Synthesis, Crystal Structure, and Electrochemical Properties of a Simple Magnesium Electrolyte for Magnesium/Sulfur Batteries

Li, Wanfei; Cheng, Shuang; Wang, Jian; Qiu, Yongcai; Zheng, Zhaohui; Lin, Hongzhen; Nanda, Sanjay; Ma, Qian; Xu, Yan; Ye, Fangmin; Liu, Meinan; Zhou, Lisha; Zhang, Yuegang

doi:10.1002/anie.201600256

Cited by 115 publications

(116 citation statements)

References 35 publications

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“…13 On the other hand, some efforts have also been made to address the dissolution of magnesium polysufide (MgS x , x ≥ 4) by using a sulfur-carbon composite 8,11,14 or fabricating new elemental selenium (Se) and selenium-sulfur solid solution (SeS 2 ) cathodes to physically restrain polysulfides, facilitate electron transport, and provide free-space to accommodate the volume change in S/polysulfides.…”

mentioning

confidence: 99%

Application of a Sulfur Cathode in Nucleophilic Electrolytes for Magnesium/Sulfur Batteries

Zeng

Wang

Yang

et al. 2017

J. Electrochem. Soc.

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We report the potential feasibility of a high-capacity and low-cost sulfur cathode that is compatible with nucleophilic electrolytes for Mg/S batteries. The electrochemical performance of sulfur in an easily prepared (PhMgCl) 2 -AlCl 3 /THF nucleophilic electrolyte depends on cathode current collectors. A sulfur cathode that uses Cu as a current collector, which is electrochemically stable in the range of operating voltage, exhibits an initial discharge capacity approximately corresponding to 659 mAh g −1 , and maintains a reversible capacity of 113 mAh g −1 after 20 cycles at a current density of 10 mA g −1 . It is different from the sulfur cathode with few capacities that uses stainless-steel as a current collector. Copper sulfides formed when sulfur is coated on a Cu current collector at 50 • C provide a strong chemical interaction between Cu and sulfur, which protects sulfur and increases its compatibility with the electrolyte. A metal-stabilized sulfur cathode provides an effective approach to improve the electrochemical performance of Mg/S batteries in nucleophilic electrolytes. There is a constant increase in the demand for low-cost, highenergy-density rechargeable batteries that utilize environmentally friendly elements for applications, such as market-competitive electric vehicles and large-scale power storage systems due to fossil energy shortage and environmental issues. Following the rapid development of electric vehicles with space available to mount battery packs, it is now necessary for batteries to possess good safety characteristics 1 and high volumetric energy density, which is more important than gravimetric energy density.2 Rechargeable magnesium batteries with magnesium as the anode may correspond to superior candidates compatible with post Li-ion batteries that contain a lithium metal anode, which provides a volumetric capacity (2062 mAh cm −3 ) exceeding that of a current graphite anode (777 mAh cm −3 ), 2 due to a relatively lower price ($2700 and $64800/ton for Mg and Li, respectively), 2,3 a higher theoretical volumetric capacity (3832 mAh cm −3 ), 2 and higher expected safety (the dendritic morphologies for magnesium deposits are lower than that for lithium). 4 Muldoon et al. first suggested an electrophilic sulfur cathode candidate with a high theoretical capacity (1671 mAh g −1 or 3459 mAh cm −3 ) corresponding to a conversion class as opposed to an insertion class. It is chemically incompatible with nucleophilic magnesium organohaloaluminate electrolytes and compatible with a non-nucleophilic electrolyte based on a recrystallized Mg complex [Mg 2 (μ-Cl) 3 (THF) 6 ][HMDSAlCl 3 ] formed from a reaction between hexamethyldisilazide magnesium chloride (HMDSMgCl) and AlCl 3 (3:1 molar ratio) in tetrahydrofuran (THF).2,4 The magnesium/sulfur (Mg/S) batteries yield a theoretical volumetric energy density exceeding 4000 Wh L −1 as compared to 2800 Wh L −1 for lithium/sulfur (Li/S) batteries.5 However, on cycling, Mg/S batteries also suffer from capacity fading, which results from low active...

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confidence: 99%

Application of a Sulfur Cathode in Nucleophilic Electrolytes for Magnesium/Sulfur Batteries

Zeng

Wang

Yang

et al. 2017

J. Electrochem. Soc.

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“…[48][49][50][51][52] − . [53] The oxidative stability of 2.5 V versus Mg on Pt electrode for this electrolyte is inferior to the reported MACC solution in a pure ethereal solvent and the ionic liquid possibly contributed to the high ionic conductivity of the electrolyte (8.5 mS/ cm). [53] More recently, Luo et al reported the beneficial effects of post-treatment with Mg powder on the electrochemical performance of MgCl 2 /AlCl 3 electrolytes in ethereal solvents.…”

Section: Combinations Of Magnesium Chloride With Aluminum-based Lewismentioning

confidence: 63%

“…10(a)]. Interestingly, the overcharging behavior is much less significant compared with the previous [29,32] 3.9 ∼2 ∼100 Yes 260@20/20 [32] 1000@71/30 [33] 236@20/50 [34] 800@167/20 [ [47,53] 3.1 [47] , 2.5 [53] 2 [47] , 8.5 [53] 99 Yes 70@17/20 [53] Mg(TFSI) 2 Prospective Article reports and an overpotential during charge and discharge was <0.4 V. The Mg-S cells were cycled for 30 times with capacity retention >86% [ Fig. 10(b)].…”

Section: Conductive Salt-based Electrolytesmentioning

confidence: 89%

“…It is fully inorganic, it was supposed to be chemically compatible with S and has recently been tested for Mg-S batteries. [53] With the nitrogen-doped graphene-sulfur (NG-S) cathode, the cell was cycled 20 times. However, the cells suffered from rapid capacity decline from 700 to 130 mAh/g in the first Prospective Article cycles, a low discharge potential (<1 V) and large overpotential (>1.5 V).…”

Section: Macc Electrolytesmentioning

confidence: 99%

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Magnesium-sulfur battery: its beginning and recent progress

Zhao‐Karger

Fichtner

2017

MRS Communications

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Rechargeable magnesium (Mg) battery has been considered as a promising candidate for future battery generations because of its potential high-energy density, its safety features and low cost. The challenges lying ahead for the realization of Mg battery in general are to develop proper electrolytes fulfilling a multitude of requirements and to discover cathode materials enabling high-energy Mg batteries. The combination of Mg anode with a sulfur cathode is one of the promising electrochemical couples due to its advantages of safety, low costs, and a high theoretical energy density of over 3200 Wh/L. However, the research on magnesium-sulfur (Mg-S) battery is just at its beginning and the development of suitable electrolytes has been the key challenge for further improvement, and, thus, in the focus of recent research. In this review, we highlight the recent progress achieved in Mg electrolytes and Mg-S batteries and discuss the major technical issues, which must be resolved for the improvement of Mg-S batteries.

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“…[2,5] The conversion-type sulfur (S) and selenium (Se) cathodes, with theoretical volumetric capacity of 3467 mAh cm −3 for S and 3268 mAh cm −3 for Se, fulfill the criteria of high energy density, high safety, materials sustainability, and cost-effective features. [6][7][8] Nevertheless, researches on rechargeable Mg/S and Mg/Se battery systems are still in the nascent stage. With regard to selenium cathodes, there are only two reports recording their Mg-ion storage performances.…”

mentioning

confidence: 99%

Self‐Established Rapid Magnesiation/De‐Magnesiation Pathways in Binary Selenium–Copper Mixtures with Significantly Enhanced Mg‐Ion Storage Reversibility

Zhang

Chen

et al. 2017

Adv Funct Materials

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Synthesis, Crystal Structure, and Electrochemical Properties of a Simple Magnesium Electrolyte for Magnesium/Sulfur Batteries

Cited by 115 publications

References 35 publications

Application of a Sulfur Cathode in Nucleophilic Electrolytes for Magnesium/Sulfur Batteries

Application of a Sulfur Cathode in Nucleophilic Electrolytes for Magnesium/Sulfur Batteries

Magnesium-sulfur battery: its beginning and recent progress

Self‐Established Rapid Magnesiation/De‐Magnesiation Pathways in Binary Selenium–Copper Mixtures with Significantly Enhanced Mg‐Ion Storage Reversibility

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