Electrodeposition of Al from a 1-butylpyrrolidine-AlCl3 ionic liquid

Pulletikurthi, Giridhar; Bödecker, Björn; Borodin, Andriy; Weidenfeller, B.; Endres, Frank

doi:10.1016/j.pnsc.2015.11.003

Cited by 48 publications

(31 citation statements)

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“…Electrodeposition is a viable alternative [12,13] due to the possibility to operate at moderate temperature (<100°C) and atmospheric pressure, thus allowing to coat a broader spectrum of substrates.…”

Section: Regarding the Deposition Section (Second Half Of Page 13): Tmentioning

confidence: 99%

Aluminium electrodeposition from a novel hydrophobic ionic liquid tetramethyl guanidinium-perfluoro-3-oxa-4,5 dichloro-pentan-sulphonate

Oriani

Cojocaru

Monzani

et al. 2017

Journal of Electroanalytical Chemistry

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Manuscript Region of Origin: SPAIN Reviewers' comments:Reviewer #1: This manuscript reports interesting results about the electrodeposition of aluminium using tetramethyl guanidium -perfluoro -3 -oxa-4,5 dichloro-pentansulphonate, a novel hydrophobic ionic liquid, which is synthesized and supplied by Solvay Specialty Polymers. The effect of temperature, aluminium and bistrifluoromethanesulfonimide lithium salt concentration, in the conductivity and electrochemical behavior of the electrolyte is evaluated and clearly discussed. However, the manuscript needs some improvements before acceptance for publication. My detailed comments are as follows:At first the authors want to acknowledge the reviewer for the fruitful comment and then we tried to answer the questions The objective of this paragraph was encourage the use of the electrodeposition for the preparation of deposits. At no time it was intended to give the impression that aluminum electrodeposition from IL was used for the first time. The paragraph has been rewritten and the suggested references included and consequently reordered. 2.Introduction section (Page 3), the phrase "Aluminium has a low reduction potential", is contrary to that reported in literature. In fact, because of the rather negative standard potential of Al, electrodeposition of Al from aqueous solutions is not possible due to hydrogen evolution at the cathode (Ref. 12 in the manuscript).The words "low reduction" was used as synonym of "very negative" potential. In the new version in order to avoid misunderstandings between potential and overpotential, the phase contains "very negative standard potential". 3.Page 10, just before the last paragraph, the authors comment that the voltammograms of Fig. 4B show the onset of reduction current at higher potentials if the aluminium content is increased. I suggest changing "higher potentials" for "more positive potentials" to avoid confusions.According to the suggestion and in order to clarify the text, in this paragraph and others the "higher/lower" comparative were substituted by "more positive/more negative" in order to avoid confusions. 4.Page 11, in the discussion of the voltammetric curves obtained in the absence and presence of LiTFSI (Fig. 7), the authors comment that LiTFSI favours the aluminium deposition process, only based in the appearance of the reduction onset at Response to Reviews Aluminium electrodeposition from a novel hydrophobic ionic liquid tetramethyl guanidium -perfluoro-3-oxa-4,5 dichloro-pentan-sulphonate

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Section: Regarding the Deposition Section (Second Half Of Page 13): Tmentioning

confidence: 99%

Aluminium electrodeposition from a novel hydrophobic ionic liquid tetramethyl guanidinium-perfluoro-3-oxa-4,5 dichloro-pentan-sulphonate

Oriani

Cojocaru

Monzani

et al. 2017

Journal of Electroanalytical Chemistry

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“…4-Pr-Py [g] 0.5750 ++ [AlCl 2 (L) n ] + (n = 1, 2) 3, 4cationic [32] 1-Bu-Pyrr [h] 0.5525 ++ [AlCl 3Àn (L) x ] + 1, 2cationic [40] G2 [i] 0.1725 ++ [AlCl 2 (L) 2 ] + 6cationic [37,38] G3 [j] 0.1725 --[ AlCl 2 (L) n ] + 6 [37,38] [a] N,N-Dimethylacetamide. compensated by the higherd ensities of the bromoaluminate systems.…”

Section: Introductionmentioning

confidence: 99%

An Investigation of the Symmetric and Asymmetric Cleavage Products in the System Aluminum Trihalide/1‐Butylimidazole

Hog

Schneider

Studer

et al. 2017

Chemistry A European J

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Mixtures of AlX (X=Cl, Br) with 1-butylimidazole (BuIm) in various ratios were investigated. The mixtures were characterized by multinuclear ( H, Al, C, and N) NMR, IR, and Raman spectroscopy and in part by single-crystal X-ray diffraction. Depending on the molar fraction x(AlBr ) of the AlBr -based mixtures, the cationic aluminum complexes [Al(BuIm) ] and [AlBr (BuIm) ] , the neutral adduct [AlBr (BuIm)], as well as the anions Br , [AlBr ] , and [Al Br ] could be identified as the products of the symmetric and asymmetric cleavage of dimeric Al Br . Furthermore, there are hints at the formation of [AlBr (BuIm) ] or related cations. Comparison of the AlBr /BuIm system with AlCl -based mixtures revealed the influence of the halide: In contrast to AlBr , the trication [Al(BuIm) ] could not be detected as main product in a 1:6 mixture of AlCl and BuIm. Additionally, [AlCl (BuIm)] crystallizes from a mixture with x(AlCl )=0.60 at room temperature, whereas the corresponding AlBr -based mixture remains liquid even at +6 °C. Three AlBr -based mixtures are liquid at room temperature, whereas all other mixtures are solids with melting points between 46 and 184 °C. The three liquid mixtures exhibit medium to high viscosities (117 to >1440 mPa s), low conductivities (0.03-0.20 mS cm ), but high densities (1.80-2.21 g cm ). Aluminum could be successfully deposited from one of the neat Lewis acidic mixtures of the AlBr -based system.

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“…For this reason, ionic liquids (ILs) have been investigated for energy storage due to their low vapor pressure and wide electrochemical windows, unfortunately with the caveat of high cost in most cases. A new class of ionic liquids, referred to as ionic liquid analogs (ILAs) or so-called deep eutectic solvents, generally formed through a mixture of a strongly Lewis acidic metal halide and Lewis basic ligand, have gained significant attention due to their comparable electrochemical and physical properties with reduced cost and minimal environmental footprint (2 (4)(5)(6).…”

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confidence: 99%

High Coulombic efficiency aluminum-ion battery using an AlCl ₃ -urea ionic liquid analog electrolyte

Angell

Pan

Rong

et al. 2017

Proc. Natl. Acad. Sci. U.S.A.

344

285

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In recent years, impressive advances in harvesting renewable energy have led to a pressing demand for the complimentary energy storage technology. Here, a high Coulombic efficiency (∼99.7%) Al battery is developed using earth-abundant aluminum as the anode, graphite as the cathode, and a cheap ionic liquid analog electrolyte made from a mixture of AlCl 3 and urea in a 1.3:1 molar ratio. The battery displays discharge voltage plateaus around 1.9 and 1.5 V (average discharge = 1.73 V) and yielded a specific cathode capacity of ∼73 mAh g −1 at a current density of 100 mA g −1 (∼1.4 C). High Coulombic efficiency over a range of charge-discharge rates and stability over ∼150-200 cycles was easily demonstrated. In situ Raman spectroscopy clearly showed chloroaluminate anion intercalation/deintercalation of graphite (positive electrode) during charge-discharge and suggested the formation of a stage 2 graphite intercalation compound when fully charged. + cations. This battery is a promising prospect for a future high-performance, low-cost energy storage device.aluminum-ion battery | urea electrolyte | ionicity | ionic liquid | energy storage C heap, high-rate (fast charge/discharge) rechargeable batteries with long cycle lives are urgently needed for grid-scale storage of renewable energy, as it is becoming increasingly important to replace fossil fuels (1). Lithium-ion batteries (LIBs) are expensive and have limited cycle life, which makes them nonideal for grid-scale energy storage. Furthermore, high-rate capability is necessary for use in the grid, under which conditions LIBs become increasingly unsafe due to the flammability of the electrolytes used. Batteries based on aluminum offer a viable alternative due to aluminum's three-electron redox properties (offers potential for high-capacity batteries), stability in the metallic state, and very high natural abundance. Furthermore, the development of these batteries based on nonflammable electrolytes of low toxicity is critical for minimizing safety hazard and environmental impact. Recently, our group developed a secondary Al battery system based on the reversible deposition/stripping of aluminum at the Al negative electrode and reversible intercalation/deintercalation of chloroaluminate anions at the graphite positive electrode in a nonflammable 1-ethyl-3-methylimidazolium chloroaluminate (EMIC-AlCl 3 ) IL electrolyte (7,8). A ratio of AlCl 3 /EMIC = 1.3 by mole was used such that Al 2 Cl 7 − was present in the (acidic) electrolyte to facilitate aluminum deposition (9). During charging, Al 2 Cl 7 − is reduced to deposit aluminum metal, and AlCl 4 − ions intercalate (to maintain neutrality) in graphite as carbon is oxidized. During discharge, this battery exhibited a cathode specific capacity of ∼70 mAh g −1 with a Coulombic efficiency (CE) of 97-98%, and ultrahigh charge/discharge rate (up to 5,000 mA g −1 ) for over 7,000 cycles. However, room for improvement exists as the parameter space for the Al battery remains largely unexplored. The three-electron redox properti...

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Electrodeposition of Al from a 1-butylpyrrolidine-AlCl3 ionic liquid

Cited by 48 publications

References 50 publications

Aluminium electrodeposition from a novel hydrophobic ionic liquid tetramethyl guanidinium-perfluoro-3-oxa-4,5 dichloro-pentan-sulphonate

Aluminium electrodeposition from a novel hydrophobic ionic liquid tetramethyl guanidinium-perfluoro-3-oxa-4,5 dichloro-pentan-sulphonate

An Investigation of the Symmetric and Asymmetric Cleavage Products in the System Aluminum Trihalide/1‐Butylimidazole

High Coulombic efficiency aluminum-ion battery using an AlCl ₃ -urea ionic liquid analog electrolyte

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Electrodeposition of Al from a 1-butylpyrrolidine-AlCl3 ionic liquid

Cited by 48 publications

References 50 publications

Aluminium electrodeposition from a novel hydrophobic ionic liquid tetramethyl guanidinium-perfluoro-3-oxa-4,5 dichloro-pentan-sulphonate

Aluminium electrodeposition from a novel hydrophobic ionic liquid tetramethyl guanidinium-perfluoro-3-oxa-4,5 dichloro-pentan-sulphonate

An Investigation of the Symmetric and Asymmetric Cleavage Products in the System Aluminum Trihalide/1‐Butylimidazole

High Coulombic efficiency aluminum-ion battery using an AlCl 3 -urea ionic liquid analog electrolyte

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High Coulombic efficiency aluminum-ion battery using an AlCl ₃ -urea ionic liquid analog electrolyte