{"schema":"pubphys.bundle/1","record":{"author":{"account_ref":null,"orcid":null},"builds_on":[],"content_schema":"pubphys.content.revision/1","content_sha256":"4e288f5b9828bf18fcb9bc50460554cd510f98bac98ce133bf433235f92e2129","created":"2026-10-15T23:43:22Z","files":[],"origin":{"assisted_by":[],"kind":"seed"},"parents":["823548a79d6fbf17b8c491181914419b7226b2d60d9c24250c7feab31f909c99","ce59fb6cd812fc05906d0c60a71c75ea22bc686bcf38e7c3ef7010834d98ee7b"],"salt":"8a80e69c242a554674337d328033e4bec9d060795972d73def76ad8fc2a5347e","schema":"pubphys.record/2","site":"pubphys.com","target":null,"type":"revision"},"content":{"answer_type":"value","assisted_by":[],"external_id":"chem.catalytic-mechanisms.ab-initio-turnover","kind":"well-posed","literature_status":"open","n":"2","parents":[],"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.","posed_since":"","precise":"For benchmark heterogeneous reactions ($\\mathrm{NH_3}$ 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.","problem_ref":"823548a79d6fbf17b8c491181914419b7226b2d60d9c24250c7feab31f909c99","references":"","settled_by":"Blind comparison of computed turnover frequencies with measurements on well-characterized single-crystal or model catalysts.","status_note":"A 2005 first-principles microkinetic model of $\\mathrm{NH_3}$ 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.","title":"First-principles prediction of absolute catalytic turnover 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