Designing a hybrid electrode toward high energy density with a staged Li+ and PF6- deintercalation/intercalation mechanism

Hao, Junnan; Yang, Fuhua; Zhang, Shilin; He, Hanna; Xia, Guanglin; Liu, Yajie; Didier, Christophe; Liu, Tongchao; Pang, Wei Kong; Peterson, Vanessa K.; Lu, Jun; Guo, Zaiping

doi:10.1073/pnas.1918442117

Designing a hybrid electrode toward high energy density with a staged Li⁺ and PF₆^- deintercalation/intercalation mechanism

Journal Article · Wed Jan 29 00:00:00 EST 2020 · Proceedings of the National Academy of Sciences of the United States of America

DOI:https://doi.org/10.1073/pnas.1918442117· OSTI ID:1632117

Hao, Junnan ^[1]; Yang, Fuhua ^[1]; ^[1]; He, Hanna ^[1]; Xia, Guanglin ^[2]; Liu, Yajie ^[1]; Didier, Christophe ^[3]; Liu, Tongchao ^[4]; Pang, Wei Kong ^[1]; Peterson, Vanessa K. ^[3]; Lu, Jun ^[4]; Guo, Zaiping ^[5]

Univ. of Wollongong, NSW (Australia)
Univ. of Wollongong, NSW (Australia); Fudan Univ., Shanghai (China)
Univ. of Wollongong, NSW (Australia); Australian Nuclear Science and Technology Organisation (ANSTO), Kirrawee, NSW (Australia)
Argonne National Lab. (ANL), Argonne, IL (United States)
Univ. of Wollongong, NSW (Australia); Zhengzhou Univ. (China)

Existing lithium-ion battery technology is struggling to meet our increasing requirements for high energy density, long lifetime, and low-cost energy storage. Here, a hybrid electrode design is developed by a straightforward reengineering of commercial electrode materials, which has revolutionized the “rocking chair” mechanism by unlocking the role of anions in the electrolyte. Our proof-of-concept hybrid LiFePO₄(LFP)/graphite electrode works with a staged deintercalation/intercalation mechanism of Li⁺cations and PF₆^-anions in a broadened voltage range, which was thoroughly studied byex situX-ray diffraction,ex situRaman spectroscopy, andoperandoneutron powder diffraction. Introducing graphite into the hybrid electrode accelerates its conductivity, facilitating the rapid extraction/insertion of Li⁺from/into the LFP phase in 2.5 to 4.0 V. This charge/discharge process, in turn, triggers the in situ formation of the cathode/electrolyte interphase (CEI) layer, reinforcing the structural integrity of the whole electrode at high voltage. Consequently, this hybrid LFP/graphite-20% electrode displays a high capacity and long-term cycling stability over 3,500 cycles at 10 C, superior to LFP and graphite cathodes. Importantly, the broadened voltage range and high capacity of the hybrid electrode enhance its energy density, which is leveraged further in a full-cell configuration.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: Australian Research Council; USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1632117

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: 6 Vol. 117; ISSN 0027-8424

Publisher:: National Academy of SciencesCopyright Statement

Country of Publication:: United States

Language:: English

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