Plating and Stripping of Calcium in an Alkyl Carbonate Electrolyte at Room Temperature

Biria, Saeid; Pathreeker, Shreyas; Li, Hansheng; Hosein, Ian D.

doi:10.1021/acsaem.9b01670

Cited by 39 publications

(58 citation statements)

References 25 publications

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“…3c). [54] The Coulombic efficiencies were high (>95%). However, the reported cathodic current densities were <0.4 mA/cm 2 , approximately two orders of magnitude lower than those attainable upon Li plating in comparable carbonate electrolyte (~tens of mA/cm 2 ).…”

Section: Successful Ca Plating and Stripping In Carbonate Electrolytesmentioning

confidence: 99%

“…increase current density and Coulombic efficiency), [16,31,32,55] though it is clear that some ion pairing does not disqualify an electrolyte system from successful Ca 2+ deposition, as with Ca(BF4)2/EC:PC. [16,54] It will be important to critically examine, first, whether this trend is categorically true through sustained exploration of additional electrolyte formulations and rigorous spectroscopy/computational efforts; and second, whether a causal effect can be established. In addition, the 'successful' systems reported so far should be tested on a range of electrode substrates, including C, stainless steel, etc., to screen for practical viability.…”

Section: Summary and Future Considerationsmentioning

confidence: 99%

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Current Understanding of Nonaqueous Electrolytes for Calcium‐Based Batteries

Melemed

Khurram

Gallant

2020

Batteries & Supercaps

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Calcium metal batteries are receiving growing research attention due to significant breakthroughs in recent years that have indicated reversible Ca plating/stripping with attractive Coulombic efficiencies (90-95%), once thought to be out of reach. While the Ca anode is often described as being surface filmcontrolled, the ability to access reversible Ca electrochemistry is highly electrolyte-dependent in general, which affects both interfacial chemistry on plated Ca along with more fundamental Ca 2+ /Ca redox properties. This mini-review describes recent progress towards a reversible Ca anode from the point of view of the most successful electrolyte chemistries identified to date. This includes, centrally, what is currently known about the Ca 2+ solvation environment in these systems. Experimental (physico-chemical and spectroscopy) and computational results are summarized for the two major solvent classescarbonates and ethers-that have yielded promising results so far. Current knowledge gaps and opportunities to improve fundamental understanding of Ca 2+ /Ca redox are also identified.

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Section: Successful Ca Plating and Stripping In Carbonate Electrolytesmentioning

confidence: 99%

Section: Summary and Future Considerationsmentioning

confidence: 99%

Current Understanding of Nonaqueous Electrolytes for Calcium‐Based Batteries

Melemed

Khurram

Gallant

2020

Batteries & Supercaps

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“…Since the publication of Ponrouch et al, there have been numerous reports of viable Ca-ion electrolytes, ranging from organic solvents [10][11][12][13][14] to ionic liquids [15,16] and polymers [17]. With several examples of successful Ca-ion cathodes [18][19][20][21], a cyclable Ca-ion rocking chair battery is within reach; in fact, there are already some functional examples of such a setup [14,22].…”

Section: Introductionmentioning

confidence: 99%

“…In choosing our electrolyte composition, we focus on polar aprotic solvents because they have a sufficient electrochemical window, minimize solution viscosity, and provide a dielectric constant high enough to dissolve many salts [7]. In addition to meeting these criteria, our first solvent, ethylene carbonate (EC), was chosen for its popularity in computational and experimental CIB research [7,11,25,29]. Despite a narrower electrochemical window, we choose tetrahydrofuran (THF) for our second solvent.…”

Section: Introductionmentioning

confidence: 99%

A Computational Comparison of Ether and Ester Electrolyte Stability on a Ca Metal Anode

Liepinya

Smeu

2021

Energy Mater Adv

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Ca-ion batteries (CIBs) have the potential to provide inexpensive energy storage, but their realization is impeded by the lack of suitable electrolytes. Motivated by recent experimental progress, we perform ab initio molecular dynamics simulations to investigate early decomposition reactions at the anode-electrolyte interface. By examining different combinations of solvent—tetrahydrofuran (THF) or ethylene carbonate (EC)—and salt—Ca(BH4)2, Ca(BF4)2, Ca(BCl4)2, and Ca(ClO4)2—we identify a variety of behavioral trends between electrolyte solutions. Next, we perform a separate trajectory with pure THF and gradually increased negative charge; despite an addition of -32e, no THF decomposition is detected. Charge analysis reveals that in a reductive environment, THF distributes excess charge evenly across its hydrocarbon backbone, while EC concentrates charge on its ester oxygens and carbonyl carbon, resulting in decomposition. Graphs of charge vs. time for both solvents reveal that EC decomposition products can be reduced by up to five electrons, while those of THF are limited to a single electron. Ultimately, we find Ca(BH4)2 and THF to be the most stable solution investigated herein, corroborating experimental evidence of its suitability as a CIB electrolyte.

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“…However, the most challenging aspects in calcium batteries are the passivation of calcium anode [ 46 ] and the lack of reliable electrolytes. [ 47 ]…”

Section: Nonaqueous Anode Chemistries Of LI Na Mg Al K and Camentioning

confidence: 99%

A Progress Report on Metal–Sulfur Batteries

Manthiram

2020

Adv Funct Materials

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Nonaqueous conversion-reaction sulfur chemistry has been attracting increasing attention over the past decade for the development of nextgeneration lithium-based batteries. Li-S batteries are currently approaching a nexus stage from lab-scale experiments to possible pragmatic applications. Inspired by the success of Li-S chemistry, other metal-sulfur batteries with a variety of metallic anodes, such as sodium, potassium, magnesium, calcium, and aluminum, have also started to attract attention. In comparison to lithium, Na, Mg, Al, K, and Ca are naturally more abundant and affordable.

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Plating and Stripping of Calcium in an Alkyl Carbonate Electrolyte at Room Temperature

Cited by 39 publications

References 25 publications

Current Understanding of Nonaqueous Electrolytes for Calcium‐Based Batteries

Current Understanding of Nonaqueous Electrolytes for Calcium‐Based Batteries

A Computational Comparison of Ether and Ester Electrolyte Stability on a Ca Metal Anode

A Progress Report on Metal–Sulfur Batteries

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