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Understanding Thermodynamic and Kinetic Contributions in Expanding the Stability Window of Aqueous Electrolytes
Open accessAbstract
Summary Aqueous electrolytes come with an intrinsic narrow electrochemical stability window (1.23 V). Expanding this window represents significant benefits in both fundamental science and practical battery applications. Recent breakthroughs made via super-concentration have resulted in >3.0 V windows, but fundamental understanding of the related mechanism is still absent. In the present work, we examined the widened window (2.55 V) of a super-concentrated (unsaturated) aqueous solution of LiNO3 through both theoretical and spectral analyses and discovered that a local structure of intimate Li+-water interaction arises at super-concentration, generating (Li+(H2O)2)n polymer-like chains to replace the ubiquitous hydrogen bonding between water molecules. Such structure is mainly responsible for the expanded electrochemical stability window. Further theoretical and experimental analyses quantitatively differentiate the contributions to this window, identifying the kinetic factor (desolvation) as the main contributor. Such molecular-level and quantitative understanding will further assist in tailor designing more effective approaches to stabilizing water electrochemically.
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Cites
“Water-in-salt” electrolyte enables high-voltage aqueous lithium-ion chemistries
Suo, L., Borodin, O., Gao, T., Olguin, M., Ho, J., Fan, X., Luo, C., Wang, C., & Xu, K. (2015) · Science · doi:10.1126/science.aab1595 · Cited by 3,821
Self-citationRunaway risk of forming toxic compounds
Hammami, A., Raymond, N., & Armand, M. (2003) · Nature · doi:10.1038/424635b · Cited by 346
Cited by
Designing Electrolyte Structure to Suppress Hydrogen Evolution Reaction in Aqueous Batteries
Nian, Q., Zhang, X., Feng, Y., Liu, S., Sun, T., Zheng, S., Ren, X., Tao, Z., Zhang, D., & Chen, J. (2021) · ACS Energy Letters · doi:10.1021/acsenergylett.1c00833 · Cited by 303
Self-citationChen, J., Vatamanu, J., Xing, L., Borodin, O., Chen, H., Guan, X., Liu, X., Xu, K., & Li, W. (2020) · Advanced Energy Materials · doi:10.1002/aenm.201902654 · Cited by 260
Self-citationLocalized Water‐In‐Salt Electrolyte for Aqueous Lithium‐Ion Batteries
Jaumaux, P., Yang, X., Zhang, B., Safaei, J., Tang, X., Zhou, D., Wang, C., & Wang, G. (2021) · Angewandte Chemie International Edition · doi:10.1002/anie.202107389 · Cited by 205
Metadata
- Authors
- Zheng, J., Tan, G., Shan, P., Liu, T., Hu, J., Feng, Y., Yang, L., Zhang, M., Chen, Z., Lin, Y., Lu, J., Neuefeind, J. C., Ren, Y., Amine, K., Wang, L.-W., Xu, K., & Pan, F.
- Venue
- Chem
- Publisher
- Elsevier BV
- Published
- 2018-12
- Volume
- 4
- Issue
- 12
- Pages
- 2872-2882
- ISSN
- 2451-9294 (ISSN-L)
- OpenAlex
- W2896229665
- Cited by
- 308
- References
- 2
- FWCI
- 9.31
- Type
- journal article
- Language
- en
- Open access
- bronze
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- Zheng, J., Tan, G., Shan, P., Liu, T., Hu, J., Feng, Y., Yang, L., Zhang, M., Chen, Z., Lin, Y., Lu, J., Neuefeind, J. C., Ren, Y., Amine, K., Wang, L.-W., Xu, K., & Pan, F. (2018). Understanding Thermodynamic and Kinetic Contributions in Expanding the Stability Window of Aqueous Electrolytes. Chem. https://doi.org/10.1016/j.chempr.2018.09.004
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