CN104383916A - Catalyst for removing low-concentration nitric oxide and preparation method and application of catalyst - Google Patents
Catalyst for removing low-concentration nitric oxide and preparation method and application of catalyst Download PDFInfo
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Abstract
The invention discloses a catalyst for removing a low-concentration nitric oxide and a preparation method and an application of the catalyst. The method comprises the following steps: dissolving a rare-earth salt and a manganese salt into 40ml of water, stirring at room temperature, dropwise adding 25ml of oxalic acid solution to participate the solution; further stirring for 1.5 hours, filtering and washing the obtained suspension liquid and then drying in a drying oven at 70 DEG C for 12 hours; and roasting in a muffle furnace for 3 hours at 400 DEG C, so as to prepare a rare-earth manganese-based composite oxide. The catalyst is applied to catalytic oxidation of the low-concentration nitric oxide, and has high nitric oxide removal rate; when the concentration of the nitric oxide is smaller than or equal to 10ppm, the removal rate of the catalyst on the nitric oxide can be up to 99%; and the catalyst has the advantages of simple preparation process, low cost and the like.
Description
Technical field
The present invention relates to the preparation that low concentration nitric oxide eliminates catalyst, be applicable to the catalytic oxidation of environmental contaminants NO, in depollution of environment field, there is application prospect.
Background technology
Mobile traffic gets more and more, and the waste gas thereupon produced is one of main source becoming municipal pollution.In order to eliminate these pollution sources, dropped into large quantifier elimination, but these technology for eliminating can not be removed pollution completely, still there is the waste gas of very low concentrations, if these toxic emissions in semi-enclosed space, as underground parking, tunnel etc., due to the restriction of exhaust system, these pollutants can not be emitted in time, through accumulating over a long period, the concentration of pollutant is increasing, causes air severe contamination.Nitrogen oxide is wherein a kind of pollutant, mainly comprises nitric oxide (90%) and nitrogen dioxide (10%), has therefore done a series of research mainly for nitric oxide production elimination herein.
Chinese invention patent discloses a series of pure phase chromium oxide catalyst, or is supported carrier or doping different metal oxides catalyst with chromium oxide, or on carrier, supports the preparation method of chromium oxide catalyst, for nitric oxide production elimination.Although these catalyst have certain activity, but in the process preparing chromium oxide, inevitably produce the oxide of high valence chrome, belong to poisonous and harmful substance, can produce serious harm to health, the use of these catalyst can cause the secondary pollution of environment.
Summary of the invention
In order to overcome the defect that above-mentioned existing low-concentration nitrogen oxide Treatment process exists, the invention provides a kind of low concentration nitric oxide and eliminating catalyst and preparation method and application.
Low concentration nitric oxide eliminates a preparation method for catalyst, and it is characterized in that, this catalyst is rear-earth-doped manganese base composite oxidate, and for the elimination of low concentration nitric oxide, concrete steps are as follows:
Rare-earth salts and manganese salt are dissolved in 40 ml waters, stirring at normal temperature also drips 25 milliliters of oxalic acid solutions and makes precipitation, continue stirring 1.5 hours, 70 DEG C of baking ovens are put into dry 12 hours after the suspension obtained is carried out filtration washing, then Muffle furnace 400 DEG C of roastings 3 hours are put into, obtained rare earth manganese base composite oxidate.
Described rare-earth salts is lanthanum nitrate, lanthanum chloride, cerous nitrate, cerous sulfate, neodymium nitrate, the one in neodymium chloride or its combination, and described manganese salt is manganese nitrate, the one in manganese chloride or its combination.
Described manganese salt and the ratio of rare-earth salts are 1 ~ 9, and rare earths salt concentration is 0.07 ~ 0.4 mol/L, and described manganese salt solution concentration is 0.4 ~ 0.7 mol/L,
Described oxalic acid solution concentration is 1.5 ~ 2.5 mol/L.
A kind of low concentration nitric oxide eliminates catalyst, prepares according to above-mentioned arbitrary described method.
A kind of low concentration nitric oxide is eliminated catalyst and is used for nitric oxide catalytic oxidation, at normal temperatures and pressures efficiently catalyzing and oxidizing nitric oxide.
Reactivity is evaluated: the catalyst of above-mentioned acquisition is passed into reaction gas at 25 DEG C, carries out active testing, total flow is 370 ~ 380 mL/min(STP).
Detailed description of the invention
Be described in detail below in conjunction with specific embodiment: the present embodiment is implemented under premised on technical solution of the present invention, give detailed embodiment and specific operation process, but protection scope of the present invention is not limited to following embodiment.
embodiment 1:
Take 4.87 g lanthanum nitrates, 2.97 g manganese chlorides are dissolved in 40 mL water, at room temperature stir, drip the oxalic acid aqueous solution of 25 mL1.78 mol/L, continuation stirring filtration washing after 1.5 hours, in 70 DEG C of baking ovens dry 12 hours, then 400 DEG C of roastings 3 hours in Muffle furnace, obtained lanthanum manganese composite oxide La1Mn1.
Taking 0.200 g La1Mn1 catalyst, to be placed in external diameter be Φ 6, and internal diameter is in the U-shaped reaction tube of Φ 4, then puts into 25 DEG C of water-baths, and pass into 10 ppm NO reaction gases, all the other are air, and air speed is 110000 mLg
-1h
-1, the highest elimination factor of NO is 10%.
embodiment 2:
Take 2.44 g lanthanum nitrates, 4.45 g manganese chlorides are dissolved in 40 mL water, at room temperature stir, drip the oxalic acid aqueous solution of 25 mL1.78 mol/L, continuation stirring filtration washing after 1.5 hours, in 70 DEG C of baking ovens dry 12 hours, then 400 DEG C of roastings 3 hours in Muffle furnace, obtained lanthanum manganese composite oxide La1Mn3.
Taking 0.200 g La1Mn3 catalyst, to be placed in external diameter be Φ 6, and internal diameter is in the U-shaped reaction tube of Φ 4, then puts into 25 DEG C of water-baths, passes into 10ppm NO reaction gas, and all the other are air, and air speed is 110000 mLg
-1h
-1, the highest elimination factor of NO is 62 %.
embodiment 3:
Take 1.62 g lanthanum nitrates, 4.95 g manganese chlorides are dissolved in 40 mL water, at room temperature stir, drip the oxalic acid aqueous solution of 25 mL1.78 mol/L, continuation stirring filtration washing after 1.5 hours, in 70 DEG C of baking ovens dry 12 hours, then 400 DEG C of roastings 3 hours in Muffle furnace, obtained lanthanum manganese composite oxide La1Mn5.
Taking 0.200 g La1Mn5 catalyst, to be placed in external diameter be Φ 6, and internal diameter is in the U-shaped reaction tube of Φ 4, then puts into 25 DEG C of water-baths, and pass into 10 ppm NO reaction gases, all the other are air, and air speed is 110000 mLg
-1h
-1, the highest elimination factor of NO is 99 %.
embodiment 4:
Take 1.22 g lanthanum nitrates, 5.19 g manganese chlorides are dissolved in 40 mL water, at room temperature stir, drip the oxalic acid aqueous solution of 25 mL1.78 mol/L, continuation stirring filtration washing after 1.5 hours, in 70 DEG C of baking ovens dry 12 hours, then 400 DEG C of roastings 3 hours in Muffle furnace, obtained lanthanum manganese composite oxide La1Mn7.
Taking 0.200 g La1Mn7 catalyst, to be placed in external diameter be Φ 6, and internal diameter is in the U-shaped reaction tube of Φ 4, then puts into 25 DEG C of water-baths, and pass into 10 ppm NO reaction gases, all the other are air, and air speed is 110000 mLg
-1h
-1, the highest elimination factor of NO is 98 %.
embodiment 5:
Take 0.94 g lanthanum nitrate, 5.34 g manganese chlorides are dissolved in 40 mL water, at room temperature stir, drip the oxalic acid aqueous solution of 25 mL1.78 mol/L, continuation stirring filtration washing after 1.5 hours, in 70 DEG C of baking ovens dry 12 hours, then 400 DEG C of roastings 3 hours in Muffle furnace, obtained lanthanum manganese composite oxide La1Mn9.
Taking 0.200 g La1Mn9 catalyst, to be placed in external diameter be Φ 6, and internal diameter is in the U-shaped reaction tube of Φ 4, then puts into 25 DEG C of water-baths, passes into 10ppm NO reaction gas, and all the other are air, and air speed is 110000 mLg
-1h
-1, the highest elimination factor of NO is 98 %.
embodiment 6:
Take 6.51 g cerous nitrates, 2.97 g manganese chlorides are dissolved in 40 mL water, at room temperature stir, drip the oxalic acid aqueous solution of 25 mL1.78 mol/L, continuation stirring filtration washing after 1.5 hours, in 70 DEG C of baking ovens dry 12 hours, then 400 DEG C of roastings 3 hours in Muffle furnace, obtained cerium manganese composite oxides Ce1Mn1.
Taking 0.200 g Ce1Mn1 catalyst, to be placed in external diameter be Φ 6, and internal diameter is in the U-shaped reaction tube of Φ 4, then puts into 25 DEG C of water-baths, and pass into 10 ppm NO reaction gases, all the other are air, and air speed is 110000 mLg
-1h
-1, the highest elimination factor of NO is 9 %.
embodiment 7:
Take 3.26 g cerous nitrates, 4.45 g manganese chlorides are dissolved in 40 mL water, at room temperature stir, drip the oxalic acid aqueous solution of 25 mL1.78 mol/L, continuation stirring filtration washing after 1.5 hours, in 70 DEG C of baking ovens dry 12 hours, then 400 DEG C of roastings 3 hours in Muffle furnace, obtained cerium manganese composite oxides Ce1Mn3.
Taking 0.200 g Ce1Mn3 catalyst, to be placed in external diameter be Φ 6, and internal diameter is in the U-shaped reaction tube of Φ 4, then puts into 25 DEG C of water-baths, and pass into 10 ppm NO reaction gases, all the other are air, and air speed is 110000 mLg
-1h
-1, the highest elimination factor of NO is 66 %.
embodiment 8:
Take 2.17 g cerous nitrates, 4.95 g manganese chlorides are dissolved in 40 mL water, at room temperature stir, drip the oxalic acid aqueous solution of 25 mL1.78 mol/L, continuation stirring filtration washing after 1.5 hours, in 70 DEG C of baking ovens dry 12 hours, then 400 DEG C of roastings 3 hours in Muffle furnace, obtained cerium manganese composite oxides Ce1Mn5.
Taking 0.200 g Ce1Mn5 catalyst, to be placed in external diameter be Φ 6, and internal diameter is in the U-shaped reaction tube of Φ 4, then puts into 25 DEG C of water-baths, and pass into 10 ppm NO reaction gases, all the other are air, and air speed is 110000 mLg
-1h
-1, the highest elimination factor of NO is 99 %.
embodiment 9:
Take 1.63 g cerous nitrates, 5.19 g manganese chlorides are dissolved in 40 mL water, at room temperature stir, drip the oxalic acid aqueous solution of 25 mL1.78 mol/L, continuation stirring filtration washing after 1.5 hours, in 70 DEG C of baking ovens dry 12 hours, then 400 DEG C of roastings 3 hours in Muffle furnace, obtained cerium manganese composite oxides Ce1Mn7.
Taking 0.200 g Ce1Mn7 catalyst, to be placed in external diameter be Φ 6, and internal diameter is in the U-shaped reaction tube of Φ 4, then puts into 25 DEG C of water-baths, and pass into 10 ppm NO reaction gases, all the other are air, and air speed is 110000 mLg
-1h
-1, the highest elimination factor of NO is 99 %.
embodiment 10:
Take 1.30 g cerous nitrates, 5.34 g manganese chlorides are dissolved in 40 mL water, at room temperature stir, drip the oxalic acid aqueous solution of 25 mL1.78 mol/L, continuation stirring filtration washing after 1.5 hours, in 70 DEG C of baking ovens dry 12 hours, then 400 DEG C of roastings 3 hours in Muffle furnace, obtained cerium manganese composite oxides Ce1Mn9.
Taking 0.200 g Ce1Mn9 catalyst, to be placed in external diameter be Φ 6, and internal diameter is in the U-shaped reaction tube of Φ 4, then puts into 25 DEG C of water-baths, passes into 10ppm NO reaction gas, and all the other are air, and air speed is 110000 mLg
-1h
-1, the highest elimination factor of NO is 98 %.
embodiment 11:
Take 6.58 g neodymium nitrates, 2.97 g manganese chlorides are dissolved in 40 mL water, at room temperature stir, drip the oxalic acid aqueous solution of 25 mL1.78 mol/L, continuation stirring filtration washing after 1.5 hours, in 70 DEG C of baking ovens dry 12 hours, then 400 DEG C of roastings 3 hours in Muffle furnace, obtained neodymium manganese composite oxide Nd1Mn1.
Taking 0.200 g Nd1Mn1 catalyst, to be placed in external diameter be Φ 6, and internal diameter is in the U-shaped reaction tube of Φ 4, then puts into 25 DEG C of water-baths, passes into 10ppm NO reaction gas, and all the other are air, and air speed is 110000 mLg
-1h
-1, the highest elimination factor of NO is 6 %.
embodiment 12:
Take 3.29 g neodymium nitrates, 4.45 g manganese chlorides are dissolved in 40 mL water, at room temperature stir, drip the oxalic acid aqueous solution of 25 mL1.78 mol/L, continuation stirring filtration washing after 1.5 hours, in 70 DEG C of baking ovens dry 12 hours, then 400 DEG C of roastings 3 hours in Muffle furnace, obtained neodymium manganese composite oxide Nd1Mn3.
Taking 0.200 g Nd1Mn3 catalyst, to be placed in external diameter be Φ 6, and internal diameter is in the U-shaped reaction tube of Φ 4, then puts into 25 DEG C of water-baths, passes into 10ppm NO reaction gas, and all the other are air, and air speed is 110000 mLg
-1h
-1, the highest elimination factor of NO is 20 %.
embodiment 13:
Take 2.19 g neodymium nitrates, 4.95 g manganese chlorides are dissolved in 40 mL water, at room temperature stir, drip the oxalic acid aqueous solution of 25 mL1.78 mol/L, continuation stirring filtration washing after 1.5 hours, in 70 DEG C of baking ovens dry 12 hours, then 400 DEG C of roastings 3 hours in Muffle furnace, obtained neodymium manganese composite oxide Nd1Mn5.
Taking 0.200 g Nd1Mn5 catalyst, to be placed in external diameter be Φ 6, and internal diameter is in the U-shaped reaction tube of Φ 4, then puts into 25 DEG C of water-baths, passes into 10ppm NO reaction gas, and all the other are air, and air speed is 110000 mLg
-1h
-1, the highest elimination factor of NO is 58 %.
embodiment 14:
Take 1.64 g neodymium nitrates, 5.19 g manganese chlorides are dissolved in 40 mL water, at room temperature stir, drip the oxalic acid aqueous solution of 25 mL1.78 mol/L, continuation stirring filtration washing after 1.5 hours, in 70 DEG C of baking ovens dry 12 hours, then 400 DEG C of roastings 3 hours in Muffle furnace, obtained neodymium manganese composite oxide Nd1Mn7.
Taking 0.200 g Nd1Mn7 catalyst, to be placed in external diameter be Φ 6, and internal diameter is in the U-shaped reaction tube of Φ 4, then puts into 25 DEG C of water-baths, and pass into 10 ppm NO reaction gases, all the other are air, and air speed is 110000 mLg
-1h
-1, the highest elimination factor of NO is 99 %.
embodiment 15:
Take 1.32 g neodymium nitrates, 5.34 g manganese chlorides are dissolved in 40 mL water, at room temperature stir, drip the oxalic acid aqueous solution of 25 mL1.78 mol/L, continuation stirring filtration washing after 1.5 hours, in 70 DEG C of baking ovens dry 12 hours, then 400 DEG C of roastings 3 hours in Muffle furnace, obtained neodymium manganese composite oxide Nd1Mn9.
Taking 0.200 g Nd1Mn9 catalyst, to be placed in external diameter be Φ 6, and internal diameter is in the U-shaped reaction tube of Φ 4, then puts into 25 DEG C of water-baths, and pass into 10 ppm NO reaction gases, all the other are air, and air speed is 110000 mLg
-1h
-1, the highest elimination factor of NO is 99 %.
Claims (6)
1. low concentration nitric oxide eliminates a preparation method for catalyst, and it is characterized in that, this catalyst is rear-earth-doped manganese base composite oxidate, and for the elimination of low concentration nitric oxide, concrete steps are as follows:
Rare-earth salts and manganese salt are dissolved in 40 ml waters, stirring at normal temperature also drips 25 milliliters of oxalic acid solutions and makes precipitation, continue stirring 1.5 hours, 70 DEG C of baking ovens are put into dry 12 hours after the suspension obtained is carried out filtration washing, then Muffle furnace 400 DEG C of roastings 3 hours are put into, obtained rare earth manganese base composite oxidate.
2. a kind of low concentration nitric oxide according to claim 1 eliminates the preparation of catalyst, it is characterized in that, described rare-earth salts is lanthanum nitrate, lanthanum chloride, cerous nitrate, cerous sulfate, neodymium nitrate, one in neodymium chloride or its combination, described manganese salt is manganese nitrate, the one in manganese chloride or its combination.
3. a kind of low concentration nitric oxide according to claim 1 and 2 eliminates the preparation of catalyst, it is characterized in that, described manganese salt and the ratio of rare-earth salts are 1 ~ 9, and rare earths salt concentration is 0.07 ~ 0.4 mol/L, and described manganese salt solution concentration is 0.4 ~ 0.7 mol/L.
4. a kind of low concentration nitric oxide according to claim 1 eliminates the preparation of catalyst, and it is characterized in that, described oxalic acid solution concentration is 1.5 ~ 2.5 mol/L.
5. low concentration nitric oxide eliminates a catalyst, and it is characterized in that, according to above-mentioned arbitrary claim, method prepares.
6. a kind of low concentration nitric oxide eliminates catalyst for nitric oxide catalytic oxidation, at normal temperatures and pressures efficiently catalyzing and oxidizing nitric oxide according to claim 5.
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Cited By (5)
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| CN104801314A (en) * | 2015-04-22 | 2015-07-29 | 上海纳米技术及应用国家工程研究中心有限公司 | Preparation of iron, cerium and manganese catalyst for eliminating low-concentration nitric oxide at normal temperature |
| CN105561973A (en) * | 2016-01-15 | 2016-05-11 | 上海交通大学 | Chromium-based NO normal temperature oxidation catalyst and preparation method and application thereof |
| CN106732644A (en) * | 2016-11-22 | 2017-05-31 | 上海纳米技术及应用国家工程研究中心有限公司 | A kind of supported by cobalt oxide cerium manganese composite oxides and preparation and application |
| CN111185154A (en) * | 2020-03-05 | 2020-05-22 | 上海纳米技术及应用国家工程研究中心有限公司 | Integral chromium-manganese-nitrogen monoxide purifying catalyst and preparation method and application thereof |
| CN111774068A (en) * | 2020-07-08 | 2020-10-16 | 上海纳米技术及应用国家工程研究中心有限公司 | Preparation method of integral manganese oxide nitric oxide purification catalyst, product and application thereof |
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Cited By (7)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN104801314A (en) * | 2015-04-22 | 2015-07-29 | 上海纳米技术及应用国家工程研究中心有限公司 | Preparation of iron, cerium and manganese catalyst for eliminating low-concentration nitric oxide at normal temperature |
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| CN106732644A (en) * | 2016-11-22 | 2017-05-31 | 上海纳米技术及应用国家工程研究中心有限公司 | A kind of supported by cobalt oxide cerium manganese composite oxides and preparation and application |
| CN111185154A (en) * | 2020-03-05 | 2020-05-22 | 上海纳米技术及应用国家工程研究中心有限公司 | Integral chromium-manganese-nitrogen monoxide purifying catalyst and preparation method and application thereof |
| CN111185154B (en) * | 2020-03-05 | 2022-04-05 | 上海纳米技术及应用国家工程研究中心有限公司 | Integral chromium-manganese-nitrogen monoxide purifying catalyst and preparation method and application thereof |
| CN111774068A (en) * | 2020-07-08 | 2020-10-16 | 上海纳米技术及应用国家工程研究中心有限公司 | Preparation method of integral manganese oxide nitric oxide purification catalyst, product and application thereof |
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