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Title: Thick Binder-Free Electrodes for Li-Ion Battery Fabricated Using Templating Approach and Spark Plasma Sintering Reveals High Areal Capacity

Abstract

The templating approach is a powerful method for preparing porous electrodes with interconnected well-controlled pore sizes and morphologies. The optimization of the pore architecture design facilitates electrolyte penetration and provides a rapid diffusion path for lithium ions, which becomes even more crucial for thick porous electrodes. In this work, NaCl microsize particles are used as a templating agent for the fabrication of 1 mm thick porous LiFePO4 and Li4Ti5O12 composite electrodes using spark plasma sintering technique. These sintered binder-free electrodes are self-supported and present a large porosity (40%) with relatively uniform pores. The electrochemical performances of half and full batteries reveal a remarkable specific areal capacity (20 mA h cm-2), which is 4 times higher than those of 100 µm thick electrodes present in conventional tape-casted Li–ion batteries (5 mA h cm-2). The 3D morphological study is carried out using full field transmission X-ray microscopy in microcomputed tomography mode to obtain tortuosity values and pore size distributions leading to a strong correlation with their electrochemical properties. These results also demonstrate that the coupling between the salt templating method and the spark plasma sintering technique turns out to be a promising way to fabricate thick electrodes with high energy density.

Authors:
 [1];  [1];  [2]; ORCiD logo [1]; ORCiD logo [1]
  1. Univ. of Picardie Jules Verne, Amiens (France). Lab. of Reactivity and Solid State Chemistry (LRCS); French Network on Electrochemical Storage of Energy (RS2E), Amiens (France)
  2. Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Publication Date:
Research Org.:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division; Ministry of Higher Education, Research and Innovation (MESRI) (France)
OSTI Identifier:
1476310
Alternate Identifier(s):
OSTI ID: 1418698
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Energy Materials
Additional Journal Information:
Journal Volume: 8; Journal Issue: 15; Journal ID: ISSN 1614-6832
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; LiFePO4/Li4Ti5O12 Li-ion batteries; SPS technique; TXM microcomputed tomography; templating approach; thick and binder-free electrodes

Citation Formats

Elango, Rakesh, Demortière, Arnaud, De Andrade, Vincent, Morcrette, Mathieu, and Seznec, Vincent. Thick Binder-Free Electrodes for Li-Ion Battery Fabricated Using Templating Approach and Spark Plasma Sintering Reveals High Areal Capacity. United States: N. p., 2018. Web. doi:10.1002/aenm.201703031.
Elango, Rakesh, Demortière, Arnaud, De Andrade, Vincent, Morcrette, Mathieu, & Seznec, Vincent. Thick Binder-Free Electrodes for Li-Ion Battery Fabricated Using Templating Approach and Spark Plasma Sintering Reveals High Areal Capacity. United States. https://doi.org/10.1002/aenm.201703031
Elango, Rakesh, Demortière, Arnaud, De Andrade, Vincent, Morcrette, Mathieu, and Seznec, Vincent. Tue . "Thick Binder-Free Electrodes for Li-Ion Battery Fabricated Using Templating Approach and Spark Plasma Sintering Reveals High Areal Capacity". United States. https://doi.org/10.1002/aenm.201703031. https://www.osti.gov/servlets/purl/1476310.
@article{osti_1476310,
title = {Thick Binder-Free Electrodes for Li-Ion Battery Fabricated Using Templating Approach and Spark Plasma Sintering Reveals High Areal Capacity},
author = {Elango, Rakesh and Demortière, Arnaud and De Andrade, Vincent and Morcrette, Mathieu and Seznec, Vincent},
abstractNote = {The templating approach is a powerful method for preparing porous electrodes with interconnected well-controlled pore sizes and morphologies. The optimization of the pore architecture design facilitates electrolyte penetration and provides a rapid diffusion path for lithium ions, which becomes even more crucial for thick porous electrodes. In this work, NaCl microsize particles are used as a templating agent for the fabrication of 1 mm thick porous LiFePO4 and Li4Ti5O12 composite electrodes using spark plasma sintering technique. These sintered binder-free electrodes are self-supported and present a large porosity (40%) with relatively uniform pores. The electrochemical performances of half and full batteries reveal a remarkable specific areal capacity (20 mA h cm-2), which is 4 times higher than those of 100 µm thick electrodes present in conventional tape-casted Li–ion batteries (5 mA h cm-2). The 3D morphological study is carried out using full field transmission X-ray microscopy in microcomputed tomography mode to obtain tortuosity values and pore size distributions leading to a strong correlation with their electrochemical properties. These results also demonstrate that the coupling between the salt templating method and the spark plasma sintering technique turns out to be a promising way to fabricate thick electrodes with high energy density.},
doi = {10.1002/aenm.201703031},
journal = {Advanced Energy Materials},
number = 15,
volume = 8,
place = {United States},
year = {Tue Jan 30 00:00:00 EST 2018},
month = {Tue Jan 30 00:00:00 EST 2018}
}

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Figures / Tables:

Figure 1 Figure 1: – Scheme showing the three steps fabrication of thick porous electrodes using NaCl particles as templating agents. SEM images of (a) Carbon coated LFP grains of 200 nm particle size, (b) As-prepared NaCl crystals showing average particle size about 10 μm, (c) 3D view and (d) cross sectionmore » of the 1mm thick LFP-NaCl-C pellet showing the NaCl templates (bright) embedded in the total volume of the electrodes obtained after SPS treatment, (e) and (f) Low and high magnification of the fractured surface of vacuum dried LFP-C porous electrode illustrating the 1mm thickness and created porosity after dissolution of NaCl in water, (g) Digital photo of LFP-C porous electrode showing 10 mm diameter, (h) and (i) shows the SEM images of top surface view of the LFP-C electrode with the uniformly distributed pores throughout the bulk electrode and square shape of the crystal can be clearly seen .« less

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