Electroreduction of carbon dioxide (CO2) into high‐value and readily collectable liquid products is vital but remains a substantial challenge due to the lack of highly efficient and robust electrocatalysts. Herein, Bi‐based metal‐organic framework (CAU‐17) derived leafy bismuth nanosheets with a hybrid Bi/BiO interface (Bi NSs) is developed, which enables CO2 reduction to formic acid (HCOOH) with high activity, selectivity, and stability. Specially, the flow cell configuration is employed to eliminate the diffusion effect of CO2 molecules and simultaneously achieve considerable current density (200 mA cm−2) for industrial application. The faradaic efficiency for transforming CO2 to HCOOH can achieve over 85 or 90% in 1 m KHCO3 or KOH for at least 10 h despite a current density that exceeds 200 mA cm−2, outperforming most of the reported CO2 electroreduction catalysts. The hybrid Bi/BiO surface of leafy bismuth nanosheets boosts the adsorption of CO2 and protects the surface structure of the as‐prepared leafy bismuth nanosheets, which benefits its activity and stability for CO2 electroreduction. This work shows that modifying electrocatalysts by surface oxygen groups is a promising pathway to regulate the activity and stability for selective CO2 reduction to HCOOH.

The electroreduction of carbon dioxide is a promising strategy to synthesize value‐added feedstocks and realize carbon neutralization. Copper catalysts are well‐known to be active for selective electroreduction of CO2 to multicarbon products, although the role played by the surface architecture is not fully understood. Herein, mesoporous Cu nanoribbons are constructed via in‐situ electrochemical reduction of Cu based metal organic frameworks for the highly selective synthesis of C2+ chemicals. With the mesoporous structure, a high C2+ Faradaic efficiency of 82.3% with a partial current density of 347.9 mA cm−2 is achieved in a flow‐cell electrolyzer. Controlled electroreduction of CO2 with Cu nanoribbons exhibited clearly greater selectivity towards C2+ products than Cu nanoleaves and Cu nanorods without porous structures. Finite difference time domain results indicate that the mesoporous structure can enhance the electric field on the catalyst surface, which increases the concentration of K+ and OH−, thus allowing the authors to promote CO2 reduction pathways towards C2+ products.

Bimetallic MIL-101(Al/Fe)–NH2 exhibits enhanced acid–base bifunctional catalytic activity due to its synergistic mechanism and hierarchical pore system.

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