CN102284294A - Iron-copper compound oxide catalyst for removing ammonia through low-temperature catalysis and preparation method thereof - Google Patents
Iron-copper compound oxide catalyst for removing ammonia through low-temperature catalysis and preparation method thereof Download PDFInfo
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- CN102284294A CN102284294A CN2010102029631A CN201010202963A CN102284294A CN 102284294 A CN102284294 A CN 102284294A CN 2010102029631 A CN2010102029631 A CN 2010102029631A CN 201010202963 A CN201010202963 A CN 201010202963A CN 102284294 A CN102284294 A CN 102284294A
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- iron
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- compound oxide
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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 discloses an iron-copper compound oxide catalyst for removing ammonia through low-temperature catalysis and a preparation method thereof, relating to the fields of catalysis and environment protection. The iron-copper compound oxide catalyst is characterized by adopting zinc oxide as a carrier and an iron-copper containing compound oxide as an active component. The integral catalyst disclosed by the invention has the characteristic that ammonia is stably reduced into nitrogen gas under the conditions of normal temperature, normal humidity and large-air-volume without input of additional energy sources such as light, heat, electricity and the like.
Description
Technical field
The present invention be a kind of low temperature absorption and catalytic decomposition remove ammonia and preparation method thereof, relate to catalysis and environmental science.It is characterized in that nano zine oxide is a carrier, is active component with copper-iron compound oxide.The characteristics of catalyst of the present invention are the inputs that does not need additional light, heat, electric equal energy source, low temperature, often under the condition of wet and big air quantity with ammonia absorption and resolve into nitrogen.
The invention still further relates to above-mentioned Preparation of catalysts method.
The invention still further relates to above-mentioned catalyst and remove the application of ammonia at low temperature.
Background technology
Ammonia is a kind of colourless and have the gas of intense stimulus stink, and ammonia is a kind of alkaline matter, and it all has corrosion and spread effect to the skin histology of contact.These character of ammonia are mainly derived from the structure of ammonia, and ammonia is made up of a nitrogen-atoms and three hydrogen atoms, and molecular weight is about 17, and are little more a lot of than the mean molecule quantity (29) of air, so lta; Nitrogen-atoms adopts sp
3Hydridization and three hydrogen atoms are formed three σ keys, a sp
3Hydridization has a pair of lone electron pair, so ammonia has alkalescence and nucleophilic performance, and attack acidity or have electropositive organic matter or inorganic matter.Ammonia enters blood by alveolar after being inhaled into lung easily, combines with hemoglobin, destroys fortune oxygen function.Suck in a short time can occur shedding tears behind a large amount of ammonias, pharyngalgia, hoarseness, cough, sputum streaked with blood silk, uncomfortable in chest, expiratory dyspnea, can be with dizzy, headache, feel sick, vomiting, weak etc., pulmonary edema, adult respiratory distress syndrome (ARDS) can take place in severe patient, simultaneously the respiratory tract symptom may take place.So alkaline matter is dark and serious to the damage ratio acidic materials of tissue.Low concentration ammonia pollutes the harm to health in the room air.Ammonia has stimulation and corrosiveness to the upper respiratory tract of animal or human's body, weakens the resistance of human body to disease.Except that corrosiveness, also can cause cardiac arrest and breath stopped during excessive concentration by the reflex of trigeminal neuralgia tip.Ammonia sucks human body with gas form usually, enters IA ammonia, and small part is neutralized by carbon dioxide, and remainder is absorbed into blood, and a spot of ammonia can excrete with sweat, urine or breathing.People can feel that least concentration is about 5ppm, the workpeople who in the indoor environment of the ammonia that contacts low concentration, works, and urea and ammonia content all increase in the urine, and urea then obviously increases in the blood.
The source of ammonia is mainly from the concrete admixture that uses in the construction in the room air, particularly in the winter time in the work progress, adding urea and ammoniacal liquor are the concrete antifreezer of primary raw material in concrete wall, these additives that contain a large amount of Ammonia materials are reduced into ammonia along with the variation of environmental factors such as humiture and slowly release from body of wall in body of wall, cause that the concentration of ammonia rolls up in the room air.In addition, the ammonia in the room air also can be from additive in the house decorative material and brightening agent.The place of preparation, transportation and the use of ammonia and the ight soil of humans and animals etc. can produce ammonia simultaneously, because being extensive use of of catalytic selectivity nitrogen oxides reduction, cause ammonia not exclusively to cause the escape of ammonia to enter atmosphere, in the exhaust system inlet chamber in transportation, storage and reaction.Therefore must adopt effective means that ammonia is removed, healthy to guarantee relevant people's.
Absorption method and photocatalytic method are the methods of ammonia contaminant in the degraded closed system air of using always at present.Yet for absorption method, when the absorption of ammonia and desorption reached balance, adsorbent will lose efficacy or need regeneration, and adopting iodine and cupric as Chinese patent CN101422722A is adsorbent, and absorption has obtained higher adsorbance to noxious materials such as ammonia.Photocatalysis has also limited it and has used widely the degradation efficiency of ammonia is low.The catalytic oxidation airborne ammonia of degrading is a kind of long-acting method.Chinese patent CN101474419A does absorption or the catalytic degradation of catalyst to ammonia with rare earth oxide, zinc oxide and oxidation (Asia) copper, has obtained good effect, and the clearance in 24 little time is 90%.As seen with absorption and catalysis contact technology very big development prospect will be arranged, earlier amino molecule will be adsorbed on the surface of catalysis, then its catalytic decomposition be fallen.
The purpose of this invention is to provide a kind of under the condition of low temperature and high humility the catalyst of absorption and efficient cracked ammonium, can stably ammonia be resolved into nitrogen.
Summary of the invention
The object of the present invention is to provide under low temperature, high humidity and ammonia can be resolved into the catalyst of the load of nitrogen.
Another object of the present invention provides above-mentioned Preparation of catalysts method.
The objective of the invention is to be achieved through the following technical solutions
Catalysis material provided by the invention, adopt redox-circumfluence method:
1. the preparation of copper-iron compound oxide powder
Redox-circumfluence method key step: according to certain molar ratio, cupric salt, strong oxidizer, nitric acid molysite are mixed in acid solution, the black precipitate that generates vigorous stirring in 90～100 ℃ the aqueous solution refluxes behind 12～48h, filter, wash, at 100～150 ℃ of drying 10～24h, obtain copper-iron compound oxide catalysis material 200～700 ℃ of roastings then.
2. the preparation of the catalysis material of copper-iron compound oxide load.
Take by weighing a certain amount of copper-iron compound oxide, add the inorganic bond in a certain proportion of deionized water and the claim 9, high-speed stirred 1～24h obtains finite concentration copper-iron compound oxide slurries.The ceramic honey comb or the porous metal foam of anticipating are immersed in above-mentioned copper-iron compound oxide slurries, take out behind dipping 0.5～5min, blow the raffinate in the most duct, 80～150 ℃ of drying 8～24h in back dry in the shade in air, roasting 1～24h under 200～800 ℃ of air obtains the catalysis material of zinc oxide load.
The technology of the present invention effect
Technique effect of the present invention is that a kind of low temperature can thoroughly be removed airborne ammonia integrated technology, feature: under the often wet condition of low temperature with air in concentration be 1～1000mg/m
3Ammonia all remove, be applicable to the elimination of ammonia in the air.
Advantage of the present invention
The catalysis material of zinc oxide load becomes nitrogen with the ammonia catalytic decomposition under the condition that does not need additional energy source, its feature: anti humility performance height, good stability, treatment effeciency height, treating capacity be big, handle fully, cost is low, do not have secondary pollution and do not have problems such as absorption is saturated;
Copper-iron compound oxide catalyst adopt the straight way cellular type ceramic honey comb or catalysis material.Pressure falls very for a short time in use, can handle the ammonia in the big air quantity.
The specific embodiment
Embodiment one
Copper-iron compound oxide powder synthetic is mantoquita and the potassium peroxydisulfate (K by solubility
2S
2O
8) mix at salpeter solution neutralisation of sulphuric acid copper, add ferric nitrate (Fe (NO simultaneously
3)
2), making the Fe/Cu mol ratio is 0～0.20, the black precipitate that generates is filtered, is washed, at 110 ℃ of dry 12h behind 100 ℃ of vigorous stirring backflow 24h, obtain the copper-iron compound oxide powder of iron then at 500 ℃ of roasting 6h, be designated as Fe-Cu-0 respectively, Fe-Cu-5, Fe-Cu-10 and Fe-Cu-20, wherein Fe-Cu represents copper-iron compound oxide, numeral Fe/Cu
TotalMol ratio percentage.
XRD analysis and HRTEM the analysis showed that this material is copper-iron compound oxide.
The performance test of catalysis material is carried out on the fixed bed reactors of continuous-flow.The powder catalytic material is pulverized the granular of making 0.25～0.50mm through compressing tablet, then the 0.5g granular is loaded in the glass tube, is that feeding contains 100mg/m under 80% the condition in low temperature (18～25 ℃) and relative humidity
3The air of ammonia, wind speed are 2.5m/s.Reactor outlet ammonia detects with the ammonia analyzer.The results are shown in Table 1.
Embodiment two
Synthesizing of copper-iron compound oxide powder with embodiment one, promptly by mantoquita and potassium peroxydisulfate (K
2S
2O
8) mix at salpeter solution neutralisation of sulphuric acid copper, add ferric nitrate (Fe (NO simultaneously
3)
2), making the Fe/Mn mol ratio is 0～0.20, the black precipitate that generates is filtered, is washed, at 110 ℃ of dry 12h behind 100 ℃ of vigorous stirring backflow 24h, obtain the copper-iron compound oxide powder of iron then at 200-800 ℃ of roasting 6h, be designated as Fe-Cu-0 respectively, Fe-Cu-5, Fe-Cu-10 and Fe-Cu-20, wherein Fe-Cu represents iron copper-iron compound oxide, numeral Fe/Cu
TotalMol ratio percentage.
XRD analysis and HRTEM the analysis showed that this material is copper-iron compound oxide.
The performance test of catalysis material is carried out on the fixed bed reactors of continuous-flow.The powder catalytic material is pulverized the granular of making 0.25～0.50mm through compressing tablet, then the 0.5g granular is loaded in the glass tube, is that feeding contains 100mg/m under 80% the condition in low temperature (18～25 ℃) and relative humidity
3The air of ammonia, wind speed are 2.5m/s.Reactor outlet ammonia detects with the ammonia analyzer.The results are shown in Table 2.
Embodiment three
1) copper-iron compound oxide powder is synthetic
Synthesizing of copper-iron compound oxide powder is identical with example one, and promptly the synthetic of iron copper-iron compound oxide powder is by mantoquita and potassium peroxydisulfate (K
2S
2O
8) mix at salpeter solution neutralisation of sulphuric acid copper, add ferric nitrate (Fe (NO simultaneously
3)
2), making the Fe/Cu mol ratio is 0～0.20, the black precipitate of generation is filtered, is washed behind 100 ℃ of vigorous stirring backflow 24h, at 110 ℃ of dry 12h, obtains the copper-iron compound oxide powder of iron then at 500 ℃ of roasting 6h.
2) preparation of the catalysis material of copper-iron compound oxide ceramic honey comb load.
Take by weighing a certain amount of copper-iron compound oxide, add the inorganic bond in a certain proportion of deionized water and the claim 9, high-speed stirred 1～24h obtains finite concentration copper-iron compound oxide slurries.The ceramic honey comb or the porous metal foam sample of anticipating are immersed in above-mentioned copper-iron compound oxide slurries, take out behind dipping 0.5～5min, blow the raffinate in the most duct, back 110 ℃ of dry 24h dry in the shade in air, roasting 6h under 500 ℃ of air obtains the catalysis material of zinc oxide load.
The performance test of catalyst is with embodiment one.The results are shown in Table 3.
Embodiment four
1) copper-iron compound oxide powder is synthetic
Synthesizing of copper-iron compound oxide powder is identical with example one, and promptly the synthetic of copper-iron compound oxide powder is by mantoquita and potassium peroxydisulfate (K
2S
2O
8) mix at salpeter solution neutralisation of sulphuric acid copper, add ferric nitrate (Fe (NO simultaneously
3)
2), making the Fe/Mn mol ratio is 0～0.20, the black precipitate of generation is filtered, is washed behind 100 ℃ of vigorous stirring backflow 24h, at 110 ℃ of dry 12h, obtains copper-iron compound oxide powder at 500 ℃ of roasting 6h then.
2) preparation of the catalysis material of copper-iron compound oxide.
Take by weighing a certain amount of copper-iron compound oxide, add the inorganic bond in a certain proportion of deionized water and the claim 9, high-speed stirred 1～24h obtains finite concentration copper-iron compound oxide slurries.The open type stephanoporate foam metal sample of anticipating is immersed in above-mentioned copper-iron compound oxide slurries, take out behind dipping 0.5～5min, blow the raffinate in the most duct, back 110 ℃ of dry 24h dry in the shade in air, roasting 6h under 500 ℃ of air obtains the catalysis material of copper-iron compound oxide.The performance test of catalysis material is with embodiment one.The results are shown in Table 3.
Embodiment five
The Preparation of catalysts of iron copper-iron compound oxide is identical with example one.
The performance test of catalysis material is with embodiment one, and the concentration of ammonia is at 10～300mg/m
3In the scope.The results are shown in Table 4.
Embodiment six
The Preparation of catalysts of iron copper-iron compound oxide is identical with example five.
The performance test of catalyst stability experiment is with embodiment one, and 30 days testing times, the ammonia concentration of inlet is 10mg/m
3, the exit concentration of ammonia is from 4.0 μ g/m
3Be upgraded to 5.0 μ g/m
3
The test result of table 1 copper-iron compound oxide powder catalytic material breakdown ammonia.(the ammonia concentration of import is 100mg/m
3)
The test result of table 2 copper-iron compound oxide fine catalyst cracked ammonium.(the ammonia concentration of import is 200mg/m
3)
The test result of the catalysis material cracked ammonium of table 3 copper-iron compound oxide (Fe-Cu-20).(the ammonia concentration of import is 200mg/m
3)
The test result of table 4 catalyst decomposes ammonia.
Claims (10)
1. the present invention is a kind of monolithic devices catalysis material of iron/copper composite oxides, it is characterized in that adopting zinc oxide carrier, is active component with the iron/copper composite oxides.
2. iron/copper composite oxides in the claim 1, the mol ratio that it is characterized in that Fe/Cu is between 0～0.20.
3. the preparation method of iron/copper composite oxide catalytic material in the claim 2 is characterized in that adopting redox-circumfluence method.
Redox-circumfluence method key step is: according to certain molar ratio, cupric salt, strong oxidizer and ferric nitrate are mixed in acid solution, the black precipitate that generates vigorous stirring in 90～100 ℃ the aqueous solution refluxes behind 12～48h, filter, wash, at 100～150 ℃ of drying 10～24h, obtain the iron/copper composite oxide catalytic material 200～700 ℃ of roastings then.
In the claim 2 in the iron/copper composite oxide catalytic material copper with and Cu
2+Exist.
In the claim 2 in the iron/copper composite oxide catalytic material iron mainly with Fe
3+Be present in the skeleton of iron/copper composite oxides.
6. the cupric salt in the claim 3 is copper acetate (Cu (CH
3COO)
2), dichloride copper (CuCl
2), copper nitrate (Cu (NO
3)
2) or copper sulphate (CuSO
4) in one or more, copper concentration is 0.1～5.0mol/l in its solution.
7. the strong oxidizer described in the claim 3 is ammonium persulfate ((NH
4)
2S
2O
8), potassium peroxydisulfate (K
2S
2O
8), sodium peroxydisulfate (Na
2S
2O
8), ozone (O
3), sodium chlorate (NaClO
3), hydrogen peroxide (H
2O
2) in the solution one or more, strong oxidizer concentration is 0.1～2.5mol/l in its solution.The mol ratio of total metal ion is between 1: 1～6: 1 in strong oxidizer and the solution.
8. the iron/copper composite oxides monolithic devices catalysis material described in the claim 1 is characterized in that its preparation method is as follows:
(1) take by weighing a certain amount of iron/copper composite oxide catalytic material, add a certain proportion of deionized water and adhesive, high-speed stirred 1～24h obtains certain density iron/copper composite oxides slurries.
(2) honeycomb ceramic carrier that will anticipate is immersed in the iron/copper composite oxides slurries that prepare, take out behind dipping 0.5～60min, blow the raffinate in the most duct, 80～130 ℃ of drying 2～24h in back that in air, dry in the shade, roasting 1～24h under 200～800 ℃ of air.
9. the adhesive described in the claim 8 is inorganic bonds such as silicate, aluminium oxide or zirconium carbonate ammonium, and the weight ratio of adhesive and iron/copper composite oxides is between 1～50%.
10. the iron/copper composite oxides integral catalyst described in the claim 1 is applicable to cryogenic absorption and cracked ammonium.
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|---|---|---|---|
| CN2010102029631A CN102284294A (en) | 2010-06-18 | 2010-06-18 | Iron-copper compound oxide catalyst for removing ammonia through low-temperature catalysis and preparation method thereof |
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|---|---|---|---|
| CN2010102029631A CN102284294A (en) | 2010-06-18 | 2010-06-18 | Iron-copper compound oxide catalyst for removing ammonia through low-temperature catalysis and preparation method thereof |
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Cited By (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN104069860A (en) * | 2014-06-27 | 2014-10-01 | 北京林业大学 | Preparation of magnetic nano copper-iron oxyhydroxide and application thereof to pollution removal by catalytic ozonation |
| CN104941442A (en) * | 2015-05-22 | 2015-09-30 | 大连理工大学 | Method for carrying out low temperature catalytic oxidation on ammonia removal pollutants |
| CN108543416A (en) * | 2018-03-05 | 2018-09-18 | 攀枝花市蓝鼎环保科技有限公司 | Processing system and its construction technology for being mixed into raw coke oven gas in coking flue gas |
| CN110201672A (en) * | 2019-07-15 | 2019-09-06 | 浙江工商大学 | A kind of ZnO/Fe-Cu-M composite catalyst and its preparation method and application for the VOCs that degrades |
| CN111068512A (en) * | 2019-12-26 | 2020-04-28 | 南京工大环境科技有限公司 | Integrated catalytic conversion system and method for reducing exhaust ammonia emission |
| CN115417694A (en) * | 2022-08-30 | 2022-12-02 | 佛山市顺德区金磊环保科技有限公司 | Catalytic honeycomb ceramic material and preparation method and application thereof |
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Cited By (9)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN104069860A (en) * | 2014-06-27 | 2014-10-01 | 北京林业大学 | Preparation of magnetic nano copper-iron oxyhydroxide and application thereof to pollution removal by catalytic ozonation |
| CN104069860B (en) * | 2014-06-27 | 2016-07-27 | 北京林业大学 | The preparation of magnetic nano copper ferrum oxyhydroxide and the application in O3 catalytic oxidation depollution thereof |
| CN104941442A (en) * | 2015-05-22 | 2015-09-30 | 大连理工大学 | Method for carrying out low temperature catalytic oxidation on ammonia removal pollutants |
| CN108543416A (en) * | 2018-03-05 | 2018-09-18 | 攀枝花市蓝鼎环保科技有限公司 | Processing system and its construction technology for being mixed into raw coke oven gas in coking flue gas |
| CN108543416B (en) * | 2018-03-05 | 2021-05-04 | 攀枝花市蓝鼎环保科技有限公司 | Treatment system for coking flue gas mixed with raw coke oven gas and construction process thereof |
| CN110201672A (en) * | 2019-07-15 | 2019-09-06 | 浙江工商大学 | A kind of ZnO/Fe-Cu-M composite catalyst and its preparation method and application for the VOCs that degrades |
| CN111068512A (en) * | 2019-12-26 | 2020-04-28 | 南京工大环境科技有限公司 | Integrated catalytic conversion system and method for reducing exhaust ammonia emission |
| CN115417694A (en) * | 2022-08-30 | 2022-12-02 | 佛山市顺德区金磊环保科技有限公司 | Catalytic honeycomb ceramic material and preparation method and application thereof |
| CN115417694B (en) * | 2022-08-30 | 2024-02-02 | 佛山市顺德区金磊环保科技有限公司 | Catalytic honeycomb ceramic material and preparation method and application thereof |
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Application publication date: 20111221 |