Enol-ketone covalent organic framework/amino-functionalized zirconium-based metal organic framework composite photocatalyst as well as preparation method and application thereof

Abstract

The invention discloses an enol-ketone covalent organic framework / amino-functionalized zirconium-based metal organic framework composite photocatalyst as well as a preparation method and an application thereof. The composite photocatalyst comprises an enol-ketone covalent organic framework and an amino-functionalized zirconium-based metal organic framework growing on the surface of the enol-ketone covalent organic framework in situ. The preparation method comprises the following steps: mixing 2-aminoterephthalic acid, an enol-ketone covalent organic framework and zirconium tetrachloride, and carrying out a hydrothermal reaction. The composite photocatalyst has the advantages of high specific surface area, multiple reaction active sites, wide light absorption range, low electron-hole pair recombination rate, good photocatalytic performance, good stability and the like, is a novel photocatalyst with stable structure and excellent catalytic performance, can effectively degrade organic pollutants, and is high in use value and good in application prospect; and the preparation method has the advantages of being simple in process, convenient to operate, wide in raw material source, low in cost, high in preparation efficiency, high in yield and the like, is suitable for large-scale preparation and facilitates industrial production.

Description

technical field [0001] The invention belongs to the technical field of material preparation and environmental catalysis, and relates to a metal-organic framework composite photocatalyst and its preparation method and application, in particular to an enol-ketone covalent organic framework / amino-functionalized zirconium-based metal-organic framework Composite photocatalyst and its preparation method and application. Background technique [0002] As environmental problems become more and more severe, as the main source of environmental pollution, water pollution from industrial organic chemicals and agricultural fertilizers has become an urgent problem to be solved. Persistent organic micropollutants, such as pharmaceuticals and personal care products, pesticides and herbicides, have been observed in natural and wastewater, however, new pollutants are difficult to treat with traditional wastewater treatment technologies. Photocatalytic technology is a technology that uses phot...

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Problems solved by technology

However, the constructed amino-functionalized UIO-66-based semiconductor heterojunction still has the following problems: simple mechanical mixing is not conducive to the formation of a structurally stable heterojunction, and at the same time, the light absorption performance is insufficient, photogenerated carriers are easy to recombine, electron-space The problems of high hole-pair recombination rate and insufficient catalytic degradation performance have not been well resolved, which severely limits the wide application of amino-functionalized zirconium-based metal-organic framework composite photocatalysts.

In addition, in the actual research process of the inventors of the present application, it is also found that in the existing covalent organic framework materials, the monomer molecules are mainly connected through the Schiff base imine group (-C=N-). The connection of the amine group (-C=N-) is reversible, which makes the covalent organic framework material have the defect of poor structural stability; in addition, in the existing method for preparing the covalent organic framework material by the solvothermal method, in When heating the solution system, the heating method used is difficult to effectively realize the simultaneous heating inside and outside the solution system. As a result, because the polycondensation reaction process is reversible, it is difficult for ordinary heating methods to maintain the reaction dynamic balance of the system, and it is difficult to ensure that the product has Good structural stability. At the same time, in order to promote the bond-forming interaction of precursors, longer reaction time and more heat energy are required, which is not conducive to large-scale preparation, and it is difficult to meet the requirements of energy saving in industrial production.

So far, there has been no report on the preparation of covalent organic framework materials by microwave-assisted heating

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