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

Abstract

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.

Authors:
 [1];  [1]; ORCiD logo [1];  [1];  [2];  [1];  [3];  [4];  [1];  [3];  [4];  [5]
  1. Univ. of Wollongong, NSW (Australia)
  2. Univ. of Wollongong, NSW (Australia); Fudan Univ., Shanghai (China)
  3. Univ. of Wollongong, NSW (Australia); Australian Nuclear Science and Technology Organisation (ANSTO), Kirrawee, NSW (Australia)
  4. Argonne National Lab. (ANL), Argonne, IL (United States)
  5. Univ. of Wollongong, NSW (Australia); Zhengzhou Univ. (China)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
Australian Research Council; USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)
OSTI Identifier:
1632117
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Proceedings of the National Academy of Sciences of the United States of America
Additional Journal Information:
Journal Volume: 117; Journal Issue: 6; Journal ID: ISSN 0027-8424
Publisher:
National Academy of Sciences
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; Li-ion battery; hybrid electrode; intercalation

Citation Formats

Hao, Junnan, Yang, Fuhua, Zhang, Shilin, He, Hanna, Xia, Guanglin, Liu, Yajie, Didier, Christophe, Liu, Tongchao, Pang, Wei Kong, Peterson, Vanessa K., Lu, Jun, and Guo, Zaiping. Designing a hybrid electrode toward high energy density with a staged Li+ and PF6- deintercalation/intercalation mechanism. United States: N. p., 2020. Web. doi:10.1073/pnas.1918442117.
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. Designing a hybrid electrode toward high energy density with a staged Li+ and PF6- deintercalation/intercalation mechanism. United States. https://doi.org/10.1073/pnas.1918442117
Hao, Junnan, Yang, Fuhua, Zhang, Shilin, He, Hanna, Xia, Guanglin, Liu, Yajie, Didier, Christophe, Liu, Tongchao, Pang, Wei Kong, Peterson, Vanessa K., Lu, Jun, and Guo, Zaiping. Wed . "Designing a hybrid electrode toward high energy density with a staged Li+ and PF6- deintercalation/intercalation mechanism". United States. https://doi.org/10.1073/pnas.1918442117. https://www.osti.gov/servlets/purl/1632117.
@article{osti_1632117,
title = {Designing a hybrid electrode toward high energy density with a staged Li+ and PF6- deintercalation/intercalation mechanism},
author = {Hao, Junnan and Yang, Fuhua and Zhang, Shilin and He, Hanna and Xia, Guanglin and Liu, Yajie and Didier, Christophe and Liu, Tongchao and Pang, Wei Kong and Peterson, Vanessa K. and Lu, Jun and Guo, Zaiping},
abstractNote = {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.},
doi = {10.1073/pnas.1918442117},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = 6,
volume = 117,
place = {United States},
year = {Wed Jan 29 00:00:00 EST 2020},
month = {Wed Jan 29 00:00:00 EST 2020}
}

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