Thermoelectricity offers a sustainable path to recover and convert waste heat into readily available electric energy, and has been studied for more than two centuries. From the controversy between Galvani and Volta on the Animal Electricity, dating back to the end of the XVIII century and anticipating Seebeck's observations, the understanding of the physical mechanisms evolved along with the development of the technology. In the XIX century Ørsted clarified some of the earliest observations of the thermoelectric phenomenon and proposed the first thermoelectric pile, while it was only after the studies on thermodynamics by Thomson, and Rayleigh's suggestion to exploit the Seebeck effect for power generation, that a diverse set of thermoelectric generators was developed.From such pioneering endeavors, technology evolved from massive, and sometimes unreliable, thermopiles to very reliable devices for sophisticated niche applications in the XX century, when Radioisotope Thermoelectric Generators for space missions and nuclear batteries for cardiac pacemakers were introduced. While some of the materials adopted to realize the first thermoelectric generators are still investigated nowadays, novel concepts and improved understanding of materials growth, processing, and characterization developed during the last 30 years has provided new avenues for the enhancement of the thermoelectric conversion efficiency, for example through nanostructuration, and favored the development of new classes of thermoelectric materials. With
The paper describes 3D structures made of liquid-crystalline elastomer (LCE) - rings, woodpiles, etc. - fabricated by two-photon absorption direct laser writing with sub-micrometer resolution while maintaining the desired molecular orientation. These results lay the foundations for creating 3D, micrometer-sized, light-controlled LCE structures.
Yb14MnSb11 is a p-type high temperature thermoelectric material that has been shown to have a peak zT of 1.3 at 1273 K and stable lifetime testing at that temperature for over 1500 h by NASA. Yb14MgSb11 is a structural analog, but the highest temperature thermoelectric properties have not yet been reported. Yb14MgSb11 has been prepared in an environmentally friendly route employing metal hydrides to provide phase pure samples with excellent control of stoichiometry. We present a comparative study employing either MgH2 or YbH2 as a reactive precursor that also facilitates milling of the elements. High purity compositions are synthesized, and their high temperature thermoelectric properties were measured on dense pellets. Temperature-dependent thermoelectric properties were measured from 300 to 1273 K. Yb14MgSb11 exhibited a peak zT = 1.2 at 1273 K due to an appreciable power factor and low-lattice thermal conductivity. Carrier concentration and hall mobility were also measured from 300 to 1275 K and ranged from 5.3 × 1020 to 1.3 × 1021 cm−3 and from 4.7 to 0.7 cm2 V−1 S−1, respectively.
Yb14MnSb11 is a member of a remarkable structural family of compounds that are classified according to the concept of Zintl. This structure type, of which the prototype is Ca14AlSb11, provides a flexible framework for tuning structure-property relationships and hence the physical and chemical properties of compounds. Compounds within this family show exceptional high temperature thermoelectric performance at temperatures above 300 K and unique magnetic and transport behavior at temperatures below 300 K. This review provides an overview of the structure variants, the magnetic properties, and the thermoelectric properties. Suggestions for directions of future research are provided. One active research area is to systematically explore more complex compositions such as Ca11Sb10, K4Pb9, Na8Si46, Ca14AlSb11 and KBa2InAs3. 3-7 The other direction is to replace the alkaline earth metals with divalent rare earth elements (Sm, Eu and Yb) along with the introduction of transition metals into structures, typically replacing the less electronegative metalloid in the anionic framework. 8-10 Combinations of these two directions led to compounds such as Yb14MnSb11, Pr4MnSb9, Eu10Mn6Sb13, Yb9Zn4+xBi9 and Cs13Nb2In6As10. 11-16 The complexity of compositions can be combined with a small flexibility in electron counting. For example, Yb14MnSb11 and Yb9Zn4+xBi9 do not strictly follow the Zintl-Klemm concept. Yb14MnSb11 has Mn 2+ instead of a group 13 element such as in Ca14AlSb11 and therefore is electron deficient, 17 and Yb9Zn4+xSb9 has interstitial Zn atoms which can be compositionally varied to achieve specific properties. 18 At the same time, the total number of valence electrons within an identical Zintl phase structure type with different elements may also vary slightly but the variance can be quite small and limited for many structure types that can be described by the Zintl concept. Therefore, with the introduction of transition elements, new electronic properties are possible, but complete transfer of electrons and clear counting of valence electrons remains a criterion for describing transition and rare earth metal containing Zintl phase compounds. Binary Zintl phase compounds which have compositions of simple ratios of elements usually adopt the structures of known oxides or halides, in which anions and cations are isolated in the structure with no covalent bonding. 2, 19 Both isolated anions, polyanions or clusters in Zintl phase compounds can provide complex compositions such as those represented by Ca11Sb10 and K4Pb9. 3, 4 Polyanions or clusters are formed to compensate for lack of enough electrons from the electropositive element to satisfy valence to form a simple one atom anion. Sb forms Sb-Sb single bonds in the Ca11Sb10 structure type resulting in Sb2 4and Sb4 2polyanions in the structure. 3 The Zintl electron counting provides the following charge balanced scenario: 11Ca 2+ + 4Sb 3-+ 2Sb2 4-+ Sb4 2-. Two types of clusters exist in K4Pb9 with the same formal oxidation state: a monocapped square antiprism and a tr...
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