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

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

Research output: Contribution to journalArticlepeer-review

Abstract

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||Zn0.25V2O5·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.

Original languageEnglish (US)
Pages (from-to)1103-1120
Number of pages18
JournalJoule
Volume6
Issue number5
DOIs
StatePublished - May 18 2022

Keywords

  • cryo-TEM
  • SEIRAS
  • Superacid
  • XPS
  • Zn anode
  • Zn metal batteries
  • Zn-ion batteries

ASJC Scopus subject areas

  • Energy(all)

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