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ACS Applied Materials & Interfaces · 2025 · IF 8.2

Tri-chamber Polysulfide/Iodide-Based Redox Flow Batteries with Improved Coulombic Efficiency

Chao Deng,Xiaoxin Li,Mustafa Kemal Bayazit,Barun Kumar Chakrabarti,Guo-Ming Weng

The polysulfide/iodide flow battery is a promising candidate for large-scale energy storage systems, but the technology suffers from a notably low Coulombic efficiency. This phenomenon arises because the crossover of hydroxide ions triggers the disproportionation reaction of I3– ions in the posolyte. To mitigate these issues, a middle chamber filled with Na2SO4 solution is created between two cation-exchange membranes to separate the posolyte and negolyte chambers of the PSIFB, thereby constructing a trichamber reactor. This middle chamber can serve as a reservoir for the cross-transportation OH– ions during charge-discharge processes, thereby minimizing their adverse effects on the posolyte. Experimental results reveal that the introduction of the middle chamber leads to a 97.3% reduction in the concentration of OH– ions within the posolyte. Furthermore, finite element analysis demonstrates that the trichamber configuration significantly reduces the flux of OH– ions entering the posolyte, achieving levels even lower than half of those in the dual-chamber structure. This innovative architecture markedly enhances the Coulombic efficiency from approximately 78% in the dual-chamber structure to around 91% in the trichamber structure with a high-concentration electrolyte (4 M NaI and 3 M Na2S2), while concurrently sustaining a highly competitive energy density of 20.05 W h Lposolyte+negolyte–1 at 75% state-of-charge. These findings demonstrate an effective strategy for improving the performance of the polysulfide/iodide flow battery through OH– management, showing potential for developing more efficient flow battery systems for renewable energy storage applications

研究领域: 电化学能源存储 · 液流电池技术 · 电化学工程 · 可再生能源存储 · 材料科学
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JOURNAL OF POWER SOURCES · 2023 · IF 9.2

Hydrogen-bond-rich composite membrane with improved conductivity and selectivity for flow battery

Maolin Fang,Lin Qiao,Min Wu,Yujiao Ye,Mingjun Yang,Shumin Liu,Huamin Zhang,Xiangkun Ma

Flow batteries have gained remarkable attention for large scale energy storage due to high safety and high efficiency. Membrane is the key component of the flow battery , directly affecting the efficiency and power density of the battery . However, the membrane development faces the challenge of the trade off between ion conductivity and ion selectivity. Herein, we propose a strategy to break the trade off, that is to improve the ion conductivity by creating rich hydrogen bonding networks in the membrane and maintain the ion selectivity via the spatial effect of the nanoparticles . A hydrogen-bond-rich composite membrane is prepared by incorporating the titanium oxynitride (TiON) nanoparticles into the SPEEK matrix, where TiON will form –OH and –NH 2 functional groups on the surface of nanoparticles in the aqueous solution. The interaction between water molecules and –OH or –NH 2 functional groups forms continuous and rich hydrogen bonding networks in the composite membrane, which remarkably improves the ion conductivity of the membrane. As a result, the iron chromium flow battery with SPEEK/TiON composite membrane exhibits excellent performance, with an energy efficiency of 82.7% at the current density of 80 mA/cm 2 , which was 4.4% higher than that with the commercial Nafion 212 membrane.

研究领域: 材料科学 · 能源存储
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Journal of Energy Chemistry · 2022 · IF 13.599

Low-cost all-iron flow battery with high performance towards long-duration energy storage

Xiaoqi Liu,Tianyu Li,Zhizhang Yuan,Xianfeng Li

Long duration energy storage (LDES) technologies are vital for wide utilization of renewable energy sources and increasing the penetration of these technologies within energy infrastructures. Herein, we propose a low-cost alkaline all-iron flow battery by coupling ferri/ferro-cyanide redox couple with ferric/ferrous-gluconate complexes redox couple. The designed all-iron flow battery demonstrates a coulombic efficiency of above 99% and an energy efficiency of ∼83% at a current density of 80 mA cm −2 , which can continuously run for more than 950 cycles. Most importantly, the battery demonstrates a coulombic efficiency of more than 99.0% and an energy efficiency of ∼83% for a long duration (∼12, 16 and 20 h per cycle) charge/discharge process. Benefiting from the low cost of iron electrolytes, the overall cost of the all-iron flow battery system can be reached as low as $76.11 per kWh based on a 10 h system with a power of 9.9 kW. This work provides a new option for next-generation cost-effective flow batteries for long duration large scale energy storage.

研究领域: 材料科学 · 能源技术
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Energy Material Advances · 2021 · IF 0

Viologen-Decorated TEMPO for Neutral Aqueous Organic Redox Flow Batteries

Shuzhi Hu,Liwen Wang,Xianzhi Yuan,Zhipeng Xiang,Mingbao Huang,Peng Luo,Yufeng Liu,Zhiyong Fu,Zhenxing Liang

A novel electroactive organic molecule, viz., 1-(1-oxyl-2,2,6,6-tetramethylpiperidin-4-yl)-1′-(3-(trimethylammonio)propyl)-4,4′-bipyridinium trichloride ((TPABPy)Cl3), is synthesized by decorating 2,2,6,6-tetramethylpiperidin-1-oxyl (TEMPO) with viologen, which is used as the positive electrolyte in neutral aqueous redox flow battery (ARFB). Extensive characterizations are performed to investigate the composition/structure and the electrochemical behavior, revealing the favorable effect of introducing the cationic viologen group on the electroactive TEMPO. Salient findings are as follows. First, the redox potential is elevated from +0.745 V for TEMPO to +0.967 V for decorated TEMPO, favoring its use as the positive electrolyte. Such an elevation originates from the electron-withdrawing effect of the viologen unit, as evidenced by the nuclear magnetic resonance and single crystal structure analysis. Second, linear sweep voltammetry reveals that the diffusion coefficient is 2.97×10−6 cm2 s−1, and the rate constant of the one-electron transfer process is 7.50×10−2 cm s−1. The two values are sufficiently high as to ensure low concentration and kinetics polarization losses during the battery operation. Third, the permeability through anion-exchange membrane is as low as 1.80×10−11 cm2 s−1. It is understandable as the positive-charged viologen unit prevents the molecule from permeating through the anion exchange membrane by the Donnan effect. Fourth, the ionic nature features a decent conductivity and thus eliminates the use of additional supporting electrolyte. Finally, a flow battery is operated with 1.50 M (TPABPy)Cl3 as the positive electrolyte, which affords a high energy density of 19.0 Wh L-1 and a stable cycling performance with capacity retention of 99.98% per cycle.

研究领域: 化学 · 能源科学
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JOURNAL OF POWER SOURCES · 2021 · IF 9.127

Intramolecular hydrogen bonds induced high solubility for efficient and stable anthraquinone based neutral aqueous organic redox flow batteries

Lixing Xia,Wenbo Huo,Huaizhi Gao,Heng Zhang,Fengming Chu,Hao Liu,Zhan'ao Tan

Solubility of redox active materials (RAMs) is key to realize high volume capacity and energy density in aqueous organic redox flow batteries (AORFBs). In anthraquinone (AQ)-based RAMs, hydrophilic groups substituted at β-sites (2,3,6,7) are expected to improve water-miscibility much better than α-sites (1,4,5,8). In this work, we find an anomalous case: 3-((9,10-dioxo-9.10-dihydroanthracen-2-yl)amino)-N,N,N-trimethylpropan-1-aminium chloride (2-DPAQCl) functioned with the hydrophilic groups surprisingly exhibits poor solubility with less than 0.05 M, however its isomer 3-((9,10-dioxo-9,10-dihydroanthracen-1-yl)amino)-N,N,N-trimethylpropan-1-aminium chloride (1-DPAQCl) shows high solubility at 1.44 M in water. The results from 1 H nuclear magnetic resonance (NMR) and infrared (IR) spectra suggest that intermolecular hydrogen bonds (HBs) are formed between N–H donors and Cl − acceptors in 2-DPAQCl, which is different from the case for 1-DPAQCl that N–H donors interact with neighboring C O acceptors as intramolecular HBs. Benefited from the intramolecular HBs, water is prone to break the interaction between solute molecules than that in 2-DPAQCl, leading to better water-solubility. Electrochemical investigations indicate that the peak-to-peak separations ΔE pp of 1-DPAQCl is very narrow in unbuffered aqueous solution as well as in buffered aqueous solution at pH 7.0, implying its highly electrochemical reversibility and facile reaction kinetics, which further indicates 1-DPAQCl is suitable to serve as a negative RAM for neutral AORFBs.

研究领域: 材料科学 · 电化学
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CHEMICAL SOCIETY REVIEWS · 2023 ·Vol. 52 ·期 17 ·6031-6074 · IF 46.2

Development of flow battery technologies using the principles of sustainable chemistry

Ziming Zhao,Xianghui Liu,Mengqi Zhang,Leyuan Zhang,Changkun Zhang,Xianfeng Li,Guihua Yu

Realizing decarbonization and sustainable energy supply by the integration of variable renewable energies has become an important direction for energy development. Flow batteries (FBs) are currently one of the most promising technologies for large-scale energy storage. This review aims to provide a comprehensive analysis of the state-of-the-art progress in FBs from the new perspectives of technological and environmental sustainability, thus guiding the future development of FB technologies. More importantly, we evaluate the current situation and future development of key materials with key aspects of green economy and decarbonization to promote sustainable development and improve the novel energy framework. Finally, we present an analysis of the current challenges and prospects on how to effectively construct low-carbon and sustainable FB materials in the future.

CAS / MDL: 135-19-3
研究领域: 能源技术 · 环境科学
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JOURNAL OF POWER SOURCES · 2025 · IF 7.9

Covalent organic framework in-situ grown on MXenes to improve ion selectivity of composite membranes for vanadium flow battery

Xiaoyang Jia,Zhongrui Lu,Kai Huai,Xiancan Yuan,Zhuoran Yang,Rui Huang,Shaoxiong Zhai,Qing Ye,Zhanfeng Deng,Jun Lin,Shaojian He

Covalent organic frameworks (COFs) are highly porous crystalline polymers with well-defined pore structures, exhibiting great potential for the use of composite membranes to separate ions with different sizes. However, COFs are mostly insoluble and poorly dispersed in common solvents, making it very difficult to well disperse COFs in polymer matrix to prepare high-quality composite membranes. In this work, a MS hybrid was prepared by in-situ growing COFs on the surface of Ti 3 C 2 T x MXenes, which helps improve the filler-matrix compatibility significantly. The synergetic effect of the two-dimensional structure of MXene nanosheets and the porosity of COF components in MS contributes to the improvement for the ion selectivity of the composite membranes (SPEEK/MS). The vanadium flow battery (VFB) loaded with the SPEEK/MS-10 membrane achieves the energy efficiency of 93 % at 40 mA cm −2 , as compared to 86 % for that with the SPEEK control membrane. Moreover, the improved cycling stability and capacity retention was achieved for the SPEEK/MS-10 based VFB. Therefore, this work provides a promising strategy to fabricate high-performance COF-based composite PEMs for the VFB applications.

CAS / MDL: 7789-24-4
研究领域: 材料科学 · 能源技术
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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

Perovskite enables high performance vanadium redox flow battery

Yingqiao Jiang,Zihe Liu,Yanrong Lv,Ao Tang,Lei Dai,Ling Wang,Zhangxing He

Perovskites have been attractive materials in electrocatalysis due to their virtues of low cost, variety, and tuned activity. Herein, we firstly demonstrate superior electrochemical kinetics of LaBO 3 (B = V, Cr, Mn) perovskites towards vanadium redox reactions in vanadium redox flow batteries (VRFBs). LaBO 3 (B = V, Cr, Mn) perovskites present the intrinsic catalysis towards V 3+ /V 2+ and VO 2+ /VO 2 + redox reactions in order of LaMnO 3  > LaCrO 3  > LaVO 3 . The catalysis is primarily attributed to activity of B-O bindings and perovskite structure that effectively promote the adsorption of vanadium ions. Moreover, perovskite contributes more active sites to vanadium redox reactions, resulting in a boosted electron exchange for redox reactions. Full cell tests demonstrate an energy efficiency (EE) of 60% at 300 mA cm −2 using graphite felt/LaMnO 3 (GF/LaMnO 3 ) electrodes. At 200 mA cm −2 , the GF/LaMnO 3 electrodes allow a 20% increase in EE of the flow cell as compared to pristine GF. The underlying catalysis mechanism of perovskite for vanadium redox reactions is also elucidated by density function theory, which lays the groundwork for future research into development of perovskite family in VRFBs.

研究领域: 材料科学 · 电化学
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Nano Energy · 2021 · IF 17.881

An organic bifunctional redox active material for symmetric aqueous redox flow battery

Gabriel Sikukuu Nambafu,Kumar Siddharth,Cheng Zhang,Tianshou Zhao,Qing Chen,Khalil Amine,Minhua Shao

Symmetric redox flow batteries utilizing a single redox active material as catholyte and anolyte, offer a plausible and unique strategy to alleviate cross-contamination issues during cycling, making them an ideal energy storage device for large scale applications. In this work, a low-cost riboflavin organic molecule is coupled with a 2,2,6,6-Tetramethylpiperidinyl-N-oxyl (TEMPO) radical molecule to form a single Riboflavin-TEMPO (RIBOTEMPO) bifunctional redox active material, which is used in both aqueous anolyte and catholyte. Cyclic voltammetry analysis of the combined molecule displays electrochemically reversible reactions for the redox couples at −0.72 V and 0.51 V versus Hg/Hg 2 SO 4 , leading to a theoretical cell voltage of 1.23 V. A symmetric cell testing demonstrated over 100 consecutive charge/discharge cycles with nearly 80% coulombic efficiency and capacity retention of 44.7% at a current density of 2.5 mA cm −2 . By utilizing a pH neutral supporting electrolyte , a low-cost, safe, and environmental-friendly redox flow battery is achieved. This work provides a pathway for the design and development of bifunctional redox active molecules for symmetric battery applications.

CAS / MDL: 14691-88-4 130-40-5
研究领域: 化学 · 能源科学 · 材料科学
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH · 2022 ·Vol. 29 ·期 50 ·76263-76274 · IF 5.19

A magnetic chitosan for efficient adsorption of vanadium (V) from aqueous solution

Zhou Anhui,Qiu Zhaofu,Yang Ji,Yan Ruiqi

The all-vanadium redox flow battery (VRFB) is becoming a promising technology for large-scale energy storage due to its advantages such as scalability and flexibility. In recent years, the VRFB has been successfully developed and put into use in many countries. It is expected that the abandoned VRFB will generate a large amount of vanadium waste. To our knowledge, there are few reports on the disposal of spent VRFBs. Herein, chitosan-coated nano-zero-valent iron (CS-Fe 0 ) is proposed for the first time as adsorbents for the treatment of spent VRFBs. It can provide a new approach to deal with the upcoming large number of spent VRFBs. The calculated maximum adsorption capacity for V(V) of chitosan and CS-Fe 0 reached 209.5 and 511.3 mg/g at 288 K, respectively. CS-Fe 0 showed better adsorption performance than chitosan under different pH conditions and is easy to be separated from the liquid phase. The Freundlich isotherm was suitable for the adsorption process of chitosan, and CS-Fe 0 was more consistent with the Langmuir isotherm. Ionic strength (0.05–0.5 M) had a positive effect on the adsorption capacity of CS-Fe 0 , and the influence of coexisting anions on CS-Fe 0 could be negligible. FTIR and XPS analyses revealed that the primary mechanisms were the electrostatic attraction of chitosan and redox of Fe 0 . The present study confirmed that CS-Fe 0 could be a potential material to efficiently trap V(V) from the VRFB electrolyte.

研究领域: 环境科学 · 材料科学
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Carbon Neutralization · 2024 · IF 0

Core-shell Ni/NiO heterostructures as catalytic cathodes enabling high-performance zinc bromine flow batteries

Longwei Li,Rongrong Li,Shaojie Zhou,Wenjun Xu,Yu Li,Jingmin Zhang,Lei Gao,Xiong Pu

Zinc bromine flow batteries (ZBFBs) are well suited for stationary energy storage due to their attractive features of high energy density and low cost. Nevertheless, the ZBFBs suffer from low power density and limited efficiency owing to the relatively severe polarization of the Br 2 /Br − redox couple. Herein, a three-dimensional (3D) hierarchical composite electrode based on core-shell Ni/NiO heterostructures anchored on graphite felt (Ni/NiO@GF) is designed to promote the kinetics of the Br 2 /Br − couple, so as to improve the power density and efficiency of the ZBFB. In this design, the highly conductive carbon felt and Ni cores provide a composite electrode with a 3D electron transporting framework to guarantee excellent electronic conductivity, while the NiO shells possess great absorption ability to Br 2 and brilliant catalytic activity for the Br 2 /Br − redox reaction to reduce the electrochemical polarization. As a result, an enhanced ZBFB with Ni/NiO@GF electrode shows an outstanding energy efficiency of 86% at 20 mA cm −2 and can be operated at a current density of up to 160 mA cm −2 with a respectable energy efficiency of 67%. These results exhibit a promising strategy to fabricate catalytic electrodes for high-performance ZBFBs.

研究领域: 电化学 · 能源存储 · 材料科学
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Journal of Energy Storage · 2025 · IF 9.8

Bimetallic MOF-derived MnCo@C electrodes for high performance vanadium flow batteries

Fuyu Chen,Zhongjie Wang,Xuhong Yin,Xiangdong Cheng,Qiang He,Hui Chen,Qinfang Zhang

The vanadium flow battery (VFB) has garnered significant attention for its potential to enable cost-effective utilization in large-scale energy storage. Nevertheless, the electrochemical activity of electrodes is limited during vanadium redox reactions, which poses a challenge to achieving high-performance VFBs. To address this, we synthesize a catalyst consisting of amorphous carbon, manganese oxide, and cobalt, to enhance VFB performance. Initially, bimetallic metal-organic frameworks with varying Mn Co ratios are synthesized using a hydrothermal method. Subsequently, the bimetallic metal-organic frameworks are carbonized to form the catalysts. The morphology, composition, electrocatalytic activity, and charging-discharging behavior of the prepared catalysts are then systematically investigated. This paper reveals that: i) the composite with a molar ratio of manganese to cobalt of 1:4, exhibits a uniform and fine particle distribution, an abundance of oxygen-containing functional groups, and exceptional electrochemical activities; ii) it enhances the energy efficiency of VFBs by 9 % compared to those utilizing raw carbon felts and by 5 % over those with mono-MnO@C or mono-Co@C electrodes at 100 mA cm −2 ; iii) it offers significant improvements in terms of operating voltages, cell capacities, high current density characteristics, and lifespan. Consequently, this work introduces a novel electrochemical catalyst for VFBs, enhancing their performance and broadening their potential applications.

CAS / MDL: 68-12-2
研究领域: 材料科学 · 能源存储
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