Impact of IrRu oxygen evolution reaction catalysts on Pt nanostructured thin films under start-up/shutdown cycling
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Cullen, David A.↗
SEARCH · Engineering Papers
Results for “Nanostructure”
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Enhanced thermal coarsening resistance in a nanostructured aluminum-cerium alloy produced by additiv
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Henderson, Hunter B.↗
Comprehensive Magnetic Study of Nanostructured Mesoporous Manganese Oxide Materials and Implications for Catalytic Behavior
Magnetic behavior of nanostructured mesoporous manganese oxide materials, designated UCT-1 and UCT-18, were studied using a combination of superconducting quantum interference device (SQUID) magnetometry and 55 Mn zero-field spin–echo nuclear magnetic resonance (NMR). Curie–Weiss fits to the magnetic susceptibility for the UCT-1 and UCT-18 samples calcined at 550 °C yielded paramagnetic moment values consistent with spin-only Mn 3+ ions in the α-Mn 2 O 3 phase ( S = 2, 4.90 μ B ). However, the magnetization and NMR results reported here clearly identify a small amount of the Mn 3 O 4 second phase (ferrimagnetic with T C ≈ 43 K) that does not appear in X-ray diffraction (XRD). We report the study resulted in the observation of fascinating magnetic behavior: (1) exchange bias, which occurs in cases where a ferromagnetic (or ferrimagnetic) phase forms a boundary with an antiferromagnetic phase and (2) a magnetic contribution attributed to uncompensated spins on the surfaces of the α-Mn 2 O 3 nanoparticles. The presence of Mn 3 O 4 and the interplay of Mn 3+ and Mn 2+ impact the catalytic properties.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Absence of Nanostructuring in NaPb m SbTe m+2 : Solid Solutions with High Thermoelectric Performance in the Intermediate Temperature Regime
Thermoelectric devices directly convert heat into electrical energy and are highly desired for emerging applications in waste heat recovery. Currently, PbTe based compounds are the leading thermoelectric materials in the intermediate temperature regime (~800 K); however, integration into commercial devices has been limited. This is largely because the performance of PbTe, which is maximized ~900 K, is too low over the temperatures of interest for most potential commercial applications (generally under 600 K). Improving the low temperature performance of PbTe based materials is therefore critical to achieve usage outside of existing niche applications. Here, we provide an in-depth study of the cubic NaPb m SbTe m+2 system of compounds (m = 1-20) and report that it is an excellent class of low- to medium-temperature thermoelectrics when m = 10-20. Here, we show that the as-cast polycrystalline ingots exhibit degenerate p-type conduction and high maximum ZTs of 1.2-1.4 at 650 K when m = 6-20. Because the ingots are found to be extremely brittle, we utilize spark plasma sintering (SPS) to prepare more mechanically robust samples, and surprisingly, find that SPS results in an undesired change in charge transport toward n-type behavior. We show this unanticipated transition from p-type behavior as ingots to n-type after SPS is due to dissolution of secondary phases that are present in the ingots into the primary matrix during the SPS process, resulting in a transformation from an inhomogeneous state to a solid solution without any observable evidence of nanoscale precipitation. This is in sharp contrast to the seemingly similar AgPb m SbTe m+2 (LAST) system, which is heavily nanostructured. The SPSed NaPb m SbTe m+2 is doped p-type by tuning the cation stoichiometry, i.e., Na 1+x Pb m-x Sb 1-y Te m+2 . The optimized compounds have very low lattice thermal conductivities of 1.1-0.55 W·m -1 ·K -1 over 300-650 K, which enhances the low intermediate temperature performance and gives rise to maximum ZT values up to 1.6 at 673 K as well as an excellent ZT avg of 1.1 over 323-673 K for m = 10, 20, making Na 1+x Pb m-x Sb 1-y Te m+2 among the highest performing PbTe-based thermoelectrics under 650 K.
Electrical conductivity↗
Computational strategies for design and discovery of nanostructured thermoelectrics
Abstract The contribution of theoretical calculations and predictions in the development of advanced high-performance thermoelectrics has been increasingly significant and has successfully guided experiments to understand as well as achieve record-breaking results. In this review, recent developments in high-performance nanostructured bulk thermoelectric materials are discussed from the viewpoint of theoretical calculations. An effective emerging strategy for boosting thermoelectric performance involves minimizing electron scattering while maximizing heat-carrying phonon scattering on many length scales. We present several important strategies and key examples that highlight the contributions of first-principles-based calculations in revealing the intricate but tractable relationships for this synergistic optimization of thermoelectric performance. The integrated optimization approach results in a fourfold design strategy for improved materials: (1) a significant reduction of the lattice thermal conductivity through multiscale hierarchical architecturing, (2) a large enhancement of the Seebeck coefficient through intramatrix electronic band convergence engineering, (3) control of the carrier mobility through band alignment between the host and second phases, and (4) design of intrinsically low-thermal-conductivity materials by maximizing vibrational anharmonicity and acoustic-mode Gruneisen parameters. These combined effects serve to enhance the power factor while reducing the lattice thermal conductivity. This review provides an improved understanding of how theory is impacting the current state of this field and helps to guide the future search for high-performance thermoelectric materials.
36 MATERIALS SCIENCE↗
Flow and extraction of energy and charge carriers in hybrid plasmonic nanostructures
Strong interactions of electromagnetic fields with plasmonic nanomaterials have been exploited in various applications. These applications have centred on plasmon-enhanced scattering rates in nearby molecules or plasmon-induced heating. A question that has emerged recently is whether it is possible to use plasmonic nanostructures in a range of hot electron (hole) applications, including photocatalysis, photovoltaics and photodetection. These applications require coupling of a plasmonic component, which amplifies the interaction of light with the material, to an attached non-plasmonic component that extracts this energy in the form of electronic excitations to perform a function. Here, in this Perspective, we discuss recent work in the emerging field of hybrid plasmonics. We focus on fundamental questions related to the nanoscopic flow of energy and excited charge carriers in these multicomponent materials. We also address critical misconceptions, challenges and opportunities that require more attention.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Modeling of threshold and dynamics behavior of organic nanostructured lasers
Organic dye molecules offer significant potential as gain media in the emerging field of optical amplification and lasing at subwavelength scales. In this article, we investigate the laser dynamics in systems comprising subwavelength-structured cavities that incorporate organic dyes. To this end, we have developed a comprehensive theoretical framework able to accurately describe the interaction of organic molecules with any arbitrary photonic structure to produce single-mode lasing. The model provides explicit analytic expressions of the threshold and slope efficiency that characterize this class of lasers, and also the duration over which lasing action can be sustained before the dye photobleaches. Both the physical properties of the dyes and the optical properties of the cavities are considered. We also systematically studied the feasibility of achieving lasing action under continuous-wave excitation in optically pumped monolithic organic dye lasers. This study suggests routes to realize an organic laser that can potentially lase with a threshold of only a few W cm -2 . In conclusion, our work puts forward a theoretical formalism that could enable the advancement of nanostructured organic-based light emitting and sensing devices.
36 MATERIALS SCIENCE↗
Excitation wavelength dependent photon anti-bunching/bunching from single quantum dots near gold nanostructures
Here, we aim to investigate the change in photon emission statistics of single CdSe/CdS core/shell quantum dots (QDs) on dielectric modified gold nanoparticle (NP) substrates as a function of the excitation wavelength. Photons emitted from single QDs are typically “anti-bunched” and are independent of the excitation wavelength. However, when QDs are coupled to plasmonic substrates, even at the low excitation power regime, we observed a significant change in photoluminescence emission behavior of single QDs; i.e. the emission transformed from incomplete photon anti-bunched to bunched when the excitation was changed from “off” to “on” plasmon resonance. Theoretical studies based on electrodynamics modeling suggested that for the QD–Au NP system, the quantum yield of single excitons decreases while that of biexcitons increases. In addition, when excited at the “on” resonance condition, the absorption is highly enhanced, resulting in an increased population of higher order excitons of the QDs. The higher order exciton emission was directly observed as an additional peak appeared at the blue side of the exciton peak of single QDs. The combined effect of the change in quantum yield and the increase in the absorption cross-section switches the photons emitted by single QDs from anti-bunched to bunched. These results provided direct evidence that not only the plasmonic nanostructures but also the excitation wavelength can effectively control the photon emission statistics of single QDs in the hybrid metal–semiconductor system. Manipulating the multiexciton–plasmon interaction in a hybrid complex like this could possibly open up new doors for applications such as entangled photon pair generation and plasmon-enhanced optoelectronic devices.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
On the importance of optical phonons to thermal conductivity in nanostructures
The contribution of optical phonons to thermal conductivity has typically been ignored. However, when the system size decreases to the nanoscale regime, optical phonons are no longer negligible. The contributions of different phonon polarizations to the thermal conductivity of silicon are discussed based on the phonon lifetimes extracted from a first principles approach. The results indicate that around room temperature, optical phonons can contribute over 20% to the thermal conductivity of nanostructures as compared to 5% in bulk materials. In addition, the temperature and size dependence of the contributions from acoustic and optical phonons are fully explored.
42 ENGINEERING↗
Femtosecond laser-induced nanostructure formation in Sb 2 Te 3
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charge transport↗
Real time x-ray studies during nanostructure formation on silicon via low energy ion beam irradiation using ultrathin iron films
Real time grazing incidence small angle x-ray scattering and x-ray fluorescence (XRF) are used to elucidate nanodot formation on silicon surfaces during low energy ion beam irradiation of ultrathin iron-coated silicon substrates. Four surface modification stages were identified: (1) surface roughening due to film erosion, (2) surface smoothing and silicon-iron mixing, (3) structure formation, and (4) structure smoothing. The results conclude that 2.5 Multiplication-Sign 10{sup 15} iron atoms in a 50 nm depth triggers surface nanopatterning with a correlated nanodots distance of 25 nm. Moreover, there is a wide window in time where the surface can have correlated nanostructures even after the removal of all the iron atoms from the sample as confirmed by XRF and ex-situ x-ray photoelectron spectroscopy (XPS). In addition, in-situ XPS results indicated silicide formation, which plays a role in the structure formation mechanism.
77 NANOSCIENCE AND NANOTECHNOLOGY↗
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. 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.
30 DIRECT ENERGY CONVERSION↗
High throughput nanostructure-initiator mass spectrometry screening of microbial growth conditions for maximal β-glucosidase production
Production of biofuels via enzymatic hydrolysis of complex plant polysaccharides is a subject of intense global interest. Microbial communities are known to express a wide range of enzymes necessary for the saccharification of lignocellulosic feedstocks and serve as a powerful reservoir for enzyme discovery. However, the growth temperature and conditions that yield high cellulase activity vary widely, and the throughput to identify optimal conditions has been limited by the slow handling and conventional analysis. A rapid method that uses small volumes of isolate culture to resolve specific enzyme activity is needed. In this work, a high throughput nanostructure-initiator mass spectrometry (NIMS)-based approach was developed for screening a thermophilic cellulolytic actinomycete, Thermobispora bispora , for β-glucosidase production under various growth conditions. Media that produced high β-glucosidase activity were found to be I/S + glucose or microcrystalline cellulose (MCC), Medium 84 + rolled oats, and M9TE + MCC at 45°C. Supernatants of cell cultures grown in M9TE + 1% MCC cleaved 2.5 times more substrate at 45°C than at all other temperatures. While T. bispora is reported to grow optimally at 60°C in Medium 84 + rolled oats and M9TE + 1% MCC, approximately 40% more conversion was observed at 45°C. This high throughput NIMS approach may provide an important tool in discovery and characterization of enzymes from environmental microbes for industrial and biofuel applications.
59 BASIC BIOLOGICAL SCIENCES↗
In situ TEM observation of calcium silicate hydrate nanostructure at high temperatures
Fire poses a substantial threat to concrete structures because calcium silicate hydrate (C-S-H) is not thermally stable at high temperatures. Herein, in situ TEM at temperatures from 20 to 800 °C was conducted to study the thermal-induced structural changes in C-S-H. We captured C-S-H shrinks at an average rate of 0.02 μm{sup 2}/{sup o}C upon heating with three stages observed, including induction, constant, and rapid periods. Our observation revealed that an 800 nm pore could be healed during pore structure evolution owing to the reconstruction and deformation among C-S-H blocks. The Ca/Si ratio was dropped at higher temperatures because of the leakage of calcium ions from the C-S-H structure to form CaO precipitates. The temperature-driven phase transformation and degradation were also detected using electron diffraction that C-S-H was transformed into metastable calcium silicate minerals above 800 °C. This work provides insights into the nanoscale transformation of C-S-H at high temperatures.
36 MATERIALS SCIENCE↗
Nanostructures of Liquid Crystal Phases in Mixtures of Bent-core and Rod-shaped Molecules
We report small angle x-ray scattering (SAXS) studies of isotropic, nematic, and smectic mesophases formed by binary mixtures of bent-core (BC) and rod-shaped (RS) molecules. While optical studies indicate that the components are fully miscible, SAXS reveals fascinating structures that are consistent with segregation on a nanoscopic scale. We find that tilted smectic clusters, which have been previously reported in both the nematic and isotropic states of the pure BC materials, are also present in mixtures with up to 50 wt% of the RS compound; this is consistent with previous dielectric and flexoelectric studies on such mixtures. Unexpectedly in this concentration range the clusters are present in the isotropic and in the induced smectic phase range, as well as throughout the nematic phase. The results in the smectic phase also reveal complex layering phenomena, providing important insight into the interaction between bent and rod-shaped molecules. These studies will be crucial in the design of promising new functional nanomaterials.
36 MATERIALS SCIENCE↗
Core–shell PdPb@Pd aerogels with multiply-twinned intermetallic nanostructures: facile synthesis with accelerated gelation kinetics and their enhanced electrocatalytic properties
Delicately engineering well-defined noble metal aerogels with favorable structural and compositional features is of vital importance for wide applications. Here, we reported a one-pot and facile method for synthesizing core–shell PdPb@Pd hydrogels/aerogels with multiply-twinned grains and an ordered intermetallic phase using sodium hypophosphite as a multifunctional reducing agent. Due to the accelerated gelation kinetics induced by increased reaction temperature and the specific function of sodium hypophosphite, the formation of hydrogels can be completed within 4 h. As a result, owing to their unique porous structure and favorable geometric and electronic effects, the optimized PdPb@Pd aerogels exhibit enhanced electrochemical performance towards ethylene glycol oxidation with a mass activity of 5.8 times higher than Pd black.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Magnetic interaction reversal in watermelon nanostructured Cr-doped Fe nanoclusters
Cr-doped core-shell Fe/Fe-oxide nanoclusters (NCs) were synthesized at varied atomic percentages of Cr from 0 at. % to 8 at. %. The low concentrations of Cr (<10 at. %) were selected in order to inhibit the complete conversion of the Fe-oxide shell to Cr{sub 2}O{sub 3} and the Fe core to FeCr alloy. The magnetic interaction in Fe/Fe-oxide NCs (∼25 nm) can be controlled by antiferromagnetic Cr-dopant. We report the origin of σ-FeCr phase at very low Cr concentration (2 at. %) unlike in previous studies, and the interaction reversal from dipolar to exchange interaction in watermelon-like Cr-doped core-shell NCs.
77 NANOSCIENCE AND NANOTECHNOLOGY↗