Article
Chemistry, Multidisciplinary
Ruiyong Chen, Peng Zhang, Zhenjun Chang, Junfeng Yan, Tobias Kraus
Summary: This study investigates the development of sustainable design strategies for aqueous electrolytes in redox flow batteries using redox-active organic materials. A green spontaneous grafting reaction is observed between a redox-active organic radical and an electrochemically activated structural modifier at room temperature through a simple mixing step. Furthermore, a physical mixing method is utilized to formulate a structured aqueous electrolyte and enables aqueous solubilization of the organic solute beyond the conventional dissolution limit, leading to a record high discharge cell voltage in aqueous non-hybrid flow cell.
Article
Chemistry, Multidisciplinary
Zhipeng Xiang, Wenjin Li, Kai Wan, Zhiyong Fu, Zhenxing Liang
Summary: This work develops an electrochemical method to quantitatively study the aggregation behavior of methyl viologen dichloride molecules and finds that aggregation behavior can effectively regulate the molecule's energy level and redox potential. It not only provides a method to investigate molecular aggregation, but also demonstrates the feasibility to tune the performance of redox flow batteries by regulating aggregation behavior.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Xiaotong Li, Yuan Yao, Chenxi Liu, Xin Jia, Jiahuang Jian, Bao Guo, Songtao Lu, Wei Qin, Qing Wang, Xiaohong Wu
Summary: In this study, a new redox-active material lithium ferrocyanide (Li-4[Fe(CN)6]) is designed, which has high electron storage capacity and cost competitiveness. The solubility of [Fe(CN)6]4- is greatly enhanced by Li+ ions due to weak intermolecular interactions, leading to improved electrochemical performance. Coupled with zinc, ZIRFBs are built, achieving unprecedentedly high [Fe(CN)6]4- concentrations and battery energy densities. The low cost of Li-4[Fe(CN)6] makes the alkaline ZIRFB have a chemical cost as low as $11 per kWh, promoting the development of economical [Fe(CN)6]4-/3--based RFBs in the future.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Electrochemistry
Elena I. Romadina, Keith J. Stevenson
Summary: Nowadays, redox flow batteries (RFBs) are being considered as a potential solution for large-scale energy storage. The use of organic materials in RFBs can accelerate the commercialization process by being more affordable, cheap, and eco-friendly. This review provides knowledge about organic anolytes and catholytes for RFBs and encourages the development of highly soluble and electrochemically stable organic redox-active materials.
ELECTROCHIMICA ACTA
(2023)
Review
Electrochemistry
Xiao Wang, Rajeev K. Gautam, Jianbing Jimmy Jiang
Summary: Redox flow batteries (RFB) are considered as one of the most promising technologies for large-scale energy storage due to their high safety, long life and decoupled energy and power design. However, the high cost and low energy density limit further development. The development of organic RFBs is driven by the cost advantage and tunable structure of organic redox-active materials. Solubility is recognized as one of the parameters that directly affect energy density.
BATTERIES & SUPERCAPS
(2022)
Article
Chemistry, Multidisciplinary
Yan Jing, Evan Wenbo Zhao, Marc-Antoni Goulet, Meisam Bahari, Eric M. Fell, Shijian Jin, Ali Davoodi, Erlendur Jonsson, Min Wu, Clare P. Grey, Roy G. Gordon, Michael J. Aziz
Summary: Aqueous organic redox flow batteries can achieve low-cost, long-lifetime energy storage by regenerating the original molecule, 2,6-dihydroxy-anthraquinone, without the need for further structural modifications.
Article
Chemistry, Multidisciplinary
Yanxin Yao, Zengyue Wang, Zhejun Li, Yi-Chun Lu
Summary: This study presents an aqueous metal anode based on tin, which effectively addresses the severe dendrite issues in redox flow batteries. Compared to state-of-the-art zinc metal anodes, the alkaline Sn electrode demonstrates superior performance in cycling life and areal capacity.
ADVANCED MATERIALS
(2021)
Article
Chemistry, Physical
Mengqi Gao, Manohar Salla, Feifei Zhang, Yongfeng Zhi, Qing Wang
Summary: Redox flow batteries (RFBs) are a reliable and durable grid-scale electricity storage technology. The performance and cost of RFB systems are largely determined by the ion-exchange membrane (IEM), which is a critical component of RFBs. This study investigates the origin and impact of membrane fouling on RFB systems, providing useful guidance for membrane selection and optimization.
JOURNAL OF POWER SOURCES
(2022)
Review
Chemistry, Multidisciplinary
Gaojing Yang, Yaxun Zhu, Zhimeng Hao, Yong Lu, Qing Zhao, Kai Zhang, Jun Chen
Summary: Traditional redox flow batteries based on toxic redox-active metal ions have deficiencies in resource utilization and environmental protection, while organic electroactive materials in aqueous redox flow batteries (ARFBs) have attracted extensive attention for low-cost and sustainable energy storage systems due to their inherent safety. This review provides an overview of the recent progress in organic electroactive materials for ARFBs, including their main reaction types and how to regulate their solubility, potential, stability, and viscosity. The characterization methods of organic electroactive materials for ARFBs and future research directions are also discussed.
ADVANCED MATERIALS
(2023)
Article
Multidisciplinary Sciences
Kritika Sharma, Shrihari Sankarasubramanian, Javier Parrondo, Vijay Ramani
Summary: The study explored the use of organic and organometallic reactants in aqueous electrolytes for cost-effective organic redox flow batteries (ORFBs) and investigated the impact of electrolyte pH and salt anions on the performance of redox active organic cations. It was found that solvent reorganizational energy (lambda) is a universal descriptor for determining the electrochemical Thiele modulus and selecting electrolyte compositions. Low pH electrolytes with methanesulfonate or chloride counterions were identified as providing the best balance of transport and kinetic requirements for the specific BTMAP-Fc/BTMAP-Vi ORFB.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2021)
Article
Chemistry, Physical
Y. Liu, Q. Chen, P. Sun, Y. Li, Z. Yang, T. Xu
Summary: The increasing energy demand of human society drives the development and utilization of renewable energy and high-performance, cost-effective energy storage technology. Aqueous organic flow battery is a novel system with decoupled capacity and power, offering a low-cost energy storage solution.
MATERIALS TODAY ENERGY
(2021)
Article
Chemistry, Physical
Youngsu Kim, Giyun Kwon, Sung-O Park, Heechan Kim, Jihyeon Kim, Kyoungoh Kim, Jaekyun Yoo, Donghwan Lee, Kisuk Kang
Summary: Micellar solubilization enables a significant enhancement in solubility of TEMPO in aqueous electrolyte, regardless of compatibility. This strategy not only improves the solubility but also enhances the cycle stability of TEMPO in the redox flow battery, leading to a higher energy density.
ADVANCED ENERGY MATERIALS
(2023)
Review
Chemistry, Physical
Yahua Liu, Qianru Chen, Xu Zhang, Jin Ran, Xiaozhao Han, Zhengjin Yang, Tongwen Xu
Summary: This paper summarizes the decomposition mechanisms of organic electrolytes in aqueous organic redox flow batteries (AORFBs) and discusses the influence of molecular engineering on the side reactions of electrolytes. It provides inspiration for designing more stable and cycling-stable electrolytes for AORFB and suggests possible directions and prospects for future research.
CURRENT OPINION IN ELECTROCHEMISTRY
(2022)
Review
Chemistry, Physical
Lois Briot, Martin Petit, Quentin Cacciuttolo, Marie-Cecile Pera
Summary: Renewable energy sources and ways to store this energy are growing exponentially, with redox flow batteries being a promising way of electrochemical storage. However, the long-term performance of these batteries is compromised due to degradations of electrodes, membrane, or organic species. Physical models play a crucial role in predicting and understanding the behavior of redox flow batteries.
JOURNAL OF POWER SOURCES
(2022)
Article
Chemistry, Physical
Aleksandr Korshunov, Anna Gibalova, Mariano Gruenebaum, Bart Jan Ravoo, Martin Winter, Isidora Cekic-Laskovic
Summary: The introduction of secondary noncovalent interactions along with primary modifications can enhance the overall performance of electrolytes for redox flow batteries. Through the formation of host-guest complexes between tailored viologens and highly water soluble cyclodextrin, significant improvements in electrochemical properties were achieved. By screening different combinations of viologen substituents in the presence of cyclodextrin, an electrochemically stable performance was demonstrated for more than 500 cycles with high energy and Coulombic efficiencies. This selective interplay between supporting electrolytes and engineered redox active materials shows promise for enhancing energy characteristics of AORFB electrolytes.
ACS APPLIED ENERGY MATERIALS
(2021)
Article
Chemistry, Multidisciplinary
Kiana Amini, Emily F. Kerr, Thomas Y. George, Abdulrahman M. Alfaraidi, Yan Jing, Tatsuhiro Tsukamoto, Roy G. Gordon, Michael J. Aziz
Summary: In this study, a stable and energy-dense anthraquinone compound with 2-2-propionate ether anthraquinone structure was synthesized and evaluated for use in an aqueous redox flow battery. The compound showed high stability and minimal degradation when subjected to different conditions and rejuvenation strategies. Degradation mechanisms, including side chain loss and anthrone formation, were identified. This study introduces a promising negolyte candidate for grid-scale aqueous organic redox flow batteries.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Aman Preet Kaur, Bertrand J. Neyhouse, Ilya A. Shkrob, Yilin Wang, N. Harsha Attanayake, Rahul Kant Jha, Qianwen Wu, Lu Zhang, Randy H. Ewoldt, Fikile R. Brushett, Susan A. Odom
Summary: Increasing concentrations of redox-active species in organic redox flow batteries can improve viability but can also lead to inefficient electrochemical cycling and low material utilization at higher current densities. We studied a highly soluble and stable redox-active couple, N-(2-(2-methoxyethoxy)ethyl)phenothiazine (MEEPT), and its bis(trifluoromethanesulfonyl)imide radical cation salt (MEEPT-TFSI), and demonstrated robust cycling performance with 1 M electrolyte concentration, achieving 94% materials utilization, 89% capacity retention, and 99.8% average coulombic efficiency over 435 h (100 full cycles). This study establishes the potential for high-performing, concentrated nonaqueous electrolytes while highlighting possible failure modes in such systems.
CHEMISTRY-AN ASIAN JOURNAL
(2023)
Article
Chemistry, Physical
Charles Tai-Chieh Wan, Kara E. Rodby, Mike L. Perry, Yet-Ming Chiang, Fikile R. Brushett
Summary: Researchers have found that the use of electrochemical purification can reduce the capacity fade rates of iron-chromium flow batteries. They have also identified a correlation between coulombic efficiency and discharge capacity decay rate, with electrochemical purification enabling cell performance equivalent to that with new materials. This method of mitigating hydrogen evolution reaction may decrease capacity maintenance needs and improve the performance of Fe-Cr flow batteries.
JOURNAL OF POWER SOURCES
(2023)
Article
Chemistry, Multidisciplinary
Charles Tai-Chieh Wan, Akram Ismail, Alexander H. Quinn, Yet-Ming Chiang, Fikile R. Brushett
Summary: Redox flow batteries (RFBs) are promising for efficient and reliable electricity delivery, integrating renewable resources and supporting aging grid infrastructure. Porous carbonaceous electrodes facilitate electrochemical reactions, electrolyte distribution, and electron conduction. Understanding electrode kinetics is crucial for improving RFB performance and reducing costs.
Article
Chemistry, Analytical
Alexis M. Fenton, Fikile R. Brushett
Summary: Voltammetry is a powerful analytical technique for evaluating electrochemical reactions and can be used to examine electrolyte solutions suitable for energy storage technologies. By evaluating electrolyte solutions using different voltammetry techniques, the accuracy of estimating electrolyte composition can be improved and analytes with similar electrode potentials can be differentiated more easily. This method can be further enhanced by including multiple voltammetry techniques in the training dataset. Overall, this study demonstrates the utility of sequential and simultaneous methods in evaluating multiple voltammetry datasets for diagnosing electrolyte solutions in electrochemical technologies.
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
(2023)
Article
Information Science & Library Science
Kara E. Rodby, Robert L. Jaffe, Elsa A. Olivetti, Fikile R. Brushett
Summary: Redox flow batteries (RFBs), particularly vanadium RFBs (VRFBs), are a promising solution for decarbonization in the power sector. However, the high and volatile price of vanadium hinders VRFB financing and deployment opportunities. This study evaluates the vanadium supply chain and identifies challenges to rapid growth. Accelerated growth is possible with increased vanadium production rates, but terawatt-hour deployment may be challenged by market conditions and resource availability, motivating the development of next-generation RFB chemistries.
INTERNATIONAL JOURNAL OF INFORMATION MANAGEMENT
(2023)
Article
Electrochemistry
Madhu V. Majji, Bertrand J. Neyhouse, Nicholas J. Matteucci, Kyle R. Lennon, Christopher T. Mallia, Alexis M. M. Fenton Jr, James W. Swan, Fikile R. Brushett
Summary: Flowable suspension-based electrodes (FSEs) have gained attention due to their improved performance and flexible operation in electrochemical flow cells. However, FSEs can exhibit non-Newtonian characteristics under certain conditions, causing large pumping losses and flow-dependent transport rates. In this study, a one-dimensional model integrating porous electrode theory and FSE rheology is developed to explore scaling relationships and design rules for electrochemical devices. The model identifies key dimensionless groups and establishes property-performance relationships for FSEs, providing guidance for practical operating envelopes.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2023)
Article
Electrochemistry
Charles Tai-Chieh Wan, Robert M. M. Darling, Yet-Ming Chiang, Fikile R. R. Brushett
Summary: Reducing the platinum (Pt) loading in polymer electrolyte fuel cells (PEFCs) is important for their widespread use, but it leads to polarization losses at higher current densities. The morphology of carbon supports in PEFC cathodes affects the deposition of Pt, resulting in different kinetic and transport resistances. In this study, we develop a model to differentiate the sink terms for Pt on the surface and in the pits of carbon supports, and assess the impact of nanoscale ohmic resistance on PEFC performance. We estimate the micropore resistances based on experimental local oxygen transport resistances and simulate polarization curves to evaluate the effect of micropore resistance.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2023)
Article
Energy & Fuels
Charles Tai-Chieh Wan, Remy Richard Jacquemond, Yet-Ming Chiang, Antoni Forner-Cuenca, Fikile R. Brushett
Summary: This article presents a new non-solvent-induced phase-separation (NIPS) technique for synthesizing macrovoid-free electrodes with well-defined across-thickness porosity gradients. The performance and surface chemistries of porosity-gradient electrodes are compared with macrovoid-containing electrodes. The results show that the porosity-gradient electrodes outperform the macrovoid-containing electrodes in electrochemical and fluid dynamic performance, regardless of the gradient direction.
Article
Chemistry, Analytical
Alexis M. Fenton Jr, Bertrand J. Neyhouse, Kevin M. Tenny, Yet -Ming Chiang, Fikile R. Brushett
Summary: Voltammetry is a widely used method in electrochemical technology to evaluate the behavior of electrolyte solutions. It allows for rapid estimation of the state-of-charge and state-of-health of electrolyte solutions by simulating the entire voltammogram. This method shows potential for advancing diagnostic methods in operating electrochemical devices.
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
(2023)
Article
Electrochemistry
Bertrand J. Neyhouse, Robert M. Darling, James D. Saraidaridis, Fikile R. Brushett
Summary: A new method called compositionally unbalanced symmetric cell cycling (CUSCC) is proposed to evaluate species crossover in redox flow batteries (RFBs). This method directly assesses crossover in redox flow cells and provides consistent results with traditional experimental techniques. The study also demonstrates the potential of CUSCC in characterizing species crossover and expanding the RFB testing toolbox.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2023)
Article
Electrochemistry
Weiran Gao, Javit Drake, Fikile R. Brushett
Summary: The concept of circulating electrolyte through the porous electrodes and separator is proposed to facilitate effective temperature regulation in lithium-ion batteries (LIBs). Through modeling and analysis, it is found that electrolyte convection can draw heat from the cell and suppress heat generation, effectively mitigating the cell temperature rise. Simulations show that with sufficient electrolyte flow, the cell can be maintained at a lower temperature while still delivering most of its capacity.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2023)
Article
Electrochemistry
Eric M. Fell, Diana De Porcellinis, Yan Jing, Valeria Gutierrez-Venegas, Thomas Y. George, Roy G. Gordon, Sergio Granados-Focil, Michael J. Aziz
Summary: We evaluated the suitability of potassium ferri-/ferrocyanide as an electroactive species for aqueous organic redox flow batteries. Our findings indicate that there is no structural decomposition of ferri-/ferrocyanide at pH values as high as 14 in the dark or in indoor light, contrasting with previous reports. Instead, a chemical reduction of ferricyanide to ferrocyanide via chemical oxygen evolution reaction leads to an apparent capacity fade. This parasitic process can be exacerbated by carbon electrodes, and the apparent capacity fade rates can be engineered through the initial system setup.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Abdulrahman M. Alfaraidi, Bryan Kudisch, Nina Ni, Jayden Thomas, Thomas Y. George, Khashayar Rajabimoghadam, Haihui Joy Jiang, Daniel G. Nocera, Michael J. Aziz, Richard Y. Liu
Summary: Separating and capturing CO2 from sources or the atmosphere is crucial for climate change mitigation. However, the current strategies have high energy costs. This study demonstrates a photochemically driven system that can capture and release CO2 using sunlight. The findings provide thermodynamic and kinetic principles for the development of solar-powered negative emission technologies.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Jinxu Gao, Kyumin Lee, Kiana Amini, Roy G. Gordon, Theodore A. Betley, Michael J. Aziz
Summary: In this study, a novel iron-based posolyte redox species, FeTPEN, with high redox potential and remarkable aqueous solubility, paired with a specific compound, demonstrated excellent performance in the redox flow battery. The post analysis of the electrolyte provides insights for future stabilization strategies.
ADVANCED FUNCTIONAL MATERIALS
(2023)
