Novel mixed-experimental-and-computational strategies

 

The reaction networks responsible for fuel oxidation in combustion devices pose a number of unique scientific challenges that arise from the richly complex and inherently multi-scale nature of these processes.  Inside the piston engines that power vehicles on the road, inside the gas turbine engines that power airplanes and the electrical grid, and, more visibly, inside the candles that illuminate the dinner table, the conversion of fuel and atmospheric oxygen to products and heat does not take place in a single step.  Rather, the conversion process frequently proceeds through thousands of intermediate chemical species, which undergo tens of thousands of elementary reactions, all of which occur at rates that are strongly dependent on the local temperature, pressure, and concentrations of other chemical species.  Furthermore, these processes are inherently multi-scale phenomena—molecular interactions control the rates of isolated elementary reactions; interactions among simultaneous elementary reactions control global system reaction rates; and global system reaction rates control global observables in ways often tightly coupled with transport phenomena.  Needless to say, enormous amounts of data are required to understand and characterize these processes; and interpreting those data require interdisciplinary, data-driven solutions that embrace the inherent multi-scale nature of these processes.

Our group develops novel approaches to understanding and characterizing these processes that focus on integrating data across multiple scales as well as developing a quantitative understanding of uncertainty sources of, pushing the limits of automation in, and strengthening the connections between both experiments and models.  Our overarching motivation for creating and implementing these strategies is to provide approaches that dramatically accelerate the pace of scientific progress in predictive modeling of fuel oxidation processes relevant to increasing fuel efficiency and decreasing formation of harmful pollutants.

Relevant publications

M.P. Burke, "Harnessing the Combined Power of Theoretical and Experimental Data through Multi-Scale Informatics," International Journal of Chemical Kinetics 48 (2016) 212-235, http://dx.doi.org/10.1002/kin.20984.

M.P. Burke, C.F. Goldsmith, S.J. Klippenstein, O. Welz, H. Huang, I.O. Antonov, J.D. Savee, D.L. Osborn, J. Zádor, C.A. Taatjes, L. Sheps, "Multiscale Informatics for Low-Temperature Propane Oxidation: Further Complexities in Studies of Complex Reactions," Journal of Physical Chemistry A 119 (2015) 7095-7115, http://dx.doi.org/10.1021/acs.jpca.5b01003.

O. Welz, M.P. Burke, I.O. Antonov, C.F. Goldsmith, J.D. Savee, D.L. Osborn, C.A. Taatjes, S.J. Klippenstein, L. Sheps, "New Insights into Low-Temperature Oxidation of Propane from Synchrotron Photoionization Mass Spectrometry and Multiscale Informatics Modeling," Journal of Physical Chemistry A 119 (2015) 7116-7129, http://dx.doi.org/10.1021/acs.jpca.5b01008.

M.P. Burke, S.J. Klippenstein, L.B. Harding, "A Quantitative Explanation for the Apparent Anomalous Temperature Dependence of OH + HO2 = H2O + O2 through Multi-Scale Modeling," Proceedings of the Combustion Institute 34 (2013) 547-555, http://dx.doi.org/10.1016/j.proci.2012.05.041.

Relevant conference presentations

R. Song, N.D. DeLuca, M.P. Burke, "Towards Autonomous Kinetic Model Improvement through Automated Experiments and Computations," Eastern States Meeting of the Combustion Institute, Princeton, New Jersey, March 2016.

M.P. Burke, "The Role of Model Structural Uncertainties in Uncertainty Quantification and Experimental Design," 9th U.S. Meeting of the Combustion Institute, Cincinnati, Ohio, May 2015 (contributed).

M.P. Burke, "Combining Theoretical and Experimental Data in Uncertainty Quantification across Multiple Scales," 15th International Conference on Numerical Combustion, Avignon, France, April 2015 (invited for Mini-Symposium on "Uncertainty Quantification in Computational Combustion").

M.P. Burke, "Multi-Scale Informatics for Low-Temperature Oxidation," 2nd International Workshop on Flame Chemistry, San Francisco, California, August 2014 (invited).

M.P. Burke (with C.F. Goldsmith, S.J. Klippenstein, L. Sheps, O. Welz, J. Zádor, H. Huang, C.A. Taatjes), "Multi-Scale Informatics for Low-Temperature Propane Oxidation," 8th U.S. Meeting of the Combustion Institute, Park City, Utah, May 2013 (contributed).

M.P. Burke (with S.J. Klippenstein, L.B. Harding), "A Quantitative Explanation for the Apparent Anomalous Temperature Dependence of OH + HO2 = H2O + O2 through Multi-Scale Modeling," 34th International Symposium on Combustion, Warsaw, Poland, August 2012 (contributed).

228 Mudd, 500 W 120th Street, New York , NY 10027    212-851-0782                
©2014 Columbia University