Electrochemical Impedance Spectroscopy for All‐Solid‐State Batteries: Theory, Methods and Future Outlook

Vadhva, Pooja; Ji, Hu; Johnson, Melissa; Stocker, Richard; Braglia, Michele; Brett, Dan J. L.; Rettie, Alexander J. E.

doi:10.1002/celc.202100108

Cited by 273 publications

(206 citation statements)

References 188 publications

(204 reference statements)

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“…The electronic conductivity was measured via direct current (DC) polarization technique ( Boulineau et al, 2012 ; Zhang et al, 2020 ; Vadhva et al, 2021 ). The Ni/Li 6 PS 5 Cl/Ni symmetrical cells were prepared in a similar way as previously mentioned.…”

Section: Methodsmentioning

confidence: 99%

Ionic and Electronic Conductivities of Lithium Argyrodite Li6PS5Cl Electrolytes Prepared via Wet Milling and Post-Annealing

et al. 2021

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Lithium argyrodite Li6PS5Cl powders are synthesized from Li2S, P2S5, and LiCl via wet milling and post-annealing at 500°C for 4 h. Organic solvents such as hexane, heptane, toluene, and xylene are used during the wet milling process. The phase evolution, powder morphology, and electrochemical properties of the wet-milled Li6PS5Cl powders and electrolytes are studied. Compared to dry milling, the processing time is significantly reduced via wet milling. The nature of the solvent does not affect the ionic conductivity significantly; however, the electronic conductivity changes noticeably. The study indicates that xylene and toluene can be used for the wet milling to synthesize Li6PS5Cl electrolyte powder with low electronic and comparable ionic conductivities. The all-solid-state cell with the xylene-processed Li6PS5Cl electrolyte exhibits the highest discharge capacity of 192.4 mAh·g−1 and a Coulombic efficiency of 81.3% for the first discharge cycle.

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Section: Methodsmentioning

confidence: 99%

Ionic and Electronic Conductivities of Lithium Argyrodite Li6PS5Cl Electrolytes Prepared via Wet Milling and Post-Annealing

et al. 2021

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“…At 60 °C, the 3(RQ) equivalent circuit model (Table S7, Supporting Information) could be simplified into the RQ model (Table S8, Supporting Information) owing to the overlapping time constants of the electrochemical processes at high temperature. [ 32 ] Therefore, the interface resistance, R int , was defined as the sum of R HF , R MF , and R LF . It was found that the R int of PAQS@CNT decreased from 1487 Ω at 25 °C to 453 Ω at 60 °C, however, still about five times as that of PTTCA@CNT (88.3 Ω).…”

Section: Resultsmentioning

confidence: 99%

Room‐Temperature All‐Solid‐State Lithium–Organic Batteries Based on Sulfide Electrolytes and Organodisulfide Cathodes

Yang

Wang

et al. 2021

Advanced Energy Materials

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All‐solid‐state design is effective to address the challenges of Lithium –organic batteries, such as the dissolution of organic electrode materials (OEMs) and the safety of the Li anode. However, previous attempts, based on carbonyl‐type OEMs failed to achieve acceptable electrochemical performance in room‐temperature all‐solid‐state Li batteries (ASSLBs). Herein, the authors report the first organodisulfide cathode, poly(trithiocyanuric acid) (PTTCA), for ASSLBs. By compositing with carbon nanotubes to enhance the electronic conductivity and using the sulfide electrolyte, Li7P3S11, to build an electrochemically favorable interface, PTTCA demonstrates an electrochemical performance superior to all the OEMs reported so far in ASSLBs at room temperature, including a reversible capacity of 410 mAh g−1, an energy density of 767 Wh kg−1, and a capacity retention of 83% after 100 cycles. It is believed that this work provides new orientation and insights for the further development of both ASSLBs and OEMs.

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“…The two semicircles in the high frequency region and medium frequency region correspond to the charge transfer resistance at cathode interfaces (R c ) and anode interfaces, respectively. [13] The equivalent circuit in Figure S19, Supporting Information, is applied for the fitting processes. The measured Nyquist plots and the simulated results are provided in 6, 32.4, 24, 34.2, 20.8, and 22.6 Ω, respectively, and the corresponding CAM mass fraction value is 50, 50, 60, 60, 70, and 70 wt%.…”

Section: Electrochemical Kinetic Evaluations Of Assbsmentioning

confidence: 99%

Revealing the Design Principles of Ni‐Rich Cathodes for All‐Solid‐State Batteries

Jiang

Zhu

Huang

et al. 2022

Advanced Energy Materials

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The highly percolated ionic/electronic pathways are the primary factors enabling the fast kinetics in electrochemical systems. [4] The composite cathodes microstructure engineering plays a critical role in building the ionic/electronic conductive channels. [5] This composite cathode microstructure can be regulated by the main components of cathode active materials (CAM) and SEs. Distinguished with the good wettability of liquid electrolytes, the rigid SEs particles lead to the insufficient contact area between CAM and SEs, leading to reducing active surfaces. [4a,6] For that reason, it is especially important for the SEs mass fraction to be optimized for effective ionic transport pathways in composite cathodes. [7] However, the achievement of both fast ionic and electronic conduction pathways is extremely difficult because the electronic transport networks are supported only by the interconnected CAM particles. This leads to the importance of composite cathode microstructure engineering. [8] There are several key factors of CAM particle size, CAM-to-SEs particle size ratio, and SEs mass fraction that have great impacts on CAM utilization and electrochemical performance. [5a,6,9] However, the effects on the electrode design of these factors are not comprehensively studied, especially on their correlations between these aspects.Herein, we studied the critical effects in terms of the particle size distribution and composition of the composite cathodes on the electrochemical properties. Two advanced popular materials of Ni-rich layered oxides LiNi 0.5 Co 0.2 Mn 0.3 O 2 (NCM) with different particle sizes and sulfide fast ion conductors Li 9.54 Si 1.74 P 1.44 S 11.7 Cl 0.3 (LSPSC) are selected to reveal these effects. The cathode composites are prepared by pressing NCM and LSPSC into a thick pellet with different component ratios. Optimized electrochemical performance suggests an approximate positive relationship between CAM particle size and electrode component ratio. The interfacial impedance changes raised from the varying electrode microstructure were also revealed by electrochemical impedance spectroscopy (EIS) techniques. In the optimized composite cathodes, effective ionic and electronic percolation networks building on highly interconnected CAM particles and highly interconnected SEs particles were demonstrated by cross-section analysis of the composite electrode. As is proved by the direct current (DC) polarization techniques, a compromise between the ionic conductivities and electronic conductivities in composite cathodes Electrode microstructure is one of the primary factors determining the electrochemical properties of all-solid-state batteries (ASSBs). However, the key principles of electrode design to realize fast ionic/electronic transport pathways are not well elucidated. Herein, the correlation between electrode microstructure and electrochemical behaviors is studied through different electrode design in terms of energy-density-related electrode composition and Ni-rich layered oxides particle siz...

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Electrochemical Impedance Spectroscopy for All‐Solid‐State Batteries: Theory, Methods and Future Outlook

Cited by 273 publications

References 188 publications

Ionic and Electronic Conductivities of Lithium Argyrodite Li6PS5Cl Electrolytes Prepared via Wet Milling and Post-Annealing

Ionic and Electronic Conductivities of Lithium Argyrodite Li6PS5Cl Electrolytes Prepared via Wet Milling and Post-Annealing

Room‐Temperature All‐Solid‐State Lithium–Organic Batteries Based on Sulfide Electrolytes and Organodisulfide Cathodes

Revealing the Design Principles of Ni‐Rich Cathodes for All‐Solid‐State Batteries

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