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- ItemMonitoring the thermally induced transition from sp3-hybridized into sp2-hybridized carbons(Amsterdam [u.a.] : Elsevier Science, 2021) Schüpfer, Dominique B.; Badaczewski, Felix; Peilstöcker, Jan; Guerra-Castro, Juan Manuel; Shim, Hwirim; Firoozabadi, Saleh; Beyer, Andreas; Volz, Kerstin; Presser, Volker; Heiliger, Christian; Smarsly, Bernd; Klar, Peter J.The preparation of carbons for technical applications is typically based on a treatment of a precursor, which is transformed into the carbon phase with the desired structural properties. During such treatment the material passes through several different structural stages, for example, starting from precursor molecules via an amorphous phase into crystalline-like phases. While the structure of non-graphitic and graphitic carbon has been well studied, the transformation stages from molecular to amorphous and non-graphitic carbon are still not fully understood. Disordered carbon often contains a mixture of sp3-, sp2-and sp1-hybridized bonds, whose analysis is difficult to interpret. We systematically address this issue by studying the transformation of purely sp3-hybridized carbons, that is, nanodiamond and adamantane, into sp2-hybridized non-graphitic and graphitic carbon. The precursor materials are thermally treated at different temperatures and the transformation stages are monitored. We employ Raman spectroscopy, WAXS and TEM to characterize the structural changes. We correlate the intensities and positions of the Raman bands with the lateral crystallite size La estimated by WAXS analysis. The behavior of the D and G Raman bands characteristic for sp2-type material formed by transforming the sp3-hybridized precursors into non-graphitic and graphitic carbon agrees well with that observed using sp2-structured precursors.
- ItemEffect of pore geometry on ultra-densified hydrogen in microporous carbons(Amsterdam [u.a.] : Elsevier Science, 2021) Tian, Mi; Lennox, Matthew J.; O’Malley, Alexander J.; Porter, Alexander J.; Krüner, Benjamin; Rudić, Svemir; Mays, Timothy J.; Düren, Tina; Presser, Volker; Terry, Lui R.; Rols, Stephane; Fang, Yanan; Dong, Zhili; Rochat, Sebastien; Ting, Valeska P.Our investigations into molecular hydrogen (H2) confined in microporous carbons with different pore geometries at 77 K have provided detailed information on effects of pore shape on densification of confined H2 at pressures up to 15 MPa. We selected three materials: a disordered, phenolic resin-based activated carbon, a graphitic carbon with slit-shaped pores (titanium carbide-derived carbon), and single-walled carbon nanotubes, all with comparable pore sizes of <1 nm. We show via a combination of in situ inelastic neutron scattering studies, high-pressure H2 adsorption measurements, and molecular modelling that both slit-shaped and cylindrical pores with a diameter of ∼0.7 nm lead to significant H2 densification compared to bulk hydrogen under the same conditions, with only subtle differences in hydrogen packing (and hence density) due to geometric constraints. While pore geometry may play some part in influencing the diffusion kinetics and packing arrangement of hydrogen molecules in pores, pore size remains the critical factor determining hydrogen storage capacities. This confirmation of the effects of pore geometry and pore size on the confinement of molecules is essential in understanding and guiding the development and scale-up of porous adsorbents that are tailored for maximising H2 storage capacities, in particular for sustainable energy applications.
- ItemBreakdown of continuum models for spherical probe adhesion tests on micropatterned surfaces(Amsterdam [u.a.] : Elsevier Science, 2021) Bettscheider, Simon; Yu, Dan; Foster, Kimberly; McMeeking, Robert; Arzt, Eduard; Hensel, René; Booth, Jamie A.The adhesion of fibrillar dry adhesives, mimicking nature's principles of contact splitting, is commonly characterized by using axisymmetric probes having either a flat punch or spherical geometry. When using spherical probes, the adhesive pull-off force measured depends strongly on the compressive preload applied when making contact and on the geometry of the probe. Together, these effects complicate comparisons of the adhesive performance of micropatterned surfaces measured in different experiments. In this work we explore these issues, extending previous theoretical treatments of this problem by considering a fully compliant backing layer with an array of discrete elastic fibrils on its surface. We compare the results of the semi-analytical model presented to existing continuum theories, particularly with respect to determining a measurement system- and procedure-independent metric for the local adhesive strength of the fibrils from the global pull-off force. It is found that the discrete nature of the interface plays a dominant role across a broad range of relevant system parameters. Accordingly, a convenient tool for simulation of a discrete array is provided. An experimental procedure is recommended for use in conjunction with this tool in order to extract a value for the local adhesive strength of the fibrils, which is independent of the other system properties (probe radius, backing layer thickness, and preload) and thus is suitable for comparison across experimental studies.
- ItemEmerging, hydrogen-driven electrochemical water purification(Amsterdam [u.a.] : Elsevier Science, 2022) Suss, M.E.; Zhang, Y.; Atlas, I.; Gendel, Y.; Ruck, E.B.; Presser, V.Energy-efficient technologies for the remediation of water and generation of drinking water is a key towards sustainable technologies. Electrochemical desalination technologies are promising alternatives towards established methods, such as reverse osmosis or nanofiltration. In the last few years, hydrogen-driven electrochemical water purification has emerged. This review article explores the concept of desalination fuel cells and capacitive-Faradaic fuel cells for ion separation.
- ItemFunctional surface microstructures inspired by nature – From adhesion and wetting principles to sustainable new devices(Amsterdam [u.a.] : Elsevier Science, 2021) Arzt, Eduard; Quan, Haocheng; McMeeking, Robert M.; Hensel, RenéIn the course of evolution nature has arrived at startling materials solutions to ensure survival. Investigations into biological surfaces, ranging from plants, insects and geckos to aquatic animals, have inspired the design of intricate surface patterns to create useful functionalities. This paper reviews the fundamental interaction mechanisms of such micropatterns with liquids, solids, and soft matter such as skin for control of wetting, self-cleaning, anti-fouling, adhesion, skin adherence, and sensing. Compared to conventional chemical strategies, the paradigm of micropatterning enables solutions with superior resource efficiency and sustainability. Associated applications range from water management and robotics to future health monitoring devices. We finally provide an overview of the relevant patterning methods as an appendix.
- ItemSodium-ion diffusion coefficients in tin phosphide determined with advanced electrochemical techniques(Amsterdam [u.a.] : Elsevier Science, 2023) Wang, Jun; Pameté, Emmanuel; Yan, Shengli; Zhao, Wenhua; Zhang, Jianhui; He, Xiaotong; Supiyeva, Zhazira; Abbas, Qamar; Pan, XuexueSodium ion insertion plays a critical role in developing robust sodium-ion technologies (batteries and hybrid supercapacitors). Diffusion coefficient values of sodium (DNa+) in tin phosphide between 0.1 V and 2.0 V vs. Na/Na+ are systematically determined by galvanostatic intermittent titration technique (GITT), electrochemical impedance spectroscopy (EIS), and potentiostatic intermittent titration technique (PITT). These values range between 4.55 × 10−12 cm2 s−1 and 1.94 × 10−8 cm2 s−1 and depend on the insertion/de-insertion current and the thickness of the electrode materials. Additionally, DNa+ values differ between the first and second cation insertion because of the solid electrolyte interface (SEI) formation. DNa+ vs. insertion potential alters non-linearly in a “W” form due to the strong interactions of Na+ with tin phosphide particles. The results reveal that GITT is a more appropriate electrochemical technique than PITT and EIS for evaluating DNa+ in tin phosphide.