基于固液氧化还原靶向反应的能量存储技术：材料、器件及动力学

doi:10.11949/0438-1157.20231268

摘要/Abstract

摘要：

随着双碳政策的推进和可再生能源的快速发展，能源存储技术成为解决能源转型和可持续发展的关键支撑。氧化还原液流电池（RFB）是一种用于大规模储能的电化学器件，具有设计灵活、存储容量大、循环寿命长、安全性高等特点。然而受氧化还原介质分子溶解度的限制，其能量密度相对较低，同时可实用化的体系较少。为解决这一问题，基于固液氧化还原靶向反应的能量存储技术应运而生。氧化还原靶向液流电池（RTFB）在提高能量密度的同时保持良好流动性，克服了传统RFB的限制。文章综述了近年来该技术在材料、器件及动力学方面的研究进展，包括各种材料的特点、器件的设计及性能、以及动力学过程的表征与建模。最后总结当前研究的不足之处并展望未来发展趋势。

关键词: 电化学, 氧化还原靶向反应, 氧化还原靶向液流电池, 电解液, 液流电池, 化学反应器

Abstract:

With the advancement of the carbon neutrality and the rapid development of renewable energy, energy storage technology has become a crucial pillar for addressing energy transition and sustainable development. Redox flow battery (RFB) is an electrochemical device used for large-scale energy storage. It has the characteristics of flexible design, large storage capacity, long cycle life, and high safety. However, limited by the solubility of redox mediator molecules, its energy density is relatively low, and there are few practical systems. To meet this challenge, energy storage technologies based on solid-liquid redox-targeted reactions, i.e. Redox-targeted flow batteries (RTFBs) have emerged to enhance energy density, maintain excellent flowability and elevate the constraint of traditional RFBs. This review provides a comprehensive perspective of recent research progress in materials, devices, and kinetics related to RTFBs including characteristics of various materials, the design and performance of devices, as well as the characterization and modeling of kinetic processes. The bottleneck of current research is summarized and the insights into future development trends are also provided.

Key words: electrochemistry, redox targeting reactions, redox-targeted flow batteries, electrolyte, flow batteries, chemical reactors

中图分类号:

TQ 152

李云璇, 刘新悦, 陈熙, 刘文, 周明月, 蓝兴英. 基于固液氧化还原靶向反应的能量存储技术：材料、器件及动力学[J]. 化工学报, DOI: 10.11949/0438-1157.20231268.

Yunxuan LI, Xinyue LIU, Xi CHEN, Wen LIU, Mingyue ZHOU, Xingying LAN. Energy storage technologies based on solid-liquid redox targeted reactions: materials, devices, and kinetics[J]. CIESC Journal, DOI: 10.11949/0438-1157.20231268.

图/表 9

图1 （a）RFB示意图[7]；（b）RTFB示意图；（c）氧化还原介质分子S与LiFePO4等绝缘电极材料发生氧化还原靶向反应的示意图[8]；(d）氧化还原介质RM+与LiFePO4的SMRT反应的能量和电荷转移过程示意图[9]

Fig. 1 (a) Schematic diagram of RFB[7];(b) Schematic diagram of RTFB; (c) The redox-targeting reaction principle of freely diffusing shuttle molecules S and insulating electrode materials such as LiFePO4[8]; (d) Energy diagram and charge transfer of SMRT reaction between RM+ and LiFePO4[9]

表1 氧化还原电对在常规和氧化还原靶向RFB中的特点

Table 1 Characteristics of redox pairs in conventional RFB and RTFB

场景	电对的作用	电对的溶解度要求	电对与电池性能关联
常规RFB	储能介质	大于1 M	决定能量密度、功率性能
氧化还原靶向RFB	传递能量+储能	大于0.05 M	决定功率性能

图2 （a）部分金属离子的标准电极电势[16]；（b）部分有机小分子的电位及等效电子浓度对比图[33]；（c）部分插层材料的标准电极电势

Fig.2 (a) Redox potential of metal ions[16]; (b) Comparison of redox potential and equivalent electron concentration of organic small molecules[33]; (c) Redox potential of intercalation materials

表2 传统液流电池电化学性能

Table 2 Electrochemical performance of traditional flow batteries

指标	全钒电池^[54]	铁铬电池^[55]	锌铁电池^[56]	锌溴电池^[57]
能量密度*	~39.5 Wh/L	~31.2 Wh/L	~25.4 Wh/L	65 Wh/L
能量效率/%	83	70~75	83	80

图3 （a）基于氧化还原靶向反应的氧化还原钠离子液流电池示意图[45]；（b）氧化还原靶向钒液流电池（RT-VRB）示意图[58]；（c）氧化还原介导的锌-空气燃料电池（RM-ZAFC）的结构和操作示意图[69]；（d）基于氧化还原靶向反应的太阳能可充电电池示意图[70]

Fig.3 (a) Schematic diagram of a redox flow sodium-ion battery based on redox-targeting reaction[45]; (b) Schematic diagram of Redox targeting vanadium flow battery (RT-VRB)[58]; (c) Schematic diagram of the structure and operation of a redox mediated zinc air fuel cell (RM-ZAFC)[69]; (d) Schematic diagram of solar rechargeable batteries based on redox-targeting reaction[70]

图4 （a）基于双层电极电化学方法的反应动力学测定方法[82]；（b）标准PB和BG、Br2氧化PB和Br-还原BG的FTIR光谱[66]；（c）PB和Br2氧化PB的Fe 2p XPS光谱[66]；（d）充电前后的正极罐中NVP的XRD图谱[45]；（e）[Fe(CN)6]4-对原始和部分还原PB的ND模式[66]；（f）从精修ND结果的中获得的原始（底部）和还原的PB（或PW，顶部）的最可能结构[66]

Fig. 4 (a) An electrochemical approach based on a double-layer electrode to determine the reaction kinetics[82]; (b) FTIR spectra of standard PB and BG, Br2-oxidized PB, and Br--reduced BG[66]; (c) Fe 2p XPS spectra of PB and Br2-oxidized PB[66]; (d) XRD patterns of NVP collected from the catholyte tank before and after charging[45]; (e) ND patterns of pristine and partially reduced PB by [Fe(CN)6]4-[66]; (f) The most probable structures of pristine (bottom) and reduced PB (or PW, top) unit cells obtained from the refinement of ND patterns[66]

图5 （a）SECM法测定氧化还原靶向反应的界面电荷转移动力学[83]；（b）添加过量锌前后DHPS电解液的原位紫外-可见光谱[84]；（c）DHPS电解液在静置、添加过量锌和放电过程中的ATR-FTIR光谱[84]；（d）平面石英反应器中还原态FL与NVP颗粒反应后的荧光显微镜图像[45]

Fig. 5 (a) Interfacial charge-transfer kinetics of redox-targeting reactions measured by SECM[83]; (b) In situ UV-Vis spectra of DHPS electrolyte before and after addition of excess zinc[84]; (c) Operando ATR-FTIR spectra of DHPS electrolyte recorded during resting, after adding excess zinc and during discharge process[84]; (d) Fluorescence microscopic images of a planar quartz reactor filled with 20 mM fully reduced FL upon reacting with a compact NVP granule assembly[45]

图6 （a）在SMRT系统中LiFePO4固体材料利用率与标称功率和能量的相关性[9]；（b）log(ineff)-η的关系图（含极化曲线）[84]；（c）NVP/MPTZ体系中SMRT反应的动力学数据[45]；（d）LFP30被Fe(CN)63-氧化的动力学[85]

Fig. 6 (a) Utilization of LiFePO4 as a function of power in an SMRT system and Correlation of power and energy at different utilizations of solid material[9]; (b) log(ineff)- η relationship (including polarization curve) [84]; (c) Kinetic data of SMRT reaction in NVP/MPTZ system[45];(d) Oxidation kinetics of LFP30 oxidized by Fe(CN)63-[85]

图7 （a）活性材料储能罐[10]；（b）一个装满LiFePO4颗粒瓶子的照片[9]；（c）去除某种物质的吸附柱[88]；（d）一种污水处理装置[89]；（e）氧化还原靶向液流电池储能技术研究的展望

Fig. 7 (a) An energy-storage tank filled with active materials[10]; (b) Photograph of a bottle filled with LiFePO4 processed into granules[9]; (c) Adsorption column to remove a substance[88]; (d) The utility model relates to a sewage treatment device[89]; (e) Outlook for future study of redox targeted flow battery energy storage technology

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