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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 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Integrating Chemical Catalysis and Biological Conversion of Carbon Intermediates for Deriving Value-Added Products from Carbon Dioxide

Carbon dioxide valorization represents an appealing approach to reducing greenhouse gases in the atmosphere. While electrocatalysis is an effective tool to reduce CO 2 into small carbon compounds, it becomes increasingly challenging to efficiently produce compounds with more carbon atoms. In contrast, while biological systems struggle to utilize CO 2 , they can readily upcycle other small carbon compounds. This project explores the use of a two-stage process that electrocatalytically converts CO 2 into methanol, formate, or acetate which is subsequently utilized by Methylotuvimicrobium alcaliphilum 20Z to produce medium chain length polyhydroxyalkanoate. A techno-economic analysis and life cycle assessment evaluates the commercial viability of the process as well as its carbon emissions. We show here an enhanced CO 2 -to-methanol electroconversion step coupled with the use of a microbial culture adapted to the process conditions to be the optimal configuration for economic potential.

09 BIOMASS FUELS↗
DOE OSTI2018

Time Lapse Charged Wellbore Casing Controlled Source Electromagnetic Surveys for Monitoring Injected Carbon Dioxide

Carbon dioxide (CO2) injection for enhanced oil recovery (EOR) and long-term carbon storage extends the life of an oil field while keeping CO2 out of the atmosphere. Monitoring CO2 migration during EOR operations is critical to maximizing production and detecting unexpected CO2 migration quickly. In this project, we monitor CO2 migration using time-lapse charged well casing controlled source electromagnetics (CSEM) at an active EOR site undergoing CO2 injection. Since the electrical conductivity of the reservoir changes as CO2 displaces other fluids, this novel survey technique aims to monitor CO2 injection effectively and unobtrusively from the surface via electromagnetic field measurements. Of four time-lapse field campaigns spaced over two years, we have completed two. Each campaign consists of a CSEM survey supplemented by magnetotelluric and time-domain electromagnetic surveys. In the CSEM survey, a transmitter delivers alternating current to the subsurface at frequencies from 0.125 Hz to 16 Hz using steel well casings as electrodes. Charged well casing surveys detect deeper conductivity contrasts than surveys that use only surface electrodes, allowing CO2 movement at the depth of the reservoir to be imaged more clearly. We transmit on two well pairs. One pair is oriented in the east-west direction, and the other is oriented in the northeast-southwest direction. Receiver stations measure orthogonal components of the electric and magnetic fields. The measurements are repeated at the same locations in each field campaign. Data differences between campaigns provide information about changes in the electrical conductivity of the subsurface. We present the latest results from this ongoing project, including modeling, survey design, data processing techniques, and preliminary results from the field campaigns.

Magnetic and electrical methods, Geomagnetic induc↗
NASA NTRS2015

Development and Preliminary Tests of an Open-Path Airborne Diode Laser Absorption Instrument for Carbon Dioxide

Carbon dioxide (CO2) is well known for its importance as an atmospheric greenhouse gas, with many sources and sinks around the globe. Understanding the fluxes of carbon into and out of the atmosphere is a complex and daunting challenge. One tool applied by scientists to measure the vertical flux of CO2 near the surface uses the eddy covariance technique, most often from towers but also from aircraft flying specific patterns over the study area. In this technique, variations of constituents of interest are correlated with fluctuations in the local vertical wind velocity. Measurement requirements are stringent, particularly with regard to precision, sensitivity to small changes, and temporal sampling rate. In addition, many aircraft have limited payload capability, so instrument size, weight, and power consumption are also important considerations. We report on the development and preliminary application of an airborne sensor for the measurement of atmospheric CO2. The instrument, modeled on the successful DLH (Diode Laser Hygrometer) series of instruments, has been tested in the laboratory and on the NASA DC-8 aircraft. Performance parameters such as accuracy, precision, sensitivity, specificity, and temporal response are discussed in the context of typical atmospheric variability and suitability for flux measurement applications. On-aircraft, in-flight data have been obtained and are discussed as well. Performance of the instrument has been promising, and continued flight testing is planned during 2016.

Diskin, Glenn S.↗
NASA NTRS2001

Sensitivity Studies for Space-Based Global Measurements of Atmospheric Carbon Dioxide

Carbon dioxide (CO2) is well known as the primary forcing agent of global warming. Although the climate forcing due to CO2 is well known, the sources and sinks of CO2 are not well understood. Currently the lack of global atmospheric CO2 observations limits our ability to diagnose the global carbon budget (e.g., finding the so-called "missing sink") and thus limits our ability to understand past climate change and predict future climate response. Space-based techniques are being developed to make high-resolution and high-precision global column CO2 measurements. One of the proposed techniques utilizes the passive remote sensing of Earth's reflected solar radiation at the weaker vibration-rotation band of CO2 in the near infrared (approx. 1.57 micron). We use a line-by-line radiative transfer model to explore the potential of this method. Results of sensitivity studies for CO2 concentration variation and geophysical conditions (i.e., atmospheric temperature, surface reflectivity, solar zenith angle, aerosol, and cirrus cloud) will be presented. We will also present sensitivity results for an O2 A-band (approx. 0.76 micron) sensor that will be needed along with CO2 to make surface pressure and cloud height measurements.

Mao, Jian-Ping↗
DOE OSTI2025

Microwave-Assisted Production of Polycarbonate Diols using Carbon Dioxide

Carbon dioxide (CO2) is a cheap and readily available resource that can be converted to value-added chemicals including fuels, polymers, and other products. One lucrative option is polycarbonate diols, which are the precursor to polyurethanes that find wide applications in automotive and aerospace industries. The traditional process for the synthesis of polycarbonate diols involves using hazardous phosgene and alcohols in a strongly basic medium that generates significant amounts of salt. Alternately, CO2 can be reacted with alkanediols over CeO2 catalysts to produce polycarbonate diols. For the current work, a microwave-assisted atmospheric flow system was investigated for converting CO2 into polycarbonate diols and was compared against a thermal system. Various parameters such as type and ratio of solvents, and the addition of dehydrating agents for the microwave system was tested. The different CeO2 catalysts used were characterized using Brunauer–Emmett–Teller (BET) surface area analysis, Raman spectroscopy, X-ray diffraction, and temperature programmed desorption (NH3-TPD and CO2-TPD).

CO2 utilization↗
DOE OSTI2015

Evidence for Carbonate Surface Complexation during Forsterite Carbonation in Wet Supercritical Carbon Dioxide

Continental flood basalts are attractive formations for geologic sequestration of carbon dioxide because of their reactive divalent-cation containing silicates, such as forsterite (Mg2SiO4), suitable for long-term trapping of CO2 mineralized as metal carbonates. The goal of this study was to investigate at a molecular level the carbonation products formed during the reaction of forsterite with supercritical CO2 (scCO2) as a function of the concentration of H2O adsorbed to the forsterite surface. Experiments were performed at 50 °C and 90 bar using an in situ IR titration capability, and post-reaction samples were examined by ex situ techniques, including SEM, XPS, FIB-TEM, TGA-MS, and MAS-NMR. Carbonation products and reaction extents varied greatly with adsorbed H2O. We show for the first time evidence of Mg-carbonate surface complexation under wet scCO2 conditions. Carbonate is found to be coordinated to Mg at the forsterite surface in a predominately bidentate fashion at adsorbed H2O concentrations below 27 µmol/m2. Above this concentration and up to 76 µmol/m2, monodentate coordinated complexes become dominant. Beyond a threshold adsorbed H2O concentration of 76 µmol/m2, crystalline carbonates continuously precipitate as magnesite, and the particles that form are hundreds of times larger than the estimated thicknesses of the adsorbed water films of about 7 to 15 Å. At an applied level, these results suggest that mineral carbonation in scCO2 dominated fluids near the wellbore and adjacent to caprocks will be insignificant and limited to surface complexation, unless adsorbed H2O concentrations are high enough to promote crystalline carbonate formation. At a fundamental level, the surface complexes and their dependence on adsorbed H2O concentration give insights regarding forsterite dissolution processes and magnesite nucleation and growth.

Environmental Molecular Sciences Laboratory↗
NASA NTRS1985

Measurements of concentrations of chlorofluoromethanes (CFMs) carbon dioxide and carbon isotope ratio in stratospheric and tropospheric air by grab-sampling systems

Measurements of concentrations of chlorofluoromethanes (CFMs), carbon dioxide and carbon isotope ratio in stratospheric and tropospheric air by grab-sampling systems are reported. The balloon-borne grab-sampling system has been launched from Sanriku Balloon Center three times since 1981. It consists of: (1) six sampling cylinders, (2) eight motor driven values, (3) control and monitor circuits, and (4) pressurized housing. Particular consideration is paid to the problem of contamination. Strict requirements are placed on the choice of materials and components, construction methods, cleaning techniques, vacuum integrity, and sampling procedures. An aluminum pressurized housing and a 4-m long inlet line are employed to prevent the sampling air from contamination by outgassing of sampling and control devices. The sampling is performed during the descent of the system. Vertical profiles of mixing ratios of CF2Cl2, CFCl3 and CH4 are given. Mixing ratios of CF2Cl2 and CFCl3 in the stratosphere do not show the discernible effect of the increase of those in the ground level background, and decrease with altitude. Decreasing rate of CFCl3 is larger than that of CF2Cl2. CH4 mixing ratio, on the other hand, shows diffusive equilibrium, as the photodissociation cross section of CH4 is small and concentrations of OH radical and 0(sup I D) are low.

Itoh, T.↗
NASA NTRS1999

CO2 Compressor Requirements for Integration of Space Station Carbon Dioxide Removal and Carbon Dioxide Reduction Assemblies

This paper describes the analysis on integration requirements, CO2 compressor in particular, for integration of Carbon Dioxide Removal Assembly (CDRA) and CO2 Reduction Assembly (CRA) as a part of the Node 3 project previously conducted at JSC/NASA. A system analysis on the volume and operation pressure range of the CO2 accumulator was conducted. The hardware and operational configurations of the CO2 compressor were developed. The performance and interface requirements of the compressor were specified. An existing Four-Bed Molecular Sieve CO2 removal computer model was modified into a CDRA model and used in analyzing the requirements of the CDRA CO2 compressor. This CDRA model was also used in analyzing CDRA operation parameters that dictate CO2 pump sizing. Strategy for the pump activation was also analyzed.

Jeng, Frank F.↗
DOE OSTI2024

Electrochemical generation of carbon-containing products from carbon dioxide and carbon monoxide

Disclosed herein is a method of electroreduction with a working electrode and counter electrode. The method includes a step of electrocatalyzing carbon monoxide and/or carbon dioxide in the presence of one or more nucleophilic co-reactants in contact with a catalytically active material present on the working electrode, thereby forming one or more carbon-containing products electrocatalytically.

Jiao, Feng↗
DOE OSTI2013

Visible-Light Photoredox Catalysis: Selective Reduction of Carbon Dioxide to Carbon Monoxide by a Nickel N-Heterocyclic Carbene-Isoquinoline Complex

The solar-driven reduction of carbon dioxide to value-added chemical fuels is a longstanding challenge in the fields of catalysis, energy science, and green chemistry. In order to develop effective CO2 fixation, several key considerations must be balanced, including (1) catalyst selectivity for promoting CO2 reduction over competing hydrogen generation from proton reduction, (2) visible-light harvesting that matches the solar spectrum, and (3) the use of cheap and earth-abundant catalytic components. In this report, we present the synthesis and characterization of a new family of earth-abundant nickel complexes supported by N-heterocyclic carbene amine ligands that exhibit high selectivity and activity for the electrocatalytic and photocatalytic conversion of CO2 to CO. Systematic changes in the carbene and amine donors of the ligand have been surveyed, and [Ni(Prbimiq1)]2+ (1c, where Prbimiq1 = bis(3-(imidazolyl)isoquinolinyl)propane) emerges as a catalyst for electrochemical reduction of CO2 with the lowest cathodic onset potential (Ecat = 1.2 V vs SCE). Using this earth-abundant catalyst with Ir(ppy)3 (where ppy = 2-phenylpyridine) and an electron donor, we have developed a visible-light photoredox system for the catalytic conversion of CO2 to CO that proceeds with high selectivity and activity and achieves turnover numbers and turnover frequencies reaching 98,000 and 3.9 s1, respectively. Further studies reveal that the overall efficiency of this solar-to-fuel cycle may be limited by the formation of the active Ni catalyst and/or the chemical reduction of CO2 to CO at the reduced nickel center and provide a starting point for improved photoredox systems for sustainable carbon-neutral energy conversion.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗
DOE OSTI2019

Oxidation of High Yield Strength Metals Tungsten and Rhenium in High-Pressure High-Temperature Experiments of Carbon Dioxide and Carbonates

The laser-heating diamond-anvil cell technique enables direct investigations of materials under high pressures and temperatures, usually confining the samples with high yield strength W and Re gaskets. This work presents experimental data that evidences the chemical reactivity between these refractory metals and CO 2 or carbonates at temperatures above 1300 °C and pressures above 6 GPa. Metal oxides and diamond are identified as reaction products. Recommendations to minimize non-desired chemical reactions in high-pressure high-temperature experiments are given.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Emerging concepts in intermediate carbon dioxide emplacement to support carbon dioxide removal

Substantial upscaling of carbon dioxide capture is possible in the coming decades but existing solutions for storage are projected to be limited in annual capacity by as much as 2–10 GtCO 2 per year until mid-century. Temporary storage of CO 2 in a solid or liquid state could prove useful for filling this gap in capacity, until more permanent and ideally lucrative CO 2 sequestration options come online. There are several concepts for reversible solid-state and chemical CO 2 storage, but their advantages and limitations have yet to be reviewed in this context. This article focuses on the physical and chemical aspects of CO 2 storage via liquid and solid chemical carriers and sorbents, and gives an overview of the energetics around their use, as well as prospects for their future development. Exciting opportunities for coupling capture and medium to high maturity multi-year storage technologies could support carbon removal in the coming decades. Highlights of the analysis are the remarkable storage capacity of oxalic acid and formic acid (CO 2 -density of 1857 kg m –3 and 1152 kg m –3 , compared with condensed liquid CO 2 at 993–1096 kg m –3 , respectively), the relative scalability and compatibility of carbonate salts for stationary storage with direct air capture, and the potential promise of multiple carriers for CO 2 transportation. Solid sorbents do not achieve such ultra-high storage capacities, but could improve storage over compressed gas tanks on a capacity and energetics basis.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

A mathematical analysis of carbon fixing materials that grow, reinforce, and self-heal from atmospheric carbon dioxide

Carbon fixing materials are a new class of self-healing, self-reinforcing materials we have introduced that utilize ambient CO 2 to chemically add to an ever extending carbon backbone. This class of materials can utilize biological or non-biological photocatalysts and support a wide range of potential backbone chemistries. However, there is no analysis to date that describes their fundamental limits in terms of chemical kinetics and mass transfer. In this computational study, we employ a reaction engineering, and materials science analysis to answer basic questions about the maximum growth rate, photocatalytic requirements and limits of applicable materials. Our proposed mathematical framework envelops three main functions required for carbon fixing materials: (1) adsorption of CO 2 from air, (2) photocatalytic reduction of CO 2 into selected monomers, and (3) polymerization of CO 2 -derived monomers. First, by performing a Damköhler number analysis, we derive criteria for the cross over from kinetic control to mass transfer limited growth, setting upper limits on performance of a potential photocatalyst. Next, we analyze photocatalytic reduction of CO 2 to single carbon products, using known catalytic pathways and kinetic data. We identify formaldehyde as a C1 intermediate having unique potential for incorporation into the material backbone of carbon fixing materials. As an example, we find that a diamond-shaped reaction network graph for CO 2 reduction, passing through CO and HCOOH intermediates, accurately describes kinetic data for cobalt-promoted TiO 2 nanoparticles at room temperature and 1 atm CO 2 . Finally, as an applied case study, we consider and analyze the example of a carbon fixing poly(oxymethylene) system with embedded catalyst promoting the photocatalytic reduction of CO 2 to formaldehyde. The latter then trimerizes to a trioxane monomer which subsequently polymerizes to polyoxymethylene. This reaction engineering analysis introduces benchmarks for carbon fixing materials with respect to achievable rates of photocatalysis, adsorption, and polymerization. These results should prove valuable for the design, evaluation, and benchmarking of this emergent and new class of environmentally sustainable materials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗