Towards All‐Solid‐State Polymer Batteries: Going Beyond PEO with Hybrid Concepts

Chen, Yi‐Hsuan; Lennartz, Peter; Liu, Kun Ling; Hsieh, Yi-Chen; Scharf, Felix; Guerdelli, Rayan; Buchheit, Annika; Grünebaum, Mariano; Kempe, Fabian; Winter, Martin; Brunklaus, Gunther

doi:10.1002/adfm.202300501

Cited by 7 publications

(3 citation statements)

References 66 publications

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“…In addition to PEO, we also investigated the influence of the external pressure on a second polymer. In this study, we utilized cross-linked GCD-PCL (xGCD-PCL), which had been previously employed in similar research . The caprolactone functional group present in the polymer contributes to increased Li + transference numbers and sufficient Li + conductivity …”

Section: Resultsmentioning

confidence: 99%

“… 31 The caprolactone functional group present in the polymer contributes to increased Li + transference numbers and sufficient Li + conductivity. 31 …”

Section: Resultsmentioning

confidence: 99%

“…Bis(trifluoromethane)-sulfonimide Li salt (LiTFSI, purity = 99.95%, Aldrich) was dried at 120 °C under reduced pressure (10 –3 mbar) for 2 days. α-Cyclodextrin grafted poly(caprolactone) (GCD-PCL, M n = 76 000 g mol –1 ) was synthesized according to a previous publication 31 and dried at 40 °C under reduced pressure (10 –3 mbar) for 5 days. PEO, GCD-PCL, benzophenone, and LiTFSI were subsequently stored inside a glovebox (MBraun Unilab, <0.1 ppm of H 2 O, <0.1 ppm of O 2 ) under an inert argon atmosphere.…”

Section: Methodsmentioning

confidence: 99%

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External Pressure in Polymer-Based Lithium Metal Batteries: An Often-Neglected Criterion When Evaluating Cycling Performance?

Roering,

Overhoff,

Liu

et al. 2024

ACS Appl. Mater. Interfaces

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Solid-state batteries based on lithium metal anodes, solid electrolytes, and composite cathodes constitute a promising battery concept for achieving high energy density. Charge carrier transport within the cells is governed by solid− solid contacts, emphasizing the importance of well-designed interfaces. A key parameter for enhancing the interfacial contacts among electrode active materials and electrolytes comprises externally applied pressure onto the cell stack, particularly in the case of ceramic electrolytes. Reports exploring the impact of external pressure on polymer-based cells are, however, scarce due to overall better wetting behavior. In this work, the consequences of externally applied pressure in view of key performance indicators, including cell longevity, rate capability, and limiting current density in single-layer pouch-type NMC622||Li cells, are evaluated employing cross-linked poly(ethylene oxide), xPEO, and cross-linked cyclodextrin grafted poly(caprolactone), xGCD-PCL. Notably, externally applied pressure substantially changes the cell's electrochemical cycling performance, strongly depending on the mechanical properties of the considered polymers. Higher external pressure potentially enhances electrode− electrolyte interfaces, thereby boosting the rate capability of pouch-type cells, despite the fact that the cell longevity may be reduced upon plastic deformation of the polymer electrolytes when passing beyond intrinsic thresholds of compressive stress. For the softer xGCD-PCL membrane, cycling of cells is only feasible in the absence of external pressure, whereas in the case of xPEO, a trade-off between enhanced rate capability and minimal membrane deformation is achieved at cell pressures of ≤0.43 MPa, which is considerably lower and more practical compared to cells employing ceramic electrolytes with ≥5 MPa external pressure.

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Section: Resultsmentioning

confidence: 99%

“… 31 The caprolactone functional group present in the polymer contributes to increased Li + transference numbers and sufficient Li + conductivity. 31 …”

Section: Resultsmentioning

confidence: 99%

Section: Methodsmentioning

confidence: 99%

See 1 more Smart Citation

External Pressure in Polymer-Based Lithium Metal Batteries: An Often-Neglected Criterion When Evaluating Cycling Performance?

Roering,

Overhoff,

Liu

et al. 2024

ACS Appl. Mater. Interfaces

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Challenges and Solutions of Solid‐State Electrolyte Film for Large‐Scale Applications

Huang,

Li,

Fan

et al. 2024

Advanced Energy Materials

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Solid‐state lithium‐ion batteries are widely accepted as the promising next‐generation energy storage technology due to higher energy density and improved safety compared to conventional lithium‐ion batteries with liquid electrolytes. Large‐area solid‐state electrolyte (SSE) films with adequate thickness control, improved ionic conductivity, and good interfacial contact can reduce internal resistance, increase the real energy density of batteries, and reduce manufacturing costs. Optimization of SSE properties at the particle scale and large‐scale preparation of SSE films are key to the development of high‐performance solid‐state lithium‐ion batteries and their industrialization. Therefore, this paper provides a comprehensive review of SSE, covering both particle‐level features like the effects of particle size, density, and air stability on the electrochemical performance, as well as four major routes for large‐scale preparation and relevant strategies for structural optimization of SSE films. In addition, the effects of large‐area SSE films on the electrochemical performance of solid‐state batteries and their applications in pouch solid‐state lithium‐ion battery systems are discussed in detail. Finally, the design principles of SSE particles and SSE films are summarized and the development direction of thin SSEs is envisaged.

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Synergistic Enhancement of Mechanical and Electrochemical Properties in Grafted Polymer/Oxide Hybrid Electrolytes

Scharf,

Krude,

Lennartz

et al. 2024

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Lithium metal batteries operated with high voltage cathodes are predestined for the realization of high energy storage systems, where solid polymer electrolytes offer a possibility to improve battery safety. Al2O3_PCL is introduced as promising hybrid electrolyte made from polycaprolactone (PCL) and Al2O3 nanoparticles that can be prepared in a one‐pot synthesis as a random mixture of linear PCL and PCL‐grafted Al2O3. Upon grafting, synergistic effects of mechanical stability and ionic conductivity are achieved. Due to the mechanical stability, manufacture of PCL‐based membranes with a thickness of 50 µm is feasible, yielding an ionic conductivity of 5·10−5 S cm−1 at 60 °C. The membrane exhibits an impressive performance of Li deposition in symmetric Li||Li cells, operating for 1200 h at a constant and low overvoltage of 54 mV and a current density of 0.2 mA cm−2. NMC622 | Al2O3_PCL | Li cells are cycled at rates of up to 1 C, achieving 140 cycles at >80% state of health. The straightforward synthesis and opportunity of upscaling as well as solvent‐free polymerization render the Al2O3_PCL hybrid material as rather safe, potentially sustainable and affordable alternative to conventional polymer‐based electrolytes.

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Towards All‐Solid‐State Polymer Batteries: Going Beyond PEO with Hybrid Concepts

Cited by 7 publications

References 66 publications

External Pressure in Polymer-Based Lithium Metal Batteries: An Often-Neglected Criterion When Evaluating Cycling Performance?

External Pressure in Polymer-Based Lithium Metal Batteries: An Often-Neglected Criterion When Evaluating Cycling Performance?

Challenges and Solutions of Solid‐State Electrolyte Film for Large‐Scale Applications

Synergistic Enhancement of Mechanical and Electrochemical Properties in Grafted Polymer/Oxide Hybrid Electrolytes

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