Characterization of the structure and chemistry of the solid–electrolyte interface by cryo-EM leads to high-performance solid-state Li-metal batteries

Lin, Ruoqian; He, Yubin; Wang, Chunyang; Zou, Peichao; Hu, Enyuan; Yang, Xiao‐Qing; Xu, Kang; Xin, Huolin L.

doi:10.1038/s41565-022-01148-7

Cited by 124 publications

(81 citation statements)

References 38 publications

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“…In contrast, the interfacial layer derived from commercial electrolyte consists of many organic components such as C–O, O–CO, and a small number of inorganic compounds, Li 2 O, owing to the interfacial reaction between carbonate solvents and Li metal (Figure S22). The SEI composed of these organic components with poor mechanical strength generally fails to impede the growth of Li dendrites . To further clearly reveal the distribution of the above components in the SEI, TOF-SIMS was performed here for both M-ILE and ILE systems.…”

Section: Resultsmentioning

confidence: 94%

“…The SEI composed of these organic components with poor mechanical strength generally fails to impede the growth of Li dendrites. 43 To further clearly reveal the distribution of the above components in the SEI, TOF-SIMS was performed here for both M-ILE and ILE systems. As shown in Figures 4l and S23, the intensity signal of LiF 2 − is higher in the M-ILE-derived SEI than that in the ILE-derived SEI at different sputter times, indicating a LiF-rich SEI layer formed in the M-ILE system.…”

Section: Resultsmentioning

confidence: 99%

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Tailoring Electrolyte Solvation for LiF-Rich Solid Electrolyte Interphase toward a Stable Li Anode

Wang

et al. 2022

ACS Nano

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A solid electrolyte interphase (SEI) with robust mechanical property and high ionic conductivity is imperative for high-performance lithium metal batteries since it can efficiently impede the growth of notorious lithium dendrites. However, it is difficult to form such a SEI directly from an electrolyte. In this work, a crowding dilutant modified ionic liquid electrolyte (M-ILE) has been developed for this purpose. Simulations and experiments indicate that the 1,2-difluorobenzene (1,2-dfBen) dilutant not only creates a crowded electrolyte environment to promote the interaction of Li+–FSI–, leading to abundant aggregate ion pairs (AGGs), but also participates in the reduction to construct a robust and high ionic-conductive SEI. With this M-ILE, Li/LiFePO4 cells achieve a capacity retention of 96% over 250 cycles with 9.5 mg cm–2 mass loading, and Li/LiNi0.5Co0.2Mn0.3O2 cells also deliver a discharge capacity of 132 mAh g–1 with a high retention of 88% after 100 cycles. Therefore, the use of a crowding diluent is considered to be an efficient way to construct an advanced SEI for a Li anode.

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Section: Resultsmentioning

confidence: 94%

Section: Resultsmentioning

confidence: 99%

Tailoring Electrolyte Solvation for LiF-Rich Solid Electrolyte Interphase toward a Stable Li Anode

Wang

et al. 2022

ACS Nano

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“…736,737 For example, the cryogenic electron microscopy has been applied for imaging of the SEI and Li plating morphologies to directly visualize the structure and reveal the function of the complex interphase at the atomic scale. 736,738 The interested reader may refer to some previous review articles for the detailed information. 23,494,694,739,740 In this section, we have mainly summarized some guidelines on the improvement of the interfacial issues for flexible and portable electrochemical energy devices.…”

Section: Chemicalmentioning

confidence: 99%

“…In addition to the existing material characterization tools, the advanced techniques especially in-situ methods are highly desired to probe and identify the buried interfaces; these ex-situ and in-situ characterization methods include the electron microscopy, X-ray computed tomography, transmission X-ray microscopy, nuclear magnetic resonance, time-of-flight secondary ion mass spectrometry, differential phase contrast scanning transmission electron microscopy, neutron depth profiling, X-ray absorption fine structure spectrum, and three-dimensional atom probe, etc. In particular, the cryogenic electron microscopy is becoming a vital tool with atomic resolution, which can maintain the native and fresh state of air-sensitive and beam-sensitive materials and/or interphases of the energy devices for high-resolution imaging. , For example, the cryogenic electron microscopy has been applied for imaging of the SEI and Li plating morphologies to directly visualize the structure and reveal the function of the complex interphase at the atomic scale. , The interested reader may refer to some previous review articles for the detailed information. ,,,, In this section, we have mainly summarized some guidelines on the improvement of the interfacial issues for flexible and portable electrochemical energy devices.…”

Section: Semi-solid/solid Electrolytes In Flexible and Portable Elect...mentioning

confidence: 99%

Opportunities of Flexible and Portable Electrochemical Devices for Energy Storage: Expanding the Spotlight onto Semi-solid/Solid Electrolytes

et al. 2022

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The ever-increasing demand for flexible and portable electronics has stimulated research and development in building advanced electrochemical energy devices which are lightweight, ultrathin, small in size, bendable, foldable, knittable, wearable, and/or stretchable. In such flexible and portable devices, semi-solid/solid electrolytes besides anodes and cathodes are the necessary components determining the energy/power performances. By serving as the ion transport channels, such semi-solid/solid electrolytes may be beneficial to resolving the issues of leakage, electrode corrosion, and metal electrode dendrite growth. In this paper, the fundamentals of semi-solid/solid electrolytes (e.g., chemical composition, ionic conductivity, electrochemical window, mechanical strength, thermal stability, and other attractive features), the electrode–electrolyte interfacial properties, and their relationships with the performance of various energy devices (e.g., supercapacitors, secondary ion batteries, metal–sulfur batteries, and metal–air batteries) are comprehensively reviewed in terms of materials synthesis and/or characterization, functional mechanisms, and device assembling for performance validation. The most recent advancements in improving the performance of electrochemical energy devices are summarized with focuses on analyzing the existing technical challenges (e.g., solid electrolyte interphase formation, metal electrode dendrite growth, polysulfide shuttle issue, electrolyte instability in half-open battery structure) and the strategies for overcoming these challenges through modification of semi-solid/solid electrolyte materials. Several possible directions for future research and development are proposed for going beyond existing technological bottlenecks and achieving desirable flexible and portable electrochemical energy devices to fulfill their practical applications. It is expected that this review may provide the readers with a comprehensive cross-technology understanding of the semi-solid/solid electrolytes for facilitating their current and future researches on the flexible and portable electrochemical energy devices.

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“…Given the XRD results, we were specifically hoping to capture the crystalline patterns that emerge in the ZNSE after cycling. Cryo-TEM is the most suitable technique for SEI characterization because it perfectly maintains the interfaces; unfortunately, cryo-TEM sample preparation is extremely difficult and relatively time-consuming, and detailed SEI structure is rarely reported in literature. , …”

mentioning

confidence: 99%

Na–K Alloy Anode for High-Performance Solid-State Sodium Metal Batteries

Cheng

Yang

et al. 2022

Nano Lett.

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Rechargeable solid-state Na metal batteries (SSNMB) can offer high operational safety and energy density. However, poor solid−solid contact between the electrodes and the electrolyte can dramatically increase interfacial resistance and Na dendrite formation, even at low current rates. Therefore, we developed a carbon-fiber-supported liquid Na−K alloy anode that ensures close anode−electrolyte contact, enabling superior cycle stability and rate capability. We then demonstrated the first cryogenic transmission electron microscopy (cryo-TEM) characterization of an SSNMB, capturing the evolution of solid− electrolyte interphase (SEI) and revealing both crystalline and amorphous phases, which could facilitate ion transport and prevent continuous side reactions. By enhancing contact between the Na− K alloy and solid-state electrolyte, these symmetric cells are capable of cycling for over 800 h without notable increased polarization and enable an unprecedented critical current density (CCD) at 40 mA cm −2 . Our liquid Na−K alloy approach offers a promising strategic avenue toward commercial SSNMBs.

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Characterization of the structure and chemistry of the solid–electrolyte interface by cryo-EM leads to high-performance solid-state Li-metal batteries

Cited by 124 publications

References 38 publications

Tailoring Electrolyte Solvation for LiF-Rich Solid Electrolyte Interphase toward a Stable Li Anode

Tailoring Electrolyte Solvation for LiF-Rich Solid Electrolyte Interphase toward a Stable Li Anode

Opportunities of Flexible and Portable Electrochemical Devices for Energy Storage: Expanding the Spotlight onto Semi-solid/Solid Electrolytes

Na–K Alloy Anode for High-Performance Solid-State Sodium Metal Batteries

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