CN103127952A - Supported nano-silver catalyst capable of eliminating formaldehyde at room temperature and preparation method thereof - Google Patents
Supported nano-silver catalyst capable of eliminating formaldehyde at room temperature and preparation method thereof Download PDFInfo
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- CN103127952A CN103127952A CN 201110392255 CN201110392255A CN103127952A CN 103127952 A CN103127952 A CN 103127952A CN 201110392255 CN201110392255 CN 201110392255 CN 201110392255 A CN201110392255 A CN 201110392255A CN 103127952 A CN103127952 A CN 103127952A
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Abstract
The invention discloses a supported nano-silver catalyst capable of eliminating formaldehyde at room temperature. The catalyst uses ZSM-5 molecular sieves as carrier, and is prepared by supported nano-silver active components through metallic oxide modifying. The catalyst is composed of, by weight, 1% to 5% of nano-silver active components, 1% to 20% of metallic oxide, and 75% to 98% of ZSM-5 molecular sieves. The invention discloses a preparation method of the supported nano-silver catalyst capable of eliminating the formaldehyde at room temperature. The preparation method is characterized by comprising the following steps: the ZSM-5 molecular sieve carrier is modified, and drying and roasting are carried out to obtain the finished catalyst after the modified carrier is put into a solution to carry out equivalent-volume impregnation at 10 DEG C to 60 DEG C. The airspeed of the catalyst at room temperature is 10000 h-1 hour, the formaldehyde removal rate of the catalyst is up to more than 93.7%, the formaldehyde is catalyzed to be oxidated into harmless water and carbon dioxide to achieve green elimination, and a preparation process is simple, easy to operate, low in cost, and free of secondary pollution.
Description
Technical field
The present invention relates to the Catalysts and its preparation method of a kind of chemical industry and atmospheric environment field of purification, particularly relate to loaded nano silver catalyst of a kind of eliminating formaldehyde at room temperature and preparation method thereof.
Background technology
Formaldehyde is a kind of of volatile organic matter, is irritative gas colourless, that have overpowering odor.Formaldehyde is prevalent in the various commodity such as finishing material in daily life, furniture, cosmetics, cleaning agent, pesticide, paper, textile fabric.In the binding agent of finishing material the release of formaldehyde is slow, reaches the more than ten years, often sucks a small amount of formaldehyde, can cause slow poisoning, the general symptoms such as headache, weak, mucous hyperemia, skin irritatin disease, allergic dermatitis occur.The removal of formaldehyde has become one of environmental issue of present extensive concern.Eliminate the method for formaldehyde under room temperature take catalytic oxidation as main, common catalyst is with ceramic honey comb, active carbon, metal oxide or composite metal oxide etc. are carrier, load Au, Pd, the noble metals such as Pt are prepared from, and the catalyst cost is higher, should not apply.Zeolite molecular sieve is because having the connected pore channel, and the duct is even, and specific area is high, and adsorption selectivity is good, is normally used for catalyst carrier.
In prior art, a kind of load type nano gold catalyst of removing formaldehyde for room air and preparation method thereof is disclosed, this catalyst is take porous cordierite ceramics as carrier, after carrier surface evenly is coated with one deck rare earth oxide or composite rare-earth oxide coating, deposit 3～10nm gold grain in coating, wherein the load capacity of gold is 1～3% of coating quality.This catalyst can effectively be removed formaldehyde in air, and purification efficiency is high, but gold is expensive, has increased the cost of catalyst, can not put in practical application.
Find again, a kind of silver-carrying nano manganese dioxide-catalyst and its preparation method and application is disclosed in prior art, the active component of the catalyst of this invention is the manganese dioxide molecular sieve of silver-colored carried with doped, be doped in the nano-manganese dioxide molecular sieve pore passage by the argent orientation and form, the load capacity of silver is 1～25%.The concentration of the formaldehyde of processing is 1.5～2000ppm, and the complete conversion temperature of the catalysis of formaldehyde is 0～120 ℃, and when reaction temperature was 100 ℃, the conversion ratio of formaldehyde was 91.2%.This catalyst preparation process is simple, cost is low, non-secondary pollution, but the conversion fully of formaldehyde is temperature required higher, can not be used for the elimination of formaldehyde under room temperature.
Summary of the invention
The object of the present invention is to provide loaded nano silver catalyst of a kind of eliminating formaldehyde at room temperature and preparation method thereof.The present invention is achieved by the following technical solutions:
The invention provides a kind of loaded nano silver catalyst of eliminating formaldehyde at room temperature, it is characterized in that, described catalyst is prepared from through metal oxide modified back loading nano silver active component take ZSM-5 molecular sieve as carrier;
Wherein catalyst quality percentage consists of: the nano silver active component is 1～5%, metal oxide is 1～20%, and ZSM-5 molecular sieve is 75～98%.
Described nano silver active component is nano-Ag particles, and its grain diameter is 2～100 nanometers.
Described metal oxide is a kind of or its combination in manganese oxide, cobalt oxide, zinc oxide, iron oxide, magnesia, zirconia, lanthana, cerium oxide, cupric oxide.
The invention provides a kind of preparation method of loaded nano silver catalyst of eliminating formaldehyde at room temperature, it is characterized in that comprising the following steps:
The first step, ZSM-5 molecular sieve support modification: the metal-nitrate solutions of preparation desired concn, be placed in one in 10～60 ℃ of incipient impregnations the ZSM-5 molecular sieve carrier after 1～20 hour, in 80～150 ℃ of dryings 2～10 hours, 450～600 ℃ of lower roastings 1～6 hour, make the modified zsm-5 zeolite carrier again;
The liquor argenti nitratis ophthalmicus of second step, preparation 0.0157 ~ 0.0785 g/ml, be placed in one in 10～60 ℃ of incipient impregnations modified support after 2～10 hours, in 60～150 ℃ of dryings 2～10 hours, then 200～500 ℃ of lower roastings 1～6 hour, make finished catalyst.
Described metal nitrate is a kind of or its combination in manganese nitrate, cobalt nitrate, zinc nitrate, ferric nitrate, magnesium nitrate, zirconium nitrate, lanthanum nitrate, cerous nitrate, copper nitrate.
The purifying property evaluation of catalysis material PARA FORMALDEHYDE PRILLS(91,95) of the present invention is carried out in U-shaped glass tube reactor, and the catalysis material consumption is 0.5 ml, and unstripped gas consists of: concentration of formaldehyde is 10～500 ppm, and all the other are air.Reaction is carried out under 20～40 ℃ of atmospheric pressure environment, and reaction gas volume air speed (GHSV) is 10000h
-1, detect concentration of formaldehyde by American I nterscan 4160 methylene oxide detecting instruments and calculate the formaldehyde clearance.
Compared with prior art, catalyst of the present invention is prepared from through metal oxide modified back loading nano silver active component take ZSM-5 molecular sieve as carrier.The present invention has the following advantages: this catalyst is when at room temperature air speed is 10000h-1, the clearance of PARA FORMALDEHYDE PRILLS(91,95) reaches more than 93.7%, make formaldehyde through catalytic oxidation become harmless water and the green elimination of carbon dioxide realization, and preparation technology, the catalyst activity component is that Nano Silver and content are low so the catalyst cost is lower, have simultaneously good water resistant vapour performance and life-span, non-secondary pollution.
The specific embodiment
The below elaborates to embodiments of the invention: the present embodiment is implemented under take technical solution of the present invention as prerequisite, provided detailed embodiment and concrete operating process, but protection scope of the present invention is not limited to following embodiment.
Comparative Examples:
Take 0.0157 g silver nitrate and be mixed with 0.5 ml solution, 0.5 g ZSM-5 molecular sieve carrier is placed in one in 25 ℃ of dipping 1 h, 120 ℃ of drying 4 h, 450 ℃ of roasting 3 h make comparative example.Ag:ZSM-5 molecular sieve=2:100 wherein.
Made sample is carried out purifying formaldehyde performance evaluation according to the afore-mentioned test condition, and in the time of 20 ℃, the initial conversion of formaldehyde is that after 76.9%, 2h, the formaldehyde conversion ratio reduces to 53.2%.
Embodiment 1:
Take 0.0514 g manganese nitrate and be dissolved in wiring solution-forming in 0.5 ml deionized water, 0.5 g ZSM-5 molecular sieve carrier is placed in one after 25 ℃ of incipient impregnation 2 h, 120 ℃ of drying 6 h, then at 600 ℃ of lower roasting 2 h, make manganese oxide modified zsm-5 zeolite carrier;
Take 0.0157 g silver nitrate and be mixed with 0.5 ml solution, manganese oxide modified zsm-5 zeolite carrier is placed in one in 25 ℃ of dipping 1 h, 120 ℃ of drying 4 h, 450 ℃ of roasting 3 h make finished catalyst.Ag:MnO wherein
2: ZSM-5 molecular sieve=2:5:100.
Made finished catalyst is carried out the purifying formaldehyde voltinism according to the afore-mentioned test condition can be estimated, and in the time of 20 ℃, the initial conversion of formaldehyde is that after 91.6%, 2h, the formaldehyde conversion ratio reduces to 85.2%.
Embodiment 2:
Take 0.063 g cerous nitrate and be dissolved in wiring solution-forming in 0.5 ml deionized water, 0.5 g ZSM-5 molecular sieve carrier is placed in one after 25 ℃ of incipient impregnation 2 h, 120 ℃ of drying 6 h, then at 600 ℃ of lower roasting 2 h, make cerium oxide modified zsm-5 zeolite carrier;
Take 0.0157 g silver nitrate and be mixed with 0.5 ml solution, cerium oxide modified zsm-5 zeolite carrier is placed in one in 25 ℃ of dipping 1 h, 120 ℃ of drying 4 h, 450 ℃ of roasting 3 h make finished catalyst.Ag:CeO wherein
2: ZSM-5 molecular sieve=2:5:100.
Made finished catalyst is carried out the purifying formaldehyde voltinism according to the afore-mentioned test condition can be estimated, and in the time of 20 ℃, the initial conversion of formaldehyde is that after 92.4%, 2h, the formaldehyde conversion ratio reduces to 76.8%.
Embodiment 3:
Take 0.076 g copper nitrate and be dissolved in wiring solution-forming in 0.5 ml deionized water, 0.5 g ZSM-5 molecular sieve carrier is placed in one after 25 ℃ of incipient impregnation 2 h, 120 ℃ of drying 6 h, then at 600 ℃ of lower roasting 2 h, make cupric oxide modified zsm-5 zeolite carrier;
Take 0.0157 g silver nitrate and be mixed with 0.5 ml solution, cupric oxide modified zsm-5 zeolite carrier is placed in one in 25 ℃ of dipping 1 h, 120 ℃ of drying 4 h, 450 ℃ of roasting 3 h make finished catalyst.Ag:CuO:ZSM-5 molecular sieve=2:5:100 wherein.
Made finished catalyst is carried out the purifying formaldehyde voltinism according to the afore-mentioned test condition can be estimated, and in the time of 20 ℃, the initial conversion of formaldehyde is that after 92.9%, 2h, the formaldehyde conversion ratio reduces to 61.4%.
Embodiment 4:
Take 0.0914 g zinc nitrate and be dissolved in wiring solution-forming in 0.5 ml deionized water, 0.5 g ZSM-5 molecular sieve carrier is placed in one after 25 ℃ of incipient impregnation 2 h, 120 ℃ of drying 6 h, then at 600 ℃ of lower roasting 2 h, make modified zinc oxide ZSM-5 molecular sieve carrier;
Take 0.0157 g silver nitrate and be mixed with 0.5 ml solution, modified zinc oxide ZSM-5 molecular sieve carrier is placed in one in 25 ℃ of dipping 1 h, 120 ℃ of drying 4 h, 450 ℃ of roasting 3 h make finished catalyst.Ag:ZnO:ZSM-5 molecular sieve=2:5:100 wherein.
Made finished catalyst is carried out the purifying formaldehyde voltinism according to the afore-mentioned test condition can be estimated, and in the time of 20 ℃, the initial conversion of formaldehyde is that after 56.8%, 2h, the formaldehyde conversion ratio reduces to 34.1%.
Embodiment 5:
Take 0.0514 g manganese nitrate and 0.063 g cerous nitrate is dissolved in wiring solution-forming in 0.5 ml deionized water, 0.5 g ZSM-5 molecular sieve carrier is placed in one after 25 ℃ of incipient impregnation 2 h, 120 ℃ of drying 6 h, at 600 ℃ of lower roasting 2 h, make manganese oxide modified zsm-5 zeolite carrier again;
Take 0.0394 g silver nitrate and be mixed with 0.5 ml solution, 0.5 g ZSM-5 molecular sieve carrier is placed in one in 25 ℃ of dipping 1 h, 120 ℃ of drying 4 h, 450 ℃ of roasting 3 h make finished catalyst.Ag:MnO wherein
2: CeO
2: ZSM-5 molecular sieve=2:5:5:100.
Made finished catalyst is carried out the purifying formaldehyde voltinism according to the afore-mentioned test condition can be estimated, and in the time of 20 ℃, the initial conversion of formaldehyde is that after 93.7%, 2h, the formaldehyde conversion ratio reduces to 91.3%.
Claims (5)
1. the loaded nano silver catalyst of an eliminating formaldehyde at room temperature, is characterized in that, described catalyst is prepared from through metal oxide modified back loading nano silver active component take ZSM-5 molecular sieve as carrier;
Wherein catalyst quality percentage consists of: the nano silver active component is 1～5%, metal oxide is 1～20%, and ZSM-5 molecular sieve is 75～98%.
2. the loaded nano silver catalyst of a kind of eliminating formaldehyde at room temperature according to claim 1, is characterized in that, described nano silver active component is nano-Ag particles, and its grain diameter is 2～100 nanometers.
3. the loaded nano silver catalyst of a kind of eliminating formaldehyde at room temperature according to claim 1, it is characterized in that, described metal oxide is a kind of or its combination in manganese oxide, cobalt oxide, zinc oxide, iron oxide, magnesia, zirconia, lanthana, cerium oxide, cupric oxide.
4. according to claim 1, or 2, or the preparation method of the loaded nano silver catalyst of 3 described a kind of eliminating formaldehyde at room temperature, it is characterized in that comprising the following steps:
The first step, ZSM-5 molecular sieve support modification: the metal-nitrate solutions of preparation desired concn, be placed in one in 10～60 ℃ of incipient impregnations the ZSM-5 molecular sieve carrier after 1～20 hour, in 80～150 ℃ of dryings 2～10 hours, 450～600 ℃ of lower roastings 1～6 hour, make the modified zsm-5 zeolite carrier again;
The liquor argenti nitratis ophthalmicus of second step, preparation 0.0157 ~ 0.0785 g/ml, be placed in one in 10～60 ℃ of incipient impregnations modified support after 2～10 hours, in 60～150 ℃ of dryings 2～10 hours, then 200～500 ℃ of lower roastings 1～6 hour, make finished catalyst.
5. the preparation method of the loaded nano silver catalyst of a kind of eliminating formaldehyde at room temperature according to claim 4, it is characterized in that, described metal nitrate is a kind of or its combination in manganese nitrate, cobalt nitrate, zinc nitrate, ferric nitrate, magnesium nitrate, zirconium nitrate, lanthanum nitrate, cerous nitrate, copper nitrate.
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2011
- 2011-12-01 CN CN 201110392255 patent/CN103127952A/en active Pending
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Application publication date: 20130605 |