Abstract

Higher energy density Li-ion batteries that can enable longer driving ranges are currently subject to intensive research interest. Increasing the thickness of electrodes and reducing the proportion of inactive components per cell is one way to achieve this. In thick electrodes, a higher electronic and ionic overpotential and mechanical failure (cracking, delamination etc.) induced by binder migration during the drying process leads to sluggish (dis)charge performance or even cell failure respectively. Here we report non-solvent induced phase inversion as a scalable, effective method to arrive at thick NMC811 electrodes.By tuning the non-solvent properties and other processing conditions to be compatible with Ni-rich electrodes, it was possible to obtain NMC811 electrodes with mass loadings up to 11 mAh/cm2 (single sided) which outperform their conventional processed counterparts in Li/NMC half cells. This improvement could be attributed to the altered carbon-binder structure, which improves the pore connectivity and lowers the electrode tortuosity factor. The rapid solvent removal also reduces the long-range binder migration during drying. With imaging and porosimetry techniques we show the structural change which leads to the observed improved electrochemical performance. The method also shows good compatibility with double sided slot-die electrode coating procedure, making this a technique with potentially high industrial feasibility towards making thicker NMC811 and other electrodes.

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