Lithium superoxide encapsulated in a benzoquinone anion matrix

Nava, Matthew; Zhang, Shiyu; Pastore, Katharine S.; Feng, Xiaowen; Lancaster, Kyle M.; Nocera, Daniel G.; Cummins, Christopher C.

doi:10.1073/pnas.2019392118

Title: Lithium superoxide encapsulated in a benzoquinone anion matrix

Journal Article · 12 December 2021 · Proceedings of the National Academy of Sciences of the United States of America

DOI: https://doi.org/10.1073/pnas.2019392118 · OSTI ID:1835470

Nava, Matthew ^[1]; Zhang, Shiyu ^[2]; Pastore, Katharine S. ^[3]; Feng, Xiaowen ^[4];

^[3];

^[4];

^[5]

Massachusetts Institute of Technology (MIT), Cambridge, MA (United States); Harvard University, Cambridge, MA (United States)
Massachusetts Institute of Technology (MIT), Cambridge, MA (United States); The Ohio State University, Columbus, OH (United States)
Cornell University, Ithaca, NY (United States)
Harvard University, Cambridge, MA (United States)
Massachusetts Institute of Technology (MIT), Cambridge, MA (United States)

Lithium peroxide is the crucial storage material in lithium–air batteries. Understanding the redox properties of this salt is paramount toward improving the performance of this class of batteries. Lithium peroxide, upon exposure to p –benzoquinone (p–C₆H₄O₂) vapor, develops a deep blue color. This blue powder can be formally described as [Li₂O₂]_0.3 • [LiO₂]_0.7 • {Li[p–C₆H₄O₂]}_0.7, though spectroscopic characterization indicates a more nuanced structural speciation. Infrared, Raman, electron paramagnetic resonance, diffuse-reflectance ultraviolet-visible and X-ray absorption spectroscopy reveal that the lithium salt of the benzoquinone radical anion forms on the surface of the lithium peroxide, indicating the occurrence of electron and lithium ion transfer in the solid state. As a result, obligate lithium superoxide is formed and encapsulated in a shell of Li[p–C₆H₄O₂] with a core of Li₂O₂. Lithium superoxide has been proposed as a critical intermediate in the charge/discharge cycle of Li–air batteries, but has yet to be isolated, owing to instability. The results reported herein provide a snapshot of lithium peroxide/superoxide chemistry in the solid state with redox mediation.

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Research Organization:: Harvard University, Cambridge, MA (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Biological and Environmental Research (BER)

Grant/Contract Number:: AC02-76SF00515; SC0017619

OSTI ID:: 1835470

Journal Information:: Proceedings of the National Academy of Sciences of the United States of America, Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Issue: 51 Vol. 118; ISSN 0027-8424

Publisher:: National Academy of SciencesCopyright Statement

Country of Publication:: United States

Language:: English

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Title: Lithium superoxide encapsulated in a benzoquinone anion matrix

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