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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 235 records · Page 13
All sourcesNASA NTRSDOE OSTI
DOE OSTI2017

Self-Assembled Fe-N-Doped Carbon Nanotube Aerogels with Single-Atom Catalyst Feature as High-Efficiency Oxygen Reduction Electrocatalysts

Finely controlled synthesis of high active and robust non-precious metal catalysts with excellent electrocatalytic efficiency towards oxygen reduction reaction is extremely vital for successful implementation of fuel cells and metal batteries. Unprecedented oxygen reduction reaction electrocatalytic performances and the diversified synthetic procedure in term of favorable structure/morphology characteristics make transition metals-derived M–N–C (M=Fe, Co) structures the most promising nanocatalysts. Herein, using the nitrogen-containing small molecular and inorganic salt as precursors and ultrathin tellurium nanowires as templates, we successfully synthesized a series of well-defined M-N-doped hollow carbon nanowire aerogels through one step hydrothermal route and subsequent facile annealing treatment. Taking advantage of the porous nanostructures, one-dimensional building block as well as homogeneity of active sites, the resultant Fe-N-doped carbon hollow nanowire aerogels exhibited excellent ORR electrocatalytic performance even better than commercial Pt/C in alkaline solution, holding great potential in fuel cell applications.

Environmental Molecular Sciences Laboratory↗
DOE OSTI2015

Magnetic self-assembly for the synthesis of magnetically exchange coupled MnBi/Fe–Co composites

Exchange coupled hard/soft MnBi/Fe–Co core/shell structured composites were synthesized using a magnetic self-assembly process. MnBi particles were prepared by arc-melting, and Fe–Co nanoparticles were synthesized by an oleic acid assisted chemical reduction method. Grinding a mixture of micron-sized MnBi and Fe–Co nanoparticles in hexane resulted in MnBi/Fe–Co core/shell structured composites. The MnBi/Fe–Co (95/5 wt%) composites showed smooth magnetic hysteresis loops, enhanced remanent magnetization, and positive values in the ΔM curve, indicating exchange coupling between MnBi and Fe–Co particles. - Graphical abstract: Both MnBi and Fe–Co particles were dispersed in hexane for grinding. Because of the oleic acid used during the Fe–Co nanoparticle synthesis, they could be well dispersed in hexane. During the grinding, the size of MnBi particles was decreased, hexane was evaporated, and the Fe–Co nanoparticles were concentrated in the solvent and magnetically attracted by MnBi particles, forming a core/shell structure. - Highlights: • Exchange coupled MnBi/Fe–Co composites are synthesized through magnetic selfassembly. • Magnetic exchange coupling is demonstrated by smooth magnetic hysteresis loops, enhanced remanent magnetization, and dominant positive peak in the ΔM curve. • The experimental results in magnetic properties are close to the theoretical calculation results.

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

Miktoarm Stars via Grafting-Through Copolymerization: Self-Assembly and the Star-to-Bottlebrush Transition

The grafting-through copolymerization of two distinct macromonomers via ring-opening metathesis polymerization is normally used to form statistical or diblock bottlebrush polymers with large total backbone degrees of polymerization (N BB ) relative to that of the side-chains (N SC ). Here, we demonstrate that Grubbs-type chemistry in the opposite limit, namely N BB << N SC , produces well-defined materials with excellent control over ensemble-averaged properties, including molar mass, dispersity, composition, and number of branch points. The dependence of self-assembly on these molecular design parameters was systematically probed using small angle X-ray scattering and self-consistent field theoretic simulations. Moreover, our analysis supports the notion that two-component bottlebrush copolymers with small N BB behave like miktoarm star polymers. The star-to-bottlebrush transition is quantifiable for both statistical and diblock sequences by unique signatures in the experimental scaling of domain spacing and simulated distribution of backbone/side-chain density within lamellar unit cells. These findings represent a conceptual framework that simplifies the synthesis of miktoarm star polymers when dispersity in the number of arms and composition can be tolerated. The analytical approach introduced to distinguish chain conformations in complex macromolecules also complements previous methods, for example form factor scattering and rheology.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Impact of Grafting Density on the Assembly and Mechanical Properties of Self-Assembled Metal–Organic Framework Monolayers

Polymer-grafted metal–organic frameworks (MOFs) can be used to form free-standing self-assembled MOF monolayers (SAMMs). Polymer chains can be introduced onto MOF surfaces through either the ligands or metal nodes using both grafting-to and grafting-from approaches. However, controlling the grafting density of polymer-grafted MOFs has not yet been achieved, because a means to control the density of grafting sites on the MOF surface has not been developed. In this study, the grafting density of polymer-grafted UiO-66 (UiO = University of Oslo) was controlled by functionalizing a portion of the Zr(IV) secondary building units (SBUs) on a UiO-66 surface with a so-called blocking agent. The remaining sites on the UiO-66 SBUs were functionalized with polymerization initiation groups, and polymers were grown from these sites to obtain particles with variable grafting densities and chain lengths that form SAMMs at an air–water interface. Even under conditions of low grafting density, these materials retain the ability to form SAMMs and their free-standing ability. Changes in particle arrangement within the monolayers were investigated using SEM imaging, and the toughness of the monolayers was evaluated using a film-on-water (FOW) method. Furthermore, coarse-grained molecular dynamics simulations were carried out to elucidate the morphology and mechanical properties of the monolayers. Findings from both experiments and simulations indicate that the toughness of SAMMs is more heavily influenced by the chain length of the grafted polymers than by the overall polymer content in the composite.

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

Improving Photocatalysis for the Reduction of CO 2 through Non-covalent Supramolecular Assembly

Here, we report the first successful enhancement of photocatalytic performance by introduction of hydrogen bonding interactions to Re bipyridine catalyst and Ru photosensitizer system (ReDAC/RuDAC) with the addition of amide substituents. This system shows a more than threefold increase in turnover number (TONCO = 100 ± 4) and quantum yield (Φ CO = 23 ± 1 %) for carbon monoxide formation compared to the control system using unsubstituted Ru photosensitizer (RuBPY) and ReDAC (TON CO = 28 ± 4 and Φ CO = 7 ± 1 %) in acetonitrile (MeCN) with BIH as sacrificial reductant. In dimethylformamide (DMF), a hydrogen bonding interrupting solvent, the ReDAC/RuDAC system showed a decrease in catalysis while the control system exhibited an increase, indicating the role of hydrogen bonding in enhancing the photocatalysis for CO 2 reduction through supramolecular assembly. RuDAC and RuBPY have demonstrated no significant differences in lifetime measurements, spectroscopic analysis, electrochemical studies and spectroelectrochemical studies, revealing that the enhancement in photocatalysis in RuDAC/ReDAC in MeCN system is not due to differences in properties unrelated to catalyst/photosensitizer association but a direct result of hydrogen bonding interactions.

14 SOLAR ENERGY↗
DOE OSTI2015

Calculation of Electrochemical Reorganization Energies for Redox Molecules at Self-Assembled Monolayer Modified Electrodes

Electrochemical electron transfer reactions play an important role in energy conversion processes with many technological applications. Electrodes modified by self-assembled monolayers (SAMs) are useful because the double layer effects are reduced. An important quantity for calculating the electron transfer rate constant is the reorganization energy, which is associated with changes in solute geometry and solvent configuration. In this Letter, an approach for calculating the electrochemical solvent reorganization energy for a redox molecule attached to or near a SAM modified electrode is presented. This integral equations formalism polarizable continuum model (IEF-PCM) approach accounts for the detailed electronic structure of the molecule, as well as the contributions from the electrode, SAM, and electronic and inertial solvent responses. The calculated total reorganization energies are in good agreement with experimental data for a series of metal complex in aqueous solution. This approach will be useful for calculating electron transfer rate constants for molecular electrocatalysts. This work was supported as part of the Center for Molecular Electrocatalysis, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences.

Ghosh, Soumya↗