The expansion of renewable energy and the growing number of electric vehicles and mobile devices are demanding improved and low-cost electrochemical energy storage. In order to meet the future needs for energy storage, novel material systems with high energy densities, readily available raw materials, and safety are required. Currently, lithium and lead mainly dominate the battery market, but apart from cobalt and phosphorous, lithium may show substantial supply challenges prospectively, as well. Therefore, the search for new chemistries will become increasingly important in the future, to diversify battery technologies. But which materials seem promising? Using a selection algorithm for the evaluation of suitable materials, the concept of a rechargeable, high-valent all-solid-state aluminum-ion battery appears promising, in which metallic aluminum is used as the negative electrode. On the one hand, this offers the advantage of a volumetric capacity four times higher (theoretically) compared to lithium analog. On the other hand, aluminum is the most abundant metal in the earth's crust. There is a mature industry and recycling infrastructure, making aluminum very cost efficient. This would make the aluminum-ion battery an important contribution to the energy transition process, which has already started globally. So far, it has not been possible to exploit this technological potential, as suitable positive electrodes and electrolyte materials are still lacking. The discovery of inorganic materials with high aluminum-ion mobility—usable as solid electrolytes or intercalation electrodes—is an innovative and required leap forward in the field of rechargeable high-valent ion batteries. In this review article, the constraints for a sustainable and seminal battery chemistry are described, and we present an assessment of the chemical elements in terms of negative electrodes, comprehensively motivate utilizing aluminum, categorize the aluminum battery field, critically review the existing positive electrodes and solid electrolytes, present a promising path for the accelerated development of novel materials and address problems of scientific communication in this field.
The precise quantification of the pyroelectric coefficient p is indispensable for the characterization of pyroelectric materials and the development of pyroelectric-based devices, such as radiation sensors or energy harvesters. A summary of the variety of techniques to measure p is given in the present review. It provides a classification after the thermal excitation and an outline of capabilities and drawbacks of the individual techniques. The main selection criteria are: the possibility to separate different contributions to the pyroelectric coefficient, to exclude thermally stimulated currents, the capability to measure p locally, and the requirement for metallic electrodes. This overview should enable the reader to choose the technique best suited for specific samples.
The disinfection of bacteria by thermally excited pyroelectric materials in aqueous environments provides opportunities for the development of new means of sanitization. However, little is known about the formation of reactive oxygen species (ROS) at the surface of the thermally excited pyroelectric materials. To investigate the pyroelectrically driven ROS generation we performed OH radical specific measurements of thermally stimulated barium titanate nanoparticles in contact with palladium nanoparticles. Through electron spin resonance measurements with the spin trap BMPO (5-tert-butoxycarbonyl 5-methyl-1-pyrroline n-oxide) and fluorescence spectroscopy of 7-hydroxycoumarin, OH radical generation was detected, which confirms the hypothesis of pyroelectric ROS production. Since pyroelectric potential changes are insufficient for direct electrochemical OH radical generation, we propose a two-step chargetransfer model facilitated by intermittent contact between the palladium and the pyroelectric nanoparticles and the pyroelectric effect as the driving force for charge transfer. ■ INTRODUCTIONCommercial water disinfection currently relies on chemical methods using chlorine-or ozone-based chemicals, whereas physical methods like thermal disinfection or ultraviolet radiation are less often employed. Due to their high oxidative potential, reactive oxygen species (ROS) are well suited as a physical means of disinfection. A completely new approach for creating ROS is the utilization of the pyroelectric effect, 1 which seems favorable when naturally occurring temperature changes can be employed for the excitation of the pyroelectric materials and, thus, offer an environmentally friendly method of water disinfection.In an aqueous solution the spontaneous polarization at the surface of a ferroelectric is screened, for example, by dissolved ions or dissociated water molecules. Changes in temperature trigger the pyroelectric effect. The imbalance of polarization and screening charges changes the effective surface potential. It was shown that these potential changes whether they stem from changes in temperature or strain can be used to drive electrochemistry between physisorbed molecular species. 1,2 For example Hong et al. demonstrated water splitting on mechanically excited surfaces of BaTiO 3 and ZnO. Gutmann et al. proposed that the observed water disinfection with thermally stimulated LiNbO 3 and LiTaO 3 is facilitated by production of ROS at the surface of the pyroelectric materials.Free radicals have high oxidation potentials, especially the OH radical whose oxidation potential is twice that of chlorine which is commonly used for disinfection. It is known that OH radicals can pull H atoms from C−H and S−H bonds and split aromatic rings. Living cells are damaged by radicals reacting with amino acids and DNA molecules. 3 Photocatalytic E. coli inactivation with TiO 2 showed cell damage caused by various ROS, such as OH radicals, hyperoxide radicals, and H 2 O 2 . 4 Basically ROS react immediately at the place of their ori...
The R 2 PdSi 3 intermetallic compounds have been reported to crystallize in a hexagonal AlB 2 -derived structure, with the rare earth atoms on the Al sites and Pd and Si atoms randomly distributed on the B sites. However, the intricate magnetic properties observed in the series of compounds have always suggested complications to the assumed structure. To clarify the situation, x-ray and neutron diffraction measurements were performed on the heavy rare earth compounds with R = Gd, Tb, Dy, Ho, Er, Tm, which revealed the existence of a crystallographic superstructure. The superstructure features a doubled unit cell in the hexagonal basal plane and an octuplication along the perpendicular c direction with respect to the primitive cell. No structural transition was observed between 300 and 1.5 K. Extended x-ray absorption fine structure (EXAFS) analysis as well as density functional theory (DFT) calculations were utilized to investigate the local environments of the respective atoms. In this paper the various experimental results will be presented and it will be shown that the superstructure is mainly due to the Pd-Si order on the B sites. A structure model will be proposed to fully describe the superstructure of Pd-Si order in R 2 PdSi 3 . The connection between the crystallographic superstructure and the magnetic properties will be discussed in the framework of the presented model.
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