A microcontact impedance study on NASICON-type Li1+xAlxTi2−x(PO4)3(0 ≤ x ≤ 0.5) single crystals

Rettenwander, Daniel; Welzl, Andreas; Pristat, Sylke; Tietz, Frank; Taibl, Stefanie; Redhammer, Günther J.; Fleig, Jürgen

doi:10.1039/c5ta08545d

Cited by 107 publications

(82 citation statements)

References 24 publications

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“…[74] H.E. Compared with the LTP, an increased concentration of Li + will lead to the migration of Li + occupying M1 (6b) sites toward the nearest M3 (36f) position in the LATP, opening fast-conducting pathways, [79,80] as has also been reported for the LAGP. Like the LZP, the conductivity of the LTP and LGP is also on the order of 10 −5 -10 −6 S cm −1 , [76,77] far lower than the conductivity of liquid electrolytes (≈10 −2 S cm −1 ).…”

Section: Nasicon-type Ssesmentioning

confidence: 72%

“…For the interfacial incompatibility, the discussion is focused on the dynamic characterization of the electrode/SSE interfaces, the origin and evolution of the interfacial resistance, and interface engineering to minimize the interfacial resistance. Compared with the LTP, an increased concentration of Li + will lead to the migration of Li + occupying M1 (6b) sites toward the nearest M3 (36f) position in the LATP, opening fast-conducting pathways, [79,80] as has also been reported for the LAGP. Stress generation, stress evolution during battery cycling, stress measurement/simulation, and ways to alleviate the stresses are outlined in detail.…”

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confidence: 77%

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Interfacial Incompatibility and Internal Stresses in All‐Solid‐State Lithium Ion Batteries

Liu

et al. 2019

Advanced Energy Materials

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The continuous depletion of fossil fuels, the increase of oil prices, and the need to decrease CO 2 emissions have stimulated intensive research on developing alternative renewable and clean energy sources. [1] Among these alternative energy sources, rechargeable Li-ion batteries (LIBs) are one of the promising candidates. To date, the LIBs basically consisting of a positive electrode (cathode), an electrolyte, and a negative electrode (anode) have widespread applications, such as portable electronic devices, pure electric vehicles (PEVs), and hybrid electric vehicles (HEVs). [2] The state-of-the-art electrolytes are usually the lithium salts (LiPF 6 , LiBF 4 , and LiCF 3 SO 3 ) dissolved in organic solvents, i.e., ethylene carbonate, propylene carbonate, polyethylene oxide, and dimethyl carbonate, [3] which exhibit excellent wetting of the electrodes and produce a fast transfer of Li + ions upon charging and discharging. However, they suffer from flammability, poor electrochemical stability, limited temperature range of operation, and low power density. [4] There is an ever-increasing demand for batteries with a higher energy and power density, although current LIBs offer volumetric and gravimetric energy densities up to 770 Wh L −1 and 260 Wh kg −1 , respectively. [5] To improve the energy/power density of LIBs, one way is to adopt high-potential cathode materials such as LiNi 0.5 Mn 1.5 O 4 (LNMO). The high-voltage plateau of LNMO (≈4.7 V vs Li/Li + ) makes its energy density 20-30% higher than the energy density of commercial LiCoO 2 and LiFePO 4 . [6] However, successful commercialization of the LNMO is restricted in high-energy LIBs due to electrolyte decomposition and side reaction of the cathodes and liquid electrolytes when operating at high voltages. [7,8] The other way to improve the energy/power density is to replace the conventional graphite anode with Li metal. The Li metal, with a low anode potential (−3.04 V vs standard hydrogen electrode) and high specific capacity (3862 mAh g −1 for the Li anode versus 372 mAh g −1 for the graphite anode), [9][10][11] has been considered as the "Holy Grail" of battery technologies. When paired with sulfur and oxygen, the theoretical energy density of Li-S (≈2567 Wh kg −1 ) and Li-O 2 (≈3505 Wh kg −1 ) batteries is far higher than the theoretical energy density of conventional LIBs (≈387 Wh kg −1 ). [12][13][14][15] When Li metal approaches the liquid electrolytes, however, unstable Li/electrolyte interface Rechargeable Li-ion batteries (LIBs) are electrochemical storage device widely applied in electric vehicles, mobile electronic devices, etc. However, traditional LIBs containing liquid electrolytes suffer from flammability, poor electrochemical stability, and limited operational temperature range. Replacement of the liquid electrolytes with inorganic solid-state electrolytes (SSEs) would solve this problem. However, several critical issues, such as poor interfacial compatibility, low ionic conductivity at ambient temperatures, etc., need to be surmounted befor...

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Section: Nasicon-type Ssesmentioning

confidence: 72%

mentioning

confidence: 77%

Interfacial Incompatibility and Internal Stresses in All‐Solid‐State Lithium Ion Batteries

Liu

et al. 2019

Advanced Energy Materials

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“…The electrochemical characterization of NSP was carried out by electrical impedance spectroscopy according to ref (14). All impedance measurements were performed between RT and 200 °C in a tube furnace using an Alpha-A High Resolution dielectric analyzer with a ZG-2 interface (Novocontrol, Germany) in the frequency range from 3 × 10 6 Hz to 10 2 Hz with a voltage amplitude of 100 mV.…”

Section: Methodsmentioning

confidence: 99%

“…Very recently, we used the same setup with microelectrodes to successfully investigate electrical bulk properties of Li 1+ x Al x Ti 2– x (PO 4 ) 3 (LATP) single crystals. 14 …”

Section: Introductionmentioning

confidence: 99%

Arrhenius Behavior of the Bulk Na-Ion Conductivity in Na₃Sc₂(PO₄)₃ Single Crystals Observed by Microcontact Impedance Spectroscopy

et al. 2018

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NASICON-based solid electrolytes with exceptionally high Na-ion conductivities are considered to enable future all solid-state Na-ion battery technologies. Despite 40 years of research the interrelation between crystal structure and Na-ion conduction is still controversially discussed and far from being fully understood. In this study, microcontact impedance spectroscopy combined with single crystal X-ray diffraction, and differential scanning calorimetry is applied to tackle the question how bulk Na-ion conductivity σbulk of sub-mm-sized flux grown Na3Sc2(PO4)3 (NSP) single crystals is influenced by supposed phase changes (α, β, and γ phase) discussed in literature. Although we found a smooth structural change at around 140 °C, which we assign to the β → γ phase transition, our conductivity data follow a single Arrhenius law from room temperature (RT) up to 220 °C. Obviously, the structural change, being mainly related to decreasing Na-ion ordering with increasing temperature, does not cause any jumps in Na-ion conductivity or any discontinuities in activation energies Ea. Bulk ion dynamics in NSP have so far rarely been documented; here, under ambient conditions, σbulk turned out to be as high as 3 × 10–4 S cm–1 at RT (Ea, bulk = 0.39 eV) when directly measured with microcontacts for individual small single crystals.

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“…Substituting Al for Ti in LTP forms Li 1+x Al x Ti 2−x (PO 4 ) 3 (LATP). This doped composite has higher ionic conductivity, lower sintering temperature, and higher crystalline stability than the un-doped one [19][20][21] and is also stable against moisture [22,23].…”

Section: Introductionmentioning

confidence: 97%

The Fabrication of All-Solid-State Lithium-Ion Batteries via Spark Plasma Sintering

Wei

Rechtin

Olevsky

2017

Metals

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Spark plasma sintering (SPS) has been successfully used to produce all-solid-state lithium-ion batteries (ASSLibs). Both regular and functionally graded electrodes are implemented into novel three-layer and five-layer battery designs together with solid-state composite electrolyte. The electrical capacities and the conductivities of the SPS-processed ASSLibs are evaluated using the galvanostatic charge-discharge test. Experimental results have shown that, compared to the three-layer battery, the five-layer battery is able to improve energy and power densities. Scanning electron microscopy (SEM) is employed to examine the microstructures of the batteries especially at the electrode-electrolyte interfaces. It reveals that the functionally graded structure can eliminate the delamination effect at the electrode-electrolyte interface and, therefore, retains better performance.

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A microcontact impedance study on NASICON-type Li_1+xAl_xTi_2−x(PO₄)₃(0 ≤ x ≤ 0.5) single crystals

Cited by 107 publications

References 24 publications

Interfacial Incompatibility and Internal Stresses in All‐Solid‐State Lithium Ion Batteries

Interfacial Incompatibility and Internal Stresses in All‐Solid‐State Lithium Ion Batteries

Arrhenius Behavior of the Bulk Na-Ion Conductivity in Na₃Sc₂(PO₄)₃ Single Crystals Observed by Microcontact Impedance Spectroscopy

The Fabrication of All-Solid-State Lithium-Ion Batteries via Spark Plasma Sintering

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A microcontact impedance study on NASICON-type Li1+xAlxTi2−x(PO4)3(0 ≤ x ≤ 0.5) single crystals

Cited by 107 publications

References 24 publications

Interfacial Incompatibility and Internal Stresses in All‐Solid‐State Lithium Ion Batteries

Interfacial Incompatibility and Internal Stresses in All‐Solid‐State Lithium Ion Batteries

Arrhenius Behavior of the Bulk Na-Ion Conductivity in Na3Sc2(PO4)3 Single Crystals Observed by Microcontact Impedance Spectroscopy

The Fabrication of All-Solid-State Lithium-Ion Batteries via Spark Plasma Sintering

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A microcontact impedance study on NASICON-type Li_1+xAl_xTi_2−x(PO₄)₃(0 ≤ x ≤ 0.5) single crystals

Arrhenius Behavior of the Bulk Na-Ion Conductivity in Na₃Sc₂(PO₄)₃ Single Crystals Observed by Microcontact Impedance Spectroscopy