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We present the first results of experiments on the electrochemically driven alloying and de-alloying of Au substrates with Li-ions from organic electrolytes studied by in situ X-ray diffraction employing synchrotron radiation. Au(111) single crystals, 111-textured thin Au films and nanometer-sized Au particles on highly oriented pyrolytic graphite (HOPG) have been examined using a specially designed in situ X-ray cell. Starting from single crystalline Au systems we could follow the structural degradation and pulverization under different electrochemical conditions. Reciprocal lattice space maps show the occurrence of powder-like intensity associated with different Li–Au alloy phases. The diffraction data from the bulk Au crystals are compared with the Au(111) thin films and the behavior of the Au nano-particles on HOPG.
Carbon coated Li3Cr2(PO4)3/C model materials were synthesized by a sol-gel route and a solid state route with calcination at 800°C under an inert atmosphere. The model materials were characterized by X-ray diffraction (XRD), neutron powder diffraction (NPD), scanning electron microscopy (SEM), laser diffraction analysis (granulometry) and thermogravimetric analysis (TGA). The electrochemical signatures obtained for the solid state (carbon coated) route synthesized compounds revealed the presence of two redox couples, Cr3+/Cr2+ and Cr4+/Cr3+, between 1.5–2.5 V and 4.0‐4.9 V vs. Li+/Li, respectively. The model materials show an initial specific charge (for lithiation) of 131mAh g−1 (sol-gel, carbon coated) and 119mAh g−1 (solid state, carbon coated), which decreases to 90mAh g−1 and 46mAh g−1, respectively, after 100 cycles. Operando XRD measurements revealed reversible structural changes in the crystal structure upon cycling, leading to the conclusion of an insertion reaction mechanism.
Flow batteries utilizing a plating reaction as the negative reaction are limited in energy capacity by the available void area in the cell stack. Large scale energy storage applications necessitate maximizing the plating density within the flow battery. Six porous negative electrode configurations using conductive and non-conductive materials are considered for use in a hybrid flow battery. Plating results using a Cu–Fe sulfate chemistry demonstrated a plating density in a carbon felt electrode (145 mAh cm−2 at 40 mA cm−2). Two layered electrode configurations were able to achieve 150 mAh cm−2 of plating density: carbon felt with non-conductive felt, and carbon felt-Daramic-carbon felt. Both electrode designs were tested with the all-iron chemistry using shallow charge/discharge cycles. The carbon felt with non-conducting felt electrode configuration maintained a voltaic efficiency of 81% over six cycles.
Electrodeposition methods were developed for the fabrication of Si composite anodes with nickel micro-nanocones hierarchical structure (MHS) current collectors for Li secondary batteries. This unique structured nickel current collector is electrodeposited in a simple process to create a complex high surface area conductive substrate, as well as to enhance the interfacial strength between active materials and substrate during cyclic lithiation/delithiation. The MHS supported Si composite anode demonstrated outstanding Li+ storage properties with reversible capacity over 800mAhg−1 (600μAhcm−2) after 100th cycle with superior retention of 99.6% per cycle. The improved performance of nickel MHS supported Si thick films indicate the potential for their application as electrode materials for high performance energy storage.
The correlation between state of charge (SoC) and open-circuit voltage (OCV) is a crucial characteristic parameter in many aspects of the battery management system (BMS). However, it is a challenging task to obtain the accurate SoC-OCV correlation with a high test efficiency. In this paper, an improved OCV characterization test is proposed to actively reduce the polarization voltage. Based on the third-order equivalent circuit model (ECM), two sets of current pulses are applied to accelerate the convergence of the battery terminal voltage, thus the test time is effectively shortened compared to the conventional incremental OCV characterization test. Furthermore, the parametric sensitivity of the imposed current excitation to battery model parameters is analyzed. Subsequently, the parametric determination method for the imposed current excitation is provided. Experiments are conducted on a lithium-ion polymer battery to prove the feasibility of the proposed test procedure. Comparison with the conventional OCV characterization test further demonstrated the superiority of the proposed test procedure.
Carbon coated LiNi0.5Mn1.5O4/C composite has been directly synthesized at 800 °C without using reducing gas or introducing additional low temperature treatments. Scanning/transmission electron microscope (S/TEM) observation shows clear coating layer on the particle's surface, which has been verified by Energy Dispersive X-Ray Spectroscopy (EDX), Raman spectra and Brunauer–Emmett–Teller (BET); and the results indicate the coating layer is amorphous carbon which significantly increases the BET surface area, and the carbon content is around 0.6 wt%. Unlike conventional low temperature coating process, the high temperature carbon coating process puts significant influence on the crystal structure in terms of degree of cation ordering and Mn3+ concentration. The LiNi0.5Mn1.5O4/C exhibits improved rate capability, smaller polarization and better cyclic performances at high rates. These improvements can be attributed to the conductive carbon layer with better chemical stability, as well as the smaller concentration of Mn3+ resulted from the high temperature coating process.
LiMn2O4 epitaxial thin films were synthesized on SrTiO3:Nb(111) and Al2O3(001) single crystal substrates by pulsed laser deposition (PLD) method and the electrochemical properties were discussed comparing with that of amorphous LiMn2O4 film on polycrystalline Au substrate. LiMn2O4 epitaxial film showed only a single plateau in charge–discharge curves and a single redox peak at the corresponding voltage of cyclic voltammograms. This phenomenon seems to originate from the effect of the epitaxy: the film is directly connected with the substrate by the chemical bond and this connection would suppress the phase transition of Li x Mn2O4 film during lithium (de-)intercalation. The discharge voltage of LiMn2O4 epitaxial film on SrTiO3 was lower than that of LiMn2O4 film on Al2O3. This lowered discharge voltage may be caused by the electronic interaction between LiMn2O4 film and SrTiO3:Nb n-type semiconductor substrate. We also attempted to measure the absorption spectrum change of LiMn2O4 epitaxial film on Al2O3 during the lithium (de-)intercalation. The absorption spectrum of LiMn2O4 hardly changed during charging and discharging. This suggests the d orbital of Mn does not concern the 4V region redox of LiMn2O4.
Carbon impression and the growing reliance on fossil fuels are two unique concerns for world emission regulatory agencies. These issues have placed electric vehicles (EVs) powered by lithium-ion batteries (LIBs) on the forefront as alternative vehicles. The LIB has noticeable features, including high energy and power density, compared with other accessible electrochemical energy storage systems. However, LIB is exceedingly nonlinear and dynamic; therefore, it generally requires an accurate online state-of-charge (SOC) estimation algorithm for real-time applications. Accurate battery modelling is an essential and primary requirement of online SOC estimation to simulate the dynamics. In this paper, different modelling methods suitable for online SOC estimation are discussed, and four groups of available online SOC estimation approaches are reviewed. After the general survey, the study explores the available Kalman filter (KF) family algorithms suitable for model-based online SOC estimation. The mathematical process and limitations of different KF family algorithms are analysed in depth and discussed. Moreover, challenging steps in the implementation of KF family algorithms in model-based online SOC estimation processes, such as selection of battery model, initial SOC and filter tuning, are elaborated for the efficient development of a battery management system, especially for EV application. The on-going research is propelled by KF-based online SOC estimation approaches distinctly emphasised through reviewing various studies for future research progression.
Herein, a new and facile synthesis of a tin-carbon nanocomposite and its electrochemical characterization is presented. Tin nanoparticles were embedded in micron-sized carbonaceous particles, thus successfully preventing the aggregation of tin nanoparticles and buffering the occurring volume strain, which accompanies the reversible (de-)alloying process. Such active material presents specific capacities of around 440 and 390mAhg−1 for applied specific currents of 0.1 and 0.2Ag−1, respectively, as lithium-ion anode using environmentally friendly and cost-efficient carboxymethyl cellulose as binder. Even more remarkably, at very high specific currents of 2, 5, and 10Ag−1, electrodes based on this composite still offer specific capacities of about 280, 240, and 187mAhg−1, respectively. In addition, this tin-carbon nanocomposite appears highly promising as anode material for sodium-ion batteries, showing very stable cycling performance in a suitable potential range, and specific capacities of more than 180, 150, 130, and 90mAhg−1 for an applied specific current of 12.2, 122, 244, and 610mAg−1, respectively, thus highlighting the high versatility of this composite active material for both Li-ion and Na-ion battery technologies.
Using 15O-water 3D positron emission tomography we investigated the effect of training in orientation discrimination upon cerebral activity in healthy human adults. When subjects are trained in this discrimination task, they learn the visuo-motor stimulus-response association required by the task and they increase their perceptual abilities in orientation discrimination. The present study was designed to investigate the rCBF modifications related to both these learning processes induced by training in orientation discrimination. PET data were acquired on two separate days (before and after training). Comparing the activation pattern related to orientation discrimination before and after the training period we observed activity decreases located in the left cerebellar cortex, in the right precentral gyrus and bilaterally in the fusiform gyri. The only region showing an activity increase was located in the body of the right caudate nucleus. These findings confirm the role of the neostriatum in skill learning and highlight the importance of mechanisms resulting in cortical and cerebellar neuronal activity decreases in this type of learning.
The discharge behaviour of Mg-Al-Pb and Mg-Al-Pb-In alloys in 3.5wt.% NaCl solution is investigated by electrochemical techniques, and compared with that of pure magnesium. The results show that Mg-Al-Pb-In alloy provides a more negative potential and exhibits a higher utilization efficiency in contrast with Mg-Al-Pb alloy and pure magnesium during the half-cell test at a large current density, and gives desirable discharge performance when used as anode for Mg- air battery. The peak power density of the Mg-air battery with Mg-Al-Pb-In anode is 94.5mW cm−2, which is comparable with those of Mg-H2O2 semi-fuel batteries. Moreover, the activation mechanism of Mg-Al-Pb-In alloy during the discharge process is also analyzed.
Sulfur is a promising cathode material with a high theoretical capacity of 1672 mAh g−1, but the challenges of the low electrical conductivity of sulfur and the high solubility of polysulfide intermediates still hinder its practical application. In this work, we design and synthesize a special carbon black nanoparticle–sulfur composite cathode material (NCB-S@NCB) with a novel structure and a high sulfur content of 84 wt% for lithium–sulfur battery application. The NCB-S@NCB composite cathode delivers a high initial discharge capacity of 1258 mAh g−1 and still maintains a reversible capacity of 865 mAh g−1 after 100 cycles with a relatively constant Coulombic efficiency around 98.0%.
Polypyrrole (Ppy) was successfully introduced into methyl substituted sulfonated poly(ether ether ketone) (SPEEK) membranes by polymerization in SPEEK solutions to improve their methanol resistance. Uniform polypyrrole (Ppy) distributed composite membranes were formed by this method by the interaction between SPEEK and Ppy. The properties of the composite membranes were characterized in detail. The composite membranes show very good proton conductive capability (25°C: 0.05–0.06scm−1) and good methanol resistance (25°C: 5.3×10−7–1.1×10−6 cm2 s−1).The methanol diffusion coefficients of composite membranes are much lower than that of pure SPEEK membranes (1.5×10−6 cm2 s−1). The composite membranes show very good potential usage in direct methanol fuel cells (DMFCs).
Guidance of cells and tissue sheets is an essential function in developing and differentiating animal tissues. In Hydra, where cells and tissue move dynamically due to constant cell proliferation towards the termini or into lateral, vegetative buds, factors essential for guidance are still unknown. Good candidates to take over this function are fibroblast growth factors (FGFs). We present the phylogeny of several Hydra FGFs and analysis of their expression patterns. One of the FGFs is expressed in all terminal regions targeted by tissue movement and at boundaries crossed by moving tissue and cells with an expression pattern slightly differing in two Hydra strains. A model addressing an involvement of this FGF in cell movement and morphogenesis is proposed: Hydra FGFf-expressing cells might serve as sources to attract tissue and cells towards the termini of the body column and across morphological boundaries. Moreover, a function in morphogenesis and/or differentiation of cells and tissue is suggested.
Fuel cells is a rapidly evolving technology with applications in many industries including transportation, and both portable and stationary power generation. The viability, efficiency and robustness of fuel-cell systems depend strongly on optimization and control of their operation. This paper presents the development of an integrated optimization and control tool for Proton Exchange Membrane Fuel-Cell (PEMFC) systems. Using a detailed simulation model, a database is generated first, which contains steady-state values of the manipulated and controlled variables over the full operational range of the fuel-cell system. In a second step, the database is utilized for producing Radial Basis Function (RBF) neural network “meta-models”. In the third step, a Non-Linear Programming Problem (NLP) is formulated, that takes into account the constraints and limitations of the system and minimizes the consumption of hydrogen, for a given value of power demand. Based on the formulation and solution of the NLP problem, a look-up table is developed, containing the optimal values of the system variables for any possible value of power demand. In the last step, a Model Predictive Control (MPC) methodology is designed, for the optimal control of the system response to successive sep-point changes of power demand. The efficiency of the produced MPC system is illustrated through a number of simulations, which show that a successful dynamic closed-loop behaviour can be achieved, while at the same time the consumption of hydrogen is minimized.
In this work, an iron-based alkaline battery using the same redox-active element featuring different coordination chemistries is developed and tested. The battery achieves a significantly low active material cost per kilowatt hour ($22 kW h−1) due to the inherently inexpensive price and availability of iron oxide and iron ferricyanide, particularly when compared with state-of-the-art vanadium redox flow batteries ($118 kW h−1) or the commercialized nickel cadmium battery ($51 kW h−1). Experimental results show that the present battery creates an equilibrium cell potential of 1.2 V and its coulombic efficiency reaches as high as 99% at a current density higher than 4 mA cm−2. Moreover, the energy efficiency can be maintained above 76% and the capacity decay rate is only 0.15% per cycle at a current density of 2 mA cm−2 over 150 cycles. With these advantages, the battery offers a promising solution for low-cost energy storage applications.
In this paper we report in situ Surface-Enhanced Raman Scattering (SERS) experiments carried out during the electrochemical deposition of gold from Au(I) cyanocomplexes in the room-temperature ionic liquid (RTIL) 1-ethyl-3-methyl-imidazolium bis(trifluoromethylsulfonyl) amide ([EMIm][TFSA]). The obtained SERS spectra indicated the co-adsorption of CN− and both anions and cations of the RTIL in the range from −1.8 to +0.3V vs. an Au quasi-reference electrode (QRE). The surface CN− peak exhibits a Stark tuning of ca. 28cm−1 V−1. The oxidation of CN− to OCN− was observed at potentials more anodic than 0.3V. The study was complemented by cyclic voltammetry, pinpointing RTIL reactivity at an Au electrode as well as CN− adsorption effects and Au(I) reduction. SEM observations allowed to identify the conditions for the achievement of continuous Au films as well as the morphological peculiarities of Au electrodeposited from [EMIm][TFSA]. XPS measurements proved that no RTIL is incorporated into the Au film, under the investigated conditions.
While entrepreneurial activity has been an important force for social and ecological sustainability; its efficacy is dependent upon the nature of market incentives. This limitation is sometimes explained by the metaphor of the prisoner's dilemma, which we term the green prison. In this prison, entrepreneurs are compelled to environmentally degrading behavior due to the divergence between individual rewards and collective goals for sustainable development. Entrepreneurs, however, can escape from the green prison by altering or creating the institutions—norms, property rights, and legislation—that establish the incentives of competitive games. We provide a variety of evidence of such entrepreneurial action and discuss its implications for theory and practice.
This study covers phase IV of a prospective clinical long-term study. Objective of this clinical investigation was to analyze the effects of a long-term prevention program on dental and oral health of teenagers at the age of 13 to 14 years. The entire study was subdivided into four phases. Phase I comprised an individual preventive care during pregnancy (“primary-primary prevention”); phase II assessed mothers and their young children until the age of 3 years (“primary prevention”); and in phase III, mothers and children at the age of 6 years were investigated. In phase IV of the study, the oral health of 13- to 14-year-old teenagers was examined (13.4 ± 0.5 years; n = 29). All phases consisted of an examination, education about oral health care, and treatment based on the concept of an early oral health care promotion. The control group consisted of randomly selected adolescents at the same age (n = 30). The following clinical parameters were assessed: decayed/missing/filled teeth (DMF-T)/decayed, missing, and filled surface teeth index, hygiene index, papilla bleeding index, Periodontal Screening Index, and Streptococcus mutans/Lactobacillus concentration in saliva. The teenagers of the “prevention” group of phase IV of our prospective study revealed a share of 89.7% caries-free dentitions (65.5% sound; 24.2% caries-free with fillings). Mean DMF-T was 0.55 ± 1.0. The control group showed a significantly higher mean DMF-T of 1.5 ± 1.5 (p < 0.05) and revealed 56.7% of caries-free dentitions (30% sound, 26.7% caries-free with restorations). Our data clearly document that an early oral health care promotion starting during pregnancy may cause a sustained and long-term improvement of the oral health of children.
Electrochemical performance and structural properties of the high-voltage cathode material Li2CoPO4F have been investigated. The cyclic voltammetry and coulometry under potential step mode in the voltage range 3.0–5.1V vs. Li revealed a structural transformation at potentials above 4.8V. This transformation occurring upon Li-extraction appears to be irreversible: the subsequent Li-insertion does not result in restoration of the initial structure, but takes place within a new “modified” framework. According to the structure refinement this modification involves the mutual rotations of (CoO4F2) octahedra and (PO4) tetrahedra accompanied by the considerable unit cell expansion which is expected to enhance the Li-transport upon subsequent cycling. The new framework demonstrates a reversible Li-insertion/extraction in a solid-solution regime with stabilized discharge capacity at around 60mAhg−1.
Polysiloxane multilayers were covalently bonded to the surface of natural graphite particles via diazonium chemistry and silylation reaction. The as-prepared graphite exhibited excellent discharge–charge behavior as negative electrode materials in lithium ion batteries. The improvement in the electrochemical performance of the graphite electrodes was attributed to the formation of a stable and flexible passive film on their surfaces. It was also revealed that the chemical compositions of the multilayers exerted influence on the electrochemical behavior of the graphite electrodes. The result of this study presents a new strategy to the formation of elastic and strong passive film on the graphite electrode via molecular design. Owing to the diversity of polysilxoane multilayers, this method also enables researchers to control the surface chemistries of carbonaceous materials with flexibility.
A Silicon-carbon composite with high silicon content is prepared via an easy and scalable approach and evaluated as anode material for lithium-ion batteries. Electrodes are manufactured using an aqueous binder, namely lithiated Poly(acrylic acid). High mass loading electrodes having areal capacities of over 3mAh/cm2 are obtained. The electrochemical behavior of the anodes is evaluated by means of galvanostatic cycling, differential capacities analysis and electrochemical impedance spectroscopy. It is found that the anodes show very good electrochemical performance not only in standard electrolytes based on carbonates solvents but also in electrolytes containing ethers, which are commonly used in Li-S batteries. Furthermore a viable approach for eliminating the irreversible capacity loss at the first cycle using Stabilized Lithium Metal Powder (SLMP) is reported. Finally we introduce a new parameter, namely efficient capacity (Ceff), which is used to estimate the benefits achievable through the utilization of silicon containing anodes over state-of-the-art graphite ones.
As animals forage, they must obtain useful targets by orchestrating appropriate actions that range from searching to chasing, biting and carrying. Here, we reveal that neurons positive for the α subunit of Ca2+/calmodulin-dependent kinase II (CaMKIIα) in the medial preoptic area (MPA) that send projections to the ventral periaqueductal gray (vPAG) mediate these target-directed actions in mice. During photostimulation of the MPA–vPAG circuit, mice vigorously engaged with 3D objects and chased moving objects. When exposed to a cricket, they hunted down the prey and bit it to kill. By applying a head-mounted object control with timely photostimulation of the MPA–vPAG circuit, we found that MPA–vPAG circuit-induced actions occurred only when the target was detected within the binocular visual field. Using this device, we successfully guided mice to navigate specified routes. Our study explains how the brain yields a strong motivation to acquire a target object along the continuum of hunting behavior.