CN110038578A - The preparation of the co-modified cobaltosic oxide catalyst of nickel barium for vinyl chloride low-temperature catalytic burning and product and application - Google Patents
The preparation of the co-modified cobaltosic oxide catalyst of nickel barium for vinyl chloride low-temperature catalytic burning and product and application Download PDFInfo
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- CN110038578A CN110038578A CN201910472955.XA CN201910472955A CN110038578A CN 110038578 A CN110038578 A CN 110038578A CN 201910472955 A CN201910472955 A CN 201910472955A CN 110038578 A CN110038578 A CN 110038578A
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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
- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/70—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper
- B01J23/76—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper combined with metals, oxides or hydroxides provided for in groups B01J23/02 - B01J23/36
- B01J23/78—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper combined with metals, oxides or hydroxides provided for in groups B01J23/02 - B01J23/36 with alkali- or alkaline earth metals
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- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F23—COMBUSTION APPARATUS; COMBUSTION PROCESSES
- F23G—CREMATION FURNACES; CONSUMING WASTE PRODUCTS BY COMBUSTION
- F23G7/00—Incinerators or other apparatus for consuming industrial waste, e.g. chemicals
- F23G7/06—Incinerators or other apparatus for consuming industrial waste, e.g. chemicals of waste gases or noxious gases, e.g. exhaust gases
- F23G7/07—Incinerators or other apparatus for consuming industrial waste, e.g. chemicals of waste gases or noxious gases, e.g. exhaust gases in which combustion takes place in the presence of catalytic material
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- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F23—COMBUSTION APPARATUS; COMBUSTION PROCESSES
- F23G—CREMATION FURNACES; CONSUMING WASTE PRODUCTS BY COMBUSTION
- F23G2209/00—Specific waste
- F23G2209/14—Gaseous waste or fumes
- F23G2209/142—Halogen gases, e.g. silane
Abstract
The present invention discloses preparation method of a kind of co-modified cobaltosic oxide catalyst of the nickel barium for vinyl chloride low-temperature catalytic burning and products thereof and application.The catalyst is the co-modified Co of Ni and Ba3O4, it is 1:1-1:5 that wherein the molar ratio of Ni+Ba and Co, which is the molar ratio of 1:10-1:20, Ni and Ba,.Using urea as precipitating reagent, catalyst is prepared using hydro-thermal method, obtains catalyst of the present invention by two-step thermal processing, and wherein the ratio between the mole of urea and total metal ion (Co+Ni+Ba) are 2:1.The features such as method for preparing catalyst is simple, active high, by-product is few, stability is good for vinyl chloride catalysis burning, eliminates chloro volatile organic matter especially suitable for low-temperature catalytic burning.
Description
Technical field
The invention belongs to be catalyzed environmental technology field, and in particular to a kind of nickel barium for vinyl chloride low-temperature catalytic burning is total
Modify preparation method of cobaltosic oxide catalyst and products thereof and application.
Background technique
Vinyl chloride (VC) is since it is with high toxicity, high carcinogenic, and on October 27th, 2017, VC was by International Agency for Research on Cancer
It is classified as first kind carcinogen, while level-one carcinogen is also classified as by Environmental Protection Agency.Its danger to natural biology and human body
Evil is huge.Therefore, stringenter environmental legislation has been formulated for the discharge of VC in countries in the world, and the control and discharge to VC propose
Increasingly higher demands.But VC is widely used in industrial process as important intermediate, is difficult to realize from source
It fully controls.How to eliminate the discharge of VC pollutant in industrial processes is the major issue that Environmental Studies person are concerned about.By
Explosive mixture is formed with air in its high toxicity and high carcinogenic, and easily.It is catalyzed in worldwide about vinyl chloride at present
The research of burning is seldom.
Catalysis burns due to low operation temperature, eliminates the features such as pollutant concentration is wide, selectivity is high, it is considered to be eliminates low
One of concentration pollutant most efficient method.Being applied to the preferable catalyst of activity in vinyl chloride catalysis burning at present is Ru/
Co3O4Catalyst, it is negative that Guo et al. (CN201710446994, RSC Adv., 2016,6,99577) has studied different carriers
The catalytic combustion properties of vinyl chloride, result of study show Ru/Co on the noble ruthenium catalyst of load3O4Catalyst is low to vinyl chloride
Temperature catalysis burning shows higher activity and stability, and activity depends on Ru and Co3O4Between mutual synergistic effect.Such as
It is many for the activity of vinyl chloride catalysis burning that cobalt-base catalyst is further increased under the premise of where reducing catalyst cost
Researchers' concern.The present invention is by Co3O4Ba and Ni is introduced in lattice to improve catalytic activity simultaneously and solve chlorine
The problem of production during ethylene catalyst combustion reaction more chloro by-products.
Summary of the invention
For overcome the deficiencies in the prior art, the activity that cobalt-base catalyst is further increased on existing Research foundation, subtracts
The generation of more chloro by-products on few catalyst, it is an object of that present invention to provide a kind of nickel for vinyl chloride low-temperature catalytic burning
The preparation method of the co-modified cobaltosic oxide catalyst of barium.
Another object of the present invention is: providing a kind of nickel for vinyl chloride low-temperature catalytic burning of above method preparation
The co-modified cobaltosic oxide catalyst prod of barium.
Another object of the present invention is to: a kind of application of the said goods is provided.
The object of the invention is realized by following proposal: a kind of co-modified four oxygen of nickel barium for vinyl chloride low-temperature catalytic burning
The preparation method for changing three Co catalysts, using urea as precipitating reagent, catalyst is prepared using hydro-thermal method, is obtained by two-step thermal processing
Catalyst of the present invention, comprising the following steps:
(1) it weighs 2.16g urea and is dissolved in the aqueous solution of urea that compound concentration in 40ml water is 0.90mol/L;
(2) according to the molar ratio that the ratio between the mole of urea and total metal ion (Co+Ni+Ba) be 2:1, Ni+Ba and Co for (1:
10) molar ratio of-(1:20), Ni and Ba are (1:1)-(1:5), calculate the amount of cabaltous nitrate hexahydrate, weigh the six of certain mass
Nitric hydrate cobalt;
(3) it is 1 according to the molar ratio that the ratio between the mole of urea and total metal ion (Co+Ni+Ba) is 2:1, Ni+Ba and Co:
The molar ratio of (10-20) and Ni and Ba are 1:(1-5), the amount of Nickelous nitrate hexahydrate is calculated, six hydration nitre of certain mass are weighed
Sour nickel;
(4) it is 1 according to the molar ratio that the ratio between the mole of urea and total metal ion (Co+Ni+Ba) is 2:1, Ni+Ba and Co:
The molar ratio of (10-20) and Ni and Ba are 1:(1-5), the amount of barium nitrate is calculated, the barium nitrate of certain mass is weighed;
(5) cobalt nitrate/nickel nitrate weighed in step (2)/(3)/(4) and barium nitrate are dissolved in together in 40ml deionized water,
And 0.5h is stirred under room temperature, obtain nickel/barium/cobalt mixed solution;
(6) under conditions of stirring, the urea liquid prepared in step (1) is added dropwise to the mixed solution in step (5) dropwise
In and stir evenly;
(7) mixed solution in step (6) is transferred in 100ml water heating kettle, in 110-130 DEG C of hydro-thermal 6h;
(8) after the presoma obtained is washed with deionized 3-5 times, continue with ethanol washing 2-3 times;
(9) presoma obtained is dried overnight under the conditions of 60 DEG C;
(10) presoma after drying is ground uniformly, roasts 2-4h in 500-600 DEG C and obtains the catalyst.
The present invention provides a kind of co-modified cobaltosic oxide catalyst of the nickel barium for vinyl chloride low-temperature catalytic burning, this is urged
Agent is prepared using claim 1 the method, which is the co-modified Co of Ni and Ba3O4, wherein Ni+Ba and Co
Molar ratio be the molar ratio of 1:10-1:20, Ni and Ba be (1-5): 1, mole of urea and total metal ion (Co+Ni+Ba)
The ratio between amount is 2:1.
The present invention provides the application that a kind of co-modified cobaltosic oxide catalyst of nickel barium is used for vinyl chloride low-temperature catalytic burning.
Heretofore described catalyst and preparation method thereof compared to existing catalyst it is characterized in that: (1) catalyst
Using the co-modified Co of Ni and Ba3O4, catalytic oxidation activity is on the one hand improved, the life of more chloro by-products is on the other hand reduced
At;(2) catalyst of the present invention transition metal substitute noble metal, reduces catalyst cost.
Specific embodiment
Comparative example 1
A kind of preparation method of the co-modified cobaltosic oxide catalyst of nickel barium for vinyl chloride low-temperature catalytic burning, step is such as
Under:
(1) it weighs 2.16g urea and is dissolved in the aqueous solution of urea that compound concentration in 40ml water is 0.90mol/L;
(2) it weighs 5.24g cabaltous nitrate hexahydrate and is dissolved in the cobalt nitrate aqueous solution that compound concentration in 40ml water is 0.45mol/L, and
0.5h is stirred under room temperature;
(3) under conditions of stirring, the cobalt nitrate that the urea liquid prepared in step (1) is added dropwise to dropwise in step (2) is molten
In liquid and stir evenly;
(4) mixed solution in step (3) is transferred in 100ml water heating kettle, in 110oC-130 oC hydro-thermal 6h;
(5) after the presoma obtained is washed with deionized 3-5 times, continue with ethanol washing 2-3 times;
(6) presoma obtained is in 60oIt is dried overnight under the conditions of C;
(7) presoma after drying is ground uniformly, in 500 oCRoasting 4h obtains catalyst of the present invention, is denoted as
Co3O4;
Embodiment 2
A kind of co-modified cobaltosic oxide catalyst of nickel barium for vinyl chloride low-temperature catalytic burning is urged using urea as precipitating reagent
Agent is prepared using hydro-thermal method, is obtained catalyst of the present invention by two-step thermal processing, is prepared as follows:
(1) it weighs 2.16g urea and is dissolved in the aqueous solution of urea that compound concentration in 40ml water is 0.90mol/L;
(2) 4.76g cabaltous nitrate hexahydrate is weighed;
(3) according to the molar ratio that the ratio between the mole of urea and total metal ion (Co+Ni+Ba) be 2:1, Ni+Ba and Co for (1:
10) molar ratio of-(1:20), Ni and Ba are (1:1)-(1:5), weigh 0.24g Nickelous nitrate hexahydrate;
(4) it is 1 according to the molar ratio that the ratio between the mole of urea and total metal ion (Co+Ni+Ba) is 2:1, Ni+Ba and Co:
The molar ratio of (10-20) and Ni and Ba are 1:(1-5), the amount of barium nitrate is calculated, 0.21g barium nitrate is weighed;
(5) cobalt nitrate/nickel nitrate weighed in step (2)/(3)/(4) and barium nitrate are dissolved in together in 40ml deionized water,
And 0.5h is stirred under room temperature, obtain nickel/barium/cobalt mixed solution;
(6) under conditions of stirring, the urea liquid prepared in step (1) is added dropwise to the mixed solution in step (5) dropwise
In and stir evenly;
(7) mixed solution in step (6) is transferred in 100ml water heating kettle, in 110 DEG C of hydro-thermal reaction 6h;
(8) after the presoma obtained is washed with deionized 5 times, continue with ethanol washing 3 times;
(9) presoma obtained is dried overnight under the conditions of 60 DEG C;
(10) presoma after drying is ground uniformly, obtains catalyst of the present invention in 500 DEG C of roasting 4h, is denoted as Co10
(Ni1Ba1)。
Embodiment 3
A kind of co-modified cobaltosic oxide catalyst of nickel barium for vinyl chloride low-temperature catalytic burning, prepares as follows:
(1) it weighs 2.16g urea and is dissolved in the aqueous solution of urea that compound concentration in 40ml water is 0.90mol/L;
(2) 4.99g cabaltous nitrate hexahydrate is weighed;
(3) 0.12g Nickelous nitrate hexahydrate is weighed;
(4) 0.11g barium nitrate is weighed;
(5) cobalt nitrate/nickel nitrate weighed in step (2)/(3)/(4) and barium nitrate are dissolved in together in 40ml deionized water,
And 0.5h is stirred under room temperature, obtain nickel/barium/cobalt mixed solution;
(6) under conditions of stirring, the urea liquid prepared in step (1) is added dropwise to the mixed solution in step (5) dropwise
In and stir evenly;
(7) mixed solution in step (6) is transferred in 100ml water heating kettle, in 110 DEG C of hydro-thermal 6h;
(8) after the presoma obtained is washed with deionized 5 times, continue with ethanol washing 3 times;
(9) presoma obtained is dried overnight under the conditions of 60 DEG C;
(10) presoma after drying is ground uniformly, obtains catalyst of the present invention in 500 DEG C of roasting 4h, is denoted as Co20
(Ni1Ba1)。
Embodiment 4
A kind of co-modified cobaltosic oxide catalyst of nickel barium for vinyl chloride low-temperature catalytic burning, prepares as follows:
(1) it weighs 2.16g urea and is dissolved in the aqueous solution of urea that compound concentration in 40ml water is 0.90mol/L;
(2) 4.76g cabaltous nitrate hexahydrate is weighed;
(3) 0.40g Nickelous nitrate hexahydrate is weighed;
(4) 0.07g barium nitrate is weighed;
(5) cobalt nitrate/nickel nitrate weighed in step (2)/(3)/(4) and barium nitrate are dissolved in together in 40ml deionized water,
And 0.5h is stirred under room temperature, obtain nickel/barium/cobalt mixed solution;
(6) under conditions of stirring, the urea liquid prepared in step (1) is added dropwise to the mixed solution in step (5) dropwise
In and stir evenly;
(7) mixed solution in step (6) is transferred in 100ml water heating kettle, in 110 DEG C of hydro-thermal reaction 6h;
(8) after the presoma obtained is washed with deionized 5 times, continue with ethanol washing 3 times;
(9) presoma obtained is dried overnight under the conditions of 60 DEG C;
(10) presoma after drying is ground uniformly, in 500DEG C roasting 4h obtain catalyst of the present invention, be denoted as Co10
(Ni5Ba1)。
Embodiment 5
A kind of co-modified cobaltosic oxide catalyst of nickel barium for vinyl chloride low-temperature catalytic burning, prepares as follows:
(1) it weighs 2.16g urea and is dissolved in the aqueous solution of urea that compound concentration in 40ml water is 0.90mol/L;
(2) 4.99g cabaltous nitrate hexahydrate is weighed;
(3) 0.21g Nickelous nitrate hexahydrate is weighed;
(4) 0.04g barium nitrate is weighed;
(5) cobalt nitrate/nickel nitrate weighed in step (2)/(3)/(4) and barium nitrate are dissolved in together in 40ml deionized water,
And 0.5h is stirred under room temperature, obtain nickel/barium/cobalt mixed solution;
(6) under conditions of stirring, the urea liquid prepared in step (1) is added dropwise to the mixed solution in step (5) dropwise
In and stir evenly;
(7) mixed solution in step (6) is transferred in 100ml water heating kettle, in 110 DEG C of hydro-thermal 6h;
(8) after the presoma obtained is washed with deionized 5 times, continue with ethanol washing 3 times;
(9) presoma obtained is dried overnight under the conditions of 60 DEG C;
(10) presoma after drying is ground uniformly, obtains catalyst of the present invention in 500 DEG C of roasting 4h, is denoted as Co20
(Ni5Ba1)。
Catalyst activity test:
Catalyst in comparative example 1 and embodiment 2-5 is used for vinyl chloride catalysis burning, for urging used in vinyl chloride catalysis burning
Agent activity rating carries out in fixed-bed micro-reactor (internal diameter 3mm quartz ampoule), and the dosage of catalyst is 200mg, and temperature is adopted
It is automatically controlled with K type thermocouple.Vinyl chloride calibrating gas is mixed with air to burn into reactor.Total flow uses matter
Flowmeter control is measured, the concentration of vinyl chloride is 0.05 vol%, and air is carrier gas, oxygen concentration 10%, reaction temperature 140-500
DEG C, it is carried out under atmospheric pressure environment.The conversion ratio of vinyl chloride and the relationship of reaction temperature are shown in Table 1, T in table50%、T90%Respectively turn
Rate reaches reaction temperature required when 50%, 90%.Reaction end gas tracks online through chromatography, and key reaction product is HCl, two
Carbonoxide, water and minimal amount of trichloro ethylene.
The activity of vinyl chloride catalysis oxidation in 1 different catalysts of table
It can be seen that the catalyst of embodiment 2 ~ 4 in high reaction velocity from above-mentioned vinyl chloride catalytic oxidation activity result
(30,000 ml·g–1·h–1), show good vinyl chloride catalytic combustion activity in low and wide range of reaction temperature;Its
In, the most preferably catalyst Co of embodiment 320(Ni1Ba1), the catalyst is 235oVinyl chloride removal rate can reach when C
90.0% or more, 500ppm benzene concentration effectively can be dropped into 50ppm or less.And the Co modified using Ni and Ba3O4As chlorine
Ethylene catalytic oxidation catalyst greatly improves the activity of catalyst and reduces more chloro by-products.
Claims (3)
1. a kind of preparation method of the co-modified cobaltosic oxide catalyst of nickel barium for vinyl chloride low-temperature catalytic burning, feature
It is using urea as precipitating reagent, catalyst is prepared using hydro-thermal method, obtains catalyst of the present invention by two-step thermal processing, is wrapped
Include following steps:
(1) it weighs 2.16g urea and is dissolved in the aqueous solution of urea that compound concentration in 40ml water is 0.90mol/L;
(2) according to the molar ratio that the ratio between the mole of urea and total metal ion (Co+Ni+Ba) be 2:1, Ni+Ba and Co for (1:
10) molar ratio of-(1:20), Ni and Ba are (1:1)-(1:5), calculate the amount of cabaltous nitrate hexahydrate, weigh the six of certain mass
Nitric hydrate cobalt;
(3) it is 1 according to the molar ratio that the ratio between the mole of urea and total metal ion (Co+Ni+Ba) is 2:1, Ni+Ba and Co:
The molar ratio of (10-20) and Ni and Ba are 1:(1-5), the amount of Nickelous nitrate hexahydrate is calculated, six hydration nitre of certain mass are weighed
Sour nickel;
(4) it is 1 according to the molar ratio that the ratio between the mole of urea and total metal ion (Co+Ni+Ba) is 2:1, Ni+Ba and Co:
The molar ratio of (10-20) and Ni and Ba are 1:(1-5), the amount of barium nitrate is calculated, the barium nitrate of certain mass is weighed;
(5) cobalt nitrate/nickel nitrate weighed in step (2)/(3)/(4) and barium nitrate are dissolved in together in 40ml deionized water,
And 0.5h is stirred under room temperature, obtain nickel/barium/cobalt mixed solution;
(6) under conditions of stirring, the urea liquid prepared in step (1) is added dropwise to the mixed solution in step (5) dropwise
In and stir evenly;
(7) mixed solution in step (6) is transferred in 100ml water heating kettle, in 110-130 DEG C of hydro-thermal 6h;
(8) after the presoma obtained is washed with deionized 3-5 times, continue with ethanol washing 2-3 times;
(9) presoma obtained is dried overnight under the conditions of 60 DEG C;
(10) presoma after drying is ground uniformly, roasts 2-4h in 500-600 DEG C and obtains the catalyst.
2. a kind of co-modified cobaltosic oxide catalyst of nickel barium for vinyl chloride low-temperature catalytic burning, which is characterized in that this is urged
Agent is prepared using claim 1 the method, which is the co-modified Co of Ni and Ba3O4, wherein Ni+Ba and Co
Molar ratio be 1:(10-20), the molar ratio of Ni and Ba is (1-5): 1, mole of urea and total metal ion (Co+Ni+Ba)
The ratio between amount is 2:1.
3. the application that a kind of co-modified cobaltosic oxide catalyst of nickel barium is used for vinyl chloride low-temperature catalytic burning.
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Cited By (4)
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CN110560063A (en) * | 2019-09-09 | 2019-12-13 | 上海纳米技术及应用国家工程研究中心有限公司 | High-temperature stable supported cobaltosic oxide catalyst with core-shell structure and preparation method and application thereof |
CN111167458A (en) * | 2020-03-18 | 2020-05-19 | 上海纳米技术及应用国家工程研究中心有限公司 | Barium carbonate-promoted cobaltosic oxide catalyst for vinyl chloride low-temperature catalytic combustion degradation |
CN112452129A (en) * | 2020-12-14 | 2021-03-09 | 苏州大学 | Ternary NiO nanosheet @ bimetal CeCuOxMethod for low-temperature heat treatment of toluene by using microchip core-shell structure composite material |
CN112569962A (en) * | 2020-12-24 | 2021-03-30 | 上海纳米技术及应用国家工程研究中心有限公司 | Mn and Ba co-promoted cobaltosic oxide catalyst for low-temperature catalytic elimination of chlorohydrocarbon, and preparation and application thereof |
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CN112452129A (en) * | 2020-12-14 | 2021-03-09 | 苏州大学 | Ternary NiO nanosheet @ bimetal CeCuOxMethod for low-temperature heat treatment of toluene by using microchip core-shell structure composite material |
CN112569962A (en) * | 2020-12-24 | 2021-03-30 | 上海纳米技术及应用国家工程研究中心有限公司 | Mn and Ba co-promoted cobaltosic oxide catalyst for low-temperature catalytic elimination of chlorohydrocarbon, and preparation and application thereof |
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