Microkinetic modeling of n-butane hydrogenolysis on Ru(0001)
Date
2024
Authors
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Publisher
University of Delaware
Abstract
Plastic waste is an untapped opportunity to reintroduce valuable resources into the value chain. Hydrogenolysis is a promising technology that achieves this while operating at milder temperatures than similar technologies. A multiscale kinetic model of n-butane hydrogenolysis on Ru is created from first-principles calculations in combination with group additivity and Brønsted-Evans-Polanyi relationships (BEP) relationships. Reaction path analysis and local sensitivity analysis are performed to determine the kinetically dominant and relevant pathways. The results of the model align well with experimental data. The most kinetically relevant step, a C-C cracking of a α, γ-bound, dehydrogenated intermediate, for n-butane appears to be unchanged by hydrogen pressure. The intermediate CH3CH2CHCH2 dictates which kinetic pathway is taken as a majority of the flux passes through this intermediate for all H2 pressures. Therefore, it could serve as a control on the selectivity. This work provides a stepping stone for building larger hydrogenolysis models from first-principles.
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Keywords
Catalysis, Hydrogenolysis, Microkinetic modeling, Multiscale modeling, Kinetic pathway