水系有机液流电池正极储能材料研究进展★

doi:10.6023/A25030069

化学学报 ›› 2025, Vol. 83 ›› Issue (8): 895-916.DOI: 10.6023/A25030069 上一篇下一篇

综述

水系有机液流电池正极储能材料研究进展^★

李国宝^a^,^b, 刘睿卿^a, 季云龙^a, 王盼^b^,^*()

^a 国科大杭州高等研究院化学与材料科学学院杭州 310024
^b 西湖大学理学院杭州 310030

投稿日期:2025-03-07 发布日期:2025-03-27
通讯作者: 王盼

作者简介:

李国宝, 博士, 国科大杭州高等研究院化学与材料科学院博士后, 2022年毕业于德累斯顿工业大学化学系, 获得理学博士学位, 师从Prof. Bernd Plieker. 主要研究方向为有机合成化学与水系有机液流电池储能材料的开发.

刘睿卿, 国科大杭州高等研究院化学与材料科学院2023级硕士研究生, 研究方向为水系有机液流电池储能材料和电化学碳捕集.

季云龙, 博士, 国科大杭州高等研究院化学与材料科学院, 研究员. 2010年本科毕业于中南大学, 2015年博士毕业于中国科学院上海有机化学研究所, 2015~2019年先后在美国亚利桑那州立大学和哈佛大学进行博士后研究, 2020~2021年在浙江理工大学工作. 2021年至今在国科大杭州高等研究院工作, 主要研究水系有机液流电池与电化学碳捕集.

王盼, 博士, 西湖大学理学院特聘研究员. 2015年获中国科学院上海有机化学研究所博士学位, 2016年至2019年在麻省理工学院MIT从事博士后研究. 2019年11月加入西湖大学. 王盼实验室聚焦于有机合成化学、能源化学和材料化学交叉领域, 致力于设计和发展新材料、探索其功能性应用.

^★ “中国青年化学家”专辑.

基金资助:
国家自然科学基金(22422803); 国家自然科学基金(22101064); 国家自然科学基金(22375167); 国家重点研发计划(2022YFB2405100); 国家重点研发计划(2022YFB2405000); 国科大杭州高等研究院专项资金(2023HIAS-Y018); 浙江省自然科学基金(XHD24B0501)

Research Progress in Positive Redox-active Materials for Aqueous Organic Redox Flow Batteries^★

Guobao Li^a^,^b, Ruiqing Liu^a, Yunlong Ji^a, Pan Wang^b^,^*()

^a School of Chemistry and Materials Science, Hangzhou Institute for Advanced Study, University of Chinese Academy of Sciences, Hangzhou 310024, China
^b School of Science, Westlake University, Hangzhou 310030, China

Received:2025-03-07 Published:2025-03-27
Contact: Pan Wang
About author:
^★ For the VSI “Rising Stars in Chemistry”.
Supported by:
National Natural Science Foundation of China(22422803); National Natural Science Foundation of China(22101064); National Natural Science Foundation of China(22375167); National Key R&D Program of China(2022YFB2405100); National Key R&D Program of China(2022YFB2405000); Research Funds of Hangzhou Institute for Advanced Study, UCAS(2023HIAS-Y018); Zhejiang Provincial Natural Science Foundation of China(XHD24B0501)

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摘要/Abstract

水系有机液流电池作为一种高效、安全、性能可调的大规模储能技术, 近年来受到广泛关注. 本综述总结了水系有机液流电池正极材料的研究进展, 重点探讨了不同类型的有机正极材料, 如二茂铁及其衍生物、铁氰化物及其他铁基配合物、氮氧自由基衍生物、醌类化合物、吩噻嗪衍生物等材料的结构特性、电化学性能与电池表现. 研究表明, 通过分子设计与功能化, 有机活性分子的氧化还原电位、溶解度和稳定性均得到显著提升, 从而优化了电池整体性能. 尽管该领域取得了显著进展, 水系有机液流电池正极材料在电池长时循环稳定性、能量密度提升和成本控制等方面仍存在诸多挑战, 亟待进一步研究解决.

关键词: 水系有机液流电池, 正极储能材料, 二茂铁衍生物, 铁基配合物, 氮氧自由基

Aqueous organic redox flow batteries (AORFBs), recognized as a promising large-scale energy storage technology due to their high efficiency, inherent safety, and tunable performance characteristics, have garnered significant research interest in recent years. This review systematically summarizes recent advances in positive redox-active materials for AORFBs, with a focused analysis of representative organic electroactive species, including ferrocene derivatives, ferrocyanides/iron-based complexes, nitroxide radicals, quinones, and phenothiazine-based compounds. Through molecular engineering strategies such as functional group modification, conjugation extension, and electronic structure modulation, critical properties of organic active materials, including redox potentials, solubility in aqueous electrolytes, and chemical and electrochemical stability, have been substantially enhanced, leading to marked improvements in battery performance metrics. Despite these advancements, the practical deployment of organic positive materials continues to face challenges related to long-term cycling stability under operational conditions, limited energy density, and cost-effectiveness in scalable synthesis and processing, requiring further research and solutions.

Key words: aqueous organic redox flow battery, positive redox-active material, ferrocene derivative, iron-based complex, nitroxide radical

引用此文

李国宝, 刘睿卿, 季云龙, 王盼. 水系有机液流电池正极储能材料研究进展^★[J]. 化学学报, 2025, 83(8): 895-916.

Guobao Li, Ruiqing Liu, Yunlong Ji, Pan Wang. Research Progress in Positive Redox-active Materials for Aqueous Organic Redox Flow Batteries^★[J]. Acta Chimica Sinica, 2025, 83(8): 895-916.

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图/表 15

图1. 液流电池装置示意图和正负极储能材料充放电过程

Figure 1. Schematic representation of the redox flow battery and its charge-discharge process

图2. 水系有机液流电池负极材料研究历程

Figure 2. Treemap of the negative electrolyte (negolyte) for AORFB

图3. 水系有机液流电池正极材料研究历程

Figure 3. Treemap of the positive electrolyte (posolyte) for AORFB

年份	负极	电压/V	功率密度/ (mW•cm⁻²)	能量效率/%	容量密度/ (Ah•L⁻¹)	循环圈数/ 时间/d	容量衰减率每圈/每天/%	Ref.
2017		1.05	125	72	18.8	500/NA	0.04/NA	[31]
2017		0.75	60	80	34.8	500/14	0.057/0.1	[32]
2020	Zn	1.20	NA	83.3	40.2	1000/NA	0.0025/NA	[33]
2020		1.10	NA	80	8	100/NA	NA/NA	[34]
2020		0.66	20.24	60	42	400/32	NA/0.168	[30]
2021	ZnBr₂	1.60	NA	83.2	NA	100/NA	0.0745/NA	[35]
2022		1.13	252.7	70	26.8	2000/53.5	0/0	[36]

表1. 二茂铁类衍生物作为正极储能活性材料应用于水系有机液流电池

Table 1. Ferrocene derivatives used as posolyte in AORFBs

图4. A) FcNCl/MV液流电池示意图[31]; B) FcNCl储能活性材料降解机理; C) BTMAP-Vi与BTMAP-Fc化学结构; D) BTMAP-Vi与BTMAP-Fc循环伏安图[32]; E) BTMAP-Vi/BTMAP-Fc液流电池循环测试[32]; F)代表性的充电/放电容量电压图[32]; G)添加或不添加400 mg LiFePO4充电/放电容量电压图[33]

Figure 4. A) Schematic representation of the FcNCl/MV AORFB[31]. Adapted with permission from [31] copyright 2017 Royal Society of Chemistry; B) Degradation mechanism of FcNCl; C) Chemical structure of the BTMAP-Vi/BTMAP-Fc; D) Cyclic voltammograms of BTMAP-Vi and BTMAP-Fc[32]; E) Cycling performance of the BTMAP-Vi/BTMAP-Fc AORFB[32]; F) Representative voltage vs capacity traces of selected cycles[32]. Adapted with permission from [32] copyright 2017 American Chemical Society; G) Voltage profiles of the flow battery with and without 400 mg LiFePO4 loaded in the posolyte tank[33]. Adapted with permission from [33] copyright 2020 Elsevier

年份	负极	电压/V		能量效率/%	容量密度/ (Ah•L⁻¹)	循环圈数/ 时间/d	容量衰减率每圈/每天/%	Ref.
2019		0.82	100	62.6	24.1	1000/45.8	0/0	[38]
2020		1.40	110	75.7	NA	215/NA	0.06/NA	[39]
2021	K₂S₂	0.97	213.9	80.97	42.9	1500/30	0.002/NA	[40]
2021		1.20	NA	70	26.8	6000/200	0.008/0.25	[41]
2022		1.30	120	80	2.6	2700/25	0.0007/0.07	[42]
2023		1.19	116	60	15.2	NA/10.5	NA/0.28	[43]
2024	Zn	1.44	NA	86.09	61.64	400/24	0.0056/0.09	[43]

表2. 铁氰化物及其他铁配合物作为正极储能活性材料应用于水系有机液流电池

Table 2. Ferricyanide and other iron complex used as posolyte in AORFBs

图5. A)不同离子[Fe(CN)6]4−浓度及其溶液电池容量密度的比较[40]; B) 1.6 mol/L [Fe(CN)6]4−/K2S2液流电池进行充放电循环[40]; C) [Fe(bipy)3]2+/MV结构式; D) [Fe(py)3]2+化学结构式; E) [Fe(py)3]2+的循环伏安图[42]; F) [Fe(Bhmbpy)3]2+/BTMAP-Vi液流电池循环测试[42]

Figure 5. A) Comparison of different [Fe(CN)6]4− concentrations and their volumetric capacity[40]; B) Cycling performance of 1.6 mol/L [Fe(CN)6]4−/K2S2 AORFB[40]. Adapted with permission from [40] copyright 2021 Elsevier Science & Technology Journals. C) Chemical structure of [Fe(bipy)3]2+/MV; D) Chemical structure of [Fe(py)3]2+ derivatives; E) CV of [Fe(py)3]2+ derivatives[42]; F) Cycling performance of the [Fe(Bhmbpy)3]2+/BTMAP-Vi AORFB[42]. Adapted with permission from [42] copyright 2022 John Wiley and Sons

图6. A)不对称铁配合物结构式; B)不同铁配合物的循环伏安图[41]; C) Na4[FeII(Dcbpy)2(CN)2]/(SPr)2V液流电池测试代表性的充电/放电容量电压图[41]; D) Na4[FeII(Dcbpy)2(CN)2]/(SPr)2V液流电池进行循环测试[41]; E) FeII(TPEN)Cl2的结构式

Figure 6. A) Structural formulae of asymmetric iron complexes; B) Cyclic voltammograms of different iron complexes[41]; C) Representative voltage vs capacity traces of selected cycles for Na4[FeII(Dcbpy)2(CN)2]/(SPr)2V AORFB[41]; D) Cycling performance of the Na4[FeII(Dcbpy)2(CN)2]/(SPr)2V AORFB[41]. Adapted with permission from [41] copyright 2021 Springer Nature; E) Structural formulae of FeII(TPEN)Cl2

图7. A) TEMPO的降解过程图; B) TMAP-TEMPO/BTMAP-Vi液流电池示意图[22]; C) TMAP-TEMPO/BTMAP-Vi液流电池进行循环测试[22]

Figure 7. A) Degradation reaction of TEMPO; B) Schematic representation of the TMAP-TEMPO/BTMAP-Vi AORFB[22]; C) Cycling performance of the TMAP-TEMPO/BTMAP-Vi AORFB[22]. Adapted with permission from [22] copyright 2019 Elsevier

年份	负极	电压/V	功率密度/ (mW•cm⁻²)	能量效率/%	容量密度/ (Ah•L⁻¹)	循环圈数/ 时间/d	容量衰减率每圈/每天/%	Ref.
2015		1.25	NA	61.5	56.3	100/NA	0.11/NA	[21]
2015		1.10	NA	80	10	10000/NA	NA/NA	[50]
2016		1.40	NA	75	54	100/NA	0/NA	[51]
2017	Zn	1.69	NA	85	26.7	1100/9	NA/NA	[52]
2019		1.19	134	86	123.8	1000/NA	0.007/NA	[22]
2019	Zn	1.64	NA	98.2	NA	400/NA	0.55/NA	[53]
2021		1.19	NA	64	67	400/NA	0.06/NA	[54]
2021		1.30	NA	70.6	37.6	100/NA	NA/NA	[55]
2021		1.31	NA	78.5	NA	500/NA	0.04/NA	[56]
2022		1.35	114	70.3	80.4	400/NA	0/NA	[48]
2022		1.57	317	84	89.8	1000/14	0.05/3.47	[57]
2022		1.61	509	80	53.6	1200/16	0.021/0.7	[58]
2022	Zn	1.71	186.7	65.5	40.2	120/16.7	0.0069/0.05	[59]
2023		1.22	325	86.1	101	400/96	0/0	[60]
2025		1.12	135	82	61.6	300/NA	0.0018/NA	[61]
2025		1.32	196	74.6	56	200/NA	0.04/0.48	[62]

表3. TEMPO衍生物作为正极储能活性材料应用于水系有机液流电池

Table 3. TEMPO derivatives used as posolyte in AORFBs

图8. A) Pyr-TEMPO/[PyrPV]Cl4液流电池示意图[57]; B) Pyr-TEMPO/[PyrPV]Cl4循环伏安图[57]; C) (TPABPy)Cl3的循环伏安图[63]; D) MIAcNH-TEMPO的循环伏安图[59]; E) 4-CO2Na-TEMPO的循环伏安图[54]; F) 4-SO3K-TEMPO的循环伏安图[52]

Figure 8. A) Schematic representation of the Pyr-TEMPO/[PyrPV]Cl4 AORFB[57]; B) CV of Pyr-TEMPO/[PyrPV]Cl4[57]. Adapted with permission from [57] copyright 2022 John Wiley and Sons; C) CV of (TPABPy)Cl3[63]. Adapted with permission from [63] copyright 2019 John Wiley and Sons; D) CV of MIAcNH-TEMPO[59]. Adapted with permission from [59] copyright 2022 John Wiley and Sons; E) CV of 4-CO2Na-TEMPO[54]. Adapted with permission from [54] copyright 2021 American Chemical Society; F) CV of 4-SO3K-TEMPO[52]. Adapted with permission from [52] copyright 2017 American Chemical Society

图9. A) CPL, CPD和CT的循环伏安曲线图[56]; B) TMA-TEMPO和TPP-TEMPO的循环伏安曲线图[61]; C) TPP-TEMPO/BTMAP-Vi液流电池进行循环测试[61]; D) Mor-TEMPO和BTMAP-Vi的循环伏安曲线图[62]; E) Mor-TEMPO/BTMAP-Vi液流电池进行循环测试[62]

Figure 9. A) CV curves of CPL, CPD and CT[56]. Adapted with permission from [56] copyright 2021 John Wiley and Sons; B) CV curves of TMA-TEMPO and TPP-TEMPO[61]; C) Cycling performance of the TPP-TEMPO/BTMAP-Vi AORFB[61]. Adapted with permission from [61] copyright 2025 Springer Nature; D) CV curves of Mor-TEMPO and BTMAP-Vi[62]; E) Cycling performance of the Mor-TEMPO/BTMAP-Vi AORFB[62]. Adapted with permission from [62] copyright 2025 Elsevier

年份	负极	电压/V	功率密度/ (mW•cm⁻²)	能量效率/%	容量密度/ (Ah•L⁻¹)		循环圈数/ 时间/d	容量衰减率每圈/每天/%	Ref.
2016		0.76	NA	70	NA		100/NA	NA	[64]
2019	Zn	1.99	NA	70.2	5.36		50/NA	0.08/2.22	[65]
2019	V(II)	1.12	NA	76	71		50/NA	0.074/0.76	[66]
2021	Zn	1.40	230	80	22.5		300/NA	NA/NA	[67]
2022	Zn	1.00	53	76.5	2.68		2500/27	0/0	[68]
2023	V(II)	1.10	NA	70	47		300/22	0.0056/0.077	[69]
2024	H₄[SiW₁₂O₄₀]	1.05	230		83	37.5	250/22	0.05/0.56	[70]
2025	V(II)	NA	203.78		86	89	5200/60	0/0	[71]
2025		0.51	NA		72.55	52.26	1000/NA	NA/NA	[72]

表4. 醌类化合物、吩噻嗪化合物和其他自由基类作为正极储能活性材料应用于水系有机液流电池

Table 4. Quinone derivatives, phenothiazine derivatives, and other radical compounds used as posolyte in AORFBs

图10. A)吩噻嗪衍生物循环伏安曲线图[66]; B)空气中稳定的MBH22+自由基; C) BHAP/V液流电池循环测试[69]

Figure 10. A) CV curves of PTZ-based derivatives[66]. Adapted with permission from [66] copyright 2019 John Wiley and Sons; B) Air-stable MBH22+ radical; C) Cycling performance of the BHAP/V AORFB stacks[69]. Adapted with permission from [69] copyright 2023 John Wiley and Sons

图11. A) THTPA双电子氧化还原过程[67]; B) PSPR的循环伏安图[68]; C) PSPR/Zn液流电池的循环测试[68]; D) SFA-Cl转化为CSFA-Cl的氯化反应过程[70]; E) PTO-PTS/V液流电池的循环测试[71]

Figure 11. A) Two-electron transfer redox pathway of THTPA[67]. Adapted with permission from [67] copyright 2021 American Chemical Society; B) CV of PSPR[68]; C) Cycling performance of the PSPR/Zn AORFB[68]. Adapted with permission from [68] copyright 2022 American Chemical Society; D) Proposed reaction pathway from SFA-Cl to CSFA-Cl[70]. Adapted with permission from [70] copyright 2024 John Wiley and Sons; E) Cycling performance of the PTO-PTS/V AORFB[71]. Adapted with permission from [71] copyright 2025 American Chemical Society

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水系有机液流电池正极储能材料研究进展^★

Research Progress in Positive Redox-active Materials for Aqueous Organic Redox Flow Batteries^★

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水系有机液流电池正极储能材料研究进展★

Research Progress in Positive Redox-active Materials for Aqueous Organic Redox Flow Batteries★

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水系有机液流电池正极储能材料研究进展^★

Research Progress in Positive Redox-active Materials for Aqueous Organic Redox Flow Batteries^★