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Oxygen Reduction Reactions in Ionic Liquids and the Formulation of a General ORR Mechanism for Li–Air Batteries
Abstract
Oxygen reduction and evolution reactions (ORRs and OERs) have been studied in ionic liquids containing singly charged cations having a range of ionic radii, or charge densities. Specifically, ORR and OER mechanisms were studied using cyclic and rotating disk electrode voltammetry in the neat ionic liquids (ILs), 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide (EMITFSI) and 1-methyl-1-butyl-pyrrolidinium bis(triflouromethanesulfonyl)imide (PYR 14 TFSI), and in their solutions containing LiTFSI, NaPF 6, KPF 6, and tetrabutylammonium hexafluorophosphate (TBAPF 6 ). A strong correlation was found between the ORR products and the ionic charge density, including those of the ionic liquids. The observed trend is explained in terms of the Lewis acidity of the cation present in the electrolyte using an acidity scale created from 13 C NMR chemical shifts and spin–lattice relaxation ( T 1 ) times of 13 C═O in solutions of these charged ions in propylene carbonate (PC). The ionic liquids lie in a continuum of a cascading Lewis acidity scale with respect to the charge density of alkali metal, IL, and TBA cations with the result that the ORR products in ionic liquids and in organic electrolytes containing any conducting cations can be predicted on the basis of a general theory based on the hard soft acid base (HSAB) concept.
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Cites
Pearson, R. G. (1963) · Journal of the American Chemical Society · doi:10.1021/ja00905a001 · Cited by 10,475
Cited by
Ionic liquids and derived materials for lithium and sodium batteries
Yang, Q., Zhang, Z., Sun, X.-G., Hu, Y.-S., Xing, H., & Dai, S. (2018) · Chemical Society Reviews · doi:10.1039/c7cs00464h · Cited by 601
Critical Challenges in Rechargeable Aprotic Li–O2 Batteries
Feng, N., He, P., & Zhou, H. (2016) · Advanced Energy Materials · doi:10.1002/aenm.201502303 · Cited by 423
Metadata
- Authors
- Allen, C. J., Hwang, J., Kautz, R., Mukerjee, S., Plichta, E. J., Hendrickson, M. A., & Abraham, K. M.
- Venue
- The Journal of Physical Chemistry C
- Publisher
- American Chemical Society (ACS)
- Published
- 2012-09-19
- Volume
- 116
- Issue
- 39
- Pages
- 20755-20764
- ISSN
- 1932-7447 (ISSN-L)
- 1932-7455
- OpenAlex
- W2328126563
- Cited by
- 209
- References
- 1
- FWCI
- 9.97
- Type
- journal article
- Language
- en
- Open access
- closed
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