Interface engineering of inorganic solid-state electrolytes for high-performance lithium metal batteries

Miao, Xianguang; Wang, Huiyang; Sun, Rui; Wang, Cheng-Xiang; Zhang, Zhiwei; Li, Zhaoqiang; Yin, Longwei

doi:10.1039/d0ee01435d

Cited by 117 publications

(63 citation statements)

References 332 publications

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“…1 H NMR (500 MHz, CDCl 3 , 23°C): δ 1.12 (m, 14H), 1.30 (m, 4H), 1.54 (m, 4H), 2.19 (t, J = 8, 2H), 2.26 (s, 4H), 3.30 (t, J = 7, 2H). 13 C NMR (125 MHz, CDCl 3 , 23°C): δ 20, 23, 25, 26.4, 26.8, 26.93, 26.96, 26.99, 27, 30.…”

Section: Methodsmentioning

confidence: 99%

“…DSC: T m = 30 °C (2 nd heating) 1 H NMR (500 MHz, DMSO-d 6 , 23°C): δ 1.24 (m, 28H), 1.38 (m, 4H), 1.59 (m, 4H), 2.03 (t, J = 7, 4H), 3.19 (m, 4H), 3.35 (m, 4H), 3.45 (t, J = 5, 4H), 4.35 (t, J = 5, 2H). 13 C NMR (125 MHz, DMSO-d 6 , 23°C): δ 21, 22, 25, 26, 28, 29.2, 29.3, 29.4, 29.5, 33, 58, 61, 62. N,N-di(11-hydroxyundecyl)pyrrolidinium PF 6 − .…”

Section: Methodsmentioning

confidence: 99%

“…1 H NMR (500 MHz, acetone-d 6 , 23°C): δ 1.29 (m, 20H), 1.39 (m, 8H), 1.48 (m, 4H), 1.85 (m, 4H), 2.26 (m, 4H), 3.45 (m, J = 8.5, 4H), 3.51 (m, 4H), 3.71 (t, J = 6.5, 4H). 13 : From the previous experiment, the bromide salt (2.000 g, 4.060 mmol) was dissolved in deionized water (10 mL) NaBPh 4 (1.667 g, 4.872 mmol) was added with vigorous stirring. The insoluble precipitate was filtered and the filter cake was washed by deionized water there times.…”

Section: Methodsmentioning

confidence: 99%

“…DSC: T g = −13 °C (second heating), no T m . 1 H NMR (500 MHz, acetone-d 6 , 23°C): δ 1.30 (m, 20H), 1.36 (m, 8H), 1.50 (m, 4H), 1.75 (m, 4H), 2.11 (m, 4H), 3.27 (m, 4H), 3.47 (m, 4H), 3.52 (m, 4H), 7.25(t, J = 7, 4H), 7.39(t, J = 7.5, 8H), 7.80(m, 8H) 13 C NMR (125 MHz, acetone-d 6 , 23°C): δ 23, 24, 27., 29.7, 30, 31.0, 31.1, 31.3 34, 61121, 125(q, 2 J(B,C) = 2), 136, 164(q, 1 J(B,C) = 50)…”

Section: Methodsmentioning

confidence: 99%

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Anion‐Rectifying Polymeric Single Lithium‐Ion Conductors

Cho

Shin

et al. 2021

Adv Funct Materials

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Polymeric single lithium (Li)-ion conductors (SICs), along with inorganic conducting materials such as sulfides and oxides, have received significant attention as promising solid-state electrolytes. Yet their practical applications have been plagued predominantly by sluggish ion transport. Here, a new class of quasi-solid-state SICs based on anion-rectifying semi-interpenetrating polymer networks (semi-IPNs) with reticulated ion nanochannels are demonstrated. This semi-IPN SIC (denoted as sSIC) features a bicontinuous and nanophase-separated linear cationic polyurethane (cPU), which supports single-ion conducting nanochannels, and ultraviolet-crosslinked triacrylate polymer, which serves as a mechanical framework. The cPU phase is preferentially swollen with a liquid electrolyte and subsequently allows anionrectifying capability and nanofluidic transport via surface charge, which enable fast Li + migration through ion nanochannels. Such facile Li + conduction is further enhanced by tuning ion-pair (i.e., freely movable anions and cations tethered to the cPU chains) interaction. Notably, the resulting sSIC provides high Li + conductivity that exceeds those of commercial carbonate liquid electrolytes. This unusual single-ion conduction behavior of the sSIC suppresses anion-triggered interfacial side reactions with Li-metal anodes and facilitates electrochemical reaction kinetics at electrodes, eventually improving rate performance and cycling retention of Li-metal cells (comprising LiNi 0.8 Co 0.1 Mn 0.1 O 2 cathodes and Li-metal anodes) compared to those based on carbonate liquid electrolytes.

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Section: Methodsmentioning

confidence: 99%

Section: Methodsmentioning

confidence: 99%

Section: Methodsmentioning

confidence: 99%

Section: Methodsmentioning

confidence: 99%

See 2 more Smart Citations

Anion‐Rectifying Polymeric Single Lithium‐Ion Conductors

Cho

Shin

et al. 2021

Adv Funct Materials

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“…Despite their solid‐state feature and ideal Li + transference number ( t Li + = 1), the inorganic solid electrolytes have suffered from interfacial/grain‐boundary resistances, thickness issues, mechanical rigidity, and dendrite growth through interstitial voids. [ 6,7 ] Recently, argyrodite‐type sulfides (Li 6 PS 5 Cl) combined with silver‐carbon composite anodes enabled the fabrication of high‐energy long‐cycling solid‐state LMBs. [ 8 ] However, the sophisticated isostatic pressing technique and high‐temperature (60 °C) operating conditions were needed to electrochemically activate the cells.…”

Section: Introductionmentioning

confidence: 99%

Single‐Ion Conducting Soft Electrolytes for Semi‐Solid Lithium Metal Batteries Enabling Cell Fabrication and Operation under Ambient Conditions

Kim

et al. 2021

Advanced Energy Materials

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Despite their potential as post lithium‐ion batteries, solid‐state Li‐metal batteries are struggling with insufficient electrochemical sustainability and ambient operation limitations. These challenges mainly stem from lack of reliable solid‐state electrolytes. Here, a new class of single‐ion conducting quasi‐solid‐state soft electrolyte (SICSE) for practical semi‐solid Li‐metal batteries (SSLMBs) is demonstrated. The SICSE consists of an ion‐rectifying compliant skeleton and a nonflammable coordinated electrolyte. Rheology‐tuned SICSE pastes, in combination with UV curing‐assisted multistage printing, allow fabrication of seamlessly integrated SSLMBs (composed of a Li metal anode and LiNi0.8Co0.1Mn0.1 cathode) without undergoing high‐pressure/high‐temperature manufacturing steps. The single‐ion conducting capability of the SICSE plays a viable role in stabilizing the interfaces with the electrodes. The resulting SSLMB full cell exhibits stable cycling performance and bipolar configurations with tunable voltages and high gravimetric/volumetric energy densities (476 Wh kgcell−1/1102 Wh Lcell−1 at four‐stacked cells with 16.656 V) under ambient operating conditions, along with low‐temperature performance, mechanical foldability, and nonflammability.

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Introducing NO₃^– into Carbonate‐Based Electrolytes via Covalent Organic Framework to Incubate Stable Interface for Li‐Metal Batteries

Wen

Ding

Yang

et al. 2021

Adv Funct Materials

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Lithium nitrate (LiNO 3 ) as an effective additive to construct stable solid electrolyte interface (SEI) is generally applied in ether-based electrolytes, but its poor solubility in carbonate-based electrolytes limits further application for Li metal batteries (LMBs). Therefore, an engineering of introducing NO 3 into carbonate-based electrolytes by synthesizing targeted covalent organic framework (EB-COF:NO 3 ) to modify Li anode for incubating a reliable SEI is reported. Its unique structure not only facilitates the desolvation process of lithium ions (Li + ) to accelerate the transport of Li + , but also releases NO 3 to form beneficial Li 3 N, LiN x O y species to in situ construct a stable SEI. With the application of EB-COF:NO 3 , the cycling and rate performance of (50 µm) Li//LiFePO 4 full cell is comprehensively improved under the conditions of poor electrolyte and high loading, significantly increasing capacity retention from 14% to 94% after 200 cycles. And the high voltage Li//LiNi 0.5 Mn 1.5 O 4 full cell still demonstrates excellent cycling stability with the capacity retention of 92% after 600 cycles. Accordingly, this strategy shares a prospect for the application of covalent organic frameworks (COFs) to build a stable SEI for high-energy-density LMBs, and also broadens the application of LiNO 3 in carbonate-based electrolytes.

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Interface engineering of inorganic solid-state electrolytes for high-performance lithium metal batteries

Abstract: This review presents the mechanisms, challenges, strategies, and perspectives in the interface engineering of inorganic-based solid-state Li metal batteries.

Cited by 117 publications

References 332 publications

Anion‐Rectifying Polymeric Single Lithium‐Ion Conductors

Anion‐Rectifying Polymeric Single Lithium‐Ion Conductors

Single‐Ion Conducting Soft Electrolytes for Semi‐Solid Lithium Metal Batteries Enabling Cell Fabrication and Operation under Ambient Conditions

Introducing NO₃^– into Carbonate‐Based Electrolytes via Covalent Organic Framework to Incubate Stable Interface for Li‐Metal Batteries

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Interface engineering of inorganic solid-state electrolytes for high-performance lithium metal batteries

Abstract: This review presents the mechanisms, challenges, strategies, and perspectives in the interface engineering of inorganic-based solid-state Li metal batteries.

Cited by 117 publications

References 332 publications

Anion‐Rectifying Polymeric Single Lithium‐Ion Conductors

Anion‐Rectifying Polymeric Single Lithium‐Ion Conductors

Single‐Ion Conducting Soft Electrolytes for Semi‐Solid Lithium Metal Batteries Enabling Cell Fabrication and Operation under Ambient Conditions

Introducing NO3– into Carbonate‐Based Electrolytes via Covalent Organic Framework to Incubate Stable Interface for Li‐Metal Batteries

Contact Info

Product

Resources

About

Introducing NO₃^– into Carbonate‐Based Electrolytes via Covalent Organic Framework to Incubate Stable Interface for Li‐Metal Batteries