Durable fast-charging lithium metal batteries designed with cross-linked polymer electrolytes and niobate-coated cathode

Chiou, Min-Huei; Borzutzki, Kristina; Thienenkamp, Johannes Helmut; Mohrhardt, Marvin; Liu, Kun-Lin; Mereacre, Valeriu; Binder, Joachim R.; Ehrenberg, Helmut; Winter, Martin; Brunklaus, Gunther

doi:10.1016/j.jpowsour.2022.231528

Cited by 10 publications

(15 citation statements)

References 82 publications

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“…To enable sufficient contact with the cathode active material, the cathode was spin-coated with 30 μL of a solution containing 10 wt % PSA in DMAc and dried afterward as reported previously . By application of oxidic coatings, in particular, LiNbO 3 , onto the NMC active material, the achievable capacity retention of battery cells with solid or liquid electrolytes may be significantly improved. − To investigate the influence of such cathode coatings onto the cell performance with composite electrolytes, commercial NMC622 as well as LiNbO 3 -coated NMC622 (c-NMC622) was subjected to constant current cycling at 0.5C and 40 °C (Figure a). The achievable discharge capacity of as-obtained NMC622 in the first cycles and at the beginning of the long-term cycling amounts to 131 mAh g –1 at 0.5C, which is higher than that in the case of cells that are operated with c-NMC622 (118 mAh g –1 ).…”

Section: Results and Discussionmentioning

confidence: 99%

Ceramic-in-Polymer Hybrid Electrolytes with Enhanced Electrochemical Performance

Overhoff

Ali

Brinkmann

et al. 2022

ACS Appl. Mater. Interfaces

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Polymer electrolytes are attractive candidates to boost the application of rechargeable lithium metal batteries. Single-ion conducting polymers may reduce polarization and lithium dendrite growth, though these materials could be mechanically overly rigid, thus requiring ion mobilizers such as organic solvents to foster transport of Li ions. An inhomogeneous mobilizer distribution and occurrence of preferential Li transport pathways eventually yield favored spots for Li plating, thereby imposing additional mechanical stress and even premature cell short circuits. In this work, we explored ceramic-in-polymer hybrid electrolytes consisting of polymer blends of single-ion conducting polymer and PVdF-HFP, including EC/PC as swelling agents and silane-functionalized LATP particles. The hybrid electrolyte features an oxide-rich layer that notably stabilizes the interphase toward Li metal, enabling single-side lithium deposition for over 700 h at a current density of 0.1 mA cm–2. The incorporated oxide particles significantly reduce the natural solvent uptake from 140 to 38 wt % despite maintaining reasonably high ionic conductivities. Its electrochemical performance was evaluated in LiNi0.6Co0.2Mn0.2O2 (NMC622)||Li metal cells, exhibiting impressive capacity retention over 300 cycles. Notably, very thin LiNbO3 coating of the cathode material further boosts the cycling stability, resulting in an overall capacity retention of 78% over more than 600 cycles, clearly highlighting the potential of hybrid electrolyte concepts.

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Section: Results and Discussionmentioning

confidence: 99%

Ceramic-in-Polymer Hybrid Electrolytes with Enhanced Electrochemical Performance

Overhoff

Ali

Brinkmann

et al. 2022

ACS Appl. Mater. Interfaces

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“…According to a previous work, a high fraction of secondary species would lead to a lower capacity retention of cells operated with these carbonate-based polymer electrolytes. Thus, the mass ratio between primary (modified PTMC-GCDs) and secondary species was set to 3:1.…”

Section: Methodsmentioning

confidence: 93%

“…Propylene carbonate (PC) and lithium bis-trifluoro-methanesulfonimide (LiTFSI) were obtained from BASF and Solvionic, respectively. LiNi 0.6 Mn 0.2 Co 0.2 O 2 (NMC622) cathode sheets (with a mass loading of 2.5 mg cm −2 and a layer thickness of 17 μm) were prepared following established protocols, 30 and a thicker NMC622 cathode sheet (6.3 mg cm −2 ) was purchased from CUSTOMCELLS.…”

Section: ■ Introductionmentioning

confidence: 99%

“…In the present work, the impacts of compatibility based on copolymer structural chemistries (e.g., electrostatic potentials) on membrane homogeneity and electrochemical cycling performance of cells are investigated. A multifunctional and carbonate-based oligomer [modified poly(trimethylene carbonate)-grafted cyclodextrins (PTMC-GCDs)] was introduced as the primary segment species due to its amorphous structure and promising electrochemical features (including a high transference number of ∼0.6 and a wide oxidative stability window of up to 5 V, as revealed by a previous work), 30 and several types of monomer species with distinct chemical bonds and polarities were explored as secondary segment species to establish various network structures in the presence of a plasticizer or mobilizer while systematically evaluating the corresponding electrolyte properties and electrochemical features in NMC622||Li-and Cu||Li-type cells. Notably, behaviors of molecular aggregations and lithium-ion coordination can be clearly elucidated by atomic force microscopy (AFM) images and molecular dynamics (MD) simulations.…”

Section: ■ Introductionmentioning

confidence: 99%

“…The multifunctional carbonate-based oligomers (modified PTMC-grafted α-cyclodextrins; M n ∼11k) with 90% modification at the terminal groups (hydroxyl group to acrylate) were prepared according to a reported procedure (please see 1 H NMR and gel permeation chromatography (GPC) data collected in Figure S1, Supporting Information). 30 1,6-Hexanediol diacrylate (HDDA, 99%, dried over 4 Å molecular sieves) and triethylene glycol diacrylate (TEGDA, 90%, dried over 4 Å molecular sieves) were received from abcr GmbH. 2,2-Dimethoxy-2-phenylacetophenone (DMPA, 99%), poly(ethylene glycol)diacrylate (PEGDA; M n 700), 2-(2ethoxyethoxy)ethyl acrylate (EOEOEA, dried over 4 Å molecular sieves), and 1,3-butanediol diacrylate (BDDA, >98%, dried over 4 Å molecular sieves) were purchased from Sigma Aldrich, Germany.…”

Section: ■ Introductionmentioning

confidence: 99%

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Selection of Polymer Segment Species Matters for Electrolyte Properties and Performance in Lithium Metal Batteries

Chiou

Verweyen

Diddens

et al. 2023

ACS Appl. Energy Mater.

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Control of homogeneous lithium deposition governs prospects of advanced cell development and practical applications of high-energy-density lithium metal batteries. Polymer electrolytes are thus explored and employed to mitigate the growth of high-surface-area lithium species while enhancing the reversibility of the lithium reservoir upon cell cycling. Herein, an in-depth understanding of the distribution of membrane properties and lithium deposition behavior affected by the selection of polymer segment species is derived. It is demonstrated that severely localized lithium deposits featuring needle-like morphologies may be readily observed when electrostatic fields (or partial charges) and the amount of Li + coordinators of the primary and secondary polymer segment species appear rather dissimilar, leading to a sudden cell failure at early stages of cell operation. In comparison, employment of optimized copolymer electrolytes enables superior cell performance at 1C even with thicker cathodes (6.3 mg cm −2 ). Additionally, the improvement of cell-cycling stability due to enhancement of similarity of dipole moments and partial charge distributions among copolymer segments are also demonstrated for different polymer systems, contributing to avoidance of undesired lithium protrusions, also reflecting a viable concept for the design of future copolymer electrolytes.

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

Chen

Lennartz

Liu

et al. 2023

Adv Funct Materials

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To go beyond polyethylene oxide in lithium metal batteries, a hybrid polymer/oligomer cell design is presented, where an ester oligomer provides high ionic conductivity of 0.2 mS cm−1 at 40 °C within thicker composite cathodes with active mass loadings of up to 11 mg cm−2 (LiNbO3‐coated) LiNi0.6Mn0.2Co0.2 (NMC622), while a 30 µm thin scaffold‐supported polymer electrolyte affords mechanical stability. Corresponding discharge capacities of the hybrid cells exceed 170 mAh g−1 (11 mg cm−2) or 160 mAh g−1 (6 mg cm−2) at rates of either 0.1 or 0.25 C. Multilayer pouch cells are projected to enable energy densities of 235 Wh L−1 (6 mg cm−2) and even up to 356 Wh L−1 (11 mg cm−2), clearly superior to other reported polymer‐based cell designs. Polyester electrolytes are environmentally benign and safer compared to common liquid electrolytes, while the straightforward synthesis and affordability of precursors render hybrid polyester electrolytes suitable candidates for future application in solid‐state lithium metal batteries.

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Durable fast-charging lithium metal batteries designed with cross-linked polymer electrolytes and niobate-coated cathode

Cited by 10 publications

References 82 publications

Ceramic-in-Polymer Hybrid Electrolytes with Enhanced Electrochemical Performance

Ceramic-in-Polymer Hybrid Electrolytes with Enhanced Electrochemical Performance

Selection of Polymer Segment Species Matters for Electrolyte Properties and Performance in Lithium Metal Batteries

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

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