An official website of the United States government
Abstract To investigate the role of interlayers on the growth, microstructure, and physical properties of 3D nanocomposite frameworks, a set of novel 3D vertically aligned nanocomposite (VAN) frameworks are assembled by a relatively thin interlayer (M) sandwiched by two consecutively grown La0.7Sr0.3MnO3(LSMO)‐ZnO VANs layers. ZnO nanopillars from the two VAN layers and the interlayer (M) create a heterogeneous 3D frame embedded in the LSMO matrix. The interlayer (M) includes yttria‐stabilized zirconia (YSZ), CeO2, SrTiO3, BaTiO3, and MgO with in‐plane matching distances increasing from ≈3.63 to ≈4.21 Å, and expected in‐plane strains ranging from tensile (≈8.81% on YSZ interlayer) to compressive (≈–6.23% on MgO interlayer). The metal‐insulator transition temperature increases from ≈133 K (M = YSZ) to ≈252 K (M = MgO), and the low‐field magnetoresistance peak value is tuned from ≈36.7% to ≈20.8%. The 3D heterogeneous frames empower excellent tunable magnetotransport properties and promising potentials for microstructure‐enabled applications.
more »
« less
Design of All‐Oxide Multilayers with High‐Temperature Stability Toward Future Thermophotovoltaic Applications
Abstract Thermophotovoltaic (TPV) technology converts heat into electricity using thermal radiation. Increasing operating temperature is a highly effective approach to improving the efficiency of TPV systems. However, most reported TPV selective emitters degrade rapidly via. oxidation as operating temperatures increase. To address this issue, replacing nanostructured oxide‐metal films with oxide–oxide films is a promising way to greatly limit oxidation, even under high‐temperature conditions. This study introduces new all‐oxide photonic crystal designs for high‐temperature stable TPV systems, overcoming limitations of metal phases and offering promising material choices. The designs utilize both yttria‐stabilized zirconia (YSZ)/MgO and CeO2/MgO combinations with a multilayer structure and stable high‐quality growth. Both designsexhibit positive optical dielectric constants with tunable reflectivity, measured via optical characterization. Thermal stability testing using in situ heating X‐ray diffraction (XRD) suggests high‐temperature stability (up to 1000 °C) of both YSZ/MgO and CeO2/MgO systems. The results demonstrate a new and promising approach to improve the high‐temperature stability of TPV systems, which can be extended to a wide range of material selection and potential designs.
more »
« less
- Award ID(s):
- 2016453
- PAR ID:
- 10487212
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Advanced Materials Interfaces
- Volume:
- 11
- Issue:
- 5
- ISSN:
- 2196-7350
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
-
The unique redox properties and high oxygen capacity of nanostructured CeO2demonstrate a wide range of applications, such as electrolytes for solid oxide fuel cells, gas sensors, and catalysis for automotive exhaust gas. Most CeO2nanomaterials are prepared by chemical synthesis or hard templating methods. An effective way to obtain highly textured, small‐radius dimensions with high specific surface area remains challenging. Here, highly textured CeO2nanostructures with various shapes ranging from nanowires to nanoporous thin films are successfully synthesized. Vertically aligned nanocomposites (VANs) of Sr3Al2O6(SAO) and CeO2are synthesized first while varying concentration ratio between them. Once the SAO is dissolved in water, the remaining CeO2forms distinct nanostructures. The thermal stability of the nanostructured CeO2is evaluated byin situheating XRD and thermal annealing tests. This method provides an alternative approach to preparing nanostructured CeO2without toxic chemical solutions or complex micro/nanofabrication techniques. These results present a novel approach to prepare nanostructured CeO2for future sensing and energy device applications.more » « less
-
Abstract We report a single atom Rh1/CeO2catalyst prepared by the high temperature (800 °C) atom trapping (AT) method which is stable under both oxidative and reductive conditions. Infrared spectroscopic and electron microscopy characterization revealed the presence of exclusively ionic Rh species. These ionic Rh species are stable even under reducing conditions (CO at 300 °C) due to the strong interaction between Rh and CeO2achieved by the AT method, leading to high and reproducible CO oxidation activity regardless of whether the catalyst is reduced or oxidized. In contrast, ionic Rh species in catalysts synthesized by a conventional impregnation approach (e. g., calcined at 350 °C) can be readily reduced to form Rh nanoclusters/nanoparticles, which are easily oxidized under oxidative conditions, leading to loss of catalytic performance. The single atom Rh1/CeO2catalysts synthesized by the AT method do not exhibit changes during redox cycling hence are promising catalysts for emission control where redox cycling is encountered, and severe oxidation (fuel cut) leads to loss of performance.more » « less
-
Abstract Encapsulation of metal nanoparticles within oxide materials has been shown as an effective strategy to improve activity, selectivity, and stability in several catalytic applications. Several approaches have been proposed to encapsulate nanoparticles, such as forming core‐shell structures, growing ordered structures (zeolites or metal‐organic frameworks) on nanoparticles, or directly depositing support materials on nanoparticles. Here, a general nanocasting method is demonstrated that can produce diverse encapsulated metal@oxide structures with different compositions (Pt, Pd, Rh) and multiple types of oxides (Al2O3, Al2O3‐CeO2, ZrO2, ZnZrOx, In2O3, Mn2O3, TiO2) while controlling the size and dispersion of nanoparticles and the porous structure of the oxide. Metal@polymer structures are first prepared, and then the oxide precursor is infiltrated into such structures and the resulting material is calcined to form the metal@oxide structures. Most Pt@oxides catalysts show similar catalytic activity, demonstrating the availability of surface Pt sites in the encapsulated structures. However, the Pt@Mn2O3sample showed much higher CO oxidation activity, while also being stable under aging conditions. This work demonstrated a robust nanocasting method to synthesize metal@oxide structures, which can be utilized in catalysis to finely tune metal‐oxide interfaces.more » « less
-
Metal–halide perovskites are promising candidates to advance optoelectronic devices but are known to suffer from rapid material degradation. Here we demonstrate that nanoconfinement is an effective strategy for the long-term stabilization of metal–halide perovskite MAPbI 3 crystals against humidity-induced degradation and temperature-induced polymorph transitions. Two-dimensional X-ray diffraction patterns of MAPbI 3 films reveal an unprecedented air-stability of up to 594 days in non-chemically modified, non-passivated MAPbI 3 films deposited on substrates imposing complete 2D confinement on the tens of nanometers length scale. Temperature-dependent X-ray diffraction analysis and optical spectroscopy further reveal the suppression of temperature-dependent phase transitions in nanoconfined MAPbI 3 crystals. Most notably, the high-temperature cubic phase of MAPbI 3 , typically stable at temperatures above 327 K, remains present until a temperature of 170 K when the perovskite crystals are nanoconfined within the 100 nm diameter pores of anodized aluminum oxide templates. Photoluminescence mapping confirms that nanoconfined MAPbI 3 crystals exhibit spatial uniformity on the tens of microns length scale, suggesting that nanoconfinement is an effective strategy for the formation of high-quality, stable MAPbI 3 crystals across large areas.more » « less
