Chemical Prelithiation of Negative Electrodes in Ambient Air for Advanced Lithium-Ion Batteries

Wang, Gongwei; Li, Feifei; Liú, Dan; Zheng, Dong; Luo, Ying; Qu, Deyu; Ding, Tianyao; Qu, Deyang

doi:10.1021/acsami.8b19416

Cited by 107 publications

(109 citation statements)

References 31 publications

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“…This process has been shown to provide both continuous extra capacity compensation and a stable SEI layer on the top surface of the Si cathode. [301] Note that careful control of prelithiation depth is critical because insufficient lithiation may not improve the initial CE, and overlithiation can cause Li nucleation and accumulation on the surface of the Si cathode. [302,303] Because of this, a highly controllable roll-to-roll scalable prelithiation technique of c-SiO x was developed.…”

Section: Prelithiation Techniquementioning

confidence: 99%

Recent Advances in Silicon‐Based Electrodes: From Fundamental Research toward Practical Applications

et al. 2021

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Section: Prelithiation Techniquementioning

confidence: 99%

Recent Advances in Silicon‐Based Electrodes: From Fundamental Research toward Practical Applications

et al. 2021

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“…[ 27–33 ] Typical prelithiation solutions consist of a strongly reductive chemicals such as lithium biphenylide (Li–Biph) and lithium naphthalenide (Li–Naph) [ 34–37 ] dissolved in a chemically stable solvent, such as dimethoxy ethane (DME) or tetrahydrofuran (THF). These prelithiation solutions have been successively used to prelithiate sulfur, [ 38 ] silicon, [ 38,39 ] phosphorous, [ 40 ] tin, [ 40 ] and hard carbon. [ 41 ] However, they failed to operate for graphite electrode, most likely due to the following two reasons: 1) all the lithiation reagents reported so far have a higher redox potential than Gr (≈0.2 V vs Li + /Li), and are therefore unable to prelithiate Gr; 2) the commonly used prelithiation solvents (such as organic ethers) are incompatible with graphite anode and may undergo a co‐intercalation reaction to destroy the Gr structure during prelithiation process.…”

Section: Introductionmentioning

confidence: 99%

Achieving Desirable Initial Coulombic Efficiencies and Full Capacity Utilization of Li‐Ion Batteries by Chemical Prelithiation of Graphite Anode

Shen

Yang

et al. 2021

Adv Funct Materials

Self Cite

128

105

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Chemical prelithiation is an effective approach to elevate the initial Coulombic efficiency (ICE) and energy utilization of Li‐ion battery electrodes. However, this approach fails to operate for the most commonly used graphite (Gr) anode, because all the prelithiation reagents reported so far have a much higher redox potential than Gr (≈0.2 V). Based on ionic solvation and coordination chemistry, for the first time, a new design strategy is proposed for prelithiation solution by selecting a strong electron‐donating, sterically hindered, and chemically stable solvent to tune the redox potential of prelithiation reagent and also to prevent the solvent co‐intercalation during prelithiation process, thus enabling a successful prelithiation of Gr anodes. By theoretical prediction and experimental evaluation, a chemical prelithiation solution, lithium biphenylide/2‐methyl tetrahydrofuran, is successfully developed, which can prelithiate Gr anodes accurately to a desired state in few minutes without destroying the lattice structure of Gr. When the prelithiated Gr anodes (pGr) are paired with the conventional cathodes, the full cells demonstrate significantly improved ICEs and higher energy densities than their counterparts using pristine Gr anodes, showing a great prospect for wide Li‐ion battery applications.

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“…[73] Those works highlighted the excellent stability of liquid anodes based on redox-active organic molecules, which is attributed to the stable redox reaction and the intact interfacial contact between the liquid electrode and the solid electrolyte. More recently, it was demonstrated that the liquid anodes with strong reducing power, that is, low redox potential, can be used for the chemical prelithiation of alloying-based anodes, such as tin, phosphorus, [74] and silicon-based anodes, [75] which are well-known to suffer from the low initial coulombic efficiency. The chemical prelithiation of the high-capacity anodes drastically improved the energy density of a full cell by minimizing the irreversible Li loss during the first charge process of the "formation cycle", thereby enabling the reversible utilization of a full fraction of the cathode materials.…”

Section: Recent Paradigm Shifts In Utilizing Redox-active Organic Commentioning

confidence: 99%

Redox‐Active Organic Compounds for Future Sustainable Energy Storage System

Lee

Hong

Kang

2020

Advanced Energy Materials

156

126

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to be promising for rechargeable battery chemistries that emit low carbon footprints during production. [4-8] Redox-active organic compounds, that is, chemicals composed of unlimited resources such as carbon, hydrogen, oxygen, nitrogen, and sulfur, among them have exhibited the great potential as a carbon-neutral option, possibly exploiting the bio-derived materials and not relying on the scarce transition metal resources, in all organic-based LIBs, owing to their chemical diversity and functional versatility. [6-8] Despite their promising potential and intensive research efforts to date, replacing the commercial electrodes in LIBs with these new electrode materials remains a great challenge due to the short cycle life and the low energy density in the electrode-and system-level. However, recent alternative approaches have demonstrated that the utilization of redox-active organic compounds in battery systems other than LIBs can be more promising, taking advantage of their chemical and functional flexibilities in diverse electrochemical configurations. In this essay, we highlight the progressive shift in exploiting the redox-active organic compounds in new battery platforms for future ESSs, as well as offer an overview of the advancements achieved during the past decade. 2. Basic Operating Mechanisms of Organic Electrode Materials The working principle of the redox-active organic compounds as active materials in electrodes can be classified into three categories, that is, n-type, [9] p-type, [10] and bipolar-type, [11] based on their capabilities to receive or release electrons in their neutral state during the electrochemical reaction. Figure 1 schematically illustrates the three types of redox reaction with the molecular structures of the representative redox-active compounds. [6,8,12] Most of the known redox-active organic compounds follow one or more of these redox mechanisms in rechargeable batteries. The n-type electrochemical reaction represents the reduction of the neutral-state organic compound electrodes, forming negatively charged molecular states, which can be reversed during the oxidation reaction. In lithium batteries, the n-type "cathodes" readily accept electrons and the corresponding number of Li-ions during the discharge process, thus generally require Li-containing anodes. Contrarily, the n-type "anodes" can be paired with the conventional LIB cathodes, such as LiMeO 2 (Menickel, cobalt, manganese, aluminum, etc.), LiFePO 4 , or LiMn 2 O 4 , which intrinsically Utilizing redox-active organic compounds for future energy storage system (ESS) has attracted great attention owing to potential cost efficiency and environmental sustainability. Beyond enriching the pool of organic electrode materials with molecular tailoring, recent scientific efforts demonstrate the innovations in various cell chemistries and configurations. Herein, recent major strategies to build better organic batteries, are highlighted: diversifying charge-carrying ions, modifying electrolytes, and utilizing liquid-type organic el...

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Chemical Prelithiation of Negative Electrodes in Ambient Air for Advanced Lithium-Ion Batteries

Cited by 107 publications

References 31 publications

Recent Advances in Silicon‐Based Electrodes: From Fundamental Research toward Practical Applications

Recent Advances in Silicon‐Based Electrodes: From Fundamental Research toward Practical Applications

Achieving Desirable Initial Coulombic Efficiencies and Full Capacity Utilization of Li‐Ion Batteries by Chemical Prelithiation of Graphite Anode

Redox‐Active Organic Compounds for Future Sustainable Energy Storage System

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