CN104258875B - For the integral catalyzer of carbon monoxide room-temperature catalytic oxidation and preparation and application - Google Patents
For the integral catalyzer of carbon monoxide room-temperature catalytic oxidation and preparation and application Download PDFInfo
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- CN104258875B CN104258875B CN201410460882.XA CN201410460882A CN104258875B CN 104258875 B CN104258875 B CN 104258875B CN 201410460882 A CN201410460882 A CN 201410460882A CN 104258875 B CN104258875 B CN 104258875B
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- Y02A50/20—Air quality improvement or preservation, e.g. vehicle emission control or emission reduction by using catalytic converters
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Abstract
The present invention relates to a kind of integral catalyzer for carbon monoxide room-temperature catalytic oxidation and preparation thereof and application.This catalyst with coating active coating cordierite honeycomb ceramic as carrier, with PdCl2And CuCl2For active component, by equi-volume impregnating by PdCl2And CuCl2It is supported on carrier, after high-temperature roasting, obtains integral catalyzer.This integral catalyzer preparation method is simple, and noble metal utilisation is high, catalysis activity is high, service life is long, can be at room temperature (0 ~ 30 DEG C), low concentration (0 ~ 100 ppm), high-speed (10000 ~ 60000 h‑1CO catalytic oxidation under the conditions of), 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 catalyzer for CO room-temperature catalytic oxidation and preparation method thereof.This catalyst is applicable to room temperature (0 ~ 30 DEG C), low concentration (0 ~ 100 ppm), high-speed (10000 ~ 60000 h-1Under the conditions of), the catalysis oxidation of CO, is particularly well-suited to the elimination of low concentration CO in the hemi-closure space such as roads and tunnels or underground parking.
Background technology
Along with the continuous rising of automobile pollution, urban traffic blocking and parking difficulty problem are increasingly sharpened.The hemi-closure spaces such as road for development tunnel and underground parking are solutions currently mainly.But this kind of hemi-closure space inner air flow is poor, auto idle speed or cold start-up cause the pollutant of discharge constantly to accumulate in space, and pollutant levels exceed country's secondary air quality standard.In environment, the existence of CO has the biggest hazardness, 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.
At present the removing method of CO is mainly based on catalytic oxidation, and the method is because having efficiency height, non-secondary pollution, the advantage such as applied widely, it has also become currently CO improvement area research and the mainstream development direction of application.CO catalyst can be divided into non-precious metal catalyst system and the big class of noble metal catalyst system two.Nonmetal CO catalyst mainly Hopcalite catalyst with CuO-MnOx composite oxides as main component (G.J. Hutchingsa, et. al.,
Appl. Catal. A 1998,166:143-152.) it is representative, it is used in mine and military gas-mask always.Although Hopcalite catalyst activity is high, but containing in vapour atmosphere, understand fast deactivation.Support type Waker-Typer catalyst (PdCl in noble metal catalyst system2–CuCl2) (Chinese invention patent CN101898137A) have the highest catalytic performance at ambient temperature, and have good water-resistance and service life CO, but relatively costly.
Vehicle tail gas triple effect catalyst (Three-way catalyst, TWCs) is that the noble-metal-supporteds such as Pd, Pt and Rh are being coated with γ-Al2O3Or on the honeycomb ceramic carrier of cerium Zirconium oxide, the tail gas that can produce during normally being exercised by automobile is converted into harmless products, but it uses temperature high, need to reach 300-900 DEG C, it is impossible to the elimination of pollutant under room temperature；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, CO can convert completely at 140 DEG C, it is impossible under normal temperature condition, the catalysis to CO aoxidizes；Chinese invention patent CN 102114428 B discloses for normal temperature oxidation CO, the integral catalyzer and preparation method thereof of formaldehyde, CO and formaldehyde can be eliminated under normal temperature condition simultaneously, antitoxin, anti humility performance is strong, stable performance, but does not the most mention service life.
Summary of the invention
For overcoming the deficiencies in the prior art, the present invention provides a kind of integral catalyzer for carbon monoxide room-temperature catalytic oxidation and preparation and application.
A kind of integral catalyzer for carbon monoxide room-temperature catalytic oxidation, it is characterised in that described catalyst carrier is the cordierite honeycomb ceramic of coating active coating；Active component is Palladous chloride. (PdCl2) and copper chloride (CuCl2)；Wherein PdCl2In Pd content in integral catalyzer be 1.0 ~ 3.0 g/L, CuCl2In Cu content in integral catalyzer be 2.0 ~ 10 g/L；It is 5 ~ 20% that active coating load capacity accounts for the mass percent at cordierite honeycomb ceramic.
The preparation method of the integral catalyzer of carbon monoxide room-temperature catalytic oxidation, it is characterised in that comprise the following steps:
(1) carrier need to coat one layer of active coating in advance:
By boehmite, γ-Al2O3Powder, isopropanol join in deionized water, add nitre acid for adjusting pH value and within 10-60 minute, form slurry to 3-4, continuation stirring under stirring condition；Being soaked by cordierite honeycomb ceramic carrier 1-15 minute in the slurry, after taking-up, high pressure air rifle purging, dries, and 30～80 DEG C of drying, then 200 ~ 800 DEG C of Muffle kiln roastings 4 hours, obtains the cordierite honeycomb ceramic of coating active coating；
(2) equi-volume impregnating is used to prepare integral catalyzer:
By PdCl2And CuCl2It is dissolved in ammonia spirit, the cordierite honeycomb ceramic of coating active coating is impregnated in the solution, after solution fully absorbs, by integral catalyzer 30～80 DEG C of drying, then 200～500 DEG C of roastings 2～8 hours.
Step (2) described equi-volume impregnating is: measured in advance is coated with the water absorption rate of the cordierite honeycomb ceramic of active coating, then adds, according to water absorption rate, the PdCl that saturated absorption is volume required2-CuCl2Ammonia spirit.
The catalysis oxidation of the integral catalyzer of carbon monoxide room-temperature catalytic oxidation carbon monoxide under the conditions of room temperature, low concentration, high-speed, is particularly well-suited to the elimination of Low Level Carbon Monoxide in the hemi-closure space such as roads and tunnels or underground parking.
Compared with the prior art, the substantive features that the present invention has are: integrated catalyst carrier mechanical strength is high, meets engineering construction requirement；Can at normal temperatures (0 ~ 30 DEG C) realize low concentration CO(0 ~ 100 ppm) effective elimination；Can be used for high-speed (10000 ~ 60000 h-1) condition；Good water-resistance and halogen-resistant poison ability；Active coating accounts for vector contg controlled (5 ~ 20%)；Using 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.
This integral catalyzer preparation method is simple, and noble metal utilisation is high, catalysis activity is high, service life is long, can be at room temperature (0 ~ 30 DEG C), low concentration (0 ~ 100 ppm), high-speed (10000 ~ 60000 h-1CO catalytic oxidation under the conditions of), it is adaptable in the hemi-closure space such as roads and tunnels or underground parking, the room temperature of low concentration CO eliminates.
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.
Embodiment
1
:
The coating of cordierite honeycomb ceramic carrier: by 40g boehmite, 10g γ-Al2O3Powder, 1.5g isopropanol join in 50g deionized water, add nitre acid for adjusting pH value and within 20 minutes, form slurry to 3-4, continuation stirring under stirring condition；Being soaked 5 minutes in the slurry by the cordierite honeycomb ceramic carrier that volume is 5cm × 5cm × 5cm, 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%.
The preparation of 2.5g/L Pd integral catalyzer: by 0.52 g PdCl2With 1.67 g CuCl2It is dissolved in 20mL strong aqua ammonia, until completely dissolved, the cordierite honeycomb ceramic carrier of the 5cm × 5cm × 5cm 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.
Evaluating catalyst method: the reaction of CO normal temperature oxidation is carried out performance evaluation in atmospheric fixed bed U-shaped reactor (internal diameter is 11 mm).Raw materials used gas component is: CO concentration is 20 ppm, and remaining is air, and total flow is 1 L/min.It is 1cm that integral catalyzer is cut into floor space2, for the cylinder of 2.5cm, (volume is 2.5cm to height3), corresponding volume air speed is 24000h-1.Atmospheric fixed bed U-shaped reactor is placed in 30 DEG C of constant temperature water baths, and unstrpped gas directly passes through beds.Using carbonyl analyzer (Thermo, Model 48i) to carry out product analysis, the lowest detection of instrument is limited to 0.04 ppm.
Test result shows, at 24000h-1Under volume space velocity, 2.5g/L Pd integral catalyzer (17.5% active coating load capacity) is 87.1% to the initial purge efficiency of CO, and catalyst uses 50h after-purification efficiency to be 83.8%.
Embodiment
2
:
The coating of cordierite honeycomb ceramic carrier is with embodiment 1.
The preparation of 2.0g/L Pd integral catalyzer: by the PdCl in embodiment 12Quality changes 0.42g into, and remaining preparation method is with embodiment 1.
Evaluating catalyst method is with embodiment 1.Test result shows, 2.0g/L Pd integral catalyzer (17.5% active coating load capacity) is 82.9% to the initial purge efficiency of CO, and catalyst uses 50h after-purification efficiency to be 78.3%.
Embodiment
3
:
The coating of cordierite honeycomb ceramic carrier is with embodiment 1.
The preparation of 1.5g/L Pd integral catalyzer: by the PdCl in embodiment 12Quality changes 0.31g into, and remaining preparation method is with embodiment 1.
Evaluating catalyst method is with embodiment 1.Test result shows, 1.5g/L Pd integral catalyzer (17.5% active coating load capacity) is 74.3% to the initial purge efficiency of CO, and catalyst uses 50h after-purification efficiency to be 67.6%.
Embodiment
4
:
The coating of cordierite honeycomb ceramic carrier: making the deionized water quality in embodiment 1 into 100g, remaining preparation method is with embodiment 1.Being weighed, the load capacity of the active coating of cordierite honeycomb ceramic carrier is 12.0%.
The preparation of 2.5g/L Pd integral catalyzer: the cordierite honeycomb ceramic carrier of 17.5% active coating load capacity in embodiment 1 makes into the cordierite honeycomb ceramic carrier of 12.0% active coating load capacity, and remaining preparation method is with embodiment 1.
Evaluating catalyst method is with embodiment 1.Test result shows, 2.5g/L Pd integral catalyzer (12.0% active coating load capacity) is 85.6% to the initial purge efficiency of CO, and catalyst uses 50h after-purification efficiency to be 81.2%.
Embodiment
5
:
The coating of cordierite honeycomb ceramic carrier is with embodiment 4.
The preparation of 2.0g/L Pd integral catalyzer: the cordierite honeycomb ceramic carrier of 17.5% active coating load capacity in embodiment 2 makes into the cordierite honeycomb ceramic carrier of 12.0% active coating load capacity, and remaining preparation method is with embodiment 2.
Evaluating catalyst method is with embodiment 1.Test result shows, 2.0g/L Pd integral catalyzer (12.0% active coating load capacity) is 81.7% to the initial purge efficiency of CO, and catalyst uses 50h after-purification efficiency to be 76.7%.
Embodiment
6
:
The coating of cordierite honeycomb ceramic carrier is with embodiment 4.
The preparation of 1.5g/L Pd integral catalyzer: the cordierite honeycomb ceramic carrier of 17.5% active coating load capacity in embodiment 3 makes into the cordierite honeycomb ceramic carrier of 12.0% active coating load capacity, and remaining preparation method is with embodiment 3.
Evaluating catalyst method is with embodiment 1.Test result shows, 1.5g/L Pd integral catalyzer (12.0% active coating load capacity) is 72.2% to the initial purge efficiency of CO, and catalyst uses 50h after-purification efficiency to be 65.8%.
Claims (4)
1. being used for a preparation method for the integral catalyzer of carbon monoxide room-temperature catalytic oxidation, described catalyst carrier is the cordierite honeycomb ceramic of coating active coating；Active component is Palladous chloride. PdCl2With copper chloride CuCl2；Wherein PdCl2In Pd content in integral catalyzer be 1.0 ~ 3.0 g/L, CuCl2In Cu content in integral catalyzer be 2.0 ~ 10 g/L；It is 5 ~ 20% that active coating load capacity accounts for the mass percent at cordierite honeycomb ceramic, it is characterised in that comprise the following steps:
(1) carrier need to coat one layer of active coating in advance:
By boehmite, γ-Al2O3Powder, isopropanol join in deionized water, add nitre acid for adjusting pH value and within 10-60 minute, form slurry to 3-4, continuation stirring under stirring condition；Being soaked by cordierite honeycomb ceramic carrier 1-15 minute in the slurry, after taking-up, high pressure air rifle purging, dries, and 30～80 DEG C of drying, then 200 ~ 800 DEG C of Muffle kiln roastings 4 hours, obtains the cordierite honeycomb ceramic of coating active coating；
(2) equi-volume impregnating is used to prepare integral catalyzer:
By PdCl2And CuCl2It is dissolved in ammonia spirit, the cordierite honeycomb ceramic of coating active coating is impregnated in the solution, after solution fully absorbs, by integral catalyzer 30～80 DEG C of drying, then 200～500 DEG C of roastings 2～8 hours.
It is used for the preparation method of the integral catalyzer of carbon monoxide room-temperature catalytic oxidation the most according to claim 1, it is characterized in that, step (2) described equi-volume impregnating is: measured in advance is coated with the water absorption rate of the cordierite honeycomb ceramic of active coating, then adds, according to water absorption rate, the PdCl that saturated absorption is volume required2-CuCl2Ammonia spirit.
The application of the catalyst obtained for the preparation method of the integral catalyzer of carbon monoxide room-temperature catalytic oxidation the most according to claim 1, it is characterised in that for room temperature, low concentration 0 ~ 100 ppm, high-speed 10000 ~ 60000 h-1Under the conditions of carbon monoxide catalysis oxidation.
The application of the catalyst obtained for the preparation method of the integral catalyzer of carbon monoxide room-temperature catalytic oxidation the most according to claim 3, it is characterised in that the elimination of Low Level Carbon Monoxide in roads and tunnels or underground parking hemi-closure space.
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Families Citing this family (9)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN105126866A (en) * | 2015-07-10 | 2015-12-09 | 上海纳米技术及应用国家工程研究中心有限公司 | Preparation method of monolithic CO normal-temperature catalyst |
| CN105126865A (en) * | 2015-07-10 | 2015-12-09 | 上海纳米技术及应用国家工程研究中心有限公司 | Low-loading-quantity high-effective palladium-copper monolithic catalyst and preparation method of same |
| CN105413708B (en) * | 2015-11-09 | 2017-12-05 | 上海纳米技术及应用国家工程研究中心有限公司 | A kind of preparation method of low concentration air pollutants scavenging material |
| 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 |
| CN106955681A (en) * | 2017-03-21 | 2017-07-18 | 中山大学惠州研究院 | A kind of preparation method of integral catalyzer for purifying formaldehyde |
| CN111135835B (en) * | 2019-12-17 | 2023-04-07 | 安徽元琛环保科技股份有限公司 | Carbon monoxide catalytic oxidation catalyst and preparation method and application thereof |
| CN111013583A (en) * | 2019-12-20 | 2020-04-17 | 萍乡学院 | Preparation method of monolithic catalyst for efficiently decomposing carbon monoxide at room temperature |
| CN114570435A (en) * | 2020-11-30 | 2022-06-03 | 中大汇智源创(北京)科技有限公司 | Honeycomb catalyst and preparation method and application 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 |
Citations (2)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN101898137A (en) * | 2010-07-22 | 2010-12-01 | 华东理工大学 | Pd-Cu catalyst for CO low-temperature oxidation and preparation method thereof |
| CN103170348A (en) * | 2011-12-22 | 2013-06-26 | 上海纳米技术及应用国家工程研究中心有限公司 | Silver-containing normal-temperature monolithic catalyst for carbon monoxide and preparation method thereof |
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| US9044734B2 (en) * | 2011-09-23 | 2015-06-02 | Basf Se | Diesel oxidation catalyst with layered structure containing ceria composition as palladium support material for enhanced HC and CO gas conversion |
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| Publication number | Priority date | Publication date | Assignee | Title |
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| CN101898137A (en) * | 2010-07-22 | 2010-12-01 | 华东理工大学 | Pd-Cu catalyst for CO low-temperature oxidation and preparation method thereof |
| CN103170348A (en) * | 2011-12-22 | 2013-06-26 | 上海纳米技术及应用国家工程研究中心有限公司 | Silver-containing normal-temperature monolithic catalyst for carbon monoxide and preparation method thereof |
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