A universal wet-chemistry synthesis of solid-state halide electrolytes for all-solid-state lithium-metal batteries

Wang, Changhong; Liang, Jianwen; Luo, Jing; Liu, Jue; Li, Xiaona; Zhao, Feipeng; Li, Ruying; Huang, Huan; Zhao, Shangqian; Zhang, Li; Wang, Jiantao; Sun, Xueliang

doi:10.1126/sciadv.abh1896

Cited by 106 publications

(97 citation statements)

References 59 publications

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“…[ 26 ] Halide SSEs can even be synthesized by a facile wet‐chemistry method using water as a solvent. [ 27,28 ] Furthermore, halide SSEs, especially chlorides and fluorides, exhibit wide electrochemical windows among all types of SSEs, which have been proven by theoretical [ 12,29 ] and experimental [ 30,31 ] studies. Until now, all the solid‐state batteries in the halide SSEs system are still focused on traditional oxide cathodes.…”

Section: Introductionmentioning

confidence: 99%

Highly Stable Halide‐Electrolyte‐Based All‐Solid‐State Li–Se Batteries

Liang

Kim

et al. 2022

Advanced Materials

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Solid‐state Li–S and Li–Se batteries are promising devices that can address the safety and electrochemical stability issues that arise from liquid‐based systems. However, solid‐state Li–Se/S batteries usually present poor cycling stability due to the high resistance interfaces and decomposition of solid electrolytes caused by their narrow electrochemical stability windows. Here, an integrated solid‐state Li–Se battery based on a halide Li3HoCl6 solid electrolyte with high ionic conductivity is presented. The intrinsic wide electrochemical stability window of the Li3HoCl6 and its stability toward Se and the lithiated species effectively inhibit degeneration of the electrolyte and the Se cathode by suppressing side reactions. The inherent thermodynamic mechanism of the lithiation/delithiation process of the Se cathode in solid is also revealed and confirmed by theoretical calculations. The battery achieves a reversible capacity of 402 mAh g−1 after 750 cycles. The electrochemical performance, thermodynamic lithiation/delithiation mechanism, and stability of metal‐halide‐based Li–Se batteries confer theoretical study and practical applicability that extends to other energy‐storage systems.

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Section: Introductionmentioning

confidence: 99%

Highly Stable Halide‐Electrolyte‐Based All‐Solid‐State Li–Se Batteries

Liang

Kim

et al. 2022

Advanced Materials

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“…In between the nonelectrified layers, dynamic electrochemical stability can be identified due to the self-decomposition of a metastable phase [71] or traversed reactive agent from electrode. [56,70] This dynamic electrochemical stability results from the reversible ion migration and depletion, and accumulation of neutral metal.…”

Section: Electrochemical Stability In Hsementioning

confidence: 99%

“…[ 85 ] A feasible artificial protection strategy is the dual solid electrolytes concept, where one solid electrolyte with reduction stability contacts with the anode, e.g., polymer and hydrides, and another solid electrolyte with high voltage tolerance is placed against the cathode. [ 6,86 ] Sun and co‐workers reported ammonium‐assisted wet chemistry to synthesize halide SSE Li 3 YCl 6 (LYCl) with an extraordinary ionic conductivity (0.345 mS cm −1 ) and high voltage compatibility [ 71 ] ( Figure a). However, LYCl should decompose upon Li metal thermodynamically to form a Li + / e − ‐conductive interphase which increases the interfacial impedance continuously (Figure 6b).…”

Section: Application and Design Strategies Of Hsementioning

confidence: 99%

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Vertically Heterostructured Solid Electrolytes for Lithium Metal Batteries

Tang

et al. 2022

Adv Funct Materials

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Solid‐state electrolytes (SSEs) have been regarded as the most attractive candidate for safe and high‐energy lithium (Li) batteries of the next generation. However, the inability of current SSEs to keep up with the performance requirements of batteries is significantly affected by complex factors, especially ionic conductivity, mechanochemical properties, and coupled ion/electron reaction at the electrified interfaces. Strategies in solid electrolyte chemistries and technologies are put forward to overcome these challenges while widening the breadth of possible applications. Among them, vertically heterostructured solid‐state electrolytes (HSE) are constructed as a most promising strategy, which can take advantage of individual SSE layers together and rationalize the stability and compatibility of electrodes. This review comprehensively summarizes the specific features of the HSE based on the current knowledge of SSE failure modes. Additionally, a detailed review of the recent progress on the HSE design in terms of organic polymer electrolytes and inorganic electrolytes is generated. Finally, the advantages and drawbacks of the design strategies are discussed. New perspectives about HSE are proposed as well.

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“…Lithium (Li) metal displays a high theoretical capacity (3860 mAh g −1 ) and a low negative electrode potential (−3.04 V vs standard hydrogen electrode), which makes it the ideal choice for the anode in next-generation high-energy batteries. [1][2][3][4][5][6][7][8] Significant efforts are being made to pair the Li-metal anode with high-capacity cathodes (e.g., high-nickel layered oxide, LiNi 1−x−y Co x Mn y O 2 (NMC)) to achieve energy densities >300 Wh kg −1 . [9][10][11][12][13] High-nickel cathodes display good stability in state-of-the-art liquid electrolytes, e.g., ether-based localized high-concentration electrolytes and carbonate-based fluorinerich electrolytes.…”

Section: Introductionmentioning

confidence: 99%

Operating High‐Energy Lithium‐Metal Pouch Cells with Reduced Stack Pressure Through a Rational Lithium‐Host Design

Ren

Shin

Manthiram

2022

Advanced Energy Materials

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cyclability under low-Li-excess and lean electrolyte conditions. [20][21][22] The formation of a stable, dense, atomically thin solid electrolyte interphase (SEI) is critical to suppress the depletion of metallic Li and liquid electrolytes. However, the relatively thin SEI usually undergoes a repeated fracture and rebuilding process over cycling. [23,24] Transitioning from liquid electrolytes to more stable inorganic solid electrolytes offers a potential pathway to enable highly reversible Li-metal anode. [7,25,26] Careful cell and material design of anode-free Li metal || NMC full cells based on sulfide solid electrolytes has enabled thousands of full cycles without degradation. [27] Though solid electrolytes, such as the sulfide-based electrolytes, are unstable with Li metal, parasitic interfacial reaction ceases when a kinetically stable interphase layer is formed. [27] Moreover, the solid electrolyte usually displays a high stiffness and good ductility than the porous separator in liquid electrolyte cells; therefore, it performs as mechanically strong support to prevent the fracture of the interphase layer. [27,28] Despite these efforts, the interface between the Li-metal anode and solid electrolyte suffers from chemomechanical degradation under practical cycling conditions (e.g., high current density). [29][30][31] First, the Li stripping reaction creates voids at the Li-metal/solid electrolyte interface, inducing a loss of ionic contact (Figure 1a). [32] Moreover, high-rate Li plating induces nonuniformity in the stress and electric fields, leading to heterogeneous Li plating, and further deteriorating the interfacial contacts. [33][34][35][36][37] An impractically high stack pressure (e.g., >1.0 MPa) is constantly required during cell operation to smooth the surface of the planar Li-metal anode. [38] With a stack pressure of above 1.0 MPa, most solid-state cells were tested with pressure jigs and a rigid sleeve to avoid the side effects of Li-metal creep in the radial direction. [39] The complicated cell design increases the manufacturing cost and dilutes the celllevel energy. In contrast, the optimized stack pressure adopted by scalable Li-ion pouch cells is usually within the range of 0.05-0.5 MPa. [40] The design of a 3D Li-metal anode potentially enables a mild stack pressure since the high surface area of the anode scaffold provides more intimate ionic contacts (Figure 1b). In addition, a small local current at the interface benefits the interface stability. [41][42][43][44][45] However, this direction has Transitioning from a liquid electrolyte to an inorganic solid electrolyte offers a potential pathway to enable highly reversible lithium-metal anodes. However, the solid-electrolyte-protected lithium-metal anode suffers from poor interfacial ionic contacts and requires an impractically high stack pressure (>1.0 MPa) to maintain the interfacial contacts. It is demonstrated here that combining a hollow silver/carbon fiber scaffold and an inorganic/ organic composite electrolyte enables a highly revers...

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A universal wet-chemistry synthesis of solid-state halide electrolytes for all-solid-state lithium-metal batteries

Cited by 106 publications

References 59 publications

Highly Stable Halide‐Electrolyte‐Based All‐Solid‐State Li–Se Batteries

Highly Stable Halide‐Electrolyte‐Based All‐Solid‐State Li–Se Batteries

Vertically Heterostructured Solid Electrolytes for Lithium Metal Batteries

Operating High‐Energy Lithium‐Metal Pouch Cells with Reduced Stack Pressure Through a Rational Lithium‐Host Design

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