Interfacial chemical bond accelerating atomic-level charge transfer in step-scheme α-Fe2O3/PbBiO2I for efficient photoconversion of amines to imines

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-Fe 2 O 3 /PbBiO 2 I (FO/PBOI) composite with abundant interface Fe O 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 Fe O 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 Fe O bonds bridged FO/PBOI can effectively enhance the activation of O 2 and benzylamine, significantly reducing the dehydrogenation barrier for the rate-limiting C 6 H 5 CH 2 NH* 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.