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. 2020 Jul 16;10(1):11813.
doi: 10.1038/s41598-020-68865-8.

Facile formulation and fabrication of the cathode using a self-lithiated carbon for all-solid-state batteries

N Delaporte  1 , A Darwiche  2 , M Léonard  2 , G Lajoie  2 , H Demers  2 , D Clément  2 , R Veillette  2 , L Rodrigue  2 , M L Trudeau  2 , C Kim  2 , K Zaghib  3
Affiliations

Facile formulation and fabrication of the cathode using a self-lithiated carbon for all-solid-state batteries

N Delaporte et al. Sci Rep. .

Abstract

We propose a innovative concept to boost the electrochemical performance of cathode composite electrodes using surface-modified carbons with hydrophilic moieties to increase their dispersion in a Lithium Nickel Manganese Cobalt Oxide (NMC) cathode and in-situ generate Li-rich carbon surfaces. Using a rapid aqueous process, the hydrophilic carbon is effectively dispersed in NMC particles followed by the conversion of its acid surface groups (e.g. -COOH), which interact with the NMC particles due to their basicity, into grafted Li salt (-COO-Li+). The solid-state batteries prepared using the cathode composites with surface-modified carbon exhibit better electrochemical performance. Such modified carbons led to a better electronic conduction path as well as facilitating Li+ ions transfer at the carbon/NMC interface due to the presence of lithiated carboxylate groups on their surface.

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Conflict of interest statement

The authors declare no competing interests.

Figures

Figure 1
Figure 1
Schematic illustration of the reaction procedures: the first step (in orange) is to graft hydrophilic molecules (different groups can be used) on carbon surface (e.g. CNT, Ketjen Black) and the second step (in red) is to in-situ generate Li salts on carbon in the presence of NMC particles.
Figure 2
Figure 2
(a,b) Photographs of a suspension of CNT–COOH in deionized water, and (c) Thermogravimetric curves for pristine CNT (—) and CNT-COOH (red dashed line) carbons.
Figure 3
Figure 3
Micro-Raman spectra for NMC (—) and NMC@CNT–COOH (red dashed line).
Figure 4
Figure 4
(a,d) SEM and (b,e) STEM-EELS images of NMC@CNT–COOH powder (representative spectrum images), and (c,f) corresponding STEM-EELS spectra.
Figure 5
Figure 5
SEM images of NMC@VGCF–COOH powder.
Figure 6
Figure 6
Photographs of NMC electrodes synthesized with (a) a mixture of unmodified NMC and Ketjen, and (b) a mixture of unmodified Ketjen and NMC@VGCF–COOH composite.
Figure 7
Figure 7
(a) SEM image and (b) XRD pattern of EG powder, (c) thermogravimetric curves of graphite and EG powders, (d) SEM image of NMC@EG powder.
Figure 8
Figure 8
(a,d) Optical and (b,c,e,f) 3D confocal microscopy images of NMC electrodes made with: (a–c) pristine NMC and unmodified Ketjen Black carbon and (d–f) the NMC@VGCF–COOH composite with the modified grafted-Ketjen-acid carbon. Magnifications of × 20 (a,b,d,e) and × 50 (c,f) were used. The arithmetic mean roughness (Ra) is given for each electrode.
Figure 9
Figure 9
(a) Galvanostatic charge/discharge profiles at a cycling rate of C/24 and (b) rate capability of three NMC electrodes synthesized with NMC and Ketjen Black (—, filled square); NMC@CNT-COOH composite and Ketjen Black (red dashed line, red filled circle); and NMC@EG composite and Ketjen Black (blue dotted line, blue filled triangle).
See this image and copyright information in PMC

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