Determining and Minimizing Resistance for Ion Transport at the Polymer/Ceramic Electrolyte Interface

Chen, X. Chelsea; Liu, Xiaoming; Pandian, Amaresh Samuthira; Lou, Kun; Delnick, Frank M.; Dudney, Nancy J.

doi:10.1021/acsenergylett.9b00495

Cited by 57 publications

(56 citation statements)

References 40 publications

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“…[ 12,63,64 ] The inclusion of a loose‐binding Li + solvent near the ceramic interface may facilitate Li + dissolution from the ceramic and therefore lead to a lower interfacial resistance. [ 65 ] Therefore, the superiority of PPC as an interfacial layer lies not only in its homogenous nature but also in its unique reaction mechanism with Li, which should be considered in future design of dendrite‐proof interphases. Interestingly, we notice that after cycling the cell, the impedance decreases further to ≈14 Ω cm 2 , such a value is even smaller than the pure inorganic Au|LLZO interface.…”

Section: Resultsmentioning

confidence: 99%

Modulating Nanoinhomogeneity at Electrode–Solid Electrolyte Interfaces for Dendrite‐Proof Solid‐State Batteries and Long‐Life Memristors

Yang

et al. 2021

Advanced Energy Materials

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Dendrite penetration in ceramic lithium conductors severely constrains the development of solid‐state batteries (SSBs) while its nanoscale origin remains unelucidated. An in situ nanoscopic electrochemical characterization technique is developed based on conductive‐atomic force microscopy (c‐AFM) to reveal the local dendrite growth kinetics. Using Li7La3Zr2O12 (LLZO) as a model system, significant local inhomogeneity is observed with a hundredfold decrease in the dendrite triggering bias at grain boundaries compared with that at grain interiors. The origin of the local weakening is assigned to the nanoscale variation of elastic modulus and lithium flux detouring. An ionic‐conductive polymeric homogenizing layer is designed which achieves a high critical current density of 1.8 mA cm–2 and a low interfacial resistance of 14 Ω cm2. Practical SSBs based on LiFePO4 cathodes can be stably cycled over 300 times. Beyond this, highly reversible electrochemical dendrite healing in LLZO is discovered using the c‐AFM electrode, based on which a model memristor with a high on/off ratio of ≈105 is demonstrated for >200 cycles. This work not only provides a novel tool to investigate and design interfaces in SSBs but also offers opportunities for solid electrolytes beyond energy applications.

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Section: Resultsmentioning

confidence: 99%

Modulating Nanoinhomogeneity at Electrode–Solid Electrolyte Interfaces for Dendrite‐Proof Solid‐State Batteries and Long‐Life Memristors

Yang

et al. 2021

Advanced Energy Materials

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“…exchange current density) as shown for LE/SE interfaces [49]. Additionally, scanning electron microscopy (SEM) is an important technique to identify structure and morphology of the interface [66]. PE/SE interface properties are strongly influenced by processing parameters.…”

Section: Solid/polymer Interfacesmentioning

confidence: 99%

“…Besides the processing parameters, the use of a plasticizer in the PE is another approach to lower the PE/ SE interface resistance. Using a NASICON-type glass ceramic and a spray-coated PEO 16 :LiTf, Chen et al showed that the PE/SE interface resistance can be reduced to virtually zero by adding a small amount of the DMC plasticizer ( ≈ 5 wt% ) [66]. Adding DMC was assumed to facilitate the Li + ion transport near the ceramic interface and the Li + ion dissolution from PEO.…”

Section: Solid/polymer Interfacesmentioning

confidence: 99%

From Liquid- to Solid-State Batteries: Ion Transfer Kinetics of Heteroionic Interfaces

Weiß

Simon

Busche

et al. 2020

Electrochem. Energ. Rev.

130

109

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Hybrid battery cells combining liquid electrolytes (LEs) with inorganic solid electrolyte (SE) separators or different SEs and polymer electrolytes (PEs), respectively, are developed to solve the issues of single-electrolyte cells. Among the issues that can be solved are detrimental shuttle effects, decomposition reactions between the electrolyte and the electrodes, and dendrite propagation. However, the introduction of new interfaces by contacting different ionic conductors leads to other problems, which cannot be neglected before commercialization is possible. The interfaces between the different types of ionic conductors (LE/SE and PE/SE) often result in significant charge-transfer resistances, which increase the internal resistance considerably. This review highlights studies evaluating the interfacial resistances and activation barriers in such systems to present an overview of the issues still hampering hybrid battery systems. The interfaces between different SEs in hybrid all-solid-state batteries (SSBs) are considered as well. In addition, a short summary of physicochemical models describing heteroionic interfaces-interfaces between two different ion conductors-is given in an attempt to explain high interface resistances. In doing so, we hope to inspire future work on the crucial topic of interface optimization toward better SSBs.

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“… 55 For SPEs with a lower concentration, R ct could not be properly extracted below 60 °C due to the low SPE conductivity inducing strong frequency superposition of the interfacial and bulk contributions. Interestingly, despite using a quite similar SPE/CE combination [PEO/LiCF 3 SO 3 (EO/Li = 16, x = 1.3 M) and Oh ], Chen et al 50 observed a disruption in their Arrhenius plot of R ct with an activation energy that doubles below the PEO melting temperature T m (from 0.36 eV for T > T m up to 0.81 eV for T < T m ), while their R ct values are similar to ours for T > T m (42 Ω·cm 2 at 70 °C compared to our value of 38 Ω·cm 2 for PEO/LiTFSI-1.7M/ Oh ).…”

Section: Methodologies Results and Discussionmentioning

confidence: 99%

Electrochemical Impedance Spectroscopy of PEO-LATP Model Multilayers: Ionic Charge Transport and Transfer

Isaac

Mangani

Devaux

et al. 2022

ACS Appl. Mater. Interfaces

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Solid-state batteries are seen as a possible revolutionary technology, with increased safety and energy density compared to their liquid-electrolyte-based counterparts. Composite polymer/ceramic electrolytes are candidates of interest to develop a reliable solid-state battery due to the potential synergy between the organic (softness ensuring good interfaces) and inorganic (high ionic transport) material properties. Multilayers made of a polymer/ceramic/polymer assembly are model composite electrolytes to investigate ionic charge transport and transfer. Here, multilayer systems are thoroughly studied by electrochemical impedance spectroscopy (EIS) using poly(ethylene oxide) (PEO)-based polymer electrolytes and a NaSICON-based ceramic electrolyte. The EIS methodology allows the decomposition of the total polarization resistance ( R p ) of the multilayer cell as being the sum of bulk electrolyte (migration, R el ), interfacial charge transfer ( R ct ), and diffusion resistance ( R dif ), i.e., R p = R el + R ct + R dif . The phenomena associated with R el , R ct , and R dif are well decoupled in frequencies, and none of the contributions is blocking for ionic transport. In addition, straightforward models to deduce R el , R dif , and t + (cationic transference number) of the multilayer based on the transport properties of the polymer and ceramic electrolytes are proposed. A kinetic model based on the Butler–Volmer framework is also presented to model R ct and its dependency with the polymer electrolyte salt concentration ( C Li + ). Interestingly, the polymer/ceramic interfacial capacitance is found to be independent of C Li + .

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Determining and Minimizing Resistance for Ion Transport at the Polymer/Ceramic Electrolyte Interface

Cited by 57 publications

References 40 publications

Modulating Nanoinhomogeneity at Electrode–Solid Electrolyte Interfaces for Dendrite‐Proof Solid‐State Batteries and Long‐Life Memristors

Modulating Nanoinhomogeneity at Electrode–Solid Electrolyte Interfaces for Dendrite‐Proof Solid‐State Batteries and Long‐Life Memristors

From Liquid- to Solid-State Batteries: Ion Transfer Kinetics of Heteroionic Interfaces

Electrochemical Impedance Spectroscopy of PEO-LATP Model Multilayers: Ionic Charge Transport and Transfer

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