Abstract
Though there are numerous intrinsic merits of metal-organic frameworks(MOFs),low charge separation efficiency has imposed heavy restrictions on their photo-catalytic application.Herein,in situ porphyrin ligand sub-stitution,as a strategy for improving the charge separation efficiency and increasing the amounts of active sites,has been designed and realized in a Hf-biphenyl dicarboxylic acid(BPDC)MOF.Specifically,a size and geometry matched meso-tetra(4-carboxyphenyl)porphyrin(TCPP)ligand was selected and doped into Hf-BPDC MOF by forming coordinating bonds with Hf centers,forming dual-ligand Hf-BPDC-TCPP MOF.The resultant Hf-BPDC-TCPP MOF showed significantly improved activity and chemical stability in the photocatalytic H2 generation(261 μmol·g-1·h-1)and tetracycline(TC)degradation reactions(95.8％),which was 48 and 1.47 folds higher than that of the Hf-BPDC MOF.Photophysical and electro-chemical studies revealed that the introduction of por-phyrin ligand could generate a stronger internal electric field for boosting the charge separation and transfer,increase the specific surface area for providing more active sites,and narrow the band gap to enhance the visible light absorption.This in situ ligand substitution method provides a promising approach to build a tunable platform for con-structing high-performance MOF photocatalysts.
基金项目
国家自然科学基金(22102064)
国家自然科学基金(21972058)
Open Project Program of Fujian Provincial Key Laboratory of Ecology-Toxicological Effects and Control for Emerging Contamina()
NETL
NSTL
万方数据