Understanding and Overcoming the Challenges Posed by Electrode/Electrolyte Interfaces in Rechargeable Magnesium Batteries

Mizuno, Fuminori; Singh, Nikhilendra; Arthur, Timothy S.; Fanson, Paul T.; Ramanathan, Mayandi; Benmayza, Aadil; Prakash, Jai; Liu, Yi‐Sheng; Glans, Per‐Anders; Guo, Jinghua

doi:10.3389/fenrg.2014.00046

Cited by 31 publications

(48 citation statements)

References 33 publications

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“…Capacity fading still remains a problem, however, as in each case the capacity fell below 50 mA h g −1 within ten cycles. Although EIS results show the amorphous layer causes an increase in charge transfer resistance with cycling [228], this layer is apparently thin enough (on the order of 1 nm [227]) that its contribution is negligible compared to the well-known issue of Mn dissolution and electrolyte decomposition catalyzed by the active material.…”

Section: Reviewmentioning

confidence: 94%

Beyond Li-ion: electrode materials for sodium- and magnesium-ion batteries

2015

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to develop and install renewable energy harvesting technologies [3]. However, their successful implementation will be dependent on reliable and robust storage devices since harvesting solar and wind energy is inherently intermittent and the majority of consumption targets cannot be readily tethered to the grid.As energy storage devices, batteries possess high portability, high energy density, high Coulombic efficiency, and long cycle life. They are ideal power sources for portable devices, automobiles, and backup power supplies; accordingly, batteries power nearly all of our mobile electronics and are used to improve the efficiency of hybrid electric vehicles [4,5]. Unfortunately, considerable improvements in performance are still required in order to meet the demands of advanced portable devices and achieve energy sustainability (e.g., through smart grid and electric vehicle technologies) [6]. These enduring needs have driven intensive research investments. While efforts have been successful, there is still significant room for improvement regarding the development and understanding of electrode materials [7]. The overall capacity and potential cycling window of many electrode materials are limited to prevent degradation over long term cycling. In addition to exploring new electrode materials, there have been strong efforts to improve those that are already utilized. Expense reduction is a priority as approximately 23% and 8% of the overall battery pack costs stem from the respective cathode and anode active materials alone [8].An alkali-ion battery consists of several electrochemical cells connected in parallel and/or in series to provide a designated current or voltage. Each electrochemical cell has two electrodes separated by an electrolyte that is electrically insulating but ionically conductive. During discharge, when the alkali-ion battery operates as a galvanic cell, alkali ions exit the negative electrode (typically carbon) and insert themselves into the positive electrode while electronsThe need for economical and sustainable energy storage drives battery research today. While Li-ion batteries are the most mature technology, scalable electrochemical energy storage applications benefit from reductions in cost and improved safety. Sodium-and magnesium-ion batteries are two technologies that may prove to be viable alternatives. Both metals are cheaper and more abundant than Li, and have better safety characteristics, while divalent magnesium has the added bonus of passing twice as much charge per atom. On the other hand, both are still emerging fields of research with challenges to overcome. For example, electrodes incorporating Na + are often pulverized under the repeated strain of shuttling the relatively large ion, while insertion and transport of Mg 2+ is often kinetically slow, which stems from larger electrostatic forces. This review provides an overview of cathode and anode materials for sodium-ion batteries, and a comprehensive summary of research on cathodes for magnesium-ion batteries. In additi...

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Section: Reviewmentioning

confidence: 94%

Beyond Li-ion: electrode materials for sodium- and magnesium-ion batteries

2015

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“…4 Understanding the evolution of this Mg film during cycling is a critical factor in the development of high-performance magnesium batteries. 7 Although the development of electrolytes for the efficient and reversible deposition and dissolution of Mg has been pursued extensively (see Refs. 1 and 2 for comprehensive reviews on this topic), much less attention has been given to the morphological evolution of the Mg deposits during cycling.…”

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confidence: 99%

Computational Examination of Orientation-Dependent Morphological Evolution during the Electrodeposition and Electrodissolution of Magnesium

DeWitt

Hahn

Zavadil

et al. 2015

J. Electrochem. Soc.

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A new model of electrodeposition and electrodissolution is developed and applied to the evolution of Mg deposits during anode cycling. The model captures Butler-Volmer kinetics, facet evolution, the spatially varying potential in the electrolyte, and the time-dependent electrolyte concentration. The model utilizes a diffuse interface approach, employing the phase field and smoothed boundary methods. Scanning electron microscope (SEM) images of magnesium deposited on a gold substrate show the formation of faceted deposits, often in the form of hexagonal prisms. Orientation-dependent reaction rate coefficients were parameterized using the experimental SEM images. Three-dimensional simulations of the growth of magnesium deposits yield deposit morphologies consistent with the experimental results. The simulations predict that the deposits become narrower and taller as the current density increases due to the depletion of the electrolyte concentration near the sides of the deposits. Increasing the distance between the deposits leads to increased depletion of the electrolyte surrounding the deposit. Two models relating the orientation-dependence of the deposition and dissolution reactions are presented. The morphology of the Mg deposit after one deposition-dissolution cycle is significantly different between the two orientation-dependence models, providing testable predictions that suggest the underlying physical mechanisms governing morphology evolution during deposition and dissolution. Magnesium batteries have garnered substantial attention as a successor to Li-ion batteries due to their potential for high energy density and safe operation.1-3 Metallic Mg anodes provide a substantially higher specific volumetric capacity (3833 mA h/cm 3 ) than either Ligraphite anodes (760 mA h/cm 3 ) or metallic Li anodes (2046 mA h/cm 3 ). 2 Furthermore, unlike metallic Li anodes, 5 metallic Mg anodes can be cycled without the formation of dendrites. 4 Dendrite growth poses a hazard because dendrites can grow across the separator to the cathode and short the battery, leading to thermal runaway. 5,6 Instead of forming dendrites, metallic Mg anodes form compact, faceted films, practically eliminating this risk. 4 Understanding the evolution of this Mg film during cycling is a critical factor in the development of high-performance magnesium batteries. 7Although the development of electrolytes for the efficient and reversible deposition and dissolution of Mg has been pursued extensively (see Refs. 1 and 2 for comprehensive reviews on this topic), much less attention has been given to the morphological evolution of the Mg deposits during cycling. SEM and AFM images of the Mg film typically show a highly faceted film with grains on the order of 1 μm in width. [8][9][10][11] However, other morphologies with either larger 10 or smaller 12,13 features have also been observed. The most comprehensive examination of the morphology of electrodeposited Mg was conducted by Matsui, 4 who examined the morphology of 1 C/cm 2 of Mg deposited at 0.5...

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“…The electroactive species in halide-based electrolytes is MgCl + or Mg 2 Cl 3 + [241][242][243][244][245][246][247][248]. The organohalo-aluminate electrolytes obtained by reaction between a Grignard reagent and AlCl 3 [241], was a subject of a review publication [249].…”

Section: Electroactive Cations 24mentioning

confidence: 99%

A comprehensive review of lithium salts and beyond for rechargeable batteries: Progress and perspectives

Mauger¹,

Julien²,

Paolella³

et al. 2018

Materials Science and Engineering: R: Reports

155

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The increasing need for energy storage has been the motivation for intensive research in batteries with different chemistries in the recent past. Among the elements of the batteries, the salts and their solvent play an important role. In particular, the cathodic stability at low potential depends importantly on the choice of the cation, while the stability at high potentials is mainly due to oxidation of anions and the ion mobility and dissociation depend primarily on the delocalization of the anion, so that many attempts are made to find the optimum choice of both the cations and anions of the salts, and their solvents. Although lithium-based batteries are almost exclusively used today, efforts are currently made to explore batteries based on sodium, aluminum, magnesium, calcium, potassium. The purpose of the present work is to review the salts and solvents that have been proposed in these different batteries and discuss their properties and their ability to be used in the near future and in the next generation of batteries.

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Understanding and Overcoming the Challenges Posed by Electrode/Electrolyte Interfaces in Rechargeable Magnesium Batteries

Cited by 31 publications

References 33 publications

Beyond Li-ion: electrode materials for sodium- and magnesium-ion batteries

Beyond Li-ion: electrode materials for sodium- and magnesium-ion batteries

Computational Examination of Orientation-Dependent Morphological Evolution during the Electrodeposition and Electrodissolution of Magnesium

A comprehensive review of lithium salts and beyond for rechargeable batteries: Progress and perspectives

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