treatment technology. The study of desalination mechanisms helps to gain a deeper understanding of ion transport and removal characteristics, thereby providing theoretical support for the design of materials and batteries. According to the basic principles of electrochemistry, electrochemical desalination mechanisms can be divided into two categories: electrosorption mechanisms and charge transfer mechanisms. The latter includes redox active conductive polymers, ion insertion (or intercalation) reactions, conversion reactions, and redox active electrolytes. Advanced characterization technologies (including in situ X-ray technology, in situ spectroscopy technology and other technologies) and computer modeling and simulation (including molecular dynamics simulation, density functional theory, and finite element analysis) play a key role in mechanism analysis.

Key words: electrochemistry, desalination, mechanism, adsorption, charge transfer

中图分类号:

P 747

齐元帅, 彭文朝, 李阳, 张凤宝, 范晓彬. 电化学脱盐机理及相关研究进展[J]. 化工学报, 2024, 75(1): 171-189.

Yuanshuai QI, Wenchao PENG, Yang LI, Fengbao ZHANG, Xiaobin FAN. Research progress on electrochemical desalination mechanisms and related studies[J]. CIESC Journal, 2024, 75(1): 171-189.

图/表 12

图1 过去20年Web of Science使用关键词“电容去离子”或“电吸附”的出版物和被引频次记录[16]

Fig.1 Record of publications and citations over the past 20 years using the keywords ‘capacitive deionization’ or ‘electrosorption’ from the Web of Science[16]

图2 离子固定化的电化学过程[17]

Fig.2 The electrochemical process of ion immobilization[17]

图3 (a) 描述带正电荷表面双电层结构的模型[20]； (b) 固-液界面处的双电层模型(以Stern模型为例)[28]

Fig.3 (a) Models for describing the structure of an electrical double layer at a positively charged surface[20]; (b) The model of electric double layer at the solid-liquid interface (taking the Stern model as an example)[28]

图4 活化控制转变为质量转移控制的过程[27]

Fig.4 The process of transforming from activation control into quality transfer control[27]

图5 (a) 离子电吸附过程的基本电荷补偿机理：未充电状态下的同离子排斥、离子交换和反离子吸附[26]；(b) 随着电极电荷增加，电荷补偿发生演变：由未充电状态经两个离子交换过程到反离子吸附[26]；(c) 随时间变化的二维多孔电极模型示意图[38]

Fig.5 (a) The fundamental mechanism of charge compensation during the ion electrosorption process: co-ion expulsion, ion exchange, and counterion adsorption in the uncharged state[26]; (b) The evolution of electric charge compensation upon increasing electrode charge, where two subsequent ion swapping events are followed by counterion adsorption[26]; (c) Schematic diagram of a two-dimensional porous electrode model that varies with time[38]

图6 (a) 通过定制表面基团的可逆电化学反应选择性去除离子[73]；(b) 阴离子选择性氧化还原电极的电化学特征[73]；(c) 引入氧化还原活性DAAQ单元和用于阳离子去除的电化学可逆醌/对苯二酚工艺[76] （1 Å=1×10-10 m）

Fig.6 (a) Selective ion removal through the reversible electrochemical reactions of tailored surface groups[73]; (b) Electrochemical characteristics of the anion-selective redox electrode[73]; (c) Introduction of redox-active DAAQ units and the electrochemically reversible quinone/hydroquinone process for cation removal[76]

图7 离子插入型电极材料（块体层状材料、2D受限流体材料以及剥离2D材料）的优缺点(a)[78]及其电化学特征(b)[78, 83-84]

Fig.7 The advantages and disadvantages of ion-insertion-type electrode materials (a)[78] and their electrochemical characteristics (b)[78, 83-84]

图8 以Ag/AgCl反应为例的离子转化型电极材料(a)及其电化学特征(b)[103]

Fig.8 Ion-conversion-type electrode materials (a) and the electrochemical characteristics (b), as exemplified for the Ag/AgCl reaction[103]

图9 (a) 氧化还原活性电解质的电化学脱盐机理[111]；(b) 各种阴极电解质和阳极电解质的氧化还原电对的标准氧化还原电势[112]

Fig.9 (a) Electrochemical desalination mechanisms with redox-active electrolytes[111]; (b) Standard redox potentials of various catholyte and anolyte redox couples[112]

图10 原位XRD技术和原位SAXS技术在电化学脱盐机理研究中的应用[114, 116, 118]

Fig.10 Application of in situ XRD and in situ SAXS in the study of electrochemical desalination mechanisms[114, 116, 118]

图11 原位FTIR技术、原位Raman技术和原位NMR技术在电化学脱盐机理研究中的应用[120, 123, 128-129]

Fig.11 Application of in situ FTIR, in situ Raman and in situ NMR in the study of electrochemical desalination mechanisms[120, 123, 128-129]

图12 原位电化学石英晶体微天平在电化学脱盐机理研究中的应用[131, 134]

Fig.12 Application of in situ electrochemical quartz crystal microbalance in the study of electrochemical desalination mechanisms[131, 134]

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