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Title: First-principles prediction of absolute catalytic turnover frequencies
Plain: Computer models can rank catalysts by trends, but they rarely predict the actual speed of a catalytic reaction. Small errors in computed energies change the predicted speed enormously.
Precise: For benchmark heterogeneous reactions (NH3 synthesis on Ru(0001) step sites, CO oxidation on Pt(111), methanol synthesis on Cu/ZnO), predict the absolute turnover frequency under specified temperature and pressure within a factor of 10 from first-principles energetics and kinetic modeling with no fitted parameters. An answer is a protocol (electronic structure accuracy, treatment of coverage, entropy and site heterogeneity) meeting this target on several reactions.
Settled by: Blind comparison of computed turnover frequencies with measurements on well-characterized single-crystal or model catalysts.
Kind: well-posed
Answer type: value
References: (empty)
Literature status: open
Status note: A 2005 first-principles microkinetic model of NH3 synthesis on Ru nanoparticles (Honkala et al., Science, https://doi.org/10.1126/science.1106435) matched measured rates to within about an order of magnitude, possibly helped by error cancellation; agreement across several reactions with controlled electronic-structure error is not established.
Posed since: (empty)