CN115591569A - Cobalt-nitrogen-carbon non-noble metal catalyst for removing formaldehyde at room temperature and preparation method thereof - Google Patents
Cobalt-nitrogen-carbon non-noble metal catalyst for removing formaldehyde at room temperature and preparation method thereof Download PDFInfo
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- WSFSSNUMVMOOMR-UHFFFAOYSA-N Formaldehyde Chemical compound O=C WSFSSNUMVMOOMR-UHFFFAOYSA-N 0.000 title claims abstract description 117
- 239000003054 catalyst Substances 0.000 title claims abstract description 52
- 229910000510 noble metal Inorganic materials 0.000 title claims abstract description 42
- 238000002360 preparation method Methods 0.000 title claims abstract description 21
- WBVDQFAPFUMTFF-UHFFFAOYSA-N [C].[N].[Co] Chemical compound [C].[N].[Co] WBVDQFAPFUMTFF-UHFFFAOYSA-N 0.000 title claims description 34
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims abstract description 27
- 229910052799 carbon Inorganic materials 0.000 claims abstract description 17
- 229910017052 cobalt Inorganic materials 0.000 claims abstract description 5
- 239000010941 cobalt Substances 0.000 claims abstract description 5
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 claims abstract description 5
- JMANVNJQNLATNU-UHFFFAOYSA-N oxalonitrile Chemical compound N#CC#N JMANVNJQNLATNU-UHFFFAOYSA-N 0.000 claims abstract description 4
- 229940011182 cobalt acetate Drugs 0.000 claims description 21
- QAHREYKOYSIQPH-UHFFFAOYSA-L cobalt(II) acetate Chemical compound [Co+2].CC([O-])=O.CC([O-])=O QAHREYKOYSIQPH-UHFFFAOYSA-L 0.000 claims description 21
- 238000003756 stirring Methods 0.000 claims description 21
- 238000001354 calcination Methods 0.000 claims description 20
- 239000012018 catalyst precursor Substances 0.000 claims description 18
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 14
- 239000003446 ligand Substances 0.000 claims description 14
- QJGQUHMNIGDVPM-UHFFFAOYSA-N nitrogen group Chemical group [N] QJGQUHMNIGDVPM-UHFFFAOYSA-N 0.000 claims description 14
- 239000007787 solid Substances 0.000 claims description 14
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 14
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 claims description 12
- 238000010438 heat treatment Methods 0.000 claims description 12
- 239000000126 substance Substances 0.000 claims description 10
- 239000002994 raw material Substances 0.000 claims description 9
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims description 7
- 238000000227 grinding Methods 0.000 claims description 7
- 238000003760 magnetic stirring Methods 0.000 claims description 7
- 239000004570 mortar (masonry) Substances 0.000 claims description 7
- 239000012299 nitrogen atmosphere Substances 0.000 claims description 7
- 239000000843 powder Substances 0.000 claims description 7
- 238000000197 pyrolysis Methods 0.000 claims description 7
- 238000005303 weighing Methods 0.000 claims description 7
- 229910052757 nitrogen Inorganic materials 0.000 claims description 6
- GEYOCULIXLDCMW-UHFFFAOYSA-N 1,2-phenylenediamine Chemical compound NC1=CC=CC=C1N GEYOCULIXLDCMW-UHFFFAOYSA-N 0.000 claims description 5
- DGEZNRSVGBDHLK-UHFFFAOYSA-N [1,10]phenanthroline Chemical compound C1=CN=C2C3=NC=CC=C3C=CC2=C1 DGEZNRSVGBDHLK-UHFFFAOYSA-N 0.000 claims description 5
- 238000001704 evaporation Methods 0.000 claims description 5
- 238000000034 method Methods 0.000 claims description 5
- 239000006229 carbon black Substances 0.000 claims description 4
- 238000007738 vacuum evaporation Methods 0.000 claims description 3
- 238000001291 vacuum drying Methods 0.000 claims description 2
- 229910000314 transition metal oxide Inorganic materials 0.000 abstract description 4
- 230000003197 catalytic effect Effects 0.000 description 8
- 239000000203 mixture Substances 0.000 description 6
- 238000001035 drying Methods 0.000 description 5
- 230000003647 oxidation Effects 0.000 description 4
- 238000007254 oxidation reaction Methods 0.000 description 4
- 238000006243 chemical reaction Methods 0.000 description 3
- 230000000694 effects Effects 0.000 description 3
- 238000010025 steaming Methods 0.000 description 3
- CODVACFVSVNQPY-UHFFFAOYSA-N [Co].[C] Chemical compound [Co].[C] CODVACFVSVNQPY-UHFFFAOYSA-N 0.000 description 2
- 239000003344 environmental pollutant Substances 0.000 description 2
- 238000011156 evaluation Methods 0.000 description 2
- 238000002474 experimental method Methods 0.000 description 2
- 239000007789 gas Substances 0.000 description 2
- 239000000463 material Substances 0.000 description 2
- 231100000719 pollutant Toxicity 0.000 description 2
- 238000005033 Fourier transform infrared spectroscopy Methods 0.000 description 1
- 229910004298 SiO 2 Inorganic materials 0.000 description 1
- 229910010413 TiO 2 Inorganic materials 0.000 description 1
- 238000002441 X-ray diffraction Methods 0.000 description 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
- 238000007664 blowing Methods 0.000 description 1
- 230000005587 bubbling Effects 0.000 description 1
- 230000000711 cancerogenic effect Effects 0.000 description 1
- 231100000315 carcinogenic Toxicity 0.000 description 1
- 238000006555 catalytic reaction Methods 0.000 description 1
- 238000005034 decoration Methods 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 150000004985 diamines Chemical class 0.000 description 1
- 238000010981 drying operation Methods 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 229910044991 metal oxide Inorganic materials 0.000 description 1
- 150000004706 metal oxides Chemical class 0.000 description 1
- WSFSSNUMVMOOMR-NJFSPNSNSA-N methanone Chemical compound O=[14CH2] WSFSSNUMVMOOMR-NJFSPNSNSA-N 0.000 description 1
- 239000000178 monomer Substances 0.000 description 1
- 238000000696 nitrogen adsorption--desorption isotherm Methods 0.000 description 1
- 230000001590 oxidative effect Effects 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
- 229910052760 oxygen Inorganic materials 0.000 description 1
- 239000011148 porous material Substances 0.000 description 1
- 239000002243 precursor Substances 0.000 description 1
- 238000000746 purification Methods 0.000 description 1
- 238000001179 sorption measurement Methods 0.000 description 1
- 231100000378 teratogenic Toxicity 0.000 description 1
- 230000003390 teratogenic effect Effects 0.000 description 1
- 229910052723 transition metal Inorganic materials 0.000 description 1
- -1 transition metal salt Chemical class 0.000 description 1
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J27/00—Catalysts comprising the elements or compounds of halogens, sulfur, selenium, tellurium, phosphorus or nitrogen; Catalysts comprising carbon compounds
- B01J27/24—Nitrogen compounds
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
- B01D53/86—Catalytic processes
- B01D53/8668—Removing organic compounds not provided for in B01D53/8603 - B01D53/8665
-
- B01J35/61—
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J37/00—Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
- B01J37/08—Heat treatment
- B01J37/082—Decomposition and pyrolysis
- B01J37/086—Decomposition of an organometallic compound, a metal complex or a metal salt of a carboxylic acid
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2257/00—Components to be removed
- B01D2257/70—Organic compounds not provided for in groups B01D2257/00 - B01D2257/602
- B01D2257/708—Volatile organic compounds V.O.C.'s
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2258/00—Sources of waste gases
- B01D2258/06—Polluted air
Abstract
The invention discloses a non-noble metal catalyst for removing formaldehyde at room temperature and a preparation method thereof, aiming at solving the problem that the removal rate of formaldehyde is low under the room temperature condition of the existing transition metal oxide, the technical scheme is that the catalyst consists of carbon nitride doped with an active component cobalt and a carbon carrier; belonging to the technical field of preparation methods of non-noble metal catalysts.
Description
Technical Field
The invention relates to a catalyst, in particular to a cobalt nitrogen carbon non-noble metal catalyst for removing formaldehyde at room temperature, and also relates to a preparation method of the cobalt nitrogen carbon non-noble metal catalyst for removing formaldehyde at room temperature, belonging to the technical field of preparation methods of non-noble metal catalysts.
Background
The indoor formaldehyde mainly comes from decoration materials such as artificial boards, and the formaldehyde with the safe concentration of more than 0.08mg/m < 3 > is probably teratogenic and carcinogenic after being contacted for a long time. At present, the catalytic oxidation method for removing indoor formaldehyde pollutants is one of the feasible methods, and the method oxidizes formaldehyde into CO through room-temperature catalytic oxidation 2 And H 2 And O achieves the purpose of removing formaldehyde pollutants.
However, the difficulty of the catalytic oxidation technology in practical application is mainly to prepare a catalyst with low temperature, high efficiency, low cost and good stability. At room temperature, the catalyst for efficiently catalyzing and oxidizing formaldehyde is mainly a noble metal-loaded catalyst, and a common carrier is mainly TiO 2 、SiO 2 And metal oxides, however, the noble metals used in these catalysts result in high raw material cost and poor stability, which is not suitable for practical applications. The transition metal oxide with abundant resources and relatively low price shows good stability, but the removal rate of formaldehyde at room temperature is generally low, and the difference is still kept from practical application. How to obtain a formaldehyde removal catalyst which is efficient, stable and low in cost at room temperature is a hot spot and a challenge in the current technical development.
Disclosure of Invention
Aiming at the defects, the invention aims to provide a non-noble metal catalyst for removing formaldehyde at room temperature, and solves the problem that the removal rate of formaldehyde is low under the room temperature condition of the existing transition metal oxide.
The second purpose of the invention is to provide a preparation method of the cobalt nitrogen carbon non-noble metal catalyst for removing formaldehyde at room temperature.
To this end, the first technical solution of the present invention is as follows:
the cobalt nitrogen carbon non-noble metal catalyst for removing formaldehyde at room temperature is composed of carbon nitride doped with cobalt simple substance and carrier.
Further, the mass ratio of the carbon nitride-doped cobalt monomer to the carrier is 1: 7-10.
Further, the nitrogen-containing ligand of the cobalt nitrogen carbon non-noble metal catalyst for removing formaldehyde at room temperature is phthalic diamine and 1, 10-phenanthroline.
Furthermore, the carrier of the cobalt nitrogen carbon non-noble metal catalyst for removing formaldehyde at room temperature is active carbon or carbon black.
The second technical scheme provided by the invention is as follows:
a preparation method of a cobalt nitrogen carbon non-noble metal catalyst for removing formaldehyde at room temperature sequentially comprises the following steps:
1) Preparation of catalyst precursor
Weighing cobalt acetate, nitrogen-containing ligand and carbon carrier according to the mass ratio of 1: 2-4: 2.5-3.5, sequentially adding the weighed cobalt acetate and nitrogen-containing ligand into absolute ethyl alcohol, and stirring in a constant-temperature magnetic stirring instrument for 0.2-1h until the cobalt acetate, nitrogen-containing ligand and carbon carrier are fully dissolved to obtain a raw material solution; then introducing the weighed carbon carrier into the solution, heating and fully stirring for 0.05-0.15h, and evaporating to dryness in vacuum for 0.5-1.5h to obtain a catalyst precursor;
2) Calcination of
Calcining and pyrolyzing the catalyst precursor prepared in the step 1) in a nitrogen atmosphere to obtain the cobalt nitrogen carbon non-noble metal catalyst.
Further, in the preparation method of the cobalt nitrogen carbon non-noble metal catalyst for removing formaldehyde at room temperature, the vacuum evaporation drying operation step in the step 1) is specifically as follows: putting the triangular beaker filled with the solution into a constant-temperature water bath kettle, keeping the water temperature at 50 ℃, connecting a vacuum circulating pump by adopting a T-shaped three-way joint, evaporating absolute ethyl alcohol under a stirring state, and then carrying out vacuum drying to obtain solid powder; and pouring the residual solid substance into an agate mortar for full grinding to prepare the catalyst precursor.
Further, in the preparation method of the cobalt nitrogen carbon non-noble metal catalyst for removing formaldehyde at room temperature, in the step 2), the calcination pyrolysis condition is under the protection of nitrogen, the temperature rise speed of the tubular furnace is 5 degrees/min, the calcination temperature is 300-900 ℃, the calcination time is 1h, and the nitrogen flow is 20mL/min.
Compared with the prior art, the technical scheme provided by the invention has the following technical advantages:
1. the cobalt nitrogen carbon non-noble metal catalyst for removing formaldehyde at room temperature provided by the invention adopts cobalt acetate, a nitrogen-containing ligand and a carbon carrier as raw materials to prepare the catalyst, and has the following advantages: the cobalt acetate is used as transition metal salt, so that the cost is low and the cobalt acetate is easy to obtain; the preparation process is simple, the steps of the preparation process of the CoNC precursor are few, the time consumption is short, and the operation is easy; the preparation condition is mild, and the preparation process is easy to control;
2. the cobalt nitrogen carbon non-noble metal catalyst for removing formaldehyde at room temperature changes the surface performance, and a plurality of stacking holes and crack holes are formed on the surface, so that the specific surface area is improved, and the adsorption capacity of the catalyst on formaldehyde in the air is enhanced; but does not affect the internal intrinsic structure of the catalyst;
3. the cobalt nitrogen carbon non-noble metal catalyst for removing formaldehyde at room temperature provided by the invention has good catalytic purification capacity, overcomes the harsh conditions such as high catalytic temperature and the like required by the traditional transition metal oxide for catalytic oxidation of formaldehyde, and has the characteristics of simple preparation, economy, environmental protection, high catalytic efficiency of 95% at room temperature, long service life of 1000h and the like.
Drawings
FIG. 1 is an XRD pattern of a cobalt nitrogen carbon non-noble metal catalyst provided in examples 2 to 5;
FIG. 2 is a FTIR plot of a cobalt nitrogen carbon non-noble metal catalyst provided in examples 2 to 5;
FIG. 3 is a nitrogen adsorption-desorption isotherm for a cobalt nitrogen carbon non-noble metal catalyst provided in examples 2 to 5;
fig. 4 is a graph of the pore size distribution of the cobalt nitrogen carbon non-noble metal catalysts provided in examples 2-5.
Detailed Description
The cobalt nitrogen carbon/carbon supported catalyst for removing formaldehyde at room temperature and the preparation method thereof according to the present invention will be further described with reference to some embodiments. The specific examples are intended to illustrate the invention in further detail and are not intended to limit the scope of the invention. Unless otherwise indicated, the methods and materials employed in the examples of the present invention are all conventionally selected in the art.
Example 1
1) Weighing 2.30g of cobalt acetate, 4.60g of phenanthroline and 6.90g of carbon black, sequentially adding the weighed cobalt acetate and the phenanthroline into 100ml of absolute ethyl alcohol, and stirring in a constant-temperature magnetic stirring instrument for 0.5h until the cobalt acetate and the phenanthroline are fully dissolved to obtain a raw material solution; then introducing the weighed carbon black into the solution, heating and fully stirring for 0.12h, transferring the solution into a triangular beaker, putting the triangular beaker into a constant-temperature water bath kettle, keeping the water temperature at 50 ℃, connecting a vacuum circulating pump by adopting a T-shaped three-way joint, evaporating anhydrous ethanol to dryness for 0.5h under the stirring state, and drying for 12h under the vacuum conditions of-0.1 MPa and 60 ℃ to obtain solid powder; pouring the residual solid substance into an agate mortar for full grinding to prepare a catalyst precursor;
2) Calcining the catalyst precursor prepared in the step 1) in a nitrogen atmosphere with the flow of 20mL/min for pyrolysis, heating at the speed of 5 DEG/min at the temperature of 700 ℃, and calcining for 1h to obtain the cobalt nitrogen carbon non-noble metal catalyst.
Example 2
1) Weighing 1.84g of cobalt acetate, 5.52g of o-phenylenediamine and 6.44g of activated carbon, sequentially adding the weighed cobalt acetate and the nitrogen-containing ligand into 100ml of absolute ethyl alcohol, and stirring in a constant-temperature magnetic stirring instrument for 1 hour until the cobalt acetate and the nitrogen-containing ligand are fully dissolved to obtain a raw material solution; then introducing the weighed active carbon into the solution, heating and fully stirring for 0.15h, transferring the solution into a triangular beaker and putting the triangular beaker into a constant-temperature water bath kettle, keeping the water temperature at 50 ℃, connecting a vacuum circulating pump by adopting a T-shaped three-way joint, steaming dry absolute ethyl alcohol for 1.2h under the stirring state, and drying for 12h under the vacuum conditions of-0.1 MPa and 60 ℃ to obtain solid powder; pouring the residual solid substance into an agate mortar for full grinding to prepare a catalyst precursor;
2) Calcining the catalyst precursor prepared in the step 1) in a nitrogen atmosphere with the flow of 20mL/min for pyrolysis, heating at the speed of 5 DEG/min at the temperature of 500 ℃, and calcining for 1h to obtain the cobalt nitrogen carbon non-noble metal catalyst.
Example 3
1) Weighing 1.84g of cobalt acetate, 7.36g of o-phenylenediamine and 4.60g of activated carbon, sequentially adding the weighed cobalt acetate and the nitrogen-containing ligand into 100ml of absolute ethyl alcohol, and placing the mixture into a constant-temperature magnetic stirring instrument to stir for 0.2h until the mixture is fully dissolved to obtain a raw material solution; then introducing the weighed active carbon into the solution, heating and fully stirring for 0.05h, transferring the solution into a triangular beaker, putting the triangular beaker into a constant-temperature water bath kettle, keeping the water temperature at 50 ℃, connecting a vacuum circulating pump by adopting a T-shaped three-way joint, evaporating anhydrous ethanol for 1.5h in a stirring state, and drying for 12h under the vacuum conditions of-0.1 MPa and 60 ℃ to obtain solid powder; pouring the residual solid substance into an agate mortar for full grinding to prepare a catalyst precursor;
2) Calcining the catalyst precursor prepared in the step 1) in a nitrogen atmosphere with the flow of 20mL/min for pyrolysis, heating at the speed of 5 DEG/min at the temperature of 300 ℃, and calcining for 1h to obtain the cobalt nitrogen carbon non-noble metal catalyst.
Example 4
1) Weighing 2.51g of cobalt acetate, 5.02g of o-phenylenediamine and 6.27g of activated carbon, sequentially adding the weighed cobalt acetate and the nitrogen-containing ligand into 100ml of absolute ethyl alcohol, and placing the mixture in a constant-temperature magnetic stirring instrument to stir for 0.6h until the mixture is fully dissolved to obtain a raw material solution; then introducing the weighed active carbon into the solution, heating and fully stirring for 0.1h, transferring the solution into a triangular beaker, putting the triangular beaker into a constant-temperature water bath kettle, keeping the water temperature at 50 ℃, connecting a vacuum circulating pump by adopting a T-shaped three-way joint, steaming dry absolute ethyl alcohol for 0.8h under the stirring state, and drying for 12h under the vacuum conditions of-0.1 MPa and 60 ℃ to obtain solid powder; pouring the residual solid substance into an agate mortar for full grinding to prepare a catalyst precursor;
2) Calcining the catalyst precursor prepared in the step 1) in a nitrogen atmosphere with the flow of 20mL/min for pyrolysis, heating at the speed of 5 DEG/min at the temperature of 700 ℃, and calcining for 1h to obtain the cobalt nitrogen carbon non-noble metal catalyst.
EXAMPLE 5 preparation of cobalt nitrogen carbon non-noble metal catalyst
1) Weighing 2.30g of cobalt acetate, 5.75g of o-phenylenediamine and 5.75g of activated carbon, sequentially adding the weighed cobalt acetate and the nitrogen-containing ligand into 100ml of absolute ethyl alcohol, and placing the mixture in a constant-temperature magnetic stirring instrument to stir for 0.8h until the mixture is fully dissolved to obtain a raw material solution; then introducing the weighed active carbon into the solution, heating and fully stirring for 0.1h, transferring the solution into a triangular beaker, putting the triangular beaker into a constant-temperature water bath kettle, keeping the water temperature at 50 ℃, connecting a vacuum circulating pump by adopting a T-shaped three-way joint, steaming dry absolute ethyl alcohol for 1.2h under the stirring state, and drying for 12h under the vacuum conditions of-0.1 MPa and 60 ℃ to obtain solid powder; pouring the residual solid substance into an agate mortar for full grinding to prepare a catalyst precursor;
2) Calcining the catalyst precursor prepared in the step 1) in a nitrogen atmosphere with the flow of 20mL/min for pyrolysis, heating at the speed of 5 DEG/min at the temperature of 900 ℃, and calcining for 1h to obtain the cobalt nitrogen carbon non-noble metal catalyst. .
In order to prove the technical scheme provided by the application, the activity evaluation experiment and data of the cobalt nitrogen carbon non-noble metal catalyst provided by the application are given below.
100mg of the catalysts prepared in examples 1 to 5 were placed in a micro fixed bed reactor to perform the experiment under the following conditions: at room temperature (20 ℃), 20% of oxygen, 80% of nitrogen, bubbling of formaldehyde gas, blowing the formaldehyde gas into the reaction system through nitrogen, controlling the concentration of formaldehyde at the inlet of the reactor to be 50ppm, and controlling the reaction space velocity (GHSV) to be 60000 ml/(g.h) SV. After 12h of stable catalysis, the activity of each catalytic sample is as follows:
TABLE 1 BET specific surface area of cobalt carbon non-noble metal catalyst
Table 2 activity evaluation results of cobalt carbon non-noble metal catalysts.
| Sample (I) | Conversion of Formaldehyde at Room temperature (%) |
| Example 1 sample | 36.5 |
| Example 2 sample | 71.6 |
| Example 3 sample | 67.8 |
| Example 4 sample | 94.6 |
| Example 5 sample | 93.3 |
Claims (7)
1. The cobalt nitrogen carbon non-noble metal catalyst for removing formaldehyde at room temperature is characterized by consisting of carbon nitride doped cobalt simple substance and carbon carrier.
2. The cobalt nitrogen carbon non-noble metal catalyst for removing formaldehyde at room temperature as claimed in claim 1, wherein the mass ratio of the carbon nitride doped cobalt simple substance to the carbon carrier is 1: 7-10.
3. The cobalt nitrogen carbon non-noble metal catalyst for removing formaldehyde at room temperature according to claim 1, wherein the nitrogen-containing ligand is o-phenylenediamine and 1, 10-phenanthroline.
4. The Co-N-C non-noble metal catalyst for removing formaldehyde at room temperature as claimed in claim 1, wherein the carrier is activated carbon or carbon black.
5. The preparation method of the cobalt nitrogen carbon non-noble metal catalyst for removing formaldehyde at room temperature is characterized by comprising the following steps in sequence:
1) Preparation of catalyst precursor
Weighing cobalt acetate, nitrogen-containing ligand and carbon carrier according to the mass ratio of 1: 2-4: 2.5-3.5, sequentially adding the weighed cobalt acetate and nitrogen-containing ligand into absolute ethyl alcohol, and stirring for 0.2-1h at room temperature in a constant-temperature magnetic stirring instrument until the cobalt acetate, nitrogen-containing ligand and carbon carrier are fully dissolved to obtain a raw material solution; then introducing the weighed carbon carrier into the solution, heating to 50 ℃, fully stirring for 0.05-0.15h, and performing vacuum evaporation for 0.5-1.5h to obtain a catalyst precursor;
2) Calcination of
Calcining and pyrolyzing the catalyst precursor prepared in the step 1) in a nitrogen atmosphere to obtain the cobalt nitrogen carbon non-noble metal catalyst.
6. The preparation method of the cobalt nitrogen carbon non-noble metal catalyst for removing formaldehyde at room temperature according to claim 5, wherein the vacuum evaporation operation step in the step 1) is specifically: placing the triangular beaker filled with the solution into a constant-temperature water bath kettle, keeping the water temperature at 50 ℃, connecting a vacuum circulating pump by adopting a T-shaped three-way joint, evaporating absolute ethyl alcohol to dryness in a stirring state, and then carrying out vacuum drying to obtain solid powder; and pouring the residual solid substance into an agate mortar for full grinding to prepare the catalyst precursor.
7. The method for preparing the cobalt nitrogen carbon non-noble metal catalyst for removing formaldehyde at room temperature according to claim 5, wherein the calcination pyrolysis condition in the step 2) is under the protection of nitrogen, the temperature rise speed of the tubular furnace is 5 °/min, the calcination temperature is 300-900 ℃, the calcination time is 1h, and the nitrogen flow is 20mL/min.
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| CN115138388A (en) * | 2022-07-01 | 2022-10-04 | 中钢集团南京新材料研究院有限公司 | High-dispersity cobalt nitrogen carbon catalyst and preparation method thereof |
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