CN105289298A - Catalytic module capable of removing formaldehyde at room temperature and preparation method thereof - Google Patents
Catalytic module capable of removing formaldehyde at room temperature and preparation method thereof Download PDFInfo
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- CN105289298A CN105289298A CN201510709013.0A CN201510709013A CN105289298A CN 105289298 A CN105289298 A CN 105289298A CN 201510709013 A CN201510709013 A CN 201510709013A CN 105289298 A CN105289298 A CN 105289298A
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Abstract
The invention discloses a catalytic module capable of removing formaldehyde at room temperature and a preparation method thereof. The catalytic module comprises a skeleton carrier, coatings and catalyst layers, the skeleton carrier is a foam ceramic structure with three-dimensional pore channels, and the foam ceramic structure is internally provided with multiple pore channels which are interwoven into a net-shaped structure and arranged in any one of the X direction, the Y direction and the Z direction; the coatings are evenly coated on the surfaces of the pore channels in the foam ceramic structure and the other surface of the foam ceramic structure, and the catalyst layers are highly dispersed on the coatings. By means of the catalytic module capable of removing the formaldehyde at the room temperature and the preparation method thereof, at the room temperature and environment humidity, low-concentration formaldehyde can be oxidized into H2O and CO2, excellent low-temperature activity and removing efficiency are achieved, and the formaldehyde removing efficiency can be kept above 98 percent at the airspeed SV equal to 50,000 h<-1>. The preparation process is simple, the precious metal load is low, and accessory equipment such as light sources and heating are not needed. The catalytic module is suitable for air purification of closed and semi-closed spaces such as living rooms, office buildings, schools, dormitories, shopping malls, furniture markets and automobiles.
Description
Technical field
The present invention relates to a kind of environmental catalysis material for purifying air and preparation method, belonging to technical field of air purification, be specifically related to catalytic module eliminating formaldehyde and preparation method thereof under a kind of room temperature.
Background technology
As everyone knows, formaldehyde is a kind of toxic gas of colourless, irritant smell at ambient temperature, be the pollutant that room air pollution Poisoning is the strongest, formaldehyde is defined as carcinogenic, mutagenesis and deforming material by the World Health Organization, is generally acknowledged allergen.Formaldehyde brings severe threat, when air formaldehyde concentration is more than 0.10mg/m to the existence of people and health
3time can the obvious stimulation upper respiratory tract.The harm of formaldehyde to children and pregnant woman is larger, and the statistics display of Environment Protect in China association, once carried out luxurious finishing in the leukemia children man of 90%, and died from the children of luxurious finishing every year up to 2,100,000, and pregnant woman's miscarriage of 70% and indoor formaldehyde exceed standard relevant.China " air quality standard " (GB/T18832-2002) specifies, the maximum permissible concentration of indoor formaldehyde is 0.10mg/m
3, under room temperature, be about 0.07ppm.Main its of formaldehyde in room air is mainly derived from building decoration and finishing material, the ornament materials such as particieboard, fiberboard, glued board, floor glue, emulsion paint that such as furniture, floor, metope, door and window etc. are used, can within considerable time slowly, continuously release formaldehyde, and constantly assemble in indoor and cause concentration of formaldehyde to exceed standard.Therefore, exploitation efficient formaldehyde purification techniques, effectively solves the important topic that Formaldehyde Pollution of Indoor Air becomes indoor air purification.
The removing method of indoor formaldehyde mainly contains absorption, low temperature plasma, photocatalysis, catalytic oxidation and bioanalysis etc.Absorption method utilizes the formaldehyde in the absorption property absorbed air of the materials such as porous carbon, molecular sieve, silica gel, aluminium oxide, formaldehyde is enriched in adsorbent by the method, do not reach degradable object, formaldehyde when in adsorbent, enrichment reaches adsorption equilibrium gradually adsorbent lost efficacy.
Catalytic oxidation is the effective removing method of formaldehyde, can be H by oxidation of formaldehyde
2o and CO
2.The catalyst of catalyze oxidation of formaldehyde mainly contains: based on the noble metal systems of Pt, Pd, Ag, Au etc., and the base metal system that transition metal (Mn, Fe, Ni, Co, Cu, Zn etc.), complex rare-earth oxidate containing valuable metal or mixture (La, Ce, Zr, Nd, Sr, Pr etc.) are representative.Huang etc. (HuangH, LeungDYC, et.al., ACSCatal, 2011, (1) 4:348 ~ 354) utilize NaBH
4reducing process has prepared 1wt%Pd/TiO
2catalyst, SV=120000mL/ (gh), relative humidity be 50% and room temperature condition under can by the formaldehyde complete oxidation of 10ppm.(ParkSJ, BaeI, et.al., Chem.Eng.J, 2012,195-196 (0): 392 ~ 402) point out that Mn can significantly improve the activity of Pd/Beta the catalyst, (SV=50000h 40 DEG C time such as Park
-1) can by formaldehyde exhaustive oxidation.(ZhangC, HeH, et.al., Catal.Today, 2007,126 (3-4): 345 ~ 350) at TiO such as Zhang
2the different noble metal of area load, 1wt%Pt/TiO
2at 20 DEG C and SV=50000h
-1can by the formaldehyde complete oxidation of 100ppm.(PengJ, WangS.Appl.Catal., B, 2007,74 (3-4): 282 ~ 291) by 0.6wt%Pt/TiO such as Peng
2for formaldehyde through catalytic oxidation, the conversion ratio of catalyst PARA FORMALDEHYDE PRILLS(91,95) when room temperature and 60 DEG C is respectively 40%, 99.6%.The Pt/TiO that Nie etc. (NieL, YuJ, et.al., Environ.Sci.Technol, 2013,47 (6): 2777-2783) utilize Na to adulterate
2catalyst oxidation of formaldehyde, can be down to 15ppm by concentration of formaldehyde by 253ppm in 60min.Patent US5585083 is by 12wt%Pt/SnO
2catalyst, can by formaldehyde exhaustive oxidation at-5 ~ 25 DEG C for eliminating formaldehyde in air, and high noble-metal-supported amount makes to improve catalyst cost, limits its application.Patent CN1698932A utilizes Au/ rare earth oxide catalyze oxidation of formaldehyde, but catalyst at a higher temperature (80 ~ 100 DEG C) PARA FORMALDEHYDE PRILLS(91,95) have good catalytic activity, limit the extensive use of catalyst.Patent CN103127952A utilizes Ag/ZSM-5 to eliminate formaldehyde at ambient temperature, does not investigate running time, water vapour to the impact of catalytic performance.Patent CN101274281A has invented a kind of Pt/Co-Ce-Sn/ cordierite honeycomb catalyst of Mo, Cu, Mn and Ti modification, is that 70% time PARA FORMALDEHYDE PRILLS(91,95) has good catalytic activity at 18 DEG C and relative humidity.Patent CN102247842A eliminates the Pt/TiO of formaldehyde under disclosing a kind of room temperature
2-SnO
2/ cordierite monolithic catalyst, under room temperature and environmental damp condition, PARA FORMALDEHYDE PRILLS(91,95) has good removal effect.Above-mentioned patent, using straight hole shape cordierite honeycomb as carrier framework, limits the extensive use of catalyst.
There is the shortcomings such as low temperature active difference, life-span short and range of application is narrow for the catalyst of oxidation of formaldehyde under room temperature, existing monoblock type catalytic module adopts straight hole shape cordierite honeycomb ceramic to be carrier framework, be unfavorable for the absorption of reaction molecular and the desorption of product molecule, reduce catalyst efficiency.
Summary of the invention
For defect and the deficiency of prior art, the object of the present invention is to provide a kind of 3D of having pore passage structure, the catalytic module of formaldehyde can be eliminated under room temperature and ambient humidity, adopt conventional metal oxides and a small amount of noble metal as the active component of catalytic module; Catalytic module oxidation of formaldehyde has excellent low temperature active and removal efficiency, there is high stability and water repelling property simultaneously, the pressure loss before and after catalytic module is low, is applicable to that room, office buildings, school, dormitory, market, furniture market, automobile etc. are airtight, purification of air in semi-enclosed space.
Another object of the present invention is to provide a kind of preparation method preparing above-mentioned catalytic module, i.e. a kind of preparation method with the catalytic module of the oxidation of formaldehyde of 3D pore structure, overcome straight pass catalytic module shortcoming in use.
The present invention realizes foregoing invention object by the following technical solutions: the catalytic module eliminating formaldehyde under a kind of room temperature, is characterized in that, comprises skeleton carrier, coating and catalyst layer,
Described skeleton carrier is the foamed ceramics structure with 3 D pore canal, has multiple duct in described foamed ceramics structure, and described duct is mutually through and be woven into a mesh structure;
Described coating uniform is coated on channel surfaces in described foamed ceramics structure and outer surface thereof, and described catalyst layer height is dispersed in coating.
On the basis of technique scheme, the present invention can also do following improvement:
Further, the material of described foamed ceramics structure is aluminium oxide, magnesia, zeolite, cordierite, mullite, dichroite-mullite compound, carborundum, silicon nitride, magnesia, zirconium-mullite, active carbon, zirconia and fused alumina zirconia a kind of or several arbitrarily mixed materials wherein, and the arranged direction of described foamed ceramics structure inner duct is the either direction in X, Y and Z-direction;
The porosity of described foamed ceramics structure is 25 ~ 90%.
Further, being made up of coating precursor powder of described coating, described coating precursor powder is Al
2o
3, Fe
2o
3, TiO
2, SiO
2, CeO
2, ZrO
2, MgO, ZMS-5, molecular sieve, APO, SAPO, active carbon, zeolite, montmorillonite, diatomite, sepiolite, a kind of or several arbitrarily mixture in attapulgite and bentonite or wherein a kind of or several arbitrarily composite oxides or wherein a kind of or any several modified material, the coated weight of described coating is 10 ~ 150g/L.
Adopt the beneficial effect of above-mentioned further technical scheme to be coating precursor powder and coating, coating precursor powder obtains final coating after process accordingly, has stronger adhesion between coating and skeleton carrier.
Further, described catalyst layer comprises active component and adjuvant component,
Described active component be in Pd, Pt, Rh, Au, Ag or Ru any one or multiple, described active component is made up of active component precursor powder, described active component precursor powder is have a kind of or several arbitrarily mixture in the metal simple-substance of above-mentioned element, oxide, alloy, organic salt or inorganic salts, and the load capacity of described active component in coating counts 0.05 ~ 10wt% by the quality of metal simple-substance corresponding in described active component;
Described adjuvant component be in Li, Na, K, Rb, Cs, Fr, Fe, Co, Ni, Cu, Mn, Mo, Ti, Ce, Zr, Pr, Nd or Zn any one or multiple, described adjuvant component is made up of adjuvant component precursor powder, described adjuvant component precursor powder is have a kind of or several arbitrarily mixture in the metal simple-substance of above-mentioned element, oxide, alloy, organic salt or inorganic salts, and the load capacity of described adjuvant component in coating counts 0.1 ~ 20wt% by the quality of metal simple-substance corresponding in described adjuvant component.
The preparation method of the catalytic module of formaldehyde is eliminated under a kind of room temperature, prepare above-mentioned catalytic module, comprise and as follows coating is coated in described foamed ceramics body structure surface by vacuum coating methods, then utilize infusion process or the precipitation method at coating surface supported catalyst layer thus obtain the step of this catalytic module, specific operation process comprises the following steps:
(1) coating precursor powder 10 ~ 40 weight portion, binding agent 0.1 ~ 20 weight portion, coalescents 0.01 ~ 5 weight portion and deionized water are mixed, the mass ratio of described deionized water and coating precursor powder is 9:1 ~ 6:4; The slurries mixed are placed on dispersion machine, under 300 ~ 550r/min, disperse 20 ~ 60min; Then with mass concentration be 5 ~ 20% nitric acid or hydrochloric acid solution the pH of slip is adjusted to pH=3 ~ 4, continue dispersion 10 ~ 30min;
(2) after the slurries of step (1) gained are transferred to beating glue 1 ~ 2h in ball mill or sand mill, transfer in vacuum coaters storage tank, then foamed ceramics structure is placed in sample bin and carries out vacuum covering 2 ~ 20min, utilize the unnecessary slip in compressed air purging duct;
(3) the foamed ceramics structure of taking-up step (2) coating slurries, is placed in 25 ~ 40 DEG C and relative humidity is under 45 ~ 90% conditions after maintenance 4 ~ 24h, dry 1 ~ 12h in 60 ~ 120 DEG C of environment; After by the foamed ceramics through super-dry at 200 ~ 550 DEG C of roasting 1 ~ 8h, obtain covering cated foamed ceramics structure;
(4) active component solution is configured, active component precursor powder is dissolved in deionized water, then ultrasonic 10 ~ 60min under agitation, add deionized water dilution, after dilution, the volume of solution is 1:1 ~ 3:1 with the ratio of the volume of foamed ceramics structure, add protective agent again, described protective agent is 1:5 ~ 1:30 with the ratio of precious metal element content in active component precursor powder, stir 30 ~ 90min, obtain activity component impregnation liquid, wherein the concentration of the corresponding metal simple-substance of active component is 5 ~ 100mmol/mL; Configuration adjuvant component solution, adjuvant component precursor powder is added deionized water dilution, the volume after dilution is 1:1 ~ 3:1 with the ratio of the volume of foamed ceramics structure, obtains adjuvant component maceration extract, and wherein adjuvant component mass concentration is 10 ~ 50%;
(5) the activity component impregnation liquid of step (4) gained and adjuvant component maceration extract Homogeneous phase mixing are obtained mixed impregnant liquor, the cated foamed ceramics of coating obtained in step (3) is placed in mixed impregnant liquor dipping 1 ~ 10min, dry in the shade under room temperature and ambient humidity, at 50 ~ 100 DEG C of drying 1 ~ 12h, then in air or nitrogen or hydrogen stream, obtain catalytic module in 200 ~ 550 DEG C of roasting 2 ~ 8h;
Or the cated foamed ceramics that covers of step (3) gained is placed in activity component impregnation liquid dipping 1 ~ 10min, at 50 ~ 100 DEG C of drying 1 ~ 12h after drying in the shade under room temperature and ambient humidity, then adjuvant component maceration extract dipping 1 ~ 30s is placed in, at 50 ~ 100 DEG C of drying 1 ~ 12h after taking-up, then in air or nitrogen or hydrogen stream, obtain catalytic module in 200 ~ 550 DEG C of roasting 2 ~ 8h;
Or the cated foamed ceramics that covers of step (3) gained is placed in adjuvant component maceration extract dipping 1 ~ 30s, at 50 ~ 100 DEG C of drying 1 ~ 12h after taking-up, then be placed in activity component impregnation liquid and flood 1 ~ 10min, at 50 ~ 100 DEG C of drying 1 ~ 12h after drying in the shade under room temperature and ambient humidity, then in air or nitrogen or hydrogen stream, obtain catalytic module in 200 ~ 550 DEG C of roasting 2 ~ 8h;
Or by the active component solution of step (4) gained and the mixing of adjuvant component dissolution homogeneity, 10 ~ 40 parts of coating precursor powder are added in mixed solution, 0.1 ~ 20 part of binding agent, 0.01 ~ 5 part of coalescents, add with the mass ratio of coating precursor powder is that the deionized water of 9:1 ~ 6:4 is carried out dilution and obtained mixed serum again, mixed serum is placed on dispersion machine and disperses 20 ~ 60min under 300 ~ 550r/min, and with mass concentration be 5 ~ 20% nitric acid or hydrochloric acid solution the pH of slip is adjusted to pH=3 ~ 4, transferred to after beating glue 1 ~ 2h in ball mill or sand mill after continuing dispersion 10 ~ 30min, transfer in vacuum coaters storage tank, then foamed ceramics structure is placed in sample bin and carries out vacuum covering 2 ~ 20min, utilize the unnecessary slip in compressed air purging duct, then 25 ~ 40 DEG C are placed in and relative humidity is under 45 ~ 90% conditions after maintenance 4 ~ 24h, dry 1 ~ 12h in 60 ~ 120 DEG C of environment, after by the foamed ceramics through super-dry at 200 ~ 550 DEG C of roasting 1 ~ 8h, obtain catalytic module.
On the basis of technique scheme, the present invention can also do following improvement:
Further, described binding agent is inorganic binder or organic binder bond.
Further, described inorganic binder comprises one in Ludox, Alumina gel, silicon-aluminum sol, waterglass, titanium colloidal sol, aluminum phosphate, aluminium dihydrogen phosphate and clay or severally arbitrarily to combine.
Further, described organic binder bond comprises one in cellulose, polyvinyl alcohol (PVA), polyethylene glycol oxide (PEO), polyacrylamide (PAM) and polyurethane or severally arbitrarily to combine.
Further, described coalescents is one in sodium metasilicate, calgon, bentonite, softex kw, lauryl sodium sulfate, neopelex, TBAB, P123, F127, polyoxyethylene laurel ether, AEO, polyethylene glycol, ethylene glycol, glycerine, butanols, isobutanol, butyl glycol ether, propylene glycol monomethyl ether, acetylacetone,2,4-pentanedione, dimethyl silicone polymer, monoethanolamine, diethanol amine, triethanolamine, acrylate and organically-modified silica alkane or any several combination.
Further, described protective agent is one in anion surfactant, cationic surfactant, nonionic surface active agent, amphoteric surfactant and compound surfactant or any several combination.
The beneficial effect of above-mentioned further technical scheme is adopted to be that the active component precursor powder described in step (4) refers to activity component metal simple substance, oxide, inorganic salts or organic salt.Presoma as Pt active component can be platinum nitrate, chloroplatinic acid, acetylacetone,2,4-pentanedione platinum etc.Different presoma has been embodied in embodiment.
Compared with prior art, catalytic module provided by the present invention has 3D pore passage structure, overcomes the shortcoming of traditional straight hole cellular integrated catalyst, improves catalytic activity and purification efficiency.The present invention has the following advantages:
(1) catalytic module oxidation of formaldehyde of the present invention has excellent low temperature active and removal efficiency, formaldehyde exhaustive oxidation can be become CO
2and H
2o, does not produce the secondary pollutions such as carbon monoxide, formic acid and methyl formate.
(2) catalytic module of the present invention has high stability and water repelling property, eliminates formaldehyde pollution under being applicable to room temperature and ambient humidity, and operationally, in scope, the removal efficiency of the formaldehyde of PARA FORMALDEHYDE PRILLS(91,95) can remain on more than 98%.
(3) duct of catalytic module of the present invention is interlaced 3D structure, there is larger apparent pore and specific area, be conducive to carrying out fast of catalytic reaction, accelerate the desorption rate of reaction molecular absorption, product molecule, and then improve reaction rate and the transformation efficiency of formaldehyde.
(4) catalytic module preparation process of the present invention is simple, easy to operate, noble-metal-supported amount is low, the pressure loss is low, does not need the affiliated facility such as light source, heating, has saved energy consumption while reducing costs.
In sum, catalytic module of the present invention, according to different demand and use occasion, can make different shape and size specifications, as cuboid, square, cylinder and curved body etc.It has good catalytic activity to the formaldehyde in air under room temperature and environmental damp condition, can be H by HCHO exhaustive oxidation
2o and CO
2, be applicable to remove family room, office buildings, market, building materials market and warehouse, the vehicles etc. are airtight, trace formaldehyde in semi-enclosed space air, in purification of air, Fresh air handing and industrial waste gas process, there is good application prospect.
Accompanying drawing explanation
Fig. 1 is the pictorial diagram of catalytic module of the present invention;
Fig. 2 is the sectional skeleton diagram of catalytic module of the present invention;
Fig. 3 is the removal efficiency of catalytic module PARA FORMALDEHYDE PRILLS(91,95) of the present invention;
Fig. 4 is catalytic module stability test curve of the present invention.
In accompanying drawing, the list of parts representated by each label is as follows:
1, skeleton carrier, 2, coating, 3, catalyst layer, 4, duct.
Detailed description of the invention
Be described principle of the present invention and feature below in conjunction with accompanying drawing, example, only for explaining the present invention, is not intended to limit scope of the present invention.
As shown in Figure 1, under a kind of room temperature, eliminate the catalytic module of formaldehyde, comprise skeleton carrier 1, coating 2 and catalyst layer 3,
Described skeleton carrier 1, for having the foamed ceramics structure of 3 D pore canal, has multiple duct 4 in described foamed ceramics structure, and described duct 4 is mutually through and be woven into a mesh structure;
Described coating 2 be evenly coated in described foamed ceramics structure duct 4 surface and outer surface on, described catalyst layer 3 is highly dispersed in coating 2.
The material of described foamed ceramics structure is aluminium oxide, magnesia, zeolite, cordierite, mullite, dichroite-mullite compound, carborundum, silicon nitride, magnesia, zirconium-mullite, active carbon, zirconia and fused alumina zirconia a kind of or several arbitrarily mixed materials wherein, and the arranged direction of described foamed ceramics structure inner duct 4 is the either direction in X, Y and Z-direction;
The porosity of described foamed ceramics structure is 25 ~ 90%.
Being made up of coating precursor powder of described coating 2, described coating precursor powder is Al
2o
3, Fe
2o
3, TiO
2, SiO
2, CeO
2, ZrO
2, MgO, ZMS-5, molecular sieve, APO, SAPO, active carbon, zeolite, montmorillonite, diatomite, sepiolite, a kind of or several arbitrarily mixture in attapulgite and bentonite or wherein a kind of or several arbitrarily composite oxides or wherein a kind of or any several modified material, the coated weight of described coating 2 is 10 ~ 150g/L.
Described catalyst layer 3 comprises active component and adjuvant component,
Described active component be in Pd, Pt, Rh, Au, Ag or Ru any one or multiple, described active component is made up of active component precursor powder, described active component precursor powder is have a kind of or several arbitrarily mixture in the metal simple-substance of above-mentioned element, oxide, alloy, organic salt or inorganic salts, and the load capacity of described active component in coating 2 counts 0.05 ~ 10wt% by the quality of metal simple-substance corresponding in described active component;
Described adjuvant component be in Li, Na, K, Rb, Cs, Fr, Fe, Co, Ni, Cu, Mn, Mo, Ti, Ce, Zr, Pr, Nd or Zn any one or multiple, described adjuvant component is made up of adjuvant component precursor powder, described adjuvant component precursor powder is have a kind of or several arbitrarily mixture in the metal simple-substance of above-mentioned element, oxide, alloy, organic salt or inorganic salts, and the load capacity of described adjuvant component in coating 2 counts 0.1 ~ 20wt% by the quality of metal simple-substance corresponding in described adjuvant component.
The preparation method of the catalytic module of formaldehyde is eliminated under a kind of room temperature, prepare above-mentioned catalytic module, comprise and as follows coating 2 is coated in described foamed ceramics body structure surface by vacuum coating methods, then utilize infusion process or the precipitation method at coating 2 catalyst supported on surface layer 3 thus obtain the step of this catalytic module, specific operation process comprises the following steps:
(1) coating precursor powder 10 ~ 40 weight portion, binding agent 0.1 ~ 20 weight portion, coalescents 0.01 ~ 5 weight portion and deionized water are mixed, the mass ratio of described deionized water and coating precursor powder is 9:1 ~ 6:4; The slurries mixed are placed on dispersion machine, under 300 ~ 550r/min, disperse 20 ~ 60min; Then with mass concentration be 5 ~ 20% nitric acid or hydrochloric acid solution the pH of slip is adjusted to pH=3 ~ 4, continue dispersion 10 ~ 30min;
(2) after the slurries of step (1) gained are transferred to beating glue 1 ~ 2h in ball mill or sand mill, transfer in vacuum coaters storage tank, then foamed ceramics structure is placed in sample bin and carries out vacuum covering 2 ~ 20min, utilize the unnecessary slip in compressed air purging duct 4;
(3) the foamed ceramics structure of taking-up step (2) coating slurries, is placed in 25 ~ 40 DEG C and relative humidity is under 45 ~ 90% conditions after maintenance 4 ~ 24h, dry 1 ~ 12h in 60 ~ 120 DEG C of environment; After by the foamed ceramics through super-dry at 200 ~ 550 DEG C of roasting 1 ~ 8h, obtain the foamed ceramics structure being covered with coating 2;
(4) active component solution is configured, active component precursor powder is dissolved in deionized water, then ultrasonic 10 ~ 60min under agitation, add deionized water dilution, after dilution, the volume of solution is 1:1 ~ 3:1 with the ratio of the volume of foamed ceramics structure, add protective agent again, described protective agent is 1:5 ~ 1:30 with the ratio of precious metal element content in active component precursor powder, stir 30 ~ 90min, obtain activity component impregnation liquid, wherein the concentration of the corresponding metal simple-substance of active component is 5 ~ 100mmol/mL; Configuration adjuvant component solution, adjuvant component precursor powder is added deionized water dilution, the volume after dilution is 1:1 ~ 3:1 with the ratio of the volume of foamed ceramics structure, obtains adjuvant component maceration extract, and wherein adjuvant component mass concentration is 10 ~ 50%;
(5) the activity component impregnation liquid of step (4) gained and adjuvant component maceration extract Homogeneous phase mixing are obtained mixed impregnant liquor, the foamed ceramics being coated with coating 2 obtained in step (3) is placed in mixed impregnant liquor dipping 1 ~ 10min, dry in the shade under room temperature and ambient humidity, at 50 ~ 100 DEG C of drying 1 ~ 12h, then in air or nitrogen or hydrogen stream, obtain catalytic module in 200 ~ 550 DEG C of roasting 2 ~ 8h;
Or the foamed ceramics being covered with coating 2 of step (3) gained is placed in activity component impregnation liquid dipping 1 ~ 10min, at 50 ~ 100 DEG C of drying 1 ~ 12h after drying in the shade under room temperature and ambient humidity, then adjuvant component maceration extract dipping 1 ~ 30s is placed in, at 50 ~ 100 DEG C of drying 1 ~ 12h after taking-up, then in air or nitrogen or hydrogen stream, obtain catalytic module in 200 ~ 550 DEG C of roasting 2 ~ 8h;
Or the foamed ceramics being covered with coating 2 of step (3) gained is placed in adjuvant component maceration extract dipping 1 ~ 30s, at 50 ~ 100 DEG C of drying 1 ~ 12h after taking-up, then be placed in activity component impregnation liquid and flood 1 ~ 10min, at 50 ~ 100 DEG C of drying 1 ~ 12h after drying in the shade under room temperature and ambient humidity, then in air or nitrogen or hydrogen stream, obtain catalytic module in 200 ~ 550 DEG C of roasting 2 ~ 8h;
Or by the active component solution of step (4) gained and the mixing of adjuvant component dissolution homogeneity, 10 ~ 40 parts of coating precursor powder are added in mixed solution, 0.1 ~ 20 part of binding agent, 0.01 ~ 5 part of coalescents, add with the mass ratio of coating precursor powder is that the deionized water of 9:1 ~ 6:4 is carried out dilution and obtained mixed serum again, mixed serum is placed on dispersion machine and disperses 20 ~ 60min under 300 ~ 550r/min, and with mass concentration be 5 ~ 20% nitric acid or hydrochloric acid solution the pH of slip is adjusted to pH=3 ~ 4, transferred to after beating glue 1 ~ 2h in ball mill or sand mill after continuing dispersion 10 ~ 30min, transfer in vacuum coaters storage tank, then foamed ceramics structure is placed in sample bin and carries out vacuum covering 2 ~ 20min, utilize the unnecessary slip in compressed air purging duct 4, then 25 ~ 40 DEG C are placed in and relative humidity is under 45 ~ 90% conditions after maintenance 4 ~ 24h, dry 1 ~ 12h in 60 ~ 120 DEG C of environment, after by the foamed ceramics through super-dry at 200 ~ 550 DEG C of roasting 1 ~ 8h, obtain catalytic module.
Described binding agent is inorganic binder or organic binder bond.
Described inorganic binder comprises one in Ludox, Alumina gel, silicon-aluminum sol, waterglass, titanium colloidal sol, aluminum phosphate, aluminium dihydrogen phosphate and clay or severally arbitrarily to combine.
Described organic binder bond comprises one in cellulose, polyvinyl alcohol (PVA), polyethylene glycol oxide (PEO), polyacrylamide (PAM) and polyurethane or severally arbitrarily to combine.
Described coalescents is sodium metasilicate, calgon, bentonite, softex kw, lauryl sodium sulfate, neopelex, TBAB, P123, F127, polyoxyethylene laurel ether, AEO, polyethylene glycol, ethylene glycol, glycerine, butanols, isobutanol, butyl glycol ether, propylene glycol monomethyl ether, acetylacetone,2,4-pentanedione, dimethyl silicone polymer, monoethanolamine, diethanol amine, triethanolamine, one in acrylate and organically-modified silica alkane or any several combination.
Described protective agent is one in anion surfactant, cationic surfactant, nonionic surface active agent, amphoteric surfactant and compound surfactant or any several combination.
In order to catalytic module of the present invention is better described, below in conjunction with embodiment, the present invention is described in detail, and embodiment is to The present invention gives detailed description of the invention and operating process, but protection scope of the present invention includes but not limited to following embodiment.
Embodiment 1 foamed ceramics body structure surface applying coating 2:
Embodiment 1-1:
By 50gTiO
2(A type), 1.5gHPMC-6000,0.25g AEO (R=C16 ~ 18, n=20) and 250mLH
2o mixes, and is placed on dispersion machine and disperses 30min under 350r/min, is pH=3 ~ 4 of the salpeter solution adjustment slip of 10%, continues dispersion 15min by concentration; Being transferred to by slurries in sand mill after beating glue 1.5h transfers in vacuum coaters storage tank, then the foam silicon carbide ceramics structure being of a size of 100 × 100 × 20mm is placed in vacuum covering 10min in sample bin, utilizes compressed air to purge unnecessary slip in duct 4.
The foamed ceramics of coating slurries is placed in the curing box maintenance 6h that 25 DEG C and relative humidity are 70%, and after 80 DEG C of dry 6h, obtain carrier 1-1 in the air stream after 400 DEG C of roasting 4.0h, coating 2 coated weight is 57.8g/L.
Embodiment 1-2:
Difference is compared with embodiment 1-1: carrier changes Al into
2o
3foamed ceramics, binding agent changes PVA-2488 into, and coalescents changes dimethyl silicone polymer into, and all the other processes, with embodiment 1-1, obtain carrier 1-2, and coating 2 coating rate is 59.3g/L.
Embodiment 1-3:
Difference is compared with embodiment 1-1: carrier changes cordierite foamed ceramics into, and all the other processes, with embodiment 1-1, obtain carrier 1-3, and coating 2 coating rate is 62.2g/L.
Embodiment 1-4:
Difference is compared with embodiment 1-1: coating material TiO
2(A type) changes γ-Al into
2o
3, binding agent is HPMC-6000, coalescents be all the other processes of dimethyl silicone polymer with embodiment 1-1, obtain carrier 1-2, coating 2 coating rate is 63.8g/L.
Embodiment 1-5:
Difference is compared with embodiment 1-1: coating material 50gTiO
2(A type) changes 40gTiO into
2(A type)+10g γ-Al
2o
3all the other processes, with embodiment 1-1, obtain carrier 1-5, and coating 2 coating rate is 64.1g/L.
Embodiment 2 load active component and adjuvant component:
Embodiment 2-1:
By 0.289gPdCl
2joining 16.4mL concentration is heat to be stirred in the hydrochloric acid solution of 0.6% to dissolve completely, spends IONS OF H after ultrasonic disperse 20min
2o is diluted to 250mL, and active component solution is 1.25:1 with the volume ratio of the foamed ceramics being covered with coating 2, adds 4.34g surfactant polyvinylpyrrolidone (PVP)
Stir 40min and obtain activity component impregnation liquid, polyvinylpyrrolidone (PVP) and PdCl
2mass ratio be 15:1; The foamed ceramics structure being covered with coating 2 of embodiment 1-1 gained is placed in activity component impregnation liquid and floods 5min, at 80 DEG C of dry 4h after drying in the shade under room temperature and ambient humidity, then obtain catalytic module 2-1 in 350 DEG C of roasting 4.0h in the air stream, the load capacity of the surperficial Pd of coating 2 counts 1.0wt% with simple substance.
By 0.289gPdCl
2joining 16.4mL concentration is heat to be stirred in the hydrochloric acid solution of 0.6% to dissolve completely, spends IONS OF H after ultrasonic disperse 20min
2o is diluted to 250mL, adds 4.34g surfactant polyvinylpyrrolidone stirring 40min and obtains activity component impregnation liquid; The foamed ceramics structure being covered with coating 2 of embodiment 1-1 gained is placed in activity component impregnation liquid and floods 5min, at 80 DEG C of dry 4h after drying in the shade under room temperature and ambient humidity, then obtain catalytic module 2-1 in 350 DEG C of roasting 4.0h in the air stream, the load capacity of the surperficial Pd of coating 2 counts 1.0wt% with simple substance.
Embodiment 2-2:
Difference is compared with embodiment 2-1: PdCl
2quality become 0.145g, hydrochloric acid solution volume becomes 8.2mL, and the quality of polyvinylpyrrolidone becomes 2.17g, and all the other processes, with embodiment 2-1, obtain catalytic module 2-2, and the load capacity of the surperficial Pd of coating 2 counts 0.5wt% with simple substance.
Embodiment 2-3:
Difference is compared with embodiment 2-1: by 0.766gH
2ptCl
66H
2o is dissolved into 250mLH
2in O, ultrasonic disperse 20min, add 11.49g polyvinylpyrrolidone and stir 40min, all the other processes, with embodiment 2-1, obtain catalytic module 2-3, and the load capacity of the surperficial Pt of coating 2 counts 2.0wt% with simple substance.
Embodiment 2-4:
Difference is compared with embodiment 2-3: by H
2ptCl
66H
2the quality of O becomes 0.383g, and polyvinylpyrrolidone quality becomes 5.75g, and all the other processes, with embodiment 2-3, obtain catalytic module 2-4, and the load capacity of the surperficial Pt of coating 2 counts 1.0wt% with simple substance.
Embodiment 2-5:
Difference is compared with embodiment 2-3: by H
2ptCl
66H
2the quality of O becomes 0.192g, and polyvinylpyrrolidone quality becomes 2.88g, and all the other processes, with embodiment 2-3, obtain catalytic module 2-5, and the load capacity of the surperficial Pt of coating 2 counts 0.5wt% with simple substance.
Embodiment 2-6:
Difference is compared with embodiment 2-3: by 0.308gK
2ptCl
4be dissolved into 250mLH
2in O, ultrasonic disperse 20min, add 5.41g softex kw and stir 40min (1:20), all the other processes, with embodiment 2-6, obtain catalytic module 2-6, and the load capacity of the surperficial Pt of coating 2 counts 1.0wt% with simple substance.
Embodiment 2-7:
By 0.308gK
2ptCl
4be dissolved into 250mLH
2in O, ultrasonic disperse 20min, adds 5.41g softex kw and stirs 40min, the foamed ceramics structure being covered with coating 2 of embodiment 1-1 gained is placed in maceration extract and floods 5min, at 80 DEG C of dry 4h after drying in the shade under room temperature and ambient humidity; Then the Na of 5% is placed in
2cO
3flood 30s in solution, at 80 DEG C of dry 4h after taking-up, obtain catalytic module 2-7 in the air stream in 350 DEG C of roasting 4.0h, the load capacity of coating 2 surperficial Pt, Na is respectively 1.0wt% and 2.0wt% in simple substance.
Embodiment 2-8:
Difference is compared with embodiment 2-7: the foamed ceramics being covered with coating 2 of embodiment 1-1 gained is placed in the Na of 5%
2cO
330s is flooded, at 80 DEG C of dry 4h in solution; Then it is flooded 5min in containing softex kw solution, at 80 DEG C of dry 4h after drying in the shade under room temperature and ambient humidity.All the other processes, with embodiment 2-7, obtain catalytic module 2-8, and the load capacity of coating 2 surperficial Pt, Li is respectively 1.0wt% and 2wt% in simple substance.
Embodiment 2-9:
Difference is compared with embodiment 2-7: by the Na of 5%
2cO
3solution changes the Li of 5% into
2cO
3solution, all the other processes, with embodiment 2-7, obtain catalytic module 2-9, and the load capacity of coating 2 surperficial Pt, Li is respectively 1.0wt% and 2wt% in simple substance.
Embodiment 3:
By 1.06gK
2ptCl
4and 2.31gNa
2cO
3be dissolved into 250mLH
2stir in O, add 50gTiO wherein
2(A type), 1.5gHPMC-6000 and 0.25g AEO (R=C16 ~ 18, n=20) mix, be placed on dispersion machine and disperse 30min under 350r/min, be pH=3 ~ 4 of the salpeter solution adjustment slurries of 10% by concentration, continue dispersion 15min.Being transferred to by slurries in sand mill after beating glue 1.5h transfers in vacuum coaters storage tank, then the foam silicon carbide ceramics structure being of a size of 100 × 100 × 20mm is placed in vacuum covering 10min in sample bin, and utilizes compressed air to purge unnecessary slip in duct 4.
The foamed ceramics structure of coating slurries is placed in the curing box maintenance 6h that 25 DEG C and relative humidity are 70%, after 80 DEG C of dry 4h, catalytic module 3 is obtained in the air stream in 350 DEG C of roasting 4.0h, coating 2 coated weight is 58.3g/L, and the load capacity of coating 2 surperficial Pt, Na is respectively 1.0wt% and 2wt% in simple substance.
Embodiment 4:
Difference from Example 3 is: coating slurries catalytic module after maintenance, drying, at 5%H
2+ 95%N
2(V/V) obtain catalytic module 3 at 350 DEG C of roasting 4.0h in air-flow, coating 2 coated weight is 58.3g/L, and the load capacity of coating 2 surperficial Pt, Na is respectively 1.0wt% and 2wt% in simple substance.
Test case:
Catalytic activity is at 1m
3laboratory Module in test, respectively for embodiment 2-1 ~ 2-8, embodiment 3 and embodiment 4, test the removal efficiency of catalytic module PARA FORMALDEHYDE PRILLS(91,95) under room temperature and environmental damp condition.Test condition is: concentration of formaldehyde is 10ppm, air balance, reaction velocity SV=50000h
-1, probe temperature is 25 DEG C, and humidity is 60%, and in gas, formaldehyde utilizes Shimadzu 2020 gas chromatograph on-line determination, utilizes purification efficiency that is initial and testing time point concentration calculating catalytic module PARA FORMALDEHYDE PRILLS(91,95).
The purification efficiency of table 1 catalytic module PARA FORMALDEHYDE PRILLS(91,95) under test case condition
As shown in Figure 3 and Figure 4, the removal efficiency of catalytic module PARA FORMALDEHYDE PRILLS(91,95) and catalytic module stability test curve, as shown in Figure 2, catalytic module PARA FORMALDEHYDE PRILLS(91,95) degraded under room temperature and environmental damp condition has excellent catalytic activity, and the degradation efficiency of PARA FORMALDEHYDE PRILLS(91,95) remains on more than 95%; In stability curve shown in Fig. 3, the degradation efficiency of catalyst module PARA FORMALDEHYDE PRILLS(91,95) remains unchanged substantially, and after running 120h continuously, the degradation efficiency of PARA FORMALDEHYDE PRILLS(91,95) still remains on more than 95%, has higher catalytic activity and stability.
Embodiment of the present invention is only to be described in detail to embodiment and operating process; but protection scope of the present invention is not limited to operating process described in embodiment and step, does not namely mean that the present invention must depend on above-mentioned preparation process and step could be implemented.The technical staff in described field should understand; any improvement in the present invention; the equivalences such as raw material, material, size selected by the present invention are replaced and the interpolation of auxiliary element and change, detailed description of the invention selection etc., all drop within protection scope of the present invention and open scope.
Claims (10)
1. eliminate a catalytic module for formaldehyde under room temperature, it is characterized in that, comprise skeleton carrier, coating and catalyst layer,
Described skeleton carrier is the foamed ceramics structure with 3 D pore canal, has multiple duct in described foamed ceramics structure, and described duct is mutually through and be woven into a mesh structure;
Described coating uniform is coated on channel surfaces in described foamed ceramics structure and outer surface thereof, and described catalyst layer height is dispersed in coating.
2. under a kind of room temperature according to claim 1, eliminate the catalytic module of formaldehyde, it is characterized in that, the material of described foamed ceramics structure is aluminium oxide, magnesia, zeolite, cordierite, mullite, dichroite-mullite compound, carborundum, silicon nitride, magnesia, zirconium-mullite, active carbon, zirconia and fused alumina zirconia a kind of or several arbitrarily mixed materials wherein, and the arranged direction of described foamed ceramics structure inner duct is the either direction in X, Y and Z-direction;
The porosity of described foamed ceramics structure is 25 ~ 90%.
3. eliminate the catalytic module of formaldehyde under a kind of room temperature according to claim 1, it is characterized in that, being made up of coating precursor powder of described coating, described coating precursor powder is Al
2o
3, Fe
2o
3, TiO
2, SiO
2, CeO
2, ZrO
2, MgO, ZMS-5, molecular sieve, APO, SAPO, active carbon, zeolite, montmorillonite, diatomite, sepiolite, a kind of or several arbitrarily mixture in attapulgite and bentonite or wherein a kind of or several arbitrarily composite oxides or wherein a kind of or any several modified material, the coated weight of described coating is 10 ~ 150g/L.
4. eliminate the catalytic module of formaldehyde under a kind of room temperature according to claim 1, it is characterized in that, described catalyst layer comprises active component and adjuvant component,
Described active component be in Pd, Pt, Rh, Au, Ag or Ru any one or multiple, described active component is made up of active component precursor powder, described active component precursor powder is have a kind of or several arbitrarily mixture in the metal simple-substance of above-mentioned element, oxide, alloy, organic salt or inorganic salts, and the load capacity of described active component in coating counts 0.05 ~ 10wt% by the quality of metal simple-substance corresponding in described active component;
Described adjuvant component be in Li, Na, K, Rb, Cs, Fr, Fe, Co, Ni, Cu, Mn, Mo, Ti, Ce, Zr, Pr, Nd or Zn any one or multiple, described adjuvant component is made up of adjuvant component precursor powder, described adjuvant component precursor powder is have a kind of or several arbitrarily mixture in the metal simple-substance of above-mentioned element, oxide, alloy, organic salt or inorganic salts, and the load capacity of described adjuvant component in coating counts 0.1 ~ 20wt% by the quality of metal simple-substance corresponding in described adjuvant component.
5. under a room temperature, eliminate the preparation method of the catalytic module of formaldehyde, it is characterized in that, the catalytic module of formaldehyde is eliminated under a kind of room temperature of preparation as described in Claims 1-4, comprise and as follows coating is coated in described foamed ceramics body structure surface by vacuum coating methods, then utilize infusion process or the precipitation method at coating surface supported catalyst layer thus obtain the step of this catalytic module, specific operation process comprises the following steps:
(1) coating precursor powder 10 ~ 40 weight portion, binding agent 0.1 ~ 20 weight portion, coalescents 0.01 ~ 5 weight portion and deionized water are mixed, the mass ratio of described deionized water and coating precursor powder is 9:1 ~ 6:4; The slurries mixed are placed on dispersion machine, under 300 ~ 550r/min, disperse 20 ~ 60min; Then with mass concentration be 5 ~ 20% nitric acid or hydrochloric acid solution the pH of slip is adjusted to pH=3 ~ 4, continue dispersion 10 ~ 30min;
(2) after the slurries of step (1) gained are transferred to beating glue 1 ~ 2h in ball mill or sand mill, transfer in vacuum coaters storage tank, then foamed ceramics structure is placed in sample bin and carries out vacuum covering 2 ~ 20min, utilize the unnecessary slip in compressed air purging duct;
(3) the foamed ceramics structure of taking-up step (2) coating slurries, is placed in 25 ~ 40 DEG C and relative humidity is under 45 ~ 90% conditions after maintenance 4 ~ 24h, dry 1 ~ 12h in 60 ~ 120 DEG C of environment; After by the foamed ceramics through super-dry at 200 ~ 550 DEG C of roasting 1 ~ 8h, obtain covering cated foamed ceramics structure;
(4) active component solution is configured, active component precursor powder is dissolved in deionized water, then ultrasonic 10 ~ 60min under agitation, add deionized water dilution, after dilution, the volume of solution is 1:1 ~ 3:1 with the ratio of the volume of foamed ceramics structure, add protective agent again, described protective agent is 1:5 ~ 1:30 with the ratio of precious metal element content in active component precursor powder, stir 30 ~ 90min, obtain activity component impregnation liquid, wherein the concentration of the corresponding metal simple-substance of active component is 5 ~ 100mmol/mL; Configuration adjuvant component solution, adjuvant component precursor powder is added deionized water dilution, the volume after dilution is 1:1 ~ 3:1 with the ratio of the volume of foamed ceramics structure, obtains adjuvant component maceration extract, and wherein adjuvant component mass concentration is 10 ~ 50%;
(5) the activity component impregnation liquid of step (4) gained and adjuvant component maceration extract Homogeneous phase mixing are obtained mixed impregnant liquor, the cated foamed ceramics of coating obtained in step (3) is placed in mixed impregnant liquor dipping 1 ~ 10min, dry in the shade under room temperature and ambient humidity, at 50 ~ 100 DEG C of drying 1 ~ 12h, then in air or nitrogen or hydrogen stream, obtain catalytic module in 200 ~ 550 DEG C of roasting 2 ~ 8h;
Or the cated foamed ceramics that covers of step (3) gained is placed in activity component impregnation liquid dipping 1 ~ 10min, at 50 ~ 100 DEG C of drying 1 ~ 12h after drying in the shade under room temperature and ambient humidity, then adjuvant component maceration extract dipping 1 ~ 30s is placed in, at 50 ~ 100 DEG C of drying 1 ~ 12h after taking-up, then in air or nitrogen or hydrogen stream, obtain catalytic module in 200 ~ 550 DEG C of roasting 2 ~ 8h;
Or the cated foamed ceramics that covers of step (3) gained is placed in adjuvant component maceration extract dipping 1 ~ 30s, at 50 ~ 100 DEG C of drying 1 ~ 12h after taking-up, then be placed in activity component impregnation liquid and flood 1 ~ 10min, at 50 ~ 100 DEG C of drying 1 ~ 12h after drying in the shade under room temperature and ambient humidity, then in air or nitrogen or hydrogen stream, obtain catalytic module in 200 ~ 550 DEG C of roasting 2 ~ 8h;
Or by the active component solution of step (4) gained and the mixing of adjuvant component dissolution homogeneity, 10 ~ 40 parts of coating precursor powder are added in mixed solution, 0.1 ~ 20 part of binding agent, 0.01 ~ 5 part of coalescents, add with the mass ratio of coating precursor powder is that the deionized water of 9:1 ~ 6:4 is carried out dilution and obtained mixed serum again, mixed serum is placed on dispersion machine and disperses 20 ~ 60min under 300 ~ 550r/min, and with mass concentration be 5 ~ 20% nitric acid or hydrochloric acid solution the pH of slip is adjusted to pH=3 ~ 4, transferred to after beating glue 1 ~ 2h in ball mill or sand mill after continuing dispersion 10 ~ 30min, transfer in vacuum coaters storage tank, then foamed ceramics structure is placed in sample bin and carries out vacuum covering 2 ~ 20min, utilize the unnecessary slip in compressed air purging duct, then 25 ~ 40 DEG C are placed in and relative humidity is under 45 ~ 90% conditions after maintenance 4 ~ 24h, dry 1 ~ 12h in 60 ~ 120 DEG C of environment, after by the foamed ceramics through super-dry at 200 ~ 550 DEG C of roasting 1 ~ 8h, obtain catalytic module.
6. eliminate the preparation method of the catalytic module of formaldehyde under a kind of room temperature according to claim 5, it is characterized in that, described binding agent is inorganic binder or organic binder bond.
7. under a kind of room temperature according to claim 6, eliminate the preparation method of the catalytic module of formaldehyde, it is characterized in that, described inorganic binder comprises one in Ludox, Alumina gel, silicon-aluminum sol, waterglass, titanium colloidal sol, aluminum phosphate, aluminium dihydrogen phosphate and clay or severally arbitrarily to combine.
8. under a kind of room temperature according to claim 6, eliminate the preparation method of the catalytic module of formaldehyde, it is characterized in that, described organic binder bond comprises one in cellulose, polyvinyl alcohol (PVA), polyethylene glycol oxide (PEO), polyacrylamide (PAM) and polyurethane or severally arbitrarily to combine.
9. eliminate the preparation method of the catalytic module of formaldehyde under a kind of room temperature according to claim 5, it is characterized in that,
Described coalescents is sodium metasilicate, calgon, bentonite, softex kw, lauryl sodium sulfate, neopelex, TBAB, P123, F127, polyoxyethylene laurel ether, AEO, polyethylene glycol, ethylene glycol, glycerine, butanols, isobutanol, butyl glycol ether, propylene glycol monomethyl ether, acetylacetone,2,4-pentanedione, dimethyl silicone polymer, monoethanolamine, diethanol amine, triethanolamine, one in acrylate and organically-modified silica alkane or any several combination.
10. under a kind of room temperature according to claim 5, eliminate the preparation method of the catalytic module of formaldehyde; it is characterized in that, described protective agent is one in anion surfactant, cationic surfactant, nonionic surface active agent, amphoteric surfactant and compound surfactant or any several combination.
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