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Authentic surface structures under reaction conditions determine the activity and selectivity of electrocatalysts, therefore, the knowledge of the structure-activity relationship can facilitate the design of efficient catalyst structures for specific reactivity requirements. However, understanding the relationship between a more realistic active surface and its performance is challenging due to the complicated interface microenvironment in electrocatalysis. Herein, we proposed a standard research paradigm to effectively decipher the structure-activity relationship in electrocatalysis, which is exemplified in the CO 2 electroreduction over SnO 2 . The proposed practice has aided in discovering authentic/resting surface states (Sn layer) of SnO 2 accountable for the electrochemical CO 2 reduction reaction (CO 2 RR) performance under electrocatalytic conditions, which then is corroborated in the subsequent CO 2 RR experiments over SnO 2 with different morphologies (nanorods, nanoparticles, and nanosheets) in combination with in situ characterizations. This proposed methodology is further extended to the SnO electrocatalysts, providing helpful insights into catalytic structures. It is believed that our proposed standard research paradigm is also applicable to other electrocatalytic systems, in the meantime, decreases the discrepancy between theory and experiments, and accelerates the design of catalyst structures that achieve sustainable performance for energy conversion., (© 2024 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.)

Data mining from computational materials database has become a popular strategy to identify unexplored catalysts. Herein, the opportunities and challenges of this strategy are analyzed by investigating a discrepancy between data mining and experiments in identifying low-cost metal oxide (MO) electrocatalysts. Based on a search engine capable of identifying stable MOs at the pH and potentials of interest, a series of MO electrocatalysts is identified as potential candidates for various reactions. Sb 2 WO 6 attracted the attention among the identified stable MOs in acid. Based on the aqueous stability diagram, Sb 2 WO 6 is stable under oxygen reduction reaction (ORR) in acidic media but rather unstable under high-pH ORR conditions. However, this contradicts to the subsequent experimental observation in alkaline ORR conditions. Based on the post-catalysis characterizations, surface state analysis, and an advanced pH-field coupled microkinetic modeling, it is found that the Sb 2 WO 6 surface will undergo electrochemical passivation under ORR potentials and form a stable and 4e-ORR active surface. The results presented here suggest that though data mining is promising for exploring electrocatalysts, a refined strategy needs to be further developed by considering the electrochemistry-induced surface stability and activity., (© 2023 The Authors. Advanced Science published by Wiley-VCH GmbH.)