Modulation of electrical and thermal transports through lattice distortion in BaTi1-xNbxO3solid solutions.

The electron and heat transports in solids are through the movement of carrier electrons and quantized lattice vibrations (phonons), which are sensitive to the lattice distortion and ionized impurities, and are essential aspects for the development of novel thermoelectric materials. In this study, we systematically investigated the modulations of electrical and thermal conductivities of BaTi1-xNbxO3solid solution (BTNO, 0 ≤ x ≤ 1) epitaxial films. At room temperature, BaTiO3belongs to tetragonal perovskite and exhibits electron conduction through doubly degenerated Ti 3d-t2gorbitals upon doping, while BaNbO3belongs to cubic perovskite and exhibits metallic electron conduction through partially filled triply degenerate Nb 4d-t2gorbitals. By controlling the Ti/Nb ratio, we found a dual modulation effect on both the lattice structures and conduction band, which affects the electrical and thermal conductivities. Similar to the SrTi1-xNbxO3solid solution (STNO, 0 ≤ x ≤ 1) system, a phase transition was detected atx âˆ¼ 0.5, at which both the electron and heat transports exhibit abrupt changes. Unlike the transition in STNO, which was attributed to a polaronic phase transition, the transition in BTNO was due to contributions from both the lattice distortion and polaron effect. By controlling the lattice distortion, conduction band, and polaronic phase transitions, the electrical and thermal conductivity of BTNO epitaxial films are modulated within a much greater range than those of the STNO epitaxial films. Due to the double contribution of electron carriers and phonon to thermal conductivity (κ), the maximumκmodulation ratio of BTNO epitaxial films was ∼6.9. Our research provides an effective route to design electrical/thermal management materials.

Vacancy Modulating Co3 Sn2 S2 Topological Semimetal for Aqueous Zinc-Ion Batteries.

Weyl semimetals (WSMs) with high electrical conductivity and suitable carrier density near the Fermi level are enticing candidates for aqueous Zn-ion batteries (AZIBs), meriting from topological surface states (TSSs). We propose a WSM Co3 Sn2 S2 cathode for AZIBs showing a discharge plateau around 1.5 V. By introducing Sn vacancies, extra redox peaks from the Sn4+ /Sn2+ transition appear, which leads to more Zn2+ transfer channels and active sites promoting charge-storage kinetics and Zn2+ storage capability. Co3 Sn1.8 S2 achieves a specific energy of 305 Wh kg-1 (0.2 Ag-1 ) and a specific power of 4900 Wkg-1 (5 Ag-1 ). Co3 Sn1.8 S2 and Znx Co3 Sn1.8 S2 benefit from better conductivity at lower temperatures; the quasi-solid Co3 Sn1.8 S2 //Zn battery delivers 126 mAh g-1 (0.6 Ag-1 ) at -30 °C and a cycling stability over 3000 cycles (2 Ag-1 ) with 85 % capacity retention at -10 °C.

Achieving band convergence by tuning the bonding ionicity in n-type Mg3 Sb2.

Identifying strategies for beneficial band engineering is crucial for the optimization of thermoelectric (TE) materials. In this study, we demonstrate the beneficial effects of ionic dopants on n-type Mg3 Sb2 . Using the band-resolved projected crystal orbital Hamilton population, the covalent characters of the bonding between Mg atoms at different sites are observed. By partially substituting the Mg at the octahedral sites with more ionic dopants, such as Ca and Yb, the conduction band minimum (CBM) of Mg3 Sb2 is altered to be more anisotropic with an enhanced band degeneracy of 7. The CBM density of states of doped Mg3 Sb2 with these dopants is significantly enlarged by band engineering. The improved Seebeck coefficients and power factors, together with the reduced lattice thermal conductivities, imply that the partial introduction of more ionic dopants in Mg3 Sb2 is a general solution for its n-type TE performance. © 2019 Wiley Periodicals, Inc.

Is it Suitable for a Journal to Bid for Publishing a Review That is Likely to be Highly Cited?

By following a recently published paper entitled "The effect of publishing a highly cited paper on a journal's impact factor: a case study of the Review of Particle Physics" in Learned Publishing, we argue that it is not suitable for journals to bid for the right to publish a review that is likely to be highly cited. A few suggestions are also provided to deal with the special case of the Review of Particle Physics phenomenon.

Thermoelectric SnTe with Band Convergence, Dense Dislocations, and Interstitials through Sn Self-Compensation and Mn Alloying.

SnTe is known as an eco-friendly analogue of PbTe without toxic elements. However, the application potentials of pure SnTe are limited because of its high hole carrier concentration derived from intrinsic Sn vacancies, which lead to a high electrical thermal conductivity and low Seebeck coefficient. In this study, Sn self-compensation and Mn alloying could significantly improve the Seebeck coefficients in the whole temperature range through simultaneous carrier concentration optimization and band engineering, thereby leading to a large improvement of the power factors. Combining precipitates and atomic-scale interstitials due to Mn alloying with dense dislocations induced by long time annealing, the lattice thermal conductivity is drastically reduced. As a result, an enhanced figure of merit (ZT) of 1.35 is achieved for the composition of Sn0.94 Mn0.09 Te at 873 K and the ZTave from 300 to 873 K is boosted to 0.78, which is of great significance for practical application. Hitherto, the ZTmax and ZTave of this work are the highest values among all single-element-doped SnTe systems.

Relationship between thermoelectric figure of merit and energy conversion efficiency.

The formula for maximum efficiency (ηmax) of heat conversion into electricity by a thermoelectric device in terms of the dimensionless figure of merit (ZT) has been widely used to assess the desirability of thermoelectric materials for devices. Unfortunately, the ηmax values vary greatly depending on how the average ZT values are used, raising questions about the applicability of ZT in the case of a large temperature difference between the hot and cold sides due to the neglect of the temperature dependences of the material properties that affect ZT. To avoid the complex numerical simulation that gives accurate efficiency, we have defined an engineering dimensionless figure of merit (ZT)eng and an engineering power factor (PF)eng as functions of the temperature difference between the cold and hot sides to predict reliably and accurately the practical conversion efficiency and output power, respectively, overcoming the reporting of unrealistic efficiency using average ZT values.

n-type thermoelectric material Mg2Sn0.75Ge0.25 for high power generation.

Thermoelectric power generation is one of the most promising techniques to use the huge amount of waste heat and solar energy. Traditionally, high thermoelectric figure-of-merit, ZT, has been the only parameter pursued for high conversion efficiency. Here, we emphasize that a high power factor (PF) is equivalently important for high power generation, in addition to high efficiency. A new n-type Mg2Sn-based material, Mg2Sn0.75Ge0.25, is a good example to meet the dual requirements in efficiency and output power. It was found that Mg2Sn0.75Ge0.25 has an average ZT of 0.9 and PF of 52 µW⋅cm(-1)⋅K(-2) over the temperature range of 25-450 °C, a peak ZT of 1.4 at 450 °C, and peak PF of 55 µW⋅cm(-1)⋅K(-2) at 350 °C. By using the energy balance of one-dimensional heat flow equation, leg efficiency and output power were calculated with Th = 400 °C and Tc = 50 °C to be of 10.5% and 6.6 W⋅cm(-2) under a temperature gradient of 150 °C⋅mm(-1), respectively.

Thermoelectric performance enhancement of Mg2Sn based solid solutions by band convergence and phonon scattering via Pb and Si/Ge substitution for Sn.

In this study, the thermoelectric properties of Mg2Sn0.98-xPbxSb0.02 were first studied, and then Mg2Sn0.93-xSixPb0.05Sb0.02 and Mg2Sn0.93-xGexPb0.05Sb0.02 were accordingly investigated. The results showed that the formation of Mg2Sn0.98-xPbxSb0.02 solid solutions effectively reduced the lattice thermal conductivity of Mg2Sn. The room temperature lattice thermal conductivity of Mg2Sn0.98Sb0.02 is ∼5.2 W m(-1) K(-1) but only ∼2.5 W m(-1) K(-1) for Mg2Sn0.73Pb0.25Sb0.02, a reduction of ∼52%. Further alloying Mg2Sn0.98-xPbxSb0.02 with Mg2Si or Mg2Ge to form Mg2Sn0.93-xSixPb0.05Sb0.02 or Mg2Sn0.93-xGexPb0.05Sb0.02 reduced the lattice thermal conductivity significantly due to enhanced phonon scattering by point defects as well as nanoparticles. Moreover, bipolar thermal conductivities were suppressed due to the larger bandgap of Mg2Si and Mg2Ge than Mg2Sn. Furthermore, similar to the pseudo-binary Mg2Sn-Mg2Si and Mg2Sn-Mg2Ge systems, band convergence was also observed in pseudo-ternary Mg2Sn0.93-xSixPb0.05Sb0.02 and Mg2Sn0.93-xGexPb0.05Sb0.02 materials. The convergence of conduction bands led to higher PFs at lower temperatures for Mg2Sn0.93-xSixPb0.05Sb0.02 and Mg2Sn0.93-xGexPb0.05Sb0.02 materials. As a result, higher peak ZTs of ∼1.3 for Mg2Sn0.63Si0.3Pb0.05Sb0.02 and ∼1.2 for Mg2Sn0.68Ge0.25Pb0.05Sb0.02 were achieved.

High thermoelectric performance by resonant dopant indium in nanostructured SnTe.

From an environmental perspective, lead-free SnTe would be preferable for solid-state waste heat recovery if its thermoelectric figure-of-merit could be brought close to that of the lead-containing chalcogenides. In this work, we studied the thermoelectric properties of nanostructured SnTe with different dopants, and found indium-doped SnTe showed extraordinarily large Seebeck coefficients that cannot be explained properly by the conventional two-valence band model. We attributed this enhancement of Seebeck coefficients to resonant levels created by the indium impurities inside the valence band, supported by the first-principles simulations. This, together with the lower thermal conductivity resulting from the decreased grain size by ball milling and hot pressing, improved both the peak and average nondimensional figure-of-merit (ZT) significantly. A peak ZT of ∼1.1 was obtained in 0.25 atom % In-doped SnTe at about 873 K.

Thermoelectrocatalysis: an emerging strategy for converting waste heat into chemical energy.

This perspective defines and explores an innovative waste heat harvesting strategy, thermoelectrocatalysis (TECatal), emphasizing materials design and potential applications in clean energy, environmental, and biomedical technologies.

High-performance cryo-temperature ionic thermoelectric liquid cell developed through a eutectic solvent strategy.

Ionic thermoelectric (i-TE) liquid cells offer an environmentally friendly, cost effective, and easy-operation route to low-grade heat recovery. However, the lowest temperature is limited by the freezing temperature of the aqueous electrolyte. Applying a eutectic solvent strategy, we fabricate a high-performance cryo-temperature i-TE liquid cell. Formamide is used as a chaotic organic solvent that destroys the hydrogen bond network between water molecules, forming a deep eutectic solvent that enables the cell to operate near cryo temperatures (down to -35 °C). After synergistic optimization of the electrode and cell structure, the as-fabricated liquid i-TE cell with cold (-35 °C) and hot (70 °C) ends achieve a high power density (17.5 W m-2) and a large two-hour energy density (27 kJ m-2). In a prototype 25-cell module, the open-circuit voltage and short-circuit current are 6.9 V and 68 mA, respectively, and the maximum power is 131 mW. The anti-freezing ability and high output performance of the as-fabricated i-TE liquid cell system are requisites for applications in frigid regions.

Polaron interfacial entropy as a route to high thermoelectric performance in DAE-doped PEDOT:PSS films.

Enhancing the thermoelectric transport properties of conductive polymer materials has been a long-term challenge, in spite of the success seen with molecular doping strategies. However, the strong coupling between the thermopower and the electrical conductivity limits thermoelectric performance. Here, we use polaron interfacial occupied entropy engineering to break through this intercoupling for a PEDOT:PSS (poly(3,4-ethylenedioxythiophene)-poly(4-styrenesulfonate)) thin film by using photochromic diarylethene (DAE) dopants coupled with UV-light modulation. With a 10-fold enhancement of the thermopower from 13.5 µV K-1 to 135.4 µV K-1 and almost unchanged electrical conductivity, the DAE-doped PEDOT:PSS thin film achieved an extremely high power factor of 521.28 µW m-1 K-2 from an original value of 6.78 µW m-1 K-2. The thermopower was positively correlated with the UV-light intensity but decreased with increasing temperature, indicating resonant coupling between the planar closed DAE molecule and PEDOT. Both the experiments and theoretical calculations consistently confirmed the formation of an interface state due to this resonant coupling. Interfacial entropy engineering of polarons could play a critical role in enhancing the thermoelectric performance of the organic film.

Effect of aluminum on the thermoelectric properties of nanostructured PbTe.

In the present work, the effect of aluminum (Al) on the thermoelectric properties of PbTe is studied. Aluminum doped PbTe samples, fabricated by a ball milling and hot pressing, have Seebeck coefficients between -100 and -200 µV K-1 and electrical conductivities of (3.6-18) × 104 S m-1 at room temperature, which means that Al is an effective donor in PbTe. The first principle calculations clearly show an increase of the density of states close to the Fermi level in the conduction band due to Al doping, which averages up the energy and effective mass of electrons, resulting in enhancement of the Seebeck coefficient. The maximum figure-of-merit ZT of 1.2 is reached at 770 K in the Al0.03PbTe sample.

Fast phase formation of double-filled p-type skutterudites by ball-milling and hot-pressing.

Filled-skutterudites are promising mid-temperature thermoelectric materials for heat-to-electricity conversion. Traditional preparation methods need a very long time annealing (7 to 14 days) to form the right skutterudite phase. Annealing is especially critical for p-type filled-skutterudites, since Fe4Sb12 needs filler atoms to enter the cage to form a stable phase. In this work, we prepared Ce and Nd double-filled p-type skutterudite materials by directly ball-milling the quenched ingot without annealing followed by hot-pressing. The results showed that with appropriate ball-milling time, a pure p-type filled-skutterudite phase can be obtained in just 5 minutes by hot-pressing. The samples prepared in this way have the same quality as those prepared by traditional long time annealing methods, and showed ZT values above 1 between 700 and 800 K. This simple and efficient method is very useful for the preparation of many other materials that are kinetically difficult to make.

Effect of silicon and sodium on thermoelectric properties of thallium-doped lead telluride-based materials.

Thallium (Tl)-doped lead telluride (Tl(0.02)Pb(0.98)Te) thermoelectric materials fabricated by ball milling and hot pressing have decent thermoelectric properties but weak mechanical strength. Addition of silicon (Si) nanoparticles strengthened the mechanical property by reducing the grain size and defect density but resulted in low electrical conductivity that was not desired for any thermoelectric materials. Fortunately, doping of sodium (Na) into the Si added Tl(0.02)Pb(0.98)Te brings back the high electrical conductivity and yields higher figure-of-merit ZT values of ∼1.7 at 770 K. The ZT improvement by Si addition and Na doping in Tl(0.02)Pb(0.98)Te sample is the direct result of concurrent electron and phonon engineering by improving the power factor and lowering the thermal conductivity, respectively.

General Figures of Merit ZQ for Thermoelectric Generators Under Constant Heat-In Flux Boundary.

The thermoelectric figure of merit ZT bridges the efficiency and material parameters for a thermoelectric device operating under constant temperature of the hot- and cold-source thermal boundary (Type-I TB). However, many application scenarios fall under the constant heat-in flux (qh ) and constant cold-source temperature (Tc ) thermal boundary (Type-II TB), for which a figure of merit is absent for more than half a century. This study aims to fill this gap and propose a figure of merit ZQD for the thermoelectric devices under the Type-II TB condition, defined as Z Q D = ( Z T c Z T c + 1 ) ( h κ ) ( q h T c ) $Z{Q}_{\mathrm{D}} = ( {\frac{{Z{T}_{\mathrm{c}}}}{{Z{T}_{\mathrm{c}} + 1}}} )( {\frac{h}{\kappa }} )( {\frac{{{q}_{\mathrm{h}}}}{{{T}_{\mathrm{c}}}}} )$ , where Z, h, and κ are the traditional figure of merit, leg height, and thermal conductivity, respectively. The effectiveness of ZQD is verified through both numerical calculations and experiments, which are more accurate and practical than ZT. Furthermore, a system-level figure of merit ZQS is suggested after considering the external thermal resistance. Finally, optimization strategies for thermoelectric systems based on ZQS are proposed, showing a 30% enhancement in the efficiency. ZQD and ZQS are expected to be widely used in the thermoelectric field.

Ultrasensitive mechanical/thermal response of a P(VDF-TrFE) sensor with a tailored network interconnection interface.

Ferroelectric polymers have great potential applications in mechanical/thermal sensing, but their sensitivity and detection limit are still not outstanding. We propose interface engineering to improve the charge collection in a ferroelectric poly(vinylidene fluoride-co-trifluoroethylene) copolymer (P(VDF-TrFE)) thin film via cross-linking with poly(3,4-ethylenedioxythiophene) doped with polystyrenesulfonate (PEDOT:PSS) layer. The as-fabricated P(VDF-TrFE)/PEDOT:PSS composite film exhibits an ultrasensitive and linear mechanical/thermal response, showing sensitivities of 2.2 V kPa-1 in the pressure range of 0.025-100 kPa and 6.4 V K-1 in the temperature change range of 0.05-10 K. A corresponding piezoelectric coefficient of -86 pC N-1 and a pyroelectric coefficient of 95 µC m-2 K-1 are achieved because more charge is collected by the network interconnection interface between PEDOT:PSS and P(VDF-TrFE), related to the increase in the dielectric properties. Our work shines a light on a device-level technique route for boosting the sensitivity of ferroelectric polymer sensors through electrode interface engineering.

Performance boost for bismuth telluride thermoelectric generator via barrier layer based on low Young's modulus and particle sliding.

The lack of desirable diffusion barrier layers currently prohibits the long-term stable service of bismuth telluride thermoelectric devices in low-grade waste heat recovery. Here we propose a new design principle of barrier layers beyond the thermal expansion matching criterion. A titanium barrier layer with loose structure is optimized, in which the low Young's modulus and particle sliding synergistically alleviates interfacial stress, while the TiTe2 reactant enables metallurgical bonding and ohmic contact between the barrier layer and the thermoelectric material, leading to a desirable interface characterized by high-thermostability, high-strength, and low-resistivity. Highly competitive conversion efficiency of 6.2% and power density of 0.51 W cm-2 are achieved for a module with leg length of 2 mm at the hot-side temperature of 523 K, and no degradation is observed following operation for 360 h, a record for stable service at this temperature, paving the way for its application in low-grade waste heat recovery.

Wide-temperature-range thermoelectric n-type Mg3(Sb,Bi)2 with high average and peak zT values.

Mg3(Sb,Bi)2 is a promising thermoelectric material suited for electronic cooling, but there is still room to optimize its low-temperature performance. This work realizes >200% enhancement in room-temperature zT by incorporating metallic inclusions (Nb or Ta) into the Mg3(Sb,Bi)2-based matrix. The electrical conductivity is boosted in the range of 300-450 K, whereas the corresponding Seebeck coefficients remain unchanged, leading to an exceptionally high room-temperature power factor >30 µW cm-1 K-2; such an unusual effect originates mainly from the modified interfacial barriers. The reduced interfacial barriers are conducive to carrier transport at low and high temperatures. Furthermore, benefiting from the reduced lattice thermal conductivity, a record-high average zT > 1.5 and a maximum zT of 2.04 at 798 K are achieved, resulting in a high thermoelectric conversion efficiency of 15%. This work demonstrates an efficient nanocomposite strategy to enhance the wide-temperature-range thermoelectric performance of n-type Mg3(Sb,Bi)2, broadening their potential for practical applications.

Bi-Deficiency Leading to High-Performance in Mg3 (Sb,Bi)2 -Based Thermoelectric Materials.

Mg3 (Sb,Bi)2 is a potential nearly-room temperature thermoelectric compound composed of earth-abundant elements. However, complex defect tuning and exceptional microstructural control are required. Prior studies have confirmed the detrimental effect of Mg vacancies (VMg ) in Mg3 (Sb,Bi)2 . This study proposes an approach to mitigating the negative scattering effect of VMg by Bi deficiency, synergistically modulating the electrical and thermal transport properties to enhance the thermoelectric performance. Positron annihilation spectrometry and Cs -corrected scanning transmission electron microscopy analyses indicated that the VMg tends to coalesce due to the introduced Bi vacancies (VBi ). The defects created by Bi deficiency effectively weaken the scattering of electrons from the intrinsic VMg and enhance phonon scattering. A peak zT of 1.82 at 773 K and high conversion efficiency of 11.3% at ∆T = 473 K are achieved in the optimized composition of Mg3 (Sb,Bi)2 by tuning the defect combination. This work demonstrates a feasible and effective approach to improving the performance of Mg3 (Sb,Bi)2 as an emerging thermoelectric material.