2026-04-17T06:57:08Zhttps://recercat.cat/oai/request

oai:recercat.cat:2072/4894152026-04-07T07:56:54Zcom_2072_300912com_2072_4427col_2072_301309

Toward Predictive Theory in Single-Atom Catalysis Ruiz-Ferrando, Andrea Mitchell, Sharon López, Núria Pérez-Ramírez, Javier Single-atom catalysis has become a central framework for experiment-theory integration, as catalytic performance is highly sensitive to the environment of individual metal atoms, a feature that electronic structure calculations are well-suited to analyze. Yet much of current theoretical practice relies on simplified single-site models and narrow reactivity windows, overlooking the intrinsic site diversity and evolution of single-atom catalysts (SAC). This Perspective discusses how SAC modeling can be reframed through a lifecycle-oriented view that integrates synthesis, activity, stability, and safety. By adopting ensemble-based descriptions and modular thermodynamic descriptors, we show how theory can be used systematically in line with the level of structural definition accessible experimentally. Using acetylene hydrochlorination as a prominent SAC application with exceptional data coherence for examining the theory-experiment interplay, wedemonstrate that site formation and evolution under synthesis and reaction conditions, as well as ensemble-driven activity trends consistent with experimental yields, can be treated quantitatively. In contrast, stability and safety are more effectively addressed through comparative, pathway-resolved analyses. More broadly, this perspective points toward a shift in how SAC modeling is framed across reactions, enabling theory to move beyond post-rationalization toward disciplined prediction. 2026-04-07T06:24:31Z 2026-04-07T06:24:31Z 2026-04-07T06:24:31Z 2026-04-03 info:eu-repo/semantics/article https://hdl.handle.net/2072/489415 https://doi.org/10.1002/advs.75156Digital Object Identifier (DOI) eng NCCR Catalysis (grant number 225147), a National Centre of Competence in Research funded by the Swiss National Science Foundation http://creativecommons.org/licenses/by/4.0/ info:eu-repo/semantics/openAccess Attribution 4.0 International Wiley RECERCAT (Dipòsit de la Recerca de Catalunya)