Search Results
Mechanically Stable, Binder‐Free, and Free‐Standing Vanadium Trioxide/Carbon Hybrid Fiber Electrodes for Lithium‐Ion Batteries
2023, Bornamehr, Behnoosh, Gallei, Markus, Husmann, Samantha, Presser, Volker
Binder is a crucial component in present-day battery electrodes but commonly contains fluorine and requires coating processing using organic (often toxic) solvents. Preparing binder-free electrodes is an attractive strategy to make battery electrode production and its end-of-use waste greener and safer. Herein, electrospinning is employed to prepare binder-free and self-standing electrodes. Such electrodes often suffer from low flexibility, and the correlation between performance and flexibility is usually overlooked. Processing parameters affect the mechanical properties of the electrodes, and for the first time it is reported that mechanical flexibility directly influences the electrochemical performance of the electrode. The importance is highlighted when processing parameters advantageous to powder materials, such as a higher heat treatment temperature, harm self-standing electrodes due to deterioration of fiber flexibility. Other strategies, such as conductive carbon addition, can be employed to improve the cell performance, but their effect on the mechanical properties of the electrodes must be considered. Rapid heat treatment achieves self-standing V2O3 with a capacity of 250 mAh g−1 at 250 mA g−1 and 390 mAh g−1 at 10 mA g−1
Selective Pb2+ removal and electrochemical regeneration of fresh and recycled FeOOH
2023, Wang, Lei, Deligniere, Lexane, Husmann, Samantha, Leiner, Regina, Bahr, Carsten, Zhang, Shengjie, Dun, Chaochao, Montemore, Matthew M., Gallei, Markus, Urban, Jeffrey J., Kim, Choonsoo, Presser, Volker
Heavy metal pollution is a key environmental problem. Selectively extracting heavy metals could accomplish water purification and resource recycling simultaneously. Adsorption is a promising approach with a facile process, adaptability for the broad concentration of feed water, and high selectivity. However, the adsorption method faces challenges in synthesizing high-performance sorbents and regenerating adsorbents effectively. FeOOH is an environmentally friendly sorbent with low-cost production on a large scale. Nevertheless, the selectivity behavior and regeneration of FeOOH are seldom studied. Therefore, we investigated the selectivity of FeOOH in a mixed solution of Co2+, Ni2+, and Pb2+ and proposed to enhance the capacity of FeOOH and regenerate it by using external charges. Without charge, the FeOOH electrode shows a Pb2+ uptake capacity of 20 mg/g. After applying a voltage of −0.2/+0.8 V, the uptake capacity increases to a maximum of 42 mg/g and the desorption ratio is 70%–80%. In 35 cycles, FeOOH shows a superior selectivity towards Pb2+ compared with Co2+ and Ni2+, with a purity of 97% ± 3% in the extracts. The high selectivity is attributed to the lower activation energy for Pb2+ sorption. The capacity retentions at the 5th and the 35th cycles are ca. 80% and ca. 50%, respectively, comparable to the chemical regeneration method. With industrially exhausted granular ferric hydroxide as the electrode material, the system exhibits a Pb2+ uptake capacity of 37.4 mg/g with high selectivity. Our work demonstrates the feasibility of regenerating FeOOH by charge and provides a new approach for recycling and upcycling FeOOH sorbent. [Figure not available: see fulltext.]
Effect of cation size of binary cation ionic liquid mixtures on capacitive energy storage
2023, Seltmann, Anna, Verkholyak, Taras, Gołowicz, Dariusz, Pameté, Emmanuel, Kuzmak, Andrij, Presser, Volker, Kondrat, Svyatoslav
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.
Functional two-dimensional high-entropy materials
2023, Nemani, Srinivasa Kartik, Torkamanzadeh, Mohammad, Wyatt, Brian C., Presser, Volker, Anasori, Babak
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.
Best practice for electrochemical water desalination data generation and analysis
2023, Torkamanzadeh, Mohammad, Kök, Cansu, Burger, Peter Rolf, Ren, Panyu, Zhang, Yuan, Lee, Juhan, Kim, Choonsoo, Presser, Volker
Electrochemical desalination shows promise for ion-selective, energy-efficient water desalination. This work reviews performance metrics commonly used for electrochemical desalination. We provide a step-by-step guide on acquiring, processing, and calculating raw desalination data, emphasizing informative and reliable figures of merit. A typical experiment uses calibrated conductivity probes to relate measured conductivity to concentration. Using a standard electrochemical desalination cell with activated carbon electrodes, we demonstrate the calculation of desalination capacity, charge efficiency, energy consumption, and ion selectivity metrics. We address potential pitfalls in performance metric calculations, including leakage current (charge) considerations and aging of conductivity probes, which can lead to inaccurate results. The relationships between pH, temperature, and conductivity are explored, highlighting their influence on final concentrations. Finally, we provide a checklist for calculating performance metrics and planning electrochemical desalination tests to ensure accuracy and reliability. Additionally, we offer simplified spreadsheet tools to aid data processing, system design, estimations, and upscaling.
Growth of titania and tin oxide from Ti2SnC via rapid thermal oxidation in air for lithium-ion battery application
2023, Jolly, Shae, Husmann, Samantha, Presser, Volker, Naguib, Michael
Herein, we report the synthesis of TiO2–SnO2–C/carbide hybrid electrode materials for Li-ion batteries (LIBs) via two different methods of controlled oxidation of layered Ti2SnC. The material was partially oxidized in an open-air furnace (OAF) or using a rapid thermal annealing (RTA) approach to obtain the desired TiO2–SnO2–C/carbide hybrid material; the carbide phase encompassed both residual Ti2SnC and TiC as a reaction product. We tested the oxidized materials as an anode in a half cell to investigate their electrochemical performance in LIBs. Analysis of the various oxidation conditions indicated the highest initial lithiation capacity of 838 mAh/g at 100 mA/g for the sample oxidized in the OAF at 700°C for 1 h. Still, the delithiation capacity dropped to 427 mAh/g and faded over cycling. Long-term cycling demonstrated that the RTA sample treated at 800°C for 30 s was the most efficient, as it demonstrated a reversible capacity of around 270 mAh/g after 150 cycles, as well as a specific capacity of about 150 mAh/g under high cycling rate (2000 mA/g). Given the materials’ promising performance, this processing method could likely be applied to many other members of the MAX family, with a wide range of energy storage applications.
Continuous wet chemical synthesis of Mo(C,N,O)x as anode materials for Li-ion batteries
2023, Abdirahman Mohamed, Mana, Arnold, Stefanie, Janka, Oliver, Quade, Antje, Schmauch, Jörg, Presser, Volker, Kickelbick, Guido
Molybdenum carbides, oxides, and mixed anionic carbide–nitride–oxides Mo(C,N,O)x are potential anode materials for lithium-ion batteries. Here we present the preparation of hybrid inorganic–organic precursors by a precipitation reaction of ammonium heptamolybdate ((NH4)6Mo7O24) with para-phenylenediamine in a continuous wet chemical process known as a microjet reactor. The mixing ratio of the two components has a crucial influence on the chemical composition of the obtained material. Pyrolysis of the precipitated precursor compounds preserved the size and morphology of the micro- to nanometer-sized starting materials. Changes in pyrolysis conditions such as temperature and time resulted in variations of the final compositions of the products, which consisted of mixtures of Mo(C,N,O)x, MoO2, Mo2C, Mo2N, and Mo. We optimized the reaction conditions to obtain carbide-rich phases. When evaluated as an anode material for application in lithium-ion battery half-cells, one of the optimized materials shows a remarkably high capacity of 933 mA h g−1 after 500 cycles. The maximum capacity is reached after an activation process caused by various conversion reactions with lithium.
Thermo-Responsive Ultrafiltration Block Copolymer Membranes Based on Polystyrene-block-poly(diethyl acrylamide)
2023, Frieß, Florian V., Hartmann, Frank, Gemmer, Lea, Pieschel, Jens, Niebuur, Bart‐Jan, Faust, Matthias, Kraus, Tobias, Presser, Volker, Gallei, Markus
Within 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.
Interlaboratory study assessing the analysis of supercapacitor electrochemistry data
2023, Gittins, Jamie W., Chen, Yuan, Arnold, Stefanie, Augustyn, Veronica, Balducci, Andrea, Brousse, Thierry, Frackowiak, Elzbieta, Gómez-Romero, Pedro, Kanwade, Archana, Köps, Lukas, Jha, Plawan Kumar, Lyu, Dongxun, Meo, Michele, Pandey, Deepak, Pang, Le, Presser, Volker, Rapisarda, Mario, Rueda-García, Daniel, Saeed, Saeed, Shirage, Parasharam M., Ślesiński, Adam, Soavi, Francesca, Thomas, Jayan, Titirici, Maria-Magdalena, Wang, Hongxia, Xu, Zhen, Yu, Aiping, Zhang, Maiwen, Forse, Alexander C.
Supercapacitors are fast-charging energy storage devices of great importance for developing robust and climate-friendly energy infrastructures for the future. Research in this field has seen rapid growth in recent years, therefore consistent reporting practices must be implemented to enable reliable comparison of device performance. Although several studies have highlighted the best practices for analysing and reporting data from such energy storage devices, there is yet to be an empirical study investigating whether researchers in the field are correctly implementing these recommendations, and which assesses the variation in reporting between different laboratories. Here we address this deficit by carrying out the first interlaboratory study of the analysis of supercapacitor electrochemistry data. We find that the use of incorrect formulae and researchers having different interpretations of key terminologies are major causes of variability in data reporting. Furthermore we highlight the more significant variation in reported results for electrochemical profiles showing non-ideal capacitive behaviour. From the insights gained through this study, we make additional recommendations to the community to help ensure consistent reporting of performance metrics moving forward.
Prussian blue and its analogues as functional template materials: control of derived structure compositions and morphologies
2023, Bornamehr, Behnoosh, Presser, Volker, Zarbin, Aldo J. G., Yamauchi, Yusuke, Husmann, Samantha
Hexacyanometallates, known as Prussian blue (PB) and its analogues (PBAs), are a class of coordination compounds with a regular and porous open structure. The PBAs are formed by the self-assembly of metallic species and cyanide groups. A uniform distribution of each element makes the PBAs robust templates to prepare hollow and highly porous (hetero)nanostructures of metal oxides, sulfides, carbides, nitrides, phosphides, and (N-doped) carbon, among other compositions. In this review, we examine methods to derive materials from PBAs focusing on the correlation between synthesis steps and derivative morphologies and composition. Insights into catalytic and electrochemical properties resulting from different derivatization strategies are also presented. We discuss challenges in manipulating the derivatives' properties, give perspectives of synthetic approaches for the target applications and present an outlook on less investigated grounds in Prussian blue derivatives.