A Full-Spectrum Porphyrin-Fullerene D-A Supramolecular Photocatalyst with Giant Built-In Electric Field for Efficient Hydrogen Production

摘要

A full-spectrum (300-850 nm) responsive donor-acceptor (D-A) supramolecular photocatalyst tetraphenylporphinesulfonate/fullerene (TPPS/C-60) is successfully constructed. The theoretical spectral efficiency of TPPS/C-60 is as high as 70%, offering the possibility of full-solar-spectrum light harvesting. The TPPS/C-60 performs a highly efficient photocatalytic H-2 evolution rate of 276.55 mu mol h(-1) (34.57 mmol g(-1) h(-1)), surpassing many reported organic photocatalysts. The D-A structure effectively promotes electron transfer from TPPS to C-60, which is beneficial to the photocatalytic reaction. Specifically, a giant internal electric field in the D-A structure is built via the enhanced molecular dipole, which dramatically promotes the charge separation (CS) efficiency by 2.35 times. Transient absorption spectra results show a long-lived CS state TPPS center dot+-C-60(center dot-) in the D-A structure, which effectively promotes participation of photogenerated electrons in the reduction reaction. Briefly, this work provides a novel approach for designing high-performance photocatalytic materials via enhancing the interfacial electric field.