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Soot precursor formation and limitations of the stabilomer grid

Proceedings of the Combustion Institute

Johansson, Karl O.; Lai, J.Y.W.; Skeen, Scott A.; Popolan-Vaida, D.M.; Wilson, K.R.; Hansen, Nils H.; Violi, A.; Michelsen, Hope A.

We have combined experimental and theoretical approaches to gain new insight into the mechanisms of PAH growth and soot formation. The experimental approach involves aerosol-mass spectrometry in conjunction with vacuum-ultraviolet photoionization of volatile species vaporizing from particles sampled from an Ar-diluted C2H2/O2 counter-flow diffusion flame at nearly atmospheric pressure (700 Torr). We recorded aerosol mass spectra at different distances from the fuel outlet for fixed ionization energies and in a fixed position while tuning the photoionization energy. The mass spectra contain a large distribution of peaks, highlighting the importance of small building blocks and showing a variety of chemical species that extends beyond the traditional classification of PAHs based on thermodynamic stability. In addition, we performed stochastic simulations of PAH growth in the flame in order to provide better insight into the chemical composition of species associated with peaks in the measured mass spectra. These simulations were conducted using a stochastic nanoparticle simulator (SNAPS). Synthesis of experimental and simulated results showed that peaks in the observed mass spectra generally consisted of a mixture of PAH isomers. At m/z =154 and 202, for example, experiments and simulations suggested that additional isomers than biphenyl and pyrene are important. Furthermore, the results highlight the importance of odd-carbon numbered species and complex growth paths. The experimental results suggest that species of higher masses can build up concentration ahead of species of lower masses. Our experimental results show, for example, that the peak at m/z = 278 appears closer to the burner outlet than the peak at m/z = 202, i.e., suggesting that a single monotonic growth mechanism is not enough.

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TYPE Conference Poster YEAR 2015
ScopusOSTI

Greenhouse Gas Source Attribution: Measurements Modeling and Uncertainty Quantification

Liu, Zhen L.; Safta, Cosmin S.; Sargsyan, Khachik S.; Najm, H.N.; van Bloemen Waanders, Bart G.; LaFranchi, Brian L.; Ivey, Mark D.; Schrader, Paul E.; Michelsen, Hope A.; Bambha, Ray B.

In this project we have developed atmospheric measurement capabilities and a suite of atmospheric modeling and analysis tools that are well suited for verifying emissions of green- house gases (GHGs) on an urban-through-regional scale. We have for the first time applied the Community Multiscale Air Quality (CMAQ) model to simulate atmospheric CO2 . This will allow for the examination of regional-scale transport and distribution of CO2 along with air pollutants traditionally studied using CMAQ at relatively high spatial and temporal resolution with the goal of leveraging emissions verification efforts for both air quality and climate. We have developed a bias-enhanced Bayesian inference approach that can remedy the well-known problem of transport model errors in atmospheric CO2 inversions. We have tested the approach using data and model outputs from the TransCom3 global CO2 inversion comparison project. We have also performed two prototyping studies on inversion approaches in the generalized convection-diffusion context. One of these studies employed Polynomial Chaos Expansion to accelerate the evaluation of a regional transport model and enable efficient Markov Chain Monte Carlo sampling of the posterior for Bayesian inference. The other approach uses de- terministic inversion of a convection-diffusion-reaction system in the presence of uncertainty. These approaches should, in principle, be applicable to realistic atmospheric problems with moderate adaptation. We outline a regional greenhouse gas source inference system that integrates (1) two ap- proaches of atmospheric dispersion simulation and (2) a class of Bayesian inference and un- certainty quantification algorithms. We use two different and complementary approaches to simulate atmospheric dispersion. Specifically, we use a Eulerian chemical transport model CMAQ and a Lagrangian Particle Dispersion Model - FLEXPART-WRF. These two models share the same WRF assimilated meteorology fields, making it possible to perform a hybrid simulation, in which the Eulerian model (CMAQ) can be used to compute the initial condi- tion needed by the Lagrangian model, while the source-receptor relationships for a large state vector can be efficiently computed using the Lagrangian model in its backward mode. In ad- dition, CMAQ has a complete treatment of atmospheric chemistry of a suite of traditional air pollutants, many of which could help attribute GHGs from different sources. The inference of emissions sources using atmospheric observations is cast as a Bayesian model calibration problem, which is solved using a variety of Bayesian techniques, such as the bias-enhanced Bayesian inference algorithm, which accounts for the intrinsic model deficiency, Polynomial Chaos Expansion to accelerate model evaluation and Markov Chain Monte Carlo sampling, and Karhunen-Lo %60 eve (KL) Expansion to reduce the dimensionality of the state space. We have established an atmospheric measurement site in Livermore, CA and are collect- ing continuous measurements of CO2 , CH4 and other species that are typically co-emitted with these GHGs. Measurements of co-emitted species can assist in attributing the GHGs to different emissions sectors. Automatic calibrations using traceable standards are performed routinely for the gas-phase measurements. We are also collecting standard meteorological data at the Livermore site as well as planetary boundary height measurements using a ceilometer. The location of the measurement site is well suited to sample air transported between the San Francisco Bay area and the California Central Valley.

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TYPE SAND Report YEAR 2014
OSTIDOI

Studies of laminar opposed-flow diffusion flames of acetylene at low-pressures with photoionization mass spectrometry

Proceedings of the Combustion Institute

Skeen, Scott A.; Yang, B.; Michelsen, Hope A.; Miller, J.A.; Violi, A.; Hansen, Nils H.

We have designed an opposed-flow flame system to investigate the chemical composition of non-premixed flames using in situ flame-sampling molecular-beam mass spectrometry with synchrotron-generated tunable vacuum-ultraviolet light as an ionization source. This paper provides details of the experimental apparatus, sampling method, and data-reduction procedures. To test the system, we have investigated the chemical composition of three low-pressure (30-50 Torr), non-premixed, opposed-flow acetylene( Ar)/O2(Ar) flames. We measured quantitative mole-fraction profiles as a function of the distance from the fuel outlet for the major species and several intermediates, including the methyl and propargyl radicals. We determined the temperature profiles of these flames by normalizing a sampling-instrument function to thermocouple measurements near the fuel outlet. A comparison of the experimental temperature and major species profiles with modeling results indicates that flame perturbations caused by the sampling probe are minimal. The observed agreement between experimental and modeled results, apparent for most combustion species, is similar to corresponding studies of premixed flames. © 2012 The Combustion Institute.

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TYPE Conference YEAR 2013
ScopusOSTI
Results 26–50 of 70
Results 26–50 of 70