Using Atomic Layer Deposition to Hinder Solvent Decomposition in Lithium Ion Batteries: First-Principles Modeling and Experimental Studies
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- Using Atomic Layer Deposition to Hinder Solvent Decomposition in Lithium Ion Batteries: First-Principles Modeling and Experimental Studies
- Leung, Kevin; Qi, Yue; Zavadil, Kevin R.; Jung, Yoon Seok; Dillon, Anne C.; Cavanagh, Andrew S.; Lee, Se-Hee; George, Steven M.
- Ab initio molecular dynamics simulation; Atomic layer deposition coatings; Battery electrode; Battery operation; Density functional theory calculations; Electrode interface; Electrolyte decomposition; Electron transfer; Ethylene carbonate; Experimental studies; First-principles calculation; First-principles modeling; Harmonic approximation; Li metal; Lithium ions; Lithium-ion battery; Main component; Microgravimetric measurements; Model platform; Molecular reorganization energy; Non-adiabatic; Oxide coating; Passivating layer; Picoseconds; Solvent decompositions; Theoretical prediction; Two-regime
- Issue Date
- AMER CHEMICAL SOC
- JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, v.133, no.37, pp.14741 - 14754
- Passivating lithium ion (Li) battery electrode surfaces to prevent electrolyte decomposition is critical for battery operations. Recent work on conformal atomic layer deposition (ALD) coating of anodes and cathodes has shown significant technological promise. ALD further provides well-characterized model platforms for understanding electrolyte decomposition initiated by electron tunneling through a passivating layer. First-principles calculations reveal two regimes of electron transfer to adsorbed ethylene carbonate molecules (EC, a main component of commercial electrolyte), depending on whether the electrode is alumina coated. On bare Li metal electrode surfaces, EC accepts electrons and decomposes within picoseconds. In contrast, constrained density functional theory calculations in an ultrahigh vacuum setting show that, with the oxide coating, e(-) tunneling to the adsorbed EC falls within the nonadiabatic regime. Here the molecular reorganization energy, computed in the harmonic approximation, plays a key role in slowing down electron transfer. Ab initio molecular dynamics simulations conducted at liquid EC electrode interfaces are consistent with the view that reactions and electron transfer occur right at the interface. Microgravirnetric measurements demonstrate that the ALD coating decreases electrolyte decomposition and corroborates the theoretical predictions.
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