Self‐Healing Properties of Alkali Metals under “High‐Energy Conditions” in Batteries

Li, Yuqian; Zhang, Liyuan; Zhang, Jiaheng; Wang, Xiuli; Gu, Changzhan; Xia, Xinhui; Tu, Jiangping

doi:10.1002/aenm.202100470

Cited by 18 publications

(19 citation statements)

References 39 publications

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“…accumulate even under a higher current density, that is, the self-healing process. [34][35][36][37][38] The Li lament growth and self-healing compete with each other and result in uctuating parameters of T and Power-law. This mutual competition also leads to huge voltage uctuations and scattering signal uctuations.…”

Section: Resultsmentioning

confidence: 99%

Revealing the dynamic evolution of Li filaments within solid electrolytes by operando small-angle neutron scattering

Yang

et al. 2022

Applied Physics Letters

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Lithium dendrite (filaments) propagation in solid electrolytes (SEs) leading to short circuits is one of the biggest obstacles to the application of all-solid-state lithium metal batteries. Due to the lack of operando techniques that can provide high resolution, the insufficient knowledge of the lithium dendrite growth inside SEs makes it difficult to suppress the dendrite growth. To reveal the mechanism of the Li filament growth in SEs, we achieved real-time monitoring of the nanoscale Li filament growth by operando small-angle neutron scattering (SANS) in representative Li6.5La3Zr1.5Nb0.5O12 SEs. On continuous plating, the Li filament growth is not simply an accumulation of Li, but there is a dynamic evolution due to the competition between the Li filament growth and self-healing. With the aid of simulations and experiments, this dynamic competition was demonstrated to be highly dependent on temperature variation. The enhanced self-healing ability of Li at elevated temperatures plays a positive role in suppressing the Li filament growth. The heat therapy improved the cell's cycle life, which provided insight into suppressing the Li filament growth. Operando SANS with high Li sensitivity provides a platform for investigating Li filaments in SEs.

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Section: Resultsmentioning

confidence: 99%

Revealing the dynamic evolution of Li filaments within solid electrolytes by operando small-angle neutron scattering

Yang

et al. 2022

Applied Physics Letters

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“…According to the standard powder diffraction file cards of Na (JCPDS: 22-0948) and K (JCPDS: 01-0500), the (110) crystal plane shows the strongest characteristic peaks (Tables S1, S2 and Figure S1). It indicates that the exposed surface of Na and K deposition is mostly the close-packed surface (110). Based on the conditions discussed above, the diffusion processes of the Na atom embedded in K (110) and the K atom embedded in Na (110) were calculated, as shown in Figure b, Video S1, and Video S2.…”

Section: Resultsmentioning

confidence: 99%

“…(c) the interfacial reaction speed on the cathode side is controlled by kinetics; (d) the atom transformation of metal atoms on the bi-metal cathode is controlled by kinetic diffusivity (the diffusion barrier of pure alkali metal atoms has been studied in our previous work); and (e) the final stable structure is decided by the thermodynamic parameters. Thus, the electrochemical reaction of multi-ion cells is more competitive than the reaction of a single metal.…”

Section: Introductionmentioning

confidence: 99%

Expounding the Initial Alloying Behavior of Na–K Liquid Alloy Electrodes

Wang

Luo

et al. 2021

ACS Appl. Mater. Interfaces

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Primary electrodeposition is an accepted strategy to elucidate the nucleation and growth kinetics of metal electrodes. Nevertheless, when confronted with the phase transition process caused by bi-active metals such as NaK liquid alloys, the research process becomes complex and elusive. Herein, we have reduced the intricate issues to relatively simple initial alloying behaviors. Two exchange diffusion mechanisms of the Na atom embedded in K crystals and K atom embedded in Na crystals are investigated by first-principles density functional theory (DFT) calculation and mechanical simulation. As a result, the process of embedding the Na atom in K crystals shows a better thermodynamic stability and lower activation barrier and structural stress than those of the other. The abovementioned conclusions are further proved by stepwise Na and K electrodeposition experiments, and the prepared NaK alloy electrode displays excellent electrochemical performance. Our findings correlate the original alloying mechanism model specification with electrodeposition experimental verification and provide strategies to achieve controllable NaK electrode construction.

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“…[ 7 ] These advantages have promoted a fast research development of PIB over the past few years, primarily focusing on anode/cathode materials and electrolyte design. [ 8–14 ]…”

Section: Introductionmentioning

confidence: 99%

“…[7] These advantages have promoted a fast research development of PIB over the past few years, primarily focusing on anode/cathode materials and electrolyte design. [8][9][10][11][12][13][14] Currently, high-voltage (2-4 V) cathode materials are receiving intense attention, [15] such as Prussian blue analogues, [16] layered metal oxides, [9,17,18] polyanionic compounds, [19] and organic cathodes. [20,21] One big challenge of these cathodes is the relatively low capacity of less than 180 mAh g −1 , which drags down the overall energy density of a full cell.…”

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confidence: 99%

High‐Performance Potassium‐Tellurium Batteries Stabilized by Interface Engineering

Zhang

Zhu

Freschi³

et al. 2022

Small

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K/K + (−2.93 V versus standard hydrogen potential). [7] These advantages have promoted a fast research development of PIB over the past few years, primarily focusing on anode/cathode materials and electrolyte design. [8][9][10][11][12][13][14] Currently, high-voltage (2-4 V) cathode materials are receiving intense attention, [15] such as Prussian blue analogues, [16] layered metal oxides, [9,17,18] polyanionic compounds, [19] and organic cathodes. [20,21] One big challenge of these cathodes is the relatively low capacity of less than 180 mAh g −1 , which drags down the overall energy density of a full cell. [22] Conversion-type sulfur (S) or selenium (Se) is expected to realize a high theoretical capacity of 1675 and 675 mAh g −1 , respectively. [23][24][25] However, the newly emerging K-S or K-Se batteries deliver unsatisfying capacity far away from their ideal value in practical applications, which was mainly caused by the dissolution of polysulfies/ polyselenides intermediates and poor electrical conductivity of S (5 × 10 −28 S cm −1 ) and Se (5 × 10 −3 S cm −1 ). [26,27] Poor electric conductivity results in sluggish reaction kinetics, low utilization of active materials, severe capacity decay, and unsatisfying rate performance. [28,29] Tellurium (Te), another chalcogen element, possesses an excellent electrical conductivity of 2 × 10 2 S cm −1 and a high volumetric capacity of 2621 mAh cm −3 (specific capacity of 420 mAh g −1 ), showing great potential as cathode materials for lithium/sodium-ion storage. [30,31] Sun et al. [32] pioneered the study of Te cathodes in PIB with an average potential of 1.6 V in 2020. They revealed a stepwise reaction mechanism (Te ↔ K 2 Te 3 ↔ K 5 Te 3 ) in the ether-based electrolyte (KTFSI in DEGDME). The major issues for this K-Te battery system were low discharge capacity and rapid capacity fading, probably caused by the large volume change of Te and the dissolution of polytellurides during cycling. [33,34] By increasing electrolyte concentration from 1 M to 5 m KTFSI in DEGDME, the battery delivered a higher capacity up to 409 mAh g −1 . However, severe capacity decay still occurred, which requires rational cathode structure design to confine the acute volume change of Te. Guo et al. [35] disclosed the K-ion storage mechanism of Te cathode in the carbonate-based electrolyte (1 m KFSI in EC:DEC) with K 2 Te as the final potassiation product via a two-electron reaction (2 K + Te ↔ K 2 Te). The excellent cycling stability was achieved with a specific capacity of 215.5 mAh g −1 after 100 cycles at 5C due to the superb immobilization of Te nanoparticles on the The emerging potassium-tellurium (K-Te) battery system is expected to realize fast reaction kinetics and excellent rate performance due to the exceptional electrical conductivity of Te. However, there has been a lack of fundamental knowledge about this new K-Te system, including the reaction mechanism and cathode structure design. Herein, a two-step reaction pathway from Te to K 2 Te 3 and ultimately to K 5 Te 3 is investig...

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Self‐Healing Properties of Alkali Metals under “High‐Energy Conditions” in Batteries

Cited by 18 publications

References 39 publications

Revealing the dynamic evolution of Li filaments within solid electrolytes by operando small-angle neutron scattering

Revealing the dynamic evolution of Li filaments within solid electrolytes by operando small-angle neutron scattering

Expounding the Initial Alloying Behavior of Na–K Liquid Alloy Electrodes

High‐Performance Potassium‐Tellurium Batteries Stabilized by Interface Engineering

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