<i>Operando</i> Measurement of Layer Breathing Modes in Lithiated Graphite

Yadegari, Hossein; Koronfel, Mohamed A.; Wang, Kang; Thornton, Daisy B.; Stephens, Ifan E. L.; Molteni, Carla; Haynes, Peter; Ryan, Mary P.

doi:10.1021/acsenergylett.1c00494

Cited by 42 publications

(28 citation statements)

References 34 publications

(73 reference statements)

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“…[ 32 ] The relative motion of graphene planes (i.e., the distortion and dislocation of graphene planes) from the shear mode will lead to changes in low‐frequency Raman signal below 200 cm −1 . [ 20 ]…”

Section: Resultsmentioning

confidence: 99%

“…[ 45 ] Meanwhile, the low‐frequency Raman signal responsive to the plane de‐coupling is still not observed, further implying that sodium ions’ interaction with defect sites belongs to the adsorption mode without any evident inner shearing (Figure 4b). [ 20 ] Consequently, the adsorption mode of sodium ions at defect sites as the surface‐controlled reaction dominates in the sloping region, and the fast electrochemical kinetics in this region can also be explained by this phenomenon.…”

Section: Resultsmentioning

confidence: 99%

“…This trend provides further evidence that the reaction of sodium ions within closed nanovoids via a kind of filling and expansion mode by interacting with more accessible sp 2 carbon atoms; this reaction increases the inner shearing stress and disordered degree of the carbon bulk phase via the dislocations of graphene planes (insets in Figure 4b). [ 20 ] As this reaction continues in the filling mode, the E 2g stretching mode of G‐band is eventually significantly suppressed (Figure S12b, Supporting Information). By linking the structural changes observed in this section with the previous kinetic analysis, we can conclude that this filling mode of sodium ions into closed nanovoids needs to overcome large energy barriers, and proceeds with slow kinetics as the diffusion‐controlled reaction.…”

Section: Resultsmentioning

confidence: 99%

“…[32] The relative motion of graphene planes (i.e., the distortion and dislocation of graphene planes) from the shear mode will lead to changes in low-frequency Raman signal below 200 cm −1 . [20] In the sloping region (>0.1 V vs Na + /Na), the D-peak becomes broader and slightly shifts to a lower wavenumber, which indicates sodium ions are interacting with defect sites (e.g., carbon vacancies, substitutional and interstitial impurities, etc. ), thus restricting A 1g breathing mode of D-band (Figure S12c, Supporting Information).…”

Section: Fundamental Mechanistic Insights Into Sodium-ion Insertion B...mentioning

confidence: 99%

“…It is important to note that operando Raman characterization of hard carbons during the electrochemical sodium‐ion storage, including the low‐frequency Raman shift region, are complicated to perform due to their broad characteristic peaks with low intensities and the intense background caused by the Rayleigh scattering at the low‐frequency Raman shift region. [ 20 ] Despite this, our design of the operando Raman cell has a remarkable resolution, making significant breakthroughs in achieving a real‐time fine spectrum analysis of hard carbons. Meanwhile, through an innovative combination of life cycle assessment (LCA) with experimental testing of sodium‐ion battery technologies, we can look across the different life‐stages of hard carbon anodes from the supply chain of raw materials to the preparation of products and recycling of waste, thus assessing the differences in the sustainability of hard carbons with and without hydrothermal pre‐treatment.…”

Section: Introductionmentioning

confidence: 99%

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The Role of Hydrothermal Carbonization in Sustainable Sodium‐Ion Battery Anodes

Wang

Guo

et al. 2022

Advanced Energy Materials

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107

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Sodium‐ion batteries as a prospective alternative to lithium‐ion batteries are facing the challenge of developing high‐performance, low‐cost and sustainable anode materials. Hard carbons are appropriate to store sodium ions, but major energy and environmental concerns during their fabrication process (i.e., high‐temperature carbonization) have not been properly assessed. Furthermore, the rational design of high‐performing hard carbon anodes is usually limited by the conventional direct carbonization of organic precursors. Here, the hydrothermal carbonization process is employed as a versatile pre‐treatment method of renewable precursors, followed by high‐temperature carbonization, for producing advanced hard carbon anodes. The critical role of hydrothermal pre‐treatment in regulating the structure for an optimized performance of hard carbon anodes is elucidated, while revealing the sodium‐ion storage mechanism using electrochemical kinetic calculations, advanced characterization and multi‐scale modeling. Furthermore, the environmental impacts of hydrothermal pre‐treatment and subsequent carbonization are evaluated using life cycle assessment compared to direct carbonization. By comparing hard carbon anodes with and without the hydrothermal pre‐treatment, it is verified that the additional hydrothermal process is responsible for enhanced electrochemical performance, increased carbon yields and reduced carbon emissions. The work provides a systematic understanding of functions and energy consumptions of hydrothermal systems to achieve next‐generation sustainable sodium‐ion batteries.

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Section: Resultsmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

Section: Fundamental Mechanistic Insights Into Sodium-ion Insertion B...mentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 3 more Smart Citations

The Role of Hydrothermal Carbonization in Sustainable Sodium‐Ion Battery Anodes

Wang

Guo

et al. 2022

Advanced Energy Materials

Self Cite

107

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Anode‐Free Alkali Metal Batteries: From Laboratory to Practicability

Xu,

Huang,

Sun

et al. 2024

Adv Funct Materials

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Anode‐free alkali metal batteries (AFAMBs) are regarded as the most promising candidates for next‐generation high‐energy systems owing to their high safety, high energy density, and low cost. However, the restricted alkali supply at the cathode, severe dendrite growth, and unstable electrode‐electrolyte interface result in low Coulombic efficiency and severely short cycle life. The optimization strategies are mainly based on laboratory‐level coin cells, but their effectiveness in practical‐level batteries is rarely discussed. This review presents a comprehensive overview of the recent developments and challenges of AFAMBs from the laboratory toward their practicability. First, the advances, major challenges, and optimization strategies are systematically summarized. More significantly, given the vast differences in battery structures and operating conditions, the gap between laboratory‐level and practical‐level batteries is particularly emphasized in this review. In addition, the failure mechanisms of practical‐level AFAMBs have been outlined and the key parameters affecting their performance are identified. Finally, insightful perspectives on practical AFAMBs are presented, aiming to provide helpful guidance for subsequent basic research to promote large‐scale commercial applications of AFAMBs.

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Achieving All‐Plateau and High‐Capacity Sodium Insertion in Topological Graphitized Carbon

Lai

Liang

et al. 2023

Advanced Materials

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Hard carbon anodes with all‐plateau capacities below 0.1 V are prerequisites to achieve high energy density sodium ion storages, which are holding promises for the future sustainable energy technologies. However, challenges in removing defects and improving the insertion of sodium ions heading off the development of hard carbon to achieve this goal. Herein, we reported a highly cross‐linked topological graphitized carbon using biomass corn cobs through a two‐step rapid thermal annealing strategy. The topological graphitized carbon constructed with long‐range graphene nanoribbons and cavities/tunnels provides a multi‐directional insertions of sodium ions whilst eliminating defects to absorb sodium ions at high voltage region. Evidences from advanced technique including in‐situ XRD, in‐situ Raman and in‐situ/ex‐situ TEM indicate that the sodium ions appear Na cluster formation between curved topological graphite layers and in the topological cavity of adjacent graphite band entanglements. The reported topological insertion mechanism enables outstanding battery performance with a single full low‐voltage plateau capacity of 290 mAh g−1, which is almost 97% of the total capacity.This article is protected by copyright. All rights reserved

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Operando Measurement of Layer Breathing Modes in Lithiated Graphite

Cited by 42 publications

References 34 publications

The Role of Hydrothermal Carbonization in Sustainable Sodium‐Ion Battery Anodes

The Role of Hydrothermal Carbonization in Sustainable Sodium‐Ion Battery Anodes

Anode‐Free Alkali Metal Batteries: From Laboratory to Practicability

Achieving All‐Plateau and High‐Capacity Sodium Insertion in Topological Graphitized Carbon

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