Lee, Boeun Choi, Jihwan Lee, Minseok Han, Seulki Jeong, Minji Yim, Taeeun Oh, Si Hyoung 2024-01-19T14:31:12Z 2024-01-19T14:31:12Z 2021-10-21 2021-06-28 2050-7488 https://pubs.kist.re.kr/handle/201004/116840 Rechargeable batteries based on MnO2/Zn aqueous chemistry have emerged as a viable alternative to Li-ion batteries (LIB), owing to their low material cost, high safety, sustainable redox chemistry, and remarkable electrochemical performance with an energy density comparable to LIBs. However, the reaction mechanism, particularly the detailed electrochemical process that leads to MnO2 deposition during the charge process, remains elusive to date despite a decade of intensive research. In this study, we utilized various structural analysis methods, including in situ Raman spectroscopy, on simulated discharged electrodes to demonstrate that the charging reaction consists of two reaction steps. These steps involve the precipitation of highly defective phyllomanganates with heavy Zn sorption in the interlayer, followed by the coincidental extraction of zinc and incorporation of manganese into vacancies in MnO6 sheets, which lead to the production of phyllomanganates with much reduced Zn content. This study sheds light on the reaction mechanism of MnO2/Zn batteries and opens new opportunities for improving their performance to commercial levels. English ROYAL SOC CHEMISTRY X-RAY-ABSORPTION STORAGE MECHANISM CHEMISTRY PERFORMANCE BIRNESSITE CATHODE MNO2 ALPHA-MNO2 DEPOSITION Unraveling the critical role of Zn-phyllomanganates in zinc ion batteries Article 10.1039/d1ta03536c 1 JOURNAL OF MATERIALS CHEMISTRY A, v.9, no.24, pp.13950 - 13957 JOURNAL OF MATERIALS CHEMISTRY A 9 24 13950 13957 scie scopus 000658795100001 2-s2.0-85108654518 Chemistry, Physical Energy & Fuels Materials Science, Multidisciplinary Chemistry Energy & Fuels Materials Science Article X-RAY-ABSORPTION STORAGE MECHANISM CHEMISTRY PERFORMANCE BIRNESSITE CATHODE MNO2 ALPHA-MNO2 DEPOSITION phyllomanganate zinc manganese oxide Raman spectroscopy