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At least 721 records · Page 40

Effect of feed composition on the production of off-gases during vitrification of simulated low-activity nuclear waste

During the vitrification of nuclear waste, hazardous and radioactive emissions are generated from the feed-to-glass conversion reactions, in addition to discharges from forced air bubbling and air inleakage. Although the major gaseous emissions are water vapor, nitrogen, and carbon dioxide, various monitored environmental pollutants are also released, such as nitrogen oxides or sulfur dioxide. In addition, reactions between organics and nitrates in the feed may also form products of incomplete combustion such as carbon monoxide and acetonitrile. Although off-gas emissions are commonly measured during both laboratory- and pilot-scale melter testing, no predictive tool is currently available to a priori estimate the composition of gaseous emissions during nuclear waste vitrification. This work forms a basis for the development of such predictive tool by measuring gas evolution from a broad range of simulated low-activity waste melter feeds using evolved gas analysis data and developing correlations between the feed and off-gas compositions. Using reaction stoichiometry and regression analysis, we demonstrate that next to the content of nitrogen and organic carbon in the feed, the gaseous emissions are affected by the feed reduction-oxidation conditions – the more the feed is reduced, the less nitrogen monoxide, and more carbon monoxide and acetonitrile evolves. In conclusion, the results presented in this work provide a first step towards reducing the amount of expensive physical melter testing and the regression analysis provides a simple tool for rapid optimization of feed composition with respect to off-gas composition.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

CO quantum yield in the photolysis of CO2 at wavelength 1470 and wavelengths 1500-1670.

The results of carbon monoxide quantum yield measurements of carbon dioxide photolysis by radiation at 1470 A and in the region from 1500 to 1670 A are presented in tabular form. The experimental technique and equipment developed by Inn and Heimerl (1971) were used. These measurements, together with some previously reported ones for a longer wavelength region, are intended to provide a uniform set of values based on the same experimental technique for the entire spectral region that is relevant to the carbon-dioxide photochemistry in the atmospheres of Mars and Venus.

Inn, E. C. Y.↗

Concentrations of CH4, CO, CO2, H2, H2O and N2O in the upper stratosphere

On 23 May 1973 a cryogenic air sampler was flown on an Aerobee rocket from White Sands Missile Range. A large air sample was collected between 40 and 50 km altitude and successfully recovered for water vapor and trace gas analysis. The results were as follows: water vapor, 4.0 (+1.3 or - 0.9) ppmV; methane, 0.37 + or - 0.01 ppmV; molecular hydrogen, 0.47 + or - 0.02 ppmV; carbon monoxide, 0.05 + or - 0.01 ppmV; carbon dioxide, 316.2 + or - 2.8 ppmV; and nitrous oxide, 3 + or - 7 ppb.

Ehhalt, D. H.↗

Second-Generation Micro-Spec: A Compact Spectrometer for Far-Infrared and Submillimeter Space Missions

Micro-Spec is a direct-detection spectrometer which integrates all the components of a diffraction-grating spectrometer onto a ≈ 10-sq.cm chip through the use of superconducting microstrip transmission lines on a single- crystal silicon substrate. The second generation of Micro-Spec is being designed to operate with a spectral re- solution of at least 512 in the far-infrared and submillimeter (420–540 GHz, 714–555 μm) wavelength range, a band of interest for NASA's experiment for cryogenic large-aperture intensity mapping called EXCLAIM. EXCLAIM will be a balloon-borne telescope that is being designed to map the emission of redshifted carbon monoxide and singly-ionized carbon lines over a redshift range 0 < z < 3.5 and it will be the first demonstration of the Micro-Spec technology in a space-like environment. This work reviews the status of the Micro-Spec design for the EXCLAIM telescope, with emphasis on the spectrometer's two-dimensional diffractive region, through which light of different wavelengths is focused on kinetic inductance detectors along the instrument focal plane. An optimization process is used to generate a geometrical configuration of the diffractive region that satisfies l range and performance. An initial optical design optimized for n terms of geometric layout, spectral purity and efficiency.

Cataldo, Giuseppe↗

u-Spec Spectrometers for the EXCLAIM Instrument

The EXperiment for Cryogenic Large-aperture Intensity Mapping (EXCLAIM) is a cryogenic balloon-borne instrument that will map carbon monoxide and singly-ionized carbon emission lines across redshifts from 0to 3.5, using an intensity mapping approach. EXCLAIM will broaden our understanding of these elemental and molecular gases, and the role they play in star formation processes across cosmic time scales. The focal plane of EXCLAIM’s cryogenic telescope features sixμ-Spec spectrometers.μ-Spec is a compact, integrated grating-analog spectrometer, which uses meandered superconducting niobium microstrip transmission lines on a single-crystal silicon dielectric to synthesize the grating. It features superconducting aluminum microwave kinetic inductance detectors (MKIDs), also in a microstrip architecture. The spectrometers for EXCLAIM couple to the telescope optics via a hybrid planar antenna coupled to a silicon lenslet. The spectrometers operate from420−540 GHz with a resolving power R=λ/∆λ= 512, and employ an array of 355 MKIDs on each spectrometer. The spectrometer design targets a noise equivalent power (NEP) of 2×10−18W/√Hz (defined at the input to the main lobe of the spectrometer lenslet beam, within a 9◦half width), enabled by the cryogenic telescope environment, the sensitive MKID detectors, and the low dielectric loss of single-crystal silicon. We report on these spectrometers under development for EXCLAIM, providing an overview of the spectrometer and component designs, the spectrometer fabrication process, fabrication developments since previous prototype demonstrations, and the current status of their development for the EXCLAIM mission.

EXCLAIM Instrument↗

Validation of Carbon Trace Gas Profile Retrievals from the NOAA-Unique Combined Atmospheric Processing System for the Cross-Track Infrared Sounder

This paper provides an overview of the validation of National Oceanic and Atmospheric Administration (NOAA) operational retrievals of atmospheric carbon trace gas profiles, specifically carbon monoxide (CO), methane (CH4) and carbon dioxide (CO2), from the NOAA-Unique Combined Atmospheric Processing System (NUCAPS), a NOAA enterprise algorithm that retrieves atmospheric profile environmental data records (EDRs) under global non-precipitating (clear to partly cloudy) conditions. Vertical information about atmospheric trace gases is obtained from the Cross-track Infrared Sounder (CrIS), an infrared Fourier transform spectrometer that measures high resolution Earth radiance spectra from NOAA operational low earth orbit (LEO) satellites, including the Suomi National Polar-orbiting Partnership (SNPP) and follow-on Joint Polar Satellite System (JPSS) series beginning with NOAA-20. The NUCAPS CO, CH4, and CO2 profile EDRs are rigorously validated in this paper using well-established independent truth datasets, namely total column data from ground-based Total Carbon Column Observing Network (TCCON) sites, and in situ vertical profile data obtained from aircraft and balloon platforms via the NASA Atmospheric Tomography (ATom) mission and NOAA AirCore sampler, respectively. Statistical analyses using these datasets demonstrate that the NUCAPS carbon gas profile EDRs generally meet JPSS Level 1 global performance requirements, with the absolute accuracy and precision of CO 5% and 15%, respectively, in layers where CrIS has vertical sensitivity; CH4 and CO2 product accuracies are both found to be within ±1%, with precisions of ≈1.5% and ⪅0.5%, respectively, throughout the tropospheric column.

satellite cal/val; error analysis; greenhouse gase↗

The Experiment for Cryogenic Large-aperture Intensity Mapping (EXCLAIM)

Submillimeter and far-IR spectroscopy provides insight into galaxy evolution through measurement of atomic and molecular line emission. The EXperiment for Cryogenic Large-Aperture Intensity Mapping (EXCLAIM) is a cryogenic balloon-borne instrument designed to carry out intensity mapping to measure the cumulative redshifted line emission from carbon monoxide and singly-ionized carbon to probe star formation in windows from the present to z=3.5. During this time, the rate of star formation dropped dramatically, while dark matter continued to cluster. Intensity mapping permits a blind and complete survey of emitting gas through statistics of cumulative brightness fluctuations. EXCLAIM achieves high sensitivity using a cryogenic telescope coupled to six integrated spectrometers with spectral resolving power R=512 and employing microwave kinetic inductance detectors. Here we summarize the status of the mission.

Maryam Rahmani↗

The Experiment for Cryogenic Large-aperture Intensity Mapping (EXCLAIM)

Submillimeter and far-IR spectroscopy provides insight into galaxy evolution through atomic and molecular line emission. The EXperiment for Cryogenic Large-Aperture Intensity Mapping (EXCLAIM) is a cryogenic balloon-borne instrument designed to carry out an intensity mapping to measure the cumulative redshifted line emission from carbon monoxide and singly-ionized carbon to probe star formation in windows from the present to z=3.5. During this time, the rate of star formation dropped dramatically, while dark matter continued to cluster. Intensity mapping permits a blind and complete survey of emitting gas through statistics of cumulative brightness fluctuations. EXCLAIM achieves high sensitivity using a cryogenic telescope coupled to six integrated spectrometers with spectral resolving power R = 512 and employing kinetic inductance detectors. Here we summarize the status of the mission.

Maryam Rahmani↗

The Experiment for Cryogenic Large-aperture Intensity Mapping (EXCLAIM)

Submillimeter and far-IR spectroscopy provides insight into galaxy evolution through measurement of atomic and molecular line emission. The EXperiment for Cryogenic Large-Aperture Intensity Mapping (EXCLAIM) is a cryogenic balloon-borne instrument designed to carry out intensity mapping to measure the cumulative redshifted line emission from carbon monoxide and singly-ionized carbon to probe star formation in windows from the present to z=3.5. During this time, the rate of star formation dropped dramatically, while dark matter continued to cluster. Intensity mapping permits a blind and complete survey of emitting gas through statistics of cumulative brightness fluctuations. EXCLAIM achieves high sensitivity using a cryogenic telescope coupled to six integrated spectrometers with spectral resolving power R=512 and employing microwave kinetic inductance detectors. Here we summarize the status of the mission.

Maryam Rahmani↗

Second-generation Micro-Spec: Spectrometer Design for the Experiment for Cryogenic Large-Aperture Intensity Mapping

Micro-Spec (μ-Spec) is a direct-detection spectrometer that integrates all the components of a diffraction-grating spectrometer onto a ∼10-cm2 chip using superconducting microstrip transmission lines on a single-crystal silicon substrate. The second-generation μ-Spec has been designed to operate with a spectral resolution of ∼512 in the far-infrared and submillimeter (420–540 GHz, 714–555 μm) wavelength range, a band of interest for NASA’s EXperiment for Cryogenic Large-Aperture Intensity Mapping (EXCLAIM). EXCLAIM will be a high-altitude balloon mission that is being designed to map the emission of redshifted carbon monoxide and singly-ionized carbon lines over a redshift range 0 < z < 3.5. EXCLAIM will be the first demonstration of the μ-Spec technology in a space-like environment. This work reviews the status of the μ-Spec design for the EXCLAIM instrument, with emphasis on the spectrometer’s two-dimensional diffractive region, through which light of different wavelengths is focused on microwave kinetic inductance detectors (MKIDs) along the spectrometer focal plane. An optimization process generates a geometrical configuration of the diffractive region that satisfies specific requirements on size, operating spectral range and performance. An initial optical design optimized for EXCLAIM is presented in terms of geometric layout, spectral purity and efficiency.

Giuseppe Cataldo↗

Imaging the photochemistry of cyclobutanone using ultrafast electron diffraction: Experimental results

We investigated the ultrafast structural dynamics of cyclobutanone following photoexcitation at λ = 200 nm using gas-phase megaelectronvolt ultrafast electron diffraction. Our investigation complements the simulation studies of the same process within this special issue. It provides information about both electronic state population and structural dynamics through well-separable inelastic and elastic electron scattering signatures. We observe the depopulation of the photoexcited S 2 state of cyclobutanone with n3s Rydberg character through its inelastic electron scattering signature with a time constant of (0.29 ± 0.2) ps toward the S 1 state. The S 1 state population undergoes ring-opening via a Norrish Type-I reaction, likely while passing through a conical intersection with S 0 . The corresponding structural changes can be tracked by elastic electron scattering signatures. These changes appear with a delay of (0.14 ± 0.05) ps with respect to the initial photoexcitation, which is less than the S 2 depopulation time constant. This behavior provides evidence for the ballistic nature of the ring-opening once the S 1 state is reached. The resulting biradical species react further within (1.2 ± 0.2) ps via two rival fragmentation channels yielding ketene and ethylene, or propene and carbon monoxide. Furthermore, our study showcases the value of both gas-phase ultrafast diffraction studies as an experimental benchmark for nonadiabatic dynamics simulation methods and the limits in the interpretation of such experimental data without comparison with such simulations.

Carbon monoxide↗

A trigold carbide cation stabilized as a labile pyridine adduct

Auration of trimethylsilyldiazomethane by an (N-heterocyclic carbene)gold alkoxide affords a stable (silyldiazoalkyl)gold complex. The reaction of this species with a gold(I) fluoride, more efficient in the presence of an added gold cation equivalent, results in auration, desilylation, and N 2 loss. The putative trigold carbide cation was isolated as its pyridine adduct, a stable N-(triauromethyl)pyridinium ion. Reaction of the cationic pyridine adduct with carbon monoxide breaks the C—N bond, forming the stable trigold ketenylidene cation. Finally, DFT studies suggest substantial negative charge at the bridging carbon in the methylpyridinium analogue and in two possible intermediates, the trigold carbide cation and the pyridine adduct of a neutral digold carbide.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Network Optimization of the Electrosynthesis of Chemicals from CO2

Carbon dioxide electroreduction (ECO2R) is gaining attention due to its capacity to mitigate CO2 emissions while using electricity that would otherwise be curtailed. Its foreseeable industrial implementation requires of holistic methods to assess the technological and economic performance of ECO2R processes and integrate them in current chemical supply chains and power systems. Here, we combine techno-economic assessment and mathematical programming to find the optimal paths to electroreduce CO2 into valuable chemicals under variable electricity prices. The proposed approach is tested with a case study addressing the CO2 capture from flue gas or direct air and its electricity-powered reduction into carbon monoxide, formic acid or multi-carbon compounds. The results obtained demonstrate the ability of the framework to build ECO2R networks and provide operation profiles that respond to fluctuating electricity prices.

carbon dioxide↗