Journal
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
Volume 20, Issue 14, Pages 9480-9487Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c8cp00761f
Keywords
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Funding
- Department of Defense (DoD) through the National Defense Science & Engineering Graduate Fellowship (NDSEG) Program
- National Science Foundation [NSF-CMMI1363203, CBET-1604483]
- Div Of Civil, Mechanical, & Manufact Inn
- Directorate For Engineering [1363203] Funding Source: National Science Foundation
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Crystal water has been shown to stabilize next-generation energy storage electrodes with structural tunnels to accommodate cation intercalation, but the stabilization mechanism is poorly understood. In this study, we present a simple physical model to explain the energetics of interactions between the electrode crystal lattice, structural water, and electrochemically cycled ions. Our model is applied to understand the effects of crystal water on sodium ion intercalation in a tunnel manganese oxide structure, and we predict that precisely controlling the crystal water concentration can optimize the ion intercalation voltage and capacity and promote stable cycling. The analysis yields a critical structural water concentration by accounting for the interplay between elastic and electrostatic contributions to the free energy. Our predictions are validated with first-principles calculations and electrochemical measurements. The theoretical framework used here can be extended to predict critical concentrations of stabilizing molecules to optimize performance in next-generation battery materials.
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