Deciphering Structure‐Activity Relationship Towards CO₂ Electroreduction over SnO₂ by A Standard Research Paradigm

Abstract

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 CO2 electroreduction over SnO2. The proposed practice has aided in discovering authentic/resting surface states (Sn layer) of SnO2 accountable for the electrochemical CO2 reduction reaction (CO2RR) performance under electrocatalytic conditions, which then is corroborated in the subsequent CO2RR experiments over SnO2 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.

Reversible Hydrogen Electrode (RHE) Scale Dependent Surface Pourbaix Diagram at Different pH

“…Li et al found that the formation of the metallic surface with abundant oxygen vacancies over the Cu oxide catalysts is the key to the high C–C coupling performance in CO 2 reduction reaction (CO 2 RR). Recently, a similar conclusion was found by Guo et al on SnO x for CO 2 RR, by combining surface Pourbaix analysis and subsequent structural evolution and activity analysis. Yang et al − identified the dual-atom catalysts’ bridge-site poisoning effect of CO* during the CO 2 RR and HO*/O* during the ORR and oxygen evolution reaction.…”