Layered manganese oxide cathode boosting high-capacity and long-term cyclability in aqueous Zinc-Ion batteries
Zhanadilov O. Kim H.J. Konarov A. Jeong J. Park J.-H. Chung K.Y. Bakenov Z. Yashiro H. Myung S.-T.
March 2024Elsevier B.V.
Energy Storage Materials
2024#67
Development of aqueous zinc-ion batteries (ZIBs) promises low-cost and safe energy storage systems. From the existing natural resources manganese-based compounds are desirable cathodes materials for aqueous ZIBs. We present a layered birnessite-type δ–K0.32MnO2·0·15H2O (MnO2) as a candidate cathode material. By adding reduced graphene oxide (rGO) to enhance electron transport, we present the electrode performance in Al pouch cells (3.2 × 3.4 cm2) achieving a high-capacity of 373 mAh g1− at 0.1C which retained over 99 % for 120 cycles. Additionally, performance is highlighted at 5C and 10C, retaining 89 % for 500 cycles and 35 % for 2,000 cycles, respectively. The main redox process involves the Mn4+/Mn3+ redox couple, accompanied by a conversion reaction through the de/protonation process. Operando XRD, operando pH measurement, and time-of-flight secondary-ion mass spectroscopy prove that the de/protonation process of solvated zinc ions [Zn(H2O)6]2+, followed by protonation of the active material leads to the formation of KxMnOOH(1- x) during discharge and vice versa during charging. The conversion reaction resulting from the de/protonation processes leads to the amorphization of the active material after the prolonged cycles. Operando pH analysis shows the influence of the pH on de/protonation of [Zn(H2O)6]2+ complex, thus implicating it as a determinant of the capacity.
Activation , Cathode , Layered manganese oxide , Protonation , Zinc aqueous battery
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Hybrid Materials Research Center, Department of Nanotechnology and Advanced Materials Engineering & Sejong Battery Institute, Sejong University, Seoul, 05006, South Korea
Department of Chemical and Materials Engineering, School of Engineering and Digital Sciences, Nazarbayev University, Kabanbay Batyr Ave. 53, Astana, 010000, Kazakhstan
Center for Energy Storage Research, Korea Institute of Science and Technology, Seoul, 02792, South Korea
Argonne National Laboratory, 700 S Cass Ave, Lemont, 60439, IL, United States
Department of Chemistry and Bioengineering, Iwate University, Ueda 4-3-5, Iwate, Morioka, 020-8551, Japan
Hybrid Materials Research Center
Department of Chemical and Materials Engineering
Center for Energy Storage Research
Argonne National Laboratory
Department of Chemistry and Bioengineering
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