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Nano Lett. 2015 Jun 10;15(6):4071-9. doi: 10.1021/acs.nanolett.5b01109. Epub 2015 May 22.

The High Performance of Crystal Water Containing Manganese Birnessite Cathodes for Magnesium Batteries.

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†Graduate School of Energy, Environment, Water, and Sustainability (EEWS) and KAIST Institute NanoCentury, Korea Advanced Institute of Science and Technology (KAIST), 291 Daehak-ro, Yuseong-gu, Daejeon 305-701, Republic of Korea.
‡Department of Electronic Chemistry, Tokyo Institute of Technology, 4259 G1-1 Nagatsuta, Midori-ku, Yokohama 226-8502, Japan.
§Department of Chemistry and Bar-Ilan Institute of Nanotechnology and Advanced Materials, Bar-Ilan University, Ramat-Gan, Israel.
∥Energy Lab., Samsung Advanced Institute of Technology (SAIT), Samsung Electronics Co., Ltd, 130 Samsung-ro, Yeongtong-gu, Suwon-si, Gyeonggi-do 443-803, Republic of Korea.
⊥Advanced Batteries Research Center, Korea Electronics Technology Institute (KETI), #25, Saenari-ro, Bundang-gu, Seongnam-si, Gyeonggi-do 463-816, Republic of Korea.


Rechargeable magnesium batteries have lately received great attention for large-scale energy storage systems due to their high volumetric capacities, low materials cost, and safe characteristic. However, the bivalency of Mg(2+) ions has made it challenging to find cathode materials operating at high voltages with decent (de)intercalation kinetics. In an effort to overcome this challenge, we adopt an unconventional approach of engaging crystal water in the layered structure of Birnessite MnO2 because the crystal water can effectively screen electrostatic interactions between Mg(2+) ions and the host anions. The crucial role of the crystal water was revealed by directly visualizing its presence and dynamic rearrangement using scanning transmission electron microscopy (STEM). Moreover, the importance of lowering desolvation energy penalty at the cathode-electrolyte interface was elucidated by working with water containing nonaqueous electrolytes. In aqueous electrolytes, the decreased interfacial energy penalty by hydration of Mg(2+) allows Birnessite MnO2 to achieve a large reversible capacity (231.1 mAh g(-1)) at high operating voltage (2.8 V vs Mg/Mg(2+)) with excellent cycle life (62.5% retention after 10000 cycles), unveiling the importance of effective charge shielding in the host and facile Mg(2+) ions transfer through the cathode's interface.


Birnessite; Magnesium batteries; aqueous batteries; charge screening; crystal water

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