Bioinspired Bi2MoO6 Electron Bridge and Carbon Nano‐Island Heterojunctions for Enhanced Photothermal Catalytic CO2 Reduction

ABSTRACT Photothermal catalysis utilizing the full solar spectrum to convert CO 2 and H 2 O into valuable products holds promise for sustainable energy solutions. However, a major challenge remains in enhancing the photothermal conversion efficiency and carrier mobility of semiconductors like Bi 2 MoO 6 , which restricts their catalytic performance. Here, we developed a facile strategy to synthesize vertically grown Bi 2 MoO 6 (BMO) nanosheets that mimic a bionic butterfly wing scale structure on a biomass‐derived carbon framework (BCF). BCF/BMO exhibits high catalytic activity, achieving a CO yield of 165 μmol/(g·h), which is an increase of eight times compared to pristine BMO. The wing scale structured BCF/BMO minimizes sunlight reflection and increases the photothermal conversion temperature. BCF consists of crystalline carbon (sp 2 ‐C region) dispersed within amorphous carbon (sp 3 ‐C hybridized regions), where the crystalline carbon forms “nano‐islands”. The N–C–O–Bi covalent bonds at the S‐scheme heterojunction interface of BCF/BMO function as electron bridges, connecting the sp 2 ‐C nano‐islands and enhancing the multilevel built‐in electric field and directional trans‐interface transport of carriers. As evidenced by DFT calculation, the rich pyridinic‐N on the carbon nano‐island can establish strong electron coupling with CO 2 , thereby accelerating the cleavage of *COOH and facilitating the formation of CO. Biomass waste‐derived carbon nano‐islands represent advanced amorphous/crystalline phase materials and offer a simple and low‐cost strategy to facilitate carrier migration. This study provides deep insights into carrier migration in photocatalysis and offers guidance for designing efficient heterojunctions inspired by biological systems.