Rechargeable Mg–Li hybrid batteries: status and challenges

Cheng, Yingwen; Chang, Hee Jung; Dong, Hui; Choi, Daiwon; Sprenkle, Vincent; Li, Jun; Yao, Yan; Li, Guosheng

doi:10.1557/jmr.2016.331

Cited by 96 publications

(84 citation statements)

References 83 publications

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“…[12][13][14][15] These complex electrolytes have enabled the usage of Mg-cathode half-cells to evaluate various cathode materials due to their capability of facile Mg deposition/stripping; [8,10,[16][17][18] however, their complicated synthesis procedure, incompatibility with oxide cathodes, sensitivity to air and moisture, low ionic conductivity, and high cost have rendered them less attractive for practical applications than conventional organic electrolytes based on simple salts (salts containing anions of PF 6 − , BF 4 − , TFSI − , etc.). One challenge is the sluggish diffusion of the bivalent Mg ion in the cathode host structures, which generates large overpotentials for Mg intercalation [3][4][5] and greatly hinders the development of practical cathode materials for RMBs. In the electrolytes based on common aprotic organic solvents (such as AN, PC, etc.…”

mentioning

confidence: 99%

Reducing Mg Anode Overpotential via Ion Conductive Surface Layer Formation by Iodine Additive

Gao

Han

et al. 2017

Advanced Energy Materials

120

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Another challenge is the development of electrolytes that can effectively utilize an Mg metal anode. Extensive effort has been put in to develop electrolytes capable of reversibly depositing/stripping Mg. Most work has focused on complex electrolytes that allow fast and reversible Mg deposition/stripping. Such electrolytes were first proposed by Aurbach's group in 2000, [8] and subsequently they developed the all phenyl complex showing high anodic stability. [9] Later, a non-nucleophilic electrolyte, Mg-HMDS, was developed by Muldoon and co-workers, and Fichtner and co-workers for Mg/S batteries. [10,11] To eliminate the organic Grignard species in the electrolyte, an all inorganic electrolyte, magnesium aluminum chloride complex, was reported. [12][13][14][15] These complex electrolytes have enabled the usage of Mg-cathode half-cells to evaluate various cathode materials due to their capability of facile Mg deposition/stripping; [8,10,[16][17][18] however, their complicated synthesis procedure, incompatibility with oxide cathodes, sensitivity to air and moisture, low ionic conductivity, and high cost have rendered them less attractive for practical applications than conventional organic electrolytes based on simple salts (salts containing anions of PF 6 − , BF 4 − , TFSI − , etc.). Unfortunately, most of these simple salt electrolytes are not compatible with Mg metal because poorly or nonconductive surface layers are normally formed on the Mg surface. In the electrolytes based on common aprotic organic solvents (such as AN, PC, etc.), the surface film is dominated by the decomposition of solvent due to their weak reduction stability, and the formed layer can block the deposition/stripping of Mg. [19] Even for solvents that are stable with Mg metal (such as glyme), the decomposition of salts or the reaction of trace moisture with Mg can still form a surface film covering the Mg surface, leading to a large overpotential for Mg deposition/stripping. [20][21][22][23] Therefore, the formation of a poorly or even nonconductive surface layer on Mg metal in common simple salt organic electrolytes is inevitable due to Mg's strong reducing ability, which remains a challenge for the application of a Mg metal anode in these simple salt electrolytes. Herein, we propose for the first time a facile approach to solve this problem by tuning the composition of the surface layer and forming an Mg ion conductive layer. By adding a small concentration of iodine (<50 × 10 −3 m) into the electrolyte, an insoluble magnesium iodide layer is formed on the surface of the Mg metal, which acts as a solid electrolyte Electrolytes that are able to reversibly deposit/strip Mg are crucial for rechargeable Mg batteries. The most studied complex electrolytes based on Lewis acid-base chemistry are expensive, difficult to be synthesized, and show limited anodic stability. Conventional electrolytes using simple salts such as Mg(TFSI) 2 can be readily synthesized, but Mg deposition/stripping in these simple salt electrolytes is accompanied by a large...

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Reducing Mg Anode Overpotential via Ion Conductive Surface Layer Formation by Iodine Additive

Gao

Han

et al. 2017

Advanced Energy Materials

120

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“…For example, in the case of Mg, a metallic Mg anode is coupled with a Li‐ion insertion electrode and a dual Mg/Li Ion electrolyte. The system therefore benefits from the Mg anode as well as the rapid and reversible insertion of Li + into the cathode . This strategy could potentially also be applied to calcium, that is, dual‐ion systems could be developed with Ca anodes, Ca/Li dual‐ion electrolytes and Li‐insertion compounds as cathodes.…”

Section: Cathodes For Calcium‐ion Batteriesmentioning

confidence: 99%

Calcium‐Ion Batteries: Current State‐of‐the‐Art and Future Perspectives

et al. 2018

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Recent developments in rechargeable battery technology have seen a shift from the well-established Li-ion technology to new chemistries to achieve the high energy density required for extended range electric vehicles and other portable applications, as well as low-cost alternatives for stationary storage. These chemistries include Li-air, Li-S, and multivalent ion technologies including Mg , Zn , Ca , and Al . While Mg battery systems have been increasingly investigated in the last few years, Ca technology has only recently been recognized as a viable option. In this first comprehensive review of Ca ion technology, the use of Ca metal anodes, alternative alloy anodes, electrolytes suitable for this system, and cathode material development are discussed. The advantages and disadvantages of Ca ion batteries including prospective achievable energy density, cost reduction due to high natural abundance, low ion mobility, the effect of ion size, and the need for elevated temperature operation are reviewed. The use of density functional theory modeling to predict the properties of Ca-ion battery materials is discussed and the extent to which this approach is successful in directing research into areas of promise is evaluated. To conclude, a summary of recent achievements is presented and areas for future research efforts evaluated.

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“…Detailed discussion of Mg dual‐salt electrolytes containing Li salts can be found in a recent review . Some of the latest studies using different cathodes in Mg dual‐salt electrolytes are collated, along with their charge‐discharge performance, in Table .…”

Section: Rechargeable Mg Batteriesmentioning

confidence: 99%

“…Studies on transition-metal oxide cathodes with various Mg dual-salt electrolytes (containing both Mg and Li/Na salts) have thus been reported. [111,113,[118][119][120][121][122][123][124][125][126] Compared to Mg salts, the monovalent property of Li and Na salts means that they have weaker electrostatic interactions and lower co-ordination numbers, making them more soluble in the solvents. For instance, [119] LiNTf 2 showed a higher solubility in diglyme than that of Mg[NTf 2 ] 2 Highly reversible charge-discharge behaviour is observed in some of these Mg hybrid systems, with reasonable output voltage and energy capacity.…”

Section: Transition-metal Compoundsmentioning

confidence: 99%

Mg Cathode Materials and Electrolytes for Rechargeable Mg Batteries: A Review

MacFarlane

Kar

2019

Batteries & Supercaps

119

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The development of energy storage devices has been motivated by the growing availability of sustainable energy sources, as well as the wider application of portable devices and a variety of electric vehicles including bicycles, scooters, cars and buses. Concerns regarding the safety of lithium batteries in certain applications, and limited lithium and cobalt resources required for conventional cathode materials, have driven researchers to develop alternatives that are safer and cheaper, thereby using more abundant metals such as sodium, magnesium, aluminium, and calcium. Among them, rechargeable magnesium batteries have drawn special interest, since Mg does not plate in a dendritic form, which opens up the possibility of the safe use of a simple metal anode. In this review, we summarize typical Mg electrolyte systems that are compatible with reversible Mg deposition and stripping, focusing on the active Mg complexes. To fabricate a rechargeable device, an appropriate cathode is necessary, which must also be abundant and compatible with the electrolytes to suitable cathode materials are also briefly discussed.

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Rechargeable Mg–Li hybrid batteries: status and challenges

Abstract: Abstract

Cited by 96 publications

References 83 publications

Reducing Mg Anode Overpotential via Ion Conductive Surface Layer Formation by Iodine Additive

Reducing Mg Anode Overpotential via Ion Conductive Surface Layer Formation by Iodine Additive

Calcium‐Ion Batteries: Current State‐of‐the‐Art and Future Perspectives

Mg Cathode Materials and Electrolytes for Rechargeable Mg Batteries: A Review

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