Rechargeable
zinc-ion batteries (ZIBs) are promising alternatives
for large-scale energy storage systems. However, instability of the
cathode during operation leads to rapid capacity fading and poor stability.
Binders play a crucial role in keeping all components in the cathode
intact during cycling. However, the impact of the binders’
chemical structure on the electrochemical reaction in ZIBs is not
well understood. Herein, the effect of the chemical structure of a
conventional polyvinylidene fluoride (PVDF) and green binders, that
is, sodium carboxymethyl cellulose (CMC) and cellulose acetate (CA),
on the performance, cyclability, and reaction of Zn/α-MnO2 aqueous batteries is investigated. Results show that a cathode
having a PVDF binder yields the highest specific capacity in a full
battery. Besides, the CMC-based ZIB is seen to attain superior cycling
stability through 500 galvanostatic charge–discharge (GCD)
cycles having no irreversible products confirmed by scanning electron
microscopy (SEM) and X-ray diffraction (XRD). It is found that the
Na+ ion in the CMC structure plays a critical role in promoting
prominent battery reactions. The CMC-based ZIB, therefore, is able
to maintain its high ionic diffusivity obtained from the galvanostatic
intermittent titration technique (GITT) during prolonged operation.
Moreover, the interaction between binders and α-MnO2 has been investigated via density-functional theory
(DFT) to affirm the high stability of the ZIB/α-MnO2 with the CMC binder. This work highlights the importance of the
selection of functional groups on the binder not only to enhance stability
but also to control the preferential reactions of batteries. Such
findings are ultimate keys for the development of low-cost, stable,
and eco-friendly energy storage devices.