High-energy lithium batteries require electrode architectures that enable high areal capacity, high active material content, and stable high-voltage operation—requirements that conventional slurry-based electrodes struggle to meet due to inefficient electron percolation, parasitic reactions, and limited processing-architecture predictability. Here we design and validate a dry-processed electrode architecture that leverages molecular-level coupling between fibrous carbon and binder to promote efficient electronic conduction while suppressing high-voltage interfacial degradation. This architecture achieves areal loadings >5 mAh cm − 2 with >99 wt% active material and supports stable operation up to 4.70 V without compromising rate capability. The 4.55 V NMC811||graphite pouch cells retain 78% capacity after 1,000 cycles at C/3-rate, with average Coulombic efficiency exceeding 99.9%. These results are achieved without material-level modifications or specialized electrolyte additives, highlighting the potential of electrode engineering alone to unlock the intrinsic performance of active materials even under demanding conditions of high areal loading and maximum active material content.
Zhang et al. (Wed,) studied this question.