Interfacial Model Deciphering High‐Voltage Electrolytes for High Energy Density, High Safety, and Fast‐Charging Lithium‐Ion Batteries

Zou, Yeguo; Cao, Zhen; Zhang, Junli; Wahyudi, Wandi; Wu, Yingqiang; Liu, Gang; Li, Qian; Cheng, Haoran; Zhang, Dongyu; Park, Geon Tae; Cavallo, Luigi; Anthopoulos, Thomas D.; Wang, Limin; Sun, Yang‐Kook; Ming, Jun

doi:10.1002/adma.202102964

Cited by 169 publications

(125 citation statements)

References 79 publications

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“…(1) the component of the CEI layer is modified with existence of AN, where formation of high-voltage unstable components resulting from the decomposition of carbonate electrolyte are effectively suppressed . (2) The interactions among lithium ion, solvent molecules, and anions play critical roles in the interfacial structure, leading to different electrochemical performance . As the AN molecule binds with Li + more tightly compared to the carbonate molecule, part of the carbonate solvent molecule is expelled from the solvation structure of the lithium ion.…”

Section: Results and Discussionmentioning

confidence: 99%

“…34 (2) The interactions among lithium ion, solvent molecules, and anions play critical roles in the interfacial structure, leading to different electrochemical performance. 51 As the AN molecule binds with Li + more tightly compared to the carbonate molecule, part of the carbonate solvent molecule is expelled from the solvation structure of the lithium ion. As a result, the decomposition of the solvent is reduced and the CEI layer rich in high-voltage stable inorganic components is generated.…”

Section: ■ Results and Discussionmentioning

confidence: 99%

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Stable Electrode/Electrolyte Interface for High-Voltage NCM 523 Cathode Constructed by Synergistic Positive and Passive Approaches

Shi

Zheng

Xiong

et al. 2021

ACS Appl. Mater. Interfaces

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Increasing the working voltage of lithium-ion batteries (LIBs) is an efficient way to increase energy density. However, high voltage triggers excessive electrolyte decomposition at the electrode−electrolyte interfaces, where the electrochemical performance such as cyclic stability and rate capability is seriously deteriorated. A new synergistic positive and passive approach is proposed in this work to construct a stable electrode−electrolyte interface at high voltage. As a positive approach, inorganic lithium sulfide salt (Li 2 S) is used as an electrolyte additive to build a stable cathode electrolyte interface (CEI) at the LiNi 0.5 Co 0.2 Mn 0.3 O 2 (NCM523) cathode surface. In a passive way, acetonitrile (AN) is applied as a solvent additive to suppress oxidative decomposition of a carbonate electrolyte via preferential solvation with a lithium ion. Because of the synergistic interaction between the positive and passive approaches, the cyclic stabilities of NCM523/Li cells improved with a tiny amount of Li 2 S (0.01 mg mL −1 ) and AN (0.5 vol %). The capacity retention increased to 80.74% after 200 cycles compared to the cells with the blank electrolyte (67.98%) and AN-containing electrolyte (75.8%). What is more, the capacity retention of the NCM523/graphite full cell is increased from 65 to 81% with the addition of the same amount of Li 2 S and AN after 180 cycles. The mechanism is revealed on the basis of the theoretical calculations and various characterizations. The products derived from the preferential adsorption and oxidation of Li 2 S on the surface of NCM523 effectively increase the content of inorganic ingredients. However, the presence of AN prevents oxidation of the solvent. This study provides new principle guiding studies on a high-voltage lithium-ion battery with excellent electrochemical performance.

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Section: Results and Discussionmentioning

confidence: 99%

Section: ■ Results and Discussionmentioning

confidence: 99%

Stable Electrode/Electrolyte Interface for High-Voltage NCM 523 Cathode Constructed by Synergistic Positive and Passive Approaches

Shi

Zheng

Xiong

et al. 2021

ACS Appl. Mater. Interfaces

View full text Add to dashboard Cite

show abstract

“…The interactions among anions and cations, solvents, co‐solvents, and additives can be changed dynamically in the whole complex electrolyte system, which brings great difficulties for us to analyze the behavior of the electrolytes 26,27 . Fortunately, advanced characterization methods and computational simulations have been developed to analyze the Li + solvation structure for studying the behavior of electrolytes 28–31 …”

Section: Introductionmentioning

confidence: 99%

“…As a function of Li salt in solvents with additives, Li + solvation structure could determine many properties of the electrolytes, and especially the structural model Li + [solvent] x [additive] y [anion] has been proposed to explain battery performance 30,32 . The precise control of solvation structure can eliminate the adverse effects of some solvent molecules 33–38 .…”

Section: Introductionmentioning

confidence: 99%

“…26,27 Fortunately, advanced characterization methods and computational simulations have been developed to analyze the Li + solvation structure for studying the behavior of electrolytes. [28][29][30][31] As a function of Li salt in solvents with additives, Li + solvation structure could determine many properties of the electrolytes, and especially the structural model Li +…”

Section: Introductionmentioning

confidence: 99%

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Structural regulation chemistry of lithium ion solvation for lithium batteries

Wang

et al. 2022

EcoMat

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The performance of Li batteries is influenced by the Li+ solvation structure, which can be precisely adjusted by the components of the electrolytes. In this review, we overview the strategies for optimizing electrolyte solvation structures from three different perspectives, including anion regulation, binding energy regulation, and additive regulation. These strategies can optimize the composition of the electrode‐electrolyte interface, enhance the anti‐oxidative stability of electrolytes as well as regulate the behaviors of anions, solvents, and Li+ during the cycling process. Moreover, we also provide our insights into these aspects as well as present perspectives on high‐performance Li batteries.

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Li‐Rich Mn–Mg Layered Oxide as a Novel Ni‐/Co‐Free Cathode

Lee

Park

Cho

et al. 2022

Adv Funct Materials

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Although Li2MnO3 exhibits high capacity via anionic oxygen redox, it suffers from rapid capacity decay owing to structural disordering accompanying irreversible Mn migration and O2 release. To promote the reversibility of the anionic redox reaction, Li1.8Mg0.3Mn0.9O3 as a novel cathode material, prepared by partially substituting Li+ and Mn4+ of Li2MnO3 with the redox‐inactive Mg2+ as a structural stabilizer is proposed. Li1.8Mg0.3Mn0.9O3 delivers a high specific capacity and energy density of ≈310 mAh g−1 and ≈915 Wh kg−1, respectively. In particular, the power‐capability and cycle performance of Li1.8Mg0.3Mn0.9O3 greatly surpass those of Li2MnO3. Through first‐principles calculations and various experiments, it is revealed that Mg substitution effectively suppresses the Mn migration by stabilizing Mn cations in the original sites at the charged state. The energetically stabilized layered structure disfavors the distortion of the MnO6 octahedra, which induces the oxygen dimer (OO) formation through the metal–oxygen decoordination, thus mitigating oxygen release.

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Interfacial Model Deciphering High‐Voltage Electrolytes for High Energy Density, High Safety, and Fast‐Charging Lithium‐Ion Batteries

Cited by 169 publications

References 79 publications

Stable Electrode/Electrolyte Interface for High-Voltage NCM 523 Cathode Constructed by Synergistic Positive and Passive Approaches

Stable Electrode/Electrolyte Interface for High-Voltage NCM 523 Cathode Constructed by Synergistic Positive and Passive Approaches

Structural regulation chemistry of lithium ion solvation for lithium batteries

Li‐Rich Mn–Mg Layered Oxide as a Novel Ni‐/Co‐Free Cathode

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