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The potential for metallic lithium batteries that exhibit high specific capacities has stimulated a large interest within the energy research field. For safety reasons, the use of metallic lithium anodes requires electrochemically stable electrolytes. However, to date there has been limited success in this area. This work introduces a solid, lithium single-ion conductor thus providing new perspectives in the field of solid-state lithium-batteries. This new-concept material (LiFT), obtained by a direct reaction of nanometric fluorinated titanium oxide (FT) with molten metallic lithium, consists of nanoparticles (NPs) with anionic surface groups that are neutralized with lithium cations. The material displays fast lithium ion transport via an efficient migration mechanism occurring at the interfaces between different nanoparticles. The electrolyte comprises 1.34 mol kg−1 of Li and a conductivity of 2.8·10−4 S cm-1 at 25 °C is demonstrated. This level of performance, in conjunction with a native electrochemical stability towards lithium, extremely low cost starting materials (TiO2) and a facile one-pot synthesis, renders this electrolyte very attractive for applications in future full solid-state lithium batteries.
NiCo2O4 nanoflake composites were synthesized by using DNA molecules as templates via in-situ assembly and subsequent thermal treatment. The obtained NiCo2O4 composites were characterized by scanning electron microscopy, energy dispersive spectroscopy, X-ray powder diffraction, thermogravimetric analysis, and X-ray photoelectron spectroscopy. Cyclic voltammetry and chronopotentiometry tests were used to investigate the electrochemical properties of the as-prepared composites. Superior performances with a good specific capacitance (1468 F/g), an extraordinary rate capability (64.9% capacity retention at 16 A/g) and an excellent cycling stability (85.5% retention after 5000 cycles) were achieved. The DNA templates were introduced as the binder of NiCo2O4 and as the conductive matrix to facilitate the electron transmission between electroactive materials and outside current collectors, which resulted in the excellent electrochemical performances of the synthesized NiCo2O4 composites. It is believed that our NiCo2O4 nanocomposites could be used as effective electrode materials for supercapacitors.
To enhance specific capacity, cycle performance and rate-capability of lithium-ion battery cathode materials, the Li[Co0.1Ni0.15Li0.2Mn0.55]O2 (LCMNO) is modified by coating them with amorphous carbons and by preparing nanocomposites with nanostructured carbons (carbon nanotube and graphene). The carbon-treated LCMNO powders and their cathodes are characterized by morphological observation, crystalline property analysis, galvanostatic charge–discharge, and electrochemical impedance spectroscopy. The LCMNO nanocomposite shows a superior discharge capacity of ca. 290mAhg−1 at low C-rates, due to a greater number of active sites embedded by nanostructured carbon species. In contrast, the carbon-coated LCMNO shows higher discharge capacity in high rate regions due to the carbon-coated layer in the carbon-coated LCMNO, suppressing the side reactions and enhancing the electrical conductivity.
The development of suitable biomarker-based microbioassays with model species with ecological relevance would help increase the cost-efficiency of routine environmental monitoring and chemical toxicity testing. The anti-inflammatory drug diclofenac has been widely reported in the environment but ecotoxicological data are scarce. The aim of this work is to assess the acute and chronic sublethal toxicity of diclofenac in relevant taxa of aquatic and riparian ecosystems (the fish Danio rerio and the fern Polystichum setiferum). Reliable biomarkers of cell viability (mitochondrial activity), plant physiology (chlorophyll), growth (DNA content) or oxidative damage (lipid peroxidation) were assessed as sensitive endpoints of toxicity. DNA quantification shows that diclofenac induces acute lethal phytotoxicity at 24 and 48 h (LOECs 30 and 0.3 μg l−1, respectively). Hormetic effects in mitochondrial activity in spores of Polystichum setiferum mask lethality, and adverse effects are only observed at 48 h (LOEC 0.3 μg l−1). In chronic exposure (1 week) LOEC for DNA is 0.03 μg l−1. Mitochondrial activity shows a strong hormetic stimulation of the surviving spore population (LOEC 0.3 μg l−1). Little changes are observed in chlorophyll autofluorescence (LOEC 0.3 μg l−1). A very short exposure (90 min) of zebrafish embryos induces a reduction of lipid peroxidation at 0.03 μg l−1. Environmental concentrations of diclofenac can be deleterious for the development of significant populations of sensitive individuals in aquatic and riparian ecosystems.
The surface energy balance includes a term for soil heat flux. Soil heat flux is difficult to measure because it includes conduction and convection heat transfer processes. Accurate representation of soil heat flux is an important consideration in many modeling and measurement applications. Yet, there remains uncertainty about what comprises soil heat flux and how surface and subsurface heat fluxes are linked in energy balance closure. The objective of this study is to demonstrate the presence of a subsurface latent heat sink, which must be considered in order to accurately link subsurface heat fluxes between depths near and at the soil surface. Measurements were performed under effectively bare surface conditions in a silty clay loam soil near Ames, IA. Soil heat flux was measured with heat-pulse sensors using the gradient heat flux approach at 1-, 3-, and 6-cm soil depths. Independent estimates of the daily latent heat sink were obtained by measuring the change of mass of microlysimeters. Heat flux measurements at the 1-cm depth deviated from heat flux measurements at other depths, even after calorimetric adjustment was made. This deviation was most pronounced shortly after rainfall, where the 1-cm soil heat flux measurement exceeded 400Wm−2. Cumulative soil heat flux measurements at the 1-cm depth exceeded measurements at the 3-cm depth by >75% over a 7-day rain-free period, whereas calorimetric adjustment allowed 3- and 6-cm depth measurements to converge. Latent heat sink estimates from the microlysimeters accounted for nearly all of the differences between the 1- and 3-cm depth heat flux measurements, indicating that the latent heat sink was distributed between the 1- and 3-cm depths shortly after the rainfall event. Results demonstrate the importance of including latent heat when attempts are made to link or extrapolate subsurface soil heat flux measurements to the surface soil heat flux.
Lithium magnesium cobalt oxide (LMCO) was synthesized with heating a reaction mixture of dehydrated magnesium cobalt hydroxide and Li2CO3 to stabilized crystal structure of LiCoO2. The sample was characterized by XRD. All diffraction lines could be indexed by assuming a hexagonal lattice. Rietvelt analysis indicated that magnesium were located at cobalt site in the layered structure. The voltage plateau around 4.1V (versus Li) for LiCoO2 was not observed for LMCO. The prismatic lithium-ion batteries of lithium magnesium cobalt oxide and graphite with γ-butyrolactone (GBL) were fabricated and examined in terms of rate capability, low temperature discharge characteristics, high-temperature storage, and safety inspection by so-called hot pot test of the positive electrolyte. Interesting phenomenon on thermal stability of the lithium magnesium cobalt oxide was reported.
The protective effect of Vitamin E and selenium was studied for the possibility of decreasing the chromosome aberrations (CA), micronuclei (MN) and sister chromatid exchanges (SCE) induced by carbon tetrachloride (CCl4) in ovine peripheral lymphocytes cultured in vitro. The cultures of lymphocytes from two healthy lambs were treated with carbon tetrachloride at concentrations of 2, 4, 8, and 16μg/ml for the last 48h of cultivation and subsequently with the same doses of CCl4 and Vitamin E and selenium. A possible metabolic modification in carbon tetrachloride genotoxicity was detected with the application of S9 fraction for 2h. No positive clastogenic effect of CCl4, and subsequently no protective effect of either antioxidant was obtained in the CA assay. In the MN assay for 48h, an increase and, respectively, a decrease in the frequency of MN was found in cultures treated with CCl4 alone and in cultures treated concurrently with CCl4, Vitamin E and selenium at concentrations of 8 and 16μg/ml (P<0.001 and P<0.01). High statistical significance was achieved in SCE assay after the treatment of ovine peripheral lymphocytes with CCl4 at all concentrations tested (P<0.001), except the lowest dose. A significant decrease in SCEs was obtained in cultures treated simultaneously with CCl4, Vitamin E and selenium (P<0.001). The highest dose (16μg/ml) was also shown to improve the cell-cycle kinetics in comparison with corresponding unprotected dose (P<0.01). Insufficient confirmation of the genotoxicity of CCl4 and the protective effect of the antioxidants, respectively were seen in cultures with metabolic activation.
Objectives Cognitive impairment is a common symptom of schizophrenia that has significant effects on quality of life and the activities of daily living. The present study examined the ability of transcranial direct current stimulation (tDCS) to improve cognitive function and clinical symptoms in patients with schizophrenia. Methods Fifty-six patients with schizophrenia were randomized to real-tDCS and sham-tDCS groups. The participants were stable for a period of 3months before study enrollment. Each group received 30min of active 2-mA tDCS or sham stimulation over the left dorsolateral prefrontal cortex (anode F3, cathode F4) once per day for 10 consecutive weekdays. The Measurement and Treatment Research to Improve Cognition in Schizophrenia Consensus Cognitive Battery (MCCB) and Wisconsin Card Sorting Test (WCST) were used to evaluate cognitive function, and the Positive and Negative Syndrome Scale (PANSS), Clinical Global Impression-Schizophrenia scale (CGI-SCH), and Calgary Depression Scale for Schizophrenia (CDSS) were used to evaluate symptoms at baseline, after 10 sessions, and at 3-month follow-up. Results There was a significant time×group interaction, indicating that MCCB working memory (P=0.008) and overall scores (P=0.031) improved over time in the real-tDCS group compared to the sham-tDCS group. There was also a significant time×group interaction for depressive symptoms as evaluated by the CGI-SCH, which decreased over time in the real-tDCS group (P=0.041). tDCS treatment combined with antipsychotic medication was generally well-tolerated and safe. Conclusions Adjunct tDCS treatment is safe and effective for improving cognitive status in patients with schizophrenia.
The concept of electrochemical capacitance comprises both double-layer grounded capacitive (non-faradaic charging) and pseudocapacitive (faradaic charging) behaviours, as has been recently demonstrated [1–3]. In this paper, we demonstrate that nanostructured compounds possessing electrochemical capacitance can be used to design suitable interfaces for label-free biosensing applications, which, moreover, do not require a redox probe to be added to biological samples before assaying. This is possible when the capacitive transducer layer of the biosensor device is kept within an appropriate length scale (for instance, thicknesses lower than 10 nm) in which mesoscopic electrochemical properties prevail. Hence, we demonstrate how the capacitive signatures of Prussian Blue nanostructured films can be envisioned as transducer signals in biosensor devices in general, going beyond traditional redox monolayers, using aqueous electrolytes. This approach is illustrated using electroactive films made of Prussian Blue nanoparticles and modified with appropriate receptors, which successfully and specifically detected interleukin-6, a small biomarker, with a limit of detection of 5.6 ± 0.3 ng mL−1. In summary, the application of Prussian Blue pseudocapacitive properties in label-free biosensor devices were demonstrated as a proof-of-concept of how such applications can be engineered.
Nafion ionomer is impregnated or incorporated in the PEM fuel cell electrodes to achieve high power density. Though many studies have been reported on the effect of Nafion content on electrode performance, best results have been reported at different Nafion loadings by different researchers. Nafion ionomer helps to increase the three-dimensional zone of catalytic activity and platinum utilization in the electrode. It also helps to retain moisture and prevent membrane dehydration especially at high current densities. An optimum Nafion content in the electrode is necessary to achieve high performance. As the platinum loading increases, the electrode thickness and Nafion thickness grows and hence the optimum Nafion content may depend on the platinum loading. In this paper, we have examined the correlation of platinum loading and optimum Nafion content in the electrode. We have found that optimum Nafion requirement depends on the platinum loading and it increases with decrease in Pt loading. For electrodes with 0.5, 0.25 and 0.1mg/cm2 Pt loading, best performance was obtained at about 20, 40 and 50% Nafion ionomer loading, respectively.
All-solid-state Li/LiPONB/TiOS microbatteries were manufactured at the pilot scale on silicon substrate. In a first attempt, the characterization of the active materials constituting the microbattery was achieved in order to determine their accurate composition, structure and morphology. Finally, a thorough electrochemical characterization was carried out on all-solid-state cells. Excellent performances were noted in terms of cycle life (with more than 1000 cycles), efficiency and self-discharge (less than 5% per year). In addition, the positive electrode highlighted a high volumetric capacity close to 90μAhcm−2 μm−1 when cycled at 100μAcm−2 between 1V and 3V vs. Li+/Li.
To investigate the contribution of lithium-ion diffusibility of lithium tungsten oxides (LWOs) to low interfacial resistance, we fabricate thin-film electrodes of 6Li-enriched LiCoO2 (6LCO) modified with various structure-types of 6Li-enriched LWOs by pulsed laser deposition. The electrodes are subjected to X-ray diffraction (XRD), electrochemical impedance spectroscopy (EIS), and secondary-ion mass spectrometry (SIMS) analyses. XRD reveals that the LWO layers have Li2WO4 structure with rhombohedral and tetragonal symmetries and amorphous states. EIS shows that the lowest interfacial resistance of the positive electrodes is given by the amorphous state, followed in order by the tetragonal and the rhombohedral symmetry, and that the diffusion coefficients of lithium-ions in the electrodes increase in the same order. SIMS demonstrates that the fastest lithium-ion self-diffusibility into the LWOs is found in the amorphous state, followed in order by tetragonal and rhombohedral symmetry. Furthermore, the amorphous state LWO modification shows smooth lithium-ion diffusion between the LWO and LCO layers after the electrochemical test. Conversely, the rhombohedral LWO modification demonstrates congested lithium-ion diffusion between the LWO and LCO layers after the test. Thus, fast lithium-ion self-diffusibility into the LWO-modified LCO contributes to enhancing the diffusion of lithium-ions, resulting in the reduction of interfacial resistance.
Polymer electrolyte membranes that consist of poly(vinyl acetate) (PVAc) and LiClO4 with different concentrations of plasticizer (N,N-dimethylformamide (DME) have been prepared by a solution-casting technique. The formation of polymer-salt complexes has been confirmed by FT-IR spectral studies. Conductivity studies have been carried out using ac impedance spectroscopy in the frequency range 42Hz–5MHz. The influence of the addition of plasticizer (DMF) on the ionic conductivity of the PVAc–LiClO4 polymer electrolyte complex has been discussed. The maximum value of bulk conductivity for PVAc(70)–DMF(20)–LiClO4(10) system is found to be 4.2×10−4 Scm−1 at 303K. The temperature dependence of the conductivity of the polymer electrolytes follows the Vogel–Tamman–Fulcher relationship. Transport properties, such as activation energy and charge carrier concentration, have been calculated from the VTF formalism. The ionic transference number of the mobile ions has been estimated by Wagner’s polarization method and is found to be ≥0.96 for all the samples.
In response to the thread of environmental and ecological degradation along with projected fossil fuel depletion the active search for efficient renewable energy conversion technologies has been attempted in various research areas including the field of thermoelectrics. Despite the availability of considerable amounts of waste and natural heat stored in warm fluids (<250 °C) a lack of environmentally friendly materials with high natural abundance, low manufacturing cost and high thermoelectric efficiency impedes the widespread use of thermoelectric generators for energy harvesting on a large scale. In this perspective, we examine the possibility of using organic conducting polymers in thermoelectric applications. We provide an overview of the background and the key concepts of organic thermoelectrics and illustrate some of the first prototypes of polymer-based organic thermoelectric generators.
The compounds SrSnO3, BaSnO3 and Ca2SnO4 have been synthesized by solid-state and/or sol–gel methods, characterized by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and scanning electron microscopy (SEM) and their electrochemical properties studied as cathodes versus Li metal in the range 0.005–1.0V. ASnO3 (A = Sr, Ba), adopt the perovskite structure whereas Ca2SnO4 has the Sr2PbO4 structure. The discharge capacities (mAhg−1) (moles of equivalent Li) on the 20th cycle at a current rate of 30mAg−1 are: SrSnO3 (solid-state) (144 (1.4)), SrSnO3 (sol–gel) (222 (2.1)), BaSnO3 (solid-state) (190 (2.2)), BaSnO3 (sol–gel) (156 (1.8)) and Ca2SnO4 (247 (2.4)). The SrSnO3 (sol–gel) with nano-particle morphology displays better galvanostatic cycling performance than SrSnO3 (solid-state). The cycling behaviour of SrSnO3 and BaSnO3 is inferior to that of Ca2SnO4 and CaSnO3, which demonstrates that ‘Ca’ is superior as a matrix element than Sr or Ba. The inferior electrochemical performance of Ca2SnO4 in comparison to CaSnO3 reveals that the higher Ca:Sn ratio in the former is not advantageous and the perovskite structure is preferable to that of Sr2PbO4 structure. The coulombic efficiencies are >98% in all cases. Cyclic voltammetry (CV) compliments the observed cycling behaviour.
Tool design is carried out for a multi-stage deep drawing and ironing process of a rectangular cup with the large aspect ratio using the result of the finite element analysis. The analysis incorporates three-dimensional continuum elements for an elasto-plastic finite element method with the explicit time integration scheme using LS-DYNA3D. The analysis simulates the five-stage deep drawing and ironing process with the thickness control of the cup wall. Simulation is performed in order to investigate the failure by tearing during the forming process at the initial state of tool design. The analysis reveals that the difference of the drawing ratio within the cross section induces non-uniform metal flow which causes severe local extension. The irregular contact condition between the blank and the die also induces non-uniform metal flow which causes local wrinkling. This paper identifies such unfavorable mechanism in the rectangular cup drawing with ironing and proposes a new tool design with the guideline for modification in the design of the process and the sequential tool shape. The finite element analysis result with the improved tool design confirms that the proposed design not only reduces the possibility of failure but also improves the quality of a deep-drawn product. The numerical result shows fair coincidence with the experimental result.
In this work, we successfully use ultralong γ-MnOOH microrods to synthesize ultralong spinel LiNi0.5Mn1.5O4 microrods through high temperature solid state reaction, which allows to drastically increase the content of residual Mn3+ ions (up to 61.3%) along with oxygen deficiency (up to 0.44) in spinel structure and improves the rate, cycling and discharge capacity of LiNi0.5Mn1.5O4 materials significantly. The excessive theoretical capacity (185 mAhg−1) is even observed at low charge and discharge rate due to the additional enhanced contribution of the Mn3+/Mn4+ redox couples. The LNMO-800 shows a little capacity decay with the increasing of the rate from 0.5 C to 1 C and 2 C, the discharge capacities were 145 mAhg−1, 144.6 mAhg−1 and 142 mAhg−1, respectively. Even at a high rate of 10 C, it still deliveres a capacity of 125.3 mAhg−1. After 1000 cycles at 1 C, the discharge capacity can still reach 120 mAhg−1, corresponding to a capacity retention of 82.3%. The high temperature (55 °C) tests also demonstrate its excellent structural stability. The LiNi0.5Mn1.5O4 microrod with ultrahigh Mn3+ content should be a promising choice for future high energy power applications.
The practice of viticulture and winemaking is highly dependent upon the weather and climate. Any future changes in the seasons, their duration, local maximum, minimum and mean temperatures, frost occurrence and heat accumulation could have a major impact on the winegrowing areas of the world. Given that the winegrowing industry has substantial energy requirements and is directly influenced by any changes in climate, the industry should be at the forefront in promoting the case of energy efficiency and the adoption of renewable technologies. Solar renewables in the form of solar thermal and photovoltaics (PVs) offer a complimentary solution to many winegrowing processes. This paper examines the limited number of world wineries that have adopted solar renewables and presents a viable case for their wide scale integration into the industry. The paper presents a range of viticultural and winemaking processes where solar energy can be directly or indirectly applied and suggests the potential for solar energy in making substantial savings in both energy use and greenhouse gas emissions. In 2005, almost 8 million hectares were under vines producing 40.2 million tonnes of grapes for crushing. The total global energy use within the winemaking industry is estimated at over 105PJ emitting nearly 16 million tonnes of CO2. If ancillary industries, such as bottle making and transportation are included, the total carbon footprint of the industry is estimated at over 76 million tonnes of CO2. This paper calculates that if the commercial winemaking establishments in the ‘developed’ wine producing regions of the world integrated a ‘small’ solar installation into their wineries, the potential savings are 18.3% or 19.24PJ of the energy used in the global winemaking industry.
LiNi1−x−yCoxAlyO2 is a commonly used Ni-rich cathode material because of its relatively low cost, excellent rate capability and high gravimetric energy density. Surface modification is an efficient way to overcome the shortcomings of Ni-rich cathodes such as poor cycling stability and poor thermal stability. A high-powered concentration-gradient cathode material with an average composition of LiNi0.815Co0.15Al0.035O2 (LGNCAO) has been successfully synthesized by using spherical concentration-gradient Ni0.815Co0.15Al0.035(OH)2 (GNCA)as the starting material. An efficient design of the Al3+ precipitation method is developed, which enables obtaining spherical GNCA with ∼10 μm particle size and high tap density. In LGNCAO, the nickel and cobalt concentration decreases gradually whereas the aluminum concentration increases from the centre to the outer layer of each particle. Electrochemical performance and storage properties of LGNCAO have been investigated comparatively. The LGNCAO displays better electrochemical performance and improved storage stability than LNCAO.