Filled skutterudites R(x)Co4Sb12 are excellent n-type thermoelectric materials owing to their high electronic mobility and high effective mass, combined with low thermal conductivity associated with ...the addition of filler atoms into the void site. The favourable electronic band structure in n-type CoSb3 is typically attributed to threefold degeneracy at the conduction band minimum accompanied by linear band behaviour at higher carrier concentrations, which is thought to be related to the increase in effective mass as the doping level increases. Using combined experimental and computational studies, we show instead that a secondary conduction band with 12 conducting carrier pockets (which converges with the primary band at high temperatures) is responsible for the extraordinary thermoelectric performance of n-type CoSb3 skutterudites. A theoretical explanation is also provided as to why the linear (or Kane-type) band feature is not beneficial for thermoelectrics.
In analyzing zT improvements due to lattice thermal conductivity (κL) reduction, electrical conductivity (σ) and total thermal conductivity (κTotal) are often used to estimate the electronic ...component of the thermal conductivity (κE) and in turn κL from κL = ∼ κTotal − LσT. The Wiedemann-Franz law, κE = LσT, where L is Lorenz number, is widely used to estimate κE from σ measurements. It is a common practice to treat L as a universal factor with 2.44 × 10−8 WΩK−2 (degenerate limit). However, significant deviations from the degenerate limit (approximately 40% or more for Kane bands) are known to occur for non-degenerate semiconductors where L converges to 1.5 × 10−8 WΩK−2 for acoustic phonon scattering. The decrease in L is correlated with an increase in thermopower (absolute value of Seebeck coefficient (S)). Thus, a first order correction to the degenerate limit of L can be based on the measured thermopower, |S|, independent of temperature or doping. We propose the equation: L=1.5+exp−|S|116 (where L is in 10−8 WΩK−2 and S in μV/K) as a satisfactory approximation for L. This equation is accurate within 5% for single parabolic band/acoustic phonon scattering assumption and within 20% for PbSe, PbS, PbTe, Si0.8Ge0.2 where more complexity is introduced, such as non-parabolic Kane bands, multiple bands, and/or alternate scattering mechanisms. The use of this equation for L rather than a constant value (when detailed band structure and scattering mechanism is not known) will significantly improve the estimation of lattice thermal conductivity.
Bi2Te3 has been recognized as an important cooling material for thermoelectric applications. Yet its thermoelectric performance could still be improved. Here we propose a band engineering strategy by ...optimizing the converging valence bands of Bi2Te3 and Sb2Te3 in the (Bi1−xSbx)2Te3 system when x=0.75. Band convergence successfully explains the sharp increase in density-of-states effective mass yet relatively constant mobility and optical band gap measurement. This band convergence picture guides the carrier concentration tuning for optimum thermoelectric performance. To synthesize homogeneous textured and optimally doped (Bi0.25Sb0.75)2Te3, excess Te was chosen as the dopant. Uniform control of the optimized thermoelectric composition was achieved by zone-melting which utilizes separate solidus and liquidus compositions to obtain zT=1.05 (at 300K) without nanostructuring.
CoSb3-based filled skutterudite has emerged as one of the most viable candidates for thermoelectric applications in automotive industry. However, the scale-up commercialization of such materials is ...still a challenge due to the scarcity and cost of constituent elements. Here we study Ce, the most earth abundant and low-cost rare earth element as a single-filling element and demonstrate that, by solubility design using a phase diagram approach, the filling fraction limit (FFL) x in CexCo4Sb12 can be increased more than twice the amount reported previously (x=0.09). This ultra-high FFL (x=0.20) enables the optimization of carrier concentration such that no additional filling elements are needed to produce a state of the art n-type skutterudite material with a zT value of 1.3 at 850 K before nano-structuring. The earth abundance and low cost of Ce would potentially facilitate a widespread application of skutterudites.
Abstract
The central theme of valleytronics lies in the manipulation of valley degree of freedom for certain materials to fulfill specific application needs. While thermoelectric (TE) materials rely ...on carriers as working medium to absorb heat and generate power, their performance is intrinsically constrained by the energy valleys to which the carriers reside. Therefore, valleytronics can be extended to the TE field to include strategies for enhancing TE performance by engineering band structures. This review focuses on the recent progress in TE materials from the perspective of valleytronics, which includes three valley parameters (valley degeneracy, valley distortion, and valley anisotropy) and their influencing factors. The underlying physical mechanisms are discussed and related strategies that enable effective tuning of valley structures for better TE performance are presented and highlighted. It is shown that valleytronics could be a powerful tool in searching for promising TE materials, understanding complex mechanisms of carrier transport, and optimizing TE performance.
Human neurodegenerative disorders often exhibit similar pathologies, suggesting a shared aetiology. Key pathological features of Parkinson's disease (PD) are also observed in other neurodegenerative ...diseases. Pantothenate Kinase-Associated Neurodegeneration (PKAN) is caused by mutations in the human PANK2 gene, which catalyzes the initial step of de novo CoA synthesis. Here, we show that fumble (fbl), the human PANK2 homolog in Drosophila, interacts with PINK1 genetically. fbl and PINK1 mutants display similar mitochondrial abnormalities, and overexpression of mitochondrial Fbl rescues PINK1 loss-of-function (LOF) defects. Dietary vitamin B5 derivatives effectively rescue CoA/acetyl-CoA levels and mitochondrial function, reversing the PINK1 deficiency phenotype. Mechanistically, Fbl regulates Ref(2)P (p62/SQSTM1 homolog) by acetylation to promote mitophagy, whereas PINK1 regulates fbl translation by anchoring mRNA molecules to the outer mitochondrial membrane. In conclusion, Fbl (or PANK2) acts downstream of PINK1, regulating CoA/acetyl-CoA metabolism to promote mitophagy, uncovering a potential therapeutic intervention strategy in PD treatment.
ER-phagy, a selective autophagy targeting the endoplasmic reticulum (ER) for lysosomal degradation through cargo receptors, plays a critical role in ER quality control and is linked to various ...diseases. However, its physiological and pathological roles remain largely unclear due to a lack of animal model studies. This study establishes Drosophila as an in vivo ER-phagy model. Starvation triggers ER-phagy across multiple fly tissues. Disturbing ER-phagy by either globally upregulating or downregulating ER-phagy receptors, Atl or Rtnl1, harms the fly. Notably, moderate upregulation of ER-phagy in fly brains by overexpressing Atl or Rtnl1 significantly attenuates age-associated neurodegenerations. Furthermore, in a Drosophila model of Alzheimer’s disease expressing human amyloid precursor protein (APP), impaired ER-phagy is observed. Enhancing ER-phagy in the APP-expressing fly brain facilitates APP degradation, significantly alleviating disease symptoms. Therefore, our findings suggest that modulating ER-phagy may offer a therapeutic strategy to treat aging and diseases associated with ER protein aggregation.
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•Downregulating ER-phagy receptors Atl or Rtnl1 impairs ER-phagy and leads to neurodegeneration•Neuronal overexpression of Atl or Rtnl1 enhances ER-phagy, improving organismal health•Accumulation of APP in the ER impairs ER-phagy•Neuronal overexpression of Atl or Rtnl1 reduces APP toxicity by enhancing its degradation
Mou et al. established Drosophila as an in vivo model to study ER-phagy. Neuronal upregulation of ER-phagy attenuates age-related degeneration and reduces toxicity of the Alzheimer’s disease-related protein APP, suggesting potential therapeutic strategies targeting ER-phagy for aging and protein-aggregation-related diseases.
N-Type skutterudites, such as Yb x Co4Sb12, have recently been shown to exhibit high valley degeneracy with possible band convergence, explaining the excellent thermoelectric efficiency of these ...materials. Using a combined theoretical and experimental approach involving temperature-dependent synchrotron diffraction, molecular orbital diagrams, and computational studies, the chemical nature of critical features in the band structure is highlighted. We identify how n-type doping on the filler site induces structural changes that are observed in both the diffraction data and computational results. Additionally, we show how chemical n-type doping slightly alters the electronic band structure, moving the high-valley degeneracy secondary conduction band closer to the primary conduction band and thus inducing band convergence.
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