CN104014358A - Supported catalyst eliminating carbon monoxide at room temperature, and preparation method and application thereof - Google Patents
Supported catalyst eliminating carbon monoxide at room temperature, and preparation method and application thereof Download PDFInfo
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- CN104014358A CN104014358A CN201410229423.0A CN201410229423A CN104014358A CN 104014358 A CN104014358 A CN 104014358A CN 201410229423 A CN201410229423 A CN 201410229423A CN 104014358 A CN104014358 A CN 104014358A
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- room temperature
- carbon monoxide
- catalyst
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02A—TECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE
- Y02A50/00—TECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE in human health protection, e.g. against extreme weather
- Y02A50/20—Air quality improvement or preservation, e.g. vehicle emission control or emission reduction by using catalytic converters
Abstract
The invention relates to a supported catalyst eliminating carbon monoxide at room temperature, and a preparation method and application thereof. The catalyst employs palladium chloride and cupric chloride as active compositions and employs a vinyl-modified mesoporous foam-like molecular sieve as a carrier. The mass percent of palladium chloride is 1-3%, the mass percent of CuCl2 is 5-10%, and the balance is the carrier. Palladium chloride and cupric chloride are supported on the carrier through a dipping method, the catalytic performance of the catalyst is improved by utilizing the interaction of the carrier and palladium chloride-cupric chloride, and the catalyst helps to realize catalytic elimination of carbon monoxide under the conditions of normal temperature, low concentration and high space velocity.
Description
Technical field
The present invention relates to a kind of room temperature and eliminate loaded catalyst of carbon monoxide and its preparation method and application, particularly for room temperature (0 ~ 30 ℃), low concentration (0 ~ 200 ppm), high-speed 30000 ~ 100000 mL/ (gh)) loaded catalyst and preparation method thereof of carbon monoxide catalytic oxidation under condition.
Background technology
CO enter after human body can and blood in hemoglobin combine, generation carbonyl haemoglobin, make hemoglobin can not with combination with oxygen, thereby cause that anoxic appears in body tissue, cause human body death by suffocation, so CO has toxicity.Under usual condition, CO is colourless, odorless, tasteless gas, therefore be easy to ignore, causes poisoning.When airborne CO concentration reaches 200 ppm, normal adults, after 2~3 hours, just there will be slight headache, weak; When reaching 400 ppm, in normal adults 1~2 hour before metopodynia, life-threatening after 3 hours; While reaching 12800 ppm, just dead in normal adults 1~3 minute.Therefore, exploitation efficiently, CO Oxidation at room temperature catalyst has stronger use value cheaply.
Pd loaded catalyst adopts traditional infusion process preparation conventionally, and preparation technology is simple, at normal temperatures CO is eliminated and has higher activity.Shen etc. adopt NH
3pd-Cu-Cl prepared by complexing infusion process
x/ Al
2o
3catalyst series is load Wacker catalyst, in the time of-30 ℃, just can make the CO of 400-1000 ppm transform completely (Y. Shen, et. al., Catal. Commun., 2010,46,8433-8435).Therefore, support type Wacker catalyst has good application prospect in the reaction of CO low-temperature oxidation.
Mesoporous foam shape molecular sieve (mesocellular foam silica, MCFs) is the mesopore silicon oxide of a kind of 3D of having meso-hole structure and ultra-large aperture.This structure is a kind of cellular mesopore foaming structure of novelty, and its spherical pore is to be communicated with and to be become three-dimensional structure by the window of homogeneous, and its pore volume is 1.0-2.4cm
3/ g, aperture between 16-42 nm, specific area 400 ~ 700 cm
2/ g, and can adjust duct parameter by adjusting composition and the reaction condition of template.Therefore MCFs is a kind of ideal catalyst carrier.By surface-functionalized processing, change molecular sieve surface nature, can improve the interaction between carrier and active component, can make active component be evenly distributed in carrier surface simultaneously, with this, improve the whole catalytic performance of catalyst.
Summary of the invention
For overcoming the deficiencies in the prior art, the invention provides a kind of room temperature and eliminate loaded catalyst of carbon monoxide and its preparation method and application.
Room temperature is eliminated a loaded catalyst for carbon monoxide, it is characterized in that, it is active component that described catalyst be take palladium bichloride and copper chloride, and the mesoporous foam shape molecular sieve after vinyl modified is carrier; Wherein the mass percent of palladium bichloride is 1~3%, CuCl
2mass percent be 5~10%, surplus is carrier.
Room temperature is eliminated a preparation method for the loaded catalyst of carbon monoxide, it is characterized in that, comprises the following steps:
(1) mesoporous foam shape molecular sieve is dissolved in hydrochloric acid solution, add ammonium fluoride and trimethylbenzene, after stirring, add ethyl orthosilicate and VTES, at 20~40 ℃, continue to stir after 12~24 hours, solution is proceeded in crystallizing kettle, and be placed in the baking oven of 90~120 ℃ and process 24 hours; Be cooled to after room temperature, by deionized water and ethanol filtering and washing, then gained white solid is joined in the ethanol solution hydrochloride of 60 ℃, stir washing and filtering after 2 hours, after crossing 50~80 ℃ of oven dryings, obtain the mesoporous foam shape molecular sieve carrier after vinyl modified;
(2) palladium bichloride and copper chloride are dissolved in ammonia spirit, under the condition stirring, add the mesoporous foam shape molecular sieve carrier after the vinyl modified that step (1) makes, at 30~80 ℃, naturally dry, then 200~500 ℃ of roastings 2~8 hours, obtain the loaded catalyst that room temperature is eliminated carbon monoxide.
The molar fraction that the described VTES of step (1) accounts for total silicon source is 5~20%.
Room temperature is eliminated the loaded catalyst of carbon monoxide for the catalytic oxidation of carbon monoxide under normal temperature, low concentration, high-speed condition.
Compared with prior art, one of remarkable advantage that a kind of room temperature of the present invention is eliminated the loaded catalyst of CO is, can realize low concentration CO(0 ~ 200 ppm at room temperature (0 ~ 30 ℃), high-speed (30000 ~ 100000 mL/ (gh))) effective elimination.
Two of the remarkable advantage of the loaded catalyst of a kind of room temperature elimination CO of the present invention is, utilizes carrier and PdCl
2-CuCl
2between interaction improve the catalytic performance of catalyst.
Three of the remarkable advantage of the loaded catalyst of a kind of room temperature elimination CO of the present invention is, employing preparation catalyst, and preparation method is simple, and noble metal dosage is low, and cost is low.
The specific embodiment
Following instance is used for illustrating in greater detail the present invention, but the present invention is not limited to this.
Comparative example:
4.00 g P123 are dissolved in the HCl solution of 150 mL 1.6 mol/L, after P123 dissolves completely, add 0.046 g NH
4f and 6.00 g trimethylbenzenes, be then warming up to solution 35 ℃ and continue to stir after 1 hour, adds 8.8 g ethyl orthosilicates, continues to stir after 20 hours at 35 ℃, solution proceeded in crystallizing kettle, and be placed in the baking oven of 100 ℃ and process 24 hours.After solution is cooled to room temperature, filters and obtain white solid, dry after 24 hours in the baking oven of 100 ° of C, white solid is put into Muffle furnace Program and be warming up to 550 ℃ of roastings 6 hours.Naturally cool to after room temperature the white powder MCFs obtaining.
By 0.033 g PdCl
2with 0.159 g CuCl
22H
2o is dissolved in 4 mL concentrated ammonia liquors, adds the MCFs carrier of 2 g under the condition stirring, and at 50 ℃, naturally dries, and then 300 ℃ of roastings, within 6 hours, obtains PdCl
2-CuCl
2/ MCFs catalyst.
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 5 mm).Raw materials used gas component is: CO concentration is 200 ppm, and all the other are air, and total flow is 500 mL/min, and catalyst quality is 0.3 g, and corresponding air speed is 100000 mL/ (gh).Atmospheric fixed bed U-shaped reactor is placed in 30 ℃ of constant temperature water baths, and unstrpped gas is directly passed through beds.Use CO analyzer (Thermo, Model 48i) to carry out product analysis, the lowest detection of instrument is limited to 0.04 ppm.
Test result shows, uses the CO conversion ratio of catalyst prepared by this method to be up to 53.6%.
Embodiment 1:
4.00 g P123 are dissolved in the HCl solution of 150 mL 1.6 mol/L, after P123 dissolves completely, add 0.046 g NH
4f and 6.00 g trimethylbenzenes, then solution is warming up to 35 ℃ and lasting stirring after 1 hour, adds 8.36 g ethyl orthosilicates and 0.40 g VTES, at 35 ℃, continue to stir after 20 hours, solution is proceeded in crystallizing kettle, and be placed in the baking oven of 100 ℃ and process 24 hours.After solution is cooled to room temperature, filter and obtain white solid, then white solid is joined in the ethanol solution hydrochloride of 60 ℃, stirs washing and filtering after 6 hours, finally by 100 ° of C oven dryings of mistake, after 24 hours, obtain V-MCFs-5%.
By 0.033g PdCl
2with 0.159g CuCl
22H
2o is dissolved in 4 mL concentrated ammonia liquors, adds the V-MCFs-5% carrier of 2 g under the condition stirring, and at 50 ℃, naturally dries, and then 300 ℃ of roastings, within 6 hours, obtains PdCl
2-CuCl
2/ V-MCFs-5% catalyst.
Evaluating catalyst method is with embodiment 1.Test result shows, the PdCl that uses this method to prepare
2-CuCl
2the CO conversion ratio of/V-MCFs-5% catalyst is up to 63.9%.
Embodiment 2:
Change the quality of ethyl orthosilicate and VTES in embodiment 2 into 7.92 g and 0.80 g, all the other preparation methods are with embodiment 2.
Evaluating catalyst method is with embodiment 1.Test result shows, the PdCl that uses this method to prepare
2-CuCl
2the CO conversion ratio of/V-MCFs-10% catalyst is up to 71.2%.
Embodiment 3:
Change the quality of ethyl orthosilicate and VTES in embodiment 2 into 7.48 g and 1.20 g, all the other preparation methods are with embodiment 2.
Evaluating catalyst method is with embodiment 1.Test result shows, the PdCl that uses this method to prepare
2-CuCl
2the CO conversion ratio of/V-MCFs-15% catalyst is up to 74.3%.
Embodiment 4:
Change the quality of ethyl orthosilicate and VTES in embodiment 2 into 7.04 g and 1.60 g, all the other preparation methods are with embodiment 2.
Evaluating catalyst method is with embodiment 1.Test result shows, the PdCl that uses this method to prepare
2-CuCl
2the CO conversion ratio of/V-MCFs-20% catalyst is up to 68.0%.
Claims (4)
1. room temperature is eliminated a loaded catalyst for carbon monoxide, it is characterized in that, it is active component that described catalyst be take palladium bichloride and copper chloride, and the mesoporous foam shape molecular sieve after vinyl modified is carrier; Wherein the mass percent of palladium bichloride is 1~3%, CuCl
2mass percent be 5~10%, surplus is carrier.
2. room temperature is eliminated the preparation method of the loaded catalyst of carbon monoxide according to claim 1, it is characterized in that, comprises the following steps:
(1) mesoporous foam shape molecular sieve is dissolved in hydrochloric acid solution, add ammonium fluoride and trimethylbenzene, after stirring, add ethyl orthosilicate and VTES, at 20~40 ℃, continue to stir after 12~24 hours, solution is proceeded in crystallizing kettle, and be placed in the baking oven of 90~120 ℃ and process 24 hours; Be cooled to after room temperature, by deionized water and ethanol filtering and washing, then gained white solid is joined in the ethanol solution hydrochloride of 60 ℃, stir washing and filtering after 2 hours, after crossing 50~80 ℃ of oven dryings, obtain the mesoporous foam shape molecular sieve carrier after vinyl modified;
(2) palladium bichloride and copper chloride are dissolved in ammonia spirit, under the condition stirring, add the mesoporous foam shape molecular sieve carrier after the vinyl modified that step (1) makes, at 30~80 ℃, naturally dry, then 200~500 ℃ of roastings 2~8 hours, obtain the loaded catalyst that room temperature is eliminated carbon monoxide.
3. room temperature is eliminated the preparation method of the loaded catalyst of carbon monoxide according to claim 2, it is characterized in that, the molar fraction that the described VTES of step (1) accounts for total silicon source is 5~20%.
4. room temperature is eliminated the loaded catalyst of carbon monoxide for the catalytic oxidation of carbon monoxide under normal temperature, low concentration, high-speed condition according to claim 1.
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Cited By (2)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
CN107876095A (en) * | 2017-11-22 | 2018-04-06 | 成都新柯力化工科技有限公司 | A kind of Metal Porous-Organic material and preparation method for indoor air purification |
CN108906117A (en) * | 2018-07-06 | 2018-11-30 | 郑州三希新材料科技有限公司 | A kind of material for air purification of novel visible color change and preparation method thereof |
Citations (3)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
CN101864410A (en) * | 2010-04-16 | 2010-10-20 | 华东理工大学 | Epoxy mesoporous molecular sieve for use in bio-enzyme immobilization and preparation method thereof |
CN103055907A (en) * | 2013-01-25 | 2013-04-24 | 华东理工大学 | High-water resistance catalyst for low-temperature oxidization of CO (Carbon Monoxide) and preparation method thereof |
CN103736511A (en) * | 2013-12-25 | 2014-04-23 | 上海纳米技术及应用国家工程研究中心有限公司 | Catalyst for carbon monoxide normal-temperature catalytic and oxidation as well as preparation method and application |
-
2014
- 2014-05-28 CN CN201410229423.0A patent/CN104014358B/en not_active Expired - Fee Related
Patent Citations (3)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
CN101864410A (en) * | 2010-04-16 | 2010-10-20 | 华东理工大学 | Epoxy mesoporous molecular sieve for use in bio-enzyme immobilization and preparation method thereof |
CN103055907A (en) * | 2013-01-25 | 2013-04-24 | 华东理工大学 | High-water resistance catalyst for low-temperature oxidization of CO (Carbon Monoxide) and preparation method thereof |
CN103736511A (en) * | 2013-12-25 | 2014-04-23 | 上海纳米技术及应用国家工程研究中心有限公司 | Catalyst for carbon monoxide normal-temperature catalytic and oxidation as well as preparation method and application |
Cited By (2)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
CN107876095A (en) * | 2017-11-22 | 2018-04-06 | 成都新柯力化工科技有限公司 | A kind of Metal Porous-Organic material and preparation method for indoor air purification |
CN108906117A (en) * | 2018-07-06 | 2018-11-30 | 郑州三希新材料科技有限公司 | A kind of material for air purification of novel visible color change and preparation method thereof |
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