High power rechargeable magnesium/iodine battery chemistry

Tian, Huajun; Gao, Tao; Li, Yong; Wang, Xiwen; Luo, Chao; Fan, Xiulin; Yang, Chengliang; Suo, Liumin; Ma, Zhaohui; Han, Wei‐Qiang; Wang, Chunsheng

doi:10.1038/ncomms14083

Cited by 283 publications

(218 citation statements)

References 35 publications

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“…[22,23] These species are not likely to form a thick surface layer covering the Mg electrode, because the high resolution Mg 2p spectrum shows a Mg 0 peak ( Mg anodes in the same electrolyte. These XPS results imply that a dense insoluble surface layer containing MgI 2 is formed on the Mg electrode in electrolytes with iodine concentrations >5 × 10 −3 m. Since MgI 2 has a high ionic conductivity but low electronic conductivity, [17,28] this surface layer is highly likely to behave as a SEI. [27] Thin though it is, the presence of such a surface layer possess larger barriers for Mg deposition/ stripping.…”

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confidence: 95%

“…Most work has focused on complex electrolytes that allow fast and reversible Mg deposition/stripping. [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.). [9] Later, a non-nucleophilic electrolyte, Mg-HMDS, was developed by Muldoon and co-workers, and Fichtner and co-workers for Mg/S batteries.…”

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confidence: 99%

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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

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125

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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

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125

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“…Magnesiumion batteries (MIBs) offer many distinct advantages over their LIB and sodiumion battery (SIB) counterparts, including the earth-abundance of magnesium (Mg), the reversible dendrite-free deposition of Mg, [2,[6][7][8][9][10][11] the divalent nature of Mg ion and its smaller ionic radius compared to lithium (Li) and sodium (Na) ions, [12][13][14] and finally the fact that metallic Mg is less reactive and therefore safer than Li and Na metals. Magnesiumion batteries (MIBs) offer many distinct advantages over their LIB and sodiumion battery (SIB) counterparts, including the earth-abundance of magnesium (Mg), the reversible dendrite-free deposition of Mg, [2,[6][7][8][9][10][11] the divalent nature of Mg ion and its smaller ionic radius compared to lithium (Li) and sodium (Na) ions, [12][13][14] and finally the fact that metallic Mg is less reactive and therefore safer than Li and Na metals.…”

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High‐Rate and Long Cycle‐Life Alloy‐Type Magnesium‐Ion Battery Anode Enabled Through (De)magnesiation‐Induced Near‐Room‐Temperature Solid–Liquid Phase Transformation

Wang

Welborn

Kumar

et al. 2019

Advanced Energy Materials

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alternative electrochemical energy storage systems are desirable to satisfy our growing demand for energy. Magnesiumion batteries (MIBs) offer many distinct advantages over their LIB and sodiumion battery (SIB) counterparts, including the earth-abundance of magnesium (Mg), the reversible dendrite-free deposition of Mg, [2,[6][7][8][9][10][11] the divalent nature of Mg ion and its smaller ionic radius compared to lithium (Li) and sodium (Na) ions, [12][13][14] and finally the fact that metallic Mg is less reactive and therefore safer than Li and Na metals. [8,[15][16][17][18][19] Despite these remarkable features, progress toward the development of practical MIBs has been impeded partly by the absence of suitable electrolytes that are compatible with Mg metal as the anode. [7,15,[20][21][22] Typically, common salts and organic solvent combinations like those used in LIBs and SIBs yield a Mg-ion-blocking film on the Mg metal anode. [7,[20][21][22][23][24] A promising way to circumvent this electrolyte issue involves the use of Mg alloy as the anode instead of pure Mg metal. Bismuth (Bi) and tin (Sn) are two promising candidate materials used as alloy-type MIB anodes, in which Mg is reversibly stored to make Mg 3 Bi 2 and Mg 2 Sn alloys, respectively. [1,[25][26][27] Unfortunately, state-of-the-art alloy-type MIB anodes can only be reversibly (dis)charged up to 200 cycles with acceptable capacity retention, [28] which is far below the 1000 cycles or more required for practical battery applications. In general, the capacity of MIB electrodes decays rapidly during cycling due to gradual material failure caused by massive volume expansions (up to 300%), and significant mechanical stresses, [27][28][29][30] which arise during solid-solid phase transformations. This occurs when a solid host MIB anode material (e.g., Bi, rhombohedral crystal structure) stores Mg to form a new solid phase material with a completely different crystal structure (e.g., β-Mg 3 Bi 2 , cubic crystal structure). [16,25] During the reverse process, Mg is removed from this new phase and transforms back to the initial host material. In doing so, the materials cracks and pulverizes into fragments, failing to restore its original shape and causing the battery to die within a few cycles. This issue represents a fundamental challenge in alloytype anodes. [31] In this work, we propose to overcome this challenge by taking advantage of the self-healing property of some Resources used in lithium-ion batteries are becoming more expensive due to their high demand, and the global cobalt market heavily depends on supplies from countries with high geopolitical risks. Alternative battery technologies including magnesium-ion batteries are therefore desirable. Progress toward practical magnesium-ion batteries are impeded by an absence of suitable anodes that can operate with conventional electrolyte solvents. Although alloy-type magnesium-ion battery anodes are compatible with common electrolyte solvents, they suffer from severe failure associated with huge volume ...

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“…Die Partikelgrçße hatte wesentlichen Einfluss auf die elektrochemische Leistung, wobei die Kapazitätsretention der Nanopartikel besser war als jene der Mikropartikel. NuLi et al [120] [123] Die Entwicklung von Kathodenmaterialien fürw iederaufladbare Mg-Batterien mit hoher Kapazität, Spannung und Lebensdauer bleibt eine schwierige Aufgabe. Das Material lieferte den grçßten Anteil seiner Kapazitätb ei etwa 1.4-1.6 V gegen Mg/Mg 2+ ,w as darauf hindeutet, dass sich die elektrochemisch aktiven Mg +2 -Ionen hauptsächlich auf spezifischen Plätzen im Kathodenmaterial befinden.…”

Section: üBergangsmetallsulfideunclassified

Magnesiumbatterien – ein Aufruf an Synthesechemiker: Elektrolyte und Kathoden dringend gesucht

Muldoon¹,

Bucur²,

Gregory³

2017

Angewandte Chemie

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Magnesiummetall ist ein hervorragendes Anodenmaterial mit einem negativen Reduktionspotential von −2.37 V gegen die Standardwasserstoffelektrode, dessen volumenspezifische Kapazität doppelt so hoch ist wie die von Lithiummetall. Ein Hauptvorteil gegenüber Lithiummetall ist, dass während des Aufladens kein Dendritenwachstum stattfindet. Dieser Aufsatz befasst sich mit aktuellen Entwicklungen bei Elektrolyten und Kathoden, und es werden wesentliche Herausforderungen auf dem Weg zu einer praktikablen Magnesiumbatterie diskutiert.

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High power rechargeable magnesium/iodine battery chemistry

Cited by 283 publications

References 35 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

High‐Rate and Long Cycle‐Life Alloy‐Type Magnesium‐Ion Battery Anode Enabled Through (De)magnesiation‐Induced Near‐Room‐Temperature Solid–Liquid Phase Transformation

Magnesiumbatterien – ein Aufruf an Synthesechemiker: Elektrolyte und Kathoden dringend gesucht

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