Thermodynamic origin of dendrite growth in metal anode batteries

Hagopian, Arthur; Doublet, Marie-Liesse; Filhol, Jean‐Sébastien

doi:10.1039/d0ee02665d

Cited by 135 publications

(123 citation statements)

References 81 publications

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“…This is a sizable fraction of the surface tension of uncharged Li, which is about 0.5 J m −2 . At sufficiently large deviations from the pzc, the surface tension becomes negative, and the electrode dissolves, as has been noted by Hagopian et al [4] . Using the same values for the capacitance, this would happen at a deviation of about 2.23 V from the pzc, or about 1 V below the deposition potential.…”

Section: Effects Of An Excess Charge Density On the Properties Of An mentioning

confidence: 59%

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The Crucial Role of Local Excess Charges in Dendrite Growth on Lithium Electrodes

Santos

Schmickler

2021

Angew Chem Int Ed

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Much theoretical effort has been spent on the causes of dendrite formation in lithium metal batteries, but a decisive factor has been overlooked: Lithium is deposited on an electrode which carries a sizable negative charge, and this charge is not distributed homogeneously on the surface. We show by explicit model calculations that the excess charge accumulates on small protrusions and creates a strong electric field, which attracts the Li+ ions and induces further growth on the tip and finally the formation of dendrites. Even a small tip consisting of a few atoms will carry an excess charge of a tenth of a unit charge or more. In addition, the negative charge on the tips locally reduces the surface tension, which further fosters dendrite growth. The same principles can also explain dendrite formation on other metals with deposition potentials below the potential of zero charge.

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Section: Effects Of An Excess Charge Density On the Properties Of An mentioning

confidence: 59%

“…Why do dendrites form spontaneously during lithium deposition, while one has to use brute force, an overpotential of several volts, to form dendrites on copper? In a very recent paper Hagopian et al [4] . proposed that dendrites form when the electrode becomes thermodynamically unstable at very negative charge densities.…”

Section: Introductionmentioning

confidence: 99%

The Crucial Role of Local Excess Charges in Dendrite Growth on Lithium Electrodes

Santos

Schmickler

2021

Angew Chem Int Ed

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“…0.5 J m −2 beträgt. Bei genügend großen Abweichungen vom pzc wird die Oberflächenspannung negativ, und die Elektrode löst sich auf, wie auch von Hagopian et al [4] . bemerkt wurde.…”

Section: Effekte Einer üBerschussladung Auf Die Eigenschaften Einer Eunclassified

“…Kann unser Modell Hinweise für die Konstruktion von Batterien mit Lithium oder ähnlichen Metallen liefern? Wie von Hagopian et al [4] . diskutiert, gibt es zwei wichtige Potentiale: das Abscheidungspotential und das Potential des Ladungsnullpunkts.…”

Section: Schlussfolgerungenunclassified

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Die entscheidende Rolle von lokalen Ladungsfluktuationen beim Wachstum von Dendriten auf Lithium‐Elektroden

Santos

Schmickler

2021

Angewandte Chemie

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Obwohl sich sehr viele theoretische Arbeiten mit der Ursache der Dendritenbildung an reinen Lithium‐Elektroden befasst haben, wurde bisher ein entscheidender Faktor übersehen: Bei der Abscheidung von Lithium ist die Elektrode stark negativ geladen, und diese Ladung ist nicht gleichmäßig über die Oberfläche verteilt. Explizite Modellrechnungen zeigen, dass sich die Überschussladung auf der Spitze kleiner Unebenheiten, die durch Fluktuationen entstehen, konzentriert. Sie erzeugt dort ein starkes elektrisches Feld, welches Lithium‐Ionen anzieht, die Spitze weiter wachsen lässt und schließlich zur Bildung von Dendriten führt. Selbst eine kleine Spitze, die nur aus wenigen Atomen besteht, trägt eine Überschussladung von der Größenordnung eines Zehntels der Elektronenladung oder mehr. Zudem erniedrigt eine negative Ladung lokal die Oberflächenspannung, was die Dendritenbildung zusätzlich begünstigt. Derselbe Mechanismus kann auch die Dendritenbildung an anderen Metallen erklären, deren Abscheidungspotential tiefer liegt als der Ladungsnullpunkt.

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Advanced Electrolytes Enabling Safe and Stable Rechargeable Li‐Metal Batteries: Progress and Prospects

Tan

Wang

Tian

et al. 2021

Adv Funct Materials

143

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Rechargeable Li-metal batteries (RLBs) can boost energy yet possess poor cycle stability and safety concerns when utilizing carbonate electrolytes. Countless effort has been invested in researching and developing electrolytes for RLBs to obtain stable and safe batteries. However, only few existing electrolytes meet the requirements for practical RLBs. In this perspective, the challenges of organic liquid electrolytes in the application in RLBs are summarized, and requirements for electrolytes for practical RLBs are proposed. This perspective briefly reviews the recent achievements of electrolytes (liquid-and solid-state) for RLBs and analyzes the corresponding drawbacks of each electrolyte. Further, possible solutions to the existing shortcomings of various electrolytes are proposed. In particular, this perspective outlines the development strategy of in situ gelation electrolytes, accompanied by a call for people using pouch cells to evaluate performance and paying more attention to battery safety research. This perspective aims to expound on the challenges and the possible research directions of RLBs electrolytes to promote practical RLBs better.

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Thermodynamic origin of dendrite growth in metal anode batteries

Abstract: The whiskers/dendrites-growth phenomenon observed on metal anode-surfaces in batteries is shown to have a thermodynamic origin taking its root from negative surface tensions associated with a symmetry breaking of the crystal shape.

Cited by 135 publications

References 81 publications

The Crucial Role of Local Excess Charges in Dendrite Growth on Lithium Electrodes

The Crucial Role of Local Excess Charges in Dendrite Growth on Lithium Electrodes

Die entscheidende Rolle von lokalen Ladungsfluktuationen beim Wachstum von Dendriten auf Lithium‐Elektroden

Advanced Electrolytes Enabling Safe and Stable Rechargeable Li‐Metal Batteries: Progress and Prospects

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