A High Potential, Low Capacity Fade Rate Iron Complex Posolyte for Aqueous Organic Flow Batteries

Gao, Jinxu; Amini, Kiana; George, Thomas Y.; Jing, Yan; Tsukamoto, Tatsuhiro; Xi, Dawei; Gordon, Roy G.; Aziz, Michael J.

doi:10.1002/aenm.202202444

Title: A High Potential, Low Capacity Fade Rate Iron Complex Posolyte for Aqueous Organic Flow Batteries

Journal Article · Fri Oct 07 00:00:00 EDT 2022 · Advanced Energy Materials

DOI:https://doi.org/10.1002/aenm.202202444· OSTI ID:1899729

^[1]; Amini, Kiana ^[2]; George, Thomas Y. ^[2]; Jing, Yan ^[1]; Tsukamoto, Tatsuhiro ^[1]; Xi, Dawei ^[2];

^[3];

^[2]

Department of Chemistry and Chemical Biology Harvard University 12 Oxford Street Cambridge MA 02138 USA
Harvard John A. Paulson School of Engineering and Applied Sciences 29 Oxford Street Cambridge MA 02138 USA
Department of Chemistry and Chemical Biology Harvard University 12 Oxford Street Cambridge MA 02138 USA, Harvard John A. Paulson School of Engineering and Applied Sciences 29 Oxford Street Cambridge MA 02138 USA

Abstract An iron complex, tris(4,4′‐bis(hydroxymethyl)‐2,2′‐bipyridine) iron dichloride is reported, which operates at near‐neutral pH with a redox potential of 0.985 V versus SHE. This high potential compound is employed in the posolyte of an aqueous flow battery, paired with bis(3‐trimethylammonio)propyl viologen tetrachloride in the negolyte, exhibiting an open‐circuit voltage of 1.3 V at near‐neutral pH. It demonstrates excellent cycling performance with a low temporal capacity fade rate of 0.07% per day over 35 days of cycling. The extended cycling lifetime is the result of low permeability and improved structural stability of the newly developed iron complex compared to that of the iron tris(bipyridine) complex. The combination of high redox potential and low capacity fade rate compares favorably with those of all previously demonstrated organic and organometallic aqueous posolytes. Extensive investigation into the possible degradation mechanisms, including post‐mortem chemical and electrochemical analyses, indicates that stepwise ligand dissociations of the iron complex are responsible for the reported capacity loss during cell cycling. This investigation provides unprecedented insight to guide further improvements of such metalorganic compounds for energy storage and conversion applications.

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Sponsoring Organization:: USDOE

Grant/Contract Number:: DE‐AC05‐76RL01830

OSTI ID:: 1899729

Journal Information:: Advanced Energy Materials, Journal Name: Advanced Energy Materials Vol. 12 Journal Issue: 44; ISSN 1614-6832

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

References (49)

Isopropyl alcohol and copper hexacyanoferrate boost performance of the iron tris‐bipyridine catholyte for near‐neutral pH aqueous redox flow batteries Bui, Huyen; Holubowitch, Nicolas E. International Journal of Energy Research, Vol. 46, Issue 5 https://doi.org/10.1002/er.7527	journal	December 2021
High-performance anthraquinone with potentially low cost for aqueous redox flow batteries Wu, Min; Bahari, Meisam; Fell, Eric M. Journal of Materials Chemistry A, Vol. 9, Issue 47 https://doi.org/10.1039/D1TA08900E	journal	January 2021
Long-Cycling Aqueous Organic Redox Flow Battery (AORFB) toward Sustainable and Safe Energy Storage Hu, Bo; DeBruler, Camden; Rhodes, Zayn Journal of the American Chemical Society, Vol. 139, Issue 3 https://doi.org/10.1021/jacs.6b10984	journal	January 2017
A Long-Lifetime All-Organic Aqueous Flow Battery Utilizing TMAP-TEMPO Radical Liu, Yahua; Goulet, Marc-Antoni; Tong, Liuchuan Chem, Vol. 5, Issue 7 https://doi.org/10.1016/j.chempr.2019.04.021	journal	July 2019
A Phosphonate‐Functionalized Quinone Redox Flow Battery at Near‐Neutral pH with Record Capacity Retention Rate Ji, Yunlong; Goulet, Marc‐Antoni; Pollack, Daniel A. Advanced Energy Materials, Vol. 9, Issue 12 https://doi.org/10.1002/aenm.201900039	journal	January 2019
A high Yielding Preparation of 2,2′-Bipyridine-1-Oxide Joachim Demnitz, F. W.; D'heni, Maria Betânia Organic Preparations and Procedures International, Vol. 30, Issue 4 https://doi.org/10.1080/00304949809355313	journal	August 1998
Investigations Into Aqueous Redox Flow Batteries Based on Ferrocene Bisulfonate Zhao, Zhiling; Zhang, Baosen; Schrage, Briana R. ACS Applied Energy Materials, Vol. 3, Issue 10 https://doi.org/10.1021/acsaem.0c02259	journal	October 2020
Analysis of Crossover-Induced Capacity Fade in Redox Flow Batteries with Non-Selective Separators Nemani, Venkat Pavan; Smith, Kyle C. Journal of The Electrochemical Society, Vol. 165, Issue 13 https://doi.org/10.1149/2.0701813jes	journal	January 2018
A biomimetic redox flow battery based on flavin mononucleotide Orita, Akihiro; Verde, Michael G.; Sakai, Masanori Nature Communications, Vol. 7, Issue 1 https://doi.org/10.1038/ncomms13230	journal	October 2016
Designer Two-Electron Storage Viologen Anolyte Materials for Neutral Aqueous Organic Redox Flow Batteries DeBruler, Camden; Hu, Bo; Moss, Jared Chem, Vol. 3, Issue 6 https://doi.org/10.1016/j.chempr.2017.11.001	journal	December 2017
Functioning Water‐Insoluble Ferrocenes for Aqueous Organic Flow Battery via Host–Guest Inclusion Li, Yuanyuan; Xu, Ziang; Liu, Yahua ChemSusChem, Vol. 14, Issue 2 https://doi.org/10.1002/cssc.202002516	journal	December 2020
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
Anthraquinone Flow Battery Reactants with Nonhydrolyzable Water-Solubilizing Chains Introduced via a Generic Cross-Coupling Method Jing, Yan; Fell, Eric M.; Wu, Min ACS Energy Letters, Vol. 7, Issue 1 https://doi.org/10.1021/acsenergylett.1c02504	journal	December 2021
Extremely Stable Anthraquinone Negolytes Synthesized from Common Precursors Wu, Min; Jing, Yan; Wong, Andrew A. Chem, Vol. 6, Issue 6 https://doi.org/10.1016/j.chempr.2020.03.021	journal	June 2020
A comparative study of all-vanadium and iron-chromium redox flow batteries for large-scale energy storage Zeng, Y. K.; Zhao, T. S.; An, L. Journal of Power Sources, Vol. 300 https://doi.org/10.1016/j.jpowsour.2015.09.100	journal	December 2015
Near Neutral pH Redox Flow Battery with Low Permeability and Long‐Lifetime Phosphonated Viologen Active Species Jin, Shijian; Fell, Eric M.; Vina‐Lopez, Lucia Advanced Energy Materials, Vol. 10, Issue 20 https://doi.org/10.1002/aenm.202000100	journal	April 2020
A higher voltage Fe( ii ) bipyridine complex for non-aqueous redox flow batteries Cammack, Claudina X.; Pratt, Harry D.; Small, Leo J. Dalton Transactions, Vol. 50, Issue 3 https://doi.org/10.1039/D0DT03927F	journal	January 2021
Electrochemical kinetics of the ferri-ferrocyanide couple on platinum Daum, Peter H.; Enke, Christie G. Analytical Chemistry, Vol. 41, Issue 4 https://doi.org/10.1021/ac60273a007	journal	April 1969
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
All-Soluble All-Iron Aqueous Redox-Flow Battery Gong, Ke; Xu, Fei; Grunewald, Jonathan B. ACS Energy Letters, Vol. 1, Issue 1 https://doi.org/10.1021/acsenergylett.6b00049	journal	May 2016
Photosensitization of TiO ₂ by [Fe ^II (2,2‘-bipyridine-4,4‘-dicarboxylic acid) ₂ (CN) ₂ ]: Band Selective Electron Injection from Ultra-Short-Lived Excited States Ferrere, Suzanne; Gregg, Brian A. Journal of the American Chemical Society, Vol. 120, Issue 4 https://doi.org/10.1021/ja973504e	journal	February 1998
A redox-flow battery with an alloxazine-based organic electrolyte Lin, Kaixiang; Gómez-Bombarelli, Rafael; Beh, Eugene S. Nature Energy, Vol. 1, Issue 9 https://doi.org/10.1038/nenergy.2016.102	journal	July 2016
A Total Organic Aqueous Redox Flow Battery Employing a Low Cost and Sustainable Methyl Viologen Anolyte and 4-HO-TEMPO Catholyte Liu, Tianbiao; Wei, Xiaoliang; Nie, Zimin Advanced Energy Materials, Vol. 6, Issue 3, 1501449 https://doi.org/10.1002/aenm.201501449	journal	December 2015
Boron Cluster Anions [B_nH_n]^2-(n= 10, 12) in Reactions of Iron(II) and Iron(III) Complexation with 2, 2′-Bipyridyl and 1, 10-Phenanthroline Avdeeva, Varvara V.; Vologzhanina, Anna V.; Goeva, Lyudmila V. Zeitschrift für anorganische und allgemeine Chemie, Vol. 640, Issue 11 https://doi.org/10.1002/zaac.201400137	journal	July 2014
Studies of Iron-Ligand Complexes for an All-Iron Flow Battery Application Hawthorne, Krista L.; Wainright, Jesse S.; Savinell, Robert F. Journal of The Electrochemical Society, Vol. 161, Issue 10 https://doi.org/10.1149/2.0761410jes	journal	January 2014
Aspects of electron transfer processes in vanadium redox-flow batteries Roznyatovskaya, Nataliya; Noack, Jens; Pinkwart, Karsten Current Opinion in Electrochemistry, Vol. 19 https://doi.org/10.1016/j.coelec.2019.10.003	journal	February 2020
Symmetry-breaking design of an organic iron complex catholyte for a long cyclability aqueous organic redox flow battery Li, Xiang; Gao, Peiyuan; Lai, Yun-Yu Nature Energy, Vol. 6, Issue 9 https://doi.org/10.1038/s41560-021-00879-6	journal	August 2021
In situ electrochemical recomposition of decomposed redox-active species in aqueous organic flow batteries Jing, Yan; Zhao, Evan Wenbo; Goulet, Marc-Antoni Nature Chemistry https://doi.org/10.1038/s41557-022-00967-4	journal	June 2022
Novel electrolyte rebalancing method for vanadium redox flow batteries Poli, Nicola; Schäffer, Michael; Trovò, Andrea Chemical Engineering Journal, Vol. 405 https://doi.org/10.1016/j.cej.2020.126583	journal	February 2021
Improvements to the Coulombic Efficiency of the Iron Electrode for an All-Iron Redox-Flow Battery Jayathilake, B. S.; Plichta, E. J.; Hendrickson, M. A. Journal of The Electrochemical Society, Vol. 165, Issue 9 https://doi.org/10.1149/2.0451809jes	journal	January 2018
Alkaline quinone flow battery Lin, K.; Chen, Q.; Gerhardt, M. R. Science, Vol. 349, Issue 6255, p. 1529-1532 https://doi.org/10.1126/science.aab3033	journal	September 2015
Dimerization of [Fe^III(bpy)₃]³⁺ in Aqueous Solutions: Elucidating a Mechanism Based on Historical Proposals, Electrochemical Data, and Computational Free Energy Analysis Holubowitch, Nicolas E.; Nguyen, Giang Inorganic Chemistry, Vol. 61, Issue 25 https://doi.org/10.1021/acs.inorgchem.2c00640	journal	June 2022
Phenothiazine‐Based Organic Catholyte for High‐Capacity and Long‐Life Aqueous Redox Flow Batteries Zhang, Changkun; Niu, Zhihui; Peng, Sangshan Advanced Materials https://doi.org/10.1002/adma.201901052	journal	April 2019
A High Energy Density Vanadium Redox Flow Battery with 3 M Vanadium Electrolyte Roe, Sarah; Menictas, Chris; Skyllas-Kazacos, Maria Journal of The Electrochemical Society, Vol. 163, Issue 1 https://doi.org/10.1149/2.0041601jes	journal	July 2015
Effect of Chelation on Iron–Chromium Redox Flow Batteries Waters, Scott E.; Robb, Brian H.; Marshak, Michael P. ACS Energy Letters, Vol. 5, Issue 6 https://doi.org/10.1021/acsenergylett.0c00761	journal	April 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
Electricity storage for intermittent renewable sources Rugolo, Jason; Aziz, Michael J. Energy & Environmental Science, Vol. 5, Issue 5 https://doi.org/10.1039/c2ee02542f	journal	January 2012
Crossover in Membranes for Aqueous Soluble Organic Redox Flow Batteries Small, Leo J.; Pratt, Harry D.; Anderson, Travis M. Journal of The Electrochemical Society, Vol. 166, Issue 12 https://doi.org/10.1149/2.0681912jes	journal	January 2019
Progress in redox flow batteries, remaining challenges and their applications in energy storage Leung, Puiki; Li, Xiaohong; Ponce de León, Carlos RSC Advances, Vol. 2, Issue 27 https://doi.org/10.1039/c2ra21342g	journal	January 2012
Long-Term Stability of Ferri/Ferrocyanide As an Electroactive Component for Redox Flow Battery Applications: On the Origin of Apparent Capacity Fade Fell, Eric M.; De Porcellinis, Diana; Jing, Yan ECS Meeting Abstracts, Vol. MA2022-02, Issue 46 https://doi.org/10.1149/MA2022-02461726mtgabs	journal	October 2022
Flow Batteries: Current Status and Trends Soloveichik, Grigorii L. Chemical Reviews, Vol. 115, Issue 20 https://doi.org/10.1021/cr500720t	journal	September 2015
Communication—Tris(bipyridyl)iron Complexes for High-Voltage Aqueous Redox Flow Batteries Ruan, Wenqing; Mao, Jiatao; Yang, Shida Journal of The Electrochemical Society, Vol. 167, Issue 10 https://doi.org/10.1149/1945-7111/ab9cc8	journal	June 2020
A stable organic dye catholyte for long-life aqueous flow batteries Li, Hongbin; Fan, Hao; Ravivarma, Mahalingam Chemical Communications, Vol. 56, Issue 89 https://doi.org/10.1039/D0CC05133K	journal	January 2020
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
Unprecedented Capacity and Stability of Ammonium Ferrocyanide Catholyte in pH Neutral Aqueous Redox Flow Batteries Luo, Jian; Hu, Bo; Debruler, Camden Joule, Vol. 3, Issue 1 https://doi.org/10.1016/j.joule.2018.10.010	journal	January 2019
Extending the Lifetime of Organic Flow Batteries via Redox State Management Goulet, Marc-Antoni; Tong, Liuchuan; Pollack, Daniel A. Journal of the American Chemical Society https://doi.org/10.1021/jacs.8b13295	journal	April 2019
Renewable energy resources: Current status, future prospects and their enabling technology Ellabban, Omar; Abu-Rub, Haitham; Blaabjerg, Frede Renewable and Sustainable Energy Reviews, Vol. 39 https://doi.org/10.1016/j.rser.2014.07.113	journal	November 2014
Spin state modulation of iron spin crossover complexes via hydrogen-bonding self-assembly Young, Michael C.; Liew, Erica; Ashby, Jonathan Chemical Communications, Vol. 49, Issue 56 https://doi.org/10.1039/c3cc42851f	journal	January 2013
A metal-free organic–inorganic aqueous flow battery Huskinson, Brian; Marshak, Michael P.; Suh, Changwon Nature, Vol. 505, Issue 7482, p. 195-198 https://doi.org/10.1038/nature12909	journal	January 2014

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