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

Abstract

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, O22–, 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 (OOCO22–) and peroxydicarbonate (O2COOCO22–). 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 tomore » more commonly recognized solution-based oxidation chemistry, will need to be mitigated to realize the long-term cyclability of rechargeable lithium–air batteries.« less

Authors:
 [1]; ORCiD logo [1];  [2]; ORCiD logo [3]; ORCiD logo [1]
+ Show Author Affiliations
  1. Harvard University, Cambridge, MA (United States)
  2. Universidad Autónoma del Estado de Morelos, Morelos (Mexico)
  3. Massachusetts Institute of Technology, Cambridge, MA (United States)
Publication Date:
Research Org.:
Harvard Univ., Cambridge, MA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)
OSTI Identifier:
1989832
Grant/Contract Number:  
SC0021639
Resource Type:
Accepted Manuscript
Journal Name:
Chemistry of Materials
Additional Journal Information:
Journal Volume: 34; Journal Issue: 9; Journal ID: ISSN 0897-4756
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; Batteries; Charge transfer; Ethers; Macrocyclic compounds; Oxides

Citation Formats

Nava, Matthew, Thorarinsdottir, Agnes E., Lopez, Nazario, Cummins, Christopher C., and Nocera, Daniel G. Chemical Challenges that the Peroxide Dianion Presents to Rechargeable Lithium–Air Batteries. United States: N. p., 2022. Web. doi:10.1021/acs.chemmater.2c00282.
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Nava, Matthew, Thorarinsdottir, Agnes E., Lopez, Nazario, Cummins, Christopher C., & Nocera, Daniel G. Chemical Challenges that the Peroxide Dianion Presents to Rechargeable Lithium–Air Batteries. United States. https://doi.org/10.1021/acs.chemmater.2c00282
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Nava, Matthew, Thorarinsdottir, Agnes E., Lopez, Nazario, Cummins, Christopher C., and Nocera, Daniel G. Thu . "Chemical Challenges that the Peroxide Dianion Presents to Rechargeable Lithium–Air Batteries". United States. https://doi.org/10.1021/acs.chemmater.2c00282. https://www.osti.gov/servlets/purl/1989832.
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@article{osti_1989832,
title = {Chemical Challenges that the Peroxide Dianion Presents to Rechargeable Lithium–Air Batteries},
author = {Nava, Matthew and Thorarinsdottir, Agnes E. and Lopez, Nazario and Cummins, Christopher C. and Nocera, Daniel G.},
abstractNote = {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, O22–, 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 (OOCO22–) and peroxydicarbonate (O2COOCO22–). 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.},
doi = {10.1021/acs.chemmater.2c00282},
journal = {Chemistry of Materials},
number = 9,
volume = 34,
place = {United States},
year = {Thu Apr 21 00:00:00 EDT 2022},
month = {Thu Apr 21 00:00:00 EDT 2022}
}
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