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Enhancing electrochemical intermediate solvation through electrolyte anion selection to increase nonaqueous Li–O 2 battery capacity

Proceedings of the National Academy of Sciences - PNAS, 2015-07, Vol.112 (30), p.9293-9298 [Peer Reviewed Journal]

ISSN: 0027-8424 ;EISSN: 1091-6490 ;DOI: 10.1073/pnas.1505728112

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  • Title:
    Enhancing electrochemical intermediate solvation through electrolyte anion selection to increase nonaqueous Li–O 2 battery capacity
  • Author: Burke, Colin M. ; Pande, Vikram ; Khetan, Abhishek ; Viswanathan, Venkatasubramanian ; McCloskey, Bryan D.
  • Is Part Of: Proceedings of the National Academy of Sciences - PNAS, 2015-07, Vol.112 (30), p.9293-9298
  • Description: Significance The Li–air battery has attracted significant interest as a potential high-energy alternative to Li-ion batteries. However, the battery discharge product, lithium peroxide, is both electronically insulative and insoluble in nonaqueous electrolytes. It therefore passivates the battery cathode as it is uniformly deposited and disallows the battery to achieve even a modest fraction of its potential electrochemical capacity. Our objective is to circumvent this challenge by enhancing the solubility of electrochemically formed intermediate species. We present a rational basis for electrolyte (i.e., solvent and salt) selection for nonaqueous Li–air batteries and demonstrate a selection criterion for an electrolyte salt that increases the stability of Li + in solution, thereby triggering a solution-based process that allows significantly improved battery capacities. Among the “beyond Li-ion” battery chemistries, nonaqueous Li–O 2 batteries have the highest theoretical specific energy and, as a result, have attracted significant research attention over the past decade. A critical scientific challenge facing nonaqueous Li–O 2 batteries is the electronically insulating nature of the primary discharge product, lithium peroxide, which passivates the battery cathode as it is formed, leading to low ultimate cell capacities. Recently, strategies to enhance solubility to circumvent this issue have been reported, but rely upon electrolyte formulations that further decrease the overall electrochemical stability of the system, thereby deleteriously affecting battery rechargeability. In this study, we report that a significant enhancement (greater than fourfold) in Li–O 2 cell capacity is possible by appropriately selecting the salt anion in the electrolyte solution. Using 7 Li NMR and modeling, we confirm that this improvement is a result of enhanced Li + stability in solution, which, in turn, induces solubility of the intermediate to Li 2 O 2 formation. Using this strategy, the challenging task of identifying an electrolyte solvent that possesses the anticorrelated properties of high intermediate solubility and solvent stability is alleviated, potentially providing a pathway to develop an electrolyte that affords both high capacity and rechargeability. We believe the model and strategy presented here will be generally useful to enhance Coulombic efficiency in many electrochemical systems (e.g., Li–S batteries) where improving intermediate stability in solution could induce desired mechanisms of product formation.
  • Publisher: United States: Proceedings of the National Academy of Sciences
  • Language: English
  • Identifier: ISSN: 0027-8424
    EISSN: 1091-6490
    DOI: 10.1073/pnas.1505728112
  • Source: Open Access: PubMed Central
    Geneva Foundation Free Medical Journals at publisher websites
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