Tuning the Reversibility of Mg Anodes via Controlled Surface Passivation by H2O/Cl– in Organic Electrolytes
Abstract
Developing a new generation of battery chemistries is a critical challenge to moving beyond current Li-ion technologies. In this work, we introduce a surface-science-based approach for understanding the complex phenomena controlling the reversibility of Mg anodes for Mg-ion batteries. In addition, we identify the profound impact of trace levels of H2O (≤3 ppm) on the kinetics of Mg deposition and determine that passive films of MgO and Mg(OH)2 are formed only after Mg deposition ceases, rather than continuously during Mg reduction. We also find that Cl– inhibits passivation through the formation of adsorbed Cl– (Mg–Cl(ad)) and/or MgCl2 on the surface, as well as through a dynamic competition with H2O in the double layer. In conclusion, this surface-science-based approach goes well beyond Mg anodes, highlighting the need for more in-depth understanding of electrolyte chemistries before a new generation of efficient and reversible battery technologies can be realized.
- Authors:
-
- Argonne National Lab. (ANL), Argonne, IL (United States). Joint Center for Energy Storage Research (JCESR) and Materials Science Division
- Argonne National Lab. (ANL), Argonne, IL (United States). Joint Center for Energy Storage Research (JCESR) and Materials Science Division; University of Ljubljana (Slovenia). Department of Chemical Engineering and Technical Safety
- Publication Date:
- Research Org.:
- Argonne National Laboratory (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1339153
- Grant/Contract Number:
- AC02-06CH11357
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Chemistry of Materials
- Additional Journal Information:
- Journal Volume: 28; Journal Issue: 22; Journal ID: ISSN 0897-4756
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Connell, Justin G., Genorio, Bostjan, Lopes, Pietro Papa, Strmcnik, Dusan, Stamenkovic, Vojislav R., and Markovic, Nenad M. Tuning the Reversibility of Mg Anodes via Controlled Surface Passivation by H2O/Cl– in Organic Electrolytes. United States: N. p., 2016.
Web. doi:10.1021/acs.chemmater.6b03227.
Connell, Justin G., Genorio, Bostjan, Lopes, Pietro Papa, Strmcnik, Dusan, Stamenkovic, Vojislav R., & Markovic, Nenad M. Tuning the Reversibility of Mg Anodes via Controlled Surface Passivation by H2O/Cl– in Organic Electrolytes. United States. https://doi.org/10.1021/acs.chemmater.6b03227
Connell, Justin G., Genorio, Bostjan, Lopes, Pietro Papa, Strmcnik, Dusan, Stamenkovic, Vojislav R., and Markovic, Nenad M. Mon .
"Tuning the Reversibility of Mg Anodes via Controlled Surface Passivation by H2O/Cl– in Organic Electrolytes". United States. https://doi.org/10.1021/acs.chemmater.6b03227. https://www.osti.gov/servlets/purl/1339153.
@article{osti_1339153,
title = {Tuning the Reversibility of Mg Anodes via Controlled Surface Passivation by H2O/Cl– in Organic Electrolytes},
author = {Connell, Justin G. and Genorio, Bostjan and Lopes, Pietro Papa and Strmcnik, Dusan and Stamenkovic, Vojislav R. and Markovic, Nenad M.},
abstractNote = {Developing a new generation of battery chemistries is a critical challenge to moving beyond current Li-ion technologies. In this work, we introduce a surface-science-based approach for understanding the complex phenomena controlling the reversibility of Mg anodes for Mg-ion batteries. In addition, we identify the profound impact of trace levels of H2O (≤3 ppm) on the kinetics of Mg deposition and determine that passive films of MgO and Mg(OH)2 are formed only after Mg deposition ceases, rather than continuously during Mg reduction. We also find that Cl– inhibits passivation through the formation of adsorbed Cl– (Mg–Cl(ad)) and/or MgCl2 on the surface, as well as through a dynamic competition with H2O in the double layer. In conclusion, this surface-science-based approach goes well beyond Mg anodes, highlighting the need for more in-depth understanding of electrolyte chemistries before a new generation of efficient and reversible battery technologies can be realized.},
doi = {10.1021/acs.chemmater.6b03227},
journal = {Chemistry of Materials},
number = 22,
volume = 28,
place = {United States},
year = {Mon Oct 17 00:00:00 EDT 2016},
month = {Mon Oct 17 00:00:00 EDT 2016}
}
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