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  • 1
    Online Resource
    Online Resource
    Elsevier BV ; 2021
    In:  Current Opinion in Electrochemistry Vol. 27 ( 2021-06), p. 100688-
    In: Current Opinion in Electrochemistry, Elsevier BV, Vol. 27 ( 2021-06), p. 100688-
    Type of Medium: Online Resource
    ISSN: 2451-9103
    Language: English
    Publisher: Elsevier BV
    Publication Date: 2021
    detail.hit.zdb_id: 2879302-X
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  • 2
    In: Advanced Functional Materials, Wiley
    Abstract: In the search for non‐enzymatic alternatives to glucose oxidase, reliable and microchip‐compatible approaches to catalyst development are highly desirable. Herein, the electrochemical behavior of thin films of VOx deposited by molecular beam epitaxy (MBE) on glassy carbon electrodes is reported . A process of partial etching during polarization is observed. Thereafter, highly active and stable traces of VOx act as catalytic centers for glucose electrooxidation. A mechanistic description of the electrochemical process is proposed based on evidence provided by voltammetric measurements. The sensors are calibrated both with potentiometric and amperometric techniques, the former showing a wide linear range (1–10 mM), good sensitivity (14.93 ± 0.39 µA cm −2 × mM –1 ) and a limit of detection (0.32 m‐M). Unlike most metal oxides, it is shown that VOx on glassy carbon is capable of successfully oxidizing glucose at −0.4 V. Such a one‐of‐kind behavior can have important ramifications for energy‐efficient integrated electrochemical sensors and non‐enzymatic glucose sensing as a whole.
    Type of Medium: Online Resource
    ISSN: 1616-301X , 1616-3028
    Language: English
    Publisher: Wiley
    Publication Date: 2023
    detail.hit.zdb_id: 2029061-5
    detail.hit.zdb_id: 2039420-2
    SSG: 11
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  • 3
    Online Resource
    Online Resource
    The Electrochemical Society ; 2022
    In:  ECS Meeting Abstracts Vol. MA2022-01, No. 23 ( 2022-07-07), p. 1148-1148
    In: ECS Meeting Abstracts, The Electrochemical Society, Vol. MA2022-01, No. 23 ( 2022-07-07), p. 1148-1148
    Abstract: Electrochemical nucleation and growth (EN & G) is the cornerstone for many (nano)material growth routes and the main factor limiting battery durability. At the same time electrochemical dissolution (ED) is the main cause of material degradation in exposed environments (corrosion) or energy conversion and storage devices. The in-depth experimental assessment of both processes is very challenging. The reasons are the random nature of initiation events (nucleation), the heterogeneity of surfaces and the (very) fast kinetics of these processes across several length scales. For all that, our current understanding of the mechanisms involved is inaccurate and incomplete [1]. During the last years, we have developed an approach based on using carbon-coated TEM grids as electrodes to combine ex-situ atomic-scale TEM characterization with electron tomography and macroscale electrochemical measurements [2,3]. This approach has brought valuable evidence of non-classical growth pathways such as growth mediated by nanocluster aggregation. Yet, it does not capture the influence of the heterogeneous nature of the surface where EN & G proceeds, nor the dynamics before, during and after nucleation [4,5]. In this contribution, we present our recent work in which we combine high-throughput nanoscale resolved electrochemistry by Scanning Electrochemical Cell Microscopy (SECCM), with ex-situ and in-situ high resolution characterization, including electrochemical transmission electron microscopy (EC-TEM), to study the electrochemical nucleation, growth, and dissolution of metal (Cu, Au, Ag and Pt) nanoparticles (NPs) [6,7]. The spatially resolved electrochemical characterization enables a one-to-one correlation between the electrochemical data and the local surface properties, which can be evaluated by different surface analytical tools. Moreover, the confinement of the electrochemical cell to the SECCM meniscus enables us to resolve a diversity of events during the electrochemical dissolution of electrodeposited NPs. EC-TEM experiments advocate that the nature of these events corresponds to the dissolution of individual NPs spanning a wide range of time [6]. The combination of SECCM and EC-TEM opens up new opportunities for the rational design of functional nanostructured materials by electrodeposition, and for the evaluation of their durability under electrochemical polarization. The ability to study these taking into account the heterogeneous nature of the supports and the differences within nanomaterial ensembles is essential for applications in electrochemical conversion and storage. References: [1] Ustarroz, J. Current Opinion in Electrochemistry . 19 (2020) 144–152. [2] Ustarroz, J et al. Journal of the American Chemical Society (2013), 135, 11550–11561. [3] Ustarroz, J et al. The Journal of Physical Chemistry C (2012), 116, 2322–2329. [4] Hussein H. E. M. et al., ACS Nano . 12, 7388–7396 (2018). [5] Harniman R. L. et al., Nat. Commun. 8, 971 (2017). [6] Bernal, M. et al. In revision (2022). [7] Torres, D. et al. To be submitted (2022).
    Type of Medium: Online Resource
    ISSN: 2151-2043
    Language: Unknown
    Publisher: The Electrochemical Society
    Publication Date: 2022
    detail.hit.zdb_id: 2438749-6
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  • 4
    Online Resource
    Online Resource
    The Electrochemical Society ; 2022
    In:  ECS Meeting Abstracts Vol. MA2022-01, No. 23 ( 2022-07-07), p. 1203-1203
    In: ECS Meeting Abstracts, The Electrochemical Society, Vol. MA2022-01, No. 23 ( 2022-07-07), p. 1203-1203
    Abstract: Electrodeposition is a convenient strategy for the synthesis of functional nanostructures, for which electrochemical nucleation and growth (EN & G) processes need to be well understood [1]. As a heterogenous process, understanding the distribution of nucleation sites on a substrate is fundamental to relate the microscopic events to the macroscopic properties of the new deposit. In this work, we have explored the EN & G process on a glassy carbon substrate with a local electrochemical approach based on the Scanning Electrochemical Cell Microscopy (SECCM), using copper as a case of study [2]. Since the studies of EN & G are extremely sensitive to the state of the surface, the diversity of the nucleation process is revealed by performing hundreds of spatially resolved experiments on the heterogeneous surface of the glassy carbon [2,3]. The spatially-resolved characterization opens up the opportunity to correlate the electrochemical information to the local surface state, which can be modified with common surface pretreatments (i. e., polishing and preanodization). This unique perspective of the EN & G can help to deconvolute the individual contributions to the overall process, bringing forward information on nucleation sites that is unavailable with the conventional macroscopic approach. [1] J. Ustarroz, Current atomic-level understanding of electrochemical nucleation and growth on low-energy surfaces, Curr. Opin. Electrochem. 19 (2020) 144–152. [2] D.Torres, M. Bernal, J. Ustarroz, distribution of copper nucleation activities on glassy carbon: a new local perspective, to be submitted 2022 [3] M. Bernal, D. Torres, S. Semsari, M. Čeh, K. Žužek Rožman, S. Šturm, J. Ustarroz, Diversity matters: Influence of surface heterogeneities in the electrochemical nucleation and dissolution of Au nanoparticles, under revision . Figure 1
    Type of Medium: Online Resource
    ISSN: 2151-2043
    Language: Unknown
    Publisher: The Electrochemical Society
    Publication Date: 2022
    detail.hit.zdb_id: 2438749-6
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  • 5
    Online Resource
    Online Resource
    The Electrochemical Society ; 2020
    In:  ECS Meeting Abstracts Vol. MA2020-01, No. 19 ( 2020-05-01), p. 1197-1197
    In: ECS Meeting Abstracts, The Electrochemical Society, Vol. MA2020-01, No. 19 ( 2020-05-01), p. 1197-1197
    Abstract: Nowadays, supporting metal nanoparticles have attracted much interest due to their fascinating physio-chemical properties and potential application in fuel cells, sensors, catalysis, solar to fuel devices and among others. One of the interesting issues from engaging physiochemical properties of supporting nanoparticles is to understand their nucleation and growth mechanism in order to get a good control of their structural and morphological parameters. Although studied for decades, however, the full details are still out of reach [1]. In this presentation, we will first review the classical theory of nucleation and growth and secondly present our recent finding and theoretical development on the growth of an isolated metal nanoparticle using a combined experimental (linear sweep voltammetry, chronoamperommetry and FESEM) and multiscale modelling approach [2-5] . In this presentation we focused on the modelling approach. The use of such a multiscale framework allows studying nanoscale electrochemical deposition as a whole, without the need to assume a dominant growth mechanism such as diffusion or kinetic control [2-5]. The simulation results reveal that the existing theory of nucleation and growth is only valid for some specific conditions. Some of the findings will be discussed in this presentation. References [1]. Ustarroz, J., Hammons, J. A., Altantzis, T., Hubin, A., Bals, S., & Terryn, H. (2013). A generalized electrochemical aggregative growth mechanism. Journal of the American Chemical Society , 135 (31), 11550-11561. [2]. Mamme, M. H., Dolgikh, O., Ustarroz, J., Simillion, H., Terryn, H., & Deconinck, J. (2016). A finite element simulation of the electrochemical growth of a single hemispherical silver nucleus. Electrochimica Acta , 197 , 307-317. [3]. Mamme, M. H., Deconinck, J., & Ustarroz, J. (2017). Transition between kinetic and diffusion control during the initial stages of electrochemical growth using numerical modelling. Electrochimica Acta , 258 , 662-668. [4]. Mamme, M. H., Köhn, C., Deconinck, J., & Ustarroz, J. (2018). Numerical insights into the early stages of nanoscale electrodeposition: nanocluster surface diffusion and aggregative growth. Nanoscale , 10 (15), 7194-7209. [5]. Cherigui, E. A. M., Sentosun, K., Mamme, M. H., Lukaczynska, M., Terryn, H., Bals, S., & Ustarroz, J. (2018). On the control and effect of water content during the electrodeposition of Ni nanostructures from deep eutectic solvents. The Journal of Physical Chemistry C , 122 (40), 23129-23142.
    Type of Medium: Online Resource
    ISSN: 2151-2043
    Language: Unknown
    Publisher: The Electrochemical Society
    Publication Date: 2020
    detail.hit.zdb_id: 2438749-6
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  • 6
    In: ECS Meeting Abstracts, The Electrochemical Society, Vol. MA2019-02, No. 17 ( 2019-09-01), p. 969-969
    Abstract: Green, stable, and wide electrochemical window deep eutectics solvents (DESs) are ideal candidates for electrochemical systems, such as batteries, supercapacitors, catalysis, electrodeposition, and many more. However, since these mixtures are highly dense and composed of only large asymmetric ionic and molecular components, short-range ion-ion, ion-molecule interactions play a dominant role both in the bulk as well as at the interface properties. This results in breakdown of the standard mean-field approximation, which is the basis of dilute solution theory. In addition, due to the hygroscopic nature of DESs, the presence of latent water is unavoidable. Therefore, understanding the DESs-electrode interface (electrical double layer structure, EDLS) together with the role of water at a molecular scale is of great importance for the widespread use of these solvents in electrochemical systems [1-3]. In this presentation, we will first review the benchmark study on conventional dilute solution electrical double layer structure and secondly present our recent findings and theoretical developments on the electrochemical interfacial structure of deep eutectic solvents using a combined experimental and a novel atomistic molecular dynamics approach. In the presentation, we focused on the computational approach. The use of such an atomistic-molecular approach allows investigation of all the possible bulk and interfacial interactions and, consequently, helps to shed light on the nanoscale electrochemical interfacial structure of DESs. Unlike the interfacial structures observed and proposed for other electrolyte-electrode interfaces (compact- diffuse double layer for dilute solution [4] ; overscreening or crowding for concentrated solutions [5]), the simulations of DESs-electrode interfacial structure show an unexpected and previously unrecognized phenomenon: the electrochemical interface is composed of a mixed layer structure followed by a mixed charged clustered layer regardless of the surface polarization [1,2] . Some of the findings will be discussed in this presentation. References [1] M. H. Mamme, S. Moors, H. Terryn, J. Deconinck, J. Ustarroz, and F. De Proft, “Atomistic Insight into the Electrical Double La yer of Choline Chloride-Urea Deep Eutectic Solvents: Clustered Interfacial Structuring”, JPCL,9:6296,2018. [2] El A. M. Cherigui, K. Sentosun, M. H. Mamme, M. Lukaczynska, S. Bals, H. Terryn, and J. Ustarroz, “On the Control and Effect of Water Content During the Electrodposition of Ni Nanostructure from Deep Eutectic Solvents”, JPCC, 122: 23129, 2018. [3] M. H. Mamme, S. Moors, El A. M. Cherigui, H. Terryn, J. Deconinck, J. Ustarroz, and F. De Proft, “Water Distribution at the Electrified interface of Deep Eutectics solvent", under review, 2019. [4] G. Jiang, C. Cheng, D. Li, J.Z. Liu, “Molecular dynamics simulations of the electric double layer capacitance of graphene electrodes in mono-valent aqueous electrolytes.” Nano Res. 9, 174−186,2016. [5] M.V. Fedorov, A. A. Kornyshev, “Ionic liquids at electrified interfaces.” Chem. Rev. 114, 2978−3036, 2014.
    Type of Medium: Online Resource
    ISSN: 2151-2043
    Language: Unknown
    Publisher: The Electrochemical Society
    Publication Date: 2019
    detail.hit.zdb_id: 2438749-6
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  • 7
    In: Electrochimica Acta, Elsevier BV, Vol. 197 ( 2016-04), p. 307-317
    Type of Medium: Online Resource
    ISSN: 0013-4686
    Language: English
    Publisher: Elsevier BV
    Publication Date: 2016
    detail.hit.zdb_id: 1483548-4
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  • 8
    In: Applied Catalysis B: Environmental, Elsevier BV, Vol. 181 ( 2016-02), p. 542-549
    Type of Medium: Online Resource
    ISSN: 0926-3373
    Language: English
    Publisher: Elsevier BV
    Publication Date: 2016
    detail.hit.zdb_id: 2017331-3
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  • 9
    In: Electrochemistry Communications, Elsevier BV, Vol. 122 ( 2021-01), p. 106878-
    Type of Medium: Online Resource
    ISSN: 1388-2481
    Language: English
    Publisher: Elsevier BV
    Publication Date: 2021
    detail.hit.zdb_id: 2027290-X
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  • 10
    Online Resource
    Online Resource
    The Electrochemical Society ; 2015
    In:  Journal of The Electrochemical Society Vol. 162, No. 9 ( 2015), p. E166-E172
    In: Journal of The Electrochemical Society, The Electrochemical Society, Vol. 162, No. 9 ( 2015), p. E166-E172
    Type of Medium: Online Resource
    ISSN: 0013-4651 , 1945-7111
    RVK:
    Language: English
    Publisher: The Electrochemical Society
    Publication Date: 2015
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