2026-04-19T11:15:23Zhttps://recercat.cat/oai/request

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

00925njm 22002777a 4500 dc Ruiz-Ferrando, Andrea author Mitchell, Sharon author López, Núria author Pérez-Ramírez, Javier author 2026-04-03 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. https://hdl.handle.net/2072/489415 https://doi.org/10.1002/advs.75156Digital Object Identifier (DOI) Toward Predictive Theory in Single-Atom Catalysis