Tuning the Reversibility of Mg Anodes via Controlled Surface Passivation by H2O/Cl– in Organic Electrolytes

Connell, Justin G.; Genorio, Bostjan; Lopes, Pietro Papa; Strmcnik, Dusan; Stamenkovic, Vojislav R.; Markovic, Nenad M.

doi:10.1021/acs.chemmater.6b03227

Tuning the Reversibility of Mg Anodes via Controlled Surface Passivation by H₂O/Cl^– in Organic Electrolytes

Journal Article · Mon Oct 17 00:00:00 EDT 2016 · Chemistry of Materials

DOI:https://doi.org/10.1021/acs.chemmater.6b03227· OSTI ID:1339153

Connell, Justin G. ^[1]; Genorio, Bostjan ^[2]; Lopes, Pietro Papa ^[1]; Strmcnik, Dusan ^[1]; Stamenkovic, Vojislav R. ^[1]; Markovic, Nenad M. ^[1]

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

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.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1339153

Journal Information:: Chemistry of Materials, Journal Name: Chemistry of Materials Journal Issue: 22 Vol. 28; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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