CN104324737B - A kind of integral normal-temperature Low Level Carbon Monoxide catalyst and preparation thereof and application - Google Patents
A kind of integral normal-temperature Low Level Carbon Monoxide catalyst and preparation thereof and application Download PDFInfo
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- CN104324737B CN104324737B CN201410616165.1A CN201410616165A CN104324737B CN 104324737 B CN104324737 B CN 104324737B CN 201410616165 A CN201410616165 A CN 201410616165A CN 104324737 B CN104324737 B CN 104324737B
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Abstract
The present invention relates to a kind of integral normal-temperature low concentration CO catalyst and preparation method thereof.This catalyst is with cordierite honeycomb ceramic as carrier, and the coating material back loading precious metals pd of coating bismuth oxide-containing is prepared from.Wherein cordierite honeycomb ceramic accounts for the mass percent of active coating is 5～20%, and precious metals pd content in integral catalyzer is 1.0～5.0 g/L.This integral catalyzer uses equi-volume impregnating to prepare, and preparation method is simple, and noble metal dosage is low and utilization rate is high, it is simple to heavy industrialization uses, at room temperature (0～40 DEG C), high-speed (～60000 h‑1), realize low concentration CO(0～50 ppm under the conditions of high humility (～100% RH)) effective elimination, it is adaptable in the hemi-closure space such as roads and tunnels or underground parking, the room temperature of low concentration CO eliminates.
Description
Technical field
The present invention relates to a kind of integral normal-temperature low concentration CO catalyst and preparation method thereof, Pu-Cu integral normal-temperature low concentration CO catalyst that a kind of bismuth oxide is modified and preparation method thereof.
Background technology
CO from commercial production and vehicle exhaust is the environmental contaminants that in air, a kind of content is more, and it can combine with the hemoglobin of human body, weakens the oxygen carrying capacity of hemoglobin, thus damages the central nervous system of people, causes people to be poisoned even dead.Carbon monoxide for volume low-concentration big present in environment, it is impossible to eliminate by the mode of physical absorption, becomes to pollute relatively low CO CO room-temperature catalytic oxidation2Be the most directly, simple, cheap and effectively eliminate the ways and means of CO in air.
Processing the pollutant in air and need bigger air speed, as used powder or granular catalyst, quickly can cause the blocking of beds, contaminated air is difficult to pass through beds so that catalytic reaction can not be carried out continuously.Integral catalyzer (monolithic
Catalysts) having the parallel channels that percent opening is bigger, the air contributing to big wind speed passes through, and CO contacts more uniform with catalyst simultaneously, and catalyst utilization is high, and the most industrial general employing integral catalyzer is for the catalytic reaction of gas.
The essential structure of integral catalyzer is made up of carrier, coating and active component three part.Conventional carrier is cordierite honeycomb ceramic, and carrier serves the effect of supporter.In order to increase the specific surface area of carrier, reduce active component consumption and make active component be more evenly distributed on carrier, need to coat last layer coating, the usually γ-Al of high-specific surface area at carrier surface2O3Or other oxides.The active component of the most conventional CO room-temperature catalytic oxidation is noble metal (Au, Pd, Pt) or non-precious metal catalyst (Hopcalite catalyst and Co3O4).
CN101612581B reports a kind of integral catalyzer that CO purifies in hydrogen-rich gas environment, and active component is Pt, and promoter is Ni, and carrier is coating α-Al2O3Mesopore-macropore carrier.Using volume impregnation method dipping active component is Pt and promoter is Ni on carrier.Carbon monoxide in hydrogen can be reduced to below 10ppm by this integral catalyzer.
CN102114428B reports a kind of for normal temperature oxidation CO, the integral catalyzer and preparation method thereof of formaldehyde, carrier is immersed in the precursor solution of complementary coating and the mixed liquor of main body coating sol, through purging, dry, calcining, then equi-volume impregnating is used, carrier is dipped in the nitrate solution mixed liquor of platinum acid chloride solution and chlorine palladium acid solution and auxiliary agent, is eventually adding reducing agent and prepares catalyst.This catalyst can eliminate CO and the formaldehyde of low concentration under normal temperature condition simultaneously, antitoxin, anti humility performance strong, stable performance.
Zhao Fuzhen et al. (Chinese Journal of Inorganic Chemistry, 2013,29(4)) have studied CuxCe1-xO2-x/ SBA-15/ the cordierite monolithic catalyst catalytic oxidation performance to CO, the catalysed reductive energy of catalyst surface and Cu0.5Ce0.5O1.5Certain relation, 50% Cu is had with the ratio of Cu, Ce0.5Ce0.5O1.5/ SBA-15/ cordierite monolithic catalyst has best catalysis activity, and CO can convert completely at 140 DEG C.
Summary of the invention
An object of the present invention is for the deficiencies in the prior art, it is provided that a kind of integral normal-temperature low concentration CO catalyst.
The two of the purpose of the present invention are to provide the preparation method of this catalyst.
A kind of integral normal-temperature Low Level Carbon Monoxide catalyst, it is characterised in that this catalyst is carrier, active coating and active component three part composition；It is 87～94.6% that described carrier accounts for the mass percent of catalyst, and described active coating is the γ-Al that bismuth oxide is modified2O3Coating, it is 5～10% that active coating accounts for the mass percent of catalyst；Described active component is Palladous chloride. and copper chloride, and it is 0.2～1% that Palladous chloride. accounts for the mass percent of catalyst, and it is 0.4～2% that copper chloride accounts for the mass percent of catalyst.
Described carrier is cordierite honeycomb ceramic, and hole density is 100～400 holes/square inch.
A kind of method preparing integral normal-temperature Low Level Carbon Monoxide catalyst, it is characterised in that concretely comprising the following steps of the method:
A. 23.2～92.8 grams of bismuth nitrate are dissolved in the salpeter solution that 1 liter of concentration is 0.1～1 mol/L, add 200 grams of γ-Al2O3Powder, is dried in 50～100 DEG C, 200～500 DEG C of Muffle kiln roastings 2～6 hours, i.e. obtains bismuth oxide modification γ-Al2O3Powder, bismuth oxide accounts for γ-Al2O3Mass percent be 5～20%；
B. the bismuth oxide modification γ-Al 50～200 grams of steps a obtained2O3Powder and 100～500g boehmites, 10～50 grams of isopropanols join in 500～1000 grams of deionized waters, furnishing pasty slurry, regulate the pH value of this slurry to 3-4 with the nitric acid of mass fraction 65%, i.e. obtain the coating material of bismuth oxide-containing；
C. cordierite honeycomb ceramic carrier be impregnated in coating material 1～5 minute, by clean for coating material purging unnecessary in duct after taking-up, 50～100 DEG C of baking ovens dry 1～5 hour, then 300～800 DEG C of Muffle kiln roastings 2～6 hours；
D. 0.20～1.00 gram of Palladous chloride. and 0.67～3.34 gram of copper chloride are dissolved in 20 milliliters of mass fractions be 5～20% ammonia spirit in, the coating that volume is 5cm × 5cm × 5cm is impregnated in the solution by the cordierite honeycomb ceramic of coating material, after solution fully absorbs, by integral catalyzer 100 DEG C of drying, then 200～500 DEG C of roastings 2～8 hours.
Described catalyst is at room temperature 0～40 DEG C, high-speed～60000 h-1, realize the catalysis oxidation of low concentration 0～50 ppm carbon monoxide under the conditions of high humility～100% RH, be particularly well-suited to the elimination of low concentration CO in the hemi-closure space such as roads and tunnels or underground parking.
The present invention utilizes bismuth oxide modification Pu-Cu integral normal-temperature low concentration CO catalyst, and this catalyst has at room temperature (0～40 DEG C), high-speed (～60000 h-1), realize low concentration CO(0～50 ppm under the conditions of high humility (～100% RH)) effective elimination, use equi-volume impregnating to prepare integral catalyzer, preparation method is simple, and noble metal utilisation is high, consumption is low, it is simple to heavy industrialization uses.
Detailed description of the invention
Hereinafter embodiments of the invention are elaborated: the present embodiment is implemented under premised on technical solution of the present invention, give detailed embodiment and concrete operating process, but protection scope of the present invention is not limited to following embodiment.
Comparative example:
By 10g γ-Al2O3Powder, 40g boehmite and 1.5g isopropanol join in 50g deionized water, add nitre acid for adjusting pH value and within 20 minutes, form coating material to 3-4, continuation stirring under stirring condition；Being immersed in by the cordierite honeycomb ceramic carrier weighed in coating material 5 minutes, after taking-up, high pressure air rifle purging, dries, 50 DEG C of drying, then at 550 DEG C of Muffle kiln roasting 4h.Being weighed, the load capacity of the active coating of cordierite honeycomb ceramic carrier is 17.5%.
By 0.52 g PdCl2With 1.67 g CuCl2It is dissolved in the ammonia that 20mL mass fraction is 20%, until completely dissolved, the cordierite honeycomb ceramic carrier of above-mentioned coating active coating is immersed in solution, after solution fully absorbs, by integral catalyzer 50 DEG C of drying, finally at 300 DEG C of Muffle kiln roasting 4h.Wherein the load capacity of Pd be the load capacity of 2.5g/L, Cu be 5g/L.
The integral catalyzer that this comparative example prepares carries out performance evaluation in atmospheric fixed bed U-shaped reactor (internal diameter is 11 mm), and reaction temperature is 30 DEG C, and CO concentration is 30 ppm, and remaining is air, and air speed is 24000 h-1, use carbonyl analyzer (Thermo, Model 48i) to carry out product analysis, the integral catalyzer that this comparative example prepares is 87.1% to the catalytic efficiency of CO.
Embodiment
1
:
Be impregnated in by activated alumina in bismuth nitrate solution, controlling bismuth oxide content is the 5% of total weight of carrier, is dried at 50 DEG C, then 300 DEG C of roastings 4 hours.
γ-the Al modified by 10g bismuth oxide2O3Powder, 40g boehmite and 1.5g isopropanol join in 50g deionized water, add nitre acid for adjusting pH value and within 20 minutes, form coating material to 3-4, continuation stirring under stirring condition；Being immersed in by the cordierite honeycomb ceramic carrier weighed in coating material 5 minutes, after taking-up, high pressure air rifle purging, dries, 50 DEG C of drying, then at 550 DEG C of Muffle kiln roasting 4h.Being weighed, the load capacity of the active coating of cordierite honeycomb ceramic carrier is 18.2%.
By 0.52 g PdCl2With 1.67 g CuCl2It is dissolved in the ammonia that 20mL mass fraction is 20%, until completely dissolved, the cordierite honeycomb ceramic carrier of above-mentioned coating active coating is immersed in solution, after solution fully absorbs, by integral catalyzer 50 DEG C of drying, finally at 300 DEG C of Muffle kiln roasting 4h.Wherein the load capacity of Pd be the load capacity of 2.5g/L, Cu be 5g/L.
The same comparative example of evaluating catalyst method.Test result shows, the integral catalyzer that this comparative example prepares is 89.5% to the catalytic efficiency of CO.
Embodiment
2
:
Making bismuth oxide content in embodiment 1 into 10%, remaining preparation method is with embodiment 1.The same comparative example of evaluating catalyst method.Test result shows, the integral catalyzer that the present embodiment prepares is 95.1% to the catalytic efficiency of CO.
Embodiment
3
:
Making bismuth oxide content in embodiment 1 into 15%, remaining preparation method is with embodiment 1.The same comparative example of evaluating catalyst method.Test result shows, the integral catalyzer that the present embodiment prepares is 92.4% to the catalytic efficiency of CO.
Embodiment
4
:
Making bismuth oxide content in embodiment 1 into 20%, remaining preparation method is with embodiment 1.The same comparative example of evaluating catalyst method.Test result shows, the integral catalyzer that the present embodiment prepares is 90.0% to the catalytic efficiency of CO.
Claims (2)
1. a preparation method for integral normal-temperature Low Level Carbon Monoxide catalyst,
Described catalyst is carrier, active coating and active component three part composition；It is 87～94.6% that described carrier accounts for the mass percent of catalyst, and described active coating is the γ-Al that bismuth oxide is modified2O3Coating, it is 5～10% that active coating accounts for the mass percent of catalyst；Described active component is Palladous chloride. and copper chloride, and it is 0.2～1% that Palladous chloride. accounts for the mass percent of catalyst, and it is 0.4～2% that copper chloride accounts for the mass percent of catalyst, it is characterised in that concretely comprising the following steps of the method:
A. 23.2～92.8 grams of bismuth nitrate are dissolved in the salpeter solution that 1 liter of concentration is 0.1～1 mol/L, add 200 grams of γ-Al2O3Powder, is dried in 50～100 DEG C, 200～500 DEG C of Muffle kiln roastings 2～6 hours, i.e. obtains bismuth oxide modification γ-Al2O3Powder, bismuth oxide accounts for γ-Al2O3Mass percent be 5～20%；
B. the bismuth oxide modification γ-Al 50～200 grams of steps a obtained2O3Powder and 100～500g boehmites, 10～50 grams of isopropanols join in 500～1000 grams of deionized waters, furnishing pasty slurry, regulate the pH value of this slurry to 3-4 with the nitric acid of mass fraction 65%, i.e. obtain the coating material of bismuth oxide-containing；
C. cordierite honeycomb ceramic carrier be impregnated in coating material 1～5 minute, by clean for coating material purging unnecessary in duct after taking-up, 50～100 DEG C of baking ovens dry 1～5 hour, then 300～800 DEG C of Muffle kiln roastings 2～6 hours；
D. 0.20～1.00 gram of Palladous chloride. and 0.67～3.34 gram of copper chloride are dissolved in 20 milliliters of mass fractions be 5～20% ammonia spirit in, the cordierite honeycomb ceramic being coated with coating material that volume is 5cm × 5cm × 5cm is impregnated in the solution, after solution fully absorbs, by integral catalyzer 100 DEG C of drying, then 200～500 DEG C of roastings 2～8 hours.
The catalyst that the preparation method of a kind of integral normal-temperature Low Level Carbon Monoxide catalyst obtainsApplication,It is characterized in that,At room temperature～40 DEG C, high-speed 60000 h-1, realize the catalysis oxidation of low concentration 50 ppm carbon monoxide under the conditions of high humility 100% RH,ForThe elimination of low concentration CO in roads and tunnels or underground parking hemi-closure space.
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| CN105268455A (en) * | 2015-11-09 | 2016-01-27 | 上海纳米技术及应用国家工程研究中心有限公司 | Preparation method for palladium-copper monolithic catalyst |
| CN106563467B (en) * | 2016-11-10 | 2019-06-21 | 上海纳米技术及应用国家工程研究中心有限公司 | A kind of monoblock type scavenging material and preparation and application for eliminating carbon monoxide in surrounding air |
| CN107376935B (en) * | 2017-07-19 | 2020-05-26 | 上海化工研究院有限公司 | A kind of monolithic catalyst for catalytic oxidation of CO at room temperature and preparation method thereof |
| CN116116431A (en) * | 2023-01-03 | 2023-05-16 | 万华化学集团股份有限公司 | Pd-Cu-X monolithic catalyst and preparation method and application thereof |
| CN116532114A (en) * | 2023-06-14 | 2023-08-04 | 山东源林硅瓷新材料有限公司 | Catalyst for carbon monoxide conversion and preparation method thereof |
| CN117299116B (en) * | 2023-08-25 | 2024-04-09 | 中节能(山东)催化剂有限公司 | Energy-saving carbon-reducing catalyst and preparation method thereof |
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