Accelerated design of vanadium redox flow battery electrolytes through tunable solvation chemistry

Murugesan, Vijayakumar; Nie, Zimin; Zhang, Xin; Gao, Peiyuan; Zhu, Zihua; Huang, Qian; Yan, Litao; Reed, David; Wang, Wei

doi:10.1016/j.xcrp.2021.100323

Title: Accelerated design of vanadium redox flow battery electrolytes through tunable solvation chemistry

Journal Article · Mon Feb 01 00:00:00 EST 2021 · Cell Reports Physical Science

DOI:https://doi.org/10.1016/j.xcrp.2021.100323· OSTI ID:1877719

; Nie, Zimin; Zhang, Xin; Gao, Peiyuan; Zhu, Zihua; Huang, Qian; Yan, Litao; Reed, David;

Operational stability of electrolytes is a persistent impediment in building redox flow battery technology. Stabilizing multiple vanadium oxidation states in aqueous solution is a primary challenge in designing reliable large-scale vanadium redox flow batteries (VRBs). Here we demonstrate that rationally selected ionic additives can stabilize the aqua vanadium solvate structures through preferential bonding and molecular interactions despite their relatively low concentrations (≤0.1 M). The competing cations (NH₄⁺ and Mg²⁺) and bonding anions (SO₄^2–, PO₄^3–, and Cl^–) introduced by bi-additives are used to tune the vanadium solvation chemistry and design an optimal electrolyte for VRB technology. Such molecular engineering of VRB electrolytes results in enhancement of the operational temperature window by 180% and energy density by more than 30% relative to traditional electrolytes. This work demonstrates that tunable solvation chemistry is a promising pathway to engineer an optimal electrolyte for targeted electrochemical systems.

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Research Organization:: Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL)

Sponsoring Organization:: USDOE Office of Science (SC), Biological and Environmental Research (BER); USDOE Office of Electricity (OE)

Grant/Contract Number:: 10673090 B2; AC05-76RL01830; 57558

OSTI ID:: 1877719

Alternate ID(s):: OSTI ID: 1774002

Report Number(s):: PNNL-SA-161062; S2666386421000035; 100323; PII: S2666386421000035

Journal Information:: Cell Reports Physical Science, Journal Name: Cell Reports Physical Science Vol. 2 Journal Issue: 2; ISSN 2666-3864

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

References (39)

Effect of the damping function in dispersion corrected density functional theory Grimme, Stefan; Ehrlich, Stephan; Goerigk, Lars Journal of Computational Chemistry, Vol. 32, Issue 7 https://doi.org/10.1002/jcc.21759	journal	March 2011
1:14 Heteropolyvanadate of phosphorus: preparation and structure Kato, R.; Kobayashi, A.; Sasaki, Y. Journal of the American Chemical Society, Vol. 102, Issue 21 https://doi.org/10.1021/ja00541a039	journal	October 1980
Intercalation of Polyvalent Cations into V₂O₅ Aerogels Le, D. B.; Passerini, S.; Coustier, F. Chemistry of Materials, Vol. 10, Issue 3, p. 682-684 https://doi.org/10.1021/cm9705101	journal	March 1998
Synthesis and crystal structure of α-NH4(VO2)(HPO4) Amoros, P.; Le Bail, A. Journal of Solid State Chemistry, Vol. 97, Issue 2 https://doi.org/10.1016/0022-4596(92)90035-T	journal	April 1992
Vanadium-51 and oxygen-17 nuclear magnetic resonance study of vanadate(V) equilibria and kinetics Heath, Elizabeth; Howarth, Oliver W. Journal of the Chemical Society, Dalton Transactions, Issue 5 https://doi.org/10.1039/dt9810001105	journal	January 1981
A thermodynamic model for vanadate in aqueous solution – equilibria and reaction enthalpies McCann, Nichola; Wagner, Michael; Hasse, Hans Dalton Trans., Vol. 42, Issue 7 https://doi.org/10.1039/C2DT31993D	journal	January 2013
A review of electrolyte additives and impurities in vanadium redox flow batteries Cao, Liuyue; Skyllas-Kazacos, Maria; Menictas, Chris Journal of Energy Chemistry, Vol. 27, Issue 5 https://doi.org/10.1016/j.jechem.2018.04.007	journal	September 2018
Vanadium Oxide Oligomers and Ordered Monolayers Supported on CeO ₂ (111): Structure and Stability Studied by Density Functional Theory Penschke, Christopher; Paier, Joachim; Sauer, Joachim The Journal of Physical Chemistry C, Vol. 122, Issue 16 https://doi.org/10.1021/acs.jpcc.8b01998	journal	April 2018
⁵¹ V magic angle spinning NMR in VOPO ₄ phases: ⁵¹ V magic angle spinning NMR in VOPO ₄ phases Siegel, Renée; Dupré, Nicolas; Quarton, Michel Magnetic Resonance in Chemistry, Vol. 42, Issue 12 https://doi.org/10.1002/mrc.1485	journal	September 2004
The crystal and molecular structure of oxovanadium(V) orthophosphate dihydrate, VOPO4,2H2O Tietze, Hr Australian Journal of Chemistry, Vol. 34, Issue 10 https://doi.org/10.1071/CH9812035	journal	January 1981
Structural Diversity of the Oxovanadium Organodiphosphonate System: A Platform for the Design of Void Channels Ouellette, Wayne; Yu, Ming Hui; O'Connor, Charles J. Inorganic Chemistry, Vol. 45, Issue 8 https://doi.org/10.1021/ic0517422	journal	April 2006
Recent Progress in Redox Flow Battery Research and Development Wang, Wei; Luo, Qingtao; Li, Bin Advanced Functional Materials, Vol. 23, Issue 8, p. 970-986 https://doi.org/10.1002/adfm.201200694	journal	September 2012
Evaluation of Precipitation Inhibitors for Supersaturated Vanadyl Electrolytes for the Vanadium Redox Battery Skyllas-Kazacos, Maria Electrochemical and Solid-State Letters, Vol. 2, Issue 3 https://doi.org/10.1149/1.1390754	journal	January 1999
Chloride supporting electrolytes for all-vanadium redox flow batteries Kim, Soowhan; Vijayakumar, M.; Wang, Wei Physical Chemistry Chemical Physics, Vol. 13, Issue 40 https://doi.org/10.1039/c1cp22638j	journal	January 2011
Investigation of Ion–Solvent Interactions in Nonaqueous Electrolytes Using in Situ Liquid SIMS Zhang, Yanyan; Su, Mao; Yu, Xiaofei Analytical Chemistry, Vol. 90, Issue 5 https://doi.org/10.1021/acs.analchem.7b04921	journal	February 2018
From ultrasoft pseudopotentials to the projector augmented-wave method Kresse, G.; Joubert, D. Physical Review B, Vol. 59, Issue 3, p. 1758-1775 https://doi.org/10.1103/PhysRevB.59.1758	journal	January 1999
Raman Study of Sulfuric Acid at Low Temperatures Tomikawa, Koichi; Kanno, Hitoshi The Journal of Physical Chemistry A, Vol. 102, Issue 30 https://doi.org/10.1021/jp980904v	journal	July 1998
In Situ Liquid Secondary Ion Mass Spectrometry: A Surprisingly Soft Ionization Process for Investigation of Halide Ion Hydration Zhang, Yanyan; Zeng, Wenjuan; Huang, Liuqin Analytical Chemistry, Vol. 91, Issue 11 https://doi.org/10.1021/acs.analchem.8b05804	journal	April 2019
Towards understanding the poor thermal stability of V5+ electrolyte solution in Vanadium Redox Flow Batteries Vijayakumar, M.; Li, Liyu; Graff, Gordon Journal of Power Sources, Vol. 196, Issue 7 https://doi.org/10.1016/j.jpowsour.2010.11.126	journal	April 2011
Vanadium phosphates on mesoporous supports: model catalysts for solid-state NMR studies of the selective oxidation of n-butane Frey, Jörg; Sang Ooi, Yean; Thomas, Bejoy Solid State Nuclear Magnetic Resonance, Vol. 35, Issue 2 https://doi.org/10.1016/j.ssnmr.2009.02.005	journal	April 2009
Synthesis and Crystal Structure of a New Vanadyl Phosphate [H _0.6 (VO) ₃ (PO ₄ ) ₃ (H ₂ O) ₃ ]·4H ₂ O and Its Conversion to Porous Products Shpeizer, Boris G.; Ouyang, Xiang; Heising, Joy M. Chemistry of Materials, Vol. 13, Issue 7 https://doi.org/10.1021/cm0008821	journal	July 2001
Synthesis and Crystal Structure of Decavanadate-Based Coordination Polymers Jin, Kang P.; Jiang, Hai J.; Wang, Yan Journal of Cluster Science, Vol. 29, Issue 4 https://doi.org/10.1007/s10876-018-1391-5	journal	May 2018
Chemistry with ADF te Velde, G.; Bickelhaupt, F. M.; Baerends, E. J. Journal of Computational Chemistry, Vol. 22, Issue 9, p. 931-967 https://doi.org/10.1002/jcc.1056	journal	January 2001
Synthetic pathways to vanadyl phosphates Beltranporter, D.; Amoros, P.; Ibanez, R. Solid State Ionics, Vol. 32-33 https://doi.org/10.1016/0167-2738(89)90203-8	journal	February 1989
Raman Microspectrometry Study of Electrochemical Lithium Intercalation into Sputtered Crystalline V 2 O 5 Thin Films Baddour-Hadjean, R.; Pereira-Ramos, J. P.; Navone, C. Chemistry of Materials, Vol. 20, Issue 5 https://doi.org/10.1021/cm702979k	journal	March 2008
The Effect of Additives on the High-Temperature Stability of the Vanadium Redox Flow Battery Positive Electrolytes Kausar, Nadeem; Mousa, Asem; Skyllas-Kazacos, Maria ChemElectroChem, Vol. 3, Issue 2 https://doi.org/10.1002/celc.201500453	journal	November 2015
⁵¹ V FT-nmr investigations of metavanadate ions in aqueous solutions Habayeb, Mahmoud Adam; Hileman Jr, O. E. Canadian Journal of Chemistry, Vol. 58, Issue 21 https://doi.org/10.1139/v80-363	journal	November 1980
⁵¹ V MAS NMR Investigation of ⁵¹ V Quadrupole Coupling and Chemical Shift Anisotropy in Divalent Metal Pyrovanadates Nielsen, Ulla Gro; Jakobsen, Hans J.; Skibsted, Jørgen The Journal of Physical Chemistry B, Vol. 105, Issue 2 https://doi.org/10.1021/jp002882u	journal	January 2001
Vanadium redox cell electrolyte optimization studies Kazacos, M.; Cheng, M.; Skyllas-Kazacos, M. Journal of Applied Electrochemistry, Vol. 20, Issue 3 https://doi.org/10.1007/BF01076057	journal	May 1990
Elucidating the higher stability of vanadium(V) cations in mixed acid based redox flow battery electrolytes Vijayakumar, M.; Wang, Wei; Nie, Zimin Journal of Power Sources, Vol. 241 https://doi.org/10.1016/j.jpowsour.2013.04.072	journal	November 2013
α-Ammonium Vanadium Hydrogen Phosphate, α-(NH ₄ )V(HPO ₄ ) ₂ Bircsak, Z.; Harrison, W. T. A. Acta Crystallographica Section C Crystal Structure Communications, Vol. 54, Issue 9 https://doi.org/10.1107/S0108270198002856	journal	September 1998
Structure of vanadium phosphate anion in solutions from17O,51V and31P NMR data Fedotov, M. A.; Maksimovskaya, R. I.; Kazanskii, L. P. Reaction Kinetics and Catalysis Letters, Vol. 16, Issue 2-3 https://doi.org/10.1007/BF02065455	journal	June 1981
Comment on “Generalized Gradient Approximation Made Simple” Zhang, Yingkai; Yang, Weitao Physical Review Letters, Vol. 80, Issue 4 https://doi.org/10.1103/PhysRevLett.80.890	journal	January 1998
A Stable Vanadium Redox-Flow Battery with High Energy Density for Large-Scale Energy Storage Li, Liyu; Kim, Soowhan; Wang, Wei Advanced Energy Materials, Vol. 1, Issue 3, p. 394-400 https://doi.org/10.1002/aenm.201100008	journal	March 2011
Structure and stability of hexa-aqua V(iii) cations in vanadium redox flow battery electrolytes Vijayakumar, M.; Li, Liyu; Nie, Zimin Physical Chemistry Chemical Physics, Vol. 14, Issue 29 https://doi.org/10.1039/c2cp40707h	journal	January 2012
Hetero and lacunary polyoxovanadate chemistry: Synthesis, reactivity and structural aspects Hayashi, Yoshihito Coordination Chemistry Reviews, Vol. 255, Issue 19-20 https://doi.org/10.1016/j.ccr.2011.02.013	journal	October 2011
Facile synthesis of ammonium vanadate nanofibers by using reflux in aqueous V 2 O 5 solution with ammonium persulfate Lee, Se Hun; Koo, Jun Mo; Oh, Seong Geun Materials Chemistry and Physics, Vol. 194 https://doi.org/10.1016/j.matchemphys.2017.03.053	journal	June 2017
Lattice Dynamics of β-V ₂ O ₅ : Raman Spectroscopic Insight into the Atomistic Structure of a High-Pressure Vanadium Pentoxide Polymorph Baddour-Hadjean, R.; Smirnov, M. B.; Smirnov, K. S. Inorganic Chemistry, Vol. 51, Issue 5 https://doi.org/10.1021/ic202651b	journal	February 2012
Understanding Aqueous Electrolyte Stability through Combined Computational and Magnetic Resonance Spectroscopy: A Case Study on Vanadium Redox Flow Battery Electrolytes Vijayakumar, Murugesan; Nie, Zimin; Walter, Eric ChemPlusChem, Vol. 80, Issue 2 https://doi.org/10.1002/cplu.201402139	journal	September 2014

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25 ENERGY STORAGE
redox flow battery
vanadium solvation
electrolyte stability
nucleation processes
additives design

Title: Accelerated design of vanadium redox flow battery electrolytes through tunable solvation chemistry

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