CN101444746B - A preparation method of CeO*-mol sieve catalyst - Google Patents
A preparation method of CeO*-mol sieve catalyst Download PDFInfo
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- CN101444746B CN101444746B CN2009100952719A CN200910095271A CN101444746B CN 101444746 B CN101444746 B CN 101444746B CN 2009100952719 A CN2009100952719 A CN 2009100952719A CN 200910095271 A CN200910095271 A CN 200910095271A CN 101444746 B CN101444746 B CN 101444746B
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- molecular sieve
- ceo
- catalyst
- preparation
- sieve catalyst
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- 239000003054 catalyst Substances 0.000 title claims abstract description 39
- 238000002360 preparation method Methods 0.000 title claims abstract description 14
- 239000002808 molecular sieve Substances 0.000 claims abstract description 44
- URGAHOPLAPQHLN-UHFFFAOYSA-N sodium aluminosilicate Chemical compound [Na+].[Al+3].[O-][Si]([O-])=O.[O-][Si]([O-])=O URGAHOPLAPQHLN-UHFFFAOYSA-N 0.000 claims abstract description 29
- HSJPMRKMPBAUAU-UHFFFAOYSA-N cerium(3+);trinitrate Chemical compound [Ce+3].[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O HSJPMRKMPBAUAU-UHFFFAOYSA-N 0.000 claims abstract description 7
- 239000002253 acid Substances 0.000 claims abstract description 6
- 239000002994 raw material Substances 0.000 claims abstract description 4
- 238000000227 grinding Methods 0.000 claims description 3
- 238000003701 mechanical milling Methods 0.000 claims description 3
- 239000000843 powder Substances 0.000 claims description 3
- 229910052684 Cerium Inorganic materials 0.000 claims description 2
- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 claims description 2
- GWXLDORMOJMVQZ-UHFFFAOYSA-N cerium Chemical compound [Ce] GWXLDORMOJMVQZ-UHFFFAOYSA-N 0.000 claims description 2
- 229910017604 nitric acid Inorganic materials 0.000 claims description 2
- 239000007787 solid Substances 0.000 claims description 2
- XSTXAVWGXDQKEL-UHFFFAOYSA-N Trichloroethylene Chemical compound ClC=C(Cl)Cl XSTXAVWGXDQKEL-UHFFFAOYSA-N 0.000 abstract description 4
- SCYULBFZEHDVBN-UHFFFAOYSA-N 1,1-Dichloroethane Chemical class CC(Cl)Cl SCYULBFZEHDVBN-UHFFFAOYSA-N 0.000 abstract description 3
- 230000015556 catabolic process Effects 0.000 abstract description 3
- 238000006731 degradation reaction Methods 0.000 abstract description 3
- 238000000034 method Methods 0.000 abstract description 3
- -1 carrene (DCM) Chemical class 0.000 abstract description 2
- 238000006555 catalytic reaction Methods 0.000 abstract description 2
- 230000000694 effects Effects 0.000 abstract description 2
- 150000002894 organic compounds Chemical class 0.000 abstract description 2
- VEXZGXHMUGYJMC-UHFFFAOYSA-M Chloride anion Chemical compound [Cl-] VEXZGXHMUGYJMC-UHFFFAOYSA-M 0.000 description 5
- 238000002485 combustion reaction Methods 0.000 description 5
- HEDRZPFGACZZDS-UHFFFAOYSA-N Chloroform Chemical compound ClC(Cl)Cl HEDRZPFGACZZDS-UHFFFAOYSA-N 0.000 description 4
- 238000007084 catalytic combustion reaction Methods 0.000 description 4
- 238000005516 engineering process Methods 0.000 description 4
- VZGDMQKNWNREIO-UHFFFAOYSA-N tetrachloromethane Chemical compound ClC(Cl)(Cl)Cl VZGDMQKNWNREIO-UHFFFAOYSA-N 0.000 description 4
- 230000008901 benefit Effects 0.000 description 3
- 230000003197 catalytic effect Effects 0.000 description 3
- MVPPADPHJFYWMZ-UHFFFAOYSA-N chlorobenzene Chemical compound ClC1=CC=CC=C1 MVPPADPHJFYWMZ-UHFFFAOYSA-N 0.000 description 3
- 239000000203 mixture Substances 0.000 description 3
- ZAMOUSCENKQFHK-UHFFFAOYSA-N Chlorine atom Chemical compound [Cl] ZAMOUSCENKQFHK-UHFFFAOYSA-N 0.000 description 2
- VEXZGXHMUGYJMC-UHFFFAOYSA-N Hydrochloric acid Chemical compound Cl VEXZGXHMUGYJMC-UHFFFAOYSA-N 0.000 description 2
- 230000008859 change Effects 0.000 description 2
- 229910052801 chlorine Inorganic materials 0.000 description 2
- 239000000460 chlorine Substances 0.000 description 2
- 239000002131 composite material Substances 0.000 description 2
- 230000008030 elimination Effects 0.000 description 2
- 238000003379 elimination reaction Methods 0.000 description 2
- 239000003344 environmental pollutant Substances 0.000 description 2
- 230000002779 inactivation Effects 0.000 description 2
- 239000000463 material Substances 0.000 description 2
- 229910052751 metal Inorganic materials 0.000 description 2
- 239000002184 metal Substances 0.000 description 2
- 229910000510 noble metal Inorganic materials 0.000 description 2
- 231100000719 pollutant Toxicity 0.000 description 2
- 229910052761 rare earth metal Inorganic materials 0.000 description 2
- 150000002910 rare earth metals Chemical class 0.000 description 2
- 229910052723 transition metal Inorganic materials 0.000 description 2
- 150000003624 transition metals Chemical class 0.000 description 2
- 239000012855 volatile organic compound Substances 0.000 description 2
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical group [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 1
- URRQVFZTEDYPPR-UHFFFAOYSA-N ClC=C(Cl)Cl.[Cl] Chemical compound ClC=C(Cl)Cl.[Cl] URRQVFZTEDYPPR-UHFFFAOYSA-N 0.000 description 1
- 239000002841 Lewis acid Substances 0.000 description 1
- 238000004458 analytical method Methods 0.000 description 1
- 239000006227 byproduct Substances 0.000 description 1
- 229910052799 carbon Inorganic materials 0.000 description 1
- 238000001311 chemical methods and process Methods 0.000 description 1
- 238000006243 chemical reaction Methods 0.000 description 1
- 229910052804 chromium Inorganic materials 0.000 description 1
- 239000012141 concentrate Substances 0.000 description 1
- 229910052802 copper Inorganic materials 0.000 description 1
- 238000009826 distribution Methods 0.000 description 1
- 229910052737 gold Inorganic materials 0.000 description 1
- 230000036541 health Effects 0.000 description 1
- 238000010438 heat treatment Methods 0.000 description 1
- 229910052741 iridium Inorganic materials 0.000 description 1
- 229910052742 iron Inorganic materials 0.000 description 1
- 150000007517 lewis acids Chemical class 0.000 description 1
- 229910052748 manganese Inorganic materials 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 229910052759 nickel Inorganic materials 0.000 description 1
- 239000003960 organic solvent Substances 0.000 description 1
- 230000003647 oxidation Effects 0.000 description 1
- 238000007254 oxidation reaction Methods 0.000 description 1
- 238000010525 oxidative degradation reaction Methods 0.000 description 1
- 229910052763 palladium Inorganic materials 0.000 description 1
- 239000002245 particle Substances 0.000 description 1
- 229910052697 platinum Inorganic materials 0.000 description 1
- 238000012805 post-processing Methods 0.000 description 1
- 238000000746 purification Methods 0.000 description 1
- 229910052703 rhodium Inorganic materials 0.000 description 1
- 229910052707 ruthenium Inorganic materials 0.000 description 1
- 239000011265 semifinished product Substances 0.000 description 1
- 238000005245 sintering Methods 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 229960002415 trichloroethylene Drugs 0.000 description 1
- UBOXGVDOUJQMTN-UHFFFAOYSA-N trichloroethylene Natural products ClCC(Cl)Cl UBOXGVDOUJQMTN-UHFFFAOYSA-N 0.000 description 1
- 238000005303 weighing Methods 0.000 description 1
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Abstract
The present invention provides a preparation method of CeO*-mol sieve catalyst which takes cerous nitrate and molecular sieve with strong acid as raw material and takes mechanical lapping method for preparation of CeO*-mol sieve catalyst, wherein mass ratio of CeO<SUB>2</SUB>/molecular sieve in the catalyst is 8/1-1/10, and molecular sieve as one of H-USY, H-SSY, H-ZSM-5 or H-BETA molecular sieve. The process is simple, cost low, and has good catalysis and degradation activity and stability to chloring-containing organic compounds like carrene (DCM), dichloroethanes (DCE) and ethinyltrichloride (TCE).
Description
Technical field
The present invention relates to a kind of preparation method of chloride organic exhaust gas combustion catalyst, particularly relate to CeO
2The preparation method of-molecular sieve catalyst.
Background technology
Chloride VOC (CVOCs) is a kind of of VOCs pollutant, common have carrene (DCM), chloroform (CF), dichloroethanes (DCE), trichloro-ethylene (TCE), carbon tetrachloride (CT), a chlorobenzene (PhCl) etc., and they are as a kind of organic solvent commonly used and the semi-finished product in the chemical process and be widely used.But this class material has great harm to environment and health.For the removal of chlorinated organics, the method for main at present employing flame combustion is carried out post processing.With the heat treatment phase ratio, catalytic combustion is because its advantage technical and economically, is handle important of VOCs pollutant purification and one of effective means very, equally, also more and more is subjected to people's attention in the application aspect the elimination CVOCs.Great majority all concentrate on following four class catalyst about the research report of CVOCs catalyst for catalytic combustion: noble metal, transition metal, rare earth and composite oxides thereof, molecular sieve and metal load type molecular sieve thereof.Yet noble metal catalyst and transition-metal catalyst as Pt, Pd, Ru, Rh, Ir, Au, Cu, Co, Ni, Mn, Fe, Cr, Ag, V etc., have advantages of high catalytic activity to the oxidative degradation of CVOCs, but are easily poisoned and inactivation by product hydrochloric acid and chlorine.Molecular screen material and metal load type molecular sieve thereof have good architectural characteristic, has Stability Analysis of Structures as Y molecular sieve, the acid strength height, characteristics such as acid density is big, have Bronsted acid center and Lewis acid centers, become the research focus in this field, yet CVOCs easily produces many chlorine of accessory substance thing on these catalyst surfaces, catalyst is carbon distribution and inactivation easily also.Rare earth and composite oxides thereof are as one pack system CeO
2Be catalyst, in the reaction of catalysis elimination CVOCs, show good oxidation susceptibility, also caused people's extensive concern.Therefore, the chloride efficiently organic exhaust gas combustion catalyst of exploitation has great importance for the extensive use of catalytic combustion technology.
Summary of the invention
The purpose of this invention is to provide a kind of chloride efficiently organic exhaust gas combustion catalyst, specifically be meant CeO
2The preparation method of-molecular sieve catalyst.
CeO provided by the invention
2The preparation method of-molecular sieve catalyst is raw material with cerous nitrate with having highly acid molecular sieve, adopts mechanical milling method to prepare CeO
2-molecular sieve catalyst.CeO in the catalyst
2The mass ratio of/molecular sieve is 8/1~1/10; CeO
2The preparation process of-molecular sieve catalyst is: by described CeO
2The mass ratio of/molecular sieve is with molecular sieve powder and the inferior cerium [Ce (NO of solid nitric acid
3)
36H
2O] direct mixed grinding, grind to make and mix, then 100 ℃ dry 2 hours down, 350 ℃ of following roastings 0.5 hour were handled 500~650 ℃ of following roastings in 2 hours again, made CeO
2-molecular sieve catalyst.
Molecular sieve of the present invention is a kind of of H-USY, H-SSY, H-ZSM-5 or H-BETA molecular sieve.
CeO of the present invention
2CeO in the-molecular sieve catalyst
2The optimum quality ratio of/molecular sieve is 2/1~1/8.
CeO provided by the present invention
2The preparation method of-molecular sieve catalyst, its advantage is: adopting the cheap cerous nitrate and the molecular sieve of suitability for industrialized production is raw material, adopts mechanical milling method to make CeO
2-molecular sieve catalyst, preparation technology is simple, and the catalyst cost is low.It is a kind of chloride efficiently organic exhaust gas combustion catalyst, this catalyst has good catalytic degradation active and stable to carrene (DCM), dichloroethanes (DCE) and trichloro-ethylene chlorine-containing organic compounds such as (TCE), and the extensive use of catalytic combustion technology is had great importance.
The specific embodiment:
Embodiment 1
Take by weighing 2.52g cerous nitrate and 8.0g molecular sieve (H-USY, H-SSY, H-ZSM-5 or H-BETA) powder respectively, mix the back and grind, it is even to be ground to mixture.Then 100 ℃ dry 2 hours down, 350 ℃ of following roastings 0.5 hour were handled 550 ℃ of following roastings in 2 hours again, made CeO
2-molecular sieve catalyst, CeO in this catalyst
2The mass ratio of/molecular sieve is 1/8.
Embodiment 2
With embodiment 1 identical operations, difference is: change the consumption of cerous nitrate into 15.14g, the consumption of H-USY molecular sieve changes 3.0g into, CeO in this catalyst
2The mass ratio of/molecular sieve is 2/1.
Embodiment 3
With embodiment 1 identical operations, difference is: change the consumption of cerous nitrate into 20.18g, the consumption of H-USY molecular sieve changes 1.0g into, changes 550 ℃ sintering temperatures into 650 ℃, CeO in this catalyst
2The mass ratio of/molecular sieve is 8/1.
Catalyst is as shown in the table to the catalytic degradation activity of chlorinated organics in 1~3 example:
Annotate: 0.3ml, particle diameter are 60-80 purpose catalyst, and air speed is 10000h
-1
Claims (2)
1. CeO
2The preparation method of-molecular sieve catalyst is characterized in that, is raw material with cerous nitrate with having highly acid molecular sieve, adopts mechanical milling method to prepare CeO
2-molecular sieve catalyst, described highly acid molecular sieve are a kind of of H-USY, H-SSY, H-ZSM-5 or H-BETA molecular sieve, CeO in the catalyst
2The mass ratio of/molecular sieve is 8/1~1/10; Preparation process is: by described CeO
2The mass ratio of/molecular sieve, with molecular sieve powder and the direct mixed grinding of the inferior cerium of solid nitric acid, grinding makes and mixes; Then 100 ℃ dry 2 hours down, 350 ℃ of following roastings 0.5 hour were handled 500~650 ℃ of following roastings in 2 hours again, made CeO
2-molecular sieve catalyst.
2. CeO according to claim 1
2The preparation method of-molecular sieve catalyst is characterized in that: described CeO
2The optimum quality ratio of/molecular sieve is 2/1~1/8.
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CN102784557A (en) * | 2011-05-18 | 2012-11-21 | 王文初 | Method and device for treating pharmaceutical and chemical waste gases |
CN102627287B (en) * | 2012-04-20 | 2014-04-16 | 浙江大学 | Method for synthesizing molecular sieve under solvent-free condition through grinding solid phase raw materials |
CN102773072A (en) * | 2012-07-29 | 2012-11-14 | 南京工业大学 | Cerium element-modified mesoporous silica adsorbent and preparation method for adsorbent and application in gasoline desulfurization |
CN108993134B (en) | 2018-07-16 | 2021-05-25 | 天津大学 | Method for degrading ester VOCs (volatile organic compounds) by using low-temperature microwave-enhanced cerium oxide-loaded palladium monatomic catalyst |
CN109126290A (en) * | 2018-09-20 | 2019-01-04 | 俞小峰 | A kind of high-strength anti-flaming air filting material and preparation method thereof |
CN112295588B (en) * | 2020-09-23 | 2024-04-02 | 山西晟莱再生资源科技有限公司 | Preparation and application of catalyst for catalytic conversion of pyrolysis oil gas of waste tires |
CN112619693B (en) * | 2021-01-11 | 2022-07-12 | 南京大学 | Low-temperature denitration catalyst and application thereof |
CN113617380A (en) * | 2021-08-17 | 2021-11-09 | 安徽工业大学 | Preparation method of HZSM-5 molecular sieve modified high-performance cerium-based denitration catalyst |
CN115518673A (en) * | 2022-10-25 | 2022-12-27 | 浙江大学 | Preparation method of Pt-CeTi composite molecular sieve catalyst for efficiently degrading VOCs (volatile organic compounds) |
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