Interfacial chemical bond accelerating atomic-level charge transfer in step-scheme α-Fe₂O₃/PbBiO₂I for efficient...

Inadequate contact interface, lack of direct electron-transfer paths and low substrate affinity are considered as the main obstacle inhibiting the heterostructure activity for the sustainable photosynthesis of value-added fine chemicals. Herein, a novel 0D/2D Step-scheme (S-scheme) α-Fe₂O₃/PbBiO₂I (FO/PBOI) composite with abundant interface FeO bonds were initially synthesized via an in-situ growth approach. The created built-in field as a powerful driving force, efficiently steering the migration of photogenerated electrons. The interfacial FeO bonds act as atomic-level transfer highway, lowering charge transfer energy barrier between the interfaces and further accelerating the S-scheme spatial charge separation. Moreover, the FeO bonds bridged FO/PBOI can effectively enhance the activation of O₂ and benzylamine, significantly reducing the dehydrogenation barrier for the rate-limiting C₆H₅CH₂NH* intermediate. The optimized FO/PBOI exhibits remarkably improved catalytic activity and general applicability for the dehydrocoupling of primary amines to imines. This work offers an atomic-scale perspective on precise charge flow steering based on interface bond for advanced organic transformations.