Polyacid-based organic-inorganic complex, preparation method thereof, and application of the polyacid-based organic-inorganic complex as photocatalyst in selective oxidation of toluene into benzaldehyde

A technology of complexes and organic ligands, which is applied in the field of polyacid-based organic-inorganic complexes, can solve problems that hinder the application of photocatalysts, and achieve high selectivity, high selectivity, and high stability.

CN111644205AActive Publication Date: 2020-09-11HENAN UNIVERSITY
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Patent Information

Authority / Receiving Office
CN · China
Patent Type
Applications(China)
Current Assignee / Owner
Publication Date
2020-09-11

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Abstract

The invention discloses a polyacid-based organic-inorganic complex. The chemical formula of the polyacid-based organic-inorganic complex is K4(H2O)8H26(C26H16N4O4)8[P6W48Fe6O180].7H2O. The complex generates photo-induced electrons and holes under the illumination condition, the holes promote formation of benzyl free radicals, the electrons reduce oxygen into superoxide free radicals to promote formation of benzaldehyde, and efficient selectivity of catalytic reaction is achieved. The catalytic process is heterogeneous, the catalyst can be recovered through centrifugal drying, cyclic utilization is realized, the catalytic efficiency is not obviously reduced, and the reaction still keeps very high selectivity. The polyacid-based organic-inorganic complex material provides a scientific basisfor the development of fine chemical engineering in China in the aspect of carbon-hydrogen bond activation.
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Description

Technical field

[0001] The present invention belongs to the technical field of preparation of polyoxometalate chemical materials, and specifically relates to a polyacid-based organic-inorganic complex (which is an example [P 6 W 48 Fe 6 O 180 ] 30- Anionic photocatalyst) and its preparation method and its application as a photocatalyst in the selective oxidation of toluene to benzaldehyde. Background technique

[0002] The selective oxidation of primary carbon-hydrogen bonds under mild conditions is a major challenge facing academia and industry. This is because the saturated C-H bond is inert and has strong thermodynamic stability. The reaction environment usually requires high temperature, high pressure and additional co-oxidants. As we all know, benzyl alcohol, benzaldehyde and benzoic acid as intermediates have important commercial value in the production of preservatives, perfumes, dyes, drugs, solvents, plasticizers and flame retardants. Among these products, benzaldehyde...

Examples

Embodiment 1

[0032] Multi-acid base organic-inorganic complex, its chemical formula is: K 4 (H 2 O) 8 H 26 (C 26 H 16 N 4 O 4 ) 8 [P 6 W 48 Fe 6 O 180 ]·7H 2 O.

[0033] The preparation method of the above-mentioned polyacid-based organic-inorganic complex, which combines DPNDI, ferrous sulfate heptahydrate and K 12 [α-H 2 P 2 W 12 O 48 ]·24H 2 O is carried out under hydrothermal conditions and specifically includes the following steps:

[0034] 1) Prepare reaction material DPNDI, specifically refer to the literature (Inorg. Chem., 2009, 48(18): 8659−8661.) method for synthesis;

[0035] 2) Dawson type polyacid K 12 [α-H 2 P 2 W 12 O 48 ]·24H 2 O prepared by the method of reference (Inorg. Synth. 27 (1990) 104-111.);

[0036] 3) Put K 12 [α-H 2 P 2 W 12 O 48 ]·24H 2 O (86.0 mg, 0.02 mmol), DPNDI (13.6 mg, 0.03 mmol) and FeSO 4 ·7H 2 O (29.2 mg, 0.10 mmol) and solvent (the solvent consists of 4 mL of distilled water and 2 mL of acetonitrile) are mixed and stirred for 12 h to disperse uniformly to ob...