Visible and even infrared(IR)light-initiated hot electrons of graphene(Gr)catalysts are a promising driven power for green,safe,and sustainable H2O2 synthesis and organic synthesis without the limitation of bandgap-do...Visible and even infrared(IR)light-initiated hot electrons of graphene(Gr)catalysts are a promising driven power for green,safe,and sustainable H2O2 synthesis and organic synthesis without the limitation of bandgap-dominated narrow light absorption to visible light confronted by conventional photocatalyst.However,the life time of photogenerated hot electrons is too short to be efficiently used for various photocatalytic reactions.Here,we proposed a straightforward method to prolong the lifetime of photogenerated hot electrons from graphene by tuning the Schottky barrier at Gr/rutile interface to facilitate the hot electron injection.The rational design of Gr-coated TiO2 heterojunctions with interface synergy-induced decrease in the formation energy of the rutile phase makes the phase transfer of TiO2 support proceed smoothly and rapidly via ball milling.The optimized Gr/rutile dyad could provide a H2O2 yield of 1.05 mM·g-1·h-1 under visible light irradiation(λ≥400 nm),which is 30 times of the state-of-the-art noble-metal-free titanium oxide-based photocatalyst,and even achieves a H2O2 yield of 0.39 mM·g-1·h-1 on photoexcitation by near-infrared-region light(~800 nm).展开更多
基金supported by the National Natural Science Foundation of China(Nos.21737002,21931005,21720102002,and 22071146)Shanghai Science and Technology Committee(Nos.19JC1412600 and 20520711600)the SJTU-MPI partner group.
文摘Visible and even infrared(IR)light-initiated hot electrons of graphene(Gr)catalysts are a promising driven power for green,safe,and sustainable H2O2 synthesis and organic synthesis without the limitation of bandgap-dominated narrow light absorption to visible light confronted by conventional photocatalyst.However,the life time of photogenerated hot electrons is too short to be efficiently used for various photocatalytic reactions.Here,we proposed a straightforward method to prolong the lifetime of photogenerated hot electrons from graphene by tuning the Schottky barrier at Gr/rutile interface to facilitate the hot electron injection.The rational design of Gr-coated TiO2 heterojunctions with interface synergy-induced decrease in the formation energy of the rutile phase makes the phase transfer of TiO2 support proceed smoothly and rapidly via ball milling.The optimized Gr/rutile dyad could provide a H2O2 yield of 1.05 mM·g-1·h-1 under visible light irradiation(λ≥400 nm),which is 30 times of the state-of-the-art noble-metal-free titanium oxide-based photocatalyst,and even achieves a H2O2 yield of 0.39 mM·g-1·h-1 on photoexcitation by near-infrared-region light(~800 nm).
