Defect chemistry and electrical properties of garnet-type Li7La3Zr2O12

Zhan, Xiaowen; Lai, Shen; Gobet, Mallory; Greenbaum, Steven; Shirpour, Mona

doi:10.1039/c7cp06768b

Cited by 76 publications

(42 citation statements)

References 59 publications

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“…For example, the lattice size of Ga‐doped LZO is different from that of Al‐doped LZO, whereas their Li‐ion conductivities are almost in the same level. We previously reported a constructive effect of oxygen vacancies on Li‐ion conductivity of the cubic Li 7 La 3 Zr 2 O 12 , where we ascribed it mainly to the trapping between electron‐holes and lithium ion vacancies . However, such trapping should only be considered at lower temperatures, as the associated pairs will be released at elevated temperatures, that is, 200‐600°C in this study.…”

Section: Resultssupporting

confidence: 77%

“…We previously reported a constructive effect of oxygen vacancies on Li-ion conductivity of the cubic Li 7 La 3 Zr 2 O 12 , where we ascribed it mainly to the trapping between electron-holes and lithium ion vacancies. 28 However, such trapping should only be considered at lower temperatures, 29,30 as the associated pairs will be released at elevated temperatures, that is, 200-600°C in this study. Further structure analyses (i.e., via DFT modeling, Li NMR, and Neutron diffraction) are necessary to fully understand the role of oxygen vacancies in determining the Li-ion mobility.…”

Section: Transport Properties and Defect Processmentioning

confidence: 99%

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Nonstoichiometry and Li‐ion transport in lithium zirconate: The role of oxygen vacancies

2018

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Understanding Li‐ion migration mechanisms and enhancing Li‐ion transport in Li2ZrO3 (LZO) is important to its role as solid absorbent for reversible CO2 capture at elevated temperatures, as ceramic breeder in nuclear reactors, and as electrode coating in high‐voltage lithium‐ion batteries (LIBs). Although defect engineering is an effective way to tune the properties of ceramics, the defect structure of LZO is largely unknown. This study reports the defect structure and electrical properties of undoped LZO and a series of cation‐doped LZOs: (i) depending on their charge states, cation dopants can control the oxygen vacancy concentration in doped LZOs; (ii) the doped LZOs with higher oxygen vacancy concentrations exhibit better Li+ conductivity, and consequently faster high‐temperature CO2 absorption. In fact, the Fe (II)‐doped LZO shows the highest Li‐ion conductivity reported for LZOs, reaching 3.3 mS/cm at ~300°C that is more than 1 order of magnitude higher than that of the undoped LZO.

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Section: Resultssupporting

confidence: 77%

Section: Transport Properties and Defect Processmentioning

confidence: 99%

Nonstoichiometry and Li‐ion transport in lithium zirconate: The role of oxygen vacancies

2018

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“…[4,5,28,[32][33][34] However, the grain boundary conductivity of ceramic SSEs is significantly lower than that of the bulk. [37] Furthermore, electrode/electrolyte interfacial resistances are typically high because of the poor solid-solid contacts at such interfaces. 26 O 11.79 was reported to be~0.25 mS cm À 1 , while the grain boundary conductivity was determined to be lower than 10 À 8 S cm À 1 .…”

Section: Introductionmentioning

confidence: 99%

A Ceramic‐PVDF Composite Membrane with Modified Interfaces as an Ion‐Conducting Electrolyte for Solid‐State Lithium‐Ion Batteries Operating at Room Temperature

Kwok

et al. 2018

ChemElectroChem

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Solid-state batteries hold great promise because of their safety and high projected energy density. However, the sizeable interfacial resistance between the electrodes and the electrolyte of such batteries is a significant bottleneck in the development of this technology. In this work, we develop a Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 (LLZTO) and polyvinylidene fluoride (PVDF) solid-state composite membrane characterized by high conductivity, tensile strength, and flexibility as well as low impedance if interfacially modified by a minute amount of liquid electrolyte. A solid-state lithium-ion battery using this electrolyte with LiFePO 4 and Li as electrodes delivers excellent rate capability and cycling stability at room temperature. In particular, the battery shows an initial discharge capacity of 155 mAh g À1 and, after 100 cycles at 1C, of 145 mAh g À1 . Even at 4C, the discharge capacity is 96 mAh g À1 . Our study suggests that the interfacially modified LLZTO-PVDF membrane is a promising electrolyte for solid-state lithium-ion batteries.

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“…Besides, the oxygen vacancies play an important role in defect equilibria and phase formation of LLZO. In the work of Shirpour et al ,. they prepared un‐doped LLZO compounds by the traditional solid‐state method.…”

Section: Lithium‐ion Batteriesmentioning

confidence: 99%

Zirconium‐Based Materials for Electrochemical Energy Storage

Wang

Xiao

et al. 2019

ChemElectroChem

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materials have emerged as momentous candidates for next-generation batteries and supercapacitors, owing to their distinctive chemical and physical properties. For instance, garnet-Li 7 La 3 Zr 2 O 12 can be used as an electrolyte for solid-state lithium-ion batteries, which delivers high bulk lithium-ion conductivities in the range of 4.0 × 10 À 4 S cm À 1 at 20°C. We provide a comprehensive review of up-to-date research progress in zirconium-based materials. The most recent advances in the field of zirconium-based electrodes, electrolytes, coatings, and separator materials for rechargeable batteries and supercapacitors are summarized. Moreover, the electrochemical performances in terms of the specific capacity, rate capability, and cycling stability of zirconium-based materials are reported. Finally, we discuss the limitations and challenges of zirconium-based energy storage materials, followed by their present status and prospects for future research. We believe that this Review will be helpful for researchers and scientists who are seeking promising materials for batteries and supercapacitors.

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Defect chemistry and electrical properties of garnet-type Li₇La₃Zr₂O₁₂

Cited by 76 publications

References 59 publications

Nonstoichiometry and Li‐ion transport in lithium zirconate: The role of oxygen vacancies

Nonstoichiometry and Li‐ion transport in lithium zirconate: The role of oxygen vacancies

A Ceramic‐PVDF Composite Membrane with Modified Interfaces as an Ion‐Conducting Electrolyte for Solid‐State Lithium‐Ion Batteries Operating at Room Temperature

Zirconium‐Based Materials for Electrochemical Energy Storage

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