Abstract
Electrodeposition of aluminum from ionic liquids has been considered a promising approach to low-temperature aluminum electrolysis. In this study, we first investigated the electrochemical stability of 1-ethyl-3-methylimidazolium chloride ([Emim][Al2Cl7]) electrolyte, which is a typically used electrolyte for aluminum electrodeposition. It was found that part of imidazole ions decomposed on the cathode during the electrolysis process, especially when the temperature was at or over 353 K. In order to enhance the stability of the electrolyte, we further studied the effects of lithium salt and lithium bis(oxalato)borate (LiBOB), on the electrochemical stability of the [Emim][Al2Cl7] ionic liquid system. It was found that the electrochemical window of the electrolyte was broadened from 2.59 to 2.74 V at 373 K by addition of 1 mol% LiBOB. With the existence of LiBOB, the reduction current density of Al2Cl7 - increased before −0.58 V and the electrodissolution of Al was more complete. The possible mechanism on the LiBOB increases the stability of the electrolyte systems also discussed based on our theoretical calculations.
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Zuca S, Galasiu I, Balu I (1984) On anode effect in aluminum electrolysis. Rev Roum Chim 29(4):309–314
Odegard R, Midtlyng SH (1991) Electrochemical and chemical-reactivity of carbon electrodeposited from cryolitic melts containing aluminum carbide. J Electrochem Soc 138(9):2612–2617
Capuano GA, Ducasse R, Davenport WG (1979) Electrodeposition of aluminium-copper alloys from alkyl benzene electrolytes. J Appl Electrochem 9(1):7–13
Jiang T, Brym MJC, Dube G, Lasia A, Brisard GM (2007) Studies on the AlCl3/dimethylsulfone (DMSO2) electrolytes for the aluminum deposition processes. Surf Coat Tech 201(14):6309–6317
Miyake M, Kubo Y, Hirato T (2014) Hull cell tests for evaluating the effects of polyethylene amines as brighteners in the electrodeposition of aluminum from dimethylsulfone-AlCl3 baths. Electrochim Acta 120:423–428
Wulf SE, Krauss W, Konys J (2014) Comparison of coating processes in the development of aluminum-based barriers for blanket applications. Fusion Eng Des 89(9–10):2368–2372
Von Brisinski LS, Goldmann D, Endres F (2014) Recovery of metals from tantalum capacitors with ionic liquids. Chemie Ingenieur Technik 86(1–2):196–199
Tsuda T, Ikeda Y, Imanishi A, Kusumoto S, Kuwabata S, Stafford GR, Hussey CL (2015) Electrodeposition of Al-W-Mn ternary alloys from the Lewis acidic aluminum chloride-1-ethyl-3-methylimidazolium chloride ionic liquid. J Electrochem Soc 162(9):D405–D411
Fang XQ, Uehara K, Kaneko S, Sato S, Tanabe T, Gunji T, Matsumoto F (2016) The effect of additives on the fabrication of electroplated bright aluminum films using AlCl3-1-ethyl-3-methylimidazolium chloride-toluene baths. Electrochemistry 84(1):17–24
Kosmus P, Steiner O, Goessler W, Gollas B, Fauler G (2016) Stability of nicotinate and dodecyl sulfate in a Lewis acidic ionic liquid for aluminum electroplating and characterization of their degradation products. Electrophoresis 37(7–8):1095–1100
Dilasari B, Jung Y, Sohn J, Kim S, Kwon K (2016) Review on corrosion behavior of metallic materials in room temperature ionic liquids. Int J Electrochem Sc 11(2):1482–1495
Endo A, Miyake M, Hirato T (2014) Electrodeposition of aluminum from 1,3-dimethyl-2-imidazolidinone/AlCl3 baths. Electrochim Acta 137:470–475
Alavianmehr MM, Taghizadehfard M, Hosseini SM (2016) Development of a perturbed hard-sphere equation of state for pure and mixture of ionic liquids. Ionics 22(5):649–660
Bakkar A, Neubert V (2015) A new method for practical electrodeposition of aluminium from ionic liquids. Electrochem Commun 51:113–116
Hurley FH, Wier TP (1951) The electrodeposition of aluminum from nonaqueous solutions at room temperature. J Electrochem Soc 98(5):207–212
Hussey CL, Xu XH (1991) Electrodissolution and electrodeposition of lead in an acidic room-temperature chloroaluminate molten salt. J Electrochem Soc 138(7):1886–1890
Pitner WR, Hussey CL, Stafford GR (1996) Electrodeposition of nickel-aluminum alloys from the aluminum chloride-1-methyl-3-ethylimidazolium chloride room temperature molten salt. J Electrochem Soc 143(1):130–138
Tsuda T, Hussey CL, Stafford GR (2004) Electrodeposition of Al-Mo alloys from the Lewis acidic aluminum chloride-1-ethyl-3-methylimidazolium chloride molten salt. J Electrochem Soc 151(6):C379–C384
Tsuda T, Arimoto S, Kuwabata S, Hussey CL (2008) Electrodeposition of Al-Mo-Ti ternary alloys in the Lewis acidic aluminum chloride-1-ethyl-3-methylimidazolium chloride room-temperature ionic liquid. J Electrochem Soc 155(4):D256–D262
Tseng CH, Chang JK, Chen JR, Tsai WT, Deng MJ, Sun IW (2010) Corrosion behaviors of materials in aluminum chloride-1-ethyl-3-methylimidazolium chloride ionic liquid. Electrochem Commun 12(8):1091–1094
Tsuda T, Ikeda Y, Arimura T, Imanishi A, Kuwabata S, Hussey CL, Stafford GR (2012) Al-W alloy deposition from Lewis acidic room-temperature chloroaluminate ionic liquid. ECS Trans 50(11):239–250
Tsuda T, Kuwabata S, Stafford GR, Hussey CL (2013) Electrodeposition of aluminum-hafnium alloy from the Lewis acidic aluminum chloride-1-ethyl-3-methylimidazolium chloride molten salt. J Solid State Electr 17(2):409–417
Tsuda T, Ikeda Y, Arimura T, Hirogaki M, Imanishi A, Kuwabata S, Stafford GR, Hussey CL (2014) Electrodeposition of Al-W alloys in the Lewis acidic aluminum chloride-1-ethyl-3-methylimidazolium chloride ionic liquid. J Electrochem Soc 161(9):D405–D412
Tian GC, Zhou XJ, Li J, Hua YX (2009) Quantum chemical aided molecular design of ionic liquids as green electrolytes for electrodeposition of active metals. Trans Nonferrous Metals Soc China 19(6):1639–1644
Lane GH (2012) Electrochemical reduction mechanisms and stabilities of some cation types used in ionic liquids and other organic salts. Electrochim Acta 83:513–528
Yue GK, Zhang SJ, Zhu YL, Lu XM, Li SC, Li ZX (2009) A promising method for electrodeposition of aluminium on stainless steel in ionic liquid. AICHE J 55(3):783–796
Zheng Y, Zhang SJ, Lu XM, Wang Q, Zuo Y, Liu L (2012) Low-temperature electrodeposition of aluminium from Lewis acidic 1-allyl-3-methylimidazolium chloroaluminate ionic liquids. Chinese J Chem Eng 20(1):130–139
Zhang QQ, Wang Q, Zhang SJ, Lu XM (2014) Effect of nicotinamide on electrodeposition of Al from aluminium chloride (AlCl3)-1-butyl-3-methylimidazolium chloride ([Bmim]Cl) ionic liquids. J Solid State Electr 18(1):257–267
Wang Q, Chen B, Zhang QQ, Lu XM, Zhang SJ (2015) Aluminum deposition from Lewis acidic 1-butyl-3-methylimidazolium chloroaluminate ionic liquid ([Bmim]Cl/AlCl3) modified with methyl nicotinate. Chemelectrochem 2(11):1794–1798
Wang Q, Zhang QQ, Chen B, Lu XM, Zhang SJ (2015) Electrodeposition of bright Al coatings from 1-butyl-3-methylimidazolium chloroaluminate ionic liquids with specific additives. J Electrochem Soc 162(8):D320–D324
Zhu YL, Katayama Y, Miura T (2010) Effects of acetonitrile on electrodeposition of Ni from a hydrophobic ionic liquid. Electrochim Acta 55(28):9019–9023
Fukui R, Katayama Y, Miura T (2011) The effect of organic additives in electrodeposition of Co from an amide-type ionic liquid. Electrochim Acta 56(3):1190–1196
Simons TJ, Bayley PM, Zhang Z, Howlett PC, MacFarlane DR, Madsen LA, Forsyth M (2014) Influence of Zn2+ and water on the transport properties of a pyrrolidinium dicyanamide ionic liquid. J Phys Chem B 118(18):4895–4905
Wang ZN, Cai YJ, Wang ZH, Chen SM, Lu XM, Zhang SJ (2013) Vinyl-functionalized imidazolium ionic liquids as new electrolyte additives for high-voltage Li-ion batteries. J Solid State Electr 17(11):2839–2848
Wang ZN, Cai YJ, Dong T, Chen SM, Lu XM (2013) Triethylbutylammonium bis (trifluoromethanesulphonyl) imide ionic liquid as an effective electrolyte additive for Li-ion batteries. Ionics 19(6):887–894
Leng MH, Chen SM, Zhang JL, Lang HY, Kang YH, Zhang SJ (2015) Effects of organic additives containing carbonyl group on electrodeposition of Al from AlCl3-[Emim]Cl ionic liquid. Acta Chim Sin 73(5):403
Liu L, Lu XM, Cai YJ, Zheng Y, Zhang SJ (2012) Influence of additives on the speciation, morphology, and nanocrystallinity of aluminium electrodeposition. Aust J Chem 65(11):1523–1528
Saruwatari H, Kuboki T, Kishi T, Mikoshiba S, Takami N (2010) Imidazolium ionic liquids containing LiBOB electrolyte for lithium battery. J Power Sources 195(5):1495–1499
Islam MM, Imase T, Okajima T, Takahashi M, Niikura Y, Kawashima N, Nakamura Y, Ohsaka T (2009) Stability of superoxide ion in imidazolium cation-based room-temperature ionic liquids. J Phys Chem A 113(5):912–916
Marcinek A, Zielonka J, Gebicki J, Gordon CM, Dunkin IR (2001) Ionic liquids: novel media for characterization of radical ions. J Phys Chem A 105(40):9305–9309
Berzins T, Delahay P (1953) Oscillographic polarographic waves for the reversible deposition of metals on solid electrodes. J Am Chem Soc 75(3):555–559
Pradhan D, Reddy RG (2014) Mechanistic study of Al electrodeposition from EMIC–AlCl3 and BMIC–AlCl3 electrolytes at low temperature. Mater Chem Phys 143(2):564–569
Keil P, Kick M, König A (2012) Long-term stability, regeneration and recycling of imidazolium-based ionic liquids. Chemie Ingenieur Technik 84(6):859–866
Abood HMA, Abbott AP, Ballantyne AD, Ryder KS (2011) Do all ionic liquids need organic cations? Characterisation of [AlCl2 · nAmide](+) AlCl4 − and comparison with imidazolium based systems. Chem Commun 47(12):3523–3525
Dong K, Song YT, Liu XM, Cheng WG, Yao XQ, Zhang SJ (2012) Understanding structures and hydrogen bonds of ionic liquids at the electronic level. J Phys Chem B 116(3):1007–1017
Acknowledgements
This work was financially supported by the 973 Project of China (No. 2015CB251401) and the National Nature Science Foundations of China (No. 21276257, 91534109, 91434203).
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Lang, H., Zhang, J., Kang, Y. et al. Effects of lithium bis(oxalato)borate on electrochemical stability of [Emim][Al2Cl7] ionic liquid for aluminum electrolysis. Ionics 23, 959–966 (2017). https://doi.org/10.1007/s11581-016-1889-5
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DOI: https://doi.org/10.1007/s11581-016-1889-5