Dissecting the Performance of Nanoporous Gold Catalysts for Oxygen-Assisted Coupling of Methanol with Fundamental Mechanistic and Kinetic Information [electronic resource]
The utility of the surface reactivity observed for model systems under ultrahigh vacuum for predicting the performance of catalytic materials under ambient flow conditions is a highly debated topic in heterogeneous catalysis. Herein we show that vast differences in selectivity observed for methanol...
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| Format: | Electronic eBook |
| Language: | English |
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Washington, D.C. : Oak Ridge, Tenn. :
United States. Department of Energy. Office of Basic Energy. Energy Frontier Research Centers (EFRC) ; Distributed by the Office of Scientific and Technical Information, U.S. Department of Energy,
2019.
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| Subjects: |
MARC
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| 245 | 0 | 0 | |a Dissecting the Performance of Nanoporous Gold Catalysts for Oxygen-Assisted Coupling of Methanol with Fundamental Mechanistic and Kinetic Information |h [electronic resource] |
| 260 | |a Washington, D.C. : |b United States. Department of Energy. Office of Basic Energy. Energy Frontier Research Centers (EFRC) ; |a Oak Ridge, Tenn. : |b Distributed by the Office of Scientific and Technical Information, U.S. Department of Energy, |c 2019. | ||
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| 500 | |a 04/09/2019. | ||
| 500 | |a "Journal ID: ISSN 2155-5435" | ||
| 500 | |a Reece, Christian ; Luneau, Mathilde ; Madix, Robert J. ; | ||
| 500 | |a USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22) | ||
| 520 | 3 | |a The utility of the surface reactivity observed for model systems under ultrahigh vacuum for predicting the performance of catalytic materials under ambient flow conditions is a highly debated topic in heterogeneous catalysis. Herein we show that vast differences in selectivity observed for methanol self-coupling across wide ranges of temperature and reactant pressure can be accurately predicted utilizing the kinetics and mechanism obtained from model studies on gold single crystals in ultrahigh vacuum regressed to fit transient pulse responses over nanoporous gold (Ag<sub>0.03</sub>Au<sub>0.97</sub>) at low pressures. Specifically, microkinetic modeling of the complex sequence of elementary steps governing this reaction predicts the dramatic effect of reactant partial pressure on the product distribution and leads to conclusion that the gas phase partial pressures of both reactants and the reaction temperature determine the changes in selectivity to methyl formate formation. Moreover, thorough analysis of the reaction network indicates that the product distribution becomes increasingly insensitive to kinetic effects at pressures approaching 1 bar, leading toward 100% selectivity methyl formate. A rigorous kinetic sensitivity analysis also demonstrates the complex interplay of the kinetics of the elementary steps and the overall catalytic behavior. | |
| 536 | |b SC0012573. | ||
| 650 | 7 | |a 37 inorganic, organic, physical, and analytical chemistry |2 local. | |
| 650 | 7 | |a Catalysis (heterogeneous) |2 local. | |
| 650 | 7 | |a Mesostructured materials |2 local. | |
| 650 | 7 | |a Materials and chemistry by design |2 local. | |
| 650 | 7 | |a Synthesis (novel materials) |2 local. | |
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