Journal
NATURE ENERGY
Volume 4, Issue 7, Pages 560-567Publisher
NATURE PORTFOLIO
DOI: 10.1038/s41560-019-0398-y
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Funding
- SFI [SFI/12/RC/2278]
- Science Foundation Ireland (SFI) [11/PI/1087]
- European Research Council (AdvGr FUTUREPRINT)
- Graphene Flagship [785219]
- Science Foundation Ireland (PIYRA)
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Increasing the energy storage capability of lithium-ion batteries necessitates maximization of their areal capacity. This requires thick electrodes performing at near-theoretical specific capacity. However, achievable electrode thicknesses are restricted by mechanical instabilities, with high-thickness performance limited by the attainable electrode conductivity. Here we show that forming a segregated network composite of carbon nanotubes with a range of lithium storage materials (for example, silicon, graphite and metal oxide particles) suppresses mechanical instabilities by toughening the composite, allowing the fabrication of high-performance electrodes with thicknesses of up to 800 mu m. Such composite electrodes display conductivities up to 1 x 10(4) S m(-1) and low charge-transfer resistances, allowing fast charge-delivery and enabling near-theoretical specific capacities, even for thick electrodes. The combination of high thickness and specific capacity leads to areal capacities of up to 45 and 30 mAh cm(-2) for anodes and cathodes, respectively. Combining optimized composite anodes and cathodes yields full cells with state-of-the-art areal capacities (29 mAh cm(-2)) and specific/volumetric energies (480 Wh kg(-1) and 1,600 Wh l(-1)).
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