Annemie Adriaens

Ghent University, Gand, Flanders, Belgium

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Publications (192)441.41 Total impact

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    ABSTRACT: This work investigates the effect of cerium salt activated nanoparticles as nanoreservoirs on the self-healing properties of silane hybrid coatings deposited on electro-galvanized steel substrates. The substrates were pre-treated with 3–glycidoxypropyl-trimethoxysilane (GPTMS) and bisphenol A (BPA), modified with cerium ion-activated CeO2-ZrO2 and CeO2-SiO2 nanoparticles. The morphology of the coating before corrosion tests was examined using atomic force microscopy (AFM). The results indicate the formation of nanostructured surfaces with relatively uniform dispersion of nanoparticles in the silane coating containing CeO2-ZrO2 nanoparticles. The corrosion behavior of the sol-gel coatings was also investigated using salt spray tests, electrochemical impedance spectroscopy (EIS), and potentiodynamic polarization tests. During the salt spray test, the samples are exposed 600 h (or 25 days), revealing the improved resistance of the coated substrate containing CeO2-ZrO2 nanoparticles. Incorporation of activated CeO2-ZrO2 nanoparticles reduces the cathodic and anodic current density by one order of magnitude and shifts the corrosion potential to more positive values compared with the coating containing CeO2-SiO2 nanoparticles. Also, the EIS test results revealed higher impedance for the coating containing activated CeO2-ZrO2 nanoparticles. Corrosion tests results suggest that the activated CeO2-ZrO2 nanoparticles are more effective as nano-structured cerium ion reservoirs and can provide prolonged release of the inhibitor ions.
    No preview · Article · Jan 2016 · Materials and Corrosion
  • Roohangiz Zandi Zand · Kim Verbeken · Annemie Adriaens
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    ABSTRACT: This chapter explores the synthesis and self-healing properties of cerium-doped silane hybrid coatings. These coatings can protect steel structures from corrosion in marine environments. The analysis covers four main areas. First, effects of cerium ions, as a dopant, and bisphenol A (BPA), as a cross-linking agent, on the microstructure and corrosion resistance of hybrid coatings are examined. The self-healing properties of silane coatings doped with cerium nitrate and ceria nanoparticles are then evaluated via comparison of intact and artificially scratched films. The third and fourth sections of the chapter examine how the concentration of cerium nitrate and activation of ceria nanoparticles with cerium nitrate affect the ability of cerium-doped silane hybrid coatings to protect against corrosion.
    No preview · Chapter · Dec 2015
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    Mark Dowsett · Matt Hand · Pieter-Jan Sabbe · Paul Thompson · Annemie Adriaens
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    ABSTRACT: We describe a novel microscopy system which can obtain chemical maps from the surfaces of heritage metals in air or a controlled environment. The microscope, x-ray excited optical microscope Mk 1 (XEOM 1), forms images from x-ray excited optical luminescence (XEOL) induced by illuminating a few square millimetres of the sample with monochromated x-rays (broad beam or macroprobe illumination). XEOL is a spectroscopy tool in its own right and can, under the right circumstances, also be a vehicle for x-ray absorption spectroscopy. This (usually) synchrotron based technique provides information on the chemical state and short-range atomic order of the top few microns of a surface. It is thus well suited to heritage metal corrosion studies and is complementary to synchrotron x-ray diffraction. Imaging can be performed by scanning the sample under an x-ray microprobe. We show elsewhere that the power density needed for image acquisition on a reasonable time-scale is high enough to damage a patina and modify its chemistry. Although the damaged region may be invisible to the human eye, the data are characteristic of the damage and not the native chemistry of the surface. A macrobeam power density can be 4 orders of magnitude smaller than that for a microbeam and no surface modification was observed on test samples. Features of the instrument are demonstrated using copper test surfaces with a spatially varying patination to establish the ground work for the imaging of copper, cuprite, nantokite and atacamite/paratacamite and a first application from a bronze chain mail link. In parallel we have developed a suite of imaging software which can process XEOM image stacks to produce reduced data sets characteristic of various aspects of the surface chemical map. These include edge-shift (oxidation state) images and edge height (high contrast) images and spectra from user defined regions of interest. The technique can map the oxidation state of a surface from shifts in the absorption edge energy across columns of pixels in an image set, and map particular compounds from their characteristic XANES spectra. Optically filtered images give improved chemical selectivity and the data sets contain as yet untapped information sources. Graphical Abstract Illuminate a surface with an x-ray macroprobe; image the visible light emitted as a function of x-ray energy
    Full-text · Article · Dec 2015 · Heritage Science
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    Farzin Arjmand · Annemie Adriaens
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    ABSTRACT: The role of cathodic polarisation on the corrosion of 316L stainless steel was investigated under static and dynamic conditions. The results reveal that the applied flow regime during the cathodic polarisation process has a direct effect on the corrosion behaviour of steel. The cathodic polarisation of steel under static conditions increases the oxygen reduction rate and shifts the corrosion potential towards nobler potentials. Under dynamic conditions depending on the regime of the applied fluid flow during cathodic and anodic polarisation, the oxygen reduction rate can increase, causing the corrosion potential of the cathodically polarised steel to shift towards more positive direction. On the other hand, the oxygen reduction rate can decrease and the corrosion potential of the cathodically polarised steel shifts towards more negative potentials.
    Full-text · Article · Jul 2015 · CORROSION REVIEWS
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    ABSTRACT: Corrosion is the major problem in the degradation of heritage metal objects. The development of appropriate treatment methods to stabilize and protect artefacts is a undeniable scientific challenge. Here we propose a new coating method to protect lead heritage metal objects. This coating is environmentally safe, stable, reversible, easy to apply and to remove, and aesthetically justified. The coating consists of a compact and thick layer of lead ditetradecanoate, which is formed upon immersion of a lead substrate in a melted sample of tetradecanoic acid at 60 °C. Coated lead samples were exposed either to an aqueous corrosive environment or to a closed chamber with high relative humidity and an oak corrosive atmosphere. The corrosion resistance of the coating was followed for 60 days by electrochemical impedance spectroscopy and X-ray diffraction. Results show an unprecedented corrosion inhibition of the new coatings.
    Full-text · Article · May 2015 · Electrochimica Acta
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    ABSTRACT: The synthesis and characterisation of a reference sample containing a distinct geometrical pattern of Cu2O (cuprite) is described. The sample is to be used as an assessment sample to evaluate a newly developed X-ray-excited optical luminescence (XEOL) microscope, built for non-destructive chemical imaging of metal and other surfaces. The sample was produced by heating in a reducing flame and subsequent air exposure. It was characterized both qualitatively and quantitatively using X-ray photoelectron spectroscopy (XPS), X-ray absorption spectroscopy in both fluorescence mode (XAS) and optical luminescence mode (XEOL-XAS), and X-ray diffraction (XRD). Results indicate the presence of a layered structure comprising a heterogeneous mixture of cuprite and tenorite (CuO) with mainly cuprite (91.4%) in the near-surface regions and larger amounts of tenorite in the top 1-3 nm. The cuprite produced via this protocol was found to provide intense optical luminescence upon X-ray bombardment, which is particularly useful during the evaluation of the microscope
    Full-text · Article · Feb 2015 · Applied Surface Science
  • Koodlur Sannegowda Lokesh · Annemie Adriaens
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    ABSTRACT: The formation of a supramolecular electropolymerized film of a polymeric palladium phthalocyanine on a glassy carbon electrode is reported here. The film was obtained by cycling monomeric palladium tetraaminephthalocyanine in dimethyl sulfoxide in the potential range -0.5 to +1.0 V. The functionalized polymerized film on the electrode was characterized using Raman spectroscopy, X-ray photoelectron spectroscopy and electrochemical methods. A polymeric phthalocyanine film was shown to form by the oxidation of peripheral amino groups. It uniformly and completely covered the electrode surface. The modified electrode surface slightly blocked the reversible redox behavior of a redox probe owing to the thick polymeric film on its surface. The modified electrode showed a redox capacitance of 146 F g-1 at 0.27 V in 0.5 M sulfuric acid.
    No preview · Article · Jan 2015 · Dyes and Pigments
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    ABSTRACT: This paper concerns a time lapse spectroelectrochemical study of the growth of lead dodecanoate layers on a lead substrate in an aqueous solution using cyclic voltammetry. In-situ synchrotron radiation X-ray diffraction measurements were carried out on station BM26A (DUBBLE) at the European Synchrotron Radiation Facility (ESRF) in France. The diffraction pattern images were taken using a two-dimensional Mar CCD camera. After deposition of the coating, a spectroelectrochemical study of a linear sweep voltammetry experiment using an acetic acid electrolyte, simulating ‘active’ lead corrosion, was carried out on both a bare and lead dodecanoate coated sample. The results show that the coating inhibits the formation of new lead corrosion products.
    Full-text · Article · Jan 2015 · Talanta
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    ABSTRACT: The surface characteristics of a lead carboxylate coating induced on a lead substrate using a dimer acid are discussed together with its effectiveness against acetic acid corrosion. Thermogravimetric analysis and differential scanning calorimetry were used to examine the thermal properties of the hydrogenated dimer acid and its corresponding sodium salt. Scanning electron microscopy with energy-dispersive spectroscopy, X-ray photoelectron spectroscopy and infrared spectroscopy were used to visualize and characterize the deposited coatings on the lead substrate. Both the free dimer acid and the corresponding sodium salt formed a protective layer of lead carboxylate complexes through a reaction with the lead substrate. Single-sine electrochemical impedance spectroscopy and potentiodynamic polarization measurements of the bare and coated samples assessed the corrosion resistance of the coatings. Under the corrosive acetic acid test conditions, the lead-dimer-coated samples corroded more slowly than the bare lead.
    No preview · Article · Jan 2015 · Journal of The Electrochemical Society
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    ABSTRACT: Several heritage systems have been studied using state-of-the-art synchrotron techniques. The cultural heritage value of silver is documented in museum collections across the globe. However, the silver surface is not as chemically stable as that of other precious metals, and is susceptible to corrosion by atmospheric gases. It is therefore of special interest to clarify these surface reactions by using in-situ, time-lapse chemical and structural analysis in controlled ambients in order to develop strategies to reduce or even prevent the atmospheric attacks. In order to study the initial corrosion processes of silver in the presence of corrosive gases in-situ time-lapse X-ray diffraction experiments were performed on the XMaS beamline at the European Synchrotron Radiation Facility, Grenoble. Highly pure silver samples were weathered with synthetic air containing 500 ppb of both H2S and ozone, at relative humidity (RH) levels, and XRD patterns were tracked every 10 min over a total weathering time of 24h. The time-lapse Synchrotron Radiation (SR)-XRD data show that pure silver exposed to those atmospheres starts to form crystalline corrosion products after only 10 minutes. Silver sulfates, silver oxides, intermediates and mixed species are formed on the sample surface over the duration of the experiment. The data collected using a newly combined environmental cell/gas flow set up introduces a set of highly useful tools for scientists who wish to study time-lapse gaseous corrosion at ambient temperature and pressure.
    Full-text · Article · Jan 2015 · Journal of Analytical Atomic Spectrometry
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    ABSTRACT: This work investigates the effect of CeO2 and ZrO2 nanoparticles on the corrosion protection performance of non-inhibited and cerium inhibited silane coatings in 3.5% and 5% NaCl solutions on electro-galvanized steel substrates. Atomic force microscopy (AFM) results show relatively uniform coating thickness and varying nanoparticle distribution depending on coating composition. The corrosion behaviour of the sol-gel coatings revealed that CeO2-ZrO2 nanoparticles reinforce the barrier properties of the silane films and seem to act as nano-reservoirs providing a prolonged release of cerium ions. This prolonged release of inhibitor from oxide nanoreservoirs confers longer protection to the metallic substrate.
    Full-text · Article · Jan 2015 · International journal of electrochemical science
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    Full-text · Article · Dec 2014
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    ABSTRACT: The hydrolysis of nantokite to form cuprite could be a reaction step in the progression of bronze disease on cupreous objects d'art. In this paper, this transformation is visualized for the first time using a time-resolved synchrotron X-ray diffraction experiment. Complete conversion of nantokite to cuprite was observed on a nantokite patina over 5 h in water using time-resolved synchrotron X-ray diffraction.
    Full-text · Article · Nov 2014 · Corrosion Science
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    Full-text · Dataset · Nov 2014
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    Full-text · Dataset · Nov 2014
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    ABSTRACT: The application of a modular system for the non-destructive chemical imaging of metal and other surfaces is described using heritage metals as an example. The custom-built X-ray-excited optical luminescence (XEOL) microscope, XEOM 1, images the chemical state and short-range atomic order of the top 200 nm of both amorphous and crystalline surfaces. A broad X-ray beam is used to illuminate large areas (up to 4 mm²) of the sample, and the resulting XEOL emission is collected simultaneously for each pixel by a charge-coupled device (CCD) sensor to form an image. The input X-ray energy is incremented across a range typical for XANES and an image collected for each increment. The use of large-footprint beams combined with parallel detection allows the power density, to be kept low and facilitates complete non-destructive XANES mapping on a reasonable timescale. In this study the microscope was evaluated by imaging copper surfaces with well-defined patterns of different corrosion products (cuprite Cu2O and nantokite CuCl). The images obtained show chemical contrast, and filtering the XEOL light allowed different corrosion products to be imaged separately. Absorption spectra extracted from software selected regions of interest exhibit characteristic XANES fingerprint spectra for the compounds present. Moreover, when the X-ray absorption edge positions were extracted from each spectrum an oxidation state map of the sample could be compiled. The results show that this method allows one to obtain non-destructive and non-invasive information at the micron-scale whilst using full-field imaging.
    Full-text · Article · Nov 2014 · Analytical Chemistry
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    ABSTRACT: Objective To assess the site-specific corrosive behaviour of the frameless IUD following long-term exposure to the uterine environment. Study design A qualitative and morphological study using X-ray diffraction (XRD) and scanning electron microscopy (SEM). Results Three GyneFix® IUDs which were in site up to 150 months were examined. In utero corroded copper sleeves were divided into 10 different groups based on their shape (U or O), orientation (inside or outside) and in utero residence time. X-ray diffraction indicated the presence of solely cuprite (Cu2O) as corrosion product on both the inside and the outside of the copper sleeves, regardless of their shape. These results were confirmed by backscattered electron micrographs recorded on the inside, the outside and the cross-section of the IUD sleeve. SEM results suggest that shape and orientation slightly affect the corrosion rate. Conclusion The apparent copper loss from both sides of GyneFix copper tubes proves that both sides are a potential copper source and therefore justifies the design of GyneFix IUD. This could be beneficial for women as the IUD could be reduced in size and therefore better tolerated. The impact on bleeding could also be minimized.
    Full-text · Article · Oct 2014 · Contraception
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    ABSTRACT: Background: Ethanolic solutions of long-chain carboxylic acids can be applied to lead metal substrates to form a coating of lead carboxylate which provides protection against atmospheric pollutants. Results and conclusions: In this paper we describe the optimal inhibitor concentration for the coating on lead. Electrochemical impedance data taken before and after immersion in media modelling oak emitted volatile organic compounds (VOCs) polluted atmospheres show that coating effectiveness decreases after exposure, but the effect is lessened if longer chain carboxylates are used.
    Full-text · Article · Jul 2014 · Heritage Science
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    Full-text · Poster · Jul 2014
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    ABSTRACT: This work investigates the effect of the ceria nanoparticle concentration on the morphology and electrochemical behavior of cerium-silane hybrid coatings deposited on electro-galvanized steel substrates. The substrates were pre-treated with 3-glycidoxypropyl-trimethoxysilane and bisphenol A, modified with cerium ion-activated CeO2 nanoparticles. The morphology of the coating before and after corrosion tests was examined using atomic force microscopy and scanning electron microscopy. The results indicate the formation of nanostructured surfaces with relatively uniform thicknesses and nanoparticle distribution. Microscopic observations explain the increased durability of the silane coating doped with the lowest content of activated ceria nanoparticles after short-term corrosion tests (456 h). The corrosion behavior of the sol- gel coatings was also investigated using natural salt spray tests, electrochemical impedance spectroscopy, and potentiodynamic polarization tests. The results show that the concentration of nanoparticles has a significant impact on the barrier properties of the silane films, which are improved for films with lower nanoparticle contents.
    Full-text · Article · Jun 2014 · Materials Chemistry and Physics

Publication Stats

1k Citations
441.41 Total Impact Points

Institutions

  • 2002-2015
    • Ghent University
      • Department of Analytical Chemistry
      Gand, Flanders, Belgium
  • 2011-2013
    • Sapienza University of Rome
      • Department of Computer Science
      Roma, Latium, Italy
  • 1989-2003
    • University of Antwerp
      • Department of Chemistry
      Antwerpen, Flanders, Belgium