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Journal ArticleDOI

On the Mechanism of Nonaqueous Li–O2 Electrochemistry on C and Its Kinetic Overpotentials: Some Implications for Li–Air Batteries

TLDR
In this paper, the authors combine quantitative differential electrochemical mass spectrometry and cyclic voltammetry to probe possible mechanisms and the kinetic overpotentials responsible for discharge and charge in a Li-O2 battery, using C as the cathode and an electrolyte based on dimethoxyethane as the solvent.
Abstract
Quantitative differential electrochemical mass spectrometry and cyclic voltammetry have been combined to probe possible mechanisms and the kinetic overpotentials, responsible for discharge and charge in a Li–O2 battery, using C as the cathode and an electrolyte based on dimethoxyethane as the solvent. Previous spectroscopy experiments (X-ray diffraction, μRaman, IR, XPS) have shown that Li2O2 is the principle product formed during Li–O2 discharge using this electrolyte/cathode combination. At all discharge potentials and charge potentials 4.0 V, the electrochemistry requires significantly more than 2e–/O2, and we take this as evidence for electrolyte decomposition. We find that sequential...

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Citations
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Journal ArticleDOI

Origin of Outstanding Stability in the Lithium Solid Electrolyte Materials: Insights from Thermodynamic Analyses Based on First-Principles Calculations

TL;DR: The results suggest that the outstanding stability of the solid electrolyte materials is not thermodynamically intrinsic but is originated from kinetic stabilizations, and general principles for developing solid electrolytes materials with enhanced stability and for engineering interfaces in all-solid-state Li-ion batteries are provided.
Journal ArticleDOI

The role of LiO2 solubility in O2 reduction in aprotic solvents and its consequences for Li-O2 batteries.

TL;DR: The unified mechanism shows that low-donor-number solvents are likely to lead to premature cell death, and that the future direction of research for lithium-oxygen batteries should focus on the search for new, stable, high-donour-number electrolytes, because they can support higher capacities and can better sustain discharge.
Journal ArticleDOI

Nonaqueous Li-air batteries: a status report.

TL;DR: This paper presents a meta-analyses of the chiral stationary phase replacement of Na6(CO3)(SO4) with Na2SO4 at the Lawrence Berkeley National Laboratory for high-performance liquid chromatography of Na2CO3 with the objective of determining theinity of the CHBMs.
Journal ArticleDOI

Solvating additives drive solution-mediated electrochemistry and enhance toroid growth in non-aqueous Li–O2 batteries

TL;DR: A general formalism describing an additive's tendency to trigger the solution process is presented, providing a rational design route for electrolytes that afford larger lithium-oxygen battery capacities.
Journal ArticleDOI

First principles study on electrochemical and chemical stability of solid electrolyte–electrode interfaces in all-solid-state Li-ion batteries

TL;DR: In this paper, the authors performed first principles calculations to evaluate the thermodynamics of the interfaces between solid electrolyte and electrode materials and to identify the chemical and electrochemical stabilities of these interfaces.
References
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Journal ArticleDOI

Origin of the Overpotential for Oxygen Reduction at a Fuel-Cell Cathode

TL;DR: In this paper, the stability of reaction intermediates of electrochemical processes on the basis of electronic structure calculations was analyzed and a detailed description of the free energy landscape of the electrochemical oxygen reduction reaction over Pt(111) as a function of applied bias was presented.
Journal ArticleDOI

Lithium−Air Battery: Promise and Challenges

TL;DR: In this article, the authors summarized the promise and challenges facing development of practical Li−air batteries and the current understanding of its chemistry, and showed that the fundamental battery chemistry during discharge is the electrochemical oxidation of lithium metal at the anode and reduction of oxygen from air at the cathode.
Journal ArticleDOI

Reactions in the Rechargeable Lithium–O2 Battery with Alkyl Carbonate Electrolytes

TL;DR: Mechanisms are proposed for the reactions on discharge and charge that are consistent with the widely observed voltage gap in Li-O(2) cells.
Journal ArticleDOI

A Critical Review of Li/Air Batteries

TL;DR: In this paper, the authors discuss the most critical challenges to developing robust, high-energy Li/air batteries and suggest future research directions to understand and overcome these challenges and predict that Li-air batteries will primarily remain a research topic for the next several years.
Journal ArticleDOI

The Lithium–Oxygen Battery with Ether-Based Electrolytes

TL;DR: It is demonstrated that ether-based electrolytes are not suitable for rechargeable Li–O2 cells, although the ethers are more stable than the organic carbonates, the Li2O2 that forms on the first discharge is accompanied by electrolyte decomposition, to give a mixture of Li2CO3, HCO2 Li, CH3CO2Li, polyethers/ esters, CO2, and H2O.
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