Abstract

Zinc metal anodes are attracting much attention to enable more economical and sustainable energy storage devices. However, like other metal anodes, dendritic growths and penetrations of porous separators are still challenging to eliminate. Introducing negative surface charges on the pore walls of separators have been exploited to enforce a uniform incoming Zn-ion flux toward more uniform electrodeposition, but penetrations induced by localized high current densities still remain in available systems. In this work, we report, for the first time, a bipolar separator that exploits the distinct electroosmotic effects of the negative and the positive surface charges. The surface charge effects on Zn dendrite growths were first verified in transparent capillary cells via operando video microscopy. By stacking the positively charged separator over the negatively charged separator as our proof-of-concept, the system offers preemptively a uniform Zn-ion flux through the negative layer yet starve-stops local metal growths that already penetrated the negative layer autonomously. Chronopotentiometry experiments with the symmetric cells reveal extended short-circuit time compared to control cells. Galvanostatic cycle-life experiments of full cells with the bipolar separator showed excellent cycle life of 5,000 cycles at the rate of 10 C, without signs of metal penetration.

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