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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
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.
Layered Nano‐Mosaic of Niobium Disulfide Heterostructures by Direct Sulfidation of Niobium Carbide MXenes for Hydrogen Evolution
2022, Husmann, Samantha, Torkamanzadeh, Mohammad, Liang, Kun, Majed, Ahmad, Dun, Chaochao, Urban, Jeffrey J., Naguib, Michael, Presser, Volker
MXene-transition metal dichalcogenide (TMD) heterostructures are synthesized through a one-step heat treatment of Nb2C and Nb4C3. These MXenes are used without delamination or any pre-treatment. Heat treatments accomplish the sacrificial transformation of these MXenes into TMD (NbS2) at 700 and 900 °C under H2S. This work investigates, for the first time, the role of starting MXene phase in the derivative morphology. It is shown that while treatment of Nb2C at 700 °C leads to the formation of pillar-like structures on the parent MXene, Nb4C3 produces nano-mosaic layered NbS2. At 900 °C, both MXene phases, of the same transition metal, fully convert into nano-mosaic layered NbS2 preserving the parent MXene's layered morphology. When tested as electrodes for hydrogen evolution reaction, Nb4C3-derived hybrids show better performance than Nb2C derivatives. The Nb4C3-derived heterostructure exhibits a low overpotential of 198 mV at 10 mA cm−2 and a Tafel slope of 122 mV dec−1, with good cycling stability in an acidic electrolyte.
Mixed Cu-Fe Sulfides Derived from Polydopamine-Coated Prussian Blue Analogue as a Lithium-Ion Battery Electrode
2022, Bornamehr, Behnoosh, Presser, Volker, Husmann, Samantha
Batteries 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.
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.
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.]
Structural and chemical characterization of MoO2/ MoS2 triple-hybrid materials using electron microscopy in up to three dimensions
2021, Frank, Anna, Gänsler, Thomas, Hieke, Stefan, Fleischmann, Simon, Husmann, Samantha, Presser, Volker, Scheu, Christina
This work presents the synthesis of MoO2/MoS2core/shell nanoparticles within a carbon nanotube networkand their detailed electron microscopy investigation in up to three dimensions. The triple-hybrid core/shellmaterial was prepared by atomic layer deposition of molybdenum oxide onto carbon nanotube networks,followed by annealing in a sulfur-containing gas atmosphere. High-resolution transmission electronmicroscopy together with electron diffraction, supported by chemical analysisviaenergy dispersive X-ray and electron energy loss spectroscopy, gave proof of a MoO2core covered by few layers of a MoS2shell within an entangled network of carbon nanotubes. To gain further insights into this complexmaterial, the analysis was completed with 3D electron tomography. By usingZ-contrast imaging, distinctreconstruction of core and shell material was possible, enabling the analysis of the 3D structure of thematerial. These investigations showed imperfections in the nanoparticles which can impact materialperformance,i.e.for faradaic charge storage or electrocatalysis.