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Etude de la croissance électrochimique de dépôts ramifiés

Abstract : This study focuses on the growth of metallic ramified branches, obtained by galvanostatic electrolysis of a stagnant aqueous solution of a metallic salt introduced within a Hele-Shaw cell. In the absence of supporting electrolyte, the electroneutrality forces enables the deposition to occur by successive nucleation/growth events, leading to ramified branches made up of nanocrystals. The main objective consist to get a better understanding and to elucidate the mechanisms of the building of the ramified electrodeposits, from the macroscale (branches) to the microscale (nanocrystals assembly). Another purpose is to exploit the formation of branch microstructure as an alternative method to produce metallic nanostructures (Cu, Zn, Fe, ..). A new experimental protocol enables the recovery, without damages, of the entire electrodeposit. The recovered branches were characterized at both macro and micro scales, by both optical and SEM observations, and the obtained data are analyzed with the support of theoretical modeling. Fluid motions are evidenced by optical observations tracking polystyrene microparticles and the determination by interferometry of the concentration field. The obtained results suggest the important role of the electroconvection on the spatial arrangement of the initial branches and therefore on the branch pattern. A morphological transition is observed on the microscale, when the applied current density j reaches a critical value j_c (concentration-dependent). Branches composed only of non-dendritic crystals were obtained for j < jc. Conversely, for j > jc , dendritic crystals appears and they predominate as j increases. A theoretical approach of the transition from nucleation/growth regime to a growth regime was elaborated. A particle size threshold was deduced by assimilating the onset of the dendritic growth to the initial morphological instability of a growing particle (crystal); the Fleury's nucleation/growth model was coupled with the Chazalviel's space charge model. The resulting threshold size is found to be the thickness of the space charge layer and its dependence on operating parameters (j,c_0) is in accordance with the experiments. Furthermore, considering an induction time before each nucleation event also promotes the (dendritic) growth instead of nucleation.
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Submitted on : Friday, September 4, 2020 - 11:44:22 AM
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  • HAL Id : tel-02930231, version 1



Chams Kharbachi. Etude de la croissance électrochimique de dépôts ramifiés. Cristallographie. Université Paul Sabatier - Toulouse III, 2019. Français. ⟨NNT : 2019TOU30244⟩. ⟨tel-02930231⟩



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