Method for preparing bi-component, multi-network nanofibrous aerogel-supported heterojunction photocatalyst and application thereof

Patent metadata

Field	Value
Publication number	US-11413608-B2
Application number	US-202016748720-A
Country	US
Kind code	B2
Filing date	Jan 21, 2020
Priority date	Jan 25, 2019
Publication date	Aug 16, 2022
Grant date	Aug 16, 2022

Abstract

A method for preparing a bi-component, multi-network nanofibrous aerogel-supported heterojunction photocatalyst includes the following steps. Step 1, preparing ammoniated polyacrylonitrile nanofibers. Step 2, dispersing the ammoniated polyacrylonitrile nanofibers in water to obtain a first solution; dispersing cellulose nanofibers in water to obtain a second solution; and mixing, heating and lyophilizing the first solution with the second solution to obtain a bi-component, multi-network nanofibrous aerogel. Step 3, adding graphite carbon nitride, a ferric-iron containing reagent, 2,5-diaminoterephthalic acid, and the bi-component, multi-network nanofiber aerogel obtained in the step 2 into a N, N-dimethylformamide solvent to obtain a third solution, and carrying out a hydrothermal reaction on the third solution for 8-24 hours to obtain the bi-component, multi-network nanofibrous aerogel-supported heterojunction photocatalyst.

First claim

What is claimed is:

1. A method for preparing a bi-component, multi-network nanofibrous aerogel-supported heterojunction photocatalyst, comprising the following steps:
step 1, preparing ammoniated polyacrylonitrile nanofibers;
step 2, dispersing the ammoniated polyacrylonitrile nanofibers in water to obtain a first solution; dispersing cellulose nanofibers in water to obtain a second solution; and mixing, heating and lyophilizing the first solution with the second solution to obtain a bi-component, multi-network nanofibrous aerogel; and
step 3, adding graphite carbon nitride, a ferric-iron containing reagent, 2,5-diaminoterephthalic acid, and the bi-component, multi-network nanofiber aerogel obtained in the step 2 into a N, N-dimethylformamide solvent to obtain a third solution, and carrying out a hydrothermal reaction on the third solution for 8-24 hours to obtain the bi-component, multi-network nanofibrous aerogel-supported heterojunction photocatalyst.

2. The method according to claim 1 , wherein, the step of preparing the ammoniated polymer nanofibers in the step 1 comprises:
step 1.1, preparing polyacrylonitrile nanofibers with a polyacrylonitrile high polymer solution as a spinning solution by a high-voltage electrostatic spinning technique;
step 1.2, placing the polyacrylonitrile nanofibers in an aqueous solution containing an ammoniating agent, adjusting a temperature to 100-180° C., and carrying out a heating reaction for 6-24 hours.

3. The method according to claim 2 , wherein,
in the step 1.1, a mass fraction of the spinning solution is 8%-15%, a spinning voltage is 10-30 kV, a flow rate of the spinning solution is 0.5-2.0 mL/h, and a collection distance is 13-22 cm;
in the step 1.2, a dosage of the polyacrylonitrile nanofibers is 2-5 g/L, and a dosage of the ammoniating reagent is 100-500 g/L; and
the ammoniating reagent is one selected from the group consisting of ethylenediamine, triethylenediamine, tetraethylenepentamine, a polyamine, and polyethyleneimine.

4. The method according to claim 1 , wherein, in the step 2, the heating is performed in an oven at 80° C. for 0.5-8 hours.

5. The method according to claim 1 , wherein, in the step 2, a mass-volume ratio of the ammoniated polyacrylonitrile nanofibers to water in the first solution is 5-20 g/L, a volume ratio of the cellulose nanofibers having a mass fraction of 5% to water in the second solution ranges from 1:5 to 1:20, and a volume ratio of the first solution and the second solution is 1:1.

6. The method according to claim 1 , wherein, in the step 3, the graphite carbon nitride is prepared by calcining melamine at 400-550° C. for 2-6 hours.

7. The method according to claim 1 , wherein, in the step 3, the ferric-iron containing reagent is one selected from the group consisting of ferric nitrate, ferric chloride, and ferric sulfate.

8. The method according to claim 1 , wherein, in the step 3, a dosage of the graphite carbon nitride is 1-5 g/L, a dosage of the ferric-iron containing reagent is 2-10 g/L, and a mass ratio of the ferric-iron containing reagent to the 2,5-diaminoterephthalic acid ranges from 1:1 to 1:5, and a dosage of the bi-component, multi-network nanofibrous aerogel is 0.5-2 g/L.

9. The method according to claim 1 , wherein, in the step 3, a temperature for the hydrothermal reaction is 120-180° C.

10. A method of using the bi-component, multi-network nanofiber aerogel-supported heterojunction photocatalyst made by the method according to claim 1 , comprising: using the bi-component, multi-network nanofiber aerogel-supported heterojunction photocatalyst in environmental pollution treatment and energy conversion.

11. The method of claim 10 , wherein, the step of preparing the ammoniated polymer nanofibers in the step 1 comprises:
step 1.1, preparing polyacrylonitrile nanofibers with a polyacrylonitrile high polymer solution as a spinning solution by a high-voltage electrostatic spinning technique;
step 1.2, placing the polyacrylonitrile nanofibers in an aqueous solution containing an ammoniating agent, adjusting a temperature to 100-180° C., and carrying out a heating reaction for 6-24 hours.

12. The method of claim 11 , wherein,
in the step 1.1, a mass fraction of the spinning solution is 8%-15%, a spinning voltage is 10-30 kV, a flow rate of the spinning solution is 0.5-2.0 mL/h, and a collection distance is 13-22 cm;
in the step 1.2, a dosage of the polyacrylonitrile nanofibers is 2-5 g/L, and a dosage of the ammoniating reagent is 100-500 g/L; and
the ammoniating reagent is one selected from a group consisting of ethylenediamine, triethylenediamine, tetraethylenepentamine, a polyamine, and polyethyleneimine.

13. The method of claim 10 , wherein, in the step 2, heating conditions are: placing in an oven for drying at 80° C. for 0.5-8 hours.

14. The method of claim 10 , wherein, in the step 2, a mass-volume ratio of the ammoniated polyacrylonitrile nanofibers to water in the first solution is 5-20 g/L, a volume ratio of a cellulose nanofiber solution having a mass fraction of 5% to water in the second solution ranges from 1:5 to 1:20, and a mixed volume ratio of the first solution and the second solution is 1:1.

15. The method of claim 10 , wherein, in the step 3, the graphite carbon nitride is prepared by the following step: calcining melamine at 400-550° C. for 2-6 hours.

16. The method of claim 10 , wherein, in the step 3, the ferric-iron containing reagent is one selected from the group consisting of ferric nitrate, ferric chloride, and ferric sulfate.

17. The method of claim 10 , wherein, in the step 3, a dosage of the graphite carbon nitride is 1-5 g/L, a dosage of the ferric-iron containing reagent is 2-10 g/L, and a mass ratio of the ferric-iron containing reagent to the 2,5-diaminoterephthalic acid ranges from 1:1 to 1:5, and a dosage of the bi-component, multi-network nanofibrous aerogel is 0.5-2 g/L.

18. The method of claim 10 , wherein, in the step 3, a temperature for the hydrothermal reaction is 120-180° C.

Assignees

• Nanjing University Of Technology

Inventors

• Liu Fuqiang
• Qiu Jinli
• Fan Pei
• Yue Cailiang
• Yuan Ranran
• Li Aimin

Classifications

• B01J35/45

  Nanoparticles · CPC title

• B01J37/0009

  Use of binding agents; Moulding; Pressing; Powdering; Granulating; Addition of materials ameliorating the mechanical properties of the product catalyst · CPC title

• B01J37/10

  in the presence of water, e.g. steam · CPC title

• B01J31/06

  containing polymers {(organometallic polymers B01J31/123; polymer-bound organometallic complexes B01J31/165; coordination polymers B01J31/1691)} · CPC title

• B01J31/1625

  immobilised by covalent linkages, i.e. pendant complexes with optional linking groups · CPC title