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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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132 records · Page 8
All sourcesNASA NTRSDOE OSTI
DOE OSTI2026

Direct Air Capture Using Trapped Small Amines in Hierarchical Nanoporous Capsules on Porous Electrospun Fibers (Final Technical Report)

This report summarizes the carbon capture research and development conducted by The State University of New York at Buffalo (UB) and GTI Energy (GTI) for award “DE-FE0031969: Direct Air Capture Using Trapped Small Amines in Hierarchical Nanoporous Capsules on Porous Electrospun Fibers” sponsored by the U.S. Department of Energy (DOE). The objective of this project is to develop an innovative sorbent structure of trapped small amines in HNC embedded in PEF for DAC. This involves tailoring both sorbent and PEF materials to achieve a compact system for DAC with high capacity for CO 2 at concentrations typically available in air and at near ambient conditions. An innovative sorbent structure of trapped small amines in hierarchical nanoporous capsules (HNC) embedded in porous electrospun fibers (PEF) was developed for direct air capture (DAC). This involves tailoring both sorbent and PEF materials to achieve a compact system for DAC with high capacity for CO 2 at concentrations typically available in air and at near ambient conditions. An interfacial polymerization process was developed, which utilized loaded amines inside mesoporous silica and trimesoyl chloride (TMC) dissolved in organic solvents as the precursors, to generate a polyamide (PA) coating layer on mesoporous silica and thus trap amines. Reaction conditions, including TMC concentration, organic solvents, reaction time, etc., for interfacial polymerization were optimized to effectively trap loaded amines, and cyclic heating-cooling operation was conducted to evaluate the coating quality. Larger pore volume mesoporous silica was also synthesized to increase amine loading and thus increase CO 2 capacity. The optimized sorbent material exhibited CO 2 capacity as high as 4.88 mmol/g under humid DAC conditions and negligible loss (<1%) during 10 cyclic heating-cooling operations. The optimized PA-coated sorbent also showed fast adsorption and desorption kinetics, with <20% t1/2 increase compared to uncoated sorbent. PEF fabrication conditions, including organic solvents for dissolving core and shell polymers, voltage, distance from the nozzle to the collection panel, etc. were adjusted to better incorporate HNC. After incorporating the optimized sorbent material into PEF, the structured sorbent had a CO 2 capacity of approximately 4.0 mmol/g under humid DAC conditions, with capacity loss of 0.17% per cycle and t1/2 increase less than 10%. A techno-economic analysis (TEA) for the process design for a DAC system based on our developed sorbent structure of trapped small amines in HNC embedded in PEF was conducted. The process design included process description and major equipment sizing and energy and mass balances in addition to scale-up research results and estimated capture cost. Aspen Adsorption Simulator was used to fit the experimentally measured breakthrough curves and extract equilibrium and kinetic data of the optimized sorbent. Our results indicated that for a DAC plant with CO 2 productivity of 3,000 tonne/year, the levelized cost of CO 2 capture was $\$$612/tonne, with the largest contribution of 44.33% from the fixed operation cost. Increasing CO 2 productivity, while maintaining similar fixed operation cost, is expected to significantly reduce the CO 2 capture cost. A sensitivity study was also conducted to understand the influence of total plant cost, sorbent cost, CO 2 concentration in the feed, sorbent mat lifetime, sorbent regeneration electricity, and adsorption blower pressure drop on the levelized cost of CO 2 capture, revealing a capture cost range of $\$$520-870/tonne.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Cooperative Atomically Dispersed Fe–N 4 and Sn–N x Moieties for Durable and More Active Oxygen Electroreduction in Fuel Cells

One grand challenge for deploying porous carbons with embedded metal–nitrogen–carbon (M–N–C) moieties as platinum group metal (PGM)-free electrocatalysts in proton-exchange membrane fuel cells is their fast degradation and inferior activity. Here, we report the modulation of the local environment at Fe–N 4 sites via the application of atomic Sn–N x sites for simultaneously improved durability and activity. We discovered that Sn–N x sites not only promote the formation of the more stable D2 FeN 4 C 10 sites but also invoke a unique D3 SnN x –Fe II N 4 site that is characterized by having atomically dispersed bridged Sn–N x and Fe–N 4 . This new D3 site exhibits significantly improved stability against demetalation and several times higher turnover frequency for the oxygen reduction reaction (ORR) due to the shift of the reaction pathway from a single-site associative mechanism to a dual-site dissociative mechanism with the adjacent Sn site facilitating a lower overpotential cleavage of the O–O bond. This mechanism bypasses the formation of the otherwise inevitable intermediate that is responsible for demetalation, where two hydroxyl intermediates bind to one Fe site. Lastly, a mesoporous Fe/Sn-PNC catalyst exhibits a positively shifted ORR half-wave potential and more than 50% lower peroxide formation. This, in combination with the stable D3 site and enriched D2 Fe sites, significantly enhanced the catalyst’s durability as demonstrated in membrane electrode assemblies using complementary accelerated durability testing protocols.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Size-Controlled Nanoparticles Embedded in a Mesoporous Architecture Leading to Efficient and Selective Hydrogenolysis of Polyolefins

A catalytic architecture, comprising a mesoporous silica shell surrounding platinum nanoparticles (NPs) supported on a solid silica sphere (mSiO2/Pt-X/SiO2; X is the mean NP diameter), catalyzes hydrogenolysis of melt-phase polyethylene (PE) into a narrow C23-centered distribution of hydrocarbons in high yield using very low Pt loadings (~10 -5 g Pt/g PE). During catalysis, a polymer chain enters a pore and contacts a Pt NP where the C–C bond cleavage occurs and then the smaller fragment exits the pore. mSiO 2 /Pt/SiO 2 resists sintering or leaching of Pt and provides high yields of liquids; however, many structural and chemical effects on catalysis are not yet resolved. Here, we report the effects of Pt NP size on activity and selectivity in PE hydrogenolysis. Time-dependent conversion and yields and a lumped kinetics model based on the competitive adsorption of long vs short chains reveal that the activity of catalytic material is highest with the smallest NPs, consistent with a structure-sensitive reaction. Remarkably, the three mSiO 2 /Pt-X/SiO 2 catalysts give equivalent selectivity. We propose that mesoscale pores in the catalytic architecture template the C 23 -centered distribution, whereas the active Pt sites influence the carbon–carbon bond cleavage rate. This conclusion provides a framework for catalyst design by separating the C–C bond cleavage activity at catalytic sites from selectivity for chain lengths of the products influenced by the structure of the catalytic architecture. The increased activity, selectivity, efficiency, and lifetime obtained using this architecture highlight the benefits of localized and confined environments for isolated catalytic particles under condensed-phase reaction conditions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

CO2 Sorption in Aminopolymer-Based Direct Air Capture Composites Through Fluorescent Detection

Aminopolymer-mesoporous oxide composites are becoming widely recognized for their ability to adsorb CO2 directly from the air. However, a better fundamental understanding of the nature of these materials under different environmental operating conditions will be necessary before they become ubiquitous in industrial direct air capture (DAC) systems. For example, gas diffusion in general is coupled with polymer segmental mobility in these composites; diffusion is therefore affected by interactions of the polymer with the pore wall of the mesoporous oxide, by the relative humidity of the air, and by electrostatic crosslinks that develop as a function of CO2 sorption. Disentangling these and additional complicated effects in order to better optimize operating conditions is a major challenge for the field. Here, we present a method for quantifying the adsorption of CO2 and moisture in a polyethylenimine (PEI) - Al2O3 composite using infrared sensing while we simultaneously monitor polymer mobility with a fluorescent probe molecule doped into the composite. Both the fluorescence intensity and shape of the emission spectra are strongly dependent on the mobility of the supporting medium. We monitor the polymer mobility and CO2 adsorption kinetics across a series of different relative humidities (RH) with this technique, and we observed that the relative difference between polymer mobility and sorption kinetics from one RH to the next are quite dramatic. We interpret these results and discuss how they can be used to inform the design of more efficient DAC systems for real-world operating conditions.

carbon capture↗
DOE OSTI2025

Metal–Oxide Interface Sites Created Using Atomic Layer Deposition and Tested for CO Oxidation

The performance of catalysts made out of Pt supported on TiO 2 thin films grown on SBA-15 (a silica mesoporous material) by atomic layer deposition (ALD) was characterized systematically by combining in situ infrared absorption spectroscopy (IR) with other techniques including electron microscopy and adsorption−desorption isothermal measurements. The titania films in the resulting high-surface-area catalysts were evenly distributed throughout the inner surface of the SBA-15 mesopores, and their thickness could be controlled at a submonolayer level, with 3 to 4 TiO 2 ALD cycles needed for the complete coverage of the silica sites. The titania films could be deposited either before or after adding the metal (Pt), which was dispersed in the form of small nanoparticles (NPs) approximately 4−6 nm in diameter, in order to exert some control on the density and nature of the Pt/TiO 2 interface sites. One important lesson deriving from this work is that such an order of deposition leads to significantly different catalysts in spite of the fact that most of their structural properties are similar. If the Pt is deposited on the titania films, the resulting metal NPs are slightly smaller than those grown on silica and display CO adsorption sites with lower surface Pt coordination numbers. On the other hand, when TiO 2 is deposited on the Pt/SBA-15 starting material, some titania grows on the metal and partially blocks its surface while also creating new interface sites where CO binds more weakly and displays lower C−O stretching frequencies. In terms of catalytic performance, the results from in situ IR CO site titration and kinetic measurements combined suggest a mechanism where CO first adsorbs on Pt atop sites and then migrates to Pt/TiO 2 interface sites, where oxidation takes place. Both types of sites appear to be similar in all the catalysts tested, but catalytic performance could be optimized by tuning their surface densities. Maximum catalytic activity was obtained when the TiO2 films were deposited first and with TiO 2 coverages of at least half a monolayer, that is, after at least 2 ALD cycles.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Atomic-Level Structure of Mesoporous Hexagonal Boron Nitride Determined by High-Resolution Solid-State Multinuclear Magnetic Resonance Spectroscopy and Density Functional Theory Calculations

Mesoporous hexagonal boron nitride (p-BN) has received significant attention over the last decade as a promising candidate for water cleaning/pollutant removal and hydrogen storage applications. In this work, high-resolution solid-state NMR spectroscopy and plane-wave density-functional theory (DFT) calculations are used to obtain an atomic-level description of p-BN. 1 H– 15 N or 1 H– 14 N heteronuclear (HETCOR) correlation experiments recorded with either conventional NMR at room temperature or dynamic nuclear polarization surface-enhanced spectroscopy (DNP-SENS) at ca. 100 K reveal NB 2 H, NBH 2 , NBH 3 + species residing on the edges of BN sheets. Ultra-high field 35.2 T 11 B NMR spectroscopy was used to resolve 11 B NMR signals from BN 3 , BN 2 O x (OH) 1–x (x = 0–1), BNO x (OH) 2–x (x = 0–2), BO x (OH) 3–x (x = 0–3), and BO x (OH) 4–x – (x = 0–4). Importantly, 2D 11 B dipolar double-quantum–single-quantum homonuclear correlation spectra reveal that many pore/defect sites are composed of boron oxide/hydroxide clusters connected to the BN framework through BN 2 O units. 1D and 2D 11 B{ 15 N} HETCOR NMR experiments, in addition to plane-wave DFT calculations of nine different structural models, further confirm the assignment of all NMR signals. The detailed structure determination of the pore and edge/defect sites within p-BN should further enable the rational design and development of next-generation p-BN-based materials. In addition, the techniques outlined here should be applicable to determine structure within other porous and/or boron-based materials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗