Abstract
Electrodeposition of aluminum (Al) from an organic non-aqueous electrolyte of ethylbenzene containing aluminum bromide is demonstrated. It is offered as a simple method for the preparation of Al coatings. This work employs distinct electrochemical techniques and explores the effects of the experimental parameters on the kinetics of the process and the quality of the final coatings. The process presented here enables deposition of pure and crystalline Al at room temperature and facilitates the production of uniform Al coatings on various metallic substrates. Morphological studies establish that the growth of Al deposits follows an island mode, and thus, the most noteworthy effect of the substrate over the morphology of the deposits originates from its impact over the nucleation stage, and the density of islands. This study is complemented by theoretical modeling for the adsorption of Al atoms at the different surfaces. Corrosion evaluation determines the dissolution mechanisms of each of the studied substrates in the examined electrolyte. These findings further corroborate the claim that this electrolyte enables the reversible electrodeposition of Al.
Similar content being viewed by others
References
Zhao Y, VanderNoot TJ (1997) Review: Electrodeposition of aluminium from nonaqueous organic electrolytic systems and room temperature molten salts. Electrochim Acta 42(1):3–13
Abbott AP, Harris RC, Hsieh Y-T, Ryder KS, Sun IW (2014) Aluminium electrodeposition under ambient conditions. Phys Chem Chem Phys 16(28):14675–14681. https://doi.org/10.1039/c4cp01508h
Bakkar A, Neubert V (2015) A new method for practical electrodeposition of aluminium from ionic liquids. Electrochem commun 51:113–116. https://doi.org/10.1016/j.elecom.2014.12.012
Zhao Y, VanderNoot TJ (1997) Electrodeposition of aluminium from room temperature AlCl3-TMPAC molten salts. Electrochim Acta 42(11):1639–1643. https://doi.org/10.1016/S0013-4686(96)00271-X
Peled E, Mitvaski A, Reger A, Gileadi E (1977) Electrochemical properties of the AlBr3 / MBr / ArH solvent system and polarography of metal ions in it. J Electroanal Chem 75(2):677–695
Sheng LY, Yang F, Xi TF, Lai C, Ye HQ (2011) Influence of heat treatment on interface of Cu/Al bimetal composite fabricated by cold rolling. Compos Part B Eng 42(6):1468–1473. https://doi.org/10.1016/j.compositesb.2011.04.045
Kim IK, Hong SI (2014) Mechanochemical joining in cold roll-cladding of tri-layered Cu/Al/Cu composite and the interface cracking behavior. Mater Des 57:625–631. https://doi.org/10.1016/j.matdes.2014.01.054
Naseri M, Reihanian M, Borhani E (2016) Bonding behavior during cold roll-cladding of tri-layered Al/brass/Al composite. J Manuf Process 24:125–137. https://doi.org/10.1016/j.jmapro.2016.08.008
Lehmkuhl H, Mehler K, Landau U (1990) The principles and techniques of electrolytic aluminum deposition and dissolution in organoaluminum electrolytes. In: Gerischer H, Tobias CW (eds) Advances in Electrochemical Science and Engineering. VCH, pp 163–226
Abbott AP, Mckenzie KJ (2006) Application of ionic liquids to the electrodeposition of metals. Phys Chem Chem Phys 8(37):4265–4279. https://doi.org/10.1039/b607329h
Tsuda T, Stafford GR, Hussey CL (2017) Review—Electrochemical surface finishing and energy storage technology with room-temperature haloaluminate ionic liquids and mixtures. J Electrochem Soc 164(8):H5007–H5017. https://doi.org/10.1149/2.0021708jes
Wade WH, Twellmeyer GO, Yntema LF (1940) The deposition potentials of metals from fused alkali chloride-aluminum chloride baths. J Electrochem Soc 78(1):77–90
Fellner P, Chrenkova-Paucirova M, Matiasovsky K (1981) Electrolytic aluminum plating in molten salt mixtures based on AlCl3. Surf Technol 14(2):101–108
Couch DE, Brenner A (1952) A hydride bath for the electrodeposition of aluminum. J Electrochem Soc 99(6):234–244
Brenner A, Chase C, Couch DE (1953) Electrodeposition of aluminum from nonaqueous solutions. 1–2
Connor JH, Brenner A (1956) Electrodeposition of metals from organic solutions II. Further studies on the electrodeposition of aluminum. J Electrochem Soc 103:657–663
Ishibashi N, Yoshio M (1972) Electrodeposition of aluminium from the NBS type bath using tetrahydrofuran-benzene mixed solvent. Electrochim Acta 17(8):1343–1352. https://doi.org/10.1016/0013-4686(72)80080-X
Yoshio M, Ishibashi N (1973) High-rate plating of aluminium from the bath containing aluminium chloride and lithium aluminium hydride in tetrahydrofuran. J Appl Electrochem 3(4):321–325. https://doi.org/10.1007/BF00613040
Dotzer R, Hauschlidt H-G, Todt E (1977) Electroplating bath and method for the electrodeposition of bright aluminum coatings
Birkle S, Stoger K (1983) Electrolyte for the electrodeposition of aluminum. 1–4
Kautek W, Birkle S (1989) Aluminum-electrocrystallization from metal-organic electrolytes. Electrochim Acta 34(8):1213–1218. https://doi.org/10.1016/0013-4686(89)87160-9
Peled E, Gileadi E (1976) The electrodeposition of aluminum from aromatic hydrocarbon. J Electrochem Soc 123(1):15–19. https://doi.org/10.1149/1.2132753
Reger A, Peled E, Gileadi E (1976) Interfacial phenomena at solid aluminum electrodes in solutions of AlBr3/KBr in aromatic hydrocarbons. J Electrochem Soc 123(5):638–642. https://doi.org/10.1149/1.2132901
Blöchl PE (1994) Projector augmented-wave method. Phys Rev B 50(24):17953–17979. https://doi.org/10.1103/PhysRevB.50.17953
Kresse G, Joubert D (1999) From ultrasoft pseudopotentials to the projector augmented-wave method. Phys Rev B - Condens Matter Mater Phys 59(3):1758–1775. https://doi.org/10.1103/PhysRevB.59.1758
Kresse G, Furthmüller J (1996) Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set. Phys Rev B - Condens Matter Mater Phys 54(16):11169–11186. https://doi.org/10.1103/PhysRevB.54.11169
Jürgen H (2008) Ab-initio simulations of materials using VASP: density-functional theory and beyond. J Comput Chem 29:2044–2078. https://doi.org/10.1002/jcc
Gunawardena G, Hills G, Montenegro I, Scharifker BR (1982) Electrochemical nucleation. Part I. General considerations. J Electroanal Chem 138:225–239. https://doi.org/10.1016/0022-0728(82)85080-8
Scharifker BR, Hills G (1983) Theoretical and experimental studies of multiple nucleation. Electrochim Acta 28(7):879–889. https://doi.org/10.1016/0013-4686(83)85163-9
Paunovic M, Schlesinger M (1998) Fundamentals of electrochemical deposition. Wiley, New Jersey.
Abyaneh MY (1982) Calculation of overlap for nucleation and three-dimensional growth of centers. Electrochim Acta 27(9):1329–1334. https://doi.org/10.1016/0013-4686(82)80156-4
Abyaneh MY (1995) Generalization of transient equations due to the growth of hemispheroids. J Electroanal Chem 387(1-2):29–34. https://doi.org/10.1016/0022-0728(94)03822-K
Isaev VA, Baraboshkin AN (1994) Three-dimensional electrochemical phase formation. J Electroanal Chem 377(1-2):33–37. https://doi.org/10.1016/0022-0728(94)03450-8
Isaev VA, Grishenkova OV, Zaykov YP (2018) On the theory of 3D multiple nucleation with kinetic controlled growth. J Electroanal Chem 818:265–269. https://doi.org/10.1016/j.jelechem.2018.04.051
Lai Y, Liu F, Li J, Zhang Z, Liu Y (2010) Nucleation and growth of selenium electrodeposition onto tin oxide electrode. J Electroanal Chem 639(1-2):187–192. https://doi.org/10.1016/j.jelechem.2009.11.026
Abbott AP, Barron JC, Frisch G, Gurman S, Ryder KS, Fernando Silva A (2011) Double layer effects on metal nucleation in deep eutectic solvents. Phys Chem Chem Phys 13(21):10224–10231. https://doi.org/10.1039/c0cp02244f
Miller MA, Wainright JS, Savinell RF (2017) Iron Electrodeposition in a Deep Eutectic Solvent for Flow Batteries. J Electrochem Soc 164(4):A796–A803. https://doi.org/10.1149/2.1141704jes
Peled E, Brand M, Gileadi E (1981) Measurement of the viscosity and specific conductivity of an aluminum plating bath— the non-Stokesian mechanism of electrolytic conductivity. J Electrochem Soc 128(8):1697. https://doi.org/10.1149/1.2127713
Reger A, Peled E, Gileadi E (1979) Mechanism of high conductivity in a medium of low dielectric constant. J Phys Chem 83(7):873–879. https://doi.org/10.1021/j100470a023
Starosvetsky D, Sezin N, Ein-Eli Y (2010) Seedless copper electroplating on Ta from a “single” electrolytic bath. Electrochim Acta 55(5):1656–1663. https://doi.org/10.1016/j.electacta.2009.10.044
Goodfellow Cambridge Limited (1995) Goodfellow Catalogue 1994/95: metals, alloys, compounds, ceramics, polymers, composites
Parretta A, Jayaraj MK, Di Nocera A et al (1996) Electrical and optical properties of opper oxide films prepared by RF magnetron sputtering. Phys Status Solidi 155:399–404. https://doi.org/10.4028/www.scientific.net/AMR.194-196.2272
Sriram S, Thayumanavan A (2013) Structural, optical and electrical properties of NiO thin films prepered by low cost spray pyrolysis technique. Int J Mater Sci Eng 1:118–121. https://doi.org/10.12720/ijmse.1.2.118-121
Guo L, Searson PC (2010) On the influence of the nucleation overpotential on island growth in electrodeposition. Electrochim Acta 55(13):4086–4091. https://doi.org/10.1016/j.electacta.2010.02.038
Elam M, Gileadi E (1979) Cyclic Voltammetry in Solutions of aluminum bromide and KBr in aromatic hydrocarbons - surface processes. J Electrochem Soc 126(9):1474–1479. https://doi.org/10.1149/1.2116019
Curtarolo S, Setyawan W, Wang S, Xue J, Yang K, Taylor RH, Nelson LJ, Hart GLW, Sanvito S, Buongiorno-Nardelli M, Mingo N, Levy O (2012) AFLOWLIB.ORG: A distributed materials properties repository from high-throughput ab initio calculations. Comput Mater Sci 58:227–235. https://doi.org/10.1016/j.commatsci.2012.02.002
Jain A, Hautier G, Moore CJ, Ping Ong S, Fischer CC, Mueller T, Persson KA, Ceder G (2011) A high-throughput infrastructure for density functional theory calculations. Comput Mater Sci 50(8):2295–2310. https://doi.org/10.1016/j.commatsci.2011.02.023
Delczeg L, Delczeg-Czirjak EK, Johansson B, Vitos L (2011) Density functional study of vacancies and surfaces in metals. J Phys Condens Matter 23(4):045006. https://doi.org/10.1088/0953-8984/23/4/045006
Patra A, Bates JE, Sun J, Perdew JP (2017) Properties of real metallic surfaces: effects of density functional semilocality and van der Waals nonlocality. Proc Natl Acad Sci U S A 114(44):E9188–E9196. https://doi.org/10.1073/pnas.1713320114
Hinnemann B, Carter EA (2007) Adsorption of Al, O, Hf, Y, Pt, and S atoms on α-Al2O3(0001). J Phys Chem C 111(19):7105–7126. https://doi.org/10.1021/jp068869c
Wang L, Zhao J (2009) Which is the lowest-energy structure of Al13 clusters: assessment of different exchange-correlation functionals in density functional theory. J Comput Theor Nanosci 6(2):449–453
Jung J, Kim JC, Han YK (2005) Structure and electronic properties of Al13X (X=F, Cl, Br, and I) clusters. Phys Rev B - Condens Matter Mater Phys 72(15):1–5. https://doi.org/10.1103/PhysRevB.72.155439
Han YK, Jung J (2004) Structure and stability of Al13I clusters. J Chem Phys 121(17):8500–8502. https://doi.org/10.1063/1.1803538
Gupta SS, Van Huis MA, Dijkstra M, Sluiter MHF (2016) Depth dependence of vacancy formation energy at (100), (110), and (111) Al surfaces: a first-principles study. Phys Rev B 93(8):085432. https://doi.org/10.1103/PhysRevB.93.085432
Nie JL, Ao L, Zhao FA, Jiang M, Zu XT (2015) A first-principles study of bulk aluminum at high pressure. Can J Phys 93(8):825–829
Aguado A, López JM (2009) Structures and stabilities of Aln+, Aln, and Aln- (n=13-34) clusters. J Chem Phys 130(6):064704. https://doi.org/10.1063/1.3075834
Ahlrichs R, Elliott SD (1999) Clusters of aluminium, a density functional study. Phys Chem Chem Phys 1(1):13–21. https://doi.org/10.1039/a807713d
Funding
The authors acknowledge the financial support from Israel Council for Higher Education (CHE) and Israel Fuel Choice Initiative, within the framework of “Israel National Research Center for Electrochemical Propulsion” (INREP) and the Grand Technion Energy Program (GTEP).
Author information
Authors and Affiliations
Corresponding author
Additional information
Publisher’s note
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Electronic supplementary material
ESM 1
(PDF 1202 kb)
Rights and permissions
About this article
Cite this article
Yitzhack, N., Tereschuk, P., Sezin, N. et al. Aluminum electrodeposition from a non-aqueous electrolyte—a combined computational and experimental study. J Solid State Electrochem 24, 2833–2846 (2020). https://doi.org/10.1007/s10008-020-04626-x
Received:
Revised:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s10008-020-04626-x