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The growing concern about the environment, associated with the continuous increase in the production of electronic equipment, such as computers, cell phones, mobile devices and consequently batteries, has induced research to develop new technologies to recycle the huge numbers of spent batteries generated in the last few years. The amount of spent NiMH batteries will tend to grow continually over the next few years. These batteries have in their chemical composition, valuable metals such as Ni, Co and rare earths. In the first stage of this work a characterization of NiMH batteries was done. Batteries from different brands and models were disembled and their components were characterized in relation to their chemical composition and main phases. In a second stage of this work, a sample of spent NiMH batteries was milled and the polymeric and metallic fractions were magnetically separated. The results obtained demonstrate that the recycling study, aimed at the recovery of Ni, Co and rare earths, is viable due to the great amount of these metals that are present batteries. It also demonstrates that magnetic separation is a very efficient process to recovery nickel alloys. However the effects of cadmium contamination (originating from fake batteries) will cause the recycling processes to be re-evaluated.
Carbon aerogel, carbon black and graphite were used to analyze the influence of conductive filler on the impedance behaviors of activated carbon based electric double layer capacitors (EDLCs). According to the electrochemical impedance spectrum (EIS) data, a new equivalent circuit model was proposed involving the kinetic characteristics of ion diffusion, furthermore, Marquardt fit procedure was applied to the EIS data to obtain the model parameter values. The results indicated that carbon aerogel could significantly decrease the resistance of EDLCs by increasing the diffusion coefficient of ions within electrodes and decreasing the interface resistance because of its suitable particle size, mesoporous structures and finely-branched particle performance.
The electrochemical behavior and the electrodeposition of dysprosium (Dy) in phosphonium-cation-based ionic liquid were investigated in this study. A new group of the room-temperature ionic liquids (RTILs) based on phosphonium cations with bis(trifluoromethylsulfonyl)amide anions was applied as novel electrolytic solutions. The cyclic voltammetric measurements resulted in one step reduction of the trivalent dysprosium ion in phosphonium-cation-based ionic liquid. On the other hand, no anodic peak ascribed to the oxidation of dysprosium metal was observed in this electroanalytical study. The diffusion coefficient and the activation energy for diffusion of the trivalent Dy complex in IL were estimated using semi-integral analysis, because it is important to analyze the diffusion properties to recover Dy through electrowinning methods. The diffusion coefficient of Dy(III) which was calculated to be 2.0 × 10−12 m2 s−1 at 25 °C, closed to that of the trivalent lanthanoid ion such as Eu(III) and Sm(III) in phosphonium-cation-based ionic liquid. In addition, the activation energy for diffusion was estimated to be 65 kJ mol−1 (0.5 M) and 49 kJ mol−1 (0.075 M). The estimated activation energy for diffusion was affected by the concentration of the electrolytic solution, since the RTILs had relatively strong electrostatic interactions between the metal cations and the solvent anions. Furthermore, the electrodeposition of Dy in phosphonium-cation-based IL was carried out using a two-electrode system constructed with a copper plate cathode and dysprosium metal anode. Energy dispersive X-ray analysis of electrodeposits showed a sharply peaked spectrum corresponding to the characteristic X-ray lines of Dy. In addition, the obtained Dy, with the exception of the surface layer, was confirmed to be in the metallic electronic state by X-ray photoelectron spectroscopy.
Hydrogen injection into and extraction from hydride-forming electrodes has been routinely investigated under the assumption that the electrode is homogeneous in structure and hydrogen transport through such electrodes is purely controlled by hydrogen diffusion. However, various kinds of abnormal behaviours in hydrogen transport, which could hardly be explained in terms of the diffusion-control model, have been quite frequently reported by many researchers. This review provides a comprehensive survey of the anomalous behaviours of hydrogen transport observed in such hydride-forming electrodes as Pd and metal-hydrides, with particular emphasis on hydrogen extraction under the impermeable boundary conditions during the potentiostatic current transient measurement involving the potential stepping. After a brief discourse on the conventional diffusion-control model, the topics related to the boundary conditions at the electrode surface during hydrogen extraction are extensively reviewed. In particular, it is shown that the diffusion-controlled constraint should be no longer valid at the electrode surface for hydrogen extraction in case hydrogen diffusion is influenced by either the interfacial charge transfer reaction or the hydrogen transfer reaction between adsorbed state on the electrode surface and absorbed state at the electrode sub-surface. Subsequently, the atypical behaviours of current transient due to hydrogen diffusion in the presence of traps and in the coexistence of two hydride phases are treated in detail. Each of the hydrogen extraction models suggested is discussed with the aid of the anodic current transients numerically calculated based upon the theoretical electrode potential curve, and then it is exemplified by hydrogen extraction from Pd and metal-hydrides in aqueous solutions.
A highly porous three-dimensional Ni–Sn alloy foam is fabricated by electro-deposition accompanied by hydrogen evolution reaction. This foam can evolve into porous and dendritic metal alloy structures. These Sn-based electrodes have been evaluated for use as anodes in lithium-ion batteries. Dendritic Ni50Sn50 alloy foam exhibits high electrochemical capacity and excellent cycle stability during charge–discharge processes. The nickel in a Ni–Sn alloy does not break off during the volume expansion/contraction sequence in battery operation cycles and supports the Sn remaining on the anodes. The voids in the tube-like porous Ni–Sn morphology enhance the mass transfer of Li+ ions and act as mechanical bumpers during the charge–discharge processes.
European national, regional, and local authorities have started to take action to make public bus transport services more effective and less polluting. Some see the possibility to move beyond a narrow focus on efficiency or carbon dioxide reductions towards an integrated sustainability perspective. This paper uses this perspective to build and test a new assessment approach that should enhance decisions on bus transport powertrains and energy carriers for Swedish medium-sized cities. The study suggests that a superiority of electric powertrains is revealed if a traditional economic analysis is integrated with a strategic sustainability perspective.
ABSTRACT Polymer electrolytes (PEs) have served as the focus of intensive research as new ion-conducting materials, especially for lithium battery applications. A new strategy to develop fast lithium-conducting PEs is reported here. The thermal, ionic transport, and electrochemical properties of polymer solutions in a glyme-Li salt solvate ionic liquid, [Li(G4)1][TFSA], composed of an equimolar mixture of lithium bis(trifluoromethanesulfonyl) amide (Li[TFSA]) and tetraglyme (G4), were characterized. Poly(ethylene oxide) (PEO), poly(methyl methacrylate) (PMMA), and poly(butyl acrylate) (PBA) were combined with [Li(G4)1][TFSA] in order to explore the effects of polymer structure on the properties. The self-diffusion coefficient ratio of the glyme and Li+ ions (D G/D Li) was investigated to evaluate the stability of the complex (solvate) cations. The D G/D Li values suggested that the [Li(G4)1]+ complex cations underwent a ligand exchange reaction between G4 and PEO in the PEO-based solution, whereas the cations remained stable (D G/D Li =1) in the PMMA- and PBA-based solutions. The robustness of the [Li(G4)1]+ complex cations in the PMMA- and PBA-based solutions was reflected in high weight-loss temperature, greater Li transference number, and high oxidative stability. Owing to the lower glass transition temperature and low affinity towards Li+ ions, the PBA-based solutions yielded superior lithium transport properties (ionic conductivity of 10−4∼10−3 Scm−1 and Li transference number as high as 0.5) among the investigated polymer solutions.
Layered Li1+x Ni0.30Co0.30Mn0.40O2 (x =0, 0.05, 0.10, 0.15) materials have been synthesized using citric acid assisted sol–gel method. The materials with excess lithium showed distinct differences in the structure and the charge and discharge characteristics. The rate capability tests were performed and compared on Li1+x Ni0.30Co0.30Mn0.40O2 (x =0, 0.05, 0.10, 0.15) cathode materials. Among these materials, Li1.10Ni0.30Co0.30Mn0.40O2 cathode demonstrated higher discharge capacity than that of the other cathodes. Upon extended cycling at 1C and 8C, Li1.10Ni0.30Co0.30Mn0.40O2 showed better capacity retention when compared to other materials with different lithium content. Li1.10Ni0.30Co0.30Mn0.40O2 exhibited 93 and 90% capacity retention where as Li1.05Ni0.30Co0.30Mn0.40O2, Li1.15Ni0.30Co0.30Mn0.40O2, and Li1.00Ni0.30Co0.30Mn0.40O2 exhibited only 84, 71, and 63% (at 1C), and 79, 66 and 40% (at 10C) capacity retention, respectively, after 40 cycles. The enhanced high rate cycleability of Li1.10Ni0.30Co0.30Mn0.40O2 cathode is attributed to the improved structural stability due to the formation of appropriate amount of Li2MnO3-like domains in the transition metal layer and decreased Li/Ni disorder (i.e., Ni content in the Li layer).
We prepared synthetic porous carbons with a three-dimensional interconnected network of ultramicroporous particles; by adjusting the synthesis parameters the size of these particles was systematically varied from 13nm to 1.4μm. Cyclic voltammetry measurements using a cavity microelectrode (CME) were performed in different chloric aqueous electrolyte solutions. The CME allows for very fast measurements (up to 10V/s) of carbon powders without the need of a binder or conductivity additive. Therewith we were able to investigate the accessibility of the ultramicropores and kinetics of the electrochemical double-layer (EDL) charging as a function of particle, inter-particular pore, effective ion and micropore size. We found, that the alkaline cations K+, Na+, Li+ and the anion Cl− can enter micropores down to a size of 0.4nm at slow charging rates independent of the particle size. However, the accessibility is decreased due to kinetic limitations for the cations Na+ and Li+ at higher scan rates, which was not observed for the smaller K+ ion. A simple model is presented, which explains the influence of the particle, inter-particular pore and micropore size on the kinetics of double-layer charging. This model suggests that first of all the carbon particle size is not a limiting factor for fast EDL charging as long as its size is smaller than a few hundred nanometers and secondly inter-particular pores with a size in the range of the particle size or larger are crucial for high-rate applications.
Li-rich layered oxide Li1.2Co0.13Ni0.13Mn0.54O2 has been successfully re-synthesized using the ascorbic acid leaching solution of spent lithium-ion batteries as the raw materials. A combination of oxalic acid co-precipitation, hydrothermal and calcination processes was applied to synthesize this material. For comparison, a fresh sample with the same composition has been also synthesized from the commercial raw materials using the same method. X-ray diffraction (XRD), scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS) and electrochemical measurements are carried out to characterize these samples. XRD results indicate that both samples have the layered α-NaFeO2 structures with a space group of R 3 ¯ m. No other crystalline phase was detected by XRD. The electrochemical results show that the re-synthesized and fresh-synthesized sample can deliver discharge capacities as high as 258.8 and 264.2 mAh g−1 at the first cycle, respectively. After 50 cycles, discharge capacities of 225.1 and 228 mAh g−1 can be obtained with capacity retention of 87.0 and 86.3%, respectively. This study suggests that the leaching solution from spent lithium ion batteries can be recycled to synthesize Li-rich cathode materials with good electrochemical performance.
Lithium-rich layered oxides (LLOs) are considered promising cathode materials for lithium-ion batteries because of their high reversible capacity, which is attributed to the exploitation of the novel anionic redox in addition to the conventional cationic redox process. Transition metal (TM) migration, which is known to be the main cause of the voltage decay in LLOs, is now understood to also be the critical factor triggering anionic redox, although this origin is still under debate. A better understanding of the specific TM migration behavior and its effect during charge/discharge would thus enable further development of this class of materials. Herein, we demonstrate that the unique TM migration during charge/discharge significantly alters the lithium diffusion mechanism/kinetics of LLO cathodes. We present clear evidence of the much more sluggish lithium diffusion occurring during discharge (lithiation) than during charge (de-lithiation), which contrasts with the traditional lithium diffusion model based on simple topotactic lithium intercalation/deintercalation in the layered framework. The reversible but asymmetric TM migration in the structure, which originates from the non-equivalent local environments around the TM during the charge and discharge processes, is shown to affect the lithium mobility. This correlation between TM migration and lithium mobility led us to propose a new lithium diffusion model for layered structures and suggests the importance of considering TM migration in designing new LLO cathode materials.
The dispersion properties of carbon black (CB) slurries as well as the accompanying electrochemical properties of Li(Ni1/3Co1/3Mn1/3)O2 (NCM) electrodes were investigated by controlling the amine value of polyurethane-based dispersants. The increase in amine value of dispersants leads to an increase in adsorption level on CB surface due to a strong acid/base interaction between dispersants and CB particles, providing the improvement of steric repulsion between particles at the solid–liquid interface. This results in the enhancement of the dispersion stability of CB and the related microstructure of the electrodes. Electrochemical experiments indicated that the rate capabilities and cycle performance of the electrodes are in good agreement with dispersion properties of CB slurries. However, it was found that the excessive addition of the dispersant was deleterious to electrochemical properties because the non-adsorbed dispersants act as an electronic conduction barrier between solid phases. Therefore, it is suggested that the amine value of dispersant and tailored amount of dispersant addition can be key roles for obtaining the optimized dispersion stability of CB and the corresponding excellent electrochemical properties of the cathode.
This paper reports the wireless Shape-Memory-Polymer actuator operated by external radio frequency magnetic fields and its application in a drug delivery device. The actuator is driven by a frequency-sensitive wireless resonant heater which is bonded directly to the Shape-Memory-Polymer and is activated only when the field frequency is tuned to the resonant frequency of heater. The heater is fabricated using a double-sided Cu-clad Polyimide with much simpler fabrication steps compared to previously reported methods. The actuation range of 140 μm as the tip opening distance is achieved at device temperature 44 °C in 30 s using 0.05 W RF power. A repeatability test shows that the actuator’s average maximum displacement is 110 μm and standard deviation of 12 μm. An experiment is conducted to demonstrate drug release with 5 μL of an acidic solution loaded in the reservoir and the device is immersed in DI water. The actuator is successfully operated in water through wireless activation. The acidic solution is released and diffused in water with an average release rate of 0.172 μL/min.
Lithium-sulfur (Li-S) batteries have attracted extensive interest due to their higher theoretical energy density than the current commercial lithium-ion batteries. However, their practical application is largely hindered by the low sulfur utilization and poor cycling stability. Restraining the shuttle effect and enhancing the electrochemical kinetics are important for developing high-performance Li-S batteries. Here we use carbon nanofibers (CNFs) supported manganese dioxide (MnO2) composite as a bifunctional coating on sulfur cathode for anchoring polysulfides and accelerating their redox reactions simultaneously. The CNFs/MnO2 composite supplies fast paths for electron transfer and ion diffusion, and greatly promotes the transformation processes of polysulfides to Li2S/Li2S2, leading to an enhanced electrochemical kinetics. The diffusion coefficient of lithium ion has been increased by 560%. As a result, the CNFs/MnO2 composite covered electrode exhibits an excellent cycling stability, its specific capacity maintains at about 600 mAh g−1 at 1C after 400 cycles, corresponding to a capacity decay as low as 0.063% per cycle, and the average coulombic efficiency reaches up to 99.66%.
An accurate state of charge (SoC) estimation of a traction battery in hybrid electric non-road vehicles, which possess higher dynamics and power densities than on-road vehicles, requires a precise battery cell terminal voltage model. This paper presents a novel methodology for non-linear system identification of battery cells to obtain precise battery models. The methodology comprises the architecture of local model networks (LMN) and optimal model based design of experiments (DoE). Three main novelties are proposed: 1) Optimal model based DoE, which aims to high dynamically excite the battery cells at load ranges frequently used in operation. 2) The integration of corresponding inputs in the LMN to regard the non-linearities SoC, relaxation, hysteresis as well as temperature effects. 3) Enhancements to the local linear model tree (LOLIMOT) construction algorithm, to achieve a physical appropriate interpretation of the LMN. The framework is applicable for different battery cell chemistries and different temperatures, and is real time capable, which is shown on an industrial PC. The accuracy of the obtained non-linear battery model is demonstrated on cells with different chemistries and temperatures. The results show significant improvement due to optimal experiment design and integration of the battery non-linearities within the LMN structure.
Amorphous nitrogen-doped carbon nanosheets was synthesized through thermal decomposition of ethylenediaminetetraacetic acid manganese disodium salt hydrate (C10H12N2O8MnNa2⿿2H2O). The as-synthesized nitrogen-doped carbon nanosheets were characterized by X-ray diffraction, scanning electron microscopy, transition electron microscopy and X-ray photoelectron spectroscopy. The N content of the as-synthesized carbon nanosheets could reach as high as 11.77at.%, with an especially high total of 7.94at.% pyridinic N pluspyrrolic N. When tested as anode material for lithium ion batteries, the optimized carbon nanosheets exhibited high capacity, excellent rate capability, and stable cyclability over 600 cycles. The specific capacity was still as high as 465.8mAhg⿿1 at 0.5C after 600 cycles,with a capacity decay from the 2nd cycle of 0.05% per cycle over 599 cycles. The excellent performance of C-600 is attributed to a synergistic effect of high surface area, numerous nanopores, high thermal stability, and low charge transfer resistance.
Nanosized MnO2 powders were grown using a green synthesis based on citrates via redox reaction between KMnO4 and natural reducing agents, i.e. lemon juice and peel extracts, without generating hazardous waste. X-ray diffraction (XRD) and Raman studies show that the samples grow as cryptomelane polymorph, α-MnO2, crystallized with the tetragonal cryptomelane structure. Both J-MnO2 prepared from lemon juice and P-MnO2 prepared from citrus peel consist of nanosized particles as observed by scanning electron microscopy (SEM) and transmission electron microscopy (TEM). Thermogravimetric analysis (TGA) confirms the typical thermal decomposition of MnO2 at temperatures of up to 500 °C. Improved electrochemical properties are obtained and discussed for P-MnO2, with a reversible capacity that reaches 160 mAh g−1 (initial capacity of 212 mAh g−1) at a current density of 10 mA g−1 and a good rate capability.
An efficient one-pot method for the synthesis of organic disulfides from aryl and alkyl halides and potassium sulfide has been described. K2S acts as an inexpensive and readily available sulfur source. A variety of symmetric diaryl and dialkyl disulfides was prepared in good to excellent yields using NiCl2·6H2O and acetylacetone as the catalytic system.
Electrodeposited crystalline Cu2Sb thin films are studied to evaluate the use of these electrodes as model systems for studying Cu2Sb as a lithium ion battery anode material. The films have been characterized with an emphasis on determining the film quality and relating the structure, composition, and morphology to the resulting electrochemical and morphological transformations that occur during electrochemical lithiation and delithiation. It is shown that electrodeposition can produce high quality films that are devoid of major defects and can be used to provide mechanistic insight on the electrochemistry of reversible lithium alloying. The CuxSb films show that the fundamental reaction mechanism remains largely unchanged for copper concentrations of 1>x>3. For the first time we show that the copper concentration greatly affects critical criteria for anode materials such as the initial coulombic efficiency and reversible capacity of the electrode material. Voltage limit experiments show that an overpotential is required to remove trapped lithium states. Additional ex-situ experiments reveal that internal strain created during the lithiation process is relieved by buckling, greatly altering the film surface area and geometry, and resulting in the formation of cracks upon delithiation. This process is only semi-reversible, and strained areas remain visible even when discharged outside the voltage window of Cu2Sb determined by differential capacity plots. The results presented here indicate that these electroplated thin films are useful as analytical tools for showing pathways to improving the performance and fundamental understanding of alloy based lithium-ion battery anodes.