Hetero‐Nanonet Rechargeable Paper Batteries: Toward Ultrahigh Energy Density and Origami Foldability

Forthcoming smart energy era is in strong pursuit of full‐fledged rechargeable power sources with reliable electrochemical performances and shape versatility. Here, as a naturally abundant/environmentally friendly cellulose‐mediated cell architecture strategy to address this challenging issue, a new class of hetero‐nanonet (HN) paper batteries based on 1D building blocks of cellulose nanofibrils (CNFs)/multiwall carbon nanotubes (MWNTs) is demonstrated. The HN paper batteries consist of CNF/MWNT‐intermingled heteronets embracing electrode active powders (CM electrodes) and microporous CNF separator membranes. The CNF/MWNT heteronet‐mediated material/structural uniqueness enables the construction of 3D bicontinuous electron/ion transport pathways in the CM electrodes, thus facilitating electrochemical reaction kinetics. Furthermore, the metallic current collectors‐free, CNF/MWNT heteronet architecture allows multiple stacking of CM electrodes in series, eventually leading to user‐tailored, ultrathick (i.e., high‐mass loading) electrodes far beyond those accessible with conventional battery technologies. Notably, the HN battery (multistacked LiNi_0.5Mn_1.5O₄ (cathode)/multistacked graphite (anode)) provides exceptionally high‐energy density (=226 Wh kg^?1 per cell at 400 W kg^?1 per cell), which surpasses the target value (=200 Wh kg^?1 at 400 W kg^?1) of long‐range (=300 miles) electric vehicle batteries. In addition, the heteronet‐enabled mechanical compliance of CM electrodes, in combination with readily deformable CNF separators, allows the fabrication of paper crane batteries via origami folding technique.