Mild pH-decoupling aqueous flow battery with practical pH recovery

Xi, Dawei; Alfaraidi, Abdulrahman M.; Gao, Jinxu; Cochard, Thomas; Faria, Luana C. I.; Yang, Zheng; George, Thomas Y.; Wang, Taobo; Gordon, Roy G.; Liu, Richard Y.; Aziz, Michael J.

doi:10.1038/s41560-024-01474-1

Title: Mild pH-decoupling aqueous flow battery with practical pH recovery

Journal Article · 18 February 2024 · Nature Energy

DOI: https://doi.org/10.1038/s41560-024-01474-1 · OSTI ID:2345159

^[1];

^[2]; Gao, Jinxu ^[2];

^[2];

^[2]; Yang, Zheng ^[2];

^[2]; Wang, Taobo ^[2];

^[2];

^[2]

Harvard Univ., Cambridge, MA (United States); Harvard University
Harvard Univ., Cambridge, MA (United States)

Establishing a pH difference between the two electrolytes (pH decoupling) of an aqueous redox flow battery (ARFB) enables cell voltages exceeding the 1.23 V thermodynamic water-splitting window, but acid–base crossover penalizes efficiency and lifetime. Here we employ mildly acidic and mildly alkaline electrolytes to mitigate crossover, achieving high round-trip energy efficiency with open circuit voltage >1.7 V. We implemented an acid–base regeneration system to periodically restore electrolytes to their initial pH values. The combined system exhibited capacity fade rate <0.07% per day, round-trip energy efficiency >85% and approximately 99% Coulombic efficiency during stable operation for over a week. Cost analysis shows that the tolerance of acid–base crossover could be increased if the pH-decoupling ARFB achieved a higher voltage output and lower resistance. Finally, this work demonstrates principles for improving lifespan, rate capability and energy efficiency in high-voltage pH-decoupling ARFBs and pH recovery concepts applicable for pH-decoupling systems.

View Accepted Manuscript (DOE)

Cite

Export

Save

Research Organization:: Harvard Univ., Cambridge, MA (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 2345159

Journal Information:: Nature Energy, Journal Name: Nature Energy Journal Issue: 4 Vol. 9; ISSN 2058-7546

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

References (40)

Pathways to low-cost electrochemical energy storage: a comparison of aqueous and nonaqueous flow batteries Darling, Robert M.; Gallagher, Kevin G.; Kowalski, Jeffrey A. Energy & Environmental Science, Vol. 7, Issue 11, p. 3459-3477 https://doi.org/10.1039/C4EE02158D	journal	January 2014
Cost-driven materials selection criteria for redox flow battery electrolytes Dmello, Rylan; Milshtein, Jarrod D.; Brushett, Fikile R. Journal of Power Sources, Vol. 330 https://doi.org/10.1016/j.jpowsour.2016.08.129	journal	October 2016
Polysulfide-based redox flow batteries with long life and low levelized cost enabled by charge-reinforced ion-selective membranes Li, Zhejun; Lu, Yi-Chun Nature Energy, Vol. 6, Issue 5 https://doi.org/10.1038/s41560-021-00804-x	journal	April 2021
High-Voltage Aqueous Redox Flow Batteries Enabled by Catalyzed Water Dissociation and Acid–Base Neutralization in Bipolar Membranes Yan, Zhifei; Wycisk, Ryszard J.; Metlay, Amy S. ACS Central Science, Vol. 7, Issue 6 https://doi.org/10.1021/acscentsci.1c00217	journal	May 2021
High Voltage Vanadium-Metal Hydride Rechargeable Semi-Flow Battery Weng, Guo-Ming; Li, Chi-Ying Vanessa; Chan, Kwong-Yu Journal of The Electrochemical Society, Vol. 160, Issue 9 https://doi.org/10.1149/2.035309jes	journal	January 2013
A High Voltage Aqueous Zinc–Organic Hybrid Flow Battery Park, Minjoon; Beh, Eugene S.; Fell, Eric M. Advanced Energy Materials, Vol. 9, Issue 25 https://doi.org/10.1002/aenm.201900694	journal	May 2019
Untapped Potential: The Need and Opportunity for High-Voltage Aqueous Redox Flow Batteries Perry, Mike L.; Rodby, Kara E.; Brushett, Fikile R. ACS Energy Letters, Vol. 7, Issue 2 https://doi.org/10.1021/acsenergylett.1c02225	journal	January 2022
Polymeric membranes with aligned zeolite nanosheets for sustainable energy storage Xia, Yongsheng; Cao, Hongyan; Xu, Fang Nature Sustainability, Vol. 5, Issue 12 https://doi.org/10.1038/s41893-022-00974-w	journal	October 2022
Stability enhancement for all‐iron aqueous redox flow battery using iron‐3‐[bis(2‐hydroxyethyl)amino]‐2‐hydroxypropanesulfonic acid complex and ferrocyanide as redox couple Shin, Mingyu; Noh, Chanho; Kwon, Yongchai International Journal of Energy Research, Vol. 46, Issue 5 https://doi.org/10.1002/er.7535	journal	December 2021
A High Potential, Low Capacity Fade Rate Iron Complex Posolyte for Aqueous Organic Flow Batteries Gao, Jinxu; Amini, Kiana; George, Thomas Y. Advanced Energy Materials, Vol. 12, Issue 44 https://doi.org/10.1002/aenm.202202444	journal	October 2022
Nafion/SiO2 hybrid membrane for vanadium redox flow battery Xi, Jingyu; Wu, Zenghua; Qiu, Xinping Journal of Power Sources, Vol. 166, Issue 2 https://doi.org/10.1016/j.jpowsour.2007.01.069	journal	April 2007
Electrolyte Lifetime in Aqueous Organic Redox Flow Batteries: A Critical Review Kwabi, David G.; Ji, Yunlong; Aziz, Michael J. Chemical Reviews, Vol. 120, Issue 14 https://doi.org/10.1021/acs.chemrev.9b00599	journal	February 2020
Electrochemical Characterization of Hydrocarbon Bipolar Membranes with Varying Junction Morphology Hohenadel, Amelia; Powers, Devon; Wycisk, Ryszard ACS Applied Energy Materials, Vol. 2, Issue 9 https://doi.org/10.1021/acsaem.9b01257	journal	August 2019
Decoupled aqueous batteries using pH-decoupling electrolytes Zhu, Yun-hai; Cui, Yang-feng; Xie, Zi-long Nature Reviews Chemistry, Vol. 6, Issue 7 https://doi.org/10.1038/s41570-022-00397-3	journal	June 2022
Assessment methods and performance metrics for redox flow batteries Yao, Yanxin; Lei, Jiafeng; Shi, Yang Nature Energy https://doi.org/10.1038/s41560-020-00772-8	journal	February 2021
High-voltage asymmetric metal–air batteries based on polymeric single-Zn2+-ion conductor Lin, Chao; Kim, Sung-Hae; Xu, Qing Matter, Vol. 4, Issue 4 https://doi.org/10.1016/j.matt.2021.01.004	journal	April 2021
Decoupling electrolytes towards stable and high-energy rechargeable aqueous zinc–manganese dioxide batteries Zhong, Cheng; Liu, Bin; Ding, Jia Nature Energy, Vol. 5, Issue 6 https://doi.org/10.1038/s41560-020-0584-y	journal	March 2020
Stable Operation of Aqueous Organic Redox Flow Batteries in Air Atmosphere Kong, Taoyi; Liu, Jun; Zhou, Xing Angewandte Chemie International Edition, Vol. 62, Issue 6 https://doi.org/10.1002/anie.202214819	journal	January 2023
A zinc–iron redox-flow battery under $100 per kW h of system capital cost Gong, Ke; Ma, Xiaoya; Conforti, Kameron M. Energy & Environmental Science, Vol. 8, Issue 10 https://doi.org/10.1039/C5EE02315G	journal	January 2015
Chelated Chromium Electrolyte Enabling High-Voltage Aqueous Flow Batteries Robb, Brian H.; Farrell, Jason M.; Marshak, Michael P. Joule, Vol. 3, Issue 10 https://doi.org/10.1016/j.joule.2019.07.002	journal	October 2019
A cost-effective alkaline polysulfide-air redox flow battery enabled by a dual-membrane cell architecture Xia, Yuhua; Ouyang, Mengzheng; Yufit, Vladimir Nature Communications, Vol. 13, Issue 1 https://doi.org/10.1038/s41467-022-30044-w	journal	May 2022
Techno-economic analyses of several redox flow batteries using levelized cost of energy storage Darling, Robert M. Current Opinion in Chemical Engineering, Vol. 37 https://doi.org/10.1016/j.coche.2022.100855	journal	September 2022
Development of efficient aqueous organic redox flow batteries using ion-sieving sulfonated polymer membranes Ye, Chunchun; Wang, Anqi; Breakwell, Charlotte Nature Communications, Vol. 13, Issue 1 https://doi.org/10.1038/s41467-022-30943-y	journal	June 2022
Emerging chemistries and molecular designs for flow batteries Zhang, Leyuan; Feng, Ruozhu; Wang, Wei Nature Reviews Chemistry, Vol. 6, Issue 8 https://doi.org/10.1038/s41570-022-00394-6	journal	June 2022
A Water-Miscible Quinone Flow Battery with High Volumetric Capacity and Energy Density Jin, Shijian; Jing, Yan; Kwabi, David G. ACS Energy Letters, Vol. 4, Issue 6 https://doi.org/10.1021/acsenergylett.9b00739	journal	May 2019
Optimization studies on a Fe/Cr redox flow battery Lopez-Atalaya, M.; Codina, G.; Perez, J. R. Journal of Power Sources, Vol. 39, Issue 2, p. 147-154 https://doi.org/10.1016/0378-7753(92)80133-V	journal	January 1992
Decoupled Redox Catalytic Hydrogen Production with a Robust Electrolyte-Borne Electron and Proton Carrier Zhang, Feifei; Zhang, Hang; Salla, Manohar Journal of the American Chemical Society, Vol. 143, Issue 1 https://doi.org/10.1021/jacs.0c09510	journal	December 2020
Mild pH-decoupling Aqueous Flow Battery with Practical pH Recovery (data) Xi, Dawei; Alfaraidi, Abdulrahman; Gao, Jinxu figshare https://doi.org/10.6084/m9.figshare.23816796.v1	dataset	January 2024
Near-frictionless ion transport within triazine framework membranes Zuo, Peipei; Ye, Chunchun; Jiao, Zhongren Nature, Vol. 617, Issue 7960 https://doi.org/10.1038/s41586-023-05888-x	journal	April 2023
Molecular Design of Fused-Ring Phenazine Derivatives for Long-Cycling Alkaline Redox Flow Batteries Wang, Caixing; Li, Xiang; Yu, Bo ACS Energy Letters, Vol. 5, Issue 2 https://doi.org/10.1021/acsenergylett.9b02676	journal	January 2020
The Development of Zn-Ce Hybrid Redox Flow Batteries for Energy Storage and Their Continuing Challenges Walsh, Frank C.; Ponce de Léon, Carlos; Berlouis, Len ChemPlusChem, Vol. 80, Issue 2 https://doi.org/10.1002/cplu.201402103	journal	November 2014
High-voltage pH differential vanadium-hydrogen flow battery Weng, Guo-Ming; Li, Chi-Ying Vanessa; Chan, Kwong-Yu Materials Today Energy, Vol. 10 https://doi.org/10.1016/j.mtener.2018.08.014	journal	December 2018
The Renaissance of the Zn-Ce Flow Battery: Dual-Membrane Configuration Enables Unprecedentedly High Efficiency Xie, Xian; Mushtaq, Faheem; Wang, Qiuhong ACS Energy Letters, Vol. 7, Issue 10 https://doi.org/10.1021/acsenergylett.2c01646	journal	September 2022
Hydrophilic microporous membranes for selective ion separation and flow-battery energy storage Tan, Rui; Wang, Anqi; Malpass-Evans, Richard Nature Materials, Vol. 19, Issue 2 https://doi.org/10.1038/s41563-019-0536-8	journal	December 2019
A multiple ion-exchange membrane design for redox flow batteries Gu, Shuang; Gong, Ke; Yan, Emily Z. Energy Environ. Sci., Vol. 7, Issue 9 https://doi.org/10.1039/C4EE00165F	journal	January 2014
Three-Chamber Design for Aqueous Acid–Base Redox Flow Batteries Metlay, Amy S.; Chyi, Brandon; Yoon, Yein ACS Energy Letters, Vol. 7, Issue 3 https://doi.org/10.1021/acsenergylett.2c00040	journal	February 2022
Alkaline Quinone Flow Battery with Long Lifetime at pH 12 Kwabi, David G.; Lin, Kaixiang; Ji, Yunlong Joule, Vol. 2, Issue 9 https://doi.org/10.1016/j.joule.2018.07.005	journal	September 2018
All iron aqueous redox flow batteries using organometallic complexes consisting of iron and 3-[bis (2-hydroxyethyl)amino]-2-hydroxypropanesulfonic acid ligand and ferrocyanide as redox couple Shin, Mingyu; Noh, Chanho; Chung, Yongjin Chemical Engineering Journal, Vol. 398 https://doi.org/10.1016/j.cej.2020.125631	journal	October 2020
A Neutral pH Aqueous Organic–Organometallic Redox Flow Battery with Extremely High Capacity Retention Beh, Eugene S.; De Porcellinis, Diana; Gracia, Rebecca L. ACS Energy Letters, Vol. 2, Issue 3 https://doi.org/10.1021/acsenergylett.7b00019	journal	February 2017
Toward High-Voltage Aqueous Batteries: Super- or Low-Concentrated Electrolyte? Chao, Dongliang; Qiao, Shi-Zhang Joule, Vol. 4, Issue 9 https://doi.org/10.1016/j.joule.2020.07.023	journal	September 2020

Similar Records

Methanesulfonic acid-based electrode-decoupled vanadium–cerium redox flow battery exhibits significantly improved capacity and cycle life

Journal Article · 2019 · Sustainable Energy & Fuels · OSTI ID:1613713

Sankarasubramanian, Shrihari; Zhang, Yunzhu; Ramani, Vijay

2013 Estorm - Invited Paper - Cathode Materials Review

Journal Article · 2014 · AIP Advances · OSTI ID:1143546

Daniel, Claus; Mohanty, Debasish; Li, Jianlin; +1 more

Cathode materials review

Journal Article · 2014 · AIP Conference Proceedings · OSTI ID:22311254

Daniel, Claus; Mohanty, Debasish; Li, Jianlin

Related Subjects

25 ENERGY STORAGE
batteries
chemical engineering

Title: Mild pH-decoupling aqueous flow battery with practical pH recovery

Citation Formats

References (40)

Linked Research (1)

Similar Records

Related Subjects