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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 469 records · Page 26
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

via machinae : Searching for stellar streams using unsupervised machine learning

ABSTRACT We develop a new machine learning algorithm, via machinae, to identify cold stellar streams in data from the Gaia telescope. via machinae is based on ANODE, a general method that uses conditional density estimation and sideband interpolation to detect local overdensities in the data in a model agnostic way. By applying ANODE to the positions, proper motions, and photometry of stars observed by Gaia, via machinae obtains a collection of those stars deemed most likely to belong to a stellar stream. We further apply an automated line-finding method based on the Hough transform to search for line-like features in patches of the sky. In this paper, we describe the via machinae algorithm in detail and demonstrate our approach on the prominent stream GD-1. Though some parts of the algorithm are tuned to increase sensitivity to cold streams, the via machinae technique itself does not rely on astrophysical assumptions, such as the potential of the Milky Way or stellar isochrones. This flexibility suggests that it may have further applications in identifying other anomalous structures within the Gaia data set, for example debris flow and globular clusters.

79 ASTRONOMY AND ASTROPHYSICS↗
NASA NTRS1988

Emission-line diagnostics for the existence of thermal accretion disks in active galactic nuclei

The use of the relative strengths of optical and UV emission lines to infer information about the EUV continuum shape is demonstrated. The FeII/H-beta line ratio is strongly dependent on spectral shape, making it a good indicator of the UV spectrum. It is shown how the gravitational influence of a massive black hole may be seen in the nature of gas streaming motions and the orbits of gas clouds in the region where the black hole potential is comparable to the stellar galactic potential.

Krolik, J. H.↗
NASA NTRS1990

Laboratory experiments on plasma contactors

Experimental results describing the operation of hollow cathode plasma contactors collecting and emitting electrons from and to an ambient plasma at current levels of the order of one ampere are presented. The voltage drops induced between a contactor and an ambient plasma are shown to be a few tens of volts at such current levels. The development of a double sheath and the production of substantial numbers of ions by electrons streaming across it are associated with the electron collection process. The development of a complex potential structure including a high potential hill just downstream of the cathode orifice is shown to characterize typical contactor emitting electrons.

Wilbur, Paul J.↗
NASA NTRS1990

Analysis of troposphere-stratosphere exchange

The overall goal is to improve our understanding of stratosphere-troposphere exchange processes in the tropics and midlatitudes. Specifically, modeling and analysis are performed using aircraft, radiosonde, and satellite data from the 1980 and 1987 NASA tropical field experiments in Panama and Australia, respectively, and the 1986 NASA jet stream field experiment in California. The objectives are to: (1) examine the structure of ozone, temperature, horizontal winds, tropospheric tracers, water and ice particles, and water vapor within, around, and above cumulus anvils in the tropics and jet streams in midlatitudes; (2) establish the presence, during each of the experimental periods, of various potential mechanisms of exchange, such as direct injection by cumulus, gravity wave fluxes, turbulent fluxes, and radiative heating; and (3) evaluate quantitatively, if possible, the mass of air transferred by these mechanisms during specific transport events.

Pfister, Leonhard↗
NASA NTRS1992

Experiments and analysis concerning the use of external burning to reduce aerospace vehicle transonic drag

The external combustion of hydrogen to reduce transonic drag was investigated. A control volume analysis is developed and indicates that the specific impulse performance of external burning is competitive with other forms of airbreathing propulsion and depends on the fuel-air ratio, freestream Mach number, and the severity of the base drag. A method is presented for sizing fuel injectors for a desired fuel-air ratio in the unconfined stream. A two-dimensional Euler analysis is also presented which indicates that the total axial force generated by external burning depends on the total amount of energy input and is independent of the transverse and streamwise distribution of heat addition. Good agreement between the Euler and control volume analysis is demonstrated. Features of the inviscid external burning flowfield are discussed. Most notably, a strong compression forms at the sonic line within the burning stream which may induce separation of the plume and prevent realization of the full performance potential. An experimental program was conducted in a Mach 1.26 free-jet to demonstrate drag reduction on a simple expansion ramp geometry, and verify hydrogen-air stability limits at external burning conditions. Stable combustion appears feasible to Mach number of between 1.4 and 2 depending on the vehicle flight trajectory. Drag reduction is demonstrated on the expansion ramp at Mach 1.26; however, force levels showed little dependence on fuel pressure or altitude in contrast to control volume analysis predictions. Various facility interference mechanisms and scaling issues were studied and are discussed.

Trefny, Charles J.↗
NASA NTRS2000

Application of Energy Integration Techniques to the Design of Advanced Life Support Systems

Exchanging heat between hot and cold streams within an advanced life support system can save energy. This savings will reduce the equivalent system mass (ESM) of the system. Different system configurations are examined under steady-state conditions for various percentages of food growth and waste treatment. The scenarios investigated represent possible design options for a Mars reference mission. Reference mission definitions are drawn from the ALSS Modeling and Analysis Reference Missions Document, which includes definitions for space station evolution, Mars landers, and a Mars base. For each scenario, streams requiring heating or cooling are identified and characterized by mass flow, supply and target temperatures and heat capacities. The Pinch Technique is applied to identify good matches for energy exchange between the hot and cold streams and to calculate the minimum external heating and cooling requirements for the system. For each pair of hot and cold streams that are matched, there will be a reduction in the amount of external heating and cooling required, and the original heating and cooling equipment will be replaced with a heat exchanger. The net cost savings can be either positive or negative for each stream pairing, and the priority for implementing each pairing can be ranked according to its potential cost savings. Using the Pinch technique, a complete system heat exchange network is developed and heat exchangers are sized to allow for calculation of ESM. The energy-integrated design typically has a lower total ESM than the original design with no energy integration. A comparison of ESM savings in each of the scenarios is made to direct future Pinch Analysis efforts.

Levri, Julie↗
NASA NTRS1944

Heat Transfer in a Turbulent Liquid or Gas Stream

The,theory of heat.transfer from a solid body to a liquid stream could he presented previously** only with limiting assumptions about the movement of the fluid (potential flow, laminar frictional flow). (See references 1, 2, and 3). For turbulent flow, the most important practical case, the previous theoretical considerations did not go beyond dimensionless formulas and certain conclusions as to the analogy between the friction factor and the unit thermal conductance, (See references 4, 5, 6, and 7,) In order to obtain numerical results, an experimental treatment of the problem was resorted to, which gave rise to numerous investigations because of the importance of this problem in many branches of technology. However, the results of these investigations frequently deviate from one another. The experimental results are especially dependent upon the overall dimensions and the specific proportions of the equipment. In the present work, the attempt will be made to develop systematically the theory of the heat transfer and of the dependence of the unit thermal conductance upon shape and dimensions, using as a basis the velocity distribution for turbulent flow set up by Prandtl and Von Karman.

Latzko, H.↗
NASA NTRS2020

Nitric Oxide Laser-Induced Fluorescence Rotational Thermometry in a Hypersonic Non-Equilibrium Flow

Spatially-resolved nitric oxide (NO) planar laser-induced fluorescence (PLIF) rotational thermometry was performed on a Mach 5 non-equilibrium flow around a blunt-body specimen in the Hypersonic Materials Environmental Test System (HyMETS) arc-heat wind tunnel at the NASA Langley Research Center. Transitions within the (0,0) band in the A(exp⁡ 2)∑(sup⁡ +) - X(exp⁡ 2)Π system of NO were excited with a 10 Hz pulsed ultra-violet laser. A multi-line fitting algorithm was applied to the PLIF spectra and transitions were filtered based on an iterative method that maximizes thermometry accuracy. NO PLIF thermometry results are compared to non-equilibrium computational fluid dynamics (CFD) simulations reported in the literature. Differences between the experiment and CFD are quantified for the free-stream, post-shock, shear-layer, and expansion-fan regions of the flow. Potential sources of error, applicable to both the CFD and experiment, are discussed.

Connor C McDougall↗
DOE OSTI2024

Probing Heavy Axion-like Particles from Massive Stars with X-rays and Gamma Rays

The hot interiors of massive stars in the later stages of their evolution provide an ideal place for the production of heavy axion-like particles (ALPs) with mass up to O(100 keV) range. We show that a fraction of these ALPs could stream out of the stellar photosphere and subsequently decay into two photons that can be potentially detected on or near the Earth. In particular, we estimate the photon flux originating from the spontaneous decay of heavy ALPs produced inside Horizontal Branch and Wolf-Rayet stars, and assess its detectability by current and future $X$-ray and gamma-ray telescopes. Our results indicate that current and future telescopes can probe axion-photon couplings down to $g_{a\gamma} \sim 4\times 10^{-11}$ GeV${}^{-1}$ for $m_a\sim 10-100$ keV, which covers new ground in the ALP parameter space.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2025

Alloy selective optical sorting of mixed post-consumer aluminum scrap streams

Shredded post-consumer non-ferrous scrap stream, also known as Zorba, contains a mixture of cast and wrought aluminum pieces with very different compositions. Cast Al pieces, with their high Si, Cu and Fe content, are a major contaminant in wrought scrap fraction, which results in downcycling of the mixed cast + wrought scrap into non-structural cast Al alloys and parts. Here, in this paper, we introduce a chemical treatment method to color-code scrap aluminum pieces by alloy family and demonstrate low-cost optical sorting of cast from wrought pieces to upgrade the scrap stream. We utilized non-acidic chemical solutions that react with (i.e., etch) the scrap pieces to produce colors based on the Al alloy chemistry of a given piece. Cast pieces with high Si and Cu fractions turned black, whereas the much leaner wrought pieces remained unreacted. We showed > 95% sorting efficiency of mixed cast and wrought pieces using a repurposed low-cost optical sorter originally designed for food sorting. We also colored wrought Al pieces by alloy families, such as 5xxx and 6xxx, using a two-step chemical etching technique, which has the potential to create a circular supply chain in which wrought aluminum alloys are sorted from the mixed scrap stream and recycled back to high-value wrought products such as sheets, extrusions, and forgings with minimal contamination from cast scrap.

Aluminum↗
DOE OSTI2021

Storage Futures Study: Economic Potential of Diurnal Storage in the U.S. Power Sector

We model the evolution of the U.S. electricity sector from 2020 through 2050 and find significant market potential (>125 GW) for diurnal energy storage across all 19 scenarios considered. Most of this storage has 4-6 hours of duration. We find that storage deployment is driven primarily by the combination of capacity value and energy time-shifting value, and that the combination of these value streams is needed for optimal storage deployment to be realized. We also find a strong correlation of PV penetration and storage market potential. Cost and performance metrics in this study focus on Li-ion batteries because the technology has more market maturity than other emerging technologies but results from this study can be generalized to any technologies that meet the cost and performance projections assumed.

25 ENERGY STORAGE↗
DOE OSTI2020

Numerical modeling and performance analysis of a membrane-based air dehumidifier using ionic liquid desiccant

Membrane-based Liquid Desiccant Air Dehumidifier (MLDAD) has the potential to overcome the shortcomings of the conventional open-tower liquid desiccant air dehumidifier. The MLDAD uses membranes with high water vapor permeability to separate air stream from the liquid desiccant and thus eliminates carry-over and the resulting corrosion issues. Recently, the ionic liquid desiccant becomes a promising alternative to conventional liquid desiccant. The ionic liquid desiccant has a large potential of dehumidification, which is also non-corrosive to metals and non-crystallizable. A two-dimensional numerical heat and mass transfer model of the MLDAD using a recently identified ionic liquid desiccant, [EMIM]OAc, is presented in this paper. We report this model can simulate the performance of the MLDAD with various designs, including different selections of liquid desiccant and membrane materials, dimensions of the MLDAD, and flow patterns. For porous membranes, this model accounts for several micro-scale mass transfer mechanisms of vapor transportation across the membrane. It can also model the mass transfer performance of dehumidifiers using non-porous membranes based on the experimentally measured membrane permeance. The numerical model was validated against the performance data available from literature and experimental tests. The maximum discrepancy of the latent effectiveness between the measured and the model-predicted results was about 6% when porous membranes were used. A parametric study was conducted with the numerical model. The results indicated that the membrane permeability, air path height, and solution to air mass ratio were the most critical parameters, determining the dehumidification performance of the MLDAD.

42 ENGINEERING↗
DOE OSTI2020

Numerical modeling and performance analysis of a membrane-based air dehumidifier using ionic liquid desiccant

Membrane-based Liquid Desiccant Air Dehumidifier (MLDAD) has the potential to overcome the shortcomings of the conventional open-tower liquid desiccant air dehumidifier. The MLDAD uses membranes with high water vapor permeability to separate air stream from the liquid desiccant and thus eliminates carry-over and the resulting corrosion issues. Recently, the ionic liquid desiccant becomes a promising alternative to conventional liquid desiccant. The ionic liquid desiccant has a large potential of dehumidification, which is also non-corrosive to metals and non-crystallizable. A two-dimensional numerical heat and mass transfer model of the MLDAD using a recently identified ionic liquid desiccant, [EMIM]OAc, is presented here. This model can simulate the performance of the MLDAD with various designs, including different selections of liquid desiccant and membrane materials, dimensions of the MLDAD, and flow patterns. For porous membranes, this model accounts for several micro-scale mass transfer mechanisms of vapor transportation across the membrane. It can also model the mass transfer performance of dehumidifiers using non-porous membranes based on the experimentally measured membrane permeance. The numerical model was validated against the performance data available from literature and experimental tests. The maximum discrepancy of the latent effectiveness between the measured and the model-predicted results was about 6% when porous membranes were used. A parametric study was conducted with the numerical model. Finally, the results indicated that the membrane permeability, air path height, and solution to air mass ratio were the most critical parameters, determining the dehumidification performance of the MLDAD.

42 ENGINEERING↗
DOE OSTI2022

Regional economic potential for recycling consumer waste electronics in the United States

Waste electronics are a growing environmental concern but also contain materials of great economic value. If properly recycled, waste electronics could enhance the sustainability of vital metal supply chains by offsetting the increasing demand for virgin mining. However, rapid changes in the size and composition of electronics complicate their end-of-life management. Here we couple material flow and geospatial analyses on over 90 critical consumer electronic products and find that over 1 billion devices, representing up to 1.5 million tonnes of mass, could be discarded annually in the United States by 2033. Emerging electronics such as connected home, health and augmented/virtual reality devices have become the fastest-growing types in the waste stream. Here we highlight policy opportunities to develop various sustainable circularity strategies around metal supply chains by showing the potential to integrate waste electronics and virgin mining pathways in western US regions, while new infrastructure designed specifically for waste electronics treatment is favourable in the central and eastern United States. Furthermore, we show the importance of building national-level refining and tear-down databases to improve electronics end-of-life management in the next decade.

29 ENERGY PLANNING, POLICY, AND ECONOMY↗
DOE OSTI2024

Reducing Economy-Wide Greenhouse Gas Emissions with Electrofuels and Biofuels as the Grid Decarbonizes

Biofuels and electrofuels have the potential to complement electrification in speeding greenhouse gas emissions reductions, especially in hard-to-decarbonize sectors. Concentrated waste CO 2 streams that can be used as a feedstock for electrofuels, however, may become less available as the share of renewable electricity increases and industries undergo decarbonization. Here, we conduct an analysis with detailed treatment of biofuels and electrofuels to probe their role in decarbonizing multiple industrial sectors and transportation. We examine how the changing availability of CO 2 could affect electrofuel production and the potential role of direct air capture in stabilizing the supply of CO 2 . The results indicate that biofuels could fulfill 12% of the total final energy demand across all U.S. sectors in 2050. Using seven industrial source points of CO 2 available in 2050, 15,388 PJ of electrofuels could be produced, which amounts to 25% of the total final energy demand. This result holds even upon decarbonization that requires direct air capture to boost the CO 2 supply. Biofuels and e-fuels have the potential to reduce economy-wide GHG emissions by 7 and 21% beyond electrification alone. However, electricity consumption and land use grow markedly with decarbonization at scale.

29 ENERGY PLANNING, POLICY, AND ECONOMY↗
DOE OSTI2023

Laboratory-Scale Coal-Derived Graphene Process (Final Report)

The Energy & Environmental Research Center (EERC) conducted a laboratory-scale coal-derived graphene (CDG) project focused on developing a technological process for making graphene from four U.S. domestic coal or coal wastes, including lignite from North Dakota, subbituminous coal from Wyoming, bituminous coal from Utah, and anthracite from Pennsylvania. The project was divided into two performance or budget periods (BPs), with BP1 comprising the up-front laboratory experiments to make graphene materials from coal beginning on May 1, 2020, to April 30, 2022. BP2 was conducted from May 1, 2022, to April 30, 2023, and was focused on analyzing the CDG process economic feasibility and the technical gaps for technological scale-up and commercialization. During this project, a few different coal-derived high-value products have been demonstrated, including graphite, graphene oxide (GO), reduced graphene oxide (rGO), and graphene quantum dots (GQDs). A new graphite microstructure was discovered and named “croissant graphite” because of the exterior morphological and textural resemblance to croissant food items sold in commercial groceries stores. The new graphite structure and the associated preparation from coal or coal waste feedstocks has been the subject of a U.S. patent application. The systematic experimental processes involving coal cleaning, upgrading, and conversion to high-value carbon products culminated into a developed upgraded coal-to-products (UCP) technology that is being pursued for potential fast-track commercialization, if funding is available. It is envisioned that commercialization of the UCP technology would increase consumption of U.S. domestic coals or coal wastes to make environmentally sustainable high-value products for the electronics industry, high-energy-storage applications, and clean energy technologies such as electric vehicle (EV) lithium-ion batteries (LIBs), for which graphite has become a critical mineral commodity. Croissant graphite microstructures, when observed by field emission scanning electron microscopy (FESEM), display wavy surface morphology and often grow from a base that is made of graphitized particles with honeycomb-like layers, which are believed to be graphene layers. While more studies are needed to fully ascertain the mechanisms of the croissant graphite microstructure formation, it is postulated that their growth may begin from curling of the graphene sheets into ribbon-like structures, and continuous growth and densification of the ribbon-like structures forms croissant microstructures. Additional studies are ongoing to evaluate the electrochemical performance of croissant graphite for LIB applications and to determine the experimental conditions necessary to tune on/off croissant formation so that it can be either optimized or suppressed depending on performance evaluation results. In addition to the discovery of croissant graphite, the graphitization process from the four coal ranks in general was successful. X-ray diffraction (XRD) analysis showed that the degree of graphitization (DoG) ranged from 12% to 80% in an early sample set, and further optimization on lignite coal produces a DoG of about 92%, which was spectacular to see as lignite is the lowest-rank coal. Thus, it is expected that the graphitization performance for higher-rank coals will be similar or better when optimized as well. The coal-derived graphite was used to make GO and rGO. Analytical characterization, e.g., by methods such as Raman spectroscopy, XRD, Fourier transform infrared (FTIR) spectroscopy and FESEM, showed that the sequence of converting the coal to graphite, exfoliating it to GO, and then chemically reducing the GO to rGO was successful. Although coal naturally contains aromatic compounds and some relatively small-sized condensed aromatic units, it does not contain graphene sheets. In the UCP process, the aromatic domains in the coals, particularly low-rank coals, are concentrated and condensed further into graphene sheets, which are ordered into a 3D stack during graphitization. The synthesized graphite is then unpacked by methods such as exfoliation to various graphene products. GQDs were synthesized from all four coal types, and their optical properties were demonstrated to be tunable by the coal precursor preprocessing treatments. In all four coal types, enhanced optical properties were observed for the produced GDQs with incremental improvements made to the coal precursors. GQDs produced from raw coal samples displayed lower ultraviolet–visible (UV–Vis) spectroscopy absorbance intensity compared to those obtained from cleaned and upgraded coal residues. The photoluminescence (PL) intensities also varied with pretreatment conditions and with the concentration of GQDs in aqueous solutions. GQDs obtained from anthracite show longer emission wavelengths and can be excited by visible light as opposed to GQDs derived from the other coal ranks. UV fluorescence 3D maps and spectra revealed that the emission wavelength at which the GQDs solutions display the highest intensity was slightly redshifted based on the coal precursor pretreatments. In low-rank coal (lignite and subbituminous) samples, two clusters were observed in the maps for GQDs, which may suggest that there are potentially two types of fluorophores in solution or two main size populations. The ability to tune the properties of GQDs based on processing methods can be exploited to make GQDs for various optical display or optoelectronics applications. The results also highlight the importance of removing coal-borne impurities to improve the quality of the coal precursor for preparation of graphene products. Coal and/or coal wastes preprocessing methods were developed and applied to clean and upgrade the coal precursors prior to graphitization and subsequent conversion to graphene products. The preprocessing methods involve high specific-gravity separations, mineral acid cleaning (no hydrofluoric acid), and subsequent upgrading by reducing the coal-borne heteroatom (nitrogen, sulfur, and oxygen) content using proprietary chemical agents. Analytical characterization revealed that the preprocessing steps were successful, with ash reductions that range from 38% to 80% and residual ash content that was below the 5 wt% initial target. Based on proximate and ultimate analysis, the heteroatom reduction reactions produced upgraded coal residues with the oxygen content reduced by 8% to 24%, with additional reductions in the nitrogen and sulfur contents. An initial assessment of the waste streams from the UCP process shows very small to negligible environmental impact due to CO 2 , NO x , and SO x because most process steps are performed under inert atmosphere with argon. Consequently, reactive oxygen environments that tend to create these species are avoided. The inorganic and potentially hazardous species are released into aqueous waste streams that are easy to handle for proper disposal. The liquid waste streams were found to contain low-level concentrations of rare-earth elements (REEs), which could be concentrated and recovered as value-added by-products. Additionally, the volatile and gaseous fractions from carbonization and heat treatment contain useful organic compounds that can also be recovered as potential valuable by-products. Thus, the UCP technology is considered an environmentally sustainable and promising emerging technology for making high-value products from coal and coal wastes, with potential additional value-added by-products. Analysis of potential markets for the coal-derived carbon products shows a strong demand in both niche market sectors and across a wide variety of other industrial sectors. Graphite is currently considered a critical mineral commodity that has a large and growing demand in the LIB industry for EV applications. Based on data from Fortune Business Insights (2022) and Marketwatch (2023) reports, the average global graphite market is projected to reach about 33 billion by 2028, growing at a compound annual growth rate (CAGR) of about 7%, with much of this growth expected to be in the LIB industry. GO and rGO have strong market potentials in various application areas, such as coatings for anticorrosion, anti-icing, and antimicrobial protection, thermal barriers, wear resistance, sensors, additive manufacturing such as 3D inks, and others. GQDs are the emerging key player in the bioimaging, photovoltaics, and light-emitting diodes (LEDs) applications, with the potential to replace traditional semiconductor quantum dots (SQDs), which are based on metallic systems that are more toxic and more expensive. Biomedical applications of GQDs are becoming more attractive because of low to no toxicity and extremely low cost compared to SQDs. The major challenges for scale-up and commercialization of coal-derived carbon products such as graphene vary from the inherent attributes of graphene itself to reluctance to accept graphene in new manufacturing processes because of the uncertainty of the unknown. The 2D nature of graphene materials with a thickness of one atom presents significant challenges to proper handling/processing, and process scale-up becomes difficult because it requires high-end, expensive equipment, even for routine handling and analysis for quality assurance and control. Pristine graphene can also be extremely difficult to work into other matrices, thus hindering downstream processibility, especially at large scale. Currently, the cost of graphene and graphene products is still high and presents an economic risk that tends to slow down investment in scaling up emerging technologies. The lack of a standard for graphene materials for quality assurance and quality control poses a great challenge not only for the markets but also for commercialization efforts. A first-look economic feasibility analysis of the UCP technology provided valuable information that suggests the UCP process would be feasible, especially when it is scaled to a pilot scale and could be more competitive at the full scale. Graphitization was found to be the most energy-consuming and most capital-intensive step in the overall process. In small laboratory- and bench-scale experiments, labor is a significant contributor to the total process costs. Although these energy, capital, and labor constraints contribute to a higher selling price for the product, a preliminary economic model suggests that the process would be feasible at large scale when the process is fully integrated, optimized, and automated.

01 COAL, LIGNITE, AND PEAT↗
DOE OSTI2022

Printing noble metal alloy films with compositional gradient

Additive manufacturing has offered great promise in fabricating materials and devices with complex structures and unique properties. In addition to complex structures, additive manufacturing also allows for local changes to material compositions and/or structure, ideal for combinatorial material investigations. Besides, advantages over freedom of design, mass customization, waste minimization and the capability to fast prototyping, the on-demand control of compositional distributions in low dimensional materials remains challenging. In this work, we demonstrate a combinatorial aerosol jet printing technique to create noble metal films with gradient compositions. Nanoparticle sizes and ink chemistry are critical for aerosol jet printing and sintering process in order to achieve defect free thin films. Ruthenium (Ru) and platinum (Pt) nanoparticles with size <5 nm were synthesized and formulated into printable inks. Further, after thermal sintering at temperature as low as 400 °C, printed nanoparticles formed highly reflective films free from microstructural defect. Alloy films of gradient compositions were realized via in-situ mixing Ru and Pt ink streams and varying the mixing ratio during the printing process. This combinatorial printing method provides great potential to rapidly transform nanoparticle inks into new materials compositions and structures unobtainable via conventional methods for high-throughput materials studies.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Integrated CO 2 Capture and Conversion to Formate with a Molecular Platinum Bis(diphosphine) Electrocatalyst

Carbon dioxide is a potentially valuable feedstock for carbon-based fuels or commodities but is only available in dilute streams. Many studies have focused on either the capture and concentration of CO 2 or the reduction of pure CO 2 streams. The direct reduction of sorbent-captured CO 2 in an integrated process would skip the energy-intensive CO 2 concentration and sorbent regeneration step. Herein, we report the electrocatalytic reduction of 1,3-bis(2,6-diisopropylphenyl)imidazolium-2-carboxylate (IPr·CO 2 ), which forms quantitatively from the reaction of sorbent 1,3-bis(2,6-diisopropylphenyl)imidazol-2-ylidene (IPr) with 10% and 0.04% CO 2 streams, by catalyst [Pt(dmpe) 2 ](PF 6 ) 2 (dmpe = 1,2-bis(dimethylphosphino)ethane) to formate with >70% Faradaic efficiencies. Unexpectedly, experimental studies indicate that the proton source phenol facilitates rapid decarboxylation of IPr·CO 2 to release CO 2 , which is the substrate for reduction. Kinetic studies determined the rate of hydride transfer from a catalytic intermediate [HPt(dmpe) 2 ](PF 6 ) to form the C–H bond in formate to be 0.22 M –1 s –1 . Further details on the mechanism, transition state energy, and structure for hydride transfer to CO 2 , a common step in CO 2 reduction, were explored using computational methods.

Chemistry↗