Simulation and fitting of complex reaction network TPR: The key is the objective function

Savara, Aditya Ashi

doi:10.1016/j.susc.2016.07.001

Title: Simulation and fitting of complex reaction network TPR: The key is the objective function

Journal Article · Thu Jul 07 00:00:00 EDT 2016 · Surface Science

DOI:https://doi.org/10.1016/j.susc.2016.07.001· OSTI ID:1271860

Savara, Aditya Ashi ^[1]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

In this research, a method has been developed for finding improved fits during simulation and fitting of data from complex reaction network temperature programmed reactions (CRN-TPR). It was found that simulation and fitting of CRN-TPR presents additional challenges relative to simulation and fitting of simpler TPR systems. The method used here can enable checking the plausibility of proposed chemical mechanisms and kinetic models. The most important finding was that when choosing an objective function, use of an objective function that is based on integrated production provides more utility in finding improved fits when compared to an objective function based on the rate of production. The response surface produced by using the integrated production is monotonic, suppresses effects from experimental noise, requires fewer points to capture the response behavior, and can be simulated numerically with smaller errors. For CRN-TPR, there is increased importance (relative to simple reaction network TPR) in resolving of peaks prior to fitting, as well as from weighting of experimental data points. Using an implicit ordinary differential equation solver was found to be inadequate for simulating CRN-TPR. Lastly, the method employed here was capable of attaining improved fits in simulation and fitting of CRN-TPR when starting with a postulated mechanism and physically realistic initial guesses for the kinetic parameters.

View Accepted Manuscript (DOE)

View Accepted Manuscript (Publisher)

Cite

Export

Save

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC05-00OR22725; ERKCC96

OSTI ID:: 1271860

Alternate ID(s):: OSTI ID: 1397364

Journal Information:: Surface Science, Vol. 653; ISSN 0039-6028

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

Citation Metrics:

Cited by: 23 works

Citation information provided by
Web of Science

References (68)

Variations in Reactivity on Different Crystallographic Orientations of Cerium Oxide Mullins, David R.; Albrecht, Peter M.; Calaza, Florencia Topics in Catalysis, Vol. 56, Issue 15-17 https://doi.org/10.1007/s11244-013-0146-7	journal	July 2013
Microkinetic simulation of catalytic reactions Stoltze, Per Progress in Surface Science, Vol. 65, Issue 3-4 https://doi.org/10.1016/S0079-6816(00)00019-8	journal	October 2000
Molecular-level descriptions of surface chemistry in kinetic models using density functional theory Gokhale, Amit A.; Kandoi, Shampa; Greeley, Jeffrey P. Chemical Engineering Science, Vol. 59, Issue 22-23 https://doi.org/10.1016/j.ces.2004.09.038	journal	November 2004
Comprehensive DFT Study of Nitrous Oxide Decomposition over Fe-ZSM-5 ^† Heyden, Andreas; Peters, Baron; Bell, Alexis T. The Journal of Physical Chemistry B, Vol. 109, Issue 5 https://doi.org/10.1021/jp040549a	journal	February 2005
Theoretical investigation of the reaction mechanism of the hydrodeoxygenation of guaiacol over a Ru(0 0 0 1) model surface Lu, Jianmin; Heyden, Andreas Journal of Catalysis, Vol. 321 https://doi.org/10.1016/j.jcat.2014.11.003	journal	January 2015
Microkinetic modeling of the decarboxylation and decarbonylation of propanoic acid over Pd(111) model surfaces based on parameters obtained from first principles Lu, Jianmin; Behtash, Sina; Faheem, Muhammad Journal of Catalysis, Vol. 305 https://doi.org/10.1016/j.jcat.2013.04.026	journal	September 2013
Detailed surface reaction mechanism in a three-way catalyst Chatterjee, Daniel; Deutschmann, Olaf; Warnatz, JÃ¼rgen Faraday Discussions, Vol. 119, Issue 1 https://doi.org/10.1039/b101968f	journal	October 2001
Identity and chemical function of gallium species inferred from microkinetic modeling studies of propane aromatization over Ga/HZSM-5 catalysts Krishnamurthy, Gowri; Bhan, Aditya; Delgass, W. Nicholas Journal of Catalysis, Vol. 271, Issue 2 https://doi.org/10.1016/j.jcat.2010.02.026	journal	May 2010
Microkinetic modeling of propane aromatization over HZSM-5 Bhan, A.; Hsu, S.; Blau, G. Journal of Catalysis, Vol. 235, Issue 1 https://doi.org/10.1016/j.jcat.2005.07.005	journal	October 2005
Numerical simulation of temperature-programmed reaction data: an application in surface chemical kinetics Ellis, Gareth; Sidaway, James; McCoustra, Martin R. S. Journal of the Chemical Society, Faraday Transactions, Vol. 94, Issue 17 https://doi.org/10.1039/a803766c	journal	January 1998
Microkinetic Simulation of Temperature-Programmed Desorption Wang, Chia-Ching; Wu, Jyun-Yi; Jiang, Jyh-Chiang The Journal of Physical Chemistry C, Vol. 117, Issue 12 https://doi.org/10.1021/jp309394p	journal	March 2013
Kinetic modeling of nitrous oxide decomposition on Fe-ZSM-5 based on parameters obtained from first-principles calculations Heyden, A.; Bell, A.; Keil, F. Journal of Catalysis, Vol. 233, Issue 1 https://doi.org/10.1016/j.jcat.2005.04.003	journal	July 2005
Applicability of non-isothermal model-free predictions for assessment of conversion vs. time curves for complex processes in isothermal and quasi-isothermal conditions Budrugeac, P. Thermochimica Acta, Vol. 558 https://doi.org/10.1016/j.tca.2013.02.001	journal	April 2013
Recent advances in numerical modeling of catalytic monolith reactors Tischer, Steffen; Deutschmann, Olaf Catalysis Today, Vol. 105, Issue 3-4 https://doi.org/10.1016/j.cattod.2005.06.061	journal	August 2005
A hybrid genetic algorithm for efficient parameter estimation of large kinetic models Katare, Santhoji; Bhan, Aditya; Caruthers, James M. Computers & Chemical Engineering, Vol. 28, Issue 12 https://doi.org/10.1016/j.compchemeng.2004.07.002	journal	November 2004
Three-way catalytic converter modelling. Numerical determination of kinetic data Dubien, C.; Schweich, D. Catalysis and Automotive Pollution Control IV, Proceedings of the Fourth International Symposium (CAPoC4) https://doi.org/10.1016/S0167-2991(98)80896-3	book	January 1998
Least squares criteria for the kinetic evaluation of thermoanalytical experiments. Examples from a char reactivity study Várhegyi, Gábor; Szabó, Piroska; Jakab, Emma Journal of Analytical and Applied Pyrolysis, Vol. 57, Issue 2 https://doi.org/10.1016/S0165-2370(00)00113-3	journal	February 2001
Evaluation of kinetic parameters from TVA data. A computer simulation approach Roche, Rodney S. Journal of Applied Polymer Science, Vol. 18, Issue 12 https://doi.org/10.1002/app.1974.070181206	journal	December 1974
Mathematical Modeling of Nitrogen Desorption from an Iridium Surface: A Study of the Effects of Surface Structure and Subsurface Oxygen1 Kurkina, E. S.; Semendyaeva, N. L.; Boronin, A. I. Kinetics and Catalysis, Vol. 42, Issue 5, p. 703-717 https://doi.org/10.1023/A:1012383900909	journal	January 2001
Análise estatística e optimização de perfis de redução termoprogramada (TPR) Nele, Marcio; Moreno, Esteban Lopez; Andrade, Heloysa Martins Carvalho Química Nova, Vol. 29, Issue 4 https://doi.org/10.1590/S0100-40422006000400003	journal	January 2006
Mathematical considerations for nonisothermal kinetics in thermal decomposition Caballero, José A.; Conesa, Juan A. Journal of Analytical and Applied Pyrolysis, Vol. 73, Issue 1 https://doi.org/10.1016/j.jaap.2004.12.003	journal	March 2005
Nonlinear parameter estimation: A case study comparison Biegler, L. T.; Damiano, J. J.; Blau, G. E. AIChE Journal, Vol. 32, Issue 1 https://doi.org/10.1002/aic.690320105	journal	January 1986
A general strategy for parameter estimation in differential—algebraic systems Bilardello, P.; Joulia, X.; Le Lann, J. M. Computers & Chemical Engineering, Vol. 17, Issue 5-6 https://doi.org/10.1016/0098-1354(93)80040-T	journal	May 1993
Performance comparison of parameter estimation techniques for unidentifiable models Graciano, J. E.; Mendoza, D. F.; Le Roux, G. A. C. Computers & Chemical Engineering, Vol. 64 https://doi.org/10.1016/j.compchemeng.2014.01.009	journal	May 2014
A Program for Fitting Rate Constants in Gas Phase Chemical Kinetics Models Byrne, G. D.; DeGregoria, A. J.; Salane, D. E. SIAM Journal on Scientific and Statistical Computing, Vol. 5, Issue 3 https://doi.org/10.1137/0905046	journal	September 1984
Application of stepwise regression for dynamic parameter estimation Shacham, Mordechai; Brauner, Neima Computers & Chemical Engineering, Vol. 69 https://doi.org/10.1016/j.compchemeng.2014.06.013	journal	October 2014
Mathematical modelling of chemical processes-obtaining the best model predictions and parameter estimates using identifiability and estimability procedures McLean, Kevin A. P.; McAuley, Kim B. The Canadian Journal of Chemical Engineering, Vol. 90, Issue 2 https://doi.org/10.1002/cjce.20660	journal	October 2011
ICTAC Kinetics Committee recommendations for performing kinetic computations on thermal analysis data Vyazovkin, Sergey; Burnham, Alan K.; Criado, José M. Thermochimica Acta, Vol. 520, Issue 1-2 https://doi.org/10.1016/j.tca.2011.03.034	journal	June 2011
Integral kinetic analysis from temperature programmed reaction data: alkaline hydrolysis of ethyl acetate as test reaction Ortiz, M. I.; Romero, A.; Irabien, A. Thermochimica Acta, Vol. 141 https://doi.org/10.1016/0040-6031(89)87052-2	journal	March 1989
First-Principles Analysis of Structure Sensitivity in NO Oxidation on Pt Bray, J. M.; Schneider, W. F. ACS Catalysis, Vol. 5, Issue 2 https://doi.org/10.1021/cs501783q	journal	January 2015
A Generalized Approach for Predicting Coverage-Dependent Reaction Parameters of Complex Surface Reactions: Application to H ₂ Oxidation over Platinum Park, Young K.; Aghalayam, Preeti; Vlachos, Dionisios G. The Journal of Physical Chemistry A, Vol. 103, Issue 40 https://doi.org/10.1021/jp9916485	journal	October 1999
DFT comparison of intrinsic WGS kinetics over Pd and Pt Clay, John P.; Greeley, Jeffrey P.; Ribeiro, Fabio H. Journal of Catalysis, Vol. 320 https://doi.org/10.1016/j.jcat.2014.09.026	journal	December 2014
Accurate coverage-dependence incorporated into first-principles kinetic models: Catalytic NO oxidation on Pt (111) Wu, C.; Schmidt, D. J.; Wolverton, C. Journal of Catalysis, Vol. 286 https://doi.org/10.1016/j.jcat.2011.10.020	journal	February 2012
The compensation effect and the manifestation of lateral interactions in thermal desorption spectroscopy Niemantsverdriet, J. W.; Markert, K.; Wandelt, K. Applied Surface Science, Vol. 31, Issue 2 https://doi.org/10.1016/0169-4332(88)90062-1	journal	February 1988
Thermal desorption analysis: Comparative test of ten commonly applied procedures de Jong, A. M.; Niemantsverdriet, J. W. Surface Science, Vol. 233, Issue 3 https://doi.org/10.1016/0039-6028(90)90649-S	journal	July 1990
Temperature-Programmed Desorption and Reaction: Applications to Supported Catalysts Falconer, John L.; Schwarz, James A. Catalysis Reviews, Vol. 25, Issue 2 https://doi.org/10.1080/01614948308079666	journal	June 1983
Review and evaluation of the approximations to the temperature integral Órfão, José J. M. AIChE Journal, Vol. 53, Issue 11 https://doi.org/10.1002/aic.11296	journal	January 2007
A New Method of Analysing Temperature-Programmed Desorption (TPD) Profiles Using an Extended Integral Equation Koch, K.; Hunger, B.; Klepel, O. Journal of Catalysis, Vol. 172, Issue 1 https://doi.org/10.1006/jcat.1997.1843	journal	November 1997
Computational aspects of kinetic analysis Brown, M. E.; Maciejewski, M.; Vyazovkin, S. Thermochimica Acta, Vol. 355, Issue 1-2 https://doi.org/10.1016/S0040-6031(00)00443-3	journal	July 2000
Computational aspects of kinetic analysis. Maciejewski, Marek Thermochimica Acta, Vol. 355, Issue 1-2 https://doi.org/10.1016/S0040-6031(00)00444-5	journal	July 2000
Computational aspects of kinetic analysis. Roduit, B. Thermochimica Acta, Vol. 355, Issue 1-2 https://doi.org/10.1016/S0040-6031(00)00447-0	journal	July 2000
Computational aspects of kinetic analysis. Vyazovkin, Sergey Thermochimica Acta, Vol. 355, Issue 1-2 https://doi.org/10.1016/S0040-6031(00)00445-7	journal	July 2000
Elucidation of Intermediates and Mechanisms in Heterogeneous Catalysis Using Infrared Spectroscopy Savara, Aditya; Weitz, Eric Annual Review of Physical Chemistry, Vol. 65, Issue 1 https://doi.org/10.1146/annurev-physchem-040513-103647	journal	April 2014
An algorithm for the identification and estimation of relevant parameters for optimization under uncertainty Müller, David; Esche, Erik; López C., Diana C. Computers & Chemical Engineering, Vol. 71 https://doi.org/10.1016/j.compchemeng.2014.07.007	journal	December 2014
Reactions of methanol on W(100) and W(100)-(5 $times; 1)C surfaces Ko, E. Journal of Catalysis, Vol. 62, Issue 2 https://doi.org/10.1016/0021-9517(80)90454-6	journal	April 1980
Analysing methods for thermal desorption spectra Kautto, E.; Kuhalainen, J.; Manninen, M. Physica Scripta, Vol. 55, Issue 5 https://doi.org/10.1088/0031-8949/55/5/016	journal	May 1997
ICTAC Kinetics Committee recommendations for collecting experimental thermal analysis data for kinetic computations Vyazovkin, Sergey; Chrissafis, Konstantinos; Di Lorenzo, Maria Laura Thermochimica Acta, Vol. 590 https://doi.org/10.1016/j.tca.2014.05.036	journal	August 2014
Sample controlled thermal analysis and kinetics Criado, J. M.; Pérez-Maqueda, L. A. Journal of Thermal Analysis and Calorimetry, Vol. 80, Issue 1 https://doi.org/10.1007/s10973-005-0609-6	journal	March 2005
Aims and methods in non-isothermal reaction kinetics Várhegyi, Gábor Journal of Analytical and Applied Pyrolysis, Vol. 79, Issue 1-2 https://doi.org/10.1016/j.jaap.2007.01.007	journal	May 2007
Nonlinear parameter estimation technique for kinetic analysis of thermal desorption data Russell, N. M.; Ekerdt, J. G. Surface Science, Vol. 364, Issue 2 https://doi.org/10.1016/0039-6028(96)00593-6	journal	August 1996
Parametric sensitivity of complex temperature-programmed desorption, reaction and reduction Stuchlý, V. Journal of Thermal Analysis, Vol. 35, Issue 3 https://doi.org/10.1007/BF02057239	journal	May 1989
A new method for the analysis of heterogeneity using a modified temperature-programmed desorption technique Vásquez, Sergio O. J. Chem. Soc., Faraday Trans., Vol. 88, Issue 14 https://doi.org/10.1039/FT9928802051	journal	January 1992
Temperature programming for isothermal desorption rate measurements DeAngelis, Michael A.; Anton, A. Brad Journal of Vacuum Science & Technology A: Vacuum, Surfaces, and Films, Vol. 10, Issue 6 https://doi.org/10.1116/1.577810	journal	November 1992
Analysis of temperature programmed desorption (TPD) data for the characterisation of catalysts containing a distribution of adsorption sites Barrie, Patrick J. Physical Chemistry Chemical Physics, Vol. 10, Issue 12 https://doi.org/10.1039/b717430f	journal	January 2008
An iterative model-free method to determine the activation energy of heterogeneous processes under arbitrary temperature programs Budrugeac, P. Thermochimica Acta, Vol. 523, Issue 1-2 https://doi.org/10.1016/j.tca.2011.05.003	journal	August 2011
Approximate simulation of coupled fast and slow reactions for stochastic chemical kinetics Haseltine, Eric L.; Rawlings, James B. The Journal of Chemical Physics, Vol. 117, Issue 15 https://doi.org/10.1063/1.1505860	journal	October 2002
Partitioning ODE systems with an application to air pollution models Zlatev, Z. Computers & Mathematics with Applications, Vol. 42, Issue 6-7 https://doi.org/10.1016/S0898-1221(01)00201-2	journal	September 2001
Direct and adjoint sensitivity analysis of chemical kinetic systems with KPP: Part I—theory and software tools Sandu, Adrian; Daescu, Dacian N.; Carmichael, Gregory R. Atmospheric Environment, Vol. 37, Issue 36 https://doi.org/10.1016/j.atmosenv.2003.08.019	journal	November 2003
A predictor–corrector algorithm for the coupling of stiff ODEs to a particle population balance Celnik, Matthew; Patterson, Robert; Kraft, Markus Journal of Computational Physics, Vol. 228, Issue 8 https://doi.org/10.1016/j.jcp.2008.12.030	journal	May 2009
Implicit–explicit Runge–Kutta methods applied to atmospheric chemistry-transport modelling Wolke, Ralf; Knoth, Oswald Environmental Modelling & Software, Vol. 15, Issue 6-7 https://doi.org/10.1016/S1364-8152(00)00034-7	journal	September 2000
Explicit methods for stiff ODEs from atmospheric chemistry Verwer, J. G.; Simpson, D. Applied Numerical Mathematics, Vol. 18, Issue 1-3 https://doi.org/10.1016/0168-9274(95)00068-6	journal	September 1995
Benchmarking stiff ode solvers for atmospheric chemistry problems-I. implicit vs explicit Sandu, A.; Verwer, J. G.; Van Loon, M. Atmospheric Environment, Vol. 31, Issue 19 https://doi.org/10.1016/S1352-2310(97)00059-9	journal	October 1997
Benchmarking stiff ode solvers for atmospheric chemistry problems II: Rosenbrock solvers Sandu, A.; Verwer, J. G.; Blom, J. G. Atmospheric Environment, Vol. 31, Issue 20 https://doi.org/10.1016/S1352-2310(97)83212-8	journal	October 1997
Gauss–Seidel Iteration for Stiff ODES from Chemical Kinetics Verwer, J. G. SIAM Journal on Scientific Computing, Vol. 15, Issue 5 https://doi.org/10.1137/0915076	journal	September 1994
Efficient formulation of the stochastic simulation algorithm for chemically reacting systems Cao, Yang; Li, Hong; Petzold, Linda The Journal of Chemical Physics, Vol. 121, Issue 9 https://doi.org/10.1063/1.1778376	journal	September 2004
A constant-time kinetic Monte Carlo algorithm for simulation of large biochemical reaction networks Slepoy, Alexander; Thompson, Aidan P.; Plimpton, Steven J. The Journal of Chemical Physics, Vol. 128, Issue 20 https://doi.org/10.1063/1.2919546	journal	May 2008
Quasiequilibrium approximation of fast reaction kinetics in stochastic biochemical systems Goutsias, John The Journal of Chemical Physics, Vol. 122, Issue 18 https://doi.org/10.1063/1.1889434	journal	May 2005
Overcoming stiffness in stochastic simulation stemming from partial equilibrium: A multiscale Monte Carlo algorithm Samant, A.; Vlachos, D. G. The Journal of Chemical Physics, Vol. 123, Issue 14 https://doi.org/10.1063/1.2046628	journal	October 2005

Cited By (5)

Microkinetic simulation and fitting of the temperature programmed reaction of methanol on CeO2(111): H2 and H2O + V production Savara, Aditya Reaction Kinetics, Mechanisms and Catalysis, Vol. 129, Issue 1 https://doi.org/10.1007/s11144-019-01710-w	journal	January 2020
A Hybrid Kinetic Analysis of the Biosolids Pyrolysis using Thermogravimetric Analyser Patel, Savankumar R.; Kundu, Sazal K.; Halder, Pobitra K. ChemistrySelect, Vol. 3, Issue 47 https://doi.org/10.1002/slct.201802957	journal	December 2018
Theoretical Parameter-Free Analysis Model for Temperature-Programmed Desorption (TPD) Spectra Xu, Jian; Deng, Junyi ACS Omega, Vol. 5, Issue 8 https://doi.org/10.1021/acsomega.9b03867	journal	February 2020
Dynamic vs static behaviour of a supported nanoparticle with reaction-induced catalytic sites in a lattice model Korobov, Alexander Scientific Reports, Vol. 10, Issue 1 https://doi.org/10.1038/s41598-020-59739-0	journal	February 2020
TAPsolver: A Python package for the simulation and analysis of TAP reactor experiments Yonge, Adam; Kunz, M. Ross; Batchu, Rakesh arXiv https://doi.org/10.48550/arxiv.2008.13584	preprint	January 2020

Similar Records

LOCO with Constraints and Improved Fitting Technique

Journal Article · Thu Jun 18 00:00:00 EDT 2009 · ICFA Beam Dyn.Newslett.44:60-69,2007 · OSTI ID:1271860

Huang, Xiaobiao; Safranek, James; Portmann, Greg

Optimal choice of directions for the reconstruction of an object from a finite number of its plane integrals

Technical Report · Sat May 01 00:00:00 EDT 1982 · OSTI ID:1271860

Tam, A M

High–throughput measurement of plant fitness traits with an object detection method using Faster R–CNN

Journal Article · Fri Feb 25 00:00:00 EST 2022 · New Phytologist · OSTI ID:1271860

Wang, Peipei; Meng, Fanrui; Donaldson, Paityn; +8 more

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Temperature programmed desorption
Temperature programmed reaction
Microkinetics
Transient kinetics
Parameter optimization

Title: Simulation and fitting of complex reaction network TPR: The key is the objective function

Citation Formats

References (68)

Cited By (5)

Similar Records

Related Subjects