Realizing horizontal magnesium platelet deposition and suppressed surface passivation for high-performance magnesium metal batteries

Yang, Gaoliang; Li, Yuanjian; Wang, Jianbiao; Lum, Yanwei; Lim, Carina Yi Jing; Ng, Man-Fai; Zhang, Chang; Chang, Zhi; Zhang, Zhonghan; Handoko, Albertus D.; Ghosh, Tanmay; Li, Shuzhou; Sofer, Zdenek; Liu, Wei; Yao, Yan; Seh, Zhi Wei

doi:10.1039/d3ee02317f

Cited by 15 publications

(2 citation statements)

References 62 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…Such energy density and stability are at the forefront of simple Mg-salt electrolytes that store Mg 2+ (Figure e and Table S2). ,,− We tested this electrolyte in different full cells to further assess its compatibility with a chalcogenide-based cathode and high-voltage Prussian blue analogue cathode. The Mg||Mo 6 S 8 full cell with Mg(HFIP) 2 electrolyte demonstrates a reduced polarization, improved rate performance (Figures S29 and S30), and outstanding stable cycling at 0.5 C (Figure f).…”

Section: Resultsmentioning

confidence: 99%

Redesigning Solvation Structure toward Passivation-Free Magnesium Metal Batteries

Long,

Liu,

et al. 2024

ACS Nano

View full text Add to dashboard Cite

Simple magnesium (Mg) salt solutions are widely considered as promising electrolytes for next-generation rechargeable Mg metal batteries (RMBs) owing to the direct Mg2+ storage mechanism. However, the passivation layer formed on Mg metal anodes in these electrolytes is considered the key challenge that limits its applicability. Numerous complex halogenide additives have been introduced to etch away the passivation layer, nevertheless, at the expense of the electrolyte’s anodic stability and cathodes’ cyclability. To overcome this dilemma, here, we design an electrolyte with a weakly coordinated solvation structure which enables passivation-free Mg deposition while maintaining a high anodic stability and cathodic compatibility. In detail, we successfully introduce a hexa-fluoroisopropyloxy (HFIP–) anion into the solvation structure of Mg2+, the weakly [Mg–HFIP]+ contact ion pair facilitates Mg2+ transportation across interfaces. As a consequence, our electrolyte shows outstanding compatibility with the RMBs. The Mg||PDI–EDA and Mg||Mo6S8 full cells use this electrolyte demonstrating a decent capacity retention of ∼80% over 400 cycles and 500 cycles, respectively. This represents a leap in cyclability over simple electrolytes in RMBs while the rest can barely cycle. This work offers an electrolyte system compatible with RMBs and brings deeper understanding of modifying the solvation structure toward practical electrolytes.

show abstract

Section: Resultsmentioning

confidence: 99%

Redesigning Solvation Structure toward Passivation-Free Magnesium Metal Batteries

Long,

Liu,

et al. 2024

ACS Nano

View full text Add to dashboard Cite

show abstract

“…The commercially available chloride-free Mg salts, such as magnesium bis(trifluoromethane sulfonyl)imide (Mg(TFSI) 2 ), magnesium trifluoromethanesulfonate (Mg(OTf) 2 ), and magnesium bis(hexamethyldisilazide) (Mg(HMDS) 2 ), have great potential to be used in low-cost Mg electrolytes. − However, due to the low reduction potential (−2.37 V vs standard hydrogen electrode) of the Mg anode and high charge density of Mg 2+ (∼120 C mm –3 ), these commercial Mg salts either react with Mg anode or exhibit limited solubility in compatible ethereal solvents, such as tetrahydrofuran (THF), 1,2-dimethoxyethane (DME), and diglyme (DG). They cause notorious passivation phenomenon, poor ionic conductivity, high overpotential, and low Coulombic efficiency (CE) in rechargeable Mg batteries .…”

Section: Introductionmentioning

confidence: 99%

Releasing Free Anions by High Donor Number Cosolvent in Noncorrosive Electrolytes of Commercially Available Magnesium Salts

Xiao,

Zhang,

Fan

et al. 2024

ACS Appl. Mater. Interfaces

View full text Add to dashboard Cite

Passivation of the magnesium (Mg) anode in the chloridefree electrolytes using commercially available Mg salts is a critical issue for rechargeable Mg batteries. Herein, a high donor number cosolvent of 1methylimidazolium (MeIm) is introduced into Mg(TFSI) 2 -and Mg-(HMDS) 2 -based electrolytes to address the passivation problem and realize highly reversible Mg plating/stripping. Theoretical calculations and experimental characterization results reveal that the strong coordination ability of MeIm with Mg 2+ can weaken the anion−cation interactions and promote the formation of free anions that have higher reduction stability, thus significantly suppressing anion-derived passivation layer formation. By adding MeIm cosolvent into Mg(TFSI) 2 -based electrolyte, the average Coulombic efficiency of the Mg//Cu cell is increased from less than 20% to over 90%, and the Mg//Mg cell can stably cycle for over 800 h with a low overpotential. In the MeIm-regulated Mg(HMDS) 2 -based electrolyte, the solvation structure change, featured by an effective separation of Mg 2+ and HMDS − , greatly increases the ionic conductivity by more than 30 times. This solvation structure regulation strategy for noncorrosive electrolytes of commercially available Mg salts has a great potential for application in future rechargeable Mg metal batteries.

show abstract

Challenges and Progress in Rechargeable Magnesium‐Ion Batteries: Materials, Interfaces, and Devices

Wang,

Zhang,

Hao

et al. 2024

Adv Funct Materials

View full text Add to dashboard Cite

Rechargeable magnesium‐ion batteries (RMBs) have garnered increasing research interest in the field of post‐lithium‐ion battery technologies owing to their potential for high energy density, enhanced safety, cost‐effectiveness, and material resourcefulness. Despite substantial advancements in RMB research, a number of intrinsic challenges remain unresolved, such as the strong Coulombic interaction between Mg2+ and the host crystal structure of cathode materials, sluggish Mg2+ diffusion kinetic, poor electrolyte compatibility, and the formation of passivation films on the Mg anode interface. These issues hinder the commercial applications of RMBs. This review provides a comprehensive overview of the progress in key areas of RMB research, including representative magnesium‐ion storage cathode/anode materials and magnesium‐ion conducting electrolytes. Additionally, recent developments in electrode‐electrolyte interface regulations and pouch‐cell fabrication are outlined, highlighting current challenges and the implementation of effective solutions. Finally, future research directions are proposed to guide the development of high‐performance RMBs with practical applications.

show abstract

Realizing horizontal magnesium platelet deposition and suppressed surface passivation for high-performance magnesium metal batteries

Abstract: Rechargeable magnesium batteries (RMBs) are emerging as promising alternatives to lithium-ion batteries due to the high volumetric capacity and natural abundance. However, challenges arising from severe passivation and uneven deposition...

Cited by 15 publications

References 62 publications

Redesigning Solvation Structure toward Passivation-Free Magnesium Metal Batteries

Redesigning Solvation Structure toward Passivation-Free Magnesium Metal Batteries

Releasing Free Anions by High Donor Number Cosolvent in Noncorrosive Electrolytes of Commercially Available Magnesium Salts

Challenges and Progress in Rechargeable Magnesium‐Ion Batteries: Materials, Interfaces, and Devices

Contact Info

Product

Resources

About