Strengthening Aqueous Electrolytes without Strengthening Water
Dr. Longteng Tang
Department of Chemistry, Oregon State University, Corvallis, OR, 97331-4003 USA
These authors contributed equally to this work.
Contribution: Data curation (lead), Formal analysis (lead), Writing - original draft (lead)
Search for more papers by this authorDr. Yunkai Xu
Department of Chemistry, Oregon State University, Corvallis, OR, 97331-4003 USA
These authors contributed equally to this work.
Contribution: Data curation (lead), Formal analysis (lead), Writing - original draft (lead)
Search for more papers by this authorWeiyi Zhang
Materials Science and Engineering, University of California, Riverside, CA, 92521 USA
These authors contributed equally to this work.
Contribution: Data curation (equal), Formal analysis (equal), Writing - original draft (equal)
Search for more papers by this authorYiming Sui
Department of Chemistry, Oregon State University, Corvallis, OR, 97331-4003 USA
Contribution: Data curation (supporting), Formal analysis (supporting), Writing - original draft (supporting)
Search for more papers by this authorAlexis Scida
Department of Chemistry, Oregon State University, Corvallis, OR, 97331-4003 USA
Contribution: Data curation (supporting), Formal analysis (supporting)
Search for more papers by this authorSean R. Tachibana
Department of Chemistry, Oregon State University, Corvallis, OR, 97331-4003 USA
Contribution: Data curation (supporting), Formal analysis (supporting)
Search for more papers by this authorMounesha Garaga
Hunter College, City University of New York, New York, NY, 10065 USA
Contribution: Data curation (supporting), Formal analysis (supporting)
Search for more papers by this authorSean K. Sandstrom
Department of Chemistry, Oregon State University, Corvallis, OR, 97331-4003 USA
Contribution: Data curation (supporting), Formal analysis (supporting)
Search for more papers by this authorNan-Chieh Chiu
Department of Chemistry, Oregon State University, Corvallis, OR, 97331-4003 USA
Contribution: Data curation (supporting), Formal analysis (supporting)
Search for more papers by this authorProf. Kyriakos C. Stylianou
Department of Chemistry, Oregon State University, Corvallis, OR, 97331-4003 USA
Contribution: Formal analysis (supporting), Supervision (supporting)
Search for more papers by this authorProf. Steve G. Greenbaum
Hunter College, City University of New York, New York, NY, 10065 USA
Contribution: Formal analysis (supporting), Supervision (supporting)
Search for more papers by this authorCorresponding Author
Prof. Peter Alex Greaney
Materials Science and Engineering, University of California, Riverside, CA, 92521 USA
Contribution: Conceptualization (supporting), Formal analysis (supporting), Funding acquisition (equal), Supervision (supporting)
Search for more papers by this authorCorresponding Author
Prof. Chong Fang
Department of Chemistry, Oregon State University, Corvallis, OR, 97331-4003 USA
Contribution: Conceptualization (supporting), Formal analysis (supporting), Funding acquisition (supporting), Supervision (supporting), Writing - original draft (supporting), Writing - review & editing (supporting)
Search for more papers by this authorCorresponding Author
Prof. Xiulei Ji
Department of Chemistry, Oregon State University, Corvallis, OR, 97331-4003 USA
Contribution: Conceptualization (lead), Formal analysis (lead), Funding acquisition (lead), Project administration (lead), Supervision (lead), Writing - original draft (supporting), Writing - review & editing (lead)
Search for more papers by this authorDr. Longteng Tang
Department of Chemistry, Oregon State University, Corvallis, OR, 97331-4003 USA
These authors contributed equally to this work.
Contribution: Data curation (lead), Formal analysis (lead), Writing - original draft (lead)
Search for more papers by this authorDr. Yunkai Xu
Department of Chemistry, Oregon State University, Corvallis, OR, 97331-4003 USA
These authors contributed equally to this work.
Contribution: Data curation (lead), Formal analysis (lead), Writing - original draft (lead)
Search for more papers by this authorWeiyi Zhang
Materials Science and Engineering, University of California, Riverside, CA, 92521 USA
These authors contributed equally to this work.
Contribution: Data curation (equal), Formal analysis (equal), Writing - original draft (equal)
Search for more papers by this authorYiming Sui
Department of Chemistry, Oregon State University, Corvallis, OR, 97331-4003 USA
Contribution: Data curation (supporting), Formal analysis (supporting), Writing - original draft (supporting)
Search for more papers by this authorAlexis Scida
Department of Chemistry, Oregon State University, Corvallis, OR, 97331-4003 USA
Contribution: Data curation (supporting), Formal analysis (supporting)
Search for more papers by this authorSean R. Tachibana
Department of Chemistry, Oregon State University, Corvallis, OR, 97331-4003 USA
Contribution: Data curation (supporting), Formal analysis (supporting)
Search for more papers by this authorMounesha Garaga
Hunter College, City University of New York, New York, NY, 10065 USA
Contribution: Data curation (supporting), Formal analysis (supporting)
Search for more papers by this authorSean K. Sandstrom
Department of Chemistry, Oregon State University, Corvallis, OR, 97331-4003 USA
Contribution: Data curation (supporting), Formal analysis (supporting)
Search for more papers by this authorNan-Chieh Chiu
Department of Chemistry, Oregon State University, Corvallis, OR, 97331-4003 USA
Contribution: Data curation (supporting), Formal analysis (supporting)
Search for more papers by this authorProf. Kyriakos C. Stylianou
Department of Chemistry, Oregon State University, Corvallis, OR, 97331-4003 USA
Contribution: Formal analysis (supporting), Supervision (supporting)
Search for more papers by this authorProf. Steve G. Greenbaum
Hunter College, City University of New York, New York, NY, 10065 USA
Contribution: Formal analysis (supporting), Supervision (supporting)
Search for more papers by this authorCorresponding Author
Prof. Peter Alex Greaney
Materials Science and Engineering, University of California, Riverside, CA, 92521 USA
Contribution: Conceptualization (supporting), Formal analysis (supporting), Funding acquisition (equal), Supervision (supporting)
Search for more papers by this authorCorresponding Author
Prof. Chong Fang
Department of Chemistry, Oregon State University, Corvallis, OR, 97331-4003 USA
Contribution: Conceptualization (supporting), Formal analysis (supporting), Funding acquisition (supporting), Supervision (supporting), Writing - original draft (supporting), Writing - review & editing (supporting)
Search for more papers by this authorCorresponding Author
Prof. Xiulei Ji
Department of Chemistry, Oregon State University, Corvallis, OR, 97331-4003 USA
Contribution: Conceptualization (lead), Formal analysis (lead), Funding acquisition (lead), Project administration (lead), Supervision (lead), Writing - original draft (supporting), Writing - review & editing (lead)
Search for more papers by this authorAbstract
Aqueous electrolytes typically suffer from poor electrochemical stability; however, eutectic aqueous solutions—25 wt.% LiCl and 62 wt.% H3PO4—cooled to −78 °C exhibit a significantly widened stability window. Integrated experimental and simulation results reveal that, upon cooling, Li+ ions become less hydrated and pair up with Cl−, ice-like water clusters form, and H⋅⋅⋅Cl− bonding strengthens. Surprisingly, this low-temperature solvation structure does not strengthen water molecules’ O−H bond, bucking the conventional wisdom that increasing water's stability requires stiffening the O−H covalent bond. We propose a more general mechanism for water's low temperature inertness in the electrolyte: less favorable solvation of OH− and H+, the byproducts of hydrogen and oxygen evolution reactions. To showcase this stability, we demonstrate an aqueous Li-ion battery using LiMn2O4 cathode and CuSe anode with a high energy density of 109 Wh/kg. These results highlight the potential of aqueous batteries for polar and extraterrestrial missions.
Conflict of interest
The authors declare no conflict of interest.
Open Research
Data Availability Statement
The main data supporting the findings of this study are available within the article and Supporting Information. Additional data are available from the corresponding authors on request.
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