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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 361 records · Page 20
All sourcesNASA NTRSDOE OSTI
DOE OSTI2017

Lattice Dislocations Enhancing Thermoelectric PbTe in Addition to Band Convergence

Phonon scattering by nanostructures and point defects has become the primary strategy for minimizing the lattice thermal conductivity (κ L ) in thermoelectric materials. However, these scatterers are only effective at the extremes of the phonon spectrum. Recently, it has been demonstrated that dislocations are effective at scattering the remaining mid-frequency phonons as well. In this work, by varying the concentration of Na in Pb 0.97 Eu 0.03 Te, it has been determined that the dominant microstructural features are point defects, lattice dislocations, and nanostructure interfaces. This study reveals that dense lattice dislocations (≈4 × 10 12 cm -2 ) are particularly effective at reducing κ L . When the dislocation concentration is maximized, one of the lowest κ L values reported for PbTe is achieved. Furthermore, due to the band convergence of the alloyed 3% mol. EuTe the electronic performance is enhanced, and a high thermoelectric figure of merit, zT, of ≈2.2 is achieved. This work not only demonstrates the effectiveness of dense lattice dislocations as a means of lowering κL, but also the importance of engineering both thermal and electronic transport simultaneously when designing high-performance thermoelectrics.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Solvent-Free Self-Assembly to the Synthesis of Nitrogen-Doped Ordered Mesoporous Polymers for Highly Selective Capture and Conversion of CO 2

A solvent-free induced self-assembly technology for the synthesis of nitrogen-doped ordered mesoporous polymers (N-OMPs) is developed, which is realized by mixing polymer precursors with block copolymer templates, curing at 140–180 °C, and calcination to remove the templates. This synthetic strategy represents a significant advancement in the preparation of functional porous polymers through a fast and scalable yet environmentally friendly route, since no solvents or catalysts are used. The synthesized N-OMPs and their derived catalysts are found to exhibit competitive CO 2 capacities (0.67–0.91 mmol g -1 at 25 °C and 0.15 bar), extraordinary CO 2 /N 2 selectivities (98–205 at 25 °C), and excellent activities for catalyzing conversion of CO 2 into cyclic carbonate (conversion >95% at 100 °C and 1.2 MPa for 1.5 h). Finally, the solvent-free technology developed in this work can also be extended to the synthesis of N-OMP/SiO 2 nanocomposites, mesoporous SiO 2 , crystalline mesoporous TiO 2 , and TiPO, demonstrating its wide applicability in porous material synthesis.

36 MATERIALS SCIENCE↗
DOE OSTI2018

“Unleaded” Perovskites: Status Quo and Future Prospects of Tin-Based Perovskite Solar Cells

The tremendous interest focused on organic–inorganic halide perovskites since 2012 derives from their unique optical and electrical properties, which make them excellent photovoltaic materials. Pb-based halide perovskite solar cells, in particular, currently stand at a record efficiency of ≈23%, fulfilling their potential toward commercialization. However, because of the toxicity concerns of Pb-based perovskite solar cells, their market prospects are hindered. In principle, Pb can be replaced with other less-toxic, environmentally benign metals. Sn-based perovskites are thus the far most promising alternative due to their very similar and perhaps even superior semiconductor characteristics. Additionally, after years of effort invested in Sn-based halide perovskites, sufficient breakthroughs have finally been achieved that make them the next runners up to the Pb halide perovskites. To help the reader better understand the nature of Sn-based halide perovskites, their optical and electrical properties are systematically discussed. Recent progress in Sn-based perovskite solar cells, focusing mainly on film fabrication methods and different device architectures, and highlighting roadblocks to progress and opportunities for future work are reviewed. Finally, a brief overview of mixed Sn/Pb-based systems with their anomalous yet beneficial optical trends are discussed. The current challenges and a future outlook for Sn-based perovskites are discussed.

14 SOLAR ENERGY↗
DOE OSTI2019

Simultaneous Bottom-Up Interfacial and Bulk Defect Passivation in Highly Efficient Planar Perovskite Solar Cells using Nonconjugated Small-Molecule Electrolytes

Recent perovskite solar cell (PSC) advances have pursued strategies for reducing interfacial energetic mismatches to mitigate energy losses, as well as to minimize interfacial and bulk defects and ion vacancies to maximize charge transfer. In this work, nonconjugated multi-zwitterionic small-molecule electrolytes (NSEs) are introduced, which act not only as charge-extracting layers for barrier-free charge collection at planar triple cation PSC cathodes but also passivate charged defects at the perovskite bulk/interface via a spontaneous bottom-up passivation effect. Implementing these synergistic properties affords NSE-based planar PSCs that deliver a remarkable power conversion efficiency of 21.18% with a maximum V OC = 1.19 V, in combination with suppressed hysteresis and enhanced environmental, thermal, and light-soaking stability. Thus, this work demonstrates that the bottom-up, simultaneous interfacial and bulk trap passivation using NSE modifiers is a promising strategy to overcome outstanding issues impeding further PSC advances.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Enhanced Thermoelectric Properties for PEDOT:PSS/Undoped Ge Thin-Film Bilayered Heterostructures

Modulation doping is one of the strategies to improve thermoelectric power factors of nanocomposites and thin-film bilayered heterostructures by effectively increasing electrical conductivity. Here, it is reported that thin-film heterostructures of heavily doped p-type organic conducting polymer, poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) and undoped thin-film Ge can enhance thermoelectric power factor by modulation doping. The maximum power factor and Seebeck coefficient of the bilayered heterostructures are 154 µW m -1 K -2 and 398 µV K -1 , respectively, corresponding to 47-fold and 41-fold increases compared to those of bulk PEDOT:PSS and 64-fold increase compared to power factor of undoped Ge. The enhancements in power factor and Seebeck coefficient are quantitatively described by the hole transfer from PEDOT:PSS to Ge, which takes into account the band alignment at the interface detected by Kraut's method. Agreement between the simulation and experiment results also implies predictability of thermoelectric performances of nanoscale bilayered heterostructures in general, when band offset, Fermi level, and individual electronic properties are available. This work can be further extended to predict performance of other nanoscale combinations of thermoelectric and other electronic materials in general.

charge transport↗
DOE OSTI2015

Enhancement of Thermoelectric Performance of n-Type PbSe by Cr Doping with Optimized Carrier Concentration

Ti, V, Cr, Nb, and Mo are found to be effective at increasing the Seebeck coefficient and power factor of n-type PbSe at temperatures below 600 K. It is found that the higher Seebeck coefficients and power factors are due to higher Hall mobility ≈1000 cm 2 V -1 s -1 at lower carrier concentration. A larger average ZT value (relevant for applications) can be obtained by an optimization of carrier concentration to ≈10 18 -10 19 cm -3 . Even though the highest room temperature power factor ≈3.3 × 10 -3 W m -1 K -2 is found in 1 at% Mo-doped PbSe, the highest ZT is achieved in Cr-doped PbSe. Combined with the lower thermal conductivity, ZT is improved to ≈0.4 at room temperature and peak ZTs of ≈1.0 are observed at ≈573 K for Pb 0.9925 Cr 0.0075 Se and ≈673 K for Pb 0.995 Cr 0.005 Se. Finally, the calculated device efficiency of Pb 0.995 Cr 0.005 Se is as high as ≈12.5% with cold side 300 K and hot side 873 K, higher than those of all the n-type PbSe materials reported in the literature.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Grain Boundary Engineering for Achieving High Thermoelectric Performance in n-Type Skutterudites

Grain or phase boundaries play a critical role in the carrier and phonon transport in bulk thermoelectric materials. Previous investigations about controlling boundaries primarily focused on the reducing grain size or forming nanoinclusions. Herein, liquid phase compaction method is first used to fabricate the Yb–filled CoSb 3 with excess Sb content, which shows the typical feature of low–angle grain boundaries with dense dislocation arrays. Seebeck coefficients show a dramatic increase via energy filtering effect through dislocation arrays with little deterioration on the carrier mobility, which significantly enhances the power factor over a broad temperature range with a high room–temperature value around 47 μW cm –2 K –1 . Simultaneously, the lattice thermal conductivity could be further suppressed via scattering phonons via dense dislocation scattering. As a result, the highest average figure of merit ZT of ≈1.08 from 300 to 850 K could be realized, comparable to the best reported result of single or triple–filled Skutterudites. Furthermore, this work clearly points out that low–angle grain boundaries fabricated by liquid phase compaction method could concurrently optimize the electrical and thermal transport properties leading to an obvious enhancement of both power factor and ZT .

36 MATERIALS SCIENCE↗
DOE OSTI2017

Highly Conductive, Lightweight, Low-Tortuosity Carbon Frameworks as Ultrathick 3D Current Collectors

The growing demand for advanced energy storage techniques and devices has driven the energy storage market to strive for higher performance, longer cycling life, and better safety. Thick electrode design enabling more electroactive materials has the potential to significantly improve the energy density on device level yet faces major challenges of slow ion transport and high deformability. In this work, inspired by natural wood materials with aligned channels along the tree growth direction, a highly conductive, lightweight, and low-tortuosity carbon framework (CF) directly carbonized from natural wood as an ultrathick 3D current collector is demonstrated. Benefiting from the uniqueness of the multichanneled CF, an ultrathick 3D electrode of lithium iron phosphate filled carbon framework with a large thickness of 800 µm and active material mass loading of 60 mg cm -2 delivers a rational capacity of 7.6 mAh cm -2 (95 Ah L -1 based on volume), long cycling life, and lower deformability with enhanced mechanical properties. This work presents a design concept for thick electrode toward high performance energy storage devices that are not limited to lithium-ion batteries.

09 BIOMASS FUELS↗
DOE OSTI2017

Band-like Charge Photogeneration at a Crystalline Organic Donor/Acceptor Interface

Organic photovoltaic cells possess desirable practical characteristics, such as the potential for low-cost fabrication on flexible substrates, but they lag behind their inorganic counterparts in performance due in part to fundamental energy loss mechanisms, such as overcoming the charge transfer (CT) state binding energy when photogenerated charge is transferred across the donor/acceptor interface. However, recent work has suggested that crystalline interfaces can reduce this binding energy due to enhanced CT state delocalization. Solar cells based on rubrene and C 60 are investigated as an archetypal system because it allows the degree of crystallinity to be moldulated from a highly disordered to highly ordered system. Using a postdeposition annealing method to transform as-deposited amorphous rubrene thin films into ones that are highly crystalline, it is shown that the CT state of a highly crystalline rubrene/C 60 heterojunction undergoes extreme delocalization parallel to the interface leading to a band-like state that exhibits a linear Stark effect. This state parallels the direct charge formation of inorganic solar cells and reduces energetic losses by 220 meV compared with 12 other archetypal heterojunctions reported in the literature.

14 SOLAR ENERGY↗
DOE OSTI2018

Photoactive Blend Morphology Engineering through Systematically Tuning Aggregation in All-Polymer Solar Cells

Polymer aggregation plays a critical role in the miscibility of materials and the performance of all-polymer solar cells (APSCs). However, many aspects of how polymer texturing and aggregation affect photoactive blend film microstructure and photovoltaic performance are poorly understood. Here the effects of aggregation in donor–acceptor blends are studied, in which the number-average molecular weights (Mns) of both an amorphous donor polymer, poly[4,8-bis(5-(2-ethylhexyl)thiophen-2-yl)benzo[1,2-b;4,5-b]dithiophene-2,6-diyl-alt-(4-(2-ethylhexyl)-3-fluorothieno[3,4-b]thiophene-)-2-carboxylate-2-6-diyl)] (PBDTT-FTTE) and a semicrystalline acceptor polymer, poly{[N,N'-bis(2-octyldodecyl)naphthalene-1,4,5,8-bis(dicarboximide)-2,6-diyl]-alt-5,5'-(2,2'-bithiophene)} (P(NDI2OD-T2)) are systematically varied. The photovoltaic performance is correlated with active layer microstructural and optoelectronic data acquired by in-depth transmission electron microscopy, grazing incidence wide-angle X-ray scattering, thermal analysis, and optical spectroscopic measurements. Coarse-grained modeling provides insight into the effects of polymer aggregation on the blend morphology. Notably, the computed average distance between the donor and the acceptor polymers correlates well with solar cell photovoltaic metrics such as short-circuit current density (Jsc) and represents a useful index for understanding/predicting active layer blend material intermixing trends. Importantly, these results demonstrate that for polymers with different texturing tendencies (amorphous/semicrystalline), the key for optimal APSC performance, photovoltaic blend morphology can be controlled via both donor and acceptor polymer aggregation.

bio-inspired↗
DOE OSTI2018

Temperature Dependent n-Type Self Doping in Nominally 19-Electron Half-Heusler Thermoelectric Materials

The discovery of a semiconducting ground state X y YZ (y = 0.8 or 0.75) in nominally 19-electron half-Heusler materials warrants a closer look at their apparently metallic properties that often make them good thermoelectric (TE) materials. Here, by systematically investigating the temperature dependence of off-stoichiometry (x) in V 0.8+x CoSb, Nb 0.8+x CoSb, and Ti 0.75+x NiSb it is found that x invariably increases with increasing temperature, leading to an n-type self-doping behavior. In addition, there is also a large phase width (range of x) associated with each phase that is temperature dependent. Thus, unlike in typical 18-electron half-Heuslers (e,g, TiNiSn), the temperature dependence of vacancy and carrier concentration (n) in nominally 19-electron half-Heuslers links its transport properties to synthesis conditions. The temperature dependence of x and n are understood using density functional theory based defect energies (E d ) and phase diagrams. E d are calculated for 21 systems which can be used in predicting solubility in this family of compounds. Using this simple strategy, suitable composition and temperature synthesis conditions are devised for obtaining an optimized n to engineer TE properties in phase-pure V 0.8+x CoSb, and the previously unexplored Ta 0.8+x CoSb.

19-electron half-Heuslers↗
DOE OSTI2019

A quantitative study of the structure-activity relationship in hierarchical zeolites using liquid-phase reactions

Micro/meso/macroporous (hierarchical) zeolites show remarkable catalytic performance for reactions involving bulky reactants. However, quantitative assessment of the microstructural characteristics contributing to the observed performance remains elusive. Here, structure–activity relationships are established for a set of micro/mesoporous self-pillared pentasil (SPP) zeolites using two parallel liquid-phase reactions (benzyl alcohol alkylation and self-etherification) based on analysis of mass transport and reaction kinetics. A reaction–diffusion mathematical model is developed that quantitatively assigns the catalytic contributions of the external surface and micropores of SPP zeolites for these reactions. In addition, the effect of the zeolite external surface structure on the corresponding catalytic activity is quantitatively assessed by comparing SPP zeolites (with MFI structure) with MCM-22 (with MWW structure). This work demonstrates that reaction–diffusion modeling allows quantitative description of the catalytic performance of hierarchical zeolites and provides a model reaction to assess nm-sized characteristic diffusion lengths in MFI.

bio-inspired↗
DOE OSTI2017

High Thermoelectric Performance of New Rhombohedral Phase of GeSe stabilized through Alloying with AgSbSe 2

GeSe is a IV–VI semiconductor, like the excellent thermoelectric materials PbTe and SnSe. Orthorhombic GeSe has been predicted theoretically to have good thermoelectric performance but is difficult to dope experimentally. Like PbTe, rhombohedral GeTe has a multivalley band structure, which is ideal for thermoelectrics and also promotes the formation of Ge vacancies to provide enough carriers for electrical transport. Herein, we investigate the thermoelectric properties of GeSe alloyed with AgSbSe 2 , which stabilizes a new rhombohedral structure with higher symmetry that leads to a multivalley Fermi surface and a dramatic increase in carrier concentration. The z T of GeAg 0.2 Sb 0.2 Se 1.4 reaches 0.86 at 710 K, which is 18 times higher than that of pristine GeSe and over four times higher than doped orthorhombic GeSe. Our results open a new avenue towards developing novel thermoelectric materials through crystal phase engineering using a strategy of entropy stabilization of high-symmetry alloys.

36 MATERIALS SCIENCE↗
DOE OSTI2015

Hematite‐Based Solar Water Splitting in Acidic Solutions: Functionalization by Mono‐ and Multilayers of Iridium Oxygen‐Evolution Catalysts

Abstract Solar water splitting in acidic solutions has important technological implications, but has not been demonstrated to date in a dual absorber photoelectrochemical cell. The lack of functionally stable water‐oxidation catalysts (WOCs) in acids is a key reason for this slow development. The only WOCs that are stable at low pH are Ir‐based systems, which are typically too expensive to be implemented broadly. It is now shown that this deficiency may be corrected by applying an ultra‐thin monolayer of a molecular Ir WOC to hematite for solar water splitting in acidic solutions. The turn‐on voltage is observed to shift cathodically by 250 mV upon the application of a monolayer of the molecular Ir WOC. When the molecular WOC is replaced by a heterogeneous multilayer derivative, stable solar water splitting for over 5 h is achieved with near‐unity Faradaic efficiency.

Li, Wei↗
DOE OSTI2016

Thinking Like a Chemist: Intuition in Thermoelectric Materials

Abstract The coupled transport properties required to create an efficient thermoelectric material necessitates a thorough understanding of the relationship between the chemistry and physics in a solid. We approach thermoelectric material design using the chemical intuition provided by molecular orbital diagrams, tight binding theory, and a classic understanding of bond strength. Concepts such as electronegativity, band width, orbital overlap, bond energy, and bond length are used to explain trends in electronic properties such as the magnitude and temperature dependence of band gap, carrier effective mass, and band degeneracy and convergence. The lattice thermal conductivity is discussed in relation to the crystal structure and bond strength, with emphasis on the importance of bond length. We provide an overview of how symmetry and bonding strength affect electron and phonon transport in solids, and how altering these properties may be used in strategies to improve thermoelectric performance.

Zeier, Wolfgang G.↗