CN103295756A - Preparation method of magnetic nitrogen-doped carbon materials - Google Patents
Preparation method of magnetic nitrogen-doped carbon materials Download PDFInfo
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- CN103295756A CN103295756A CN2013102138806A CN201310213880A CN103295756A CN 103295756 A CN103295756 A CN 103295756A CN 2013102138806 A CN2013102138806 A CN 2013102138806A CN 201310213880 A CN201310213880 A CN 201310213880A CN 103295756 A CN103295756 A CN 103295756A
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- 239000003575 carbonaceous material Substances 0.000 title claims abstract description 37
- 238000002360 preparation method Methods 0.000 title claims abstract description 25
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims abstract description 40
- 229910052799 carbon Inorganic materials 0.000 claims abstract description 40
- 239000012046 mixed solvent Substances 0.000 claims abstract description 25
- 238000003763 carbonization Methods 0.000 claims abstract description 20
- VEXZGXHMUGYJMC-UHFFFAOYSA-N Hydrochloric acid Chemical compound Cl VEXZGXHMUGYJMC-UHFFFAOYSA-N 0.000 claims abstract description 18
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims abstract description 15
- DHMQDGOQFOQNFH-UHFFFAOYSA-N Glycine Chemical compound NCC(O)=O DHMQDGOQFOQNFH-UHFFFAOYSA-N 0.000 claims abstract description 12
- 239000008367 deionised water Substances 0.000 claims abstract description 11
- 229910021641 deionized water Inorganic materials 0.000 claims abstract description 11
- 239000002904 solvent Substances 0.000 claims abstract description 11
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 11
- NQXWGWZJXJUMQB-UHFFFAOYSA-K iron trichloride hexahydrate Chemical compound O.O.O.O.O.O.[Cl-].Cl[Fe+]Cl NQXWGWZJXJUMQB-UHFFFAOYSA-K 0.000 claims abstract description 10
- 230000003647 oxidation Effects 0.000 claims abstract description 9
- 238000007254 oxidation reaction Methods 0.000 claims abstract description 9
- 239000003795 chemical substances by application Substances 0.000 claims abstract description 8
- 239000004471 Glycine Substances 0.000 claims abstract description 7
- 229920000877 Melamine resin Polymers 0.000 claims abstract description 7
- JDSHMPZPIAZGSV-UHFFFAOYSA-N melamine Chemical compound NC1=NC(N)=NC(N)=N1 JDSHMPZPIAZGSV-UHFFFAOYSA-N 0.000 claims abstract description 7
- 150000001720 carbohydrates Chemical class 0.000 claims abstract description 5
- 238000000227 grinding Methods 0.000 claims abstract description 3
- QJGQUHMNIGDVPM-UHFFFAOYSA-N nitrogen group Chemical group [N] QJGQUHMNIGDVPM-UHFFFAOYSA-N 0.000 claims description 13
- 229930006000 Sucrose Natural products 0.000 claims description 5
- 239000005720 sucrose Substances 0.000 claims description 5
- WQZGKKKJIJFFOK-GASJEMHNSA-N Glucose Natural products OC[C@H]1OC(O)[C@H](O)[C@@H](O)[C@@H]1O WQZGKKKJIJFFOK-GASJEMHNSA-N 0.000 claims description 4
- 235000014633 carbohydrates Nutrition 0.000 claims description 4
- 239000008103 glucose Substances 0.000 claims description 4
- 229920002472 Starch Polymers 0.000 claims description 2
- 238000013019 agitation Methods 0.000 claims description 2
- WQZGKKKJIJFFOK-VFUOTHLCSA-N beta-D-glucose Chemical compound OC[C@H]1O[C@@H](O)[C@H](O)[C@@H](O)[C@@H]1O WQZGKKKJIJFFOK-VFUOTHLCSA-N 0.000 claims description 2
- 239000001913 cellulose Substances 0.000 claims description 2
- 229920002678 cellulose Polymers 0.000 claims description 2
- 125000003630 glycyl group Chemical group [H]N([H])C([H])([H])C(*)=O 0.000 claims description 2
- 239000008107 starch Substances 0.000 claims description 2
- 235000019698 starch Nutrition 0.000 claims description 2
- 125000000185 sucrose group Chemical group 0.000 claims 1
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 abstract description 30
- 229910052757 nitrogen Inorganic materials 0.000 abstract description 15
- 238000000034 method Methods 0.000 abstract description 5
- 239000003054 catalyst Substances 0.000 abstract description 2
- 238000006243 chemical reaction Methods 0.000 abstract description 2
- 238000010000 carbonizing Methods 0.000 abstract 2
- 239000003990 capacitor Substances 0.000 abstract 1
- 238000001704 evaporation Methods 0.000 abstract 1
- 229940044631 ferric chloride hexahydrate Drugs 0.000 abstract 1
- 239000000446 fuel Substances 0.000 abstract 1
- 238000002156 mixing Methods 0.000 abstract 1
- 239000000463 material Substances 0.000 description 11
- 238000001069 Raman spectroscopy Methods 0.000 description 4
- CZMRCDWAGMRECN-UGDNZRGBSA-N Sucrose Chemical compound O[C@H]1[C@H](O)[C@@H](CO)O[C@@]1(CO)O[C@@H]1[C@H](O)[C@@H](O)[C@H](O)[C@@H](CO)O1 CZMRCDWAGMRECN-UGDNZRGBSA-N 0.000 description 4
- XEEYBQQBJWHFJM-UHFFFAOYSA-N iron Substances [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 4
- 229920002261 Corn starch Polymers 0.000 description 2
- DQMUQFUTDWISTM-UHFFFAOYSA-N O.[O-2].[Fe+2].[Fe+2].[O-2] Chemical compound O.[O-2].[Fe+2].[Fe+2].[O-2] DQMUQFUTDWISTM-UHFFFAOYSA-N 0.000 description 2
- 238000002441 X-ray diffraction Methods 0.000 description 2
- 239000008120 corn starch Substances 0.000 description 2
- 229940099112 cornstarch Drugs 0.000 description 2
- 235000019441 ethanol Nutrition 0.000 description 2
- 239000000843 powder Substances 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- 238000012360 testing method Methods 0.000 description 2
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 1
- 230000010757 Reduction Activity Effects 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- 150000001721 carbon Chemical group 0.000 description 1
- 229910003460 diamond Inorganic materials 0.000 description 1
- 239000010432 diamond Substances 0.000 description 1
- 230000005611 electricity Effects 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 230000005307 ferromagnetism Effects 0.000 description 1
- 229910002804 graphite Inorganic materials 0.000 description 1
- 239000010439 graphite Substances 0.000 description 1
- 238000005087 graphitization Methods 0.000 description 1
- 229910052739 hydrogen Inorganic materials 0.000 description 1
- 239000001257 hydrogen Substances 0.000 description 1
- 229910052742 iron Inorganic materials 0.000 description 1
- 230000001788 irregular Effects 0.000 description 1
- 230000005389 magnetism Effects 0.000 description 1
- 238000005272 metallurgy Methods 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 239000002243 precursor Substances 0.000 description 1
- 238000000197 pyrolysis Methods 0.000 description 1
- 230000001105 regulatory effect Effects 0.000 description 1
- -1 sucrose Chemical class 0.000 description 1
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Abstract
The invention provides a preparation method of magnetic nitrogen-doped carbon materials. The method includes: using concentrated hydrochloric acid to adjust pH of mixed solvent of anhydrous ethanol and deionized water to 1-3, sequentially and fully dissolving or dispersing oxidation carbonization agent (ferric chloride hexahydrate), carbon source (saccharides), nitrogen source (glycine or melamine), mixing well, evaporating solvent, carbonizing at 60-80 DEG C for 40-50 hours, grinding carbonized products, and carbonizing the ground carbonized products at 180-200 DEG C for 4-6 hours to obtain the magnetic nitrogen-doped carbon materials which are promising in application prospect in fields such as fuel cell catalysts and super capacitors. The preparation method is mild in reaction condition, low in cost, simple to operate, and easy to control nitrogen contents in the nitrogen-doped carbon materials.
Description
Technical field
The invention belongs to the material with carbon element technical field, relate to a kind of nitrogen-doped carbon preparation methods, relate in particular to a kind of magnetic nitrogen-doped carbon preparation methods.
Background technology
Carbon is the topmost component of all organisms on the earth.Different one-tenth key modes has caused forming the material with carbon element of multiple different existence forms between the carbon atom, the soft satiny graphite of matter that existing common layer structure is formed, the also hard diamond of not urging of the preciousness of being made up of tetrahedral structure.Material with carbon element is with advantages such as its good heat resistance, high thermal conductivity coefficient, good chemical inertia, high conductivity, be widely used in metallurgy, chemical industry, machinery, electricity, field such as aviation.In recent years, material with carbon element had also received very big concern in the electrochemical applications field, especially in the fuel-cell catalyst application facet.In material with carbon element, add the nitrogen element, can obviously improve the hydrogen reduction activity of material with carbon element.Studies show that the performance of nitrogen-doped carbon material and the doping of nitrogen have direct relation.The high temperature pyrolysis nitrogenous precursor is to obtain nitrogen-doped carbon material one of method the most easily.But be subjected to the restriction of nitrogen content in the presoma, the nitrogen doping is difficult to control.
Summary of the invention
The objective of the invention is in order to solve problems of the prior art, a kind of magnetic nitrogen-doped carbon preparation methods is provided.
Magnetic nitrogen-doped carbon preparation methods of the present invention, after the mixed solvent of ethanol and deionized water transferred pH to 1 ~ 3 with concentrated hydrochloric acid, under agitation successively oxidation carburization agent, carbon source, nitrogenous source fully are dissolved or dispersed in the mixed solvent and mix, boil off solvent then, in 60 ℃ ~ 80 ℃ following carbonization 40 ~ 50h, carbonized product again in 180 ~ 200 ℃ of following carbonization 3 ~ 6h, namely obtains magnetic nitrogen-doped carbon material after grinding.
Described carbon source is carbohydrate (as sucrose, glucose, starch, cellulose etc.); Described nitrogenous source is glycine or melamine; Described oxidation carburization agent is Iron(III) chloride hexahydrate.
In the described mixed solvent, the volume ratio of ethanol and deionized water is 1:1 ~ 1:2.
The mass ratio of described nitrogenous source and carbon source is 1:10 ~ 1:50.
The mass ratio of described oxidation carburization agent and carbon source is 1:2 ~ 1:3.
The described solvent that boils off is in convection oven, carries out under 60 ~ 70 ℃.
Fig. 1 is the Raman spectrogram of a carbonized product of the present invention, and contrasts with C powder (XC-72).As can be seen from Figure 1, the nitrogen-doped carbon material has begun to have formed the G peak, but very irregular, illustrates that carbon source and nitrogenous source have only the small part carbonization.
Fig. 2 is the Raman spectrogram of the magnetic nitrogen-doped carbon material for preparing of the present invention, and contrasts with C powder (XC-72).As can be seen from Figure 2, the D peak of the nitrogen-doped carbon material of the present invention preparation and G peak all clearly, and the G peak illustrate material with carbon element degree of graphitization of formation than higher apparently higher than the D peak, the basic carbonization of carbon source and nitrogenous source is complete.
Fig. 3 is the X-ray diffraction spectrogram of the nitrogen-doped carbon material of the present invention's preparation.Test condition is 40kV, and 30mA uses Cu target ray tube.As can be seen from Figure 3, at 2 θ=24.8 degree tangible carbon characteristic peak is arranged, illustrate that carbon source and nitrogenous source are carbonized, also shown the characteristic peak of di-iron trioxide simultaneously, a part of Fe is described in nitrogen material with carbon element forming process
3+Form with di-iron trioxide still is present in the material with carbon element.
Fig. 4 carries out the picture that magnetic is tested for using permanent magnet to the nitrogen-doped carbon material of the present invention's preparation.Fig. 4 A is that the nitrogen-doped carbon material is placed in the sample bottle under no permanent magnet condition, and the nitrogen-doped carbon material places the sample bottle bottom naturally; Fig. 4 B puts a permanent magnet on the sample bottle next door that sample is housed, and finds that the nitrogen-doped carbon material of the present invention's preparation is all drawn close to permanent magnet one side, illustrates that the nitrogen-doped carbon material of the present invention's preparation has magnetic.This illustrates nitrogen-doped carbon material in forming process, a part of Fe
3+Change into Fe or tri-iron tetroxide and shown ferromagnetism.
After testing, the nitrogen content of the magnetic nitrogen-doped carbon material of the present invention's preparation is 0.9% ~ 12.5%.
The present invention is relative, and prior art has the following advantages:
1, be carbon source with carbohydrates such as sucrose, belong to renewable resource, cost is low;
2, be nitrogenous source with glycine or melamine, pollution-free, environmental protection.
3, be the oxidation carburization agent with the Iron(III) chloride hexahydrate, the oxidation carbonization of carbon source, nitrogenous source is realized under lower temperature, the reaction condition gentleness, cost is low, and easy operating is controlled, and has guaranteed the magnetic of nitrogen-doped carbon material simultaneously;
4, the nitrogen content in the nitrogen-doped carbon material can be controlled by regulating carbon source and nitrogenous source ratio.
5, the nitrogen-doped carbon material of the present invention's preparation has magnetic, is convenient to separate.
Description of drawings
Fig. 1 prepares the Raman spectrogram of a carbonized product in the material with carbon element process for the present invention;
Fig. 2 is the Raman spectrogram of the nitrogen-doped carbon material of the present invention's preparation;
Fig. 3 is the X-ray diffraction spectrogram of the nitrogen-doped carbon material of the present invention's preparation;
Fig. 4 is the nitrogen-doped carbon magnetism of material resolution chart of the present invention's preparation.
Embodiment
Be described further below by the preparation of specific embodiment to magnetic nitrogen-doped carbon material of the present invention.
Embodiment 1
(1) absolute ethyl alcohol and deionized water are mixed with the volume ratio of 1:1 form mixed solvent 40mL, and with concentrated hydrochloric acid regulator solution pH=2;
(2) with 0.60g Iron(III) chloride hexahydrate (FeCl
36H
2O) and 1.50g sucrose join in the mixed solvent successively, and stirred 20 minutes;
(3) the 0.033g glycine is joined in the mixed solvent, stirred 0.5 hour;
(4) mixed system is placed convection oven, in 60 ℃ of first solvent evaporated, again in 80 ℃ of carbonization 40h, get carbonized product one time;
(5) carbonized products place convection oven after milled processed, at 200 ℃ of following carbonization 4h, namely obtain magnetic nitrogen-doped carbon material.The nitrogen content of this nitrogen-doped carbon material is 0.93%.
Embodiment 2
(1) absolute ethyl alcohol and deionized water are mixed with the volume ratio of 1:1.5 form mixed solvent 40mL, and with concentrated hydrochloric acid regulator solution pH=1;
(2) with 0.60g Iron(III) chloride hexahydrate (FeCl
36H
2O) and 1.20g glucose join in the mixed solvent successively, and stirred 20 minutes;
(3) the 0.062g glycine is joined in the mixed solvent, stirred 0.5 hour;
(4) mixed system is placed convection oven, in 70 ℃ of first solvent evaporated, again in 60 ℃ of carbonization 40h, get carbonized product one time;
(5) carbonized products place convection oven after milled processed, at 190 ℃ of following carbonization 6h, namely obtain magnetic nitrogen-doped carbon material.The nitrogen content of this nitrogen-doped carbon material is 2.1%.
Embodiment 3
(1) absolute ethyl alcohol and deionized water are mixed with the volume ratio of 1:2 form mixed solvent 40mL, and with concentrated hydrochloric acid regulator solution pH=2;
(2) with 0.60g Iron(III) chloride hexahydrate (FeCl
36H
2O) and the 1.80g cornstarch join in the mixed solvent successively, and stirred 20 minutes;
(3) the 0.167g glycine is joined in the mixed solvent, stirred 0.5 hour;
(4) mixed system is placed convection oven, in 65 ℃ of first solvent evaporated, again in 80 ℃ of carbonization 48h, get carbonized product one time;
(5) carbonized products place convection oven after milled processed, at 190 ℃ of following carbonization 6h, namely obtain magnetic nitrogen-doped carbon material.The nitrogen content of this nitrogen-doped carbon material is 3.2%.
Embodiment 4
(1) absolute ethyl alcohol and deionized water are mixed with the volume ratio of 1:1.5 form mixed solvent 40mL, and with concentrated hydrochloric acid regulator solution pH=3;
(2) with 0.60g Iron(III) chloride hexahydrate (FeCl
36H
2O) and 1.50g sucrose join in the mixed solvent successively, and stirred 20 minutes;
(3) the 0.092g melamine is joined in the mixed solvent, stirred 0.5 hour;
(4) mixed system is placed convection oven, in 70 ℃ of first solvent evaporated, again in 70 ℃ of carbonization 45h, get carbonized product one time;
(5) carbonized products place convection oven after milled processed, at 180 ℃ of following carbonization 5h, namely obtain magnetic nitrogen-doped carbon material.The nitrogen content of this nitrogen-doped carbon material is 8.6%.
Embodiment 5
(1) absolute ethyl alcohol and deionized water are mixed with the volume ratio of 1:2 form mixed solvent 40mL, and with concentrated hydrochloric acid regulator solution pH=1;
(2) with 0.60g Iron(III) chloride hexahydrate (FeCl
36H
2O) and 1.20g glucose join in the mixed solvent successively, and stirred 20 minutes;
(3) the 0.093g melamine is joined in the mixed solvent, stirred 0.5 hour;
(4) mixed system is placed convection oven, in 65 ℃ of first solvent evaporated, again in 60 ℃ of carbonization 48h, get carbonized product one time;
(5) carbonized products place convection oven after milled processed, at 185 ℃ of following carbonization 4h, namely obtain magnetic nitrogen-doped carbon material.The nitrogen content of this nitrogen-doped carbon material is 10.9%.
Embodiment 6
(1) absolute ethyl alcohol and deionized water are mixed with the volume ratio of 1:1 form mixed solvent 40mL, and with concentrated hydrochloric acid regulator solution pH=2;
(2) with 0.60g Iron(III) chloride hexahydrate (FeCl
36H
2O) and the 1.80g cornstarch join in the mixed solvent successively, and stirred 20 minutes;
(3) the 0.140g melamine is joined in the mixed solvent, stirred 0.5 hour;
(4) mixed system is placed convection oven, in 60 ℃ of first solvent evaporated, again in 80 ℃ of carbonization 50h, get carbonized product one time;
(5) carbonized products place convection oven after milled processed, at 185 ℃ of following carbonization 6h, namely obtain magnetic nitrogen-doped carbon material.The nitrogen content of this nitrogen-doped carbon material is 10.4%.
Claims (6)
1. magnetic nitrogen-doped carbon preparation methods, after the mixed solvent of absolute ethyl alcohol and deionized water transferred pH to 1～3 with concentrated hydrochloric acid, under agitation successively oxidation carburization agent, carbon source, nitrogenous source fully are dissolved or dispersed in the mixed solvent and mix, boil off solvent then, in 60 ℃～80 ℃ following carbonization 40～50h, carbonized product again in 180～200 ℃ of following carbonization 4～6h, namely obtains magnetic nitrogen-doped carbon material after grinding;
Described carbon source is carbohydrate; Described nitrogenous source is glycine or melamine; Described oxidation carburization agent is Iron(III) chloride hexahydrate.
2. magnetic nitrogen-doped carbon preparation methods according to claim 1, it is characterized in that: in the described mixed solvent, the volume ratio of absolute ethyl alcohol and deionized water is 1:1～1:2.
3. magnetic nitrogen-doped carbon preparation methods according to claim 1, it is characterized in that: described carbohydrate is sucrose, glucose, starch, cellulose.
4. magnetic nitrogen-doped carbon preparation methods according to claim 1, it is characterized in that: the mass ratio of described nitrogenous source and carbon source is 1:10～1:50.
5. magnetic nitrogen-doped carbon preparation methods according to claim 1, it is characterized in that: the mass ratio of described oxidation carburization agent and carbon source is 1:2～1:3.
6. magnetic nitrogen-doped carbon preparation methods according to claim 1, it is characterized in that: the described solvent that boils off is in convection oven, carries out under 60～70 ℃.
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Cited By (8)
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| CN103599784A (en) * | 2013-11-19 | 2014-02-26 | 西北师范大学 | Iron and nitrogen doped non-noble metal catalyst as well as preparation method and application thereof |
| CN103706328A (en) * | 2014-01-17 | 2014-04-09 | 湖南大学 | Nitrogen hybridized magnetic ordered mesoporous carbon adsorbent, and preparation method and application thereof |
| CN106299368A (en) * | 2016-07-23 | 2017-01-04 | 天津大学 | A kind of method preparing N doping cellular disordered carbon material |
| CN109012565A (en) * | 2018-08-07 | 2018-12-18 | 华南理工大学 | A kind of method of the magnetic carbon material Adsorption heavy metal ions in wastewater of nitrating |
| CN109382106A (en) * | 2017-08-03 | 2019-02-26 | 中国科学院大连化学物理研究所 | A kind of electroreduction carbon dioxide catalysis material and its preparation and application |
| CN109468121A (en) * | 2018-11-05 | 2019-03-15 | 西北工业大学 | A kind of preparation method of the spherical magnetic porous carbon particle of N doping |
| CN111477882A (en) * | 2020-01-21 | 2020-07-31 | 天津大学 | Iron oxide-nitrogen-doped carbon material, and preparation method and application thereof |
| CN113101962A (en) * | 2021-04-25 | 2021-07-13 | 山西中科国蕴环保科技有限公司 | Porous carbon layer protection catalyst for activating persulfate, preparation method and application |
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Cited By (11)
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| CN103599784A (en) * | 2013-11-19 | 2014-02-26 | 西北师范大学 | Iron and nitrogen doped non-noble metal catalyst as well as preparation method and application thereof |
| CN103599784B (en) * | 2013-11-19 | 2015-10-07 | 西北师范大学 | The non-precious metal catalyst of a kind of iron, N doping and Synthesis and applications thereof |
| CN103706328A (en) * | 2014-01-17 | 2014-04-09 | 湖南大学 | Nitrogen hybridized magnetic ordered mesoporous carbon adsorbent, and preparation method and application thereof |
| CN106299368A (en) * | 2016-07-23 | 2017-01-04 | 天津大学 | A kind of method preparing N doping cellular disordered carbon material |
| CN109382106A (en) * | 2017-08-03 | 2019-02-26 | 中国科学院大连化学物理研究所 | A kind of electroreduction carbon dioxide catalysis material and its preparation and application |
| US11105009B2 (en) | 2017-08-03 | 2021-08-31 | Dalian Institute Of Chemical Physics, Chinese Academy Of Sciences | Graphene material inlaid with single metal atoms and preparing method and application thereof |
| CN109382106B (en) * | 2017-08-03 | 2021-09-21 | 中国科学院大连化学物理研究所 | Electro-reduction carbon dioxide catalytic material and preparation and application thereof |
| CN109012565A (en) * | 2018-08-07 | 2018-12-18 | 华南理工大学 | A kind of method of the magnetic carbon material Adsorption heavy metal ions in wastewater of nitrating |
| CN109468121A (en) * | 2018-11-05 | 2019-03-15 | 西北工业大学 | A kind of preparation method of the spherical magnetic porous carbon particle of N doping |
| CN111477882A (en) * | 2020-01-21 | 2020-07-31 | 天津大学 | Iron oxide-nitrogen-doped carbon material, and preparation method and application thereof |
| CN113101962A (en) * | 2021-04-25 | 2021-07-13 | 山西中科国蕴环保科技有限公司 | Porous carbon layer protection catalyst for activating persulfate, preparation method and application |
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