Solvating power series of electrolyte solvents for lithium batteries

Su, Chi‐Cheung; He, Meinan; Amine, Rachid; Rojas, Tomás; Cheng, Lei; Ngo, Anh T.; Amine, Khalil

doi:10.1039/c9ee00141g

Cited by 177 publications

(169 citation statements)

References 40 publications

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“…By testing Zn electrolytes with a rigorous protocol designed with the ultimate goal of a RZMB in mind, it is possible to establish correlations between electrochemical performance and fundamental electrolyte properties, potentially guiding future electrolyte development. Echoing the work by Amine and co-workers, [29,30] we examined the role of the electrolyte solvent in the kinetics of interfacial charge transfer reactions and the deposition of a passivating interphase on the electrode surface. In the case of lithiumion batteries or batteries with Li metal anodes, it has been argued that the solvating strength of the electrolyte solvents should be lessened to promote salt aggregation, so that preferential reduction of fluorinated anions can outcompete solvent reduction, leading to an inorganic and dense solid electrolyte interphase (SEI).…”

Section: Resultsmentioning

confidence: 99%

Critical Factors Dictating Reversibility of the Zinc Metal Anode

Schroeder

Pollard

et al. 2020

Energy & Environ Materials

144

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With high energy density and improved safety, rechargeable battery chemistries with a zinc (Zn) metal anode offer promising and sustainable alternatives to those based on lithium metal or lithium‐ion intercalation/alloying anode materials; however, the poor electrochemical reversibility of Zn plating/stripping, induced by parasitic reactions with both aqueous and non‐aqueous electrolytes, presently limits the practical appeal of these systems. Although recent efforts in rechargeable Zn metal batteries (RZMBs) have achieved certain advancements in Zn metal reversibility, as quantified by the Coulombic efficiency (CE), a standard protocol for CE has not been established, and results across chemistries and systems are often conflicting. More importantly, there is still an insufficient understanding regarding the critical factors dictating Zn reversibility. In this work, a rigorous, established protocol for determining CE of lithium metal anodes is transplanted to the Zn chemistry and is used for systematically examining how a series of factors including current collector chemistry, current density, temperature, and the upper voltage limit during stripping affect the measured reversibility of different Zn electrolytes. With support from density functional theory calculations, this standardized Zn CE protocol is then leveraged to identify an important correlation between electrolyte solvation strength toward Zn2+ and the measured Zn CE in the corresponding electrolyte, providing new guidance for future development and evaluation of Zn electrolytes.

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Section: Resultsmentioning

confidence: 99%

Critical Factors Dictating Reversibility of the Zinc Metal Anode

Schroeder

Pollard

et al. 2020

Energy & Environ Materials

144

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Section: Summary and Perspectivementioning

confidence: 99%

“…further found that the solvating power of individual organic solvents critically determining the electrochemical performance of LIBs. [ 162 ] Using a newly developed internally referenced diffusion‐ordered spectroscopy technique and diffusion coefficient‐coordination ratio ( D –α) analysis, they have identified the solvating power of most organic solvents (Figure 34c). As a result, by using a combination of low solvating power (FEMC and FEC), the NCM622/Li cell demonstrated much better cycle performance (Figure 34d) and coulombic efficiency (Figure 34e) than GENII electrolyte (EC and EMC).…”

Section: Strategies To Advance Ni‐rich Layered Cathodes Under Harsh Omentioning

confidence: 99%

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Challenges and Strategies to Advance High‐Energy Nickel‐Rich Layered Lithium Transition Metal Oxide Cathodes for Harsh Operation

Liu

Daali

et al. 2020

Adv Funct Materials

Self Cite

202

134

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Nickel-rich layered lithium transition metal oxides (LiNi 1−x−y Co x Mn y O 2 and LiNi 1−x−y Co x Al y O 2 , x + y ≤ 0.2) are the most attractive cathode materials for the next generation lithium-ion batteries for automotive application. However, they suffer from structural/interfacial instability during repeated charge/discharge, resulting in severe performance degradation and serious safety concerns. This work provides a comprehensive review about challenges and strategies to advance nickel-rich layered cathodes specifically for harsh (high-voltage, hightemperature, and fast charging) operations. Firstly, the degradation pathways of nickel-rich cathodes including surface/interface degradation, undesired cathode-electrolytes parasitic reactions, gas evolution, inter/intragranular cracking, and electrical/ionic isolation are discussed. Then, recent achievements in stabilizing the structure/interface of nickel-rich cathodes via surface coating, cation/anion doping, composition tailoring, morphology engineering, and electrolytes optimization are summarized. Moreover, challenges and strategies to improve the performance of Ni-rich cathodes at the electrode level are discussed. Outlook and perspectives to promote the practical application of nickel-rich layered cathodes toward automotive application are provided as well.

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“…Yet how the electrolyte species interact with the Li metal electrode under electrochemical conditions and affect the performance of Li metal batteries (LMBs) are not well understood. Solvation of the Li + ion is considered to be important to the chemistry at the electrode/electrolyte interface . Various techniques, including vibrational spectroscopy (FTIR or Raman), electrospray ionization mass spectrometry, and nuclear magnetic resonance spectroscopy have been employed to study the structure of the solvation sheath and to understand the interfacial chemistry on the molecular level.…”

Section: Figurementioning

confidence: 99%

Solvent Molecule Cooperation Enhancing Lithium Metal Battery Performance at Both Electrodes

Han

Zhong

et al. 2020

Angewandte Chemie

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Developing electrolytes compatible with efficient and reversible cycling of electrodes is critical to the success of rechargeable Li metal batteries (LMBs). The Coulombic efficiencies and cycle lives of LMBs with ethylene carbonate (EC), dimethyl carbonate, ethylene sulfite (ES), and their combinations as electrolyte solvents show that in a binary‐solvent electrolyte the extent of electrolyte decomposition on the electrode surface is dependent on the solvent component that dominates the solvation sheath of Li+. This knowledge led to the development of an EC‐ES electrolyte exhibiting high performance for Li||LiFePO4 batteries. Carbonate molecules occupy the solvation sheath and improve the Coulombic efficiencies of both the anode and cathode. Sulfite molecules lead to desirable morphology and composition of the solid electrolyte interphase and extend the cycle life of the Li metal anode. The cooperation between these components provides a new example of electrolyte optimization for improved LMBs.

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Solvating power series of electrolyte solvents for lithium batteries

Abstract: From dictating the redox potential of electrolyte solvents to shaping the stability of solid-electrolyte interfaces, solvation plays a critical role in the electrochemistry of electrolytes.

Cited by 177 publications

References 40 publications

Critical Factors Dictating Reversibility of the Zinc Metal Anode

Critical Factors Dictating Reversibility of the Zinc Metal Anode

Challenges and Strategies to Advance High‐Energy Nickel‐Rich Layered Lithium Transition Metal Oxide Cathodes for Harsh Operation

Solvent Molecule Cooperation Enhancing Lithium Metal Battery Performance at Both Electrodes

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