Advances in studying interfacial reactions in rechargeable batteries by photoelectron spectroscopy

Källquist, Ida; Ruyet, Ronan Le; Liu, Haidong; Mogensen, Ronnie; Lee, Ming-Tao; Edström, Kristina; Naylor, Andrew J.

doi:10.1039/d2ta03242b

Cited by 22 publications

(16 citation statements)

References 234 publications

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“…The shift of the C=O peak in PCHC is ascribed to the weakened electron withdrawing effects of bound negative inductive groups. 50,51 The O 1s pattern of the compound proves the existence of organic compounds. While PCHC maintains a stable component of the O=C, O−C, and O−F functional groups, the ratio for O−C is increased in CHC during cycling, which might be related to the organic phase transition during growth of the SEI.…”

Section: Resultsmentioning

confidence: 95%

Weakly Solvating Few-Layer-Carbon Interface toward High Initial Coulombic Efficiency and Cyclability Hard Carbon Anodes

Zhao,

Huang

2024

ACS Nano

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The carbonaceous anodes in sodium ion batteries suffer from low initial Coulombic efficiency (ICE) and poor cyclability due to rampant solid electrolyte interface (SEI) growth. The concept of the weakly solvating electrolyte (WSE) has been popularized for SEI regulation on the anode by adjusting the cation solvation structure. Nevertheless, the effects on the solvation sheath from the electrode/electrolyte interface are ignored in most WSE applications. In this work, we extend the WSE from the bulk electrolyte to the electrolyte/carbon interface. By recycling asphalt wastes into sp 2 C enriched fewlayer carbon on hard carbon, a weakly solvating interface is fabricated with lower adsorption energy to electrolyte solvent molecules than a pristine anode (−0.89 vs −1.08 eV for Na/diglyme). Accordingly, more anionic groups are attracted into the solvent-weakened solvation sheath during sodiation (2.30 vs 1.96 coordination number for PF 6 − ). The anion-mediated contact ion pairs facilitate a thin, inorganic-rich SEI layer with a homogeneous distribution, which confers a high ICE of 97.9% and a high capacity of 335.6 mA h g −1 at 1 C (89.5% retention, 1000 cycles). The full battery also manifests an energy density of 209 W h kg −1 . This interfacial design is applicable in both ether-and ester-based electrolytes, which is promising in cost-effective modification for carbonaceous electrodes.

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Section: Resultsmentioning

confidence: 95%

Weakly Solvating Few-Layer-Carbon Interface toward High Initial Coulombic Efficiency and Cyclability Hard Carbon Anodes

Zhao,

Huang

2024

ACS Nano

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“…It is well-known that the SEI layer plays a critical role in the electrochemical behaviors of batteries − as the instability of the SEI is the main cause of electrolyte depletion. To further clarify and understand the reason for electrolyte depletion during electrochemical lithium plating/stripping with both conventional and reservoir methods, XPS was used to analyze the SEI layer formed on Ni foam at various stages of plating/stripping cycles (Figure S7a) including preliminary SEI (discharge to 0.0 V), plated Li, stripped half of the plated lithium (reservoir method), and fully stripped sample (conventional method).…”

Section: Resultsmentioning

confidence: 99%

Assessing Coulombic Efficiency in Lithium Metal Anodes

et al. 2023

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Although lithium metal and anode-free rechargeable batteries (LMBs and AFBs) are phenomenal energy storage systems, the formation of lithium deposits with high surfaces during repeated plating−stripping cycles has hindered their practical applications. Recently, extensive efforts have been made to prevent the growth of high-surface lithium deposition, e.g., electrolyte modification, artificial coating deposition, lithiophilic current collectors, composite lithium metal electrodes, etc. In most of these approaches, Coulombic efficiency (CE) has been used as a quantifiable indicator for the reversibility of the LMBs and AFBs. The interpretation and validation of research results, however, are challenging since the measurement of CE is affected by several parameters related to battery assembly and testing. This study aims to unveil the interplay of several potentially overlooked parameters regulating the CE, such as stripping cutoff voltage, electrolyte quantity, precycling to form a solid electrode interphase (SEI), and electrode surface modification, by applying two alternative electrochemical methods. The hidden aspects of nucleation overpotential revealed by studying these parameters, as well as their influence on the composition and stability of the SEI, are discussed. Overall, this work provides an insightful understanding of the methods and parameters used for assessing the performance of LMBs and AFBs.

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“…However, XPS is even more surface-sensitive than ATR-IR, as its probing depth is typically in the range of several nanometers. Therefore, extra precautions should be taken to prevent sample degradation during disassembly and washing. ,− Interpretation of XPS is strongly influenced by the peak fitting process, and quantification is possible only through systematic investigation of standard samples, which is unfortunately rarely done in the battery literature . XPS investigation within the bulk of the electrodes can be performed with the help of sample sputtering, but sample degradation during the sputtering should be carefully investigated beforehand.…”

Section: Investigation Of the Electrochemical Mechanismmentioning

confidence: 99%

Organic Cathodes, a Path toward Future Sustainable Batteries: Mirage or Realistic Future?

Bitenc,

Pirnat,

Lužanin

et al. 2024

Chem. Mater.

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Organic active materials are seen as next-generation battery materials that could circumvent the sustainability and cost limitations connected with the current Li-ion battery technology while at the same time enabling novel battery functionalities like a bioderived feedstock, biodegradability, and mechanical flexibility. Many promising research results have recently been published. However, the reproducibility and comparison of the literature results are somehow limited due to highly variable electrode formulations and electrochemical testing conditions. In this Perspective, we provide a critical view of the organic cathode active materials and suggest future guidelines for electrochemical characterization, capacity evaluation, and mechanistic investigation to facilitate reproducibility and benchmarking of literature results, leading to the accelerated development of organic electrode active materials for practical applications.

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Advances in studying interfacial reactions in rechargeable batteries by photoelectron spectroscopy

Abstract: Many of the challenges faced in the development of lithium-ion batteries (LIBs) and next-generation technologies stem from the (electro)chemical interactions between the electrolyte and electrodes during operation. It is at...

Cited by 22 publications

References 234 publications

Weakly Solvating Few-Layer-Carbon Interface toward High Initial Coulombic Efficiency and Cyclability Hard Carbon Anodes

Weakly Solvating Few-Layer-Carbon Interface toward High Initial Coulombic Efficiency and Cyclability Hard Carbon Anodes

Assessing Coulombic Efficiency in Lithium Metal Anodes

Organic Cathodes, a Path toward Future Sustainable Batteries: Mirage or Realistic Future?

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