Method for preparing supported catalyst for heterogeneous catalytic ozonation

Patent metadata

Field	Value
Publication number	US-10618043-B2
Application number	US-201715710807-A
Country	US
Kind code	B2
Filing date	Sep 20, 2017
Priority date	Mar 14, 2017
Publication date	Apr 14, 2020
Grant date	Apr 14, 2020

Abstract

A method for preparing a catalyst, including: 1) uniformly mixing attapulgite, lithium-manganese spinel (Li—Mn spinel), manganese dioxide powders to form mixed raw material; adding water to the mixed raw material; stirring and mixing the mixed raw material and the water for between 5 and 15 min to yield a reaction mixture; 2) feeding the reaction mixture in 1) to a pelletizer to prepare spherical particles or hollow cylindrical particles; drying the spherical particles or the hollow cylindrical particles to yield a precursor; 3) heating the precursor in a muffle furnace, and calcining the precursor to yield a crude catalyst; 4) mixing the crude catalyst with an acid solution; alternating between ultrasound and microwave to wash the crude catalyst; and 5) washing the crude catalyst in 4) with water; and drying the catalyst for 12 hrs in air at 105° C.

First claim

The invention claimed is:

1. A method for preparing a catalyst, the method comprising:
1) uniformly mixing attapulgite, lithium-manganese (Li—Mn) spinel, and manganese dioxide powders to form mixed raw material; adding water to the mixed raw material, wherein, a weight ratio of the attapulgite to the Li—Mn spinel to the manganese dioxide powders and to the water is 100:1-3:1-20:80-90; stirring and mixing the mixed raw material and the water for between 5 and 15 min to yield a reaction mixture;
2) feeding the reaction mixture in 1) to a pelletizer to prepare spherical particles or hollow cylindrical particles, a diameter of the spherical particles being between 3 and 4 mm; drying the spherical particles or the hollow cylindrical particles in a drying oven for between 0.5 and 2.5 hr(s) at 105° C. in air to yield a precursor;
3) heating the precursor prepared in 2) to a temperature between 400 and 1000° C. at a rate of 200° C./h in a muffle furnace, and calcining the precursor for between 2 and 24 hrs to yield a crude catalyst;
4) mixing the crude catalyst prepared in 3) with an acid solution, a weight ratio of the catalyst to the acid solution being 10:50; alternating between ultrasound and microwave to wash the crude catalyst for 30 min; and
5) washing the crude catalyst from 4) using water until a pH value of a resulting washing solution is constant; and drying the crude catalyst for 12 hrs in air at 105° C. to yield the catalyst.

2. The method of claim 1 , wherein
in 1), the attapulgite, the Li—Mn spinel, the manganese dioxide powders, and the water are uniformly mixed and stirred for 15 min to form the mixed raw material, and the weight ratio of the attapulgite to the Li—Mn spinel to the manganese dioxide powders and to the water is 100:2:20:85;
in 2), the diameter of the spherical particles is 4 mm; the spherical particles are dried for 2 hrs at 105° C. in air to yield the precursor; and
in 3), the precursor prepared in 2) is heated to 1000° C. at a rate of 200° C./h in the muffle furnace, and is calcined for 2 hrs.

3. The method of claim 1 , wherein a particle size of the Li—Mn spinel is between 50 and 200 nm.

4. The method of claim 2 , wherein a particle size of the Li—Mn spinel is between 50 and 200 nm.

5. The method of claim 1 , wherein in 2), an inner diameter of the hollow cylindrical particles is 1 mm, and an outer diameter of the hollow cylindrical particles is 4 mm; a cylindrical core is filled with the hollow cylindrical particles, and the cylindrical particles are dried for 2 hrs at 105° C. in air to yield the precursor.

6. The method of claim 1 , wherein the acid solution comprises hydrochloric acid, SnCl 4 .5H 2 O, acetic acid, and water, and a molar ratio thereof is 1:1:2-4:10-15.

7. The method of claim 1 , wherein the crude catalyst is washed under ultrasonic condition for between 3 and 5 min, then washed under microwave radiation for between 1 and 2 min, and repeat above washing steps; an ultrasonic power is between 25 and 80 KHz, and a microwave power is between 2 and 50 W.

Assignees

• Nanjing University Of Technology

Inventors

• Xu Ke
• Wen Shuhan
• Ren Hongqiang
• Geng Jinju

Classifications

• C02F1/78

  with ozone {(C02F1/4672 takes precedence)} · CPC title

• B01J23/005 Primary

  Spinels · CPC title

• B01J23/34

  Manganese · CPC title

• B01J21/005

  Spinels · CPC title

• B01J37/343

  of ultrasonic wave energy · CPC title