Insights into interfacial speciation and deposition morphology evolution at Mg-electrolyte interfaces under practical conditions

Song, Zuwei; Zhang, Zhonghua; Du, Aobing; Dong, Shamu; Li, Guicun; Cui, Guanglei

doi:10.1016/j.jechem.2020.02.019

Cited by 32 publications

(16 citation statements)

References 34 publications

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“…Some work has also demonstrated that cycling Mg metal in this electrolyte can cause dendrite growth (Ding et al, 2018), although the deposits are not long and branch-like and have other formation characteristics that are different from dendrites. However, it is now more well-known that spherical Mg deposits can grow through separators and create soft-shorts in many different Mg electrolytes (Yoo et al, 2017;Merrill and Schaefer, 2019;Eaves-Rathert et al, 2020;Song et al, 2020). Results in the current work support the observation that soft-shorting is the origin of the overpotential decrease in Mg-Mg symmetric cells.…”

Section: Introductionsupporting

confidence: 83%

“…This characteristic of the symmetric cells is being discussed in the literature-some researchers initially said that a sharp overpotential decrease may be due to stabilization of the interface, not necessarily shorting (Tutusaus et al, 2017). However, more recent studies have demonstrated Mg growth through separators indicating clearer soft-shorting phenomena (Yoo et al, 2017;Merrill and Schaefer, 2019;Eaves-Rathert et al, 2020;Song et al, 2020). For the samples here, we also believe that a soft-short may have occurred as pieces of the glass fiber separator can be seen attached to deposits in Figure 5B.…”

Section: Discussionsupporting

confidence: 60%

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Al2O3 Thin Films on Magnesium: Assessing the Impact of an Artificial Solid Electrolyte Interphase

et al. 2021

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Among the many emerging technologies under investigation as alternatives to the successful Lithium-ion battery, the magnesium battery is promising due to the wide availability of magnesium, its high volumetric capacity, and the possibility for safety improvements. One of the largest challenges facing rechargeable magnesium batteries is the formation of a passivation layer at the Mg metal anode interface when reactive species in the electrolyte are reduced at the electrode-electrolyte interface. To control the solid electrolyte interphase in Lithium batteries, protective layers called artificial solid electrolyte interphase (ASEI) layers have been successful in improving Li metal anode performance. The approach of protecting Mg metal anodes from electrolyte degradation has been demonstrated by fewer studies in the literature than Li systems. In this work, we discuss the properties of Al2O3 thin films deposited using atomic layer deposition as an artificial solid electrolyte interphase at the Mg anode. Our results demonstrate that Al2O3 does prevent electrolyte degradation due to the reductive nature of Mg. However, undesirable properties such as defects and layer breakdown lead to Mg growth that causes soft-shorting. The soft-shorting occurs with and without the protection layer, indicating the ALD layer does not prevent it and hinders Al2O3 from being an ideal candidate for a protection layer. Crucial effects of this layer on Mg electrochemistry at the interface were observed, including growth of Mg deposits leading to soft-shorting of the cell whose morphology showed a dependence on the Al2O3 layer. These results may provide guidelines for the future design and development of protective ASEI layers for Mg anodes.

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Section: Introductionsupporting

confidence: 83%

Section: Discussionsupporting

confidence: 60%

Al2O3 Thin Films on Magnesium: Assessing the Impact of an Artificial Solid Electrolyte Interphase

et al. 2021

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“…Our previous work shows that both the pure Mg 2+ and hybrid Mg 2+ /A + electrolytes had good interface compatibility with the Mg anode . The concentration of the TFSI – anion was well-controlled as TFSI – has a tendency to decompose on the Mg anode. − …”

Section: Resultsmentioning

confidence: 96%

Rechargeable Mg²⁺/Li⁺, Mg²⁺/Na⁺, and Mg²⁺/K⁺ Hybrid Batteries Based on Layered VS₂

Peng

et al. 2021

ACS Appl. Mater. Interfaces

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Rechargeable Mg batteries have great potential in next-generation scalable energy-storage applications, but the electrochemical performance is limited by the Mg-intercalation cathodes. Hybrid batteries based on dual-cation (Mg2+ and alkali metal cations) electrolytes would not only improve the electrochemical performance but also induce the co-intercalation of Mg2+ with alkali metal cations. As previous reports overwhelmingly focus on Mg2+/Li+ hybrid batteries, in this work, Mg2+/Na+ and Mg2+/K+ hybrid batteries are constructed using a typical layered VS2 cathode and studied in comparison with Mg2+/Li+ batteries. It is observed that Mg2+ could co-intercalate into VS2 with Li+, Na+, or K+. However, Mg-intercalation is irreversible in the Mg2+/Li+ system, and co-intercalation of Mg2+ and K+ would cause a collapse of VS2. Comparatively, the co-intercalation of Mg2+ and Na+ into VS2 exhibits the highest reversibility, and the Mg2+/Na+ hybrid battery shows the best cycling stability without capacity fading within 1000 cycles. Our work highlights the co-intercalation reversibility of a non-pre-expanded layered disulfide cathode and delivers insights for the development of high-performance rechargeable Mg metal batteries.

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“…It is believed that the water and oxygen contents in glove box, the purity of as‐received salts are important factors in determining Mg deposition/dissolution properties. [ 42 ] For Grignard‐based magnesium organohaloaluminate electrolytes, trace water will affect the overpotential for Mg deposition by coordinating the Mg ions and retard the formation of the electroactive species for Mg deposition. [ 43 ] For the magnesium (II) bis (trifluoromethane sulfonyl) imide (Mg(TFSI) 2 )/diglyme electrolyte, trace H 2 O (≤3 ppm) can suppress the reversibility of the Mg anode by forming a passivated film containing MgO and Mg(OH) 2 and slowing deposition kinetics due to the strong solvation of Mg 2+ by water.…”

Section: Electrolytic Conditioningmentioning

confidence: 99%

A Review of Magnesium Aluminum Chloride Complex Electrolytes for Mg Batteries

Guan

Huo

et al. 2021

Adv Funct Materials

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Developing suitable electrolytes with high oxidation decomposition potential, low cost, and good compatibility with electrode materials has been a critical challenge in realizing practical magnesium batteries. The emerging magnesium aluminum chloride complex (MACC) electrolytes based on inorganic chloride salts exhibit high Coulombic efficiencies for magnesium batteries. This review summarizes recent studies of MACC electrolytes, focusing on the synthesis, characterization, and chemical environment of Mg species, electrolytic conditioning of electrolytes, and their application in typical magnesium batteries. The electrolyte evolution and influencing factor of electrolytic conditioning are discussed, and several kinds of conditioning‐free MACC electrolytes are further introduced. Finally, future trends and perspectives in this field are discussed.

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Insights into interfacial speciation and deposition morphology evolution at Mg-electrolyte interfaces under practical conditions

Cited by 32 publications

References 34 publications

Al2O3 Thin Films on Magnesium: Assessing the Impact of an Artificial Solid Electrolyte Interphase

Al2O3 Thin Films on Magnesium: Assessing the Impact of an Artificial Solid Electrolyte Interphase

Rechargeable Mg²⁺/Li⁺, Mg²⁺/Na⁺, and Mg²⁺/K⁺ Hybrid Batteries Based on Layered VS₂

A Review of Magnesium Aluminum Chloride Complex Electrolytes for Mg Batteries

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Insights into interfacial speciation and deposition morphology evolution at Mg-electrolyte interfaces under practical conditions

Cited by 32 publications

References 34 publications

Al2O3 Thin Films on Magnesium: Assessing the Impact of an Artificial Solid Electrolyte Interphase

Al2O3 Thin Films on Magnesium: Assessing the Impact of an Artificial Solid Electrolyte Interphase

Rechargeable Mg2+/Li+, Mg2+/Na+, and Mg2+/K+ Hybrid Batteries Based on Layered VS2

A Review of Magnesium Aluminum Chloride Complex Electrolytes for Mg Batteries

Contact Info

Product

Resources

About

Rechargeable Mg²⁺/Li⁺, Mg²⁺/Na⁺, and Mg²⁺/K⁺ Hybrid Batteries Based on Layered VS₂