电容去离子除氯电极的构建及其脱盐性能研究进展

电容去离子技术(Capacitive deionization,CDI)是一种新兴的脱盐技术,通过在电极两端施加较低的外加电场除去水中的带电离子和分子,由于其较低的能耗和可持续性而备受关注。基于储能电池领域近年来的迅猛发展,CDI电极材料实现了从以双电层作用机理为代表的碳材料到法拉第电极材料的跨越,使得脱盐性能有了大幅度提升。Na⁺的去除与Cl^-的去除同等重要,然而,CDI中针对氯离子高效去除的电极材料研究关注较少。本文从CDI装置的构型演变发展出发,系统地归纳与梳理了CDI中关于脱氯电极材料的分类,对比了不同类型脱氯电极材料的特点,并总结了Cl^-去除的机理,分别为基于双电层的电吸附、转化反应、离子插层和氧化还原反应。本文是首篇关于CDI阳极材料的进展综述和展望,为CDI除氯电极的后续研究提供理论基础和研究思路。     

海水淡化用碳基电极材料及电容去离子技术研究进展

电容去离子技术(Capacitive Deionization,CDI)可以通过断电或电极反接方式使盐离子脱附,达到电极再生的目的,实现电极的可循环利用,其在海水淡化处理技术中具有独特的优势,逐渐成为一种缓和淡水资源紧缺和水污染的极具前景的技术手段。近年来,CDI处理技术正在向电极高效、无二次污染方向转变,未来将进一步聚焦碳基电极材料功能化(碳材料,钛碳化物MXenes,掺杂改性石墨烯材料)、装置和工艺设计优化等重要方向。为深入研究CDI海水淡化技术机理,进一步探索CDI方法在实际应用中的潜力,分别对CDI的脱盐机理、电极材料、装置和工艺设计对电吸附效率和性能的研究进展进行了总结,回顾CDI脱盐效果与电极材料、CDI电池装置设计等因素之间的密切关系,并对CDI技术在海水淡化中的研究发展提出展望。     

石墨烯基电极材料的设计和构建及其在电容去离子中的应用

电容去离子(CDI)是一种通过静电力作用将离子从水中去除的技术,电极是整个装置中为最为核心的部件,石墨烯因具有优异的导电性和巨大的比表面积等优势成为当前CDI电极材料的研究热点之一。目前对于CDI石墨烯电极的研究主要集中于石墨烯电极的合成,然而有关CDI性能与石墨烯电极制作工艺及电极材料自身结构之间的关系,缺少相关综述。本文系统介绍了CDI的基本原理与性能指标,综述了石墨烯电极材料的研究进展与电极制作工艺,重点分析、归纳和总结了石墨烯材料的特性(孔隙结构、导电性、亲疏水性)对CDI性能的影响,最后对CDI中石墨烯电极材料今后的发展进行了总结和展望。     

钙钛矿型LaCoO3电化学储锂的形貌调制效应

采用不同方法制备了块状(Bulk)、 纳米球状(NPs)及三维有序多孔(3DPF)钙钛矿型LaCoO₃电极材料, 并考察了材料的形貌、 结构与电化学储锂之间的相关性. 结果表明, 不同形貌的电极材料均呈钙钛矿型晶体结构, 但电化学储锂性能却表现出巨大差异: 在500 mA/g的电流密度下, 块状、 纳米球状及三维有序多孔LaCoO₃电极经350次循环后放电比容量分别为157, 579和648 mA·h/g. 电化学性能的迥异主要归因于所制备的纳米及多孔结构使活性材料与电解液之间的接触面积增大, 反应活性位点明显增多, 传质电阻降低, 从而使电子传输和Li离子的嵌入/脱嵌过程得到显著改善.     

电容去离子过渡金属基电极设计及应用研究进展北大核心CSCD

电容去离子(Capacitive deionization,CDI)作为一种新兴的水淡化和离子分离方法,由于其离子选择性高、水回收率高和能耗低等优点受到广泛关注。与传统的基于碳电极的CDI相比,新兴的法拉第电极通过离子捕获的法拉第反应,提供了使得CDI的脱盐性能大幅提升的独特机会。而过渡金属基电极由于其高度可逆的法拉第响应,相对较高的导电性以及出色的理论赝电容值等优势,在CDI电极设计领域受到广泛关注。本文系统地归纳和梳理了过渡金属基电极在CDI应用中的材料分类,总结了针对其本征缺陷所进行改性工程,主要包括导电材料耦合、功能结构工程和缺陷工程等,并对其在海水淡化中的性能进行了总结;此外,从离子选择性分离、金属离子去除和营养元素回收等方面介绍了过渡金属基电极在CDI中的特定应用。最后,概述了剩余的挑战和研究方向,为未来的过渡金属基电极的开发与研究提供指导。     

嵌锂石墨充电机制的abinitio和DFT理论研究

用ab initio/HFt DFT/B3LYP方法探究了在锂离子二次电池中锂离子在石墨负 电极材料里可逆脱过程。理论计算结果表明，嵌锂石墨LIG充放电机制是锂在石黑 碳层间可闹乱子嵌脱，同时伴随着锂与碳层间发生电荷连续转移和碳层堆积方式改 变的协同过程；计算结果也明确证实，嵌锂石墨嵌入脱出锂离子的过程就是锂离子 二次电池储存与释放能量的过程，提出的嵌锂石墨充放电机制较好地丰富了固体电 解质相界面SEI机理和单电子还原机理。     

嵌锂石墨充电机制的abinitio和DFT理论研究

用ab initio/HFt DFT/B3LYP方法探究了在锂离子二次电池中锂离子在石墨负 电极材料里可逆脱过程。理论计算结果表明，嵌锂石墨LIG充放电机制是锂在石黑 碳层间可闹乱子嵌脱，同时伴随着锂与碳层间发生电荷连续转移和碳层堆积方式改 变的协同过程；计算结果也明确证实，嵌锂石墨嵌入脱出锂离子的过程就是锂离子 二次电池储存与释放能量的过程，提出的嵌锂石墨充放电机制较好地丰富了固体电 解质相界面SEI机理和单电子还原机理。     

电容去离子用功能化电极吸附材料的设计与构建

电容去离子(CDI)是近年来新兴的一种脱盐技术,由于其具有节能环保、实用性强等优势而倍受青睐。作为该技术核心的电极吸附材料,应具有高比表面积、良好导电性、亲水性、适宜孔隙结构、优异的稳定性等特点。这将有效保障该CDI器件不仅具有高CDI脱盐效率,而且拥有更强的循环稳定性。本文结合我们前期研究工作,针对吸附电极的制备、结构与性能构效关系的差异,综述了近年来多种功能化电极材料在CDI技术应用中的最新进展。     

电容去离子脱盐装置构型的研究进展

电容去离子(CDI)技术是一种新型的海水淡化技术,因其具有环境友好、操作简单和能耗低等优势而受到广大研究者的关注。在CDI技术中,电吸附的性能与装置的构型有着密切的联系。本文综述了目前常见的几种CDI装置,包括膜电容去离子(MCDI)、流动电极电容去离子(FCDI)、杂化电极电容去离子(HCDI)、反式电极电容去离子(i-CDI)以及脱盐电池(DB),对这几种装置的发展历程和装置构型进行介绍,最后,对CDI的装置构型在未来的研究发展方向进行了展望,以期为CDI装置在电脱盐领域的研究和应用提供参考。     

有序中孔纳米多晶TiO~2薄膜的Li^+嵌脱行为

以三嵌段高分子非离子表面活性剂为结构导向剂,在非水条件下,合成了具有均一孔径分布(6.5nm)、高比表面积的稳定的中孔纳米多晶TiO~2薄膜。用循环伏安与电位阶跃技术研究了薄膜的Li^+离子嵌入反应。结果表明,由非离子表面活性剂导向而成的中孔TiO~2薄膜具有较大的Li^+离子嵌入容量,伏安特性中双电层电容效应非常显著,Li^+离子在脱嵌过程中电荷传递系数在0.15～0.4之间,嵌入系数为(4.7～55)×10^-^1^2cm^2/s。这些结果显示了具有大的比表面中孔TiO~2薄膜具有不同一般Li^+离子嵌入TiO~2薄膜的电化学反应特征。     

Relation between the charge efficiency of activated carbon fiber and its desalination performance

Four types of activated carbon fibers (ACFs) with different specific surface areas (SSA) were used as electrode materials for water desalination using capacitive deionization (CDI). The carbon fibers were characterized by scanning electron microscopy and N(2) adsorption at 77 K, and the CDI process was investigated by studying the salt adsorption, charge transfer, and also the charge efficiency of the electric double layers that are formed within the micropores inside the carbon electrodes. It is found that the physical adsorption capacity of NaCl by the ACFs increases with increasing Brunauer-Emmett-Teller (BET) surface area of the fibers. However, the two ACF materials with the highest BET surface area have the lowest electrosorptive capability. Experiments indicate that the charge efficiency of the double layers is a key property of the ACF-based electrodes because the ACF material which has the maximum charge efficiency also shows the highest salt adsorption capacity for CDI.     

Electrode Materials for Desalination of Water via Capacitive Deionization

Recent years have seen the emergence of capacitive deionization (CDI) as a promising desalination technique for converting sea and wastewater into potable water, due to its energy efficiency and eco-friendly nature. However, its low salt removal capacity and parasitic reactions have limited its effectiveness. As a result, the development of porous carbon nanomaterials as electrode materials have been explored, while taking into account of material characteristics such as morphology, wettability, high conductivity, chemical robustness, cyclic stability, specific surface area, and ease of production. To tackle the parasitic reaction issue, membrane capacitive deionization (mCDI) was proposed which utilizes ion-exchange membranes coupled to the electrode. Fabrication techniques along with the experimental parameters used to evaluate the desalination performance of different materials are discussed in this review to provide an overview of improvements made for CDI and mCDI desalination purposes     

Graphene–carbon 2D heterostructures with hierarchically-porous P,N-doped layered architecture for capacitive deionization

Exploring a new-family of carbon-based desalinators to optimize their performances beyond the current commercial benchmark is of significance for the development of practically useful capacitive deionization (CDI) materials. Here, we have fabricated a hierarchically porous N,P-doped carbon–graphene 2D heterostructure (denoted NPC/rGO) by using metal–organic framework (MOF)-nanoparticle-driven assembly on graphene oxide (GO) nanosheets followed by stepwise pyrolysis and phosphorization procedures. The resulting NPC/rGO-based CDI desalinator exhibits ultrahigh deionization performance with a salt adsorption capacity of 39.34 mg g⁻¹ in a 1000 mg L⁻¹ NaCl solution at 1.2 V over 30 min with good cycling stability over 50 cycles. The excellent performance is attributed to the high specific surface area, high conductivity, favorable meso-/microporous structure together with nitrogen and phosphorus heteroatom co-doping, all of which are beneficial for the accommodation of ions and charge transport during the CDI process. More importantly, NPC/rGO exhibits a state-of-the-art CDI performance compared to the commercial benchmark and most of the previously reported carbon materials, highlighting the significance of the MOF nanoparticle-driven assembly strategy and graphene–carbon 2D heterostructures for CDI applications.

MOF nanoparticle-driven assembly on 2D nanosheets produces the graphene–carbon heterostructure with hierarchically-porous P,N-doped layered architecture.     

Role of titania incorporated on activated carbon cloth for capacitive deionization of NaCl solution

Adsorption isotherms of NaCl on activated carbon cloth (ACC) and titania-incorporated activated carbon cloth (Ti-ACC) under an electric field were investigated to deduce the role of titania in capacitive deionization (CDI) of NaCl. Electrosorption of NaCl on the ACC was significantly increased by titania incorporation, whereas its physical adsorption was considerably decreased, resulting in an improved performance of the Ti-ACC as a CDI electrode. Langmuir isotherms based on a localized and fixed amount of adsorption were suitable for the simulation of electrosorption and physical adsorption of ions on the ACC electrodes. The variances of q(m) and b of Langmuir isotherms with electric potential indicate increases in the number of ions per adsorption site and in electrosorption strength of ions by titania incorporation. A cyclic voltammetric study for ion adsorption on ACC electrodes confirms the reversibility between electrosorption and desorption of ions, regardless of titania incorporation.     

The electrochemistry of activated carbonaceous materials: past, present, and future

Carbonaceous materials are widely used in electrochemistry. All allotropic forms of carbons??graphite, glassy carbon, amorphous carbon, fullerenes, nanotubes, and doped diamond??are used as important electrode materials in all fields of modern electrochemistry. Examples include graphite and amorphous carbons as anode materials in high-energy density rechargeable Li batteries, porous carbon electrodes in sensors and fuel cells, nano-amorphous carbon as a conducting agent in many kinds of composite electrodes (e.g., cathodes based on intercalation inorganic host materials for batteries), glassy carbon and doped diamond as stable robust and high stability electrode materials for all aspects of basic electrochemical studies, and more. Amorphous carbons can be activated to form very high specific surface area (yet stable) electrode materials which can be used for electrostatic energy storage and conversion [electrical double-layer capacitors (EDLC)] and separation techniques based on electro-adsorption, such as water desalination by capacitive de-ionization (CDI). Apart from the many practical aspects of activated carbon electrodes, there are many highly interesting and important basic aspects related to their study, including transport phenomena, molecular sieving behavior, correlation between electrochemical behavior and surface chemistry, and more. In this article, we review several important aspects related to these electrode materials, in a time perspective (past, present, and future), with the emphasis on their importance to EDLC devices and CDI processes.