Browsing by Author "Giebeler, L."
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- ItemAmorphous Li-Al-based compounds: A novel approach for designing high performance electrode materials for Li-ion batteries(Basel : MDPI AG, 2013) Thoss, F.; Giebeler, L.; Thomas, J.; Oswald, S.; Potzger, K.; Reuther, H.; Ehrenberg, H.; Eckert, J.A new amorphous compound with the initial atomic composition Al43Li43Y6Ni8 applied as electrode material for Li-ion batteries is investigated. Unlike other amorphous compounds so-far investigated as anode materials, it already contains Li as a base element in the uncycled state. The amorphous compound powder is prepared by high energy ball milling of a master alloy. It shows a strongly enhanced specific capacity in contrast to amorphous alloys without Li in the initial state. Therewith, by enabling a reversible (de)lithiation of metallic electrodes without the phase transition caused volume changes it offers the possibility of much increased specific capacities than conventional graphite anodes. According to the charge rate (C-rate), the specific capacity is reversible over 20 cycles at minimum in contrast to conventional crystalline intermetallic phases failing by volume changes. The delithiation process occurs quasi-continuously over a voltage range of nearly 4 V, while the lithiation is mainly observed between 0.1 V and 1.5 V. That way, the electrode is applicable for different potential needs. The electrode stays amorphous during cycling, thus avoiding volume changes. The cycling performance is further enhanced by a significant amount of Fe introduced as wear debris from the milling tools, which acts as a promoting element.
- ItemAnodically fabricated TiO2–SnO2 nanotubes and their application in lithium ion batteries(Cambridge : Royal Society of Chemistry, 2016) Madian, M.; Klose, M.; Jaumann, T.; Gebert, A.; Oswald, S.; Ismail, N.; Eychmüller, A.; Eckerta, J.; Giebeler, L.Developing novel electrode materials is a substantial issue to improve the performance of lithium ion batteries. In the present study, single phase Ti–Sn alloys with different Sn contents of 1 to 10 at% were used to fabricate Ti–Sn–O nanotubes via a straight-forward anodic oxidation step in an ethylene glycolbased solution containing NH4F. Various characterization tools such as SEM, EDXS, TEM, XPS and Raman spectroscopy were used to characterize the grown nanotube films. Our results reveal the successful formation of mixed TiO2/SnO2 nanotubes in the applied voltage range of 10–40 V. The as-formed nanotubes are amorphous and their dimensions are precisely controlled by tuning the formation voltage which turns Ti–Sn–O nanotubes into highly attractive materials for various applications. As an example, the Ti–Sn–O nanotubes offer promising properties as anode materials in lithium ion batteries. The electrochemical performance of the grown nanotubes was evaluated against a Li/Li+ electrode at a current density of 504 mA cm2. The results demonstrate that TiO2/SnO2 nanotubes prepared at 40 V on a TiSn1 alloy substrate display an average 1.4 fold increase in areal capacity with excellent cycling stability over more than 400 cycles compared to the pure TiO2 nanotubes fabricated and tested under identical conditions. This electrode was tested at current densities of 50, 100, 252, 504 and 1008 mA cm2 exhibiting average capacities of 780, 660, 490, and 405 mA cm2 (i.e. 410, 345, 305 and 212 mA h g1), respectively. The remarkably improved electrochemical performance is attributed to enhanced lithium ion diffusion which originates from the presence of SnO2 nanotubes and the high surface area of the mixed oxide tubes. The TiO2/SnO2 electrodes retain their original tubular structure after electrochemical cycling with only slight changes in their morphology.
- ItemBinding energy referencing for XPS in Alkali metal-based battery materials research (II): Application to complex composite electrodes(Basel : MDPI AG, 2018) Oswald, S.; Thoss, F.; Zier, M.; Hoffmann, M.; Jaumann, T.; Herklotz, M.; Nikolowski, K.; Scheiba, F.; Kohl, M.; Giebeler, L.; Mikhailova, D.; Ehrenberg, H.X-ray photoelectron spectroscopy (XPS) is a key method for studying (electro-)chemical changes in metal-ion battery electrode materials. In a recent publication, we pointed out a conflict in binding energy (BE) scale referencing at alkali metal samples, which is manifested in systematic deviations of the BEs up to several eV due to a specific interaction between the highly reactive alkali metal in contact with non-conducting surrounding species. The consequences of this phenomenon for XPS data interpretation are discussed in the present manuscript. Investigations of phenomena at surface-electrolyte interphase regions for a wide range of materials for both lithium and sodium-based applications are explained, ranging from oxide-based cathode materials via alloys and carbon-based anodes including appropriate reference chemicals. Depending on material class and alkaline content, specific solutions are proposed for choosing the correct reference BE to accurately define the BE scale. In conclusion, the different approaches for the use of reference elements, such as aliphatic carbon, implanted noble gas or surface metals, partially lack practicability and can lead to misinterpretation for application in battery materials. Thus, this manuscript provides exemplary alternative solutions.
- ItemAn efficient two-polymer binder for high-performance silicon nanoparticle-based lithium-ion batteries: A systematic case study with commercial polyacrylic acid and polyvinyl butyral polymers(Pennington, NJ : Electrochemical Society Inc., 2019) Urbanski, A.; Omar, A.; Guo, J.; Janke, A.; Reuter, U.; Malanin, M.; Schmidt, F.; Jehnichen, D.; Holzschuh, M.; Simon, F.; Eichhorn, K.-J.; Giebeler, L.; Uhlmann, P.Silicon is one of the most promising anode materials for high energy density lithium ion batteries (LIBs) due to its high theoretical capacity and natural abundance. Unfortunately, significant challenges arise due to the large volume change of silicon upon lithiation/delithiation which inhibit its broad commercialization. An advanced binder can, in principle, reversibly buffer the volume change, and maintain strong adhesion toward various components as well as the current collector. In this work, we present the first report on the applicability of polyvinyl butyral (PVB) polymer as a binder component for silicon nanoparticles-based LIBs. Characteristic binder properties of commercial PVB and polyacrylic acid (PAA) polymers are compared. The work focuses on polymer mixtures of PVB polymers with PAA, for an improved binder composition which incorporates their individual advantages. Different ratios of polymers are systematically studied to understand the effect of particular polymer chains, functional groups and mass fractions, on the electrochemical performance. We demonstrate a high-performance polymer mixture which exhibits good binder-particle interaction and strong adhesion to Cu-foil. PAA/PVB-based electrode with a Si loading of ∼1 mg/cm2 tested between 0.01 and 1.2 V vs. Li/Li+ demonstrate specific capacities as high as 2170 mAh/g after the first hundred cycles. © The Author(s) 2019.
- ItemElectrodeposited metal-organic framework films as self-assembled hierarchically superstructured supports for stable omniphobic surface coatings(London : Nature Publishing Group, 2018) Sablowski, J.; Linnemann, J.; Hempel, S.; Hoffmann, V.; Unz, S.; Beckmann, M.; Giebeler, L.Superhierarchically rough films are rapidly synthesised on metal substrates via electrochemically triggered self-assembly of meso/macroporous-structured metal-organic framework (MOF) crystals. These coatings are applied to immobilise a functional oil with low surface energy to provide stable coatings repellent to a wide range of hydrophobic as well as hydrophilic fluids. Such omniphobic surfaces are highly interesting for several applications such as anti-fouling, anti-icing, and dropwise condensation, and become easily scalable with the presented bottom-up fabrication approach. As investigated by environmental scanning electron microscopy (ESEM), the presented perfluorinated oil-infused Cu-BTC coating constitutes of a flat liquid-covered surface with protruding edges of octahedral superstructured MOF crystals. Water and non-polar diiodomethane droplets form considerably high contact angles and even low-surface-tension fluids, e.g. acetone, form droplets on the infused coating. The repellent properties towards the test fluids do not change upon extended water spraying in contrast to oil-infused porous copper oxide or native copper surfaces. It is discussed in detail, how the presented electrodeposited MOF films grow and provide a proficient surface morphology to stabilise the functional oil film due to hemiwicking.
- ItemThe impact of surface morphology on the magnetovolume transition in magnetocaloric LaFe11.8Si1.2(New York : American Institute of Physics, 2016) Waske, A.; Lovell, E.; Funk, A.; Sellschopp, K.; Rack, A.; Giebeler, L.; Gostin, P.F.; Fähler, S.; Cohen, L.F.First order magnetocaloric materials reach high entropy changes but at the same time exhibit hysteresis losses which depend on the sample’s microstructure. We use non-destructive 3D X-ray microtomography to understand the role of surface morphology for the magnetovolume transition of LaFe11.8Si1.2. The technique provides unique information on the spatial distribution of the volume change at the transition and its relationship with the surface morphology. Complementary Hall probe imaging confirms that on a morphologically complex surface minimization of strain energy dominates. Our findings sketch the way for a tailored surface morphology with low hysteresis without changing the underlying phase transition.
- ItemIn situ Raman spectroscopy on silicon nanowire anodes integrated in lithium ion batteries(Pennington, NJ : Electrochemical Society Inc., 2019) Krause, A.; Tkacheva, O.; Omar, A.; Langklotz, U.; Giebeler, L.; Dörfler, S.; Fauth, F.; Mikolajick, T.; Weber, W.M.Rapid decay of silicon anodes during lithiation poses a significant challenge in application of silicon as an anode material in lithium ion batteries. In situ Raman spectroscopy is a powerful method to study the relationship between structural and electrochemical data during electrode cycling and to allow the observation of amorphous as well as liquid and transient species in a battery cell. Herein, we present in situ Raman spectroscopy on high capacity electrode using uncoated and carbon-coated silicon nanowires during first lithiation and delithiation cycle in an optimized lithium ion battery setup and complement the results with operando X-ray reflection diffraction measurements. During lithiation, we were able to detect a new Raman signal at 1859 cm−1 especially on uncoated silicon nanowires. The detailed in situ Raman measurement of the first lithiation/delithiation cycle allowed to differentiate between morphology changes of the electrode as well as interphase formation from electrolyte components.
- ItemPreparation and cycling performance of iron or iron oxide containing amorphous Al-Li alloys as electrodes(Basel : MDPI AG, 2014) Thoss, F.; Giebeler, L.; Weißer, K.; Feller, J.; Eckert, J.Crystalline phase transitions cause volume changes, which entails a fast destroying of the electrode. Non-crystalline states may avoid this circumstance. Herein we present structural and electrochemical investigations of pre-lithiated, amorphous Al39Li43Fe13Si5-powders, to be used as electrode material for Li-ion batteries. Powders of master alloys with the compositions Al39Li43Fe13Si5 and Al39Li43Fe13Si5 + 5 mass-% FeO were prepared via ball milling and achieved amorphous/nanocrystalline states after 56 and 21.6 h, respectively. In contrast to their Li-free amorphous pendant Al78Fe13Si9, both powders showed specific capacities of about 400 and 700 Ah/kgAl, respectively, after the third cycle.