Chemical Challenges that the Peroxide Dianion Presents to Rechargeable Lithium–Air Batteries

Nava, Matthew; Thorarinsdottir, Agnes E.; Lopez, Nazario; Cummins, Christopher C.; Nocera, Daniel G.

doi:10.1021/acs.chemmater.2c00282

Title: Chemical Challenges that the Peroxide Dianion Presents to Rechargeable Lithium–Air Batteries

Journal Article · Thu Apr 21 00:00:00 EDT 2022 · Chemistry of Materials

DOI:https://doi.org/10.1021/acs.chemmater.2c00282· OSTI ID:1989832

Nava, Matthew ^[1];

^[1]; Lopez, Nazario ^[2];

^[3];

^[1]

Harvard University, Cambridge, MA (United States)
Universidad Autónoma del Estado de Morelos, Morelos (Mexico)
Massachusetts Institute of Technology, Cambridge, MA (United States)

Understanding the fundamental redox reactions and processes that occur in lithium–air and, more generally, metal–air batteries is important to the progress of this promising energy-storage technology. Knowledge of the chemistry of the peroxide dianion, O₂^2–, is especially crucial, as the dianion is at the nexus of the charge/discharge cycle of lithium–air batteries. The intrinsic electron transfer properties and redox chemistry of peroxide dianion are poorly defined because it is difficult to isolate the dianion free of protons and metal ions. We review the results of (i) the electron transfer kinetics and (ii) the redox reaction chemistry of isolated peroxide dianion encapsulated within the cavity of a hexacarboxamide cryptand. With regard to the former, electron transfer kinetics measurements provide fundamental Marcus parameters that will be useful for models that seek to disentangle the precise contributions of Li⁺ ion-coupled electron transfer, electron transfer across the Li₂O₂ solid particle interface, and charge hopping among Li₂O₂ particles. With regard to the latter, an underappreciated chemistry of peroxide dianion with CO₂ produces peroxymonocarbonate (OOCO₂^2–) and peroxydicarbonate (O₂COOCO₂^2–). An autocatalytic cycle will lead to oxidative degradation of traditional organic electrolytes and other vulnerable cell components employed in lithium–air batteries. Furthermore, this peroxycarbonate-derived chemistry, in addition to more commonly recognized solution-based oxidation chemistry, will need to be mitigated to realize the long-term cyclability of rechargeable lithium–air batteries.

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Research Organization:: Harvard Univ., Cambridge, MA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)

Grant/Contract Number:: SC0021639

OSTI ID:: 1989832

Journal Information:: Chemistry of Materials, Vol. 34, Issue 9; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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