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

doi:10.6023/A25030069

Acta Chimica Sinica ›› 2025, Vol. 83 ›› Issue (8): 895-916.DOI: 10.6023/A25030069 Previous Articles Next Articles

Review

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)

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

Cite this article

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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Fig. & Tab. 15

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

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

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]

Table 1. Ferrocene derivatives used as posolyte in AORFBs

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]

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

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

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

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]

Table 3. TEMPO derivatives used as posolyte in AORFBs

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

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]

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

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

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★

RichHTML

PDF

Knowledge

Abstract

Cite this article

share this article

Fig. & Tab. 15

References 74

Related Articles 4

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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^★