Diffusion-limited model for a lithium/air battery with an organic electrolyte

Sandhu, Sarwan S.; Fellner, Joseph P.; Brutchen, George W.

doi:10.1016/j.jpowsour.2006.09.099

Cited by 159 publications

(158 citation statements)

References 4 publications

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“…4,5 The suggestion that electrical passivation was a central issue resulted from comparing the discharge capacity of typical Li-O 2 batteries with large surface area porous C cathodes to that observed with low surface area glassy carbon (GC) electrodes, where clogging and O 2 transport issues were negligible. Although the absolute magnitudes of the capacity were different in the two cases, both showed the same qualitative discharge behavior, i.e., a relatively stable discharge potential at ∼2.6 V to a certain discharge capacity, followed by a sudden decrease in output potential to <2.0 V (defined as death of the cell).…”

Section: Introductionmentioning

confidence: 99%

Electrical conductivity in Li2O2 and its role in determining capacity limitations in non-aqueous Li-O2 batteries

Viswanathan

Thygesen

Hummelshøj

et al. 2011

The Journal of Chemical Physics

541

661

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New photoacoustic cell design for studying aqueous solutions and gels Rev. Sci. Instrum. 82, 084903 (2011) Electric response of a cell of hydrogel: Role of the electrodes Appl. Phys. Lett. 98, 064101 (2011) Effect of the gate electrode on the response of organic electrochemical transistors APL: Org. Electron. Photonics 3, 205 (2010) Effect of the gate electrode on the response of organic electrochemical transistors Appl. Phys. Lett. 97, 123304 (2010) Note: Fixture for characterizing electrochemical devices in-operando in traditional vacuum systems Rev. Sci. Instrum. 81, 086104 (2010) Additional information on J. Chem. Phys. Non-aqueous Li-air or Li-O 2 cells show considerable promise as a very high energy density battery couple. Such cells, however, show sudden death at capacities far below their theoretical capacity and this, among other problems, limits their practicality. In this paper, we show that this sudden death arises from limited charge transport through the growing Li 2 O 2 film to the Li 2 O 2 -electrolyte interface, and this limitation defines a critical film thickness, above which it is not possible to support electrochemistry at the Li 2 O 2 -electrolyte interface. We report both electrochemical experiments using a reversible internal redox couple and a first principles metal-insulator-metal charge transport model to probe the electrical conductivity through Li 2 O 2 films produced during Li-O 2 discharge. Both experiment and theory show a "sudden death" in charge transport when film thickness is ∼5 to 10 nm. The theoretical model shows that this occurs when the tunneling current through the film can no longer support the electrochemical current. Thus, engineering charge transport through Li 2 O 2 is a serious challenge if Li-O 2 batteries are ever to reach their potential.

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Section: Introductionmentioning

confidence: 99%

Electrical conductivity in Li2O2 and its role in determining capacity limitations in non-aqueous Li-O2 batteries

Viswanathan

Thygesen

Hummelshøj

et al. 2011

The Journal of Chemical Physics

541

661

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“…Existing models of Li-O 2 batteries are either macroscopic or atomistic. Cell-level models propose pore blocking due to reaction products [34][35][36][37][38] and surface passivation [24,39]. Atomistic models discuss the surface structure of Li 2 O 2 crystals [40][41][42][43][44], the kinetics of the oxygen reduction/evolution in aprotic electrolytes [40,44,45], and the electron conductivity of Li 2 O 2 [24,41,46].…”

mentioning

confidence: 99%

Rate-Dependent Morphology of Li₂O₂ Growth in Li–O₂ Batteries

Horstmann

Gallant

Mitchell

et al. 2013

J. Phys. Chem. Lett.

150

191

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Compact solid discharge products enable energy storage devices with high gravimetric and volumetric energy densities, but solid deposits on active surfaces can disturb charge transport and induce mechanical stress. In this Letter we develop a nanoscale continuum model for the growth of Li 2 O 2 crystals in lithium-oxygen batteries with organic electrolytes, based on a theory of electrochemical non-equilibrium thermodynamics originally applied to Li-ion batteries. As in the case of lithium insertion in phase-separating LiFePO 4 nanoparticles, the theory predicts a transition from complex to uniform morphologies of Li 2 O 2 with increasing current. Discrete particle growth at low discharge rates becomes suppressed at high rates, resulting in a film of electronically insulating Li 2 O 2 that limits cell performance. We predict that the transition between these surface growth modes occurs at current densities close to the exchange current density of the cathode reaction, consistent with experimental observations.

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“…For example, the average theoretical energy density for the Li-air battery is 8170 Wh·kg -1 . Although the energy density of the Li-air battery is lower than the energy density of gasoline/air which is 11,860 Wh·kg -1 [2], the operation efficiency of the former is higher than the maximum efficiency of the heat engine.…”

Section: Introductionmentioning

confidence: 93%

Fundamental principals of battery design: Porous electrodes

2014

AIP Conference Proceedings

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Abstract. The fundamental aspects of a porous electrode from electrochemistry and material chemistry standpoints are discussed in the light of battery engineering designs. For example, the ionic diffusion, the electrode-electrolyte interface, interfacial charge transfer and electrode catalytic processes are discussed. The discussion of such fundamental electrochemical aspects is in conjunction with the design of batteries, e.g. the electrochemical assessable surface area for porous electrode and electrode catalytic reactions. The porous electrodes used as a gas diffusion electrode and the electrode in a supercapacitor are discussed to demonstrate the application of electrochemical principals in battery design.

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Diffusion-limited model for a lithium/air battery with an organic electrolyte

Cited by 159 publications

References 4 publications

Electrical conductivity in Li2O2 and its role in determining capacity limitations in non-aqueous Li-O2 batteries

Electrical conductivity in Li2O2 and its role in determining capacity limitations in non-aqueous Li-O2 batteries

Rate-Dependent Morphology of Li₂O₂ Growth in Li–O₂ Batteries

Fundamental principals of battery design: Porous electrodes

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Diffusion-limited model for a lithium/air battery with an organic electrolyte

Cited by 159 publications

References 4 publications

Electrical conductivity in Li2O2 and its role in determining capacity limitations in non-aqueous Li-O2 batteries

Electrical conductivity in Li2O2 and its role in determining capacity limitations in non-aqueous Li-O2 batteries

Rate-Dependent Morphology of Li2O2 Growth in Li–O2 Batteries

Fundamental principals of battery design: Porous electrodes

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Rate-Dependent Morphology of Li₂O₂ Growth in Li–O₂ Batteries