Higher alcohol synthesis is a highly desirable reaction for a sustainable fuel production, but no process has been commercialized yet. The main problem is the lack of a selective and active catalyst. In quest for better catalysts we performed extensive DFT calculations on transition metal (111) surfaces to investigate intermediates and transition states of syngas conversion reactions. The results were used to build a micro-kinetic model, including CH4, CH3OH, CH3CHO and CH3CH2OH as products for CO hydrogenation. We show which requirements a good catalyst needs to meet to be selective for higher oxygenate formation. On terrace sites C-O bond splitting is decreased and thus alkane formation can be suppressed. This leads to an increase in selectivity towards molecules where the C-O bond is preserved. Making use of the BEEF ensemble an uncertainty estimation results in probabilistic predictions for activity and selectivity. This insight can be used to rationalize catalyst design.

Selective catalysts for higher alcohol synthesis: A combined DFT and micro-kinetic modeling study

255th National Meeting (2018)

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