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- ItemCarbons and electrolytes for advanced supercapacitors(Hoboken, NJ : Wiley, 2014) Presser, VolkerElectrical energy storage (EES) is one of the most critical areas of technological research around the world. Storing and efficiently using electricity generated by intermittent sources and the transition of our transportation fleet to electric drive depend fundamentally on the development of EES systems with high energy and power densities. Supercapacitors are promising devices for highly efficient energy storage and power management, yet they still suffer from moderate energy densities compared to batteries. To establish a detailed understanding of the science and technology of carbon/carbon supercapacitors, this review discusses the basic principles of the electrical double-layer (EDL), especially regarding the correlation between ion size/ion solvation and the pore size of porous carbon electrodes. We summarize the key aspects of various carbon materials synthesized for use in supercapacitors. With the objective of improving the energy density, the last two sections are dedicated to strategies to increase the capacitance by either introducing pseudocapacitive materials or by using novel electrolytes that allow to increasing the cell voltage. In particular, advances in ionic liquids, but also in the field of organic electrolytes, are discussed and electrode mass balancing is expanded because of its importance to create higher performance asymmetric electrochemical capacitors.
- ItemMixed Cu-Fe Sulfides Derived from Polydopamine-Coated Prussian Blue Analogue as a Lithium-Ion Battery Electrode(Washington, DC : ACS Publications, 2022) Bornamehr, Behnoosh; Presser, Volker; Husmann, SamanthaBatteries employing transition-metal sulfides enable high-charge storage capacities, but polysulfide shuttling and volume expansion cause structural disintegration and early capacity fading. The design of heterostructures combining metal sulfides and carbon with an optimized morphology can effectively address these issues. Our work introduces dopamine-coated copper Prussian blue (CuPB) analogue as a template to prepare nanostructured mixed copper-iron sulfide electrodes. The material was prepared by coprecipitation of CuPB with in situ dopamine polymerization, followed by thermal sulfidation. Dopamine controls the particle size and favors K-rich CuPB due to its polymerization mechanism. While the presence of the coating prevents particle agglomeration during thermal sulfidation, its thickness demonstrates a key effect on the electrochemical performance of the derived sulfides. After a two-step activation process during cycling, the C-coated KCuFeS2electrodes showed capacities up to 800 mAh/g at 10 mA/g with nearly 100% capacity recovery after rate handling and a capacity of 380 mAh/g at 250 mA/g after 500 cycles.
- 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.
- ItemEnhanced electrochemical energy storage by nanoscopic decoration of endohedral and exohedral carbon with vanadium oxide via atomic layer deposition(Washington D.C. : American Chemical Society, 2016) Fleischmann, Simon; Jäckel, Nicolas; Zeiger, Marco; Krüner, Benjamin; Grobelsek, Ingrid; Formanek, Petr; Choudhury, Soumyadip; Weingarth, Daniel; Presser, VolkerAtomic layer deposition (ALD) is a facile process to decorate carbon surfaces with redox-active nanolayers. This is a particularly attractive route to obtain hybrid electrode materials for high performance electrochemical energy storage applications. Using activated carbon and carbon onions as representatives of substrate materials with large internal or external surface area, respectively, we have studied the enhanced energy storage capacity of vanadium oxide coatings. While the internal porosity of activated carbon readily becomes blocked by obstructing nanopores, carbon onions enable the continued deposition of vanadia within their large interparticle voids. Electrochemical benchmarking in lithium perchlorate in acetonitrile (1 M LiClO4) showed a maximum capacity of 122 mAh/g when using vanadia coated activated carbon and 129 mAh/g for vanadia coated carbon onions. There is an optimum amount of vanadia between 50 and 65 wt % for both substrates that results in an ideal balance between redox-activity and electrical conductivity of the hybrid electrode. Assembling asymmetric (charge balanced) full-cells, a maximum specific energy of 38 Wh/kg and 29 Wh/kg was found for carbon onions and activated carbon, respectively. The stability of both systems is promising, with a capacity retention of ∼85–91% after 7000 cycles for full-cell measurements.
- ItemSelf-Activation of Inorganic-Organic Hybrids Derived through Continuous Synthesis of Polyoxomolybdate and para-Phenylenediamine Enables Very High Lithium-Ion Storage Capacity(Weinheim : Wiley-VCH, 2023) Mohamed, Mana Abdirahman; Arnold, Stefanie; Janka, Oliver; Quade, Antje; Presser, Volker; Kickelbick, GuidoInorganic-organic hybrid materials with redox-active components were prepared by an aqueous precipitation reaction of ammonium heptamolybdate (AHM) with para-phenylenediamine (PPD). A scalable and low-energy continuous wet chemical synthesis process, known as the microjet process, was used to prepare particles with large surface area in the submicrometer range with high purity and reproducibility on a large scale. Two different crystalline hybrid products were formed depending on the ratio of molybdate to organic ligand and pH. A ratio of para-phenylenediamine to ammonium heptamolybdate from 1 : 1 to 5 : 1 resulted in the compound [C6H10N2]2[Mo8O26] ⋅ 6 H2O, while higher PPD ratios from 9 : 1 to 30 : 1 yielded a composition of [C6H9N2]4[NH4]2[Mo7O24] ⋅ 3 H2O. The electrochemical behavior of the two products was tested in a battery cell environment. Only the second of the two hybrid materials showed an exceptionally high capacity of 1084 mAh g−1 at 100 mA g−1 after 150 cycles. The maximum capacity was reached after an induction phase, which can be explained by a combination of a conversion reaction with lithium to Li2MoO4 and an additional in situ polymerization of PPD. The final hybrid material is a promising material for lithium-ion battery (LIB) applications.
- ItemComment on "Synthesis, characterization and growth mechanism of flower-like vanadium carbide hierarchical nanocrystals"(Cambridge : Royal Society of Chemistry, 2012) Presser, Volker; Vakifahmetoglu, CekdarThis Letter is in response to a recent paper by Ma et al. (CrystEngComm, 2010, 12, 750-754) which arguably studied vanadium carbide nanostructures whereas all available evidence indicates the study of vanadium oxide. We feel that it is important to communicate to the community several inconsistencies so that the interesting material reported can be seen in the right light, especially with several groups nowadays having reported similar structures from vanadium oxide synthesis.
- ItemOne-step synthesis of nanocrystalline transition metal oxides on thin sheets of disordered graphitic carbon by oxidation of MXenes(Cambridge : Royal Society of Chemistry, 2014) Naguib, Michael; Mashtalir, Olhar; Lukatskaya, Maria R.; Dyatkin, Boris; Zhang, Chuanfang; Presser, Volker; Gogotsi, Yuri; Barsoum, Michael W.Herein we show that heating 2D Ti3C2 in air results in TiO2 nanocrystals enmeshed in thin sheets of disordered graphitic carbon structures that can handle extremely high cycling rates when tested as anodes in lithium ion batteries. Oxidation of 2D Ti3C2 in either CO2 or pressurized water also resulted in TiO2–C hybrid structures. Similarly, other hybrids can be produced, as we show here for Nb2O5/C from 2D Nb2C.
- ItemDye-Loaded Mechanochromic and pH-Responsive Elastomeric Opal Films(Weinheim : Wiley-VCH, 2021) Winter, Tamara; Boehm, Anna; Presser, Volker; Gallei, MarkusIn this work, the preparation and fabrication of elastomeric opal films revealing reversible mechanochromic and pH-responsive features are reported. The core–interlayer–shell (CIS) particles are synthesized via stepwise emulsion polymerization leading to hard core (polystyrene), crosslinked interlayer (poly(methyl methacrylate-co-allyl methacrylate), and soft poly(ethyl acrylate-co-butyl acrylate-co-(2-hydroxyethyl) methacrylate) shell particles featuring a size of 294.9 ± 14.8 nm. This particle architecture enables the application of the melt-shear organization technique leading to elastomeric opal films with orange, respectively, green brilliant reflection colors dependent on the angle of view. Moreover, the hydroxyl moieties as part of the particle shell are advantageously used for subsequent thermally induced crosslinking reactions enabling the preparation of reversibly tunable mechanochromic structural colors based on Bragg's law of diffraction. Additionally, the CIS particles can be loaded upon extrusion or chemically by a postfunctionalization strategy with organic dyes implying pH-responsive features. This convenient protocol for preparing multi-responsive, reversibly stretch-tunable opal films is expected to enable a new material family for anti-counterfeiting applications based on external triggers.
- ItemThermo-Responsive Ultrafiltration Block Copolymer Membranes Based on Polystyrene-block-poly(diethyl acrylamide)(Weinheim : Wiley-VCH GmbH, 2023) Frieß, Florian V.; Hartmann, Frank; Gemmer, Lea; Pieschel, Jens; Niebuur, Bart‐Jan; Faust, Matthias; Kraus, Tobias; Presser, Volker; Gallei, MarkusWithin the present work, a thermo-responsive ultrafiltration membrane is manufactured based on a polystyrene-block-poly(diethyl acrylamide) block copolymer (BCP). The poly(diethyl acrylamide) block segment features a lower critical solution temperature (LCST) in water, similar to the well-known poly(N-isopropylacrylamide), but having increased biocompatibility and without exhibiting a hysteresis of the thermally induced switching behavior. The BCP is synthesized via sequential “living” anionic polymerization protocols and analyzed by 1H-NMR spectroscopy, size exclusion chromatography, and differential scanning calorimetry. The resulting morphology in the bulk state is investigated by transmission electron microscopy (TEM) and small-angle X-ray scattering (SAXS) revealing the intended hexagonal cylindrical morphology. The BCPs form micelles in a binary mixture of tetrahydrofuran and dimethylformamide, where BCP composition and solvent affinities are discussed in light of the expected structure of these micelles and the resulting BCP membrane formation. The membranes are manufactured using the non-solvent induced phase separation (NIPS) process and are characterized via scanning electron microscopy (SEM) and water permeation measurements. The latter are carried out at room temperature and at 50 °C revealing up to a 23-fold increase of the permeance, when crossing the LCST of the poly(diethyl acrylamide) block segment in water.