In-situ reconstructed In doped SnO2 amorphous–crystalline heterostructure for highly efficient CO2 electroreduction with a dynamic structure-function relationship.

While amorphous metal oxides exhibit potential advantages in terms of energy conversion and storage, they undergo unavoidable and uncontrollable reconstruction during electrocatalysis. Monitoring the probable reconstruction of catalytic materials during operation is crucial for identifying the practical active sites. In this study, the amorphous In-doped SnO x (a-In-SnO x) was selected for the in-situ reconstruction of highly active structures. In/ex-situ electron microscopy revealed that the intricate reconstruction of a-In-SnO x could be divided into three states: initial, activated, and deactivated. The a-In-SnO x reconstructed amorphous–crystalline In-doped SnO 2 heterostructure for highly efficient CO 2 electroreduction. Benefiting from the heterostructure, the amorphous-crystalline In-doped SnO 2 (a/c-In-SnO 2) exhibited potential CO 2 RR performance with a maximum Faraday efficiency of 94.6% at −1.0 V (vs. RHE) and a current density of 209 mA cm–2 at −1.4 V (vs. RHE). This work represents significant advancements in design of active amorphous–crystalline heterostructures during the reconstruction process and establishes a dynamic evolution mechanism. [Display omitted] • An amorphous engineering strategy was explored for developing advanced electrocatalysts for CO 2 RR. • A universal regulation for the reconstruction process of amorphous materials during CO 2 RR was summarized. • A dynamic structure-function relationship was established on the amorphous In-SnO x with three states. • The in-situ formed amorphous–crystalline In-SnO 2 heterostructure was demonstrated to be highly active for CO 2 RR. [ABSTRACT FROM AUTHOR]