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Water-Solid Interface Engineering Stabilizes K-Birnessite Cathode
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DOI：10.1002/adfm.202108267.png)
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Abstract
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Crystal water mediated ion hydration and transport is a fundamental physicochemical process in a wide range of applications and natural processes, such as crystal water containing battery materials. In this context, K-Birnessite with interlaminar H2O (K0.21MnO2.0.31H(2)O) is reported for nonaqueous potassium-ion storage with enhanced capacity and rate performance. It is clarified that the water-solid interface plays an important role in building and stabilizing the K-Birnessite layered structure and facilitating the K+ diffusion for the K-ion battery system. In addition to the enlarged ionic channel dimensions and effective shielding of the electrostatic interaction with K+, the concerted diffusion of K+/H2O with the rotation of H2O molecules is further revealed to account for the quite low activation energies by first-principles simulations. Moreover, the interlayer H2O exerts on the electronic structures, and thus on the electrochemical voltage to result in the competition between the split of crystal field ( backward difference (JT)) and the electronic superexchange interaction (O-w-K-O) in the K-Birnessite structure. The results provide new insights into hydrated ion kinetics and open an exciting direction for battery material design.
Keywords:
concerted diffusion
potassium-ion batteries
structure stabilization
water-solid interface
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