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Bimetallic sulfides are expected to realize efficient CO2 electroreduction into formate over a wide potential window, however, they will undergo in situ structural evolution under the reaction conditions. Therefore, clarifying the structural evolution process, the real active site and the catalytic mechanism is significant. Here, taking Cu2SnS3 as an example, we unveiled that Cu2SnS3 occurred self‐adapted phase separation toward forming the stable SnO2@CuS and SnO2@Cu2O heterojunction during the electrochemical process. Calculations illustrated that the strongly coupled interfaces as real active sites driven the electron self‐flow from Sn4+ to Cu+, thereby promoting the delocalized Sn sites to combine HCOO* with H*. Cu2SnS3 nanosheets achieve over 83.4 % formate selectivity in a wide potential range from −0.6 V to −1.1 V. Our findings provide insight into the structural evolution process and performance‐enhanced origin of ternary sulfides under the CO2 electroreduction. [ABSTRACT FROM AUTHOR]

As a way to drive chemical reactions by renewable solar energy, photocatalytic technology is an appealing strategy for carbon recycle and value‐added CO2 utilization mimicking the natural photosynthetic system to remedy energy and environmental problems. During the recent decades of exploration, extensive research has been reported on 2D nanomaterials in photocatalytic CO2 reduction because of their unique structural properties. This review highlights the ongoing development of modification strategies for 2D nanomaterials from the viewpoints of defect engineering, surface modification, and hybrid construction, following the sequence of inside‐to‐outside design of the photocatalysts. These methodologies can expand the scope of light absorption, promote the separation of photogenerated charge carriers, and enhance the adsorption and activation of CO2, thus effectively improve the photocatalytic efficiency. The future challenges and opportunities for developing modified 2D photocatalysts are also discussed. It is hoped that this review can provide useful guidelines toward further research on 2D nanocatalysis for CO2 photocatalytic conversion. [ABSTRACT FROM AUTHOR]