An end-to-end framework for reactivity in heterogeneous catalysis

The rationalization of catalytic processes relies on the fundamental understanding of competing reaction mechanisms driving reactants to products. The list of elementary steps composing the reaction networks is proposed based on chemical intuition and evaluated via density functional theory. This ap...

Descripción completa

Detalles Bibliográficos
Autores: Morandi, Santiago, Loveday, Oliver, Renningholtz, Tim, Pablo-García, Sergio, Vargas-Hernández, Rodrigo A., Seemakurthi, Ranga Rohit, Sanz Berman, Pol, García-Muelas, Rodrigo, Aspuru-Guzik, Alán, López, Núria
Tipo de recurso: artículo
Fecha de publicación:2026
País:España
Institución:Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)
Repositorio:Recercat. Dipósit de la Recerca de Catalunya
OAI Identifier:oai:recercat.cat:2072/489363
Acceso en línea:https://hdl.handle.net/2072/489363
https://doi.org/10.1038/s44286-026-00361-8
Access Level:acceso abierto
Palabra clave:Química
54
Descripción
Sumario:The rationalization of catalytic processes relies on the fundamental understanding of competing reaction mechanisms driving reactants to products. The list of elementary steps composing the reaction networks is proposed based on chemical intuition and evaluated via density functional theory. This approach is limited by the size of the network and disregards alternative paths. Here we present the Catalytic Automated Reaction Evaluator (CARE), a flexible end-to-end framework for heterogeneous catalysis composed of (1) a rule-based reaction network generator, (2) a thermodynamic and kinetic parameter evaluator powered by state-of-the-art machine learning models and (3) a fast microkinetic solver. CARE reproduces the experimental activity trends in methanol decomposition, identifies the selectivity to C3 products in CO2 electroreduction and generates the Fischer–Tropsch synthesis mechanism including 370,000 reactions reaching C6 products. This comprehensive framework enables the exploration of thermal and electrocatalytic reactions previously not amenable to atomistic simulations.