CN104667947A - Block distributed noble metal composite oxide VOCs catalyst and preparation method thereof - Google Patents
Block distributed noble metal composite oxide VOCs catalyst and preparation method thereof Download PDFInfo
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- CN104667947A CN104667947A CN201510075529.4A CN201510075529A CN104667947A CN 104667947 A CN104667947 A CN 104667947A CN 201510075529 A CN201510075529 A CN 201510075529A CN 104667947 A CN104667947 A CN 104667947A
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Abstract
The invention belongs to the technical field of environmental protection and in particular relates to a block distributed noble metal composite oxide VOCs catalyst and a preparation method thereof. According to the technical scheme disclosed by the invention, for the block distributed noble metal composite oxide VOCs catalyst, cordierite honeycomb ceramics are taken as a carrier, and a basic coating is distributed on a honeycomb pore channel of the carrier, wherein the materials of the basic coating include gamma-Al2O3, ceria-zirconium solid solutions and oxide catalysts; and noble metal catalyst layers are distributed on the materials of the basic coating. According to the catalyst prepared by the invention, fast light-off of the catalyst can be realized, and the activity is greatly improved. Moreover, according to combustion heat generated after fast light-off, the catalytic reaction can be accelerated, so the indexes of the catalyst disclosed by the invention, such as the light-off temperature and conversion rate of organic gases, are superior to those of various existing catalysts.
Description
Technical field
The invention belongs to environmental protection technical field, particularly relate to a kind of block distributed noble metal composite oxide VOCs catalyst and preparation method.
Background technology
VOCs(VOC) main from industries such as petrochemical industry, chemical synthesis, bio-pharmaceuticals, refuse disposal, sewage disposal, organic solvent, leather, printing and dyeing, chemical assistant, feed manufacturing, causing very large impact to health and environment, is the main producers thing of PM2.5.Current national government and environmental protection department pay much attention to its problem of environmental pollution brought, and the discharge standard about VOCs is constantly adding sternly.
Foul gas Treatment process mainstream technology is thermal oxidation method both at home and abroad at present, namely utilizes the method such as high-temp combustion, heat-accumulation combustion to carry out thermal oxide decomposition to VOCs, more thoroughly VOCs can be oxidized to innocuous gas.
Increasing thermal oxide equipment in view of the feature of gas treatment, needs thermal oxide equipment can be fully oxidized by VOCs within very short time, the secondary pollutions such as oxynitrides, bioxin can be produced due to high-temp combustion, so have employed the mode of catalytic oxidation.The use of catalyst, can reduce reaction temperature greatly, play the effect of saving energy consumption and avoiding secondary pollution, and catalyst serves more and more important effect in thermal oxide equipment.
The forms such as current VOCs catalyst many employings noble metal, spinel oxides, perofskite type oxide, these catalyst materials cut both ways.As best in noble metal catalyst catalytic effect, but expensive and anti-Poisoning is poor, and the organic gas of oxide catalyst for process has certain selective and effect relative to noble metal less stable.
Therefore, reasonably designing catalyst material, enable that catalyst is more effective to play a role, make catalytic effect and economy can reach good unification, and increase the Stability and adaptability of catalyst, is technical problem urgently to be resolved hurrily at present.
Summary of the invention
The object of the invention is to, overcome the deficiencies in the prior art, provide a kind of block distributed noble metal composite oxide VOCS catalyst and preparation method, this technology adopts the carrier of cordierite honeycomb ceramic as catalyst of Heat stability is good, the honeycomb duct of carrier is distributed with subcoat, and the material of subcoat is γ-Al
2o
3, cerium zirconium sosoloid and oxide catalyst, subcoat is distributed with noble metal catalyst coating.
With catalyst prepared by this technology, compare simple noble metal catalyst, greatly can reduce the use amount of noble metal, and pass through the corresponding block of less noble metal reasonable layout in coating, good catalytic action can be played by some large molecules stronger to non-oxidizability in VOCs, reach fast oxidative effect.Meanwhile, by oxide catalyst reasonable layout lower for cost at the bottom of coating and internal microcellular structure, effectively catalysis can be carried out to micro-molecular gas.The reasonable layout of two kinds of catalyst materials, can play good catalytic effect, greatly reduces again the use amount of noble metal, has saved cost.
For solving the problems of the technologies described above, technical scheme of the present invention is: a kind of block distributed noble metal composite oxide VOC
scatalyst, with cordierite honeycomb ceramic as carrier, the honeycomb duct of carrier is distributed with subcoat, and base coating material comprises γ-Al
2o
3, cerium zirconium sosoloid and oxide catalyst.The cerium zirconium ratio of cerium zirconium sosoloid is (3 ~ 7): (7 ~ 3), and oxide catalytic materials is Mn-Cu-Fe-Co composite oxide, mass ratio MnO:CuO:Fe
2o
3: Co
3o
4=(5 ~ 8): (2 ~ 4): (1 ~ 3): (1 ~ 2), the mass ratio of γ-Al2O3, cerium zirconium sosoloid, oxide catalyst is (15 ~ 25): 1:(2 ~ 10).In subcoat preparation process, oxide catalyst fully mixes with aluminium oxide, and evenly and go deep into its microcellular structure, the thickness of subcoat is 0.4 ~ 0.5mm to substep.Base coating material is distributed with noble metal catalyst layer, and the more distribution and concentrations of noble metal catalyst are at the surface location of subcoat.
Precious metal catalyst agent material of the present invention is porpezite Pd.
A preparation method for block distributed noble metal composite oxide VOCS catalyst, comprises the following steps:
1) subcoat slurry is prepared: oxide catalytic materials, γ-Al
2o
3mix in mass ratio with cerium zirconium sosoloid, and add clear water and carry out grinding in 8 ~ 12 hours, grinding disposed slurry solid containing being 25% ~ 35%, powder diameter is 5 ~ 20 μm;
2) apply subcoat: be 200cpsi(hole count/square inch with hole order number) cordierite honeycomb ceramic as carrier, by carrier impregnation in subcoat slurry, slurry is made to be distributed on the pore passage structure of cordierite honeycomb ceramic carrier, and blow out slurry unnecessary in honeycomb ceramic carrier hole with the Compressed Gas of 0.1MPa, 110 DEG C of-120 DEG C of dryings 2 ~ 2.5 hours, 450 ~ 500 DEG C of roasting 5-6 hour; Slurry like this containing metal oxide just completes the distribution in cordierite honeycomb ceramic carrier duct.The subcoat total content of ceramic monolith reaches 80 ~ 100g/L, and coating layer thickness is 0.4 ~ 0.5mm.
3) noble metal catalyst coating is applied: it is in the palladium nitrate solution of 0.5 ~ 5% that semi-finished product previous step made immerse mass concentration, flood and take out after 20 ~ 30 seconds, remaining liq in duct is blown away with 0.1MPa compressed air, again 110 DEG C of-120 DEG C of air dryings 2 ~ 2.5 hours, and roasting 3 ~ 4 hours in 500 DEG C ~ 550 DEG C air, cooling, obtains catalyst final products.Bullion content reaches 0.2 ~ 0.5g/L, and coating layer thickness is ignored.
The present invention adopts multiple step format coated technique, and reach the object of catalyst block distribution, oxide catalyst is more distributed in the internal gutter structure of high-specific surface area coating material, carries out catalytic action for the Small molecular more easily entering duct.Noble metal catalyst is more enriched in the surface of coating material and outside pore passage structure, carries out catalytic action for the large molecule being not easy to enter duct.The compound use of two kinds of catalyst, can either fall the use amount of noble metal, reduce costs, and also can reach good catalytic effect simultaneously.
The noble metal catalyst material selection porpezite Pd of this patent, compared to Pd-Pt system noble metal conventional at present, material unit price reduces by 60%, and noble metal total amount reduces by 70%, and oxidisability is better, and initiation temperature is lower.Oxide catalytic materials selects Mn-Cu-Fe-Co composite oxide, to different VOC
sapplicability stronger.
Rational coated technique is the key of different catalysts material being carried out block distribution, the catalyst of patent of the present invention adopts substep coated technique: first, namely oxide catalytic materials adds in the lump and jointly grinds in the process of lapping of base material, thus subcoat microcellular structure in import oxide catalytic materials fully.Slurry after grinding is distributed in the duct of cordierite ceramic honeycomb carrier by infusion process, and the carrier after dipping carries out drying and roasting.Then, noble metal catalyst material soaking imports coating structure, is more enriched in the surface structure of coating.
The invention has the beneficial effects as follows: catalyst prepared by the present invention, a small amount of noble metal catalyst is enriched in coating surface and shallow-layer, and can make catalyst Fast light-off, activity improves greatly.And the combustion heat produced after Fast light-off can promote accelerating of catalytic reaction, so be better than current various catalyst in the index such as conversion ratio of initiation temperature, organic gas.Complete oxidation large molecular gas is not thoroughly had, the micro-molecular gas that its incomplete reaction produces on top layer, and VOC
sin other micro-molecular gas, coating bottom sheaf space can be diffused into, carry out catalytic oxidation by oxide catalyst.
The present invention, by appropriate design catalyst material, can make VOC
sgas is Fast light-off also fully reaction within short time and little space, reaches the object of Purge gas, catalyst technology of the present invention, can be applicable to the VOC of chemical industry, application, printing, printing and dyeing etc. association area
son thermal oxidation equipment, above-mentioned technology, has taken into account catalyst cost and performance, achieves satisfied effect.
Detailed description of the invention
embodiment 1
A kind of block distributed noble metal composite oxide VOC
scatalyst, with cordierite honeycomb ceramic as carrier, the honeycomb duct of carrier is distributed with subcoat, and base coating material comprises γ-Al
2o
3, cerium zirconium sosoloid and oxide catalyst.The cerium zirconium ratio of cerium zirconium sosoloid is 6:4, and oxide catalytic materials is Mn-Cu-Fe-Co composite oxide, and its total content is 15 g/L, mass ratio MnO:CuO:Fe
2o
3: Co
3o
4the mass ratio of=8:3:1.5:2, γ-Al2O3, cerium zirconium sosoloid, oxide catalyst is 20:1:7.5.In subcoat preparation process, oxide catalyst fully mixes with aluminium oxide, and evenly and go deep into its microcellular structure, the thickness of subcoat is 0.4 ~ 0.5mm to substep.Base coating material is distributed with noble metal catalyst layer, and the more distribution and concentrations of noble metal catalyst are at the surface location of subcoat, and bullion content is 0.2g/L, and precious metal catalyst agent material of the present invention is porpezite Pd.
A preparation method for block distributed noble metal composite oxide VOCS catalyst, comprises the following steps:
1) subcoat slurry is prepared: oxide catalytic materials, γ-Al
2o
3mix in mass ratio with cerium zirconium sosoloid, and add clear water and carry out grinding in 8-12 hour, grinding disposed slurry solid containing being 25% ~ 35%, powder diameter is 5 ~ 20 μm;
2) apply subcoat: be 200cpsi(hole count/square inch with hole order number) cordierite honeycomb ceramic as carrier, by carrier impregnation in subcoat slurry, slurry is made to be distributed on the pore passage structure of cordierite honeycomb ceramic carrier, and blow out slurry unnecessary in honeycomb ceramic carrier hole with the Compressed Gas of 0.1MPa, through 110 DEG C of-120 DEG C of dry 2-2.5 hour, 450 DEG C-500 DEG C roasting 5-6 hour; The base coating material total content of ceramic monolith is 80 ~ 100g/L, and coating layer thickness is 0.4 ~ 0.5mm.
3) noble metal catalyst coating is applied: it is in the palladium nitrate solution of 0.5 ~ 5% that semi-finished product previous step made immerse mass concentration, flood and take out after 20 ~ 30 seconds, remaining liq in duct is blown away with 0.1MPa compressed air, again 110 DEG C of-120 DEG C of air dryings 2 ~ 2.5 hours, and roasting 3 ~ 4 hours in 500 DEG C ~ 550 DEG C air, cooling, obtain catalyst final products, coating layer thickness is ignored.
Following table 1 is the noble metal catalyst of catalyst of the present invention and prior art, oxide catalyst contrasts processing certain test effect printing waste gas.
Table 1
embodiment 2
A kind of block distributed noble metal composite oxide VOC
scatalyst, with cordierite honeycomb ceramic as carrier, the honeycomb duct of carrier is distributed with subcoat, and base coating material comprises γ-Al
2o
3, cerium zirconium sosoloid and oxide catalyst etc.The cerium zirconium ratio of cerium zirconium sosoloid is 4:6, and oxide catalytic materials is Mn-Cu-Fe-Co composite oxide, and total content is 12 g/L, mass ratio MnO:CuO:Fe
2o
3: Co
3o
4the mass ratio of=7:3:2:1, γ-Al2O3, cerium zirconium sosoloid, oxide catalyst is 25:1:8.In subcoat preparation process, oxide catalyst fully mixes with aluminium oxide, and evenly and go deep into its microcellular structure, the thickness of subcoat is 0.4 ~ 0.5mm to substep.Base coating material is distributed with noble metal catalyst layer, and the more distribution and concentrations of noble metal catalyst are at the surface location of subcoat, and bullion content is 0.4g/L, and precious metal catalyst agent material of the present invention is porpezite Pd.
A preparation method for block distributed noble metal composite oxide VOCS catalyst, with embodiment 1.
Following table 2 is the noble metal catalyst of catalyst of the present invention and prior art, oxide catalyst is processing the test effect contrast table of certain coating waste gas.
Table 2
embodiment 3
A kind of block distributed noble metal composite oxide VOC
scatalyst, with cordierite honeycomb ceramic as carrier, the honeycomb duct of carrier is distributed with subcoat, and base coating material comprises γ-Al
2o
3, cerium zirconium sosoloid and oxide catalyst etc.The cerium zirconium ratio of cerium zirconium sosoloid is 3:7, and oxide catalytic materials is Mn-Cu-Fe-Co composite oxide, and total content is 20 g/L, mass ratio MnO:CuO:Fe
2o
3: Co
3o
4the mass ratio of=6:3:2:1, γ-Al2O3, cerium zirconium sosoloid, oxide catalyst is 15:1:6.In subcoat preparation process, oxide catalyst fully mixes with aluminium oxide, and evenly and go deep into its microcellular structure, the thickness of subcoat is 0.4 ~ 0.5mm to substep.Base coating material is distributed with noble metal catalyst layer, and the more distribution and concentrations of noble metal catalyst are at the surface location of subcoat, and bullion content is 0.4g/L, and precious metal catalyst agent material of the present invention is porpezite Pd.
A preparation method for block distributed noble metal composite oxide VOCS catalyst, with embodiment 1.
Following table 3 is the noble metal catalyst of catalyst of the present invention and prior art, oxide catalyst is processing the test effect contrast table of certain chemical emission.
Table 3
Claims (7)
1. a block distributed noble metal composite oxide VOC
scatalyst, is characterized in that: with cordierite honeycomb ceramic as carrier, the honeycomb duct of carrier is distributed with subcoat, and the material of described subcoat is γ-Al
2o
3, cerium zirconium sosoloid and oxide catalyst, subcoat is distributed with noble metal catalyst coating.
2. described block distributed noble metal composite oxide VOC according to claim 1
scatalyst, is characterized in that: the cerium zirconium mass ratio of described cerium zirconium sosoloid is (3 ~ 7): (7 ~ 3).
3. block distributed noble metal composite oxide VOC according to claim 1
scatalyst, is characterized in that: described oxide catalytic materials is Mn-Cu-Fe-Co composite oxide, mass ratio MnO:CuO:Fe
2o
3: Co
3o
4=(5 ~ 8): (2 ~ 4): (1 ~ 3): (1 ~ 2).
4. block distributed noble metal composite oxide VOCS catalyst according to claim 1, is characterized in that: described γ-Al
2o
3, cerium zirconium sosoloid, oxide catalyst mass ratio be (15 ~ 25): 1:(2 ~ 10).
5. block distributed noble metal composite oxide VOC according to claim 1
scatalyst, is characterized in that: the thickness of described subcoat is 0.4 ~ 0.5mm.
6. block distributed noble metal composite oxide VOC according to claim 1
scatalyst, is characterized in that: described precious metal catalyst agent material is porpezite Pd.
7. a block distributed noble metal composite oxide VOC
sthe preparation method of catalyst, is characterized in that: comprise the following steps:
1) subcoat slurry is prepared: oxide catalytic materials, γ-Al
2o
3mix in mass ratio with cerium zirconium sosoloid, and add clear water and carry out grinding in 8 ~ 12 hours, grinding disposed slurry solid containing being 25% ~ 35%, powder diameter is 5 ~ 20 μm;
2) apply subcoat: be 200cpsi(hole count/square inch with hole order number) cordierite honeycomb ceramic as carrier, by carrier impregnation in subcoat slurry, slurry is made to be distributed on the pore passage structure of cordierite honeycomb ceramic carrier, and blow out slurry unnecessary in honeycomb ceramic carrier hole with the Compressed Gas of 0.1MPa, through 110 ~ 120 DEG C of dryings 2 ~ 2.5 hours, 450 ~ 500 DEG C of roasting 5-6 hour;
3) noble metal catalyst coating is applied: it is in the palladium nitrate solution of 0.5 ~ 5% that semi-finished product previous step made immerse mass concentration, flood and take out after 20 ~ 30 seconds, remaining liq in duct is blown away with 0.1MPa compressed air, again 110 ~ 120 DEG C of air dryings 2 ~ 2.5 hours, and roasting 3 ~ 4 hours in 500 ~ 550 DEG C of air, cooling, obtains catalyst final products.
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| CN106607056A (en) * | 2016-12-30 | 2017-05-03 | 北京化工大学常州先进材料研究院 | Graphene supported noble metal composite oxide VOCs catalyst and preparation method thereof |
| CN106732576A (en) * | 2015-11-19 | 2017-05-31 | 中国石油化工股份有限公司 | A kind of catalyst for catalytic oxidation and its preparation method and application |
| 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 |
| CN114950423A (en) * | 2022-06-08 | 2022-08-30 | 重庆大学 | Indoor low-concentration formaldehyde purification catalyst product and preparation method thereof |
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Cited By (7)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN106732576A (en) * | 2015-11-19 | 2017-05-31 | 中国石油化工股份有限公司 | A kind of catalyst for catalytic oxidation and its preparation method and application |
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| CN106607056A (en) * | 2016-12-30 | 2017-05-03 | 北京化工大学常州先进材料研究院 | Graphene supported noble metal composite oxide VOCs catalyst and preparation method 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 |
| CN114950423A (en) * | 2022-06-08 | 2022-08-30 | 重庆大学 | Indoor low-concentration formaldehyde purification catalyst product and preparation method thereof |
| CN114950423B (en) * | 2022-06-08 | 2023-06-09 | 重庆大学 | Indoor low-concentration formaldehyde purification catalyst product and preparation method thereof |
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