Limiting Current Density in Single-Ion-Conducting and Conventional Block Copolymer Electrolytes

Hoffman, Zach J.; Ho, Alec S.; Chakraborty, Saheli; Balsara, Nitash P.

doi:10.1149/1945-7111/ac613b

Cited by 10 publications

(18 citation statements)

References 36 publications

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“…A low transference number leads to generation of salt concentration gradients within dual-ion conducting electrolytes upon passage of current, and at high currents when the rate of diffusion cannot compensate for the rate of Li on the reducing electrode, a complete depletion of lithium salt can occur which are reflected in steep overpotentials during Li//Li symmetric cell cycling. [29][30][31] Indeed, because of the higher transference number of the Trilayer CPE w/ Porous Scaffold ("high solids"), flatter overpotentials are observed during cycling of the Li//Li symmetric cells compared to that of a pure-cross-linked PEO + LiTFSI membrane of similar thickness (Figure 4a), at currents up to 0.2 mA cm −2 . At higher currents, the polymer electrolyte and the Trilayer CPE w/ Porous Scaffold ("high solids") both presented steep overpotentials.…”

Section: Resultsmentioning

confidence: 99%

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Role of Scaffold Architecture and Excess Surface Polymer Layers in a 3D‐Interconnected Ceramic/Polymer Composite Electrolyte

Sahore

Armstrong

Tang

et al. 2023

Advanced Energy Materials

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3D‐interconnected ceramic/polymer composite electrolytes offer promise to combine the benefits of both ceramic and polymer electrolytes. However, an in‐depth understanding of the role of the ceramic scaffold's architecture, and the associated polymer/ceramic interfaces on the electrochemical properties of such composite electrolytes is still incomplete. Here, these factors are systematically evaluated using an interconnected composite electrolyte with a tunable and well‐defined architecture. The ionic conductivity of the ceramic scaffold is strongly dependent on its porosity and tortuosity, as demonstrated experimentally and via theoretical modeling. The connectivity of the ceramic framework avoids the high interfacial impedance at the polymer/ceramic electrolyte interface within the composite. However, this work discovers that the interfacial impedance between the bulk composite and excess surface polymer layers of the composite membrane dominates the overall impedance, resulting in a 1–2 order drop of ionic conductivity compared to the ceramic scaffold. Despite the high impedance interfaces, an improved Li+ transference number is found compared to the neat polymer (0.29 vs 0.05), attributed to the ceramic phase's contributions toward ion transport. This leads to flatter overpotentials in lithium symmetric cell cycling. These results are expected to guide future research directions toward scalable manufacturing of composite electrolytes with optimized architecture and interfaces.

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Section: Resultsmentioning

confidence: 99%

“…Composite electrolytes with simply dispersed ceramic particles in high volume fractions yielded similar (ref. [31]) or higher (ref. [33]) ionic conductivities to ours.…”

Section: Resultsmentioning

confidence: 99%

Role of Scaffold Architecture and Excess Surface Polymer Layers in a 3D‐Interconnected Ceramic/Polymer Composite Electrolyte

Sahore

Armstrong

Tang

et al. 2023

Advanced Energy Materials

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“…This concentration polarization‐induced cell failure is commonly observed when operating the battery above the limiting current density. As the current passes through the electrolyte, anions accumulate near the Li 0 stripping side, while salt depletion occurs near the Li 0 plating side [30] . Above the limiting current density and with increasing operation time, the salt concentration near the Li 0 plating side reaches zero, leading to Li 0 whisker formation and cell failure [6,7b] .…”

Section: Resultsmentioning

confidence: 99%

“…As the current passes through the electrolyte, anions accumulate near the Li 0 stripping side, while salt depletion occurs near the Li 0 plating side. [30] Above the limiting current density and with increasing operation time, the salt concentration near the Li 0 plating side reaches zero, leading to Li 0 whisker formation and cell failure. [6,7b] In contrast, the SIC-3 electrolyte with covalently tethered anions distributed homogeneously within the polymer matrix minimized anion accumulation and salt depletion.…”

Section: Methodsmentioning

confidence: 99%

Anion‐tethered Single Lithium‐ion Conducting Polyelectrolytes through UV‐induced Free Radical Polymerization for Improved Morphological Stability of Lithium Metal Anodes

He,

Wang,

Zou

et al. 2023

Angew Chem Int Ed

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Single Li+ ion conducting polyelectrolytes (SICs), which feature covalently tethered counter‐anions along their backbone, have the potential to mitigate dendrite formation by reducing concentration polarization and preventing salt depletion. However, due to their low ionic conductivity and complicated synthetic procedure, the successful validation of these claimed advantages in lithium metal (Li0) anode batteries remains limited. In this study, we fabricated a SIC electrolyte using a single‐step UV polymerization approach. The resulting electrolyte exhibited a high Li+ transference number (t+) of 0.85 and demonstrated good Li+ conductivity (6.3×10−5 S/cm at room temperature), which is comparable to that of a benchmark dual ion conductor (DIC, 9.1×10−5 S/cm). Benefitting from the high transference number of SIC, it displayed a three‐fold higher critical current density (2.4 mA/cm2) compared to DIC (0.8 mA/cm2) by successfully suppressing concentration polarization‐induced short‐circuiting. Additionally, the t+ significantly influenced the deposition behavior of Li0, with SIC yielding a uniform, compact, and mosaic‐like morphology, while the low t+ DIC resulted in a porous morphology with Li0 whiskers. Using the SIC electrolyte, Li0||LiFePO4 cells exhibited stable operation for 4500 cycles with 70.5 % capacity retention at 22 °C.

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“…The diffusion rate of Zn 2+ has a maximum value, which can be revealed by diffusion-limited current density term J lim . [62][63][64] It is acknowledged that the deposition roughness is determined by fraction of the current density (j/J lim ) at which the electrodeposition is conducted. [60] The formation mechanism of electrodeposition landscape can be divided into two regimes: below and above the limiting current density.…”

Section: Mass Transfermentioning

confidence: 99%

Artificial Interphase Layer for Stabilized Zn Anodes: Progress and Prospects

Zhang

Shi

et al. 2022

Small

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The burgeoning Li‐ion battery is regarded as a powerful energy storage system by virtue of its high energy density. However, inescapable issues concerning safety and cost aspects retard its prospect in certain application scenarios. Accordingly, strenuous efforts have been devoted to the development of the emerging aqueous Zn‐ion battery (AZIB) as an alternative to inflammable organic batteries. In particular, the instability from the anode side severely impedes the commercialization of AZIB. Constructing an artificial interphase layer (AIL) has been widely employed as an effective strategy to stabilize the Zn anode. This review specializes in the state‐of‐the‐art of AIL design for Zn anode protection, encompassing the preparation methods, mechanism investigations, and device performances based on the classification of functional materials. To begin with, the origins of Zn instability are interpreted from the perspective of electrical field, mass transfer, and nucleation process, followed by a comprehensive summary with respect to functions of AIL and its designing criteria. In the end, current challenges and future outlooks based upon theoretical and experimental considerations are included.

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Limiting Current Density in Single-Ion-Conducting and Conventional Block Copolymer Electrolytes

Cited by 10 publications

References 36 publications

Role of Scaffold Architecture and Excess Surface Polymer Layers in a 3D‐Interconnected Ceramic/Polymer Composite Electrolyte

Role of Scaffold Architecture and Excess Surface Polymer Layers in a 3D‐Interconnected Ceramic/Polymer Composite Electrolyte

Anion‐tethered Single Lithium‐ion Conducting Polyelectrolytes through UV‐induced Free Radical Polymerization for Improved Morphological Stability of Lithium Metal Anodes

Artificial Interphase Layer for Stabilized Zn Anodes: Progress and Prospects

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