Magnetic Fe2O3 nanospheres with PNH surface modification and application hereof in water treatment

Patent metadata

Field	Value
Publication number	US-11325110-B2
Application number	US-202016907080-A
Country	US
Kind code	B2
Filing date	Jun 19, 2020
Priority date	Jun 20, 2019
Publication date	May 10, 2022
Grant date	May 10, 2022

Abstract

The present invention provides a magnetic Fe2O3 nanosphere with PNH surface modification and application thereof in water treatment. First, 2,2-bipyridyl-5,5′-dicarboxylic acid is reacted with thionyl chloride to obtain 2,2-bipyridyl-5,5′-diacid chloride; then 2,2-bipyridyl-5,5′-diacid chloride and 1,4,8,11-tetraazacyclotetradecane react in the presence of triethylamine to obtain a polynitrogen heterocyclic polymer; the polynitrogen heterocyclic polymer is added into an aqueous solution with iron salt to obtain a magnetic Fe2O3 nanosphere with PNH surface modification which has strong light absorption ability, which improves its ability to catalyze in degradation of tetracycline under visible light, so that the pollutants are removed from water.

First claim

What is claimed is:

1. A method for preparing a magnetic Fe 2 O 3 nanosphere with PNH (polynitrogen heterocyclic polymer) surface modification, comprising the following steps:
(1) reacting 2,2-bipyridyl-5,5′-dicarboxylic acid with thionyl chloride to obtain 2,2-bipyridyl-5,5′-diacid chloride; then, in the presence of triethylamine, reacting 2,2-bipyridyl-5,5′-diacid chloride with 1,4,8,11-tetraazacyclotetradecane to obtain a polynitrogen heterocyclic polymer;
(2) adding the polynitrogen heterocyclic polymer to an aqueous solution of iron salt to obtain the magnetic Fe 2 O 3 nanosphere with PNH surface modification.

2. The method according to claim 1 , wherein in the step (1), said 2,2-bipyridyl-5,5′-dicarboxylic acid is dissolved in thionyl chloride, the reaction of 2,2-bipyridyl-5,5′-dicarboxylic acid with thionyl chloride is carried out at 110 to 115° C. for 10 to 12 hours to obtain the 2,2-bipyridyl-5,5′-diacid chloride.

3. The method according to claim 1 , wherein in the step (1), the reaction time of said 2,2-bipyridyl-5,5′-diacid chloride and said 1,4,8,11-tetraazacyclotetradecane is 24 to 48 hours, and the reaction temperature is 45 to 50° C.

4. The method according to claim 1 , wherein in the step (1), after the reaction of said 2,2-bipyridyl-5,5′-diacid chloride and said 1,4,8,11-tetraazacyclotetradecane, the reaction system is washed successively with KOH aqueous solution, chloroform and ethanol, then placed in DMF (Dimethylformamide) and heated at 140-150° C. for 12 hours, then filtered, and the obtained solid is dried to obtain a polynitrogen heterocyclic polymer.

5. The method according to claim 1 , wherein in the step (2), the reaction temperature is 140 to 180° C., and the reaction time is 10 to 20 hours.

6. The method according to claim 1 , wherein in the step (2), after the reaction is finished, the product is sequentially washed with ethanol and deionized water, and then dried to obtain the magnetic Fe 2 O 3 nanosphere with PNH surface modification.

7. The method according to claim 1 , wherein the molar ratio of said 2,2-bipyridyl-5,5′-diacid chloride and said 1,4,8,11-tetraazacyclotetradecane is 1:(2 to 2.1); the mass ratio of said polynitrogen heterocyclic polymer and said iron salt is 1:(0.5 to 2); and said iron salt is FeCl 3 .

8. The method according to claim 1 , further comprising adding the magnetic Fe 2 O 3 nanosphere with PNH surface modification into water containing organic pollutants, then adding hydrogen peroxide, under illumination to complete degradation of organic pollutants in water.

Assignees

• Univ Soochow

Inventors

• Lu Jianmei
• Xu Qingfeng

Classifications

• B01J2235/05

  Nuclear magnetic resonance [NMR] · CPC title

• B01J2235/00

  Indexing scheme associated with group B01J35/00, related to the analysis techniques used to determine the catalysts form or properties · CPC title

• B01J2235/30

  Scanning electron microscopy; Transmission electron microscopy · CPC title

• B01J2235/15

  X-ray diffraction · CPC title

• B01J35/45

  Nanoparticles · CPC title