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- ItemHigh-performance Li-O2 batteries with trilayered Pd/MnOx/Pd nanomembranes(Hoboken, NJ : Wiley, 2015) Lu, Xueyi; Deng, Junwen; Si, Wenping; Sun, Xiaolei; Liu, Xianghong; Liu, Bo; Liu, Lifeng; Oswald, Steffen; Baunack, Stefan; Grafe, Hans Joachim; Yan, Chenglin; Schmidt, Oliver G.Trilayered Pd/MnOx/Pd nanomembranes are fabricated as the cathode catalysts for Li‐O2 batteries. The combination of Pd and MnOx facilitates the transport of electrons, lithium ions, and oxygen‐containing intermediates, thus effectively decomposing the discharge product Li2O2 and significantly lowering the charge overpotential and enhancing the power efficiency. This is promising for future environmentally friendly applications.
- ItemDirectly Anodized Sulfur-Doped TiO2 Nanotubes as Improved Anodes for Li-ion Batteries(Basel : MDPI, 2020) Sabaghi, Davood; Madian, Mahmoud; Omar, Ahmad; Oswald, Steffen; Uhlemann, Margitta; Maghrebi, Morteza; Baniadam, Majid; Mikhailova, DariaTiO2 represents one of the promising anode materials for lithium ion batteries due to its high thermal and chemical stability, relatively high theoretical specific capacity and low cost. However, the electrochemical performance, particularly for mesoporous TiO2, is limited and must be further developed. Elemental doping is a viable route to enhance rate capability and discharge capacity of TiO2 anodes in Li-ion batteries. Usually, elemental doping requires elevated temperatures, which represents a challenge, particularly for sulfur as a dopant. In this work, S-doped TiO2 nanotubes were successfully synthesized in situ during the electrochemical anodization of a titanium substrate at room temperature. The electrochemical anodization bath represented an ethylene glycol-based solution containing NH4F along with Na2S2O5 as the sulfur source. The S-doped TiO2 anodes demonstrated a higher areal discharge capacity of 95 µAh·cm−2 at a current rate of 100 µA·cm−2 after 100 cycles, as compared to the pure TiO2 nanotubes (60 µAh·cm−2). S-TiO2 also exhibited a significantly improved rate capability up to 2500 µA·cm−2 as compared to undoped TiO2. The improved electrochemical performance, as compared to pure TiO2 nanotubes, is attributed to a lower impedance in S-doped TiO2 nanotubes (STNTs). Thus, the direct S-doping during the anodization process is a promising and cost-effective route towards improved TiO2 anodes for Li-ion batteries.
- ItemAuger- and X-ray Photoelectron Spectroscopy at Metallic Li Material: Chemical Shifts Related to Sample Preparation, Gas Atmosphere, and Ion and Electron Beam Effects(Basel : MDPI, 2022) Oswald, SteffenLi-based batteries are a key element in reaching a sustainable energy economy in the near future. The understanding of the very complex electrochemical processes is necessary for the optimization of their performance. X-ray photoelectron spectroscopy (XPS) is an accepted method used to improve understanding around the chemical processes at the electrode surfaces. Nevertheless, its application is limited because the surfaces under investigation are mostly rough and inhomogeneous. Local elemental analysis, such as Auger electron spectroscopy (AES), could assist XPS to gain more insight into the chemical processes at the surfaces. In this paper, some challenges in using electron spectroscopy are discussed, such as binding energy (BE) referencing for the quantitative study of chemical shifts, gas atmospheric influences, or beam damage (including both AE and XP spectroscopy). Carefully prepared and surface-modified metallic lithium material is used as model surface, considering that Li is the key element for most battery applications.
- ItemA High-Voltage, Dendrite-Free, and Durable Zn–Graphite Battery(Weinheim : Wiley-VCH, 2019) Wang, Gang; Kohn, Benjamin; Scheler, Ulrich; Wang, Faxing; Oswald, Steffen; Löffler, Markus; Tan, Deming; Zhang, Panpan; Zhang, Jian; Feng, XinliangThe intrinsic advantages of metallic Zn, like high theoretical capacity (820 mAh g−1), high abundance, low toxicity, and high safety have driven the recent booming development of rechargeable Zn batteries. However, the lack of high-voltage electrolyte and cathode materials restricts the cell voltage mostly to below 2 V. Moreover, dendrite formation and the poor rechargeability of the Zn anode hinder the long-term operation of Zn batteries. Here a high-voltage and durable Zn–graphite battery, which is enabled by a LiPF6-containing hybrid electrolyte, is reported. The presence of LiPF6 efficiently suppresses the anodic oxidation of Zn electrolyte and leads to a super-wide electrochemical stability window of 4 V (vs Zn/Zn2+). Both dendrite-free Zn plating/stripping and reversible dual-anion intercalation into the graphite cathode are realized in the hybrid electrolyte. The resultant Zn–graphite battery performs stably at a high voltage of 2.8 V with a record midpoint discharge voltage of 2.2 V. After 2000 cycles at a high charge–discharge rate, high capacity retention of 97.5% is achieved with ≈100% Coulombic efficiency. © 2019 The Authors. Published by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
- ItemEvaluation of surface cleaning procedures for CTGS substrates for SAW technology with XPS(Basel : MDPI, 2017) Brachmann, Erik; Seifert, Marietta; Oswald, Steffen; Menzel, Siegfried B.; Gemming, ThomasA highly efficient and reproducible cleaning procedure of piezoelectric substrates is essential in surface acoustic waves (SAW) technology to fabricate high-quality SAW devices, especially for new applications such SAW sensors wherein new materials for piezoelectric substrates and interdigital transducers are used. Therefore, the development and critical evaluation of cleaning procedures for each material system that is under consideration becomes crucial. Contaminants like particles or the presence of organic/inorganic material on the substrate can dramatically influence and alter the properties of the thin film substrate composite, such as wettability, film adhesion, film texture, and so on. In this article, focus is given to different cleaning processes like SC-1 and SC-2, UV-ozone treatment, as well as cleaning by first-contact polymer Opticlean, which are applied for removal of contaminants from the piezoelectric substrate Ca 3 TaGa 3 Si 2 O 14 . By means of X-ray photoelectron spectroscopy, the presence of the most critical contaminants such as carbon, sodium, and iron removed through different cleaning procedures were studied and significant differences were observed between the outcomes of these procedures. Based on these results, a two-step cleaning process, combining SC-1 at a reduced temperature at 30 ∘ C instead of 80 ∘ C and a subsequent UV-ozone cleaning directly prior to deposition of the metallization, is suggested to achieve the lowest residual contamination level.
- ItemThe Influence of the Composition of Ru100−xAlx (x = 50, 55, 60, 67) Thin Films on Their Thermal Stability(Basel : MDPI, 2017-3-10) Seifert, Marietta; Rane, Gayatri K.; Oswald, Steffen; Menzel, Siegfried B.; Gemming, ThomasRuAl thin films possess a high potential as a high temperature stable metallization for surface acoustic wave devices. During the annealing process of the Ru-Al films, Al2O3 is formed at the surface of the films even under high vacuum conditions, so that the composition of a deposited Ru50Al50 film is shifted to a Ru-rich alloy. To compensate for this effect, the Al content is systematically increased during the deposition of the Ru-Al films. Three Al-rich alloys—Ru45Al55, Ru40Al60 and Ru33Al67—were analyzed concerning their behavior after high temperature treatment under high vacuum and air conditions in comparison to the initial Ru50Al50 sample. Although the films’ cross sections show a more homogeneous structure in the case of the Al-rich films, the RuAl phase formation is reduced with increasing Al content.
- ItemRole of 1,3-dioxolane and LiNO3 addition on the long term stability of nanostructured silicon/carbon anodes for rechargeable lithium batteries(Pennington, NJ : ECS, 2016) Jaumann, Tony; Balach, Juan; Klose, Markus; Oswald, Steffen; Eckert, Jürgen; Giebeler, LarsIn order to utilize silicon as alternative anode for unfavorable lithium metal in lithium – sulfur (Li–S) batteries, a profound understanding of the interfacial characteristics in ether-based electrolytes is required. Herein, the solid electrolyte interface (SEI) of a nanostructured silicon/carbon anode after long-term cycling in an ether-based electrolyte for Li–S batteries is investigated. The role of LiNO3 and 1,3-dioxolane (DOL) in dimethoxy ethane (DME) solutions as typically used electrolyte components on the electrochemical performance and interfacial characteristics on silicon are evaluated. Because of the high surface area of our nanostructured electrode owing to the silicon particle size of around 5 nm and the porous carbon scaffold, the interfacial characteristics dominate the overall electrochemical reversibility opening a detailed analysis. We show that the use of DME/DOL solutions under ambient temperature causes higher degradation of electrolyte components compared to carbonate-based electrolytes used for Li–ion batteries (LIB). This behavior of DME/DOL mixtures is associated with different SEI component formation and it is demonstrated that LiNO3 addition can significantly stabilize the cycle performance of nanostructured silicon/carbon anodes. A careful post-mortem analysis and a discussion in context to carbonate-based electrolyte solutions helps to understand the degradation mechanism of silicon-based anodes in rechargeable lithium-based batteries.
- ItemLifetime vs. rate capability: Understanding the role of FEC and VC in high-energy Li-ion batteries with nano-silicon anodes(Amsterdam : Elsevier, 2016) Jaumann, Tony; Balach, Juan; Langklotz, Ulrike; Sauchuk, Viktar; Fritsch, Marco; Michaelis, Alexander; Teltevskij, Valerij; Mikhailova, Daria; Oswald, Steffen; Klose, Markus; Stephani, Guenter; Hauser, Ralf; Eckert, Jürgen; Giebeler, LarsFluoroethylene carbonate (FEC) and vinylene carbonate (VC) are the most frequently used electrolyte components to enhance the lifetime of anode materials in Li-ion batteries, but for silicon it is still ambiguous when FEC or VC is more beneficial. Herein, a nanostructured silicon/carbon anode derived from low-cost HSiCl3 is tailored by the rational choice of the electrolyte component, to obtain an anode material outperforming current complex silicon structures. We demonstrate highly reversible areal capacities of up to 5 mA h/cm2 at 4.4 mg/cm2 mass loading, a specific capacity of 1280 mA h/gElectrode, a capacity retention of 81% after 500 deep-discharge cycles versus lithium metal and successful full-cell tests with high-voltage cathodes meeting the requirements for real application. Electrochemical impedance spectroscopy and post-mortem investigation provide new insights in tailoring the interfacial properties of silicon-based anodes for high performance anode materials based on an alloying mechanism with large volume changes. The role of fluorine in the FEC-derived interfacial layer is discussed in comparison with the VC-derived layer and possible degradation mechanisms are proposed. We believe that this study gives a valuable understanding and provides new strategies on the facile use of additives for highly reversible silicon anodes in Li-ion batteries.
- ItemSEI-component formation on sub 5 nm sized silicon nanoparticles in Li-ion batteries: The role of electrode preparation, FEC addition and binders(Cambridge : Royal Society of Chemistry, 2015) Jaumann, Tony; Balach, Juan; Klose, Markus; Oswald, Steffen; Langklotz, Ulrike; Michaelis, Alexander; Eckert, Jürgen; Giebeler, LarsSilicon is a promising negative electrode for secondary lithium-based batteries, but the electrochemical reversibility of particularly nanostructured silicon electrodes drastically depends on their interfacial characteristics, commonly known as the solid electrolyte interface (SEI). The beneficial origin of certain electrolyte additives or different binders is still discussed controversially owing to the challenging peculiarities of interfacial post-mortem investigations of electrodes. In this work, we address the common difficulties of SEI investigations of porous silicon/carbon nanostructures and study the addition of a fluoroethylene carbonate (FEC) as a stabilizing additive as well as the use of two different binders, carboxymethyl cellulose/styrene-butadiene rubber (CMC/SBR) and polyacrylic acid (PAA), for the SEI formation. The electrode is composed of silicon nanocrystallites below 5 nm diameter allowing a detailed investigation of interfacial characteristics of silicon owing to the high surface area. We first performed galvanostatic long-term cycling (400 times) and carried out comprehensive ex situ characterization of the cycled nanocrystalline silicon electrodes with XRD, EDXS, TEM and XPS. We modified the preparation of the electrode for post-mortem characterization to distinguish between electrolyte components and the actual SEI. The impact of the FEC additive and two different binders on the interfacial layer is studied and the occurrence of diverse compounds, in particular LiF, Li2O and phosphates, is discussed. These results help to understand general issues in SEI formation and to pave the way for the development of advanced electrolytes allowing for a long-term performance of nanostructured Si-based electrodes.
- ItemStudy of TiAl thin films on piezoelectric CTGS substrates as an alternative metallization system for high-temperature SAW devices(Rio de Janeiro : Elsevier, 2021) Seifert, Marietta; Lattner, Eric; Menzel, Siegfried B.; Oswald, Steffen; Gemming, ThomasTi/Al multilayer films with a total thickness of 200 nm were deposited on the high-temperature (HT) stable piezoelectric Ca3TaGa3Si2O14 (CTGS) as well as on thermally oxidized Si (SiO2/Si) reference substrates. The Ti–Al films were characterized regarding their suitability as an alternative metallization for electrodes in HT surface acoustic wave devices. These films provide the advantage of significantly lower costs and in addition also a significantly lower density as compared to Pt, which allows a greater flexibility in device design. To realize a thermal stability of the films, AlNO cover as well as barrier layers at the interface to the substrate were applied. The samples were annealed for 10 h at up to 800 °C in high vacuum (HV) and at 600 °C in air and analyzed regarding the γ-TiAl phase formation, film morphology, and possible degradation. The Ti/Al films were prepared either by magnetron sputtering or by e-beam evaporation and the different behavior arising from the different deposition method was analyzed and discussed. For the evaporated Ti/Al films, AlNO barriers with a lower O content were used to evaluate the influence of the composition of the AlNO on the HT stability. The sputter-deposited Ti/Al films showed an improved γ-TiAl phase formation and HT stability (on SiO2/Si up to 800 °C in HV and 600 °C in air, on CTGS with a slight oxidation after annealing at 800 °C in HV) as compared to the evaporated samples, which were only stable up to 600 °C in HV and in air.