A weakly ion pairing electrolyte designed for high voltage magnesium batteries

Li, Chang; Guha, Rishabh D.; Shyamsunder, Abhinandan; Persson, Kristin A.; Nazar, Linda F.

doi:10.1039/d3ee02861e

Cited by 12 publications

(4 citation statements)

References 52 publications

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“…The EIS profiles are fitted by the equivalent circuit (Figure S20, Supporting Information). [56] The Mg/Mg cell with the MBTO-2 electrolyte exhibits a distinct semicircle after cycling (Figure 5l). This semicircle could be further resolved into two semicircles (R SEI and R ct ) at high and medium frequencies.…”

Section: Resultsmentioning

confidence: 99%

Asymmetric SO₃CF₃⁻‐Grafted Boron‐Center Anion Enables Boron‐Containing Interphase for High‐Performance Rechargeable Mg Batteries

Huang,

Tan,

Chen

et al. 2024

Adv Funct Materials

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Mg(SO3CF3)2 (Mg(OTf)2) is a simple and cost‐effective magnesium salt, which can promote the future applications of rechargeable magnesium batteries (RMBs). However, the simple Mg(OTf)2/ether electrolytes suffer from poor electrochemical properties due to the low solubility of Mg(OTf)2 and the serious decomposition passivation of the [Mg2+‐OTf−] ion pair on Mg. Herein, the OTf− anion is successfully grafted on low‐cost fluoride boronic esters (B(OCxHyF2x‐y+1)3) to obtain the asymmetric and weak‐coordination boron‐center [B(OCxHyF2x‐y+1)3OTf]− anion in ether electrolytes. The ‐OCH2CF3 (TFE) groups in B(TFE)3 effectively realize the charge delocalization of the OTf− and B‐O plane, restraining the independent decomposition of the [Mg2+‐OTf−] ion pair. The co‐decomposition of the asymmetric [B(TFE)3OTf]− induces the formation of the B‐containing organic/inorganic interphase, thus achieving a reversible Mg plating/stripping. After the further solubilization reaction, the obtained electrolyte exhibits a high average coulombic efficiency of 98.13% and long‐term cycling stability (1000 h). Notably, the long cycling life (capacity retention of 90.2% after 600 cycles at 1 C) and high‐rate capacity (43.0 mAh g−1 at 5 C) of the Mg/Mo6S8 full cell demonstrate a favorable electrolyte/cathode compatibility. This work brings new insights to design the new‐type and low‐cost Mg‐salts and high‐performance electrolytes for commercial RMBs.

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Section: Resultsmentioning

confidence: 99%

Asymmetric SO₃CF₃⁻‐Grafted Boron‐Center Anion Enables Boron‐Containing Interphase for High‐Performance Rechargeable Mg Batteries

Huang,

Tan,

Chen

et al. 2024

Adv Funct Materials

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“…This is still an ongoing challenge that awaits more careful design of electrolytes. Inspiringly, the recent discovery of viable cosolvents, either methoxyethyl‐amine [ 33 ] or triethyl phosphate, [ 50 ] has demonstrated its feasibility to enable stable cycling for up to 3.5 V and up to 400 cycles.…”

Section: The Compatibility Between Cathode and Electrolytementioning

confidence: 99%

“…Furthermore, the complicated reaction mechanism for Mg 2+ desolvation calls for more dedicated investigation and delicate structural design of both the inner shell and outer shell of the solvation structure. [ 50 ] While cathode interfacial chemistries in RMBs remain largely unexplored, the interfacial process at the Mg anode site has been intensively studied. The established principle and mechanism for Mg 2+ de‐solvation at the anode site offer valuable insights for a similar cathode process.…”

Section: Perspectives and Challengesmentioning

confidence: 99%

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Understanding the Cathode‐Electrolyte Interfacial Chemistry in Rechargeable Magnesium Batteries

Shi,

Wang,

Wang

et al. 2024

Advanced Science

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Rechargeable magnesium batteries (RMBs) have garnered significant attention due to their potential to provide high energy density, utilize earth‐abundant raw materials, and employ metal anode safely. Currently, the lack of applicable cathode materials has become one of the bottleneck issues for fully exploiting the technological advantages of RMBs. Recent studies on Mg cathodes reveal divergent storage performance depending on the electrolyte formulation, posing interfacial issues as a previously overlooked challenge. This minireview begins with an introduction of representative cathode‐electrolyte interfacial phenomena in RMBs, elaborating on the unique solvation behavior of Mg2+, which lays the foundation for interfacial chemistries. It is followed by presenting recently developed strategies targeting the promotion of Mg2+ desolvation in the electrolyte and alternative cointercalation approaches to circumvent the desolvation step. In addition, efforts to enhance the cathode‐electrolyte compatibility via electrolyte development and interfacial engineering are highlighted. Based on the abovementioned discussions, this minireview finally puts forward perspectives and challenges on the establishment of a stable interface and fast interfacial chemistry for RMBs.

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Challenges and Progress in Anode‐Electrolyte Interfaces for Rechargeable Divalent Metal Batteries

Wang,

Riedel,

Zhao‐Karger

2024

Advanced Energy Materials

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Divalent metal batteries have attracted considerable attention in scientific exploration for sustainable energy storage solutions owing to the abundant reserves of magnesium (Mg) and calcium (Ca), the competitive low redox potentials of the Mg/Mg2+ (–2.37 V vs SHE) and Ca/Ca2+ (–2.87 V vs SHE) couples, as well as the high theoretical capacities of both metal anodes. However, the development of these batteries faces fundamental challenges stemming from the limited cycling stability and efficiency of Mg/Ca metal anodes. These issues primarily originate from the sluggish electrochemical redox kinetics of the divalent metals, particularly at the anode‐electrolyte interfaces. This comprehensive review provides an up‐to‐date overview of advancements in the field of the anode‐electrolyte interface for divalent metal batteries, covering aspects ranging from its formation, morphology, and composition to their influence on the reversible electrochemical deposition of divalent metals. Recent approaches aimed at enhancing the performance of metallic Mg and Ca anodes across various electrolytes are summarized and discussed, with the goal of providing insights for the development of new strategies in future research.

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A weakly ion pairing electrolyte designed for high voltage magnesium batteries

Abstract: We report a solvent-designed Mg(TFSI)2 electrolyte, which facilitates ion pair dissociation, nanoscale Mg nucleation/growth, and dendrite-free Mg plating/stripping at 2 mA h cm−2, enabling full cell operation up to 3.5 V at a 2C rate for 400 cycles.

Cited by 12 publications

References 52 publications

Asymmetric SO₃CF₃⁻‐Grafted Boron‐Center Anion Enables Boron‐Containing Interphase for High‐Performance Rechargeable Mg Batteries

Asymmetric SO₃CF₃⁻‐Grafted Boron‐Center Anion Enables Boron‐Containing Interphase for High‐Performance Rechargeable Mg Batteries

Understanding the Cathode‐Electrolyte Interfacial Chemistry in Rechargeable Magnesium Batteries

Challenges and Progress in Anode‐Electrolyte Interfaces for Rechargeable Divalent Metal Batteries

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A weakly ion pairing electrolyte designed for high voltage magnesium batteries

Abstract: We report a solvent-designed Mg(TFSI)2 electrolyte, which facilitates ion pair dissociation, nanoscale Mg nucleation/growth, and dendrite-free Mg plating/stripping at 2 mA h cm−2, enabling full cell operation up to 3.5 V at a 2C rate for 400 cycles.

Cited by 12 publications

References 52 publications

Asymmetric SO3CF3−‐Grafted Boron‐Center Anion Enables Boron‐Containing Interphase for High‐Performance Rechargeable Mg Batteries

Asymmetric SO3CF3−‐Grafted Boron‐Center Anion Enables Boron‐Containing Interphase for High‐Performance Rechargeable Mg Batteries

Understanding the Cathode‐Electrolyte Interfacial Chemistry in Rechargeable Magnesium Batteries

Challenges and Progress in Anode‐Electrolyte Interfaces for Rechargeable Divalent Metal Batteries

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Asymmetric SO₃CF₃⁻‐Grafted Boron‐Center Anion Enables Boron‐Containing Interphase for High‐Performance Rechargeable Mg Batteries

Asymmetric SO₃CF₃⁻‐Grafted Boron‐Center Anion Enables Boron‐Containing Interphase for High‐Performance Rechargeable Mg Batteries