Journal
JOURNAL OF CATALYSIS
Volume 338, Issue -, Pages 273-283Publisher
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcat.2016.03.013
Keywords
Ethanol; Hydrodeoxygenation; Density functional theory; Microkinetic modeling; Uncertainty quantification; Sensitivity analysis; Linear scaling relations; Bronsted-Evans-Polanyi correlations
Categories
Funding
- Catalysis Center for Energy Innovation (CCEI), an Energy Frontier Research Center - U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC0001004]
- U.S.Department of Energy Office of Science, Office of Advanced Scientific Computing Research, and Applied Mathematics program [DE-SC0010549]
- U.S. Department of Energy, Office of Basic Energy Sciences [DE-AC02-98CH10886]
- U.S. Department of Energy (DOE) [DE-SC0010549] Funding Source: U.S. Department of Energy (DOE)
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We introduce for the first time uncertainty quantification and global sensitivity analysis to assess the effect of error in linear scaling relations (LSRs) and Bronsted-Evans-Polanyi (BEP) relations on activity and selectivity maps of microkinetic models, which have recently been used for in silico prediction of new materials. The method is applied to ethanol hydrodeoxygenation (HDO). Selectivity trends are driven by adsorbate thermochemistry rather than kinetics. Uncertainty quantification calculations show that the most likely location of the maximum conversion can be estimated to be within about 10 kcal/mol in the C and 0 binding energies. Broad selectivity trends are even more robust. Model rates show uncertainties of 2-3 orders of magnitude about the median. Uncertainty in the activity predictions is dominated by that of the LSRs. Our calculations demonstrate that there is a common initial mechanism of ethanol HDO and decomposition, and the stability of decomposition products is crucial to determining the selectivity. (C) 2016 Elsevier Inc. All rights reserved.
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