660 Technische Chemie
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Chemical and Structural Comparison of Different Commercial Food Supplements for Silicon Uptake
(2023)
Various food supplements for silicon uptake were compared in terms of their structures and chemical compositions. In particular, we analyzed the silanol group content, which can be an indicator of the uptake of the siliceous species in the human body. We analyzed the commercial products Original Silicea Balsam®, Flügge Siliceous Earth Powder, Pure Colloidal Silicon, and BioSil® by applying various methods such as FTIR, 29Si NMR, and TGA. The Si-OH group content of the samples containing pure silica was the highest for the Original Silicea Balsam followed by the Pure Colloidal Silicon. The siliceous earth powder revealed the lowest content of such groups and the densest structure. BioSil® contained a considerable concentration of organic molecules that stabilized orthosilicic acid. The study may help to understand the silicon uptake behavior of different food supplements depending on their chemical structure.
Ionic liquid mixtures show promise as electrolytes for supercapacitors with nanoporous electrodes. Herein, we investigate theoretically and with experiments how binary electrolytes comprising a common anion and two types of differently-sized cations affect capacitive energy storage. We find that such electrolytes can enhance the capacitance of single nanopores and nanoporous electrodes under potential differences negative relative to the potential of zero charge. For a two-electrode cell, however, they are beneficial only at low and intermediate cell voltages, while a neat ionic liquid performs better at higher voltages. We reveal subtle effects of how the distribution of pores accessible to different types of ions correlates with charge storage and suggest approaches to increase capacitance and stored energy density with ionic liquid mixtures.
Printed electronic paper identifies its interest in flexible organic electronics and sustainable and clean energy applications because of its straightforward production method, cost-effectiveness, and positive environmental impact. However, current limitations include restricted material thickness and the use of supporting substrate for printing. Here, 2D and 3D electronic patterned paper are fabricated from direct ink writing (DIW) nanocellulose and PEDOT:PSS-based materials using syringe deposition and 3D printing. The conductor patterns are integrated in the bulk of the paper, while non-conductive sections are used as support to form free-standing paper. The strong interface between the patterns of electronic patterned paper gives mechanical stability for practical handling. The conductive paper-based electrode has 202 S cm−1 and is capable of handling electric current up to 0.7 A, which can be used for high-power devices. Printed supercapacitor papers show high specific energy of 4.05 Wh kg−1, specific power of 4615 W kg−1 at 0.06 A g−1, and capacitance retention above 95% after 2000 cycles. The new design structure of electronic patterned papers presents a solution for additive manufacturing of paper-based composites for supercapacitors, wearable electronics, or sensors for smart packaging.
Microalloyed steels contain small quantities (≤ 0.5 wt%) of the microalloying elements Ti, Nb, V. Judicious combination of TMCP parameters and microalloyed steel composition leads to formation of desirable nm-sized carbide, nitride, carbonitride inclusions which improve steel mechanical properties. TMCP optimisation relies on understanding the interrelation between TMCP parameters and precipitate properties. A characterisation routine was developed in the group to provide statistically meaningful data on precipitates size distribution and chemical composition.[1] Precipitates with diameters below 10nm could not be investigated with the existing routine. Such precipitates are of interest because they play a key role in precipitation hardening. This thesis extends the existing characterisation routine to sub-10nm precipitates extracted from microalloyed steels. Electrolytic extraction was investigated as alternative extraction process to reduce undesired particle loss during chemical extraction. The suitability of various electrolytes to provide a stable colloidal suspension for colloidal analysis was assessed. Chemically extracted precipitates underwent differential centrifugation to isolate sub-10nm precipitates and enable their size and chemical composition characterisation. Improvements in precipitate analysis were achieved by implementation of speed-ramp analytical ultracentrifugation and precipitate number density determination.
As industrial and agricultural activities expand along with a growing global population, numerous regions are experiencing shortages of water and essential metals. To address these challenges, electrochemical separation methods utilizing electroactive materials and interfaces offer an efficient and straightforward approach to water purification and targeted ion extraction. Although carbon-based materials have been extensively studied and have the advantages of stability and low cost, they suffer from low desalination capacity, particularly for high-salinity water, and low selectivity. This dissertation investigates the potential of Faradaic materials and processes for electrochemical ion/water separation, as well as ion/ion separation, with a focus on alkali and alkaline earth metal ions, which are vital for industrial development but challenging to separate. The study includes synthesizing several Faradaic materials to achieve high ion removal capacity in seawater desalination. This work also develops a strategy to exploit the nuanced differences of ion intercalation kinetics in 2D material to achieve specific ion separation. The study also examines the selectivity and stability of LiFePO4 and presents new ways to optimize its performance. Finally, the study establishes a novel electrochemical process based on redox flow batteries, which promises a more efficient and continuous extraction of lithium ions from seawater.
In recent decades, a new type of electric energy storage system has emerged with the principle that the electric charge can be stored not only at the interface between the electrode and the electrolyte, but also in the electrolyte by the redox activities of the bulk electrolyte itself. Such redox electrolytes are promising for non-flow energy storage (redox electrolyte aided hybrid energy storage systems, REHES) particularly when they are combined with electrodes made of nanoporous carbon. In this PhD work, I have established a fundamental understanding regarding ion diffusion, process kinetics, and adsorption of redox ions. For that, different REHES systems have been investigated including tetrapropylammonium iodide, zinc iodide, potassium iodide, potassium ferricyanide, vanadyl sulfate, tin sulfate, and tin fluoride. The basic understanding of REHES systems enabled the targeted improvement of the device performance throughout this PhD work. Compared to the energy storage capacity of a conventional (non-redox) electrical double layer capacitor of 4 Wh/kg (ca. 80 F/g), the use of the ZnI2 redox electrolyte yielded significantly higher performance of up to 226 Wh/kg. Furthermore, the specific power was also enhanced from 1.3 kW/kg to 20 kW/kg. As a key conclusion, this PhD work demonstrates the high attractiveness of REHES systems not only from a performance point of view, but also regarding low cost and simplicity of the system.
Electrospun carbon hybrid fibers as binder-free electrodes for electrochemical energy storage
(2018)
There is a great need for the development and improvement of electrochemical energy storage devices for applications ranging from energy and power management to portable electronic devices. My work explores electrode materials for devices with higher energy storage capacity and rate handling, namely electrical double-layer capacitors, lithium-ion batteries, and sodium-ion batteries. To this end, I report the synthesis and properties of electrospun fiber mats composed of nanoporous carbon, transition metal oxide/carbon hybrid material, or silicon oxycarbide. Based on a comprehensive array of structural and chemical analysis and electrochemical benchmarking, this work evaluates the potential and drawbacks of electrospun materials as electrodes. Key findings demonstrate that electrospinning of molecular precursor is an attractive approach for the synthesis of carbon and hybrid fiber mats as free-standing electrodes. By following a one-pot synthesis approach, material properties such as phase composition, crystal structure, and phase distribution are well tuned to achieve the desired electrochemical properties. Compared to polymer-bound free-standing electrodes, the continuous fiber network yields a superior gravimetric electrochemical performance, related to the absence of additives and the continuous path for electron transport. However, the large interfiber space and low electrode density limit the usefulness of adopting electrospun fiber mats to size-sensitive applications
Supercapacitors are highly valued energy storage devices with high power density, fast charging ability, and exceptional cycling stability. A profound understanding of their charging mechanisms is crucial for continuous performance enhancement. Electrochemical quartz crystal microbalance (EQCM), a detection means that provides in situ mass change information during charging–discharging processes at the nanogram level, has received greatly significant attention during the past decade due to its high sensitivity, non-destructiveness and low cost. Since being used to track ionic fluxes in porous carbons in 2009, EQCM has played a pivotal role in understanding the charging mechanisms of supercapacitors. Herein, we review the critical progress of EQCM hitherto, including theory fundamentals and applications in supercapacitors. Finally, we discuss the fundamental effects of ion desolvation and transport on the performance of supercapacitors. The advantages and defects of applying EQCM in supercapacitors are thoroughly examined, and future directions are proposed.
Multiple principal element or high-entropy materials have recently been studied in the two-dimensional (2D) materials phase space. These promising classes of materials combine the unique behavior of solid-solution and entropy-stabilized systems with high aspect ratios and atomically thin characteristics of 2D materials. The current experimental space of these materials includes 2D transition metal oxides, carbides/carbonitrides/nitrides (MXenes), dichalcogenides, and hydrotalcites. However, high-entropy 2D materials have the potential to expand into other types, such as 2D metal-organic frameworks, 2D transition metal carbo-chalcogenides, and 2D transition metal borides (MBenes). Here, we discuss the entropy stabilization from bulk to 2D systems, the effects of disordered multi-valent elements on lattice distortion and local electronic structures and elucidate how these local changes influence the catalytic and electrochemical behavior of these 2D high-entropy materials. We also provide a perspective on 2D high-entropy materials research and its challenges and discuss the importance of this emerging field of nanomaterials in designing tunable compositions with unique electronic structures for energy, catalytic, electronic, and structural applications.
