Prospects of halide-based all-solid-state batteries: From material design to practical application

Wang, Changhong; Liang, Jianwen; Kim, Jung Tae; Sun, Xueliang

doi:10.1126/sciadv.adc9516

Cited by 158 publications

(123 citation statements)

References 117 publications

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“…In 2018, Asano et al reported that the ternary halides Li 3 YCl 6 and Li 3 YBr 6 have ionic conductivities of ∼1 × 10 –3 S/cm and showcased ASSBs with Coulombic efficiencies of 94% using (uncoated) LiCoO 2 as the active material in the cathode composite. Since then, the material family Li 3 M(III)X 6 (M(III) = Y, In, Sc, lanthanides; X = Cl, Br, I)) and other halide solid electrolytes have gained renewed interest in the scientific community due to their favorable combination of ionic conductivity (∼mS/cm) and high-voltage cathode compatibility. − More recently, Zhou et al reached a milestone in the development of ASSBs using a Li 2 In x Sc 0.66– x Cl 4 electrolyte. The ASSB with this electrolyte possessing a 2 × 10 –3 S/cm ionic conductivity and a 4.7 × 10 –10 S/cm electronic conductivity, reached 3000 cycles at 80% capacity retention when cycled between 2.8–4.3 V vs Li/Li + using LiNi 0.85 Co 0.1 Mn 0.05 O 2 as the cathode (6.21 mg/cm 2 ) at 3C .…”

Section: Introductionmentioning

confidence: 99%

Investigation of Structure, Ionic Conductivity, and Electrochemical Stability of Halogen Substitution in Solid-State Ion Conductor Li₃YBr_xCl_6–x

Maas

Zhao

et al. 2022

J. Phys. Chem. C

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Li 3 YX 6 (X = Cl, Br) materials are Li-ion conductors that can be used as solid electrolytes in all solid-state batteries. Solid electrolytes ideally have high ionic conductivity and (electro)chemical compatibility with the electrodes. It was proven that introducing Br to Li 3 YCl 6 increases ionic conductivity but, according to thermodynamic calculations, should also reduce oxidative stability. In this paper, the trade-off between ionic conductivity and electrochemical stability in Li 3 YBr x Cl 6−x halogensubstituted compounds is investigated. The compositions of Li 3 YBr 1.5 Cl 4.5 and Li 3 YBr 4.5 Cl 1.5 are reported for the first time, along with a consistent analysis of the whole Li 3 YBr x Cl 6−x (x = 0− 6) tie-line. The results show that, while Br-rich materials are more conductive (5.36 × 10 −3 S/cm at 30 °C for x = 4.5), the oxidative stability is lower (∼3 V compared to ∼3.5 V). Small Br content (x = 1.5) does not affect oxidative stability but substantially increases ionic conductivity compared to pristine Li 3 YCl 6 (2.1 compared to 0.049 × 10 −3 S/cm at 30 °C). This work highlights that optimization of substitutions in the anion framework provide prolific and rational avenues for tailoring the properties of solid electrolytes.

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Section: Introductionmentioning

confidence: 99%

Investigation of Structure, Ionic Conductivity, and Electrochemical Stability of Halogen Substitution in Solid-State Ion Conductor Li₃YBr_xCl_6–x

Maas

Zhao

et al. 2022

J. Phys. Chem. C

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“…Due to the wellknown instability of the halide SE against metal, we tested these cathode composites in cells that used a bilayer separator with Li6PS5Cl and Li3InCl6 layers against In/LiIn as an anode. 52,53 Moreover, in this configuration we can truly focus on the effect of the cathode additives, namely the Li3InCl6|CP composites, on the performance of the cells. Figure 6b shows exemplary charge-discharge curves for the NMC622|Li3InCl6 catholyte, with an initial discharge capacity of 120 mAh/g that decays over the course of 30 cycles to ca.…”

Section: Figure 1 Crystal Structure and Electron Microscopy Character...mentioning

confidence: 99%

Water-mediated synthesis of halide solid electrolyte and conducting polymer hybrid materials for all solid-state batteries

Nazmutdinova

Rosenbach

Schmidt

et al. 2023

Preprint

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Over the last decades, we have seen an increase in the number of new materials that can be incorporated into all-solid-state batteries (ASSBs). Halide solid electrolytes have attracted significant attention due to their superior stability against oxide-based cathode active materials when compared to sulfide-based solid electrolytes. Nonetheless, the dynamicity of interparticle contact during cycling in ASSBs hinders their stability and performance. Therefore, inactive materials such as electronically conductive additives and polymer binders are needed to compensate the contact-loss reducing the energy density of the resulting cells. Here, we present an aqueous approach for the preparation of halide solid electrolyte-conductive polymer hybrid composites with Li3InCl6 and poly(3,4-ethylendioxythiophene)/poly(styrene sulfonate) (PEDOT:PSS) in one-pot. The resulting composites combine the properties of a solid electrolyte with a conductive additive and a binder together with into a single hybrid material. Together with other analytical techniques, Kelvin Probe Force Microscopy (KPFM) imaging showed a successful synthesis of the hybrid materials and revealed that the conductive polymer (CP), namely PEDOT:PSS, is located at the surface/grain of the Li3InCl6. Upon incorporation of such composites in sulfide solid-state half-cells with lithium nickel manganese cobalt oxide (NMC) cathode active material (CAM) we observe an increase in the partial electronic transport of the catholytes with increasing CP content, which correlates an increase in the initial discharge capacities. This study sets the stage to explore the preparation of multi-functional catholytes without the necessity of organic solvents, extremely high temperatures or special environments.

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“…[96,114] However, the non-Li cations in HSSEs, such as Sc 3+ and In 3+ , have low abundance in the earth's crust and are expensive. [115] In addition to their abundance, extracting the metal halides from their earth crust minerals can cause severe environmental risks. The purification processes can be complex, which can further increase their cost.…”

Section: Costmentioning

confidence: 99%

Halide Solid‐State Electrolytes: Stability and Application for High Voltage All‐Solid‐State Li Batteries

Nikodimos

Hwang

2022

Advanced Energy Materials

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used in many batteries. Traditional Li-ion batteries have reached a point of development bottleneck due to their safety issues of the flammable liquid electrolytes and low energy density. [1,2] To meet the goal of manufacturing electronic vehicles, scientists are working on batteries that have a higher energy density and are safer. [3,4] All-solid-state Li batteries (ASSLBs), which are made up completely of solid components, are a promising candidate for future energy storage generation with better safety, [5][6][7][8] and higher energy density. [9][10][11] Solid electrolytes with good overall characteristics are critical for ASSLBs to be realized. [12] Several attempts have been undertaken in recent decades to build solid electrolytes with good Li + conductivity, such as polymer solid electrolytes, [13][14][15][16][17][18] sulfide solid electrolytes, [19][20][21] oxide solid electrolytes, [22][23][24][25][26][27][28] anti-perovskites, [29][30][31] and lithium phosphorous oxynitrides. [32][33][34][35][36] Oxide-based solid electrolytes, such as garnet and NASICON-type, have good chemical stability with cathode materials but are brittle and have a poor contact surface with the cathode, [37] and we may need to use a liquid electrolyte to improve interface wettability. [37][38][39][40] Considering their high Li + conductivity and ductility sulfide solid electrolytes have been extensively explored among the numerous types of solid electrolytes. [41][42][43][44][45] Li 10 GeP 2 S 12 (LGPS), for example, has a high ionic conductivity of more than 10 mS cm −1 , which is almost equivalent to those of the conventional liquid electrolytes. [43] On the other hand, sulfide-based solid electrolytes have poor hydrolysis stability, chemical instability issues with electrodes, and a narrow electrochemical window (ECW). [46][47][48] Sulfides are not chemically or electrochemically compatible with typical 4 V cathode active materials, [49,50] because they are oxidized at a low potential (≈2.5 V vs Li + /Li). [51][52][53] To solve these problems, particles of cathode active materials must be coated with chemically compatible, an ionically conductive, and electrically insulating material, [54] which leads to a myriad of new challenges. In this regard, numerous researchers have used several oxides as potential coating materials, such as

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Prospects of halide-based all-solid-state batteries: From material design to practical application

Cited by 158 publications

References 117 publications

Investigation of Structure, Ionic Conductivity, and Electrochemical Stability of Halogen Substitution in Solid-State Ion Conductor Li₃YBr_xCl_6–x

Investigation of Structure, Ionic Conductivity, and Electrochemical Stability of Halogen Substitution in Solid-State Ion Conductor Li₃YBr_xCl_6–x

Water-mediated synthesis of halide solid electrolyte and conducting polymer hybrid materials for all solid-state batteries

Halide Solid‐State Electrolytes: Stability and Application for High Voltage All‐Solid‐State Li Batteries

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Prospects of halide-based all-solid-state batteries: From material design to practical application

Cited by 158 publications

References 117 publications

Investigation of Structure, Ionic Conductivity, and Electrochemical Stability of Halogen Substitution in Solid-State Ion Conductor Li3YBrxCl6–x

Investigation of Structure, Ionic Conductivity, and Electrochemical Stability of Halogen Substitution in Solid-State Ion Conductor Li3YBrxCl6–x

Water-mediated synthesis of halide solid electrolyte and conducting polymer hybrid materials for all solid-state batteries

Halide Solid‐State Electrolytes: Stability and Application for High Voltage All‐Solid‐State Li Batteries

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Investigation of Structure, Ionic Conductivity, and Electrochemical Stability of Halogen Substitution in Solid-State Ion Conductor Li₃YBr_xCl_6–x

Investigation of Structure, Ionic Conductivity, and Electrochemical Stability of Halogen Substitution in Solid-State Ion Conductor Li₃YBr_xCl_6–x