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Boosting lithium ion conductivity of antiperovskite solid electrolyte by potassium ions substitution for cation clusters.

ABSTRACT: Solid-state electrolytes with high ionic conductivities are crucial for the development of all-solid-state lithium batteries, and there is a strong correlation between the ionic conductivities and underlying lattice structures of solid-state electrolytes. Here, we report a lattice manipulation method of replacing [Li₂OH]⁺ clusters with potassium ions in antiperovskite solid-state electrolyte (Li₂OH)_0.99K_0.01Cl, which leads to a remarkable increase in ionic conductivity (4.5 × 10^‒3 mS cm^‒1, 25 °C). Mechanistic analysis indicates that the lattice manipulation method leads to the stabilization of the cubic phase and lattice contraction for the antiperovskite, and causes significant changes in Li-ion transport trajectories and migration barriers. Also, the Li||LiFePO₄ all-solid-state battery (excess Li and loading of 1.78 mg cm^‒2 for LiFePO₄) employing (Li₂OH)_0.99K_0.01Cl electrolyte delivers a specific capacity of 116.4 mAh g^‒1 at the 150th cycle with a capacity retention of 96.1% at 80 mA g^‒1 and 120 °C, which indicates potential application prospects of antiperovskite electrolyte in all-solid-state lithium batteries.

SUBMITTER: Gao L

PROVIDER: S-EPMC10603071 | biostudies-literature | 2023 Oct

REPOSITORIES: biostudies-literature

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Boosting lithium ion conductivity of antiperovskite solid electrolyte by potassium ions substitution for cation clusters.

Gao Lei L Zhang Xinyu X Zhu Jinlong J Han Songbai S Zhang Hao H Wang Liping L Zhao Ruo R Gao Song S Li Shuai S Wang Yonggang Y Huang Dubin D Zhao Yusheng Y Zou Ruqiang R

Nature communications 20231026 1

Solid-state electrolytes with high ionic conductivities are crucial for the development of all-solid-state lithium batteries, and there is a strong correlation between the ionic conductivities and underlying lattice structures of solid-state electrolytes. Here, we report a lattice manipulation method of replacing [Li2OH]+ clusters with potassium ions in antiperovskite solid-state electrolyte (Li2OH)0.99K0.01Cl, which leads to a remarkable in ...[more]

PMID: 37884502

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Project description:ConspectusResearch at historically black colleges and universities (HBCUs) started with humble beginnings by G. W. Carver at Tuskegee Institute AL, the nation's first HBCU. He is now remembered as the man who transformed one crop, peanuts to more than 300 useful products such as food, beverages, medicines, cosmetics, and chemicals. However, research was not the focus of most of the newly founded HBCUs to provide, primarily, liberal arts education and training in agriculture for the black minority. HBCUs remained segregated, lacking facilities such as libraries and scientific/research equipment comparable to those at traditionally white institutions. While the Civil Rights Act of 1964 heralded the dawn of "equal opportunity" and progressive desegregation in the South, many public HBCUs had to close or merge with white institutions due to loss of funding and/or students. In order to remain competitive in enrollment and financial support of the best talents, HBCUs have been expanding their research and federal contracts by working in collaboration with research-intensive institutions and/or minority-serving institutions (MSIs). Albany State University (ASU), an HBCU with a great tradition of in-house and extramural undergraduate research, has partnered with the laboratory of Dr. John Miller at Brookhaven National Laboratory (BNL) to offer the best training and mentorship to our undergraduates. Students synthesized and performed conductivity measurements on a new generation of ion-pair salts. One of these constitutes, potentially, a nonaqueous electrolyte for the next generation of high-energy-density batteries owing to its electrochemical properties.The quest for rechargeable batteries with greater energy density and capable of shorter recharge time at the "pump" for electrical vehicles (EVs) is leading the development of electrolytes with higher ionic mobility and greater limiting conductivity. In order to achieve high energy density, it is vital for an electrolyte to be electrochemically stable while operating at high voltages.The development of a weakly coordinating anion/cation electrolyte for energy storage applications offers a challenge of technological significance. This class of electrolytes is advantageous for the investigation of electrode processes in low-polarity solvents. The improvement arises from the optimization of both ionic conductivity and solubility of the ion pair formed between a substituted tetra-arylphosphonium (TAPR) cation and tetrakis-fluoroarylborate (TFAB), a weakly coordinating anion. The chemical "push-pull" between cation and anion affords a highly conducting ion pair in low-polarity solvents such as tetrahydrofuran (THF) and tert-butyl methyl ether (TBME). The limiting conductivity value of the salt, namely, tetra-p-methoxy-phenylphosphonium-tetrakis(pentafluorophenyl)borate or TAPR/TFAB (R = p-OCH3), is in the range of lithium hexafluorophosphate (LiPF6) used in lithium-ion batteries (LIBs). This TAPR/TFAB salt can improve the efficiency and stability of batteries over those of existing and commonly used electrolytes by optimizing the conductivity tailored to the redox-active molecules. LiPF6 dissolved in carbonate solvents is unstable with high-voltage electrodes that are required to achieve greater energy density. In contrast, the TAPOMe/TFAB salt is stable and has a good solubility profile in low-polarity solvents given its relatively great size. And it constitutes a low-cost supporting electrolyte capable of bringing nonaqueous energy storage devices to compete with existing technologies.

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Boosting lithium ion conductivity of antiperovskite solid electrolyte by potassium ions substitution for cation clusters.

Publications

Boosting lithium ion conductivity of antiperovskite solid electrolyte by potassium ions substitution for cation clusters.

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