Highly reversible Zn anode with a practical areal capacity enabled by a sustainable electrolyte and superacid interfacial chemistry

Li, Chang; Shyamsunder, Abhinandan; Hoane, Alexis Grace; Long, Daniel M.; Kwok, Chun Yuen; Kotula, Paul G.; Zavadil, Kevin R.; Gewirth, Andrew A.; Nazar, Linda F.

doi:10.1016/j.joule.2022.04.017

Highly reversible Zn anode with a practical areal capacity enabled by a sustainable electrolyte and superacid interfacial chemistry

Journal Article · Wed May 18 00:00:00 EDT 2022 · Joule

DOI:https://doi.org/10.1016/j.joule.2022.04.017· OSTI ID:1872004

Li, Chang ^[1]; Shyamsunder, Abhinandan ^[1]; Hoane, Alexis Grace ^[2]; Long, Daniel M. ^[3]; Kwok, Chun Yuen ^[4]; Kotula, Paul G. ^[5]; Zavadil, Kevin R. ^[1]; Gewirth, Andrew A. ^[2]; Nazar, Linda F. ^[1]

Univ. of Waterloo, ON (Canada); Argonne National Lab. (ANL), Argonne, IL (United States)
Argonne National Lab. (ANL), Argonne, IL (United States); Univ. of Illinois at Urbana-Champaign, IL (United States)
Argonne National Lab. (ANL), Argonne, IL (United States); Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Univ. of Waterloo, ON (Canada)
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)

Aqueous zinc-metal batteries are plagued by poor Zn reversibility owing to zinc dendrite and layered double hydroxide (LDH) formation. Here, we introduce a novel additive—N,N-dimethylformamidium trifluoromethanesulfonate (DOTf)—in a low-cost aqueous electrolyte that can very effectively address these issues. The initial water-assisted dissociation of DOTf into triflic superacid creates a robust nanostructured solid-electrolyte interface (SEI)—revealed by operando spectroscopy and cryomicroscopy—which excludes water and enables dense Zn deposition. We demonstrate excellent Zn plating/stripping in a Zn||Cu asymmetric cell for more than 3,500 cycles. Furthermore, near 100% CE is realized at a combined high current density of 4 mA cm^-2 and an areal capacity of 4 mAh cm^-2 over long-term cycling. Zn||Zn_0.25V₂O₅·nH₂O full cells retain ~83% of their capacity after 1,000 cycles with mass-limited Zn anodes. By restricting the depth of discharge, the cathodes exhibit less proton intercalation and LDH formation with an extended lifetime of 2,000 cycles.

View Accepted Manuscript (DOE)

Research Organization:: Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States)

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

Grant/Contract Number:: NA0003525

OSTI ID:: 1872004

Report Number(s):: SAND2022-6489J; 706092

Journal Information:: Joule, Journal Name: Joule Journal Issue: 5 Vol. 6; ISSN 2542-4351

Publisher:: Elsevier - Cell PressCopyright Statement

Country of Publication:: United States

Language:: English

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