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- ItemElectrochemical growth mechanism of nanoporous platinum layers([London] : Macmillan Publishers Limited, part of Springer Nature, 2021) Stanca, Sarmiza-Elena; Vogt, Oliver; Zieger, Gabriel; Ihring, Andreas; Dellith, Jan; Undisz, Andreas; Rettenmayr, Markus; Schmidt, HeidemariePorous platinum is a frequently used catalyst material in electrosynthesis and a robust broadband absorber in thermoelectrics. Pore size distribution and localization determine its properties by a large extent. However, the pore formation mechanism during the growth of the material remains unclear. In this work we elucidate the mechanism underlying electrochemical growth of nanoporous platinum layers and its control by ionic concentration and current density during electrolysis. The electrode kinetics and reduction steps of PtCl4 on platinum electrodes are investigated by cyclic voltammetry and impedance measurements. Cyclic voltammograms show three reduction steps: two steps relate to the platinum cation reduction, and one step relates to the hydrogen reduction. Hydrogen is not involved in the reduction of PtCl4, however it enables the formation of nanopores in the layers. These findings contribute to the understanding of electrochemical growth of nanoporous platinum layers in isopropanol with thickness of 100 nm to 500 nm.
- ItemStructure of Ni(OH)2 intermediates determines the efficiency of NiO-based photocathodes – a case study using novel mesoporous NiO nanostars(Cambridge : RSC, 2019) Wahyuono, Ruri Agung; Dellith, Andrea; Schmidt, Christa; Dellith, Jan; Ignaszak, Anna; Seyring, Martin; Rettenmayr, Markus; Fize, Jennifer; Artero, Vincent; Chavarot-Kerlidou, Murielle; Dietzek, BenjaminWe report the wet chemical synthesis of mesoporous NiO nanostars (NS) as photocathode material for dye-sensitized solar cells (DSSCs). The growth mechanism of NiO NS as a new morphology of NiO is assessed by TEM and spectroscopic investigations. The NiO NS are obtained upon annealing of preformed β-Ni(OH)2 into pristine NiO with low defect concentrations and favorable electronic configuration for dye sensitization. The NiO NS consist of fibers self-assembled from nanoparticles yielding a specific surface area of 44.9 m2 g-1. They possess a band gap of 3.83 eV and can be sensitized by molecular photosensitizers bearing a range of anchoring groups, e.g. carboxylic acid, phosphonic acid, and pyridine. The performance of NiO NS-based photocathodes in photoelectrochemical application is compared to that of other NiO morphologies, i.e. nanoparticles and nanoflakes, under identical conditions. Sensitization of NiO NS with the benchmark organic dye P1 leads to p-DSSCs with a high photocurrent up to 3.91 mA cm-2 whilst the photoelectrochemical activity of the NiO NS photocathode in aqueous medium in the presence of an irreversible electron acceptor is reflected by generation of a photocurrent up to 23 μA cm-2 © 2019 The Royal Society of Chemistry.
- ItemPlasma-based VAD process for multiply doped glass powders and high-performance fiber preforms with outstanding homogeneity(Hoboken, NJ : Wiley Interscience, 2020) Trautvetter, Tom; Schäfer, Jan; Benzine, Omar; Methling, Ralf; Baierl, Hardy; Reichel, Volker; Dellith, Jan; Köpp, Daniel; Hempel, Frank; Stankov, Marjan; Baeva, Margarita; Foest, Rüdiger; Wondraczek, Lothar; Wondraczek, Katrin; Bartelt, HartmutAn innovative approach using the vapor axial deposition (VAD), for the preparation of silica-based high-power fiber laser preforms, is described in this study. The VAD uses a plasma deposition system operating at atmospheric pressure, fed by a single, chemically adapted solution containing precursors of laser-active dopants (e.g., Yb2O3), glass-modifier species (e.g., Al2O3), and the silica matrix. The approach enables simultaneous doping with multiple optically active species and overcomes some of the current technological limitations encountered with well-established fiber preform technologies in terms of dopant distribution, doping levels, and achievable active core diameter. The deposition of co-doped silica with outstanding homogeneity is proven by Raman spectroscopy and electron probe microanalysis. Yb2O3 concentrations are realized up to 0.3 mol% in SiO2, with simultaneous doping of 3 mol% of Al2O3.
- ItemModification of Surface Bond Au Nanospheres by Chemically and Plasmonically Induced Pd Deposition(Basel : MDPI, 2021) Stolle, Heike Lisa Kerstin Stephanie; Csáki, Andrea; Dellith, Jan; Fritzsche, WolfgangIn this work we investigated methods of modifying gold nanospheres bound to a silicon surface by depositing palladium onto the surfaces of single nanoparticles. Bimetallic Au-Pd nanoparticles can thus be gained for use in catalysis or sensor technology. For Pd deposition, two methods were chosen. The first method was the reduction of palladium acetate by ascorbic acid, in which the amounts of palladium acetate and ascorbic acid were varied. In the second method we utilized light-induced metal deposition by making use of the plasmonic effect. Through this method, the surface bond nanoparticles were irradiated with light of wavelengths capable of inducing plasmon resonance. The generation of hot electrons on the particle surface then reduced the palladium acetate in the vicinity of the gold nanoparticle, resulting in palladium-covered gold nanospheres. In our studies we demonstrated the effect of both enhancement methods by monitoring the particle heights over enhancement time by atomic force microscopy (AFM), and investigated the influence of ascorbic acid/Pd acetate concentration as well as the impact of the irradiated wavelengths on the enhancement effect. It could thus be proven that both methods were valid for obtaining a deposition of Pd on the surface of the gold nanoparticles. Deposition of Pd on the gold particles using the light-assisted method could be observed, indicating the impact of the plasmonic effect and hot electron for Pd acetate reduction on the gold particle surface. In the case of the reduction method with ascorbic acid, in addition to Pd deposition on the gold nanoparticle surface, larger pure Pd particles and extended clusters were also generated. The reduction with ascorbic acid however led to a considerably thicker Pd layer of up to 54 nm in comparison to up to 11 nm for the light-induced metal deposition with light resonant to the particle absorption wavelength. Likewise, it could be demonstrated that light of non-resonant wavelengths was not capable of initiating Pd deposition, since a growth of only 1.6 nm (maximum) was observed for the Pd layer.
- ItemZnO nanoflowers-based photoanodes: aqueous chemical synthesis, microstructure and optical properties(Berlin : de Gruyter, 2016) Wahyuono, Ruri Agung; Schmidt, Christa; Dellith, Andrea; Dellith, Jan; Schulz, Martin; Seyring, Martin; Rettenmayr, Markus; Plentz, Jonathan; Dietzek, BenjaminWe have developed an efficient, low temperature, synthetic route for ZnO nanoflowers (NFs) as photoanode material. This alternative route yields small flowerlike nanostructures, built from densely self-assembled tip-ended rod structures. The obtained ZnO NFs possess a large bandgap of 3.27 - 3.39 eV, enabling the generation of an average open current voltage of 0.56 V. Additionally, they show a high internal light harvesting of 14.6•10-7A-mol-1. The growth mechanism and self-assembly of ZnO NFs were studied in detail by joint spectroscopic-TEM investigations. It is shown that the ZnO crystallite size increases with increasing annealing temperatures and that the stress and the improved crystallinity are induced by annealing and reduce the lattice strain and the dislocation density. The bandgaps of ZnO are affected by the lattice strain revealing an optimal region of lattice strain to gain high bandgap energies. The properties of the synthesized ZnO NFs are compared with other morphologies, i.e. ZnO spherical aggregates (SPs) and ZnO nanorods (NRs), and are tested as electrode materials in dye-sensitized solar cells.
- ItemPorous spherical gold nanoparticles via a laser induced process(Cambridge : Royal Society of Chemistry, 2022) Schmidl, Gabriele; Raugust, Marc; Jia, Guobin; Dellith, Andrea; Dellith, Jan; Schmidl, Frank; Plentz, JonathanNanoparticles consisting of a mixture of several metals and also porous nanoparticles due to their special structure exhibit properties that find applications in spectroscopic detection or catalysis. Different approaches of top down or bottom up technologies exist for the fabrication of such particles. We present a novel combined approach for the fabrication of spherical porous gold nanoparticles on low-cost glass substrates under ambient conditions using a UV-laser induced particle preparation process with subsequent wet chemical selective etching. In this preparation route, nanometer-sized branched structures are formed in spherical particles. The laser process, which is applied to a silver/gold bilayer system with different individual layer thicknesses, generates spherical mixed particles in a nanosecond range and influences the properties of the fabricated nanoparticles, such as the size and the mixture and thus the spectral response. The subsequent etching process is performed by selective wet chemical removal of silver from the nanoparticles with diluted nitric acid. The gold to silver ratio was investigated by energy-dispersive X-ray spectroscopy. The porosity depends on laser parameters and film thickness as well as on etching parameters such as time. After etching, the surface area of the remaining Au nanoparticles increases which makes these particles interesting for catalysis and also as carrier particles for substances. Such substances can be positioned at defined locations or be released in appropriate environments. Absorbance spectra are also analyzed to show how the altered fractured shape of the particles changes localized plasmon resonances of the resultingt particles.
- ItemSelf-Assembled Graphene/MWCNT Bilayers as Platinum- Free Counter Electrode in Dye-Sensitized Solar Cells(Weinheim : Wiley-VCH Verl., 2019) Wahyuono, Ruri Agung; Jia, Guobin; Plentz, Jonathan; Dellith, Andrea; Dellith, Jan; Herrmann-Westendorf, Felix; Seyring, Martin; Presselt, Martin; Andrä, Gudrun; Rettenmayr, Markus; Dietzek, BenjaminWe describe the preparation and properties of bilayers of graphene- and multi-walled carbon nanotubes (MWCNTs) as an alternative to conventionally used platinum-based counter electrode for dye-sensitized solar cells (DSSC). The counter electrodes were prepared by a simple and easy-to-implement double self-assembly process. The preparation allows for controlling the surface roughness of electrode in a layer-by-layer deposition. Annealing under N2 atmosphere improves the electrode's conductivity and the catalytic activity of graphene and MWCNTs to reduce the I3 − species within the electrolyte of the DSSC. The performance of different counter-electrodes is compared for ZnO photoanode-based DSSCs. Bilayer electrodes show higher power conversion efficiencies than monolayer graphene electrodes or monolayer MWCNTs electrodes. The bilayer graphene (bottom)/MWCNTs (top) counter electrode-based DSSC exhibits a maximum power conversion efficiency of 4.1 % exceeding the efficiency of a reference DSSC with a thin film platinum counter electrode (efficiency of 3.4 %). In addition, the double self-assembled counter electrodes are mechanically stable, which enables their recycling for DSSCs fabrication without significant loss of the solar cell performance. © 2019 The Authors. Published by Wiley-VCH Verlag GmbH & Co. KGaA.
- ItemApplication of Thermal Response Measurements to Investigate Enhanced Water Adsorption Kinetics in Ball-Milled C2N-Type Materials(Weinheim : Wiley-VCH-Verl., 2022) Du, Shengjun; Leistenschneider, Desirée; Xiao, Jing; Dellith, Jan; Troschke, Erik; Oschatz, MartinSorption-based water capture is an attractive solution to provide potable water in arid regions. Heteroatom-decorated microporous carbons with hydrophilic character are promising candidates for water adsorption at low humidity, but the strong affinity between the polar carbon pore walls and water molecules can hinder the water transport within the narrow pore system. To reduce the limitations of mass transfer, C2N-type carbon materials obtained from the thermal condensation of a molecular hexaazatriphenylene-hexacarbonitrile (HAT-CN) precursor were treated mechanochemically via ball milling. Scanning electron microscopy as well as static light scattering reveal that large pristine C2N-type particles were split up to a smaller size after ball milling, thus increasing the pore accessibility which consequently leads to faster occupation of the water vapor adsorption sites. The major aim of this work is to demonstrate the applicability of thermal response measurements to track these enhanced kinetics of water adsorption. The adsorption rate constant of a C2N material condensed at 700 °C remarkably increased from 0.026 s−1 to 0.036 s−1 upon ball milling, while maintaining remarkably high water vapor capacity. This work confirms the advantages of small particle sizes in ultramicroporous materials on their vapor adsorption kinetics. It is demonstrated that thermal response measurements are a valuable and time-saving method to investigate water adsorption kinetics, capacities, and cycling stability.