Enabling the conventional TFSI-based electrolytes for high-performance Mg/Li hybrid batteries by Mg electrode interfacial regulation

Zhang, Rupeng; Cui, Can; Xiao, Rang; Ruinan, L.; Mu, Tiansheng; Huo, Hua; Ma, Yulin; Yin, Geping; Zuo, Pengjian

doi:10.1016/j.cej.2022.136592

Cited by 7 publications

(11 citation statements)

References 29 publications

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“…Benefiting from the Cu 2+ (de)intercalation electronic structure evolution, Mo 6 S 8 demonstrates the best discharge specific capacity and is superior to other Mo 6 S 8 cathode-based secondary ion batteries in the literature, such as aluminum ion batteries (AIBs), magnesium ion batteries (MIBs), zinc ion batteries (ZIBs), sodium ion batteries (SIBs), and lithium-ion battery (LIB) systems (Figures f and S23–S25). ,,− …”

Section: Resultsmentioning

confidence: 99%

Accumulative Delocalized Mo 4d Electrons to Bound the Volume Expansion and Accelerate Kinetics in Mo₆S₈ Cathode for High-Performance Aqueous Cu²⁺ Storage

Ren,

Sun,

Lei

et al. 2023

ACS Nano

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Electronic structure defines the conductivity and ion absorption characteristics of a functional electrode, significantly affecting the charge transfer capability in batteries, while it is rarely thought to be involved in mesoscopic volume and diffusion kinetics of the host lattice for promoting ion storage. Here, we first correlate the evolution in electronic structure of the Mo 6 S 8 cathode with the ability to bound volume expansion and accelerate diffusion kinetics for high-performance aqueous Cu 2+ storage. Operando synchrotron energydispersive X-ray absorption spectroscopy reveals that accumulative delocalized Mo 4d electrons enhance the Mo−Mo interaction with distinctly contracting and uniformizing Mo 6 clusters during the reduction of Mo 6 S 8 , which potently restrain lattice expansion and release space to promote Cu 2+ diffusion kinetics. Operando synchrotron X-ray diffraction and comprehensive characterizations further validate the structural and electrochemical properties induced by the Cu 2+ intercalation electronic structure, endowing the Mo 6 S 8 cathode a high specific capacity with small volume expansion, fast ions diffusion, and long-term cycling stability.

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Section: Resultsmentioning

confidence: 99%

Accumulative Delocalized Mo 4d Electrons to Bound the Volume Expansion and Accelerate Kinetics in Mo₆S₈ Cathode for High-Performance Aqueous Cu²⁺ Storage

Ren,

Sun,

Lei

et al. 2023

ACS Nano

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“…For further verification of the effect of the I-rich interphase, the XPS analysis of Mg 2p and O 1s was conducted for bare Mg and LiI–Mg after the cycle (Figure c, d). For bare Mg, the main two peaks of MgO (50.3 eV) and MgCO 3 (51.9 eV) came from the inevitable oxidation of Mg and the side reaction between Mg anode and electrolytes . These undesired ingredients formed the compact and Mg 2+ -nonconducting film on the anode, hampering the continuous anode reaction and causing a near absent fresh Mg signal.…”

Section: Resultsmentioning

confidence: 99%

Interfacial Reconstruction Toward Reversible Mg Anode in Conventional Electrolytes

Wang,

Huang,

et al. 2023

ACS Appl. Mater. Interfaces

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Rechargeable magnesium batteries are considered with great potential as sustainable, economic-friendly, safe energy storage techniques. Whereas, the Mg metal anode exhibits limited plating/stripping behavior in the conventional electrolytes due to the severe passivation. Herein, a facile LiI solution treatment is reported to reconstruct the interphase between Mg metal anode and electrolytes, converting the original passivation film to I-riched solid electrolyte interphase with the ability of rapid Mg2+ migration, which can reduce the overpotential for Mg anode plating/stripping from 2 to 0.4 V at 0.1 mA cm–2. In addition, Li+ from the LiI precursor can be released and shuttles to the Mo6S8 cathode side, promoting cointercalation of Mg2+. With the simultaneous improvement of the anode and cathode, the Mg//Mo6S8 full cell delivers a decreasing voltage hysteresis (0.1 V) and much enhanced specific capacity (80.8 mAh g–1). This work provides a maneuverable anode treatment for constructing a passivation-against interphase between Mg metal anode and the conventional electrolytes, contributing an insight for the development toward high-performance Mg batteries.

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“…They cause notorious passivation phenomenon, poor ionic conductivity, high overpotential, and low Coulombic efficiency (CE) in rechargeable Mg batteries . Currently, building an artificial solid-electrolyte interphase (SEI) layer on the Mg anode surface is the most common solution to prevent passivation. − However, SEI may not be stable under continuous volumetric or morphological change of the anode during Mg plating/stripping, and it cannot address the low ionic conductivity problem in chlorine-free electrolytes, such as Mg(HMDS) 2 -based electrolyte. , …”

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

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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.

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Enabling the conventional TFSI-based electrolytes for high-performance Mg/Li hybrid batteries by Mg electrode interfacial regulation

Cited by 7 publications

References 29 publications

Accumulative Delocalized Mo 4d Electrons to Bound the Volume Expansion and Accelerate Kinetics in Mo₆S₈ Cathode for High-Performance Aqueous Cu²⁺ Storage

Accumulative Delocalized Mo 4d Electrons to Bound the Volume Expansion and Accelerate Kinetics in Mo₆S₈ Cathode for High-Performance Aqueous Cu²⁺ Storage

Interfacial Reconstruction Toward Reversible Mg Anode in Conventional Electrolytes

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

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Enabling the conventional TFSI-based electrolytes for high-performance Mg/Li hybrid batteries by Mg electrode interfacial regulation

Cited by 7 publications

References 29 publications

Accumulative Delocalized Mo 4d Electrons to Bound the Volume Expansion and Accelerate Kinetics in Mo6S8 Cathode for High-Performance Aqueous Cu2+ Storage

Accumulative Delocalized Mo 4d Electrons to Bound the Volume Expansion and Accelerate Kinetics in Mo6S8 Cathode for High-Performance Aqueous Cu2+ Storage

Interfacial Reconstruction Toward Reversible Mg Anode in Conventional Electrolytes

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

Contact Info

Product

Resources

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Accumulative Delocalized Mo 4d Electrons to Bound the Volume Expansion and Accelerate Kinetics in Mo₆S₈ Cathode for High-Performance Aqueous Cu²⁺ Storage

Accumulative Delocalized Mo 4d Electrons to Bound the Volume Expansion and Accelerate Kinetics in Mo₆S₈ Cathode for High-Performance Aqueous Cu²⁺ Storage