Spatio-Temporal Organization in a Morphochemical Electrodeposition Model: Analysis and Numerical Simulation of Spiral Waves

Lacitignola, Deborah; Bozzini, Benedetto; Sgura, Ivonne

doi:10.1007/s10440-014-9910-3

Cited by 21 publications

(25 citation statements)

References 20 publications

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“…Thanks to chemical sensitivity, ptychographic data encode information about both shape and amount of electrodeposited material, allowing to quantify variations originated by to a given sequence of growth steps. In keeping with our previous observations on Mn (Kourousias et al 2016;Bozzini et al 2017b) and with the predictions of the DIB model (in particular Lacitignola et al 2014), the evolution of the individual Co aggregates shows that global growth is indeed accompanied by local dissolution events.…”

Section: In Situ Imaging After Incremental Growthsupporting

confidence: 56%

“…The wealth of morphochemical information gleaned by-in situ ptychography calls for a modelling environment able to profit from the raw data collected with high precision in view of developing physico-chemical insight. In this context, the DIB model for electrochemical phase-formation (Bozzini et al 2012c;Lacitignola et al 2014;Gianoncelli et al 2015) in conjunction with parameter-identification tools able to extract compact kinetic data in an automated way (D'Autilia et al 2017;Sgura et al 2018) is a promising platform for the development of knowledge-based electrochemical material design and battery control. Even though the specific focus of this paper is on electrodeposition, the ) at the electrode/electrolyte interface, measured after 100 and 110 growth cycles.…”

Section: Discussionmentioning

confidence: 99%

“…Adding nominally 10% of material is not expected to change the catalytic performance (Bocchetta et al 2016), but can provide precious mechanistic information in the framework of the DIB model of electrodeposition based on the feedback of electrodeposit morphology on chemical localization (Bozzini et al 2012c;Lacitignola et al 2014;Gianoncelli et al 2015). Thus, after the second growth step, we recorded diffractograms with the same procedure described above, again scanning the energy across the Co L 3 -edge.…”

Section: In Situ Imaging After Incremental Growthmentioning

confidence: 99%

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Monitoring dynamic electrochemical processes with in situ ptychography

et al. 2018

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The present work reports novel soft X-ray Fresnel CDI ptychography results, demonstrating the potential of this method for dynamic in situ studies. Specifically, in situ ptychography experiments explored the electrochemical fabrication of Codoped Mn-oxide/polypyrrole nanocomposites for sustainable and cost-effective fuel-cell air-electrodes. Oxygen-reduction catalysts based on Mn-oxides exhibit relatively high activity, but poor durability: doping with Co has been shown to improve both reduction rate and stability. In this study, we examine the chemical state distribution of the catalytically crucial Co dopant to elucidate details of the Co dopant incorporation into the Mn/polymer matrix. The measurements were performed using a custom-made three-electrode thin-layer microcell, developed at the TwinMic beamline of Elettra Synchrotron during a series of experiments that were continued at the SXRI beamline of the Australian Synchrotron. Our time-resolved ptychography-based investigation was carried out in situ after two representative growth steps, controlled by electrochemical bias. In addition to the observation of morphological changes, we retrieved the spectroscopic information, provided by multiple ptychographic energy scans across Co L 3 -edge, shedding light on the doping mechanism and demonstrating a general approach for the molecular-level investigation complex multimaterial electrodeposition processes.

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Section: In Situ Imaging After Incremental Growthsupporting

confidence: 56%

Section: Discussionmentioning

confidence: 99%

Section: In Situ Imaging After Incremental Growthmentioning

confidence: 99%

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Monitoring dynamic electrochemical processes with in situ ptychography

et al. 2018

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“…We have, however, found complex spatio-temporal behaviour for this system, but not in the immediate vicinity of the TH point and for parameter choices well inside the Hopf region, where the local system kinetics exhibits an oscillatory regime. This phenomenology appears to be related to the system capability to support spiral wave behaviour in the Hopf region as well as an intriguing phenomenon of spiral break up, that we have pointed up in a recent paper [41].…”

Section: Discussionmentioning

confidence: 72%

Spatio-temporal organization in a morphochemical electrodeposition model: Hopf and Turing instabilities and their interplay

2014

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In this paper, we investigate from a theoretical point of view the 2D reaction-diffusion system for electrodeposition coupling morphology and surface chemistry, presented and experimentally validated in Bozzini et al. (2013 J. Solid State Electr. 17, 467-479). We analyse the mechanisms responsible for spatio-temporal organization. As a first step, spatially uniform dynamics is discussed and the occurrence of a supercritical Hopf bifurcation for the local kinetics is proved. In the spatial case, initiation of morphological patterns induced by diffusion is shown to occur in a suitable region of the parameter space. The intriguing interplay between Hopf and Turing instability is also considered, by investigating the spatio-temporal behaviour of the system in the neighbourhood of the codimensiontwo Turing-Hopf bifurcation point. An ADI (Alternating Direction Implicit) scheme based on high-order finite differences in space is applied to obtain numerical approximations of Turing patterns at the steady state and for the simulation of the oscillating Turing-Hopf dynamics.

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“…A comprehensive discussion of the physics underlying this model and an extensive experimental validation are expounded in the studies of Lacitignola et al [61,62] and Bozzini et al [63,66] Here, we briefly recall its basic factors, and in the Appendix, we propose an extension that allows to simulate XRF maps and i-t transients, which will be employed for the study of electrodeposited Mn-Mg-Cu/PPy composites.…”

Section: Mathematical Modelling Of Xrf Maps: the Methodsmentioning

confidence: 98%

High‐lateral resolution X‐ray fluorescence microspectroscopy and dynamic mathematical modelling as tools for the study of electrodeposited electrocatalysts

et al. 2015

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In this paper, we report on the use of high-space resolution soft X-ray fluorescence microspectroscopy for the study of electrodeposited composites containing catalytic ternary metal nanostructures. X-ray fluorescence maps are interpreted in terms of a dynamic mathematical model of the electrode morphology and metal space distribution, allowing to reproduce the observed space patterns and electrochemical transients by assigning an appropriate set of electrokinetic parameters. The discussed materials-science case is the electrochemical growth of a Mn-Mg-Cu-polypyrrole nanocomposite electrocatalyst material -free of expensive Pt and environmentally unfriendly Co -with promising performance for fuel-cell oxygen electrodes. The synergy of high-resolution compositional mapping with electrokinetic modelling not only provides the general rationale for quantitative use of potentially large compositional distribution datasets but also yields unprecedented insight into the specific catalyst synthesis process. The expounded application is just a prototypical case study of a more general approach, which can be employed for the understanding of electrochemical material science processes, both in situ and ex situ, as well as for the characterisation of the corresponding products, with no other limitations in principle than X-ray transmission and beam damage.

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Spatio-Temporal Organization in a Morphochemical Electrodeposition Model: Analysis and Numerical Simulation of Spiral Waves

Cited by 21 publications

References 20 publications

Monitoring dynamic electrochemical processes with in situ ptychography

Monitoring dynamic electrochemical processes with in situ ptychography

Spatio-temporal organization in a morphochemical electrodeposition model: Hopf and Turing instabilities and their interplay

High‐lateral resolution X‐ray fluorescence microspectroscopy and dynamic mathematical modelling as tools for the study of electrodeposited electrocatalysts

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