锌—铈液流电池正极电解液的研究
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摘要
本论文对锌-铈液流电池用正极电解液进行了比较全面而深入的研究,共有六章,主要内容如下：
液流电池储能技术是一种高效的、大规模电化学储能技术,在可再生能源发电、智能电网建设等方面有广阔的应用前景。本章重点对全钒液流电池、全铬液流电池、多硫化钠-溴液流电池、锌-溴液流电池、可溶性铅酸液流电池和锌-铈液流电池等的工作原理、特点和国内外研究现状进行了综述,对部分活性物质的化学性质进行了比较详细的介绍。
本章研究了甲基磺酸介质中的Ce3+/Ce4+电极过程动力学及电解液稳定性。在石墨电极上测得Ce3+/Ce4+电极反应的标准速率常数是4.06×10-4cm s-1; Ce3+的扩散系数为5.18～5.56×10-6cm2s-1, Ce4+的扩散系数为2.56～2.68×10-cm2s-1。沉淀生成的速率与温度、浓度及充电深度有关,电解液中甲基磺酸的最佳浓度范围为2～3mol dm-3。电流密度为20mA cm-2时,锌-铈液流电池的能量效率为74.8%。
本章研究了混酸(CH3SO3H&H2SO4)介质中的Ce3+/Ce4+电极过程动力学及电解液的稳定性。在混酸介质中,Ce3+/Ce4+电极反应的标准速率常数是4.17×10-4cm s-1; Ce3+/Ce4+扩散系数比在单一酸介质中(CH3SO3H或H2SO4)都要大。铈盐在混酸中的溶解性比在硫酸中的要好,1mol dm-3Ce3++2mol dm-3CH3SO3H+0.5mol dm-3H2SO4电解液在温度高达313K时能稳定存在一个月以上。锌-铈液流电池使用混酸介质时的能量效率比使用单一甲基磺酸介质时的高。
本章研究了磺基水杨酸、DTPA、乙酸钴等添加剂对Ce3+/Ce4+电极反应动力学及电解液稳定性的影响。磺基水杨酸和DTPA等对电极反应动力学和电解液稳定性都有正面作用。乙酸钴对电极反应有正面作用,但不能改善电解液稳定性。
本章研究了多电对混合液在提高电池单位体积能量密度方面的应用。充放电实验结果显示,锌-铈&亚硝基红盐液流电池以及锌-铈＆铁液流电池的充放电容量均比锌-铈液流电池的要大。锌-铈&铁液流电池的大电流充放电性能好于锌-铈＆亚硝基红盐液流电池。
本章概述了论文的一些重要结论,以及液流电池的市场前景、发展瓶颈和发展方向。指出锌-铈液流电池技术的开发是把我国稀土资源优势变为技术优势的重要方面和重要方向。
Investigation of Ce3+/Ce4+electrolyte for zinc-cerium redox flow battery application has been intensively carried out. This paper is divided into six parts:
Redox flow cell technology is a new electrical energy storage technology with advantages of large scale and high efficiency. It can meet the great demands of boosting the wide application of the renewable resources, facilitating the construction of smart grid and accomplishing the target for energy saving and emission reduction. In this charpter, we centre around the introduction to the working principles, characteristics, research status at home and abroad of the all-vanadium, all-chromium, sodium polysulfide-bromine, zinc-bromine, soluble lead and zinc-cerium redox flow battery et al.. Chemical properties of some redox couples have been introduced detailedly.
Electrode process and electrolyte stability of Ce3+/Ce4+in methane sulfonic acid (MSA) media were investigated. The standard rate constant of the Ce3+/Ce4+electrode reaction on graphite is4.06×10-4cm s-1. The diffusion coefficient of Ce3+in MSA is5.18～5.56×10-6cm2s-1,it is2.56～2.68×10-6cm2s-1for Ce4+. The rate of electrolyte precipitation is dependent on temperature, cerium and MSA concentrations as well as the state of charge of the electrolyte. The energy efficiency of zinc-cerium redox flow cell is74.8%at20mA cm-2current.
Electrode process and electrolyte stability of Ce3+/Ce4+in mixed acid media were investigated. The standard rate constant of the Ce3+/Ce4+electrode reaction in mixed acid media is4.17×10-4cm s-1. The diffusion coefficients of Ce3+/Ce4+in mixed acid are larger than that in single acid. The solubility of cerium salt in mixed acid is larger than that in sulfuric acid; a solution of1mol dm-3Ce3+/Ce4++2mol dm-3CH3SO3H+0.5mol dm-3H2SO4is sufficiently stable for30days at temperatures up to313K. Energy efficiency of the test cell using mixed acid electrolyte is higher than that using single CH3SO3H electrolyte.
The effect of additives (sulfosalicylic acid, DTPA, Cobaltous acetate et al.) on kinetics of Ce3+/Ce4+electrode reaction and solubility of Ce3+/Ce4+electrolyte was investigated. Some additives (Sulfosalicylic acid and DTPA et al.) can improve kinetics of Ce3+/Ce4+electrode reaction and solubility of Ce3+/Ce4+electrolyte; Cobaltous acetate only has positive effect on kinetics of Ce3+/Ce4+electrode reaction without improvement of electrolyte stability.
Study of mixed electrolyte used in redox flow cell to improve volume special energy was carried out. The results show that, charge-discharge capacity of zinc-cerium&nitroso as well as zinc-cerium&ferrum redox flow cell is larger than that of zinc-cerium redox flow cell. Performance of zinc-cerium&ferrum redox flow cell is better than that of zinc-cerium&nitroso redox flow cell at large charge-discharge current.
Some important conclusions, market prospect, development bottleneck and development direction about redox flow battery were summarized in this charpter. It is pointed out that development of zinc-cerium redox flow battery technology is important area and direction for change step by step from country with rich rare earths sources to strong country with technology.
液流电池储能技术是一种高效的、大规模电化学储能技术,在可再生能源发电、智能电网建设等方面有广阔的应用前景。本章重点对全钒液流电池、全铬液流电池、多硫化钠-溴液流电池、锌-溴液流电池、可溶性铅酸液流电池和锌-铈液流电池等的工作原理、特点和国内外研究现状进行了综述,对部分活性物质的化学性质进行了比较详细的介绍。
本章研究了甲基磺酸介质中的Ce3+/Ce4+电极过程动力学及电解液稳定性。在石墨电极上测得Ce3+/Ce4+电极反应的标准速率常数是4.06×10-4cm s-1; Ce3+的扩散系数为5.18～5.56×10-6cm2s-1, Ce4+的扩散系数为2.56～2.68×10-cm2s-1。沉淀生成的速率与温度、浓度及充电深度有关,电解液中甲基磺酸的最佳浓度范围为2～3mol dm-3。电流密度为20mA cm-2时,锌-铈液流电池的能量效率为74.8%。
本章研究了混酸(CH3SO3H&H2SO4)介质中的Ce3+/Ce4+电极过程动力学及电解液的稳定性。在混酸介质中,Ce3+/Ce4+电极反应的标准速率常数是4.17×10-4cm s-1; Ce3+/Ce4+扩散系数比在单一酸介质中(CH3SO3H或H2SO4)都要大。铈盐在混酸中的溶解性比在硫酸中的要好,1mol dm-3Ce3++2mol dm-3CH3SO3H+0.5mol dm-3H2SO4电解液在温度高达313K时能稳定存在一个月以上。锌-铈液流电池使用混酸介质时的能量效率比使用单一甲基磺酸介质时的高。
本章研究了磺基水杨酸、DTPA、乙酸钴等添加剂对Ce3+/Ce4+电极反应动力学及电解液稳定性的影响。磺基水杨酸和DTPA等对电极反应动力学和电解液稳定性都有正面作用。乙酸钴对电极反应有正面作用,但不能改善电解液稳定性。
本章研究了多电对混合液在提高电池单位体积能量密度方面的应用。充放电实验结果显示,锌-铈&亚硝基红盐液流电池以及锌-铈＆铁液流电池的充放电容量均比锌-铈液流电池的要大。锌-铈&铁液流电池的大电流充放电性能好于锌-铈＆亚硝基红盐液流电池。
本章概述了论文的一些重要结论,以及液流电池的市场前景、发展瓶颈和发展方向。指出锌-铈液流电池技术的开发是把我国稀土资源优势变为技术优势的重要方面和重要方向。
Investigation of Ce3+/Ce4+electrolyte for zinc-cerium redox flow battery application has been intensively carried out. This paper is divided into six parts:
Redox flow cell technology is a new electrical energy storage technology with advantages of large scale and high efficiency. It can meet the great demands of boosting the wide application of the renewable resources, facilitating the construction of smart grid and accomplishing the target for energy saving and emission reduction. In this charpter, we centre around the introduction to the working principles, characteristics, research status at home and abroad of the all-vanadium, all-chromium, sodium polysulfide-bromine, zinc-bromine, soluble lead and zinc-cerium redox flow battery et al.. Chemical properties of some redox couples have been introduced detailedly.
Electrode process and electrolyte stability of Ce3+/Ce4+in methane sulfonic acid (MSA) media were investigated. The standard rate constant of the Ce3+/Ce4+electrode reaction on graphite is4.06×10-4cm s-1. The diffusion coefficient of Ce3+in MSA is5.18～5.56×10-6cm2s-1,it is2.56～2.68×10-6cm2s-1for Ce4+. The rate of electrolyte precipitation is dependent on temperature, cerium and MSA concentrations as well as the state of charge of the electrolyte. The energy efficiency of zinc-cerium redox flow cell is74.8%at20mA cm-2current.
Electrode process and electrolyte stability of Ce3+/Ce4+in mixed acid media were investigated. The standard rate constant of the Ce3+/Ce4+electrode reaction in mixed acid media is4.17×10-4cm s-1. The diffusion coefficients of Ce3+/Ce4+in mixed acid are larger than that in single acid. The solubility of cerium salt in mixed acid is larger than that in sulfuric acid; a solution of1mol dm-3Ce3+/Ce4++2mol dm-3CH3SO3H+0.5mol dm-3H2SO4is sufficiently stable for30days at temperatures up to313K. Energy efficiency of the test cell using mixed acid electrolyte is higher than that using single CH3SO3H electrolyte.
The effect of additives (sulfosalicylic acid, DTPA, Cobaltous acetate et al.) on kinetics of Ce3+/Ce4+electrode reaction and solubility of Ce3+/Ce4+electrolyte was investigated. Some additives (Sulfosalicylic acid and DTPA et al.) can improve kinetics of Ce3+/Ce4+electrode reaction and solubility of Ce3+/Ce4+electrolyte; Cobaltous acetate only has positive effect on kinetics of Ce3+/Ce4+electrode reaction without improvement of electrolyte stability.
Study of mixed electrolyte used in redox flow cell to improve volume special energy was carried out. The results show that, charge-discharge capacity of zinc-cerium&nitroso as well as zinc-cerium&ferrum redox flow cell is larger than that of zinc-cerium redox flow cell. Performance of zinc-cerium&ferrum redox flow cell is better than that of zinc-cerium&nitroso redox flow cell at large charge-discharge current.
Some important conclusions, market prospect, development bottleneck and development direction about redox flow battery were summarized in this charpter. It is pointed out that development of zinc-cerium redox flow battery technology is important area and direction for change step by step from country with rich rare earths sources to strong country with technology.
引文
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