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Find NASA NTRS and DOE OSTI research on heat transfer and thermal systems. Search heat pipes, cooling and thermal management in report titles and abstracts.

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All sourcesNASA NTRSDOE OSTI
DOE OSTI2018

Thermally Activated Delayed Fluorescence (TADF) Path toward Efficient Electroluminescence in Purely Organic Materials: Molecular Level Insight

Since the seminal work of Tang and Vanslyke in 1987 on small-molecule emitters and that of Friend and co-workers in 1990 on conjugated-polymer emitters, organic light-emitting diodes (OLEDs) have attracted much attention from academia as well as industry, as the OLED market is estimated to reach the $30B mark by the end of 2018. In these first-generation organic emitters, on the basis of simple spin statistics, electrical excitation resulted in the formation of ~25% singlet excitons and ~75% triplet excitons. Radiative decay of the singlet excitons to the singlet ground state leads to a prompt fluorescence emission, while the triplet excitons only lead to weak phosphorescence due to the very small spin-orbit couplings present in purely organic molecules. The consequence is a ca. 75% energy loss, which triggered wide-ranging efforts to try and harvest as many of the triplet excitons as possible. In 1998, Thompson, Forrest, and their co-workers reported second-generation OLED emitters based on coordination complexes with heavy transition metals (e.g., iridium or platinum). Here, the triplet excitons stimulate efficient and fast phosphorescence due to the strong spin-orbit couplings enabled by the heavy-metal atoms. Internal quantum efficiencies (IQE) up to 100% have been reported, which means that for every electron injected into the device, a photon is emitted. Here, while these second-generation emitters are those mainly exploited in current OLED applications, there is strong impetus from both cost and environmental standpoints to find new ways of exploiting purely organic emitters, which in addition can offer greater flexibility to fine tune the electronic and optical properties by exploiting the synthetic organic chemistry toolbox.

36 MATERIALS SCIENCE↗
DOE OSTI2019

In Situ Study of Particle Precipitation in Metal-Doped CeO2 during Thermal Treatment and Ion Irradiation for Emulation of Irradiating Fuels

Metallic particles formed in oxide fuels (e.g., UO 2 ) during neutron irradiation have an adverse impact on fuel performance. A fundamental investigation of particle precipitation is needed to predict the fuel performance and potentially improve fuel designs and operations. In this study, we report on the precipitation of Mo-dominant β-phase particles in polycrystalline CeO 2 (surrogate for UO 2 ) films doped with Mo, Pd, Rh, Ru, and Re (surrogate for Tc). In situ heating scanning transmission electron microscopy indicates that particle precipitation starts at ~1073 K with a limited particle growth to ~10 nm. While particle concentration increases with increasing temperature, particle size remains largely unchanged up to 1273 K. There is a dramatic change in the microstructure following vacuum annealing at 1373 K, probably due to phase transition of reduced cerium oxide. At the high temperature, particles grow up to 75 nm or larger with distinctive facets. The particles are predominantly composed of Mo with a body-centered cubic structure (β phase). An oxide layer was observed after storage at ambient conditions. In situ heating X-ray photoelectron spectroscopy reveals an increasing reduction of Ce charge state from 4+ to 3+ in the doped CeO 2 film at temperatures from 673 to 1273 K. In situ ion irradiation transmission electron microscopy with 2 MeV Al 2+ ions up to a dose of ~20 displacements per atom at nominally room temperature does not lead to precipitation of visible particles. However, irradiation with 1.7 MeV Au 3+ ions to ~10 dpa at 973 K produces ~2 nm sized pure Pd particles; Au 3+ irradiation at 1173 K appears to result in precipitates of ~6 nm in size. Some of the defects produced by ion irradiation could be nucleation sites for precipitation, leading to generation of smaller particles with a higher concentration.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

Stabilizing High Metal Loadings of Thermally Stable Platinum Single Atoms on an Industrial Catalyst Support

Single atom catalysts have attracted attention because of improved atom efficiency, higher reactivity, and better selectivity. A major challenge is to achieve high surface concentrations while preventing these atoms from agglomeration at elevated temperatures. Here we investigate the formation of Pt single atoms on an industrial catalyst support. Using a combination of surface sensitive techniques such as XPS and LEIS, X-ray absorption spectroscopy, electron microscopy, as well as density functional theory, we demonstrate that cerium oxide can support Pt single atoms at high metal loading (3 wt% Pt), without forming any clusters or 3D aggregates when heated in air at 800 °C. The mechanism of trapping involves a reaction of the mobile PtO2 with under-coordinated cerium cations present at CeO2(111) step edges, allowing Pt to achieve a stable square planar configuration. The strong interaction of mobile single atom species with the support, present during catalyst sintering and regeneration, helps explain the sinter-resistance of ceria-supported metal catalysts.

Kunwar, Deepak↗