Engineering topics

Terryn, Herman

Publications and source records attributed to Terryn, Herman.

5 records

DOE OSTI2017

Water Adsorption and Dissociation on Polycrystalline Copper Oxides: Effects of Environmental Contamination and Experimental Protocol

We use ambient-pressure X-ray photoelectron spectroscopy (APXPS) to study chemical changes, including hydroxylation and water adsorption, at copper oxide surfaces from ultrahigh vacuum to ambient relative humidities of ~5%. Polycrystalline CuO and Cu 2 O surfaces were prepared by selective oxidation of metallic copper foils. For both oxides, hydroxylation occurs readily, even at high-vacuum conditions. Hydroxylation on both oxides plateaus near ~0.01% relative humidity (RH) at a coverage of ~1 monolayer. In contrast to previous studies, neither oxide shows significant accumulation of molecular water; rather, both surfaces show a high affinity for adventitious carbon contaminants. Results of isobaric and isothermic experiments are compared, and the strengths and potential drawbacks of each method are discussed. We also provide critical evaluations of the effects of the hot filament of the ion pressure gauge on the reactivity of gas-phase species, the peak fitting procedure on the quantitative analysis of spectra, and rigorous accounting of carbon contamination on data analysis and interpretation. Lastly, this work underscores the importance of considering experimental design and data analysis protocols during APXPS experiments with water vapor in order to minimize misinterpretations arising from these factors.

36 MATERIALS SCIENCE↗

DOE OSTI2017

Unravelling the Chemical Influence of Water on the PMMA/Aluminum Oxide Hybrid Interface In Situ

Understanding the stability of chemical interactions at the polymer/metal oxide interface under humid conditions is vital to understand the long-term durability of hybrid systems. Therefore, the interface of ultrathin PMMA films on native aluminum oxide, deposited by reactive adsorption, was studied. The characterization of the interface of the coated substrates was performed using ambient pressure X-ray photoelectron spectroscopy (APXPS), Fourier transform infrared spectroscopy in the Kretschmann geometry (ATR-FTIR Kretschmann) and time-of-flight secondary ion mass spectrometry (ToF-SIMS). The formation of hydrogen bonds and carboxylate ionic bonds at the interface are observed. The formed ionic bond is stable up to 5 Torr water vapour pressure as shown by APXPS. However, when the coated samples are exposed to an excess of aqueous electrolyte, an increase in the amount of carboxylate bonds at the interface, as a result of hydrolysis of the methoxy group, is observed by ATR-FTIR Kretschmann. In conclusion, these observations, supported by ToF-SIMS spectra, lead to the proposal of an adsorption mechanism of PMMA on aluminum oxide, which shows the formation of methanol at the interface and the effect of water molecules on the different interfacial interactions.

36 MATERIALS SCIENCE↗

DOE OSTI2017

Fatigue Performance of Ti-6Al-4V Additively Manufactured Specimens with Integrated Capillaries of an Embedded Structural Health Monitoring System

Additive manufacturing (AM) of metals offers new possibilities for the production of complex structures. Up to now, investigations on the mechanical response of AM metallic parts show a significant spread and unexpected failures cannot be excluded. In this work, we focus on the detection of fatigue cracks through the integration of a Structural Health Monitoring (SHM) system in Ti-6Al-4V specimens. The working principle of the presented system is based on the integration of small capillaries that are capable of detecting fatigue cracks. Four-point bending fatigue tests have been performed on Ti-6Al-4V specimens with integrated capillaries and compared to the reference specimenswithout capillaries. Specimens were produced by conventional subtractive manufacturing of wrought material and AM, using the laser based Directed Energy Deposition (DED) process. In this study, we investigated the effect of the presence of the capillary on the fatigue strength and fatigue initiation location. Finite element (FEM) simulations were performed to validate the experimental test results. The presence of a drilled capillary in the specimens did not alter the fatigue initiation location. However, the laser based DED production process introduced roughness on the capillary surface that altered the fatigue initiation location to the capillary surface. The fatigue performance was greatly reduced when considering a printed capillary. It is concluded that the surface quality of the integrated capillary is of primary importance in order not to influence the structural integrity of the component to be monitored.

36 MATERIALS SCIENCE↗

DOE OSTI2017

In Situ Characterization of the Initial Effect of Water on Molecular Interactions at the Interface of Organic/Inorganic Hybrid Systems

Probing initial interactions at the interface of hybrid systems under humid conditions has the potential to reveal the local chemical environment at solid/solid interfaces under real-world, technologically relevant conditions. Here in this paper, we show that ambient pressure X-ray photoelectron spectroscopy (APXPS) with a conventional X-ray source can be used to study the effects of water exposure on the interaction of a nanometer-thin polyacrylic acid (PAA) layer with a native aluminum oxide surface. The formation of a carboxylate ionic bond at the interface is characterized both with APXPS and in situ attenuated total reflectance Fourier transform infrared spectroscopy in the Kretschmann geometry (ATR-FTIR Kretschmann). When water is dosed in the APXPS chamber up to 5 Torr (~28% relative humidity), an increase in the amount of ionic bonds at the interface is observed. To confirm our APXPS interpretation, complementary ATR-FTIR Kretschmann experiments on a similar model system, which is exposed to an aqueous electrolyte, are conducted. These spectra demonstrate that water leads to an increased wet adhesion through increased ionic bond formation.

36 MATERIALS SCIENCE↗

DOE OSTI2016

Supported Silver Nanoparticle and Near-Interface Solution Dynamics in a Deep Eutectic Solvent

Type III deep eutectic solvents (DES) have attracted significant interest as both environmentally friendly and functional solvents that are, in some ways, advantageous to traditional aqueous systems. While these solvents continue to produce remarkable thin films and nanoparticle assemblies, their interactions with metallic surfaces are complex and difficult to manipulate. In this study, the near-surface region (2–600 nm) of a carbon surface is investigated immediately following silver nanoparticle nucleation and growth. This is accomplished, in situ, using a novel grazing transmission small-angle X-ray scattering approach with simultaneous voltammetry and electrochemical impedance spectroscopy. With this physical and electrochemical approach, the time evolution of three distinct surface interaction phenomena is observed: aggregation and coalescence of Ag nanoparticles, multilayer perturbations induced by nonaggregated Ag nanoparticles, and a stepwise transport of dissolved Ag species from the carbon surface. The multilayer perturbations contain charge-separated regions of positively charged choline-ethylene and negatively charged Ag and Cl species. Both aggregation-coalescence and the stepwise decrease in Ag precursor near the surface are observed to be very slow (~2 h) processes, as both ion and particle transport are significantly impeded in a DES as compared to aqueous electrolytes. Finally, altogether, this study shows how the unique chemistry of the DES changes near the surface and in the presence of nanoparticles that adsorb the constituent species.

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