Electrostatic Shielding Guides Lateral Deposition for Stable Interphase toward Reversible Magnesium Metal Anodes

Wang, Jiahe; Zhao, Wanyu; Dou, Huanglin; Wan, Bingxin; Zhang, Yijie; Li, Wanfei; Zhao, Xiaoli; Yang, Xiaowei

doi:10.1021/acsami.0c03603

Cited by 40 publications

(30 citation statements)

References 40 publications

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“…To investigate the competitive TFSI – /rPDI adsorption behavior, we first exploited alternating current voltammetry (ACV) to probe the potential of zero charge (PZC), which is strongly related to the adsorbed species at the interface. As shown in Figure S1b, the PZC shifted to a more positive value (1.00 V) with the addition of rPDI compared to pristine electrolyte (0.88 V), indicating that rPDI anions adsorbed more strongly on the Mg surface than TFSI – , which is consistent with other anion-adsorbed systems reported in previous literature. − The preferential adsorption of rPDI on the Mg surface was further confirmed via density functional theory (DFT) calculations. From Figure a, the adsorption energy of rPDI is −0.872 eV, which is much higher than that of TFSI – (−0.359 eV), indicating that rPDI is more likely to occupy the Mg anode surface.…”

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confidence: 87%

Non-passivating Anion Adsorption Enables Reversible Magnesium Redox in Simple Non-nucleophilic Electrolytes

et al. 2021

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Magnesium batteries suffer from low power density and poor cycle life due to severe Mg passivation. Using nucleophilic electrolytes is effective to stabilize the Mg anode, but it prohibits the use of organic and conversion cathodes due to chemical reactivity. Here, we report an effective non-passivating anion additive, the reduced perylene diimide–ethylene diamine (rPDI), to enable fast and reversible Mg deposition/dissolution in a simple non-nucleophilic electrolyte. The rPDI additive exhibits higher adsorption energy than the TFSI– salt on the Mg surface, preventing TFSI– decomposition and Mg anode passivation. Using 0.2 mM rPDI additives, we demonstrated a Mg–organic full cell achieving a high power density (2.0 mW cm–2) and a stable cycle life (>200 cycles). Our study provides a facile and effective strategy for non-nucleophilic electrolytes, enabling the combination of Mg anode with a wide variety of organic and conversion cathodes beyond intercalation chemistries.

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confidence: 87%

Non-passivating Anion Adsorption Enables Reversible Magnesium Redox in Simple Non-nucleophilic Electrolytes

et al. 2021

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“…Electrostatic shielding is also a good strategy to modify the magnesium anodes. Wang and co-workers obtained an alleviated passivation on the magnesium anodes by adding cathodically stable cations, namely Pyr 14 + , in the electrolytes (Figure e) . After cycling, a dark, thin, and dense film forms on the magnesium anode surface.…”

Section: Anode Materials Improvement Strategiesmentioning

confidence: 97%

“…Wang and co-workers obtained an alleviated passivation on the magnesium anodes by adding cathodically stable cations, namely Pyr 14 + , in the electrolytes (Figure 12e). 95 After cycling, a dark, thin, and dense film forms on the magnesium anode surface. Pyr 14 + replaces Mg-ions on the electrode to form an electrostatic shielding which can alleviate the concentration of Mg-ions and lead to lateral Mg deposition.…”

Section: Anode Materials Improvement Strategiesmentioning

confidence: 99%

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Current Design Strategies for Rechargeable Magnesium-Based Batteries

et al. 2021

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As a next-generation electrochemical energy storage technology, rechargeable magnesium (Mg)-based batteries have attracted wide attention because they possess a high volumetric energy density, low safety concern, and abundant sources in the earth's crust. While a few reviews have summarized and discussed the advances in both cathode and anode materials, a comprehensive and profound review focusing on the material design strategies that are both representative of and peculiar to the performance improvement of rechargeable Mg-based batteries is rare. In this mini-review, all nine of the material design strategies and approaches to improve Mgion storage properties of cathode materials have been comprehensively examined from both internal and external aspects. Material design concepts are especially highlighted, focusing on designing "soft" anion-based materials, intercalating solvated or complex ions, expanding the interlayer of layered cathode materials, doping heteroatoms into crystal lattice, size tailoring, designing metastable-phase materials, and developing organic materials. To achieve a better anode, strategies based on the artificial interlayer design, efficient electrolyte screening, and alternative anodes exploration are also accumulated and analyzed. The strategy advances toward Mg−S and Mg−Se batteries are summarized. The advantages and disadvantages of allcollected material design strategies and approaches are critically discussed from practical application perspectives. This minireview is expected to provide a clear research clue on how to rationally improve the reliability and feasibility of rechargeable Mg-based batteries and give some insights for the future research of Mg-based batteries as well as other multivalent-ion battery chemistries.

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“…Alkali-metal and Zn-metal anodes have been extensively studied in the past few years for alkali-metal and Zn-metal batteries, respectively. In addition to alkali-metal and Znmetal anodes, Ca-metal, Mg-metal, Al-metal, and Fe-metal anodes have also been probed recently for Ca-metal, [36,140] Mgmetal, [35,[141][142][143][144][145] Al-metal, [37] and Fe-metal batteries, [38] respectively. However, their investigation is limited.…”

Section: Other Metal Anodesmentioning

confidence: 99%

Recent Advances of Emerging 2D MXene for Stable and Dendrite‐Free Metal Anodes

Wei

Yuan

et al. 2020

Adv Funct Materials

176

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Metal anodes based on a plating/stripping electrochemistry such as metallic Li, Na, K, Zn, Mg, Ca, Al, and Fe have attracted widespread attention over the past several years because of their high theoretical specific capacity, low electrochemical potential, and superior electronic conductivity. Metal anodes can be paired with cathodes to construct high-energy-density rechargeable metal batteries. However, inherent issues including large volume changes, uncontrollable growth of dangerous dendrites, and an unstable solid electrolyte interphase (SEI) hinder their further development. MXene as an emerging 2D material has shown great potential to address the inherent issues of metal anodes due to its 2D structure, abundant surface functional groups, and the ability to construct macroscopic architectures. To date, under the assistance of MXene, various strategies have been proposed to achieve stable and dendrite-free metal anodes, such as MXene-based host design, designing metalphilic MXene-based substrates, modifying the metal surface with MXene, constructing MXene arrays, and decorating separators or electrolytes with MXene. Herein the applications and advances of MXene in stable and dendrite-free metal anodes are carefully summarized and analyzed. Some perspectives and outlooks for future research are also proposed.

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Electrostatic Shielding Guides Lateral Deposition for Stable Interphase toward Reversible Magnesium Metal Anodes

Cited by 40 publications

References 40 publications

Non-passivating Anion Adsorption Enables Reversible Magnesium Redox in Simple Non-nucleophilic Electrolytes

Non-passivating Anion Adsorption Enables Reversible Magnesium Redox in Simple Non-nucleophilic Electrolytes

Current Design Strategies for Rechargeable Magnesium-Based Batteries

Recent Advances of Emerging 2D MXene for Stable and Dendrite‐Free Metal Anodes

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