Zinc-ion
batteries show great potential as the next-generation
power source due to their nontoxic, low-cost, and safe properties.
However, issues with zinc anodes, such as dendrite growth and parasitic
hydrogen evolution reactions (HERs), must be addressed to commercialize
them. Solutions, such as quasi-solid-state electrolytes made from
synthetic polymer hydrogels, have been proposed to improve battery
flexibility and energy density. However, most polymers used are nonbiodegradable,
posing a challenge to sustainability. In this study, hydrogels made
from biodegradable poly(vinyl alcohol) and protein nanofibrils from
pea protein, a renewable plant-based source, are used as an electrolyte
in aqueous zinc-ion batteries. Results show that the flexible and
biodegradable hydrogel can enhance the zinc anode stability and effectively
restrict HER. This phenomenon is because of the hydrogen-bond network
between nanofibril functional groups and water molecules. In addition,
the interaction between functional groups on nanofibrils and Zn2+ constructs ion channels for the even migration of Zn2+, avoiding dendrite growth. The Zn||Zn symmetric cell using
the hydrogel electrolyte exhibits a long lifespan of over 3000 h and
improved capacity retention in the Zn||AC-I2 hybrid ion
batteries by suppressing cathode material dissolution. This study
suggests the potential of biodegradable hydrogels as a sustainable
and effective solution for biodegradable soft powering sources.