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“Nanoporous Dealloyed Metal Materials Processing and Applications?A Review”. Scandura G, Kumari P, Palmisano G, Karanikolos GN, Orwa J, Dumee LF, Industrial and engineering chemistry research (2023). http://doi.org/10.1021/ACS.IECR.2C03952
Abstract: The development of porous metal materials with pore geometries and sizes at the nanoscale offers promising opportunities for the development of smart responsive interfaces for separation and catalytic applications and as building blocks for complex composite materials. Dealloying is an innovative technique based on selective removal of a sacrificial metal from a metal alloy to engineer surface textures and pores across significant thicknesses. Dealloyed structures may be processed over large scales and for a range of source alloys, offering unprecedented manufacturing opportunities. This review presents the operations and challenges of dealloying routes and discusses avenues for process optimizations and improvements, aiming at the development of scalable nanoporous materials. The potential of dealloyed materials for catalytic and sensing applications is expanded and benchmarked against reference materials. Future prospects and applications of dealloyed materials toward surface reactivity control and pore architecture development are highlighted.
Keywords: A1 Journal article; Sustainable Energy, Air and Water Technology (DuEL)
Impact Factor: 4.2
DOI: 10.1021/ACS.IECR.2C03952
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“A novel mechanistic modelling approach for microbial selection dynamics : towards improved design and control of raceway reactors for purple bacteria”. Alloul A, Moradvandi A, Puyol D, Molina R, Gardella G, Vlaeminck SE, De Schutter B, Abraham E, Lindeboom REF, Weissbrodt DG, Bioresource technology 390, 129844 (2023). http://doi.org/10.1016/J.BIORTECH.2023.129844
Abstract: Purple phototrophic bacteria (PPB) show an underexplored potential for resource recovery from wastewater. Raceway reactors offer a more affordable full-scale solution on wastewater and enable useful additional aerobic processes. Current mathematical models of PPB systems provide useful mechanistic insights, but do not represent the full metabolic versatility of PPB and thus require further advancement to simulate the process for technology development and control. In this study, a new modelling approach for PPB that integrates the photoheterotrophic, and both anaerobic and aerobic chemoheterotrophic metabolic pathways through an empirical parallel metabolic growth constant was proposed. It aimed the modelling of microbial selection dynamics in competition with aerobic and anaerobic microbial community under different operational scenarios. A sensitivity analysis was carried out to identify the most influential parameters within the model and calibrate them based on experimental data. Process perturbation scenarios were simulated, which showed a good performance of the model.
Keywords: A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL)
Impact Factor: 11.4
DOI: 10.1016/J.BIORTECH.2023.129844
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“Nucleation and growth of bipyramidal Yb:LiYF₄, nanocrystals : growing up in a hot environment”. Mulder JTT, Jenkinson K, Toso S, Prato M, Evers WHH, Bals S, Manna L, Houtepen AJJ, Chemistry of materials 35, 5311 (2023). http://doi.org/10.1021/ACS.CHEMMATER.3C00502
Abstract: Lanthanide-doped LiYF4 (Ln:YLF) is commonlyused fora broad variety of optical applications, such as lasing, photon upconversionand optical refrigeration. When synthesized as nanocrystals (NCs),this material is also of interest for biological applications andfundamental physical studies. Until now, it was unclear how Ln:YLFNCs grow from their ionic precursors into tetragonal NCs with a well-defined,bipyramidal shape and uniform dopant distribution. Here, we studythe nucleation and growth of ytterbium-doped LiYF4 (Yb:YLF),as a template for general Ln:YLF NC syntheses. We show that the formationof bipyramidal Yb:YLF NCs is a multistep process starting with theformation of amorphous Yb:YLF spheres. Over time, these spheres growvia Ostwald ripening and crystallize, resulting in bipyramidal Yb:YLFNCs. We further show that prolonged heating of the NCs results inthe degradation of the NCs, observed by the presence of large LiFcubes and small, irregular Yb:YLF NCs. Due to the similarity in chemicalnature of all lanthanide ions our work sheds light on the formationstages of Ln:YLF NCs in general.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 8.6
DOI: 10.1021/ACS.CHEMMATER.3C00502
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“Optimizing control strategies for urine nitrification : narrow pH control band enhances process stability and reduces nitrous oxide emissions”. Faust V, Boon N, Ganigué, R, Vlaeminck SE, Udert KM, Frontiers in environmental science 11, 1275152 (2023). http://doi.org/10.3389/FENVS.2023.1275152
Abstract: Nitrification is well-suited for urine stabilization. No base dosage is required if the pH is controlled within an appropriate operating range by urine feeding, producing an ammonium-nitrate fertilizer. However, the process is highly dependent on the selected pH set-points and is susceptible to process failures such as nitrite accumulation or the growth of acid-tolerant ammonia-oxidizing bacteria. To address the need for a robust and reliable process in decentralized applications, two different strategies were tested: operating a two-position pH controller (inflow on/off) with a narrow pH control band at 6.20/6.25 (∆pH = 0.05, narrow-pH) vs. a wider pH control band at 6.00/6.50 (∆pH = 0.50, wide-pH). These variations in pH also cause variations in the chemical speciation of ammonia and nitrite and, as shown, the microbial production of nitrite. It was hypothesized that the higher fluctuations would result in greater microbial diversity and, thus, a more robust process. The diversity of nitrifiers was higher in the wide-pH reactor, while the diversity of the entire microbiome was similar in both systems. However, the wide-pH reactor was more susceptible to tested process disturbances caused by increasing pH or temperature, decreasing dissolved oxygen, or an influent stop. In addition, with an emission factor of 0.47%, the nitrous oxide (N2O) emissions from the wide-pH reactor were twice as high as the N2O emissions from the narrow-pH reactor, most likely due to the nitrite fluctuations. Based on these results, a narrow control band is recommended for pH control in urine nitrification.
Keywords: A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL)
DOI: 10.3389/FENVS.2023.1275152
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“Partial hydrolysis of diphosphonate ester during the formation of hybrid Tio₂, nanoparticles : role of acid concentration”. Ramesha BM, Pawlak B, Arenas Esteban D, Reekmans G, Bals S, Marchal W, Carleer R, Adriaensens P, Meynen V, ChemPhysChem : a European journal of chemical physics and physical chemistry , e202300437 (2023). http://doi.org/10.1002/CPHC.202300437
Abstract: In the present work, a method was utilized to control the in‐situ partial hydrolysis of a diphosphonate ester in presence of a titania precursor and in function of acid content and its impact on the hybrid nanoparticles was assessed. The hydrolysis degree of organodiphosphonate ester linkers during the formation of hybrid organic‐inorganic metal oxide nanoparticles, are relatively underexplored . Quantitative solution NMR spectroscopy revealed that during the synthesis of TiO2 nanoparticles, an increase in acid concentration introduces a higher degree of partial hydrolysis of the TEPD linker into diverse acid/ester derivatives of TEPD. Increasing the HCl/Ti ratio from 1 to 3, resulted in an increase in degree of partial hydrolysis of the TEPD linker in solution from 4% to 18.8% under the here applied conditions. As a result of the difference in partial hydrolysis, the linker‐TiO2 bonding was altered. Upon subsequent drying of the colloidal TiO2 solution, different textures, at nanoscale and macroscopic scale, were obtained dependent on the HCl/Ti ratio and thus the degree of hydrolysis of TEPD. Understanding such linker‐TiO2 nanoparticle surface dynamics is crucial for making hybrid organic‐inorganic materials (i.e. (porous) metal phosphonates) employed in applications such as electronic/photonic devices, separation technology and heterogeneous catalysts.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT); Laboratory of adsorption and catalysis (LADCA)
Impact Factor: 2.9
DOI: 10.1002/CPHC.202300437
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“Phase object reconstruction for 4D-STEM using deep learning”. Friedrich T, Yu C-P, Verbeeck J, Van Aert S, Microscopy and microanalysis 29, 395 (2023). http://doi.org/10.1093/MICMIC/OZAC002
Abstract: In this study, we explore the possibility to use deep learning for the reconstruction of phase images from 4D scanning transmission electron microscopy (4D-STEM) data. The process can be divided into two main steps. First, the complex electron wave function is recovered for a convergent beam electron diffraction pattern (CBED) using a convolutional neural network (CNN). Subsequently, a corresponding patch of the phase object is recovered using the phase object approximation. Repeating this for each scan position in a 4D-STEM dataset and combining the patches by complex summation yields the full-phase object. Each patch is recovered from a kernel of 3x3 adjacent CBEDs only, which eliminates common, large memory requirements and enables live processing during an experiment. The machine learning pipeline, data generation, and the reconstruction algorithm are presented. We demonstrate that the CNN can retrieve phase information beyond the aperture angle, enabling super-resolution imaging. The image contrast formation is evaluated showing a dependence on the thickness and atomic column type. Columns containing light and heavy elements can be imaged simultaneously and are distinguishable. The combination of super-resolution, good noise robustness, and intuitive image contrast characteristics makes the approach unique among live imaging methods in 4D-STEM.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 2.8
Times cited: 1
DOI: 10.1093/MICMIC/OZAC002
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“Photo-responsive metal-organic frameworks –, design strategies and emerging applications in photocatalysis and adsorption”. Scandura G, Eid S, Alnajjar AA, Paul T, Karanikolos GN, Shetty D, Omer K, Alqerem R, Juma A, Wang H, Arafat HA, Dumee LF, Materials Advances 4, 1258 (2023). http://doi.org/10.1039/D2MA01022D
Abstract: Stimuli-responsive metal-organic frameworks (MOFs) are highly versatile porous materials with the ability to respond to different external stimuli, including temperature, pressure, pH, and light. The MOF properties can switch reversibly under specific light irradiation, opening the doors to various applications. This review focuses on design strategies to obtain photo-responsive MOFs, namely (i) encapsulation of photo-switchable molecules as guests in MOF porous structures, (ii) fabrication of MOF composites, (iii) post-synthesis modification, and (iv) synthesis of MOFs with photo-responsive ligands. The most recent reports from the literature are herein reviewed and analyzed in terms of material chemistry and performance. Comparisons between the different strategies are performed and future challenges are discussed. The critical aspect of the fatigue of photo-responsive MOFs applied for prolonged cycling of irradiation is also discussed.
Keywords: A1 Journal article; Sustainable Energy, Air and Water Technology (DuEL)
DOI: 10.1039/D2MA01022D
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“Photothermal heating of Au nanorods and nanospheres : temperature characteristics and strength of convective forces”. Borah R, Kumar A, Samantaray M, Desai A, Tseng F-G, Plasmonics 18, 1449 (2023). http://doi.org/10.1007/S11468-023-01855-4
Abstract: The nanoscale photothermal effect and the optofluidic convection around plasmonic nanoparticles drive the application of such nanoparticles in micro-environment. In this work, heat transfer and fluid flow around Au nanospheres and nanorods in water medium under continuous and pulsed wave laser irradiance was investigated using an FEM based numerical framework. Au nanospheres of a wide range of diameter: 40 nm = Diameter (D) = 180 nm and relatively large nanorods (diameter: 50 nm) with varying aspect ratio (1 = Aspect ratio (A) = 5) and orientation (0 degrees = ? = 90 degrees, ? = 0 degrees, 90 degrees) with respect to the incident EM radiation were investigated for continuous wave (CW) and pulsed wave laser. It was found that although nanorods can attain much higher temperature than nanospheres, orientation of a nanorod is an important factor to be carefully considered in applications. In micro-scale spherical and hemispherical confinements (diameter < 14.4 p.m), the convective velocity fields around nanoparticles is in the order of 10-9 m/s, with only a weak effect of the slip or no-slip boundary condition on the confining walls. Importantly, the size of the confinement has a strong effect leading to an order of magnitude stronger convection for 14.4 p.m (diameter) spherical confinement as compared to 3.6 p.m confinement. Additionally close proximity of the nanoparticles to the confining walls strongly reduces (by an order of magnitude) the convective currents. The results reported herein provides important insights for the use of photothermal nanoparticles in microscale confined space (e.g. cellular environment) for applications such as optical tweezers, photoporation, etc.
Keywords: A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL)
Impact Factor: 3
DOI: 10.1007/S11468-023-01855-4
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“Picometer-precision few-tilt ptychotomography of 2D materials”. Hofer C, Mustonen K, Skakalova V, Pennycook TJ, 2D materials 10, 035029 (2023). http://doi.org/10.1088/2053-1583/ACDD80
Abstract: From ripples to defects, edges and grain boundaries, the 3D atomic structure of 2D materials is critical to their properties. However the damage inflicted by conventional 3D analysis precludes its use with fragile 2D materials, particularly for the analysis of local defects. Here we dramatically increase the potential for precise local 3D atomic structure analysis of 2D materials, with both greatly improved dose efficiency and sensitivity to light elements. We demonstrate light atoms can now be located in complex 2D materials with picometer precision at doses 30 times lower than previously possible. Moreover we demonstrate this using WS2, in which the light atoms are practically invisible to conventional methods at low doses. The key advance is combining the concept of few tilt tomography with highly dose efficient ptychography in scanning transmission electron microscopy. We further demonstrate the method experimentally with the even more challenging and newly discovered 2D CuI, leveraging a new extremely high temporal resolution camera.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 5.5
DOI: 10.1088/2053-1583/ACDD80
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“Plant and microbial science and technology as cornerstones to Bioregenerative Life Support Systems in space”. De Micco V, Amitrano C, Mastroleo F, Aronne G, Battistelli A, Carnero-Diaz E, De Pascale S, Detrell G, Dussap C-G, Ganigué, R, Jakobsen ØM, Poulet L, Van Houdt R, Verseux C, Vlaeminck SE, Willaert R, Leys N, NPJ microgravity 9, 69 (2023). http://doi.org/10.1038/S41526-023-00317-9
Abstract: Long-term human space exploration missions require environmental control and closed Life Support Systems (LSS) capable of producing and recycling resources, thus fulfilling all the essential metabolic needs for human survival in harsh space environments, both during travel and on orbital/planetary stations. This will become increasingly necessary as missions reach farther away from Earth, thereby limiting the technical and economic feasibility of resupplying resources from Earth. Further incorporation of biological elements into state-of-the-art (mostly abiotic) LSS, leading to bioregenerative LSS (BLSS), is needed for additional resource recovery, food production, and waste treatment solutions, and to enable more self-sustainable missions to the Moon and Mars. There is a whole suite of functions crucial to sustain human presence in Low Earth Orbit (LEO) and successful settlement on Moon or Mars such as environmental control, air regeneration, waste management, water supply, food production, cabin/habitat pressurization, radiation protection, energy supply, and means for transportation, communication, and recreation. In this paper, we focus on air, water and food production, and waste management, and address some aspects of radiation protection and recreation. We briefly discuss existing knowledge, highlight open gaps, and propose possible future experiments in the short-, medium-, and long-term to achieve the targets of crewed space exploration also leading to possible benefits on Earth.
Keywords: A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL)
DOI: 10.1038/S41526-023-00317-9
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“Plasma-catalytic ammonia synthesis : packed catalysts act as plasma modifiers”. Ndayirinde C, Gorbanev Y, Ciocarlan R-G, De Meyer R, Smets A, Vlasov E, Bals S, Cool P, Bogaerts A, Catalysis today 419, 114156 (2023). http://doi.org/10.1016/J.CATTOD.2023.114156
Abstract: We studied the plasma-catalytic production of NH3 from H2 and N2 in a dielectric barrier discharge plasma reactor using five different Co-based catalysts supported on Al2O3, namely Co/Al2O3, CoCe/Al2O3, CoLa/Al2O3, CoCeLa/Al2O3 and CoCeMg/Al2O3. The catalysts were characterized via several techniques, including SEM-EDX, and their performance was compared. The best performing catalyst was found to be CoLa/Al2O3, but the dif-ferences in NH3 concentration, energy consumption and production rate between the different catalysts were limited under the same conditions (i.e. feed gas, flow rate and ratio, and applied power). At the same time, the plasma properties, such as the plasma power and current profile, varied significantly depending on the catalyst. Taken together, these findings suggest that in the production of NH3 by plasma catalysis, our catalysts act as plasma modifiers, i.e., they change the discharge properties and hence the gas phase plasma chemistry. Importantly, this effect dominates over the direct catalytic effect (as e.g. in thermal catalysis) defined by the chemistry on the catalyst surface.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT); Laboratory of adsorption and catalysis (LADCA); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 5.3
Times cited: 3
DOI: 10.1016/J.CATTOD.2023.114156
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“Probing confined vortices with a superconducting nanobridge”. Foltyn M, Norowski K, Wyszynski MJ, De Arruda AS, Milošević, MV, Zgirski M, Physical review applied 19, 044073 (2023). http://doi.org/10.1103/PHYSREVAPPLIED.19.044073
Abstract: We realize a superconducting nanodevice in which vortex traps in the form of an aluminum square are integrated with a Dayem nanobridge. We perform field cooling of the traps arriving to different vortex configurations, dependent on the applied magnetic field, to demonstrate that the switching current of the bridge is highly sensitive to the presence and location of vortices in the trap. Our measurements exhibit unprecedented precision and ability to detect the first and successive vortex entries into all fabricated traps, from few hundred nm to 2 mu m in size. The experimental results are corroborated by Ginzburg-Landau simulations, which reveal the subtle yet crucial changes in the density of the superconducting condensate in the vicinity of the bridge with every additional vortex entry and relocation inside the trap. An ease of integration and simplicity make our design a convenient platform for studying dynamics of vortices in strongly confining geometries, involving a promise to manipulate vortex states electronically with simultaneous in situ control and monitoring.
Keywords: A1 Journal article; Condensed Matter Theory (CMT)
Impact Factor: 4.6
DOI: 10.1103/PHYSREVAPPLIED.19.044073
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Friedrich T (2023) Quantifying atomic structures using neural networks from 4D scanning transmission electron microscopy (STEM) datasets. 127 p
Abstract: Nanoscience and nanotechnologies are of immense importance across many fields of science and for numerous practical applications. In this context, scanning transmission electron microscopy (STEM) and 4D-STEM are among the most powerful characterization methods at the atomic scale. Annular dark-field (ADF)-STEM can be used to quantify atomic structures in 3D by counting atoms based on a single projection image. In 4D-STEM a full diffraction pattern is recorded at each scan step, which enables more dose efficient imaging and the utilization of various advanced imaging modalities, which can however be complex and slow. Both, STEM and 4D-STEM suffer from noise and distortions. In the first section of this work the most important of these distortions are discussed and it is shown how image restoration with a dedicated convolutional neural network (CNN) can be beneficial for atomic structure quantifications in ADF-STEM. In the second part, a new 4D-STEM imaging method real-time-integrated-centre-of-mass (riCOM) is introduced, which is a very dose-efficient and fast algorithm that enables unprecedented live-imaging capabilities for 4D-STEM. It is based on the integrated centre-of-mass approach, but is reformulated with variable integration ranges and optional filters, which allows for a tunable contrast transfer function. This enables the imaging of light and heavy elements simultaneously at very low doses. In the third part another new 4D-STEM method, coined AIRPI (AI-assisted rapid phase imaging) is introduced, which uses a CNN to retrieve a patch of the specimen's phase image for each scan position, based on the diffraction patterns in the probe's immediate surroundings. This allows also live imaging in principle and surpasses comparable state-of-the-art algorithms in terms of resolution also at low doses. Different atomic columns can be reliably distinguished over a wide range of atomic numbers, enabling a very good image interpretability. Further, AIRPI can recover low frequency image components, which preserves thickness information. This is a unique and important feature which could make quantitative 4D-STEM feasible.
Keywords: Doctoral thesis; Electron microscopy for materials research (EMAT)
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“Restructuring of titanium oxide overlayers over nickel nanoparticles during catalysis”. Monai M, Jenkinson K, Melcherts AEM, Louwen JN, Irmak EA, Van Aert S, Altantzis T, Vogt C, van der Stam W, Duchon T, Smid B, Groeneveld E, Berben P, Bals S, Weckhuysen BM, Science 380, 644 (2023). http://doi.org/10.1126/SCIENCE.ADF6984
Abstract: Reducible supports can affect the performance of metal catalysts by the formation of suboxide overlayers upon reduction, a process referred to as the strong metal-support interaction (SMSI). A combination of operando electron microscopy and vibrational spectroscopy revealed that thin TiOx overlayers formed on nickel/titanium dioxide catalysts during 400 degrees C reduction were completely removed under carbon dioxide hydrogenation conditions. Conversely, after 600 degrees C reduction, exposure to carbon dioxide hydrogenation reaction conditions led to only partial reexposure of nickel, forming interfacial sites in contact with TiOx and favoring carbon-carbon coupling by providing a carbon species reservoir. Our findings challenge the conventional understanding of SMSIs and call for more-detailed operando investigations of nanocatalysts at the single-particle level to revisit static models of structure-activity relationships.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT)
Impact Factor: 56.9
Times cited: 29
DOI: 10.1126/SCIENCE.ADF6984
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Zhang K (2023) Revealing the correlation between titania support properties and propylphosphonic acid modification by in-depth characterization. XVI, 262 p
Abstract: Grafting organophosphonic acids modification (PAs) on metal oxides has shown to be a flexible technology to tune the surface properties of metal oxides for various applications. Nevertheless, there are still puzzles that need to be addressed, such as the correlations between metal oxides properties (types of surface reactive sites) and the modification (modification degree), the correlations between metal oxides properties and the properties of modified surfaces. Moreover, the currently used liquid-phase method for the grafting has associated impeding effects of solvent on tailoring the modification degrees, and also causes the formation of metal phosphonate side products. The solid-phase method can induce the unwanted changes in crystal phase of supports. Based on these questions, the three titania supports with divergent surface properties were selected as the metal oxides supports investigated, propylphosphonic acid (3PA) modification was carried out under the same synthesis conditions: four different concentrations, two solvents (water or toluene), and one reaction time (4 h) and temperature (90 ). MeOH chemisorption was introduced to probe the surface (un)reactive sites for 3PA modification. On the other hand, MeOH chemisorption and inverse gas chromatography (IGC) were combined to characterize the changes in surface polarity and acidic properties induced by the modification. Next, a solid-phase method, manual grinding, was proposed to graft 3PA on titania, avoiding the impeding effects of solvent on improving modification degree and the formation of the titania phosphonate side products, as well as preserving the crystal phase. The results indicate that methanol chemisorption can qualitatively analyze the surface active sites that are consumed by 3PA modification, its chemisorption capacity shows the consistent trend with the maximum modification degree, hereby revealing the kinds of interactions that are important in controlling surface coverage. Titania supports is found to play an important role in changes in surface polarity and acidic properties by charactering the three modified titania samples at a similar modification degree using the methanol chemisorption coupled with in-situ infrared and thermogravimetric-mass spectrometer, and the IGC. Moreover, IGC provides additional information about the changes in binding modes. Furthermore, grafting 3PA modification on titania was achieved by manual grinding. Compared to the liquid-phase method, the maximum modification degree obtained by the manual grinding is 25 % higher while using 83.3 % or 75.0% lower amounts of expensive 3PA and limiting the formation of titania phosphonate side products. Compared to the reactive milling method, the proposed manual grinding method preserves the crystal phase(s) of titania.
Keywords: Doctoral thesis; Laboratory of adsorption and catalysis (LADCA)
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“Roadmap on structured waves”. Bliokh KY, Karimi E, Padgett MJ, Alonso MA, Dennis MR, Dudley A, Forbes A, Zahedpour S, Hancock SW, Milchberg HM, Rotter S, Nori F, Ozdemir SK, Bender N, Cao H, Corkum PB, Hernandez-Garcia C, Ren H, Kivshar Y, Silveirinha MG, Engheta N, Rauschenbeutel A, Schneeweiss P, Volz J, Leykam D, Smirnova DA, Rong K, Wang B, Hasman E, Picardi MF, Zayats AV, Rodriguez-Fortuno FJ, Yang C, Ren J, Khanikaev AB, Alu A, Brasselet E, Shats M, Verbeeck J, Schattschneider P, Sarenac D, Cory DG, Pushin DA, Birk M, Gorlach A, Kaminer I, Cardano F, Marrucci L, Krenn M, Marquardt F, Journal of optics 25, 103001 (2023). http://doi.org/10.1088/2040-8986/ACEA92
Abstract: Structured waves are ubiquitous for all areas of wave physics, both classical and quantum, where the wavefields are inhomogeneous and cannot be approximated by a single plane wave. Even the interference of two plane waves, or of a single inhomogeneous (evanescent) wave, provides a number of nontrivial phenomena and additional functionalities as compared to a single plane wave. Complex wavefields with inhomogeneities in the amplitude, phase, and polarization, including topological----- structures and singularities, underpin modern nanooptics and photonics, yet they are equally important, e.g. for quantum matter waves, acoustics, water waves, etc. Structured waves are crucial in optical and electron microscopy, wave propagation and scattering, imaging, communications, quantum optics, topological and non-Hermitian wave systems, quantum condensed-matter systems, optomechanics, plasmonics and metamaterials, optical and acoustic manipulation, and so forth. This Roadmap is written collectively by prominent researchers and aims to survey the role of structured waves in various areas of wave physics. Providing background, current research, and anticipating future developments, it will be of interest to a wide cross-disciplinary audience.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 2.1
Times cited: 7
DOI: 10.1088/2040-8986/ACEA92
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Derks K (2023) Scanning Michael Sweerts and Michaelina Wautier : uncovering the working methods of 17th-century Brussels artists by means of MA-XRF examination. 634 p
Abstract: This dissertation focuses on the materials and techniques used by the Brussels artists Michael Sweerts (1618-1664) and Michaelina Wautier (1614-1689). It tries to answer the following research questions: 1.Did 17th-century Brussels-based artists use idiosyncratic painting materials and techniques, and can their work be distinguished from paintings created in other artistic centers based on these materials and techniques? 2.How did Sweerts and Wautier influence each other’s work? In order to answer the research questions, a selection of relevant and representative paintings from Sweerts’ and Wautier’s oeuvre has been studied with MA-XRF scanning and microscopic examination. The results are discussed in volume 2 of this dissertation, and form the basis upon which the chapters in volume 1 are built. MA-XRF scanning is a non-destructive imaging technique based on the technique of X-ray fluorescence (XRF). The technique allows for the collection of elemental information about the materials present in a work of art. The work presented in this dissertation has shed more light on the working methods of Sweerts and Wautier. It has shown they both showed an openness and willingness to continue learning and developing as an artist. Wautier did not feel constrained to work only in one genre and apparently carried on developing her skills throughout her career, as evidenced by Flower Garland with Butterfly. She might have trained with a specialized artist to master their idiosyncratic working methods and this diverse genre. This suggests that Wautier had an interest in art education. Sweerts too had a passion for art education: he was involved in the drawing academy of Camillo Pamphilj in Rome, and later established his own academy for life drawing in Brussels. Sweerts’ work clearly shows the influence of his Italian contemporaries. Whilst living in Rome, he adapted his working methods to local customs such as working on brightly colored grounds. Wautier’s oeuvre shows that she was open to explore different genres and that she took inspiration from her contemporaries, including Theodoor van Loon and Daniël Seghers. In doing so, she furthered the development of different genres as she added original elements to her compositions. It is the conclusion of this dissertation that Michaelina Wautier can thus be considered one of the innovative artists of mid-17th-century Flemish painting, who inspired other artists in the Low Countries, including Michael Sweerts.
Keywords: Doctoral thesis; Art; Antwerp Cultural Heritage Sciences (ARCHES); Antwerp X-ray Imaging and Spectroscopy (AXIS)
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“Simon Stevin as a central figure in the development of abstract algebra and generic programming”. Gielis J, Symmetry : culture and science 34, 155 (2023). http://doi.org/10.26830/SYMMETRY_2023_2_155
Abstract: Simon Stevin (1548-1620) is mainly known for the decimal system and his Clootkrans proof. His influence is also profound in infinitesimal calculus, mechanics, and even in abstract algebra and today’s conception of polynomials, algorithms, and generic programming. Here we review his influence as assessed in generic programming. According to Dr. Stepanov, one of the most influential researchers in generic programming, Stevin’s work on polynomials can be regarded as the essence of generic programming: an algorithm from one domain can be applied in another similar domain.
Keywords: A1 Journal article; Sustainable Energy, Air and Water Technology (DuEL)
DOI: 10.26830/SYMMETRY_2023_2_155
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“Solvothermal synthesis of mesoporous TiO2 with tunable surface area, crystal size and surface hydroxylation for efficient photocatalytic acetaldehyde degradation”. Zhang K, Wang J, Ninakanti R, Verbruggen SW, Chemical engineering journal 474, 145188 (2023). http://doi.org/10.1016/J.CEJ.2023.145188
Abstract: Photocatalytic acetaldehyde degradation exhibits satisfactory performance only at relatively low acetaldehyde flow rates, predominately below 10 × 10-3 mL/min, leaving ample room for improvement. Therefore, it is necessary to prepare more efficient photocatalysts for acetaldehyde degradation. Moreover, the impact of the interaction strength between the titania surface and surface water on the photocatalytic acetaldehyde efficiency is poorly understood. To address these issues, in this work a series of (0 0 1)-faceted anatase titania samples with various surface properties and structures were synthesized via a solvothermal method and tested at high acetaldehyde flow rates under UV light irradiation. With increasing solvothermal time, the pore volume, surface area, and the abundance of surface OH groups all increased, while the crystallite size decreased. These were all identified to be beneficial to promote the degradation performance. When the solvothermal temperature was 180 ℃ and the reaction time was 5 h, the prepared sample displayed the most efficient performance at 19.25× 10-3 mL/min of acetaldehyde (conversion of (74 ± 1)% versus (29 ± 1)% for P25), and achieved a 100 % conversion at 16 × 10-3 mL/min. A weaker interaction strength between surface water and the titania surface was found to improve the acetaldehyde adsorption capacity, thereby promoting the acetaldehyde degradation efficiency. The stability of the best performing sample was tested over 48 h, demonstrating a highly stable performance with no signs of deactivation. Even at a relative humidity of 30 %, the acetaldehyde conversion retains 82% of its efficiency in a dry atmosphere, highlighting its potential in practical applications.
Keywords: A1 Journal article; Engineering sciences. Technology; Laboratory of adsorption and catalysis (LADCA)
Impact Factor: 15.1
DOI: 10.1016/J.CEJ.2023.145188
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“Spontaneous skyrmion conformal lattice and transverse motion during dc and ac compression”. Bellizotti Souza JC, Vizarim NP, Reichhardt CJO, Reichhardt C, Venegas PA, New journal of physics 25, 053020 (2023). http://doi.org/10.1088/1367-2630/ACD46F
Abstract: We use atomistic-based simulations to investigate the behavior of ferromagnetic skyrmions being continuously compressed against a rigid wall under dc and ac drives. The compressed skyrmions can be annihilated close to the wall and form a conformal crystal with both a size and a density gradient, making it distinct from conformal crystals observed previously for superconducting vortices and colloidal particles. For both dc and ac driving, the skyrmions can move transverse to the compression direction due to a combination of density and size gradients. Forces in the compression direction are converted by the Magnus force into transverse motion. Under ac driving, the amount of skyrmion annihilation is reduced and we find a skyrmion Magnus ratchet pump. We also observe shear banding in which skyrmions near the wall move up to twice as fast as skyrmions further from the wall. When we vary the magnitude of the applied drive, we find a critical current above which the skyrmions are completely annihilated during a time scale that depends on the magnitude of the drive. By varying the magnetic parameters, we find that the transverse motion is strongly dependent on the skyrmion size. Smaller skyrmions are more rigid, which interferes with the size gradient and destroys the transverse motion. We also confirm the role of the size gradient by comparing our atomistic simulations with a particle-based model, where we find that the transverse motion is only transient. Our results are relevant for applications where skyrmions encounter repulsive magnetic walls, domain walls, or interfaces.
Keywords: A1 Journal article; Condensed Matter Theory (CMT)
Impact Factor: 3.3
DOI: 10.1088/1367-2630/ACD46F
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“Stomatal shape described by a superellipse in four Magnoliaceae species”. Li Q, Niklas KJJ, Niinemets U, Zhang L, Yu K, Gielis J, Gao J, Shi P, Botany letters , 1 (2023). http://doi.org/10.1080/23818107.2023.2234443
Abstract: Stomata are essential for the exchange of water vapour and atmospheric gases between vascular plants and their external environments. The stomatal geometries of many plants appear to be elliptical. However, prior studies have not tested whether this is a mathematical reality, particularly since many natural shapes that appear to be ellipses are superellipses with greater or smaller edge curvature than predicted for an ellipse. Compared with the ellipse equation, the superellipse equation includes an additional parameter that allows generation of a larger range of shapes. We randomly selected 240 stomata from each of four Magnoliaceae species to test whether the stomatal geometries are superellipses or ellipses. The stomatal geometries for most stomata (943/960) were found to be described better using the superellipse equation. The traditional “elliptical stomata hypothesis” resulted in an underestimation of the area of stomata, whereas the superellipse equation accurately predicted stomatal area. This finding has important implications for the estimation of stomatal area in studies looking at stomatal shape, geometry, and function.
Keywords: A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL)
Impact Factor: 1.5
DOI: 10.1080/23818107.2023.2234443
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“Superconductivity in functionalized niobium-carbide MXenes”. Sevik C, Bekaert J, Milošević, MV, Nanoscale 15, 8792 (2023). http://doi.org/10.1039/D3NR00347G
Abstract: We detail the effects of Cl and S functionalization on the superconducting properties of layered (bulk) and monolayer niobium carbide (Nb2C) MXene crystals, based on first-principles calculations combined with Eliashberg theory. For bulk layered Nb2CCl2, the calculated superconducting transition temperature (T-c) is in very good agreement with the recently measured value of 6 K. We show that T-c is enhanced to 10 K for monolayer Nb2CCl2, due to an increase in the density of states at the Fermi level, and the corresponding electron-phonon coupling. We further demonstrate feasible gate- and strain-induced enhancements of T-c for both bulk-layered and monolayer Nb2CCl2 crystals, resulting in T-c values of around 38 K. In the S-functionalized Nb2CCl2 crystals, our calculations reveal the importance of phonon softening in understanding their superconducting properties. Finally, we predict that Nb3C2S2 in bulk-layered and monolayer forms is also superconducting, with a T-c of around 28 K. Considering that Nb2C is not superconducting in pristine form, our findings promote functionalization as a pathway towards robust superconductivity in MXenes.
Keywords: A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT)
Impact Factor: 6.7
DOI: 10.1039/D3NR00347G
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“Suppressing hydrogen blistering in a magnesium-rich healable laser powder bed fusion aluminum alloy analyzed by in-situ high resolution techniques”. Gheysen J, Kashiwar A, Idrissi H, Villanova J, Simar A, Materials &, design 231, 112024 (2023). http://doi.org/10.1016/J.MATDES.2023.112024
Abstract: Hydrogen blistering, i.e. precipitation of supersaturated hydrogen at elevated temperatures, increases porosity during heat treatments in 4xxx series Al alloys manufactured by laser powder bed fusion (LPBF), as demonstrated by 3D X-ray nano-imaging in AlSi12. This paper proposes the design of a healable Al alloy to suppress hydrogen blistering and improve the damage management. The strategy consists of solute atoms diffusing towards nano-voids and precipitating on their surface, thereby filling the damage sites. A new healable Al alloy was thus developed and successfully manufactured by LPBF. 3D X-ray nano-imaging evidenced that the addition of Mg in 4xxx series Al alloys suppresses the hydrogen blistering. This is expectedly due to Mg in solid solution which increases the hydrogen solubility in the Al matrix and due to the healing of these hydrogen pores. Moreover, a significant healing of voids smaller than 500 nm diameter is observed. In-situ heating inside transmission electron microscopy pointed out that Al matrix diffuses inside the fractured Mg2Si particles, thereby demonstrating the healing ability of the new alloy. This has opened the doors to development of new healable Al alloys manufactured by LPBF as well as to new post-treatments to tailor mechanical properties and microstructure without hydrogen blistering.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 8.4
DOI: 10.1016/J.MATDES.2023.112024
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“Surfactant layers on gold nanorods”. Mosquera J, Wang D, Bals S, Liz-Marzan LM, Accounts of chemical research 56, 1204 (2023). http://doi.org/10.1021/ACS.ACCOUNTS.3C00101
Abstract: Gold nanorods (Au NRs) are an exceptionally promising tool in nanotechnology due to three key factors: (i) their strong interaction with electromagnetic radiation, stemming from their plasmonic nature, (ii) the ease with which the resonance frequency of their longitudinal plasmon mode can be tuned from the visible to the near-infrared region of the electromagnetic spect r u m based on their aspect ratio, and (iii) their simple and cost-effective preparation through seed-mediated chemical growth. In this synthetic method, surfactants play a critical role in controlling the size, shape, and colloidal stabi l i t y of Au NRs. For example, surfactants can stabilize specific crystallographic facets during the formation of Au NRs, leading to t h e formation of NRs with specific morphologies. The process of surfactant adsorption onto the NR surface may result in various assemblies of surfactant molecules, such as spherical micelles, elongated micelles, or bilayers. Again, the assembly mode is critical toward determining the further availabi l i t y of the Au NR surface to the surrounding medium. Despite its importance and a great deal of research effort, the interaction between Au NPs and surfactants remains insufficiently understood, because the assembly process is influenced by numerous factors, including the chemical nature of the surfactant, the surface morphology of Au NPs, and solution parameters. Therefore, gaining a more comprehensive understanding of these interactions is essential to unlock the full potential of the seed-mediated growth method and the applications of plasmonic NPs. A plethora of characterization techniques have been applied to reach such an understanding , but many open questions remain. In this Account, we review the current knowledge on the interactions between surfactants and Au NRs. We briefly introduce the state-of-the-art methods for synthesizing Au NRs and highlight the crucial role of cationic surfactants during this process. The self-assembly and organization of surfactants on the Au NR surface is then discussed to better understand their role in seed-mediated growth. Subsequently, we provide examples and elucidate how chemical additives can be used to modulate micellar assemblies, in turn allowing for a finer control over the growth of Au NRs, including chiral NRs. Next, we review the main experimental characterization and computational modeling techniques that have been applied to shed light on the arrangement of surfactants on Au NRs and summarize the advantages and disadvantages for each technique. The Account ends with a “Conclusions and Outlook” section, outlining promising future research directions and developments that we consider are sti l l required, mostly related to the application of electron microscopy in liquid and in 3D. Finally, we remark on the potential of exploiting machine learning techniques to predict synthetic routes for NPs with predefined structures and properties.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 18.3
Times cited: 8
DOI: 10.1021/ACS.ACCOUNTS.3C00101
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“Synthesis and characterization of a highly electroactive composite based on Au nanoparticles supported on nanoporous activated carbon for electrocatalysis”. Moggia G, Hoekx S, Daems N, Bals S, Breugelmans T, ChemElectroChem , 1 (2023). http://doi.org/10.1002/CELC.202300293
Abstract: A facile, “one-pot”, chemical approach to synthesize gold-based nanoparticles finely dispersed on porous activated carbon (Norit) was demonstrated in this work. The pH of the synthesis bath played a critical role in determining the optimal gold-carbon interaction, which enabled a successful deposition of the gold nanoparticles onto the carbon matrix with a maximized metal utilization of 93 %. The obtained AuNP/C nanocomposite was characterized using SEM, HAADF-STEM electron tomography and electrochemical techniques. It was found that the Au nanoparticles, with diameters between 5 and 20 nm, were evenly distributed over the carbon matrix, both inside and outside the pores. Electrochemical characterization indicated that the composite had a very large electroactive surface area (EASA), as high as 282.4 m2 gAu-1. By exploiting its very high EASA, the catalyst was intended to boost the productivity of glucaric acid in the electrooxidation of its precursor, gluconic acid. However, cyclic voltammetry experiments revealed a very limited reactivity towards gluconic acid oxidation, due to the spacial hindrance of gluconic acid molecule which prevented diffusion inside the catalyst nanopores. On the other hand, the as-synthesized nanocomposite promises to be effective towards the ORR, and might thus find potential application as anode catalyst for fuel cells as well as for the scalability of all those electrochemical reactions involving small molecules with high diffusivity and catalysed by noble metals (i. e. CO2, CH4, N2, etc..). Electrocatalysis: Gold nanoparticles with diameter between 5 and 20 nm evenly distributed onto porous activated carbon (Norit) were obtained using a facile “one-pot” chemical synthesis technique with very high metal utilization. The AuNP/C nanocomposite was characterized using SEM, HAADF-STEM electron tomography and electrochemical techniques, revealing a very large electroactive surface area (EASA). The figure shows the HAADF-STEM image (a) and the respective EDX elemental distribution (b) for the AuNP/C composite with 9.3 % Au-loading developed in this work (Au is marked in red and C in green).image
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT)
Impact Factor: 4
Times cited: 1
DOI: 10.1002/CELC.202300293
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Hasnat Rubel A (2023) Theoretical characterization and optimization of nano-engineered superconducting scanning probe tip. viii, 145 p
Abstract: Using state-of-the-art simulation methods, we optimized the performance of nanoscale superconducting scanning probe tips for advanced spatial imaging of magnetic fields. The systematic studies of the tips’ static properties as a function of the tilted magnetic field, geometric parameters, and material parameters were carried out. The sensitivity of different superconducting quantum interference devices (SQUIDs) to the magnetic field emanating from the magnetic nanoparticle, where the location of a magnetic nanoparticle is considered below the primary loop's center, was examined as a function of the primary and secondary loop dimensions. The main objective of the research was to characterize and optimize the performance of a nano-sized SQUID-on-tip (SOT) device. Optimal SOT sensitivity was sought, for different loop sizes, arm linewidth, and lead dimensions. Moreover, we revealed that a constriction in the loop arms of the SOT can substantially improve the sensitivity of the device. Finally, the properties of the theta-SOT device were examined in the presence of in-plane and out-of-plane magnetic field components, enabling nanoscale imaging of 3D distributions of the magnetic field. Altogether, the obtained results deliver an engineering solution for the optimum performance of the SOT device in desired conditions.
Keywords: Doctoral thesis; Engineering sciences. Technology; Condensed Matter Theory (CMT)
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“Thermoelectric properties and scattering mechanisms in natural PbS”. Zuniga-Puelles E, Levytskyi V, Özden A, Guerel T, Bulut N, Himcinschi C, Sevik C, Kortus J, Gumeniuk R, Physical review B 107, 195203 (2023). http://doi.org/10.1103/PHYSREVB.107.195203
Abstract: X-ray diffraction and energy dispersive x-ray spectroscopic analyses showed a natural galena (PbS) crystal from Freiberg in Saxony (Germany) to be a single phase specimen [rock salt (NaCl) structure type, space group Fm3m, a = 5.932(1) angstrom] with stoichiometric composition and an enhanced dislocation density (8 approximate to 1011 cm-2). The latter parameter leads to an increase of the electrical resistivity in the high-temperature regime, as well as to the appearance of phonon resonance with a characteristic frequency coPR = 3.8(1) THz. Being in the same range (i.e., 3-5.5 THz) with the sulfur optical modes of highest group velocities, it results in a drastic reduction (by similar to 75%) of thermal conductivity (K) at lower temperatures (i.e., < 100 K), as well as in the appearance of a characteristic minimum in K at T approximate to 30 K. Furthermore, the studied galena is characterized by phonon-drag behavior and by temperature dependent switch of the charge carrier scattering mechanism regime (i.e., scattering on dislocations for T < 100 K, on acoustic phonons for 100 K < T < 170 K and on both acoustic and optical phonons for 170 K < T < 300 K). The combined theoretical calculation and optical spectroscopic study confirm this mineral to be a direct gap degenerate semiconductor. The possible origins of the second-order Raman spectrum are discussed.
Keywords: A1 Journal article; Condensed Matter Theory (CMT)
Impact Factor: 3.7
DOI: 10.1103/PHYSREVB.107.195203
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“Total electron yield (TEY) detection mode Cr K-edge XANES spectroscopy as a direct method to probe the composition of the surface of darkened chrome yellow (PbCr1-xSxO4) and potassium chromate paints”. Monico L, d'Acapito F, Cotte M, Janssens K, Romani A, Ricci G, Miliani C, Cartechini L, Nuclear instruments and methods in physics research: B: beam interactions with materials and atoms 539, 141 (2023). http://doi.org/10.1016/J.NIMB.2023.03.040
Abstract: The darkening of chromate-pigments, including chrome yellows (PbCr1-xSxO4), is a surface phenomenon affecting late 19th-early 20th c. paintings, such as those by Van Gogh. Exploring analytical strategies that contribute to a deep understanding of darkening is therefore significant for the long-term conservation of unique masterpieces. Here, we examined the capabilities of Cr K-edge XANES spectroscopy collected at the same time in X-ray fluorescence yield (XFY) and total electron yield (TEY) detection modes to selectively study the surface composition of darkened oil paint mock-ups composed of chrome yellow (PbCr0.2S0.8O4) or potassium chromate. By discussing advantages and drawbacks in using XFY/TEY modes in relation to XFY & mu;-XANES analysis from sectioned samples, we aim at assessing if TEY-XANES spectroscopy: (i) is a selective surface method to determine the abundance of different Cr-species from paint fragments; (ii) can contribute to optimize the analytical strategy by limiting time consuming sample preparation procedures; (iii) can decrease the probability of radiation damage.
Keywords: A1 Journal article; Engineering sciences. Technology; Antwerp X-ray Imaging and Spectroscopy (AXIS)
Impact Factor: 1.3
DOI: 10.1016/J.NIMB.2023.03.040
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“Towards a novel strategy for soot removal from water-soluble materials : the synergetic effect of hydrogels and cyclomethicone on gelatine emulsion-based photographs”. Ortega Saez N, Arno R, Marchetti A, Cauberghs S, Janssens K, Van der Snickt G, Al-Emam E, Heritage science 11, 78 (2023). http://doi.org/10.1186/S40494-023-00916-5
Abstract: Gels are a popular cleaning method for paper conservators and a lot of research has been done concerning gel cleaning of paper objects over the last 15 years. Despite the close interconnection between the conservation fields of paper and photographic material, research on using gels for cleaning photographs is very scarce. However, gels can provide an excellent cleaning method for photographic material. Cleaning silver gelatine prints with aqueous solvents is very complex due to the hydrophilic properties and fragility of the gelatine layer which makes mechanical cleaning difficult. The properties of gels ensure better control over the flow and evaporation of the solvent, facilitating the cleaning process. This study is the first insight into the viability of using gellan gum gel and polyvinyl acetate-borax (PVAc-borax) gel to clean contaminants from the surface of silver gelatine photographs. It is based on self-made samples that were artificially aged and contaminated with soot. Water, ethanol (EtOH), and Kodak Photo-flo were studied as solvents to remove the soot from the silver gelatine-based prints. These solvents were loaded into the aforementioned gels and applied to the samples in two different methods. These gel cleaning methods were subsequently compared with traditional cleaning methods. In addition, the usage of cyclomethicone D4 as a protective mask for the gelatine layer was studied. Measuring methods used to evaluate the cleaning were visual comparison, microscopic observation, and densitometry. ATR-FTIR measurements were also conducted to investigate potential side-effects of the cleaning methods on the prints, such as unwanted chemical transformations or the presence of gel residues after the treatments. Most of the gel cleaning methods within this study proved to be inadequate, with the exception of the gellan gum gel loaded with 30% EtOH. It was used as a granulated gel applied mechanically on a print saturated with cyclomethicone (octamethylcyclotetrasiloxane D4). Cyclomethicone proved to be a very effective protective barrier for the water-sensitive gelatine layer with minimal reduction in cleaning effectiveness.
Keywords: A1 Journal article; Engineering sciences. Technology; Art; Antwerp Cultural Heritage Sciences (ARCHES); Antwerp X-ray Imaging and Spectroscopy (AXIS)
Impact Factor: 2.5
DOI: 10.1186/S40494-023-00916-5
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“Transdermal on-demand drug delivery based on an iontophoretic hollow microneedle array system”. Detamornrat U, Parrilla M, Domínguez-Robles J, Anjani QK, Larrañeta E, De Wael K, Donnelly RF, Lab on a chip 23, 2304 (2023). http://doi.org/10.1039/D3LC00160A
Abstract: Transdermal drug delivery has emerged as an alternative administration route for therapeutic drugs, overcoming current issues in oral and parenteral administration. However, this technology is hindered by the low permeability of the stratum corneum of the skin. In this work, we develop a synergic combination of two enhancing technologies to contribute to an improved and on-demand drug delivery through an iontophoretic system coupled with hollow microneedles (HMNs). For the first time, a polymeric HMN array coupled with integrated iontophoresis for the delivery of charged molecules and macromolecules (e.g. proteins) is devised. To prove the concept, methylene blue, fluorescein sodium, lidocaine hydrochloride, and bovine serum albumin-fluorescein isothiocyanate conjugate (BSA-FITC) were first tested in an in vitro setup using 1.5% agarose gel model. Subsequently, the ex vivo drug permeation study using a Franz diffusion cell was conducted, exhibiting a 61-fold, 43-fold, 54-fold, and 17-fold increment of the permeation of methylene blue, fluorescein sodium, lidocaine hydrochloride, and BSA-FITC, respectively, during the application of 1 mA cm(-2) current for 6 h. Moreover, the total amount of drug delivered (i.e. in the skin and receptor compartment) was analysed to untangle the different delivery profiles according to the types of molecule. Finally, the integration of the anode and cathode into an iontophoretic hollow microneedle array system (IHMAS) offers the full miniaturisation of the concept. Overall, the IHMAS device provides a versatile wearable technology for transdermal on-demand drug delivery that can improve the administration of personalised doses, and potentially enhance precision medicine.
Keywords: A1 Journal article; Engineering sciences. Technology; Antwerp Electrochemical and Analytical Sciences Lab (A-Sense Lab)
Impact Factor: 6.1
DOI: 10.1039/D3LC00160A
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