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Monatomic catalyst for activating persulfate to generate pure singlet oxygen as well as preparation method and application thereof

A technology for activating persulfate and singlet oxygen, used in catalyst activation/preparation, physical/chemical process catalysts, organic compound/hydride/coordination complex catalysts, etc. poor selectivity of organic pollutants, etc.

Active Publication Date: 2021-07-02
NANCHANG HANGKONG UNIVERSITY
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

However, the supports of SACs mainly include nitrogen-doped carbon and defect-rich materials, but the various forms of nitrogen in the above-mentioned supports, the complex types of defects, and the low content lead to inhomogeneous active sites in SACs, making SACs in AOP, There are usually free radicals (hydroxyl radicals (·OH), sulfate radicals (·SO4-), superoxide radicals (·O2-) etc.) and non-free radicals (singlet oxygen (1O2) etc.) It has disadvantages such as poor selectivity in degrading organic pollutants and poor ability to resist interference from environmental media.

Method used

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  • Monatomic catalyst for activating persulfate to generate pure singlet oxygen as well as preparation method and application thereof
  • Monatomic catalyst for activating persulfate to generate pure singlet oxygen as well as preparation method and application thereof
  • Monatomic catalyst for activating persulfate to generate pure singlet oxygen as well as preparation method and application thereof

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preparation example Construction

[0043] The present invention also provides the activated persulfate described in the above technical scheme to generate pure 1 o 2 The preparation method of SACs comprises the following steps:

[0044] Mix organic acid ligands, soluble iron salts and water for complexation reaction to obtain iron-organic complex solution;

[0045] Mixing the iron-organic complex solution, cyanuric acid and cyanamide compound for self-assembly reaction to obtain a precursor;

[0046] The precursor is subjected to pyrolysis to obtain the activated persulfate to generate pure 1 o 2 of SACs.

[0047] In the present invention, unless otherwise specified, the raw materials used in the present invention are preferably commercially available products.

[0048] The invention mixes the organic acid ligand, soluble iron salt and water to carry out the complexation reaction to obtain the iron-organic complex solution.

[0049] In the present invention, the organic acid ligand preferably includes one...

Embodiment 1

[0075] (1) Weigh 643mg of oxalic acid, add to 50mL of deionized water and dissolve to obtain solution A;

[0076] (2) Weigh 288 mg of ferric nitrate, add it into solution A, and stir for 10 minutes to obtain solution B;

[0077] (3) Weigh 2.46g cyanuric acid and 3g melamine respectively, add 350mL deionized water, heat and dissolve at 80°C to obtain solutions C and D;

[0078] (4) Mix solutions B and C to obtain solution E;

[0079](5) Add solution D to E for mixing, stir for 4 hours, filter with suction, wash the obtained precipitate with water, and dry at 90°C for 3 hours to obtain the precursor;

[0080] (6) Put the precursor obtained in (5) in a tube furnace, raise the temperature to 600°C at 5°C / min under the protection of argon atmosphere and keep it for 4h to obtain SACs, and use ICP-AES to test the Fe content of the obtained SACs 7.0% of the mass of SACs, recorded as 7.0% Fe 1 CN.

Embodiment 2

[0082] (1) Weigh 643mg of oxalic acid, add to 50mL of deionized water and dissolve to obtain solution A;

[0083] (2) Weigh 432 mg of ferric nitrate, add it into solution A, and stir for 10 minutes to obtain solution B;

[0084] (3) Weigh 2.46g cyanuric acid and 3g melamine respectively, add 350mL deionized water, heat and dissolve at 80°C to obtain solutions C and D;

[0085] (4) Mix solutions B and C to obtain solution E;

[0086] (5) Add solution D to E for mixing, stir for 4 hours, filter with suction, wash the obtained precipitate with water, and dry at 90°C for 3 hours to obtain the precursor;

[0087] (6) Put the precursor obtained in (5) in a tube furnace, raise the temperature to 600°C at 5°C / min under the protection of argon atmosphere and keep it for 4h to obtain SACs, and use ICP-AES to test the Fe content of the obtained SACs 8.0% of the mass of SACs, recorded as 8.0% Fe 1 CN.

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Abstract

The invention belongs to the field of monoatomic catalytic degradation of refractory organic pollutants, and provides a monoatomic catalyst for activating persulfate to generate pure singlet oxygen (<1>O2) as well as a preparation method and application thereof. The monatomic catalyst comprises a carrier and an iron monatomic loaded on the carrier, the carrier is a graphite phase carbon nitride nanosheet; the iron monatomic is combined on the carrier by an Fe-N4 coordination structure. The graphite phase carbon nitride nanosheet is used as a carrier, so that the surrounding environment of iron monatomic is uniform, the monatomic is only converted into <1>O2 when persulfate is activated, <1>O2 has good selectivity and anti-interference capability, and the monatomic catalyst provided by the invention has excellent selectivity and anti-interference capability when organic pollutants are degraded. Meanwhile, the mass of iron monatomic in the monatomic catalyst is 7-12% of the mass of the monatomic catalyst, so that the persulfate activation efficiency of the monatomic catalyst is improved.

Description

technical field [0001] The invention relates to the field of single-atom catalytic degradation of refractory organic pollutants, in particular to a single-atom catalyst for activating persulfate to generate pure singlet oxygen, a preparation method and application thereof. Background technique [0002] In recent years, single-atom catalysts (SACs) with the advantages of high activity, high atom utilization and high selectivity have been widely used in energy, chemistry and other fields, providing new ideas for efficient energy conversion and catalytic organic reactions. In addition, the advantages of SACs make them attract more and more attention in environmental governance. Among them, in terms of single-atom catalytic advanced oxidation technology (AOP), SACs such as Mn, Fe, and Co can efficiently activate peroxymonosulfate (PMS), peroxodisulfate (PDS) and H 2 o 2 , to achieve efficient degradation of refractory organic pollutants in water. However, the supports of SACs...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J27/24B01J31/18B01J37/08C02F1/72C02F101/34C02F101/36
CPCB01J27/24B01J31/1805B01J35/0013B01J35/0093B01J37/082C02F1/725C02F2101/345C02F2101/36B01J23/745B82Y30/00C01B13/0211B82Y40/00Y02W10/37B01J35/023B01J37/0018
Inventor 邹建平张龙帅江训恒钟子嫒巫飞尧罗雯婧祝顺鹏龙锐林刘海燕
Owner NANCHANG HANGKONG UNIVERSITY