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Wu, Daren; King, Steven T.; Sadique, Nahian; Ma, Lu; Ehrlich, Steven N.; Ghose, Sanjit; Bai, Jianming; Zhong, Hui; Yan, Shan; Bock, David C.; Takeuchi, Esther S.; Marschilok, Amy C.; Housel, Lisa M.; Wang, Lei; Takeuchi, Kenneth J.
Journal of materials chemistry. A, Materials for energy and sustainability, 08/2023, Volume: 11, Issue: 30Journal Article
Aqueous Zn/MnO 2 batteries with mildly acidic electrolytes are promising candidates for low cost, high safety electrochemical energy storage for grid-scale applications. However, the complexity of the chemistry results in conflicting reports of operation principles, making rational improvements challenging. In this work, operando synchrotron X-ray diffraction (XRD) and X-ray absorption spectroscopy (XAS) as well as ex situ Raman spectroscopy, XRD, and XAS characterization were used to probe the mechanism of aqueous Zn/α-MnO 2 batteries with ZnSO 4 electrolyte. A multi-stage Mn dissolution–conversion charge storage mechanism was revealed, which consists of reversible solid-aqueous phase transformation via Mn dissolution–deposition reactions and a solid redox mechanism via Zn-ion insertion. This mechanism is supported by thermodynamic calculations paired with in situ electrolyte pH measurements to provide further mechanistic insights. The findings establish a detailed charge storage mechanism for aqueous Zn/α-MnO 2 batteries with a well resolved reversible layered charge product structure, that can serve as a reference for future studies on advancing the reversibility and stability of aqueous Zn/α-MnO 2 batteries.
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