An ultra-thick solvent-free electrode based on non-conservative pulsed shear field mixing

Abstract

Despite being extensively expected as an eco-friendly and cost-effective electrode manufacturing technique in batteries, the solvent-free (SF) technique still suffers from poor mechanical stability and inhomogeneous mixing, especially for ultra-thick electrode. Herein, we pivot from unusual shear force field regulation, proposing a pulsed mixing (PM) strategy to redefine energy release criterion. Mechanical evaluation and X-ray Nano-CT tomography demonstrate that PM strategy can construct uniform and robust SF ultra-thick electrode with 3D charge transfer highway and deeply interconnected charge carrier permeable network by optimizing dynamic connections among electroactive materials. As a proof of concept, an unprecedented ultra-high mass loading of 121 mg cm⁻² can be achieved in a SF LiMn₂O₄ (LMO) electrode with a capacity of 11.6 mA h cm⁻², and appealing cyclability over 30 times. Furthermore, the thick SF LMO (58 mg cm⁻²) displays a high-capacity retention of 93 % over 100 cycles at 0.1 C. Even the assembled SF LMO||Si/C full cell also exhibits good cycle stability with a capacity retention of 87.5 % after 100 cycles. The finding signifies a paradigm innovate and introduces transformative opportunities for the design of high-performance and green batteries.