摘要
Lead halide perovskite quantum dots(LHP QDs)have been revealed to possess great potential in photocatalytic applications including CO_(2)reduction;which however suffer from poor stability.Herein;a high crystalline hydrazine-linked three-dimensional(3D)covalent organic framework;USTB-17;was fabricated from the reaction between 12-connected building block and 4-connected 3;5;7-tetrakis(4-aldophenyl)-adamantane.Post-modification with Ni2+affords the metallic framework USTB-17(Ni)followed by sequential deposition of the CH_(3)NH_(2)PbI3(MAPbI3)perovskite QDs into its pores;generating the USTB-17(Ni)@MAPbI3 composite.Powder X-ray diffraction analysis together with theoretical simulations and transmission electron microscopy discloses the crystalline nature of USTB-17;USTB-17(Ni);and USTB-17(Ni)@MAPbI3 with an unprecedented noninterpenetrated hpt topology.The close contact of QDs inside the COF pores with the Ni catalytic site locating at the pore surface of COF allows a rapid transfer of the photogenerated electrons in QDs to the Ni catalytic sites;enhancing the photocatalytic activity for CO_(2)reduction.This endows USTB-17(Ni)@MAPbI3 with efficient photocatalysis performance for photocatalytic CO_(2)reduction with CO generation rate of 365μmol g^(-1)h^(-1)and CO selectivity up to 96%under visible-light irradiation;7 times higher than that of USTB-17(Ni).After four cycles of reactions;the photocatalytic CO generation rate remains almost unchanged;demonstrating its excellent cycle stability.
基金
supported by the National Natural Science Foundation of China(22235001,22175020)
the Fundamental Research Funds for the Central Universities,and University of Science and Technology Beijing.
