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NASA NTRS1994

Active chlorine and nitric oxide formation from chemical rocket plume afterburning

Chlorine and oxides of nitrogen (NO(x)) released into the atmosphere contribute to acid rain (ground level or low-altitude sources) and ozone depletion from the stratosphere (high-altitude sources). Rocket engines have the potential for forming or activating these pollutants in the rocket plume. For instance, H2/O2 rockets can produce thermal NO(x) in their plumes. Emphasis, in the past, has been placed on determining the impact of chlorine release on the stratosphere. To date, very little, if any, information is available to understand what contribution NO(x) emissions from ground-based engine testing and actual rocket launches have on the atmosphere. The goal of this work is to estimate the afterburning emissions from chemical rocket plumes and determine their local stratospheric impact. Our study focuses on the space shuttle rocket motors, which include both the solid rocket boosters (SRB's) and the liquid propellant main engines (SSME's). Rocket plume afterburning is modeled employing a one-dimensional model incorporating two chemical kinetic systems: chemical and thermal equilibria with overlayed nitric oxide chemical kinetics (semi equilibrium) and full finite-rate chemical kinetics. Additionally, the local atmospheric impact immediately following a launch is modeled as the emissions diffuse and chemically react in the stratosphere.

Leone, D. M.↗

NASA NTRS1998

EOS Interdisciplinary Investigation: Observational and Modeling Studies of Radiative, Chemical, and Dynamical Interactions in the Earth's Atmosphere

A 3-dimensional model of atmospheric dynamics and photochemistry has been developed from the primitive equations in isentropic coordinates. The model extends from the upper troposphere through the middle atmosphere and is driven by observed dynamical and chemical structure in the troposphere. The model's formulation is entirely spectral: Horizontal structure is represented in terms of vector Hough functions, which explicitly partition the motion into its rotational and divergent components. This formulation enables the model's computational performance to be increased dramatically by filtering high-frequency gravity waves, which do not affect PV conservation. Vertical structure is represented in terms of eigenfunctions that follow from the primitive equations in isentropic coordinates. The model's fully spectral formulation enables scale-selective dissipation, necessary for numerical stability, to be applied at 6th order-in all 3 coordinate directions. This feature leaves all but the shortest vertical scales undamped and, consequently, allows potential vorticity and chemical tracers to be conserved quite accurately, distinctly better than in the model's layered counterpart. These dynamical features are complemented by a basic but fairly complete treatment of gas phase photochemistry, which accounts for some 48 chemical species, diurnally-varying SW absorption by O2 and O3, and LW cooling calculated via a detailed band calculation of radiative transfer. Driven by observed tropospheric structure, the 3D model reproduces observed structure in the middle atmosphere, inclusive of transport by the Brewer-Dobson circulation and accompanying chemical variations. Calculated residual motion is consistent with diabatic cooling rates, poleward transport, and descent in the polar night derived from satellite measurements of chemical tracers made from LIMS, SAGE, and UARS. The model also reproduces the observed structure of chemical species like O3, HNO3, and ClO. At the same time, it provides a respectable 3D simulation of the wintertime increase of midlatitude total ozone, as well as its geographical structure observed by Nimbus-7 TOMS. The 3D model has been used to explore the origin of diabatic upwelling in the tropical lower stratosphere, which has been related to planetary wave absorption in the winter- time stratosphere, as well as to influences from tropospheric convection at the tropical tropopause.

Salby, Murry L.↗

NASA NTRS1998

Chemical Gas Sensors for Aerospace Applications

Chemical sensors often need to be specifically designed (or tailored) to operate in a given environment. It is often the case that a chemical sensor that meets the needs of one application will not function adequately in another application. The more demanding the environment and specialized the requirement, the greater the need to adapt exiting sensor technologies to meet these requirements or, as necessary, develop new sensor technologies. Aerospace (aeronautic and space) applications are particularly challenging since often these applications have specifications which have not previously been the emphasis of commercial suppliers. Further, the chemical sensing needs of aerospace applications have changed over the years to reflect the changing emphasis of society. Three chemical sensing applications of particular interest to the National Aeronautics and Space Administration (NASA) which illustrate these trends are launch vehicle leak detection, emission monitoring, and fire detection. Each of these applications reflects efforts ongoing throughout NASA. As described in NASA's "Three Pillars for Success", a document which outlines NASA's long term response to achieve the nation's priorities in aerospace transportation, agency wide objectives include: improving safety and decreasing the cost of space travel, significantly decreasing the amount of emissions produced by aeronautic engines, and improving the safety of commercial airline travel. As will be discussed below, chemical sensing in leak detection, emission monitoring, and fire detection will help enable the agency to meet these objectives. Each application has vastly different problems associated with the measurement of chemical species. Nonetheless, the development of a common base technology can address the measurement needs of a number of applications.

Hunter, Gary W.↗

NASA NTRS2001

Thermal and Chemical Characterization of Non-metallic Materials Using Coupled Thermogravimetric Analysis and Infrared Spectroscopy

Thermogravimetric analysis (TGA) is widely employed in the thermal characterization of non-metallic materials, yielding valuable information on decomposition characteristics of a sample over a wide temperature range. However, a potential wealth of chemical information is lost during the process, with the evolving gases generated during thermal decomposition escaping through the exhaust line. Fourier Transform-Infrared spectroscopy (FT-IR) is a powerful analytical technique for determining many chemical constituents while in any material state, in this application, the gas phase. By linking these two techniques, evolving gases generated during the TGA process are directed into an appropriately equipped infrared spectrometer for chemical speciation. Consequently, both thermal decomposition and chemical characterization of a material may be obtained in a single sample run. In practice, a heated transfer line is employed to connect the two instruments while a purge gas stream directs the evolving gases into the FT-IR, The purge gas can be either high purity air or an inert gas such as nitrogen to allow oxidative and pyrolytic processes to be examined, respectively. The FT-IR data is collected real-time, allowing continuous monitoring of chemical compositional changes over the course of thermal decomposition. Using this coupled technique, an array of diverse materials has been examined, including composites, plastics, rubber, fiberglass epoxy resins, polycarbonates, silicones, lubricants and fluorocarbon materials. The benefit of combining these two methodologies is of particular importance in the aerospace community, where newly developing materials have little available data with which to refer. By providing both thermal and chemical data simultaneously, a more definitive and comprehensive characterization of the material is possible. Additionally, this procedure has been found to be a viable screening technique for certain materials, with the generated data useful in the selection of other appropriate analytical procedures for further material characterization.

Huff, Timothy L.↗

NASA NTRS1999

Development of a Computational Chemical Vapor Deposition Model: Applications to Indium Nitride and Dicyanovinylaniline

A computational chemical vapor deposition (CVD) model is presented, that couples chemical reaction mechanisms with fluid dynamic simulations for vapor deposition experiments. The chemical properties of the systems under investigation are evaluated using quantum, molecular and statistical mechanics models. The fluid dynamic computations are performed using the CFD-ACE program, which can simulate multispecies transport, heat and mass transfer, gas phase chemistry, chemistry of adsorbed species, pulsed reactant flow and variable gravity conditions. Two experimental setups are being studied, in order to fabricate films of: (a) indium nitride (InN) from the gas or surface phase reaction of trimethylindium and ammonia; and (b) 4-(1,1)dicyanovinyl-dimethylaminoaniline (DCVA) by vapor deposition. Modeling of these setups requires knowledge of three groups of properties: thermodynamic properties (heat capacity), transport properties (diffusion, viscosity, and thermal conductivity), and kinetic properties (rate constants for all possible elementary chemical reactions). These properties are evaluated using computational methods whenever experimental data is not available for the species or for the elementary reactions. The chemical vapor deposition model is applied to InN and DCVA. Several possible InN mechanisms are proposed and analyzed. The CVD model simulations of InN show that the deposition rate of InN is more efficient when pulsing chemistry is used under conditions of high pressure and microgravity. An analysis of the chemical properties of DCVA show that DCVA dimers may form under certain conditions of physical vapor transport. CVD simulations of the DCVA system suggest that deposition of the DCVA dimer may play a small role in the film and crystal growth processes.

Cardelino, Carlos↗

NASA NTRS2002

Thermal and Chemical Characterization of Non-Metallic Materials Using Coupled Thermogravimetric Analysis and Infrared Spectroscopy

Thermogravimetric analysis (TGA) is widely employed in the thermal characterization of non-metallic materials, yielding valuable information on decomposition characteristics of a sample over a wide temperature range. However, a potential wealth of chemical information is lost during the process, with the evolving gases generated during thermal decomposition escaping through the exhaust line. Fourier Transform-Infrared spectroscopy (FT-IR) is a powerful analytical technique for determining many chemical constituents while in any material state, in this application, the gas phase. By linking these two techniques, evolving gases generated during the TGA process are directed into an appropriately equipped infrared spectrometer for chemical speciation. Consequently, both thermal decomposition and chemical characterization of a material may be obtained in a single sample run. In practice, a heated transfer line is employed to connect the two instruments while a purge gas stream directs the evolving gases into the FT-IR. The purge gas can be either high purity air or an inert gas such as nitrogen to allow oxidative and pyrolytic processes to be examined, respectively. The FT-IR data is collected realtime, allowing continuous monitoring of chemical compositional changes over the course of thermal decomposition. Using this coupled technique, an array of diverse materials has been examined, including composites, plastics, rubber, fiberglass epoxy resins, polycarbonates, silicones, lubricants and fluorocarbon materials. The benefit of combining these two methodologies is of particular importance in the aerospace community, where newly developing materials have little available data with which to refer. By providing both thermal and chemical data simultaneously, a more definitive and comprehensive characterization of the material is possible. Additionally, this procedure has been found to be a viable screening technique for certain materials, with the generated data useful in the selection of other appropriate analytical procedures for further material characterization.

Huff, Timothy L.↗

NASA NTRS2005

Solar Electric and Chemical Propulsion for a Titan Mission

Systems analyses were performed for a Titan Explorer Mission characterized by Earth-Saturn transfer stages using solar electric power generation and propulsion systems for primary interplanetary propulsion, and chemical propulsion for capture at Titan. An examination of a range of system factors was performed to determine their effect on the payload delivery capability to Titan. The effect of varying launch vehicle type, solar array power level, ion thruster number, specific impulse, trip time, and Titan capture stage chemical propellant choice was investigated. The major purpose of the study was to demonstrate the efficacy of applying advanced ion propulsion system technologies like NASA's Evolutionary Xenon Thruster (NEXT), coupled with state-of-the-art (SOA) and advanced chemical technologies to a Flagship class mission. This study demonstrated that a NASA Design Reference Mission (DRM) payload of 406 kg could be successfully delivered to Titan using the baseline advanced ion propulsion system in conjunction with SOA chemical propulsion for Titan capture. In addition, the SEPS/Chemical system of this study is compared to an all- chemical NASA DRM mission. Results showed that the NEXT- based SEPS/Chemical system was able to deliver the required payload to Titan in 5 years less transfer time and on a smaller launch vehicle than the SOA chemical option.

Cupples, Michael↗

NASA NTRS2007

Sampling and Chemical Analysis of Potable Water for ISS Expeditions 12 and 13

The crews of Expeditions 12 and 13 aboard the International Space Station (ISS) continued to rely on potable water from two different sources, regenerated humidity condensate and Russian ground-supplied water. The Space Shuttle launched twice during the 12- months spanning both expeditions and docked with the ISS for delivery of hardware and supplies. However, no Shuttle potable water was transferred to the station during either of these missions. The chemical quality of the ISS onboard potable water supplies was verified by performing ground analyses of archival water samples at the Johnson Space Center (JSC) Water and Food Analytical Laboratory (WAFAL). Since no Shuttle flights launched during Expedition 12 and there was restricted return volume on the Russian Soyuz vehicle, only one chemical archive potable water sample was collected with U.S. hardware and returned during Expedition 12. This sample was collected in March 2006 and returned on Soyuz 11. The number and sensitivity of the chemical analyses performed on this sample were limited due to low sample volume. Shuttle flights STS-121 (ULF1.1) and STS-115 (12A) docked with the ISS in July and September of 2006, respectively. These flights returned to Earth with eight chemical archive potable water samples that were collected with U.S. hardware during Expedition 13. The average collected volume increased for these samples, allowing full chemical characterization to be performed. This paper presents a discussion of the results from chemical analyses performed on Expeditions 12 and 13 archive potable water samples. In addition to the results from the U.S. samples analyzed, results from pre-flight samples of Russian potable water delivered to the ISS on Progress vehicles and in-flight samples collected with Russian hardware during Expeditions 12 and 13 and analyzed at JSC are also discussed.

Straub, John E. II↗

NASA NTRS2004

Multilayer article having stabilized zirconia outer layer and chemical barrier layer

A multilayer article includes a substrate that includes at least one of a ceramic compound and a Si-containing metal alloy. An outer layer includes stabilized zirconia. Intermediate layers are located between the outer layer and the substrate and include a mullite-containing layer and a chemical barrier layer. The mullite-containing layer includes 1) mullite or 2) mullite and an alkaline earth metal aluminosilicate. The chemical barrier layer is located between the mullite-containing layer and the outer layer. The chemical barrier layer includes at least one of mullite, hafnia, hafnium silicate and rare earth silicate (e.g., at least one of RE.sub.2 SiO.sub.5 and RE.sub.2 Si.sub.2 O.sub.7 where RE is Sc or Yb). The multilayer article is characterized by the combination of the chemical barrier layer and by its lack of a layer consisting essentially of barium strontium aluminosilicate between the mullite-containing layer and the chemical barrier layer. Such a barium strontium aluminosilicate layer may undesirably lead to the formation of a low melting glass or unnecessarily increase the layer thickness with concomitant reduced durability of the multilayer article. In particular, the chemical barrier layer may include at least one of hafnia, hafnium silicate and rare earth silicate.

Lee, Kang N.↗

NASA NTRS2009

Thermal Decomposition of an Impure (Roxbury) Siderite: Relevance to the Presence of Chemically Pure Magnetite Crystals in ALH84001 Carbonate Disks

The question of the origin of nanophase magnetite in Martian meteorite ALH84001 has been widely debated for nearly a decade. Golden et al. have reported producing nearly chemically pure magnetite from thermal decomposition of chemically impure siderite [(Fe, Mg, Mn)CO3]. This claim is significant for three reasons: first, it has been argued that chemically pure magnetite present in the carbonate disks in Martian meteorite ALH84001 could have formed by the thermal decomposition of the impure carbonate matrix in which they are embedded; second, the chemical purity of magnetite has been previously used to identify biogenic magnetite; and, third, previous studies of thermal decomposition of impure (Mg,Ca,Mn)-siderites, which have been investigated under a wide variety of conditions by numerous researchers, invariably yields a mixed metal oxide phase as the product and not chemically pure magnetite. The explanation for this observation is that these siderites all possess the same crystallographic structure (Calcite; R3c) so solid solutions between these carbonates are readily formed and can be viewed on an atomic scale as two chemically different but structurally similar lattices.

McKay, D.S.↗

NASA NTRS2004

Chemical Reaction and Flow Modeling in Fullerene and Nanotube Production

The development of processes to produce fullerenes and carbon nanotubes has largely been empirical. Fullerenes were first discovered in the soot produced by laser ablation of graphite [1]and then in the soot of electric arc evaporated carbon. Techniques and conditions for producing larger and larger quantities of fullerenes depended mainly on trial and error empirical variations of these processes, with attempts to scale them up by using larger electrodes and targets and higher power. Various concepts of how fullerenes and carbon nanotubes were formed were put forth, but very little was done based on chemical kinetics of the reactions. This was mainly due to the complex mixture of species and complex nature of conditions in the reactors. Temperatures in the reactors varied from several thousand degrees Kelvin down to near room temperature. There are hundreds of species possible, ranging from atomic carbon to large clusters of carbonaceous soot, and metallic catalyst atoms to metal clusters, to complexes of metals and carbon. Most of the chemical kinetics of the reactions and the thermodynamic properties of clusters and complexes have only been approximated. In addition, flow conditions in the reactors are transient or unsteady, and three dimensional, with steep spatial gradients of temperature and species concentrations. All these factors make computational simulations of reactors very complex and challenging. This article addresses the development of the chemical reaction involved in fullerene production and extends this to production of carbon nanotubes by the laser ablation/oven process and by the electric arc evaporation process. In addition, the high-pressure carbon monoxide (HiPco) process is discussed. The article is in several parts. The first one addresses the thermochemical aspects of modeling; and considers the development of chemical rate equations, estimates of reaction rates, and thermodynamic properties where they are available. The second part addresses modeling of the arc process for fullerene and carbon nanotube production using O-D, 1-D and 2-D fluid flow models. The third part addresses simulations of the pulsed laser ablation process using time-dependent techniques in 2-D, and a steady state 2-D simulation of a continuous laser ablation process. The fourth part addresses steady state modeling in O-D and 2-D of the HiPco process. In each of the simulations, there is a variety of simplifications that are made that enable one to concentrate on one aspect or another of the process. There are simplifications that can be made to the chemical reaction models , e.g. reduction in number of species by lumping some of them together in a representative species. Other simulations are carried out by eliminating the chemistry altogether in order to concentrate on the fluid dynamics. When solving problems with a large number of species in more than one spatial dimension, it is almost imperative that the problem be decoupled by solving for the fluid dynamics to find the fluid motion and temperature history of "particles" of fluid moving through a reactor. Then one can solve the chemical rate equations with complex chemistry following the temperature and pressure history. One difficulty is that often mixing with an ambient gas is involved. Therefore, one needs to take dilution and mixing into account. This changes the ratio of carbon species to background gas. Commercially available codes may have no provision for including dilution as part of the input. One must the write special solvers for including dilution in decoupled problems. The article addresses both ful1erene production and single-walled carbon nanotube (SWNT) production. There are at least two schemes or concepts of SWNT growth. This article will only address growth in the gas phase by carbon and catalyst cluster growth and SW T formation by the addition of carbon. There are other models that conceive of SWNT growth as a phase separation process from clusters me up carbon and metal catalyst, with the carbon precipitating from the cluster as it cools. We will not deal with that concept in this article. Further research is needed to determine the rates at which these composite clusters form, evaporate, and segregate.

Scott, Carl D.↗

NASA NTRS2013

A Combined Solar Electric and Storable Chemical Propulsion Vehicle for Piloted Mars Missions

The Mars Design Reference Architecture (DRA) 5.0 explored a piloted Mars mission in the 2030 timeframe, focusing on architecture and technology choices. The DRA 5.0 focused on nuclear thermal and cryogenic chemical propulsion system options for the mission. Follow-on work explored both nuclear and solar electric options. One enticing option that was found in a NASA Collaborative Modeling for Parametric Assessment of Space Systems (COMPASS) design study used a combination of a 1-MW-class solar electric propulsion (SEP) system combined with storable chemical systems derived from the planned Orion crew vehicle. It was found that by using each propulsion system at the appropriate phase of the mission, the entire SEP stage and habitat could be placed into orbit with just two planned Space Launch System (SLS) heavy lift launch vehicles assuming the crew would meet up at the Earth-Moon (E-M) L2 point on a separate heavy-lift launch. These appropriate phases use high-thrust chemical propulsion only in gravity wells when the vehicle is piloted and solar electric propulsion for every other phase. Thus the SEP system performs the spiral of the unmanned vehicle from low Earth orbit (LEO) to E-M L2 where the vehicle meets up with the multi-purpose crew vehicle. From here SEP is used to place the vehicle on a trajectory to Mars. With SEP providing a large portion of the required capture and departure changes in velocity (delta V) at Mars, the delta V provided by the chemical propulsion is reduced by a factor of five from what would be needed with chemical propulsion alone at Mars. This trajectory also allows the SEP and habitat vehicle to arrive in the highly elliptic 1-sol parking orbit compatible with envisioned Mars landing concepts. This paper explores mission options using between SEP and chemical propulsion, the design of the SEP system including the solar array and electric propulsion systems, and packaging in the SLS shroud. Design trades of stay time, power level, specific impulse and propellant type are discussed.

Mercer, Carolyn R.↗

NASA NTRS2013

Chemical Microsensor Development for Aerospace Applications

Numerous aerospace applications, including low-false-alarm fire detection, environmental monitoring, fuel leak detection, and engine emission monitoring, would benefit greatly from robust and low weight, cost, and power consumption chemical microsensors. NASA Glenn Research Center has been working to develop a variety of chemical microsensors with these attributes to address the aforementioned applications. Chemical microsensors using different material platforms and sensing mechanisms have been produced. Approaches using electrochemical cells, resistors, and Schottky diode platforms, combined with nano-based materials, high temperature solid electrolytes, and room temperature polymer electrolytes have been realized to enable different types of microsensors. By understanding the application needs and chemical gas species to be detected, sensing materials and unique microfabrication processes were selected and applied. The chemical microsensors were designed utilizing simple structures and the least number of microfabrication processes possible, while maintaining high yield and low cost. In this presentation, an overview of carbon dioxide (CO2), oxygen (O2), and hydrogen/hydrocarbons (H2/CxHy) microsensors and their fabrication, testing results, and applications will be described. Particular challenges associated with improving the H2/CxHy microsensor contact wire-bonding pad will be discussed. These microsensors represent our research approach and serve as major tools as we expand our sensor development toolbox. Our ultimate goal is to develop robust chemical microsensor systems for aerospace and commercial applications.

hydrogen sensors↗

NASA NTRS2014

A Combined Solar Electric and Storable Chemical Propulsion Vehicle for Piloted Mars Missions

Mercer, Carolyn R.↗

NASA NTRS2021

Perseverance’s Scanning Habitable Environments with Raman and Luminescence for Organics and Chemicals (SHERLOC) Investigation

The Scanning Habitable Environments with Raman and Luminescence for Organics and Chemicals (SHERLOC) is a robotic arm-mounted instrument on NASA’s Perseverance rover. SHERLOC has two primary boresights. The Spectroscopy boresight generates spatially resolved chemical maps using fluorescence and Raman spectroscopy coupled to microscopic images (10.1 μm/pixel). The second boresight is a Wide Angle Topographic Sensor for Operations and eNgineering (WATSON); a copy of the Mars Science Laboratory (MSL) Mars Hand Lens Imager (MAHLI) that obtains color images from microscopic scales (∼13 μm/pixel) to infinity. SHERLOC Spectroscopy focuses a 40 μs pulsed deep UV neon-copper laser (248.6 nm), to a ∼100 μm spot on a target at a working distance of ∼48 mm. Fluorescence emissions from organics, and Raman scattered photons from organics and minerals, are spectrally resolved with a single diffractive grating spectrograph with a spectral range of 250 to ∼370 nm. Because the fluorescence and Raman regions are naturally separated with deep UV excitation (<250 nm), the Raman region ∼ 800 – 4000 cm−1 (250 to 273 nm) and the fluorescence region (274 to ∼370 nm) are acquired simultaneously without time gating or additional mechanisms. SHERLOC science begins by using an Autofocus Context Imager (ACI) to obtain target focus and acquire 10.1 μm/pixel greyscale images. Chemical maps of organic and mineral signatures are acquired by the orchestration of an internal scanning mirror that moves the focused laser spot across discrete points on the target surface where spectra are captured on the spectrometer detector. ACI images and chemical maps (< 100 μm/mapping pixel) will enable the first Mars in situ view of the spatial distribution and interaction between organics, minerals, and chemicals important to the assessment of potential biogenicity (containing CHNOPS). Single robotic arm placement chemical maps can cover areas up to 7x7 mm in area and, with the < 10 min acquisition time per map, larger mosaics are possible with arm movements. This microscopic view of the organic geochemistry of a target at the Perseverance field site, when combined with the other instruments, such as Mastcam-Z, PIXL, and SuperCam, will enable unprecedented analysis of geological materials for both scientific research and determination of which samples to collect and cache for Mars sample return.

Rohit Bhartia↗

DOE OSTI2022

Computational Workflow for Accelerated Molecular Design Using Quantum Chemical Simulations and Deep Learning Models

Efficient methods for searching the chemical space of molecular compounds are needed to automate and accelerate the design of new functional molecules such as pharmaceuticals. Given the high cost in both resources and time for experimental efforts, computational approaches play a key role in guiding the selection of promising molecules for further investigation. Here, we construct a workflow to accelerate design by combining approximate quantum chemical methods [i.e. density-functional tight-binding (DFTB)], a graph convolutional neural network (GCNN) surrogate model for chemical property prediction, and a masked language model (MLM) for molecule generation. Property data from the DFTB calculations are used to train the surrogate model; the surrogate model is used to score candidates generated by the MLM. The surrogate reduces computation time by orders of magnitude compared to the DFTB calculations, enabling an increased search of chemical space. Furthermore, the MLM generates a diverse set of chemical modifications based on pre-training from a large compound library. We utilize the workflow to search for near-infrared photoactive molecules by minimizing the predicted HOMO-LUMO gap as the target property. Our results show that the workflow can generate optimized molecules outside of the original training set, which suggests that iterations of the workflow could be useful for searching vast chemical spaces in a wide range of design problems.

Blanchard, Andrew↗

DOE OSTI2023

Using Co-Optimized Machine Learned Manifolds for Modeling Chemically Reacting Flows

Chemically reacting flows play a key role in a wide range of engineered systems, from chemical and polymer processing to combustion-based energy conversion technologies. Simulations of these flows involve solving a coupled set of partial differential equations for mass, momentum, energy, and all relevant chemical species in the system. Chemical reaction pathways may be extremely complex and involve hundreds or more intermediate species, with reactions that occur over timescales varying by several orders of magnitude - presenting a significant numerical stiffness challenge. The combination of these factors makes simulation of chemically reacting flows vastly more expensive than nonreactive simulations, and often makes direct solution of the governing equations intractable. It is necessary to apply lower-fidelity models in place of the detailed governing equations in order to reduce computational cost to enable reacting flow simulation tools to be used in the engineering design process. Many of the models employed for this purpose are based on reducing the dimension of the thermochemical state, motivated by the observation that the observed thermochemical states in a system lie on a low-dimensional manifold in thermochemical state space. This behavior occurs due to the fast equilibration of certain reactive and transport processes, and physics-based manifold models rely on idealized assumptions about the balance of timescales and the way in which chemistry and transport are coupled. In this work, we apply a novel method for data-driven manifold-based modeling that can leverage data from high-fidelity reacting flow simulations to improve model accuracy in cases where the physics-based modeling assumptions break down. The approach is designed to be broadly applicable across chemically reacting flow systems but is applied here to turbulent combustion modeling.

machine learning↗

DOE OSTI2020

Evaluation of a New Chemical Mechanism for 2-Amino-2-methyl-1-propanol in a Reactive Environment from CSIRO Smog Chamber Experiments

Amines are considered as an emerging class of atmospheric pollutants that are of great importance to atmospheric chemistry and new particle formation. As a typical amine, 2-amino-2-methyl-1-propanol (AMP) is one of the proposed solvents for capturing CO 2 from flue gas streams in amine-based post-combustion CO 2 capture plants, and it is expected to result in AMP emission and secondary products formation in the atmosphere. However, the current knowledge of its atmospheric chemistry and kinetics is poorly understood, particularly in a reactive environment. As such, in this work we used the CSIRO smog chamber to study the photo-oxidation of AMP in the presence of VOCs–NOx surrogate mixtures over a range of initial amine concentrations. O 3 formation was significantly inhibited when AMP was added to the surrogate VOCs–NOx mixtures, implying that AMP could alter known atmospheric chemical reaction pathways and the prevailing reactivity. Simultaneously, a large amount of AMP-derived secondary aerosol was formed, with a considerably high aerosol mass yield (i.e. ratio of aerosol formed to reacted AMP) of 1.06±0.20. Based on updated knowledge of its kinetics, oxidation pathways and product yields, we have developed a new mechanism (designated as CSIAMP-19) and integrated into the Carbon Bond 6 (CB6) chemical mechanism, and evaluated it against available smog chamber data. Compared with the existing AMP mechanism (designated as CarterAMP-08), the modified CB6 with CSIAMP-19 mechanism improves prediction against AMP–VOCs–NOx experiments across a range of initial AMP concentrations, within ±10% model error for gross ozone production. Our results contribute to scientific understanding of AMP photochemistry and to the development of the chemical mechanism of other amines. The updated AMP chemical reactions scheme can be further embedded into the chemical transport model for regional modelling scenarios where AMP-related emissions are of concern.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗