Abstract
<jats:p>Replacing fluorinated binders with sustainable alternatives is a key challenge for advancing environmentally compatible battery technologies, particularly in aqueous systems, where sustainability in all components is generally expected. Here, a free-standing α-MnO2 composite cathode based on a hydrophilic bacterial cellulose (BC) scaffold is explored as a fluorine-free alternative to conventional PVdF and slurry-based electrodes for mildly acidic Zn-MnO2 batteries. The composite integrates BC with conductive carbon (Super P), whose dispersion is improved by chemical oxidation, enabling the formation of a homogeneous and percolating conductive network above ~40 wt.% carbon content. Electrochemical evaluation in a ZnSO4/MnSO4 electrolyte showed that BC-based electrodes sustain reversible MnO2 electrochemistry with performance comparable to that of PVdF-based counterparts, despite markedly different electrode architectures and compositions. The results further indicate that neither the binder chemistry nor the scaffold composition fundamentally alters the dissolution-mediated Mn redox mechanism, whereas the capacity retention and rate capability are primarily governed by the transport homogeneity and active material loading. The BC scaffold provides a hydrophilic, porous microenvironment that supports electrolyte accessibility and maintains electrochemical functionality in highly porous, free-standing electrodes. Although no intrinsic performance advantage over PVdF has been established, this study demonstrates that fluorinated binders are not required to sustain MnO2 electrochemistry, opening a pathway toward bio-derived, water-processable, and structurally robust cathodes for sustainable aqueous Zn batteries.</jats:p>