CN109012695A - A kind of preparation method, thus obtained structural catalyst and its application of the structural catalyst of catalysis oxidation formaldehyde - Google Patents
A kind of preparation method, thus obtained structural catalyst and its application of the structural catalyst of catalysis oxidation formaldehyde Download PDFInfo
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- CN109012695A CN109012695A CN201810941101.7A CN201810941101A CN109012695A CN 109012695 A CN109012695 A CN 109012695A CN 201810941101 A CN201810941101 A CN 201810941101A CN 109012695 A CN109012695 A CN 109012695A
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- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
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Abstract
The present invention relates to a kind of preparation methods of the structural catalyst of catalysis oxidation formaldehyde comprising following steps: S1, provides integrated vigorous nurse body carrier；And S2, integrated vigorous nurse body carrier is placed in Fe (NO3)3Precursor solution in impregnate, be dried to obtain load Fe vigorous nurse body；The vigorous nurse body for loading Fe is placed in H2PtCl6It is impregnated in solution, is dried to obtain the vigorous nurse body of load Fe and Pt；It is restored using vigorous nurse body of the liquid phase reduction to load Fe and Pt, is dried to obtain structural catalyst.The present invention also provides a kind of structural catalysts obtained according to above-mentioned preparation method.The present invention also provides a kind of applications of above-mentioned structural catalyst.Structural catalyst according to the present invention can not only fast and effeciently catalysis oxidation high-concentration formaldehyde at room temperature, and being capable of catalytic oxidation of low-concentration formaldehyde.
Description
Technical field
The present invention relates to catalyst and environmental protection technical field, and in particular to a kind of structuring of catalysis oxidation formaldehyde is urged
The preparation method of agent, thus obtained structural catalyst and its application.
Background technique
Formaldehyde Pollution of Indoor Air problem is gradually concerned by people in recent years.United nations environment health organization generally acknowledges formaldehyde
It is one of generally acknowledged allergen and strong mutagen for carcinogenic and cause deformed material.In order to meet people increasingly to health
Higher pursuit, the improvement of Formaldehyde Pollution of Indoor Air is extremely urgent.
Control Formaldehyde Pollution of Indoor Air mainly has ventilation method, plant purification method, low-temperature plasma method, room temperature absorption at present
Method, photocatalytic oxidation.Indoor and outdoor ventilation is one of simplest minimizing technology, although windowing ventilation can reduce formaldehyde
Concentration, but formaldehyde is continuously discharged into interior, and ventilation will cannot thoroughly remove formaldehyde.For using the public of central air-conditioning
In place and office block and summer, winter using air-conditioning can not the place of long-time ventilation be all not applicable.
The plant purification time is longer, and efficiency is lower, and the relationship ratio between plant purification ability and the formaldehyde amount of interior space release
More difficult determination.Non-thermal plasma trap is that medium discharge is made to generate a large amount of electronics, ion, atom, freedom using external energy
The aggregates such as base, chemically react between aggregate and formaldehyde molecule, so that formaldehyde is excited, dissociates, decomposes, but it sets
Standby at high cost, operating cost is high, is easy to produce O3Equal secondary pollutions.Room temperature absorption method is to utilize Van der Waals force by formaldehyde absorbing
Achieve the effect that purifying formaldehyde on the surface of the adsorbents such as active carbon, when temperature, humidity, wind speed variation, the first of absorption
Aldehyde may be re-released into air, cause secondary pollution.The principle of photocatalysis Formaldehyde decomposition is under light illumination, to utilize catalysis
Formaldehyde molecule is adsorbed on its surface by agent, is further oxidized to carbon dioxide and water.And in light-catalyzed reaction, Formaldehyde decomposition
Generate the intermediate products such as formates, cause secondary pollution, and photocatalysis method processing super low concentration formaldehyde (1ppm with
Under) require more exacting terms.
Traditional catalytic oxidation catalysis oxidation formaldehyde at room temperature or under conditions of heating, but this method is applied mostly
In the formaldehyde (> 80ppm) of higher concentration decomposes, and indoor formaldehyde concentration is generally in 1ppm hereinafter, this environmental condition is to catalysis
The catalytic oxidation performance of agent has high requirement.Existing catalyst is generally difficult to catalytic oxidation of low-concentration formaldehyde, especially difficult
It is purified with the formaldehyde to concentration lower than 1ppm.
Summary of the invention
In order to solve the problems, such as it is above-mentioned it is of the existing technology can not eliminate low concentration formaldehyde, the present invention is intended to provide one kind is urged
Change preparation method, thus obtained structural catalyst and its application of the structural catalyst of oxidation formaldehyde.
The present invention provides a kind of preparation method of the structural catalyst of catalysis oxidation formaldehyde comprising following steps: S1,
There is provided integration vigorous nurse body (AlOOH) carrier；And S2, integrated vigorous nurse body (AlOOH) carrier is placed in Fe (NO3)3Forerunner
It is impregnated in liquid solution, is dried to obtain the vigorous nurse body of load Fe；The vigorous nurse body for loading Fe is placed in H2PtCl6It is impregnated in solution, it is dry
Obtain the vigorous nurse body of load Fe and Pt；It is restored using vigorous nurse body of the liquid phase reduction to load Fe and Pt, is dried to obtain knot
Structure catalyst.Preparation method according to the present invention will be expensive using dipping with plate or netted vigorous nurse body (AlOOH) for carrier
Pt metal and transition-metal Fe are supported on AlOOH, be successfully prepared it is a kind of can be by the formaldehyde in air under atmospheric pressure at room
Quickly and efficiently it is catalyzed into the water of nonhazardous and the catalyst of carbon dioxide.
The step S1 is specifically included: S11, is carried out pre-treatment to aluminium net or aluminium sheet with highly basic and strong acid and is obtained pre-treatment aluminium
Net or pre-treatment aluminium sheet；S12, pre-treatment aluminium net or pre-treatment aluminium sheet are immersed in anodizing tank and carry out anodic oxidation on surface
One layer of pellumina is formed, oxidation aluminium net or alumina plate are obtained；And S13, after aoxidizing aluminium net or alumina plate by roasting
It is hydrated to form vigorous nurse body (AlOOH) carrier of integration rich in hydroxyl.It should be understood that vigorous nurse body (AlOOH) carrier of the integration
It is closed by aluminium net or aluminium sheet by anodic oxidation, hot water, concrete technology strong operability is easy to amplify.
In the step S11, which is NaOH solution.It is highly preferred that the highly basic is the NaOH solution of 5-15wt%.
In a preferred embodiment, which is the NaOH solution of 10wt%.Preferably, which is HNO3Solution.More preferably
Ground, the strong acid are the HNO of 5-15wt%3Solution.In a preferred embodiment, which is the HNO of 10wt%3Solution.
In the step S12, pre-treatment aluminium net or pre-treatment aluminium sheet are placed in 2-10wt% oxalic acid solution Anodic oxygen
Change.Preferably, the current density when anodic oxidation is 20-100A/m2.Preferably, the current density when anodic oxidation is
20-50A/m2.In a preferred embodiment, the current density when anodic oxidation is 25A/m2.Preferably, the anodic oxygen
Change carries out at 10-30 DEG C.In a preferred embodiment, which carries out at 20 DEG C.Preferably, the anodic oxygen
Change and carries out 5-18h.It is highly preferred that the anodic oxidation carries out 10-14h.
In the step S13, which carries out at 100-400 DEG C, to decompose remaining oxalic acid on aluminium net or aluminium sheet.
It is highly preferred that the roasting carries out at 250-300 DEG C.In a preferred embodiment, which carries out at 350 DEG C.It is excellent
Selection of land, the hydration carry out in 60-100 DEG C of hot water.It is highly preferred that the hydration carries out in 70-85 DEG C of hot water.At one
In preferred embodiment, which carries out in 70 DEG C of hot water.Preferably, which carries out 0.5-3h.It is highly preferred that the water
It closes and carries out 40min-80min.In a preferred embodiment, which carries out 1h.
In the step S2, the precursor solution is the Fe (NO of 0.1-0.8g/L3)3Precursor solution.It is preferred that
Ground, vigorous dipping temperature of nurse body (AlOOH) carrier in precursor solution of integration is 20-30 DEG C.In a preferred implementation
In example, vigorous dipping temperature of nurse body (AlOOH) carrier in precursor solution of integration is 25 DEG C.Preferably, the vigorous nurse of integration
Dip time of body (AlOOH) carrier in precursor solution is 6-12h.In a preferred embodiment, the vigorous nurse of integration
Dip time of body (AlOOH) carrier in precursor solution is 8h.Preferably, 8-16h is dried at room temperature obtain load Fe's
Vigorous nurse body.In a preferred embodiment, 12h is dried at room temperature obtain the vigorous nurse body of load Fe.
In the step S2, the H2PtCl6Solution is the H of 0.1-0.8g/L2PtCl6Solution.It is preferred real at one
It applies in example, the H2PtCl6Solution is the H of 0.4g/L2PtCl6Solution.Preferably, the vigorous nurse body of Fe is loaded in H2PtCl6Solution
In dipping temperature be 50-70 DEG C.In a preferred embodiment, the vigorous nurse body of Fe is loaded in H2PtCl6Dipping in solution
Temperature is 60 DEG C.Preferably, the vigorous nurse body of Fe is loaded in H2PtCl6Dip time in solution is 2-12h.It is preferred at one
In embodiment, the vigorous nurse body of Fe is loaded in H2PtCl6Dip time in solution is 4h.Preferably, 8-16h is dried at room temperature to obtain
To the vigorous nurse body of load Fe and Pt.In a preferred embodiment, 12h is dried at room temperature obtain the Bo Mu of load Fe and Pt
Body.
In the step S2, the vigorous nurse body for loading Fe and Pt is placed in sodium borohydride solution and is restored, make Pt and Fe from
Positive valence state becomes zero valence.Preferably, sodium borohydride solution is the sodium borohydride solution of 0.01-0.05mol/L.It is preferred at one
In embodiment, sodium borohydride solution is the sodium borohydride solution of 0.01mol/L.Preferably, reduction reaction at 20-30 DEG C into
Row.In a preferred embodiment, reduction reaction carries out at 25 DEG C.Preferably, reduction reaction carries out 0.5-3h.At one
In preferred embodiment, reduction reaction carries out 1h.Preferably, 8-16h is dried at room temperature obtain structural catalyst.It is excellent at one
In the embodiment of choosing, 12h is dried at room temperature and obtains structural catalyst.
The present invention also provides a kind of structural catalysts obtained according to above-mentioned preparation method, wherein the structuring is urged
Agent has the FeOOH hydroxyl from the Al-OH hydroxyl of vigorous nurse body (AlOOH) and from Fe.The result shows that this has two
The structural catalyst of kind hydroxyl has more excellent low concentration formaldehyde clean-up effect, especially purifies super low concentration at room temperature
The hydroxyl groups of the effect of formaldehyde, FeOOH plane of crystal exposure therein are more active, can supplement the quantity of hydroxyl, raising is urged
Agent captures the ability of formaldehyde, so that the progress for promoting catalysis to react, improves catalytic efficiency.
Preferably, the Pt of the Fe and 0.3-2.4wt% of structural catalyst load 1.5-5.5wt%.It is highly preferred that should
Structural catalyst loads the Pt of the Fe and 0.5-1.5wt% of 3.1-5.5wt%.In a preferred embodiment, the structure
Change the Pt of the Fe and 1.2wt% of catalyst load 3.1-4.1wt%.
The present invention also provides a kind of applications of above-mentioned structural catalyst, wherein the content of the formaldehyde in application environment
Greater than 0.08ppm.Particularly, the content of the formaldehyde in application environment is less than 1ppm.Experimental data shows 600ppm first at 25 DEG C
Aldehyde conversion ratio reaches 80%, and 45 DEG C or so formaldehyde convert completely；1ppm formaldehyde decomposed safety value in 25 minutes when room temperature
0.08ppm。
Structural catalyst according to the present invention can not only fast and effeciently catalysis oxidation high-concentration formaldehyde at room temperature,
And it being capable of catalytic oxidation of low-concentration formaldehyde.Moreover, structural catalyst preparation pressure drop is low, heat and mass transfer performance is good, is easy to
Plastotype has good industrial prospect, is suitable for hermetic and half-hermetic spaces formaldehyde pollutants and purifies.In addition, compared to tradition
The integral catalyzers such as ceramics, cordierite, the drop resistant of structural catalyst according to the present invention, resistance to brittle fracture more preferably, are saved
Economic loss brought by more catalyst changeout improves the utilization rate of catalyst activity component.Moreover, the structural catalyst can
Directly to be used with netted or platy morphology, also can be applied in the equipment such as air-conditioning, electric fan, can also well with city
Air purifier on field carries out miniature combination, is easy to industrialize.
Detailed description of the invention
Fig. 1 is the scanning electron microscopy of vigorous nurse body (AlOOH) carrier of integration that preparation method according to the present invention obtains
Mirror photo；
Fig. 2 is the scanning electron microscopy for the Pt/Fe/AlOOH integration catalyst that preparation method according to the present invention obtains
Mirror photo；
Fig. 3 is vigorous nurse body (AlOOH) carrier of integration and Pt/Fe/AlOOH mono- that preparation method according to the present invention obtains
Body catalyst removes the catalytic efficiency schematic diagram of formaldehyde；
Fig. 4 is the obtained Pt/Fe/AlOOH integration catalyst of preparation method according to the present invention except the another of formaldehyde urges
Change efficiency schematic diagram；
Fig. 5 is vigorous nurse body (AlOOH) carrier of integration and Pt that preparation method according to the present invention obtains1.2/Fe3.8/
The X-ray diffractogram of AlOOH integration catalyst；
Fig. 6 is the Pt that preparation method according to the present invention obtains1.2/Fe3.8The thermogravimetric analysis of/AlOOH integration catalyst
Figure.
Specific embodiment
With reference to the accompanying drawing, presently preferred embodiments of the present invention is provided, and is described in detail.
Preparation method according to the present invention includes providing integration vigorous nurse body (AlOOH) carrier first, specific steps packet
It includes: respectively with 10wt%NaOH solution and 10wt%HNO3After solution carries out pre-treatment 4min and 2min to aluminium net or aluminium sheet；It will
Pre-treatment aluminium net or pre-treatment aluminium sheet are immersed in anodizing tank progress anodic oxidation and obtain oxidation aluminium net or alumina plate, specifically
Ground, it is 25A/m that preceding processing aluminium net or preceding processing aluminium sheet, which are placed in current density, at 20 DEG C2, 2-10wt% oxalic acid solution middle-jiao yang, function of the spleen and stomach
Pole aoxidizes 8-16h, is rinsed well with deionized water, air-dries under room temperature；1h is roasted at 350 DEG C, then at 70 DEG C after roasting
It is hydrated 60-70min in deionized water, obtains integrated vigorous nurse body (AlOOH) carrier under room temperature after dry 12h.The integration is vigorous
Scanning electron microscope (SEM) photo of nurse body (AlOOH) carrier is as shown in Figure 1, as seen from the figure, with honeycomb abundant
Porous structure, provide active sites for the absorption of formaldehyde.
Preparation method according to the present invention includes forming Pt/Fe/AlOOH integration catalyst, specific steps packet first
It includes: integrated vigorous nurse body (AlOOH) carrier is respectively placed in the Fe (NO of 0.2,0.4,0.5,0.6,0.8g/L3)3Presoma it is molten
Liquid after impregnating 8h at 25 DEG C, dries 12h at room temperature and obtains the vigorous nurse body of load Fe；The vigorous nurse body for loading Fe is placed in
The H of 0.4g/L2PtCl6In solution, the NaOH of 0.1mol/L is added dropwise to pH of mixed=12, after impregnating 4h at 60 DEG C, room temperature
Lower dry 12h obtains the vigorous nurse body of load Fe and Pt；It is carried out using vigorous nurse body of the liquid phase reduction to load Fe and Pt obtained
Reduction, makes Pt and Fe become zero valence from positive valence state.Specifically, the vigorous nurse body for loading Fe and Pt is placed in concentration is 0.01mol/L
Sodium borohydride solution in restore 1h at 25 DEG C, dry 12h, obtains Pt/Fe/AlOOH integration catalyst under room temperature.It should
The SEM photograph of Pt/Fe/AlOOH integration catalyst is as shown in Fig. 2, as seen from the figure, surface retains honeycomb structure knot abundant
Structure, and Fe is evenly dispersed in its surface.
The load capacity of the Pt and Fe of the Pt/Fe/AlOOH integration catalyst that preparation method according to the present invention obtains are as follows
Shown in table 1.
Table 1
The Pt/Fe/AlOOH integration catalyst that preparation method according to the present invention obtains is applied to high-concentration formaldehyde catalysis
In combustion system, specifically, Pt/Fe/AlOOH integration catalyst is 0.3g, concentration of formaldehyde 200ppm, air speed 3000-
150,000L/ (gh), corresponding catalyst are as shown in Figure 3 except the catalytic efficiency of formaldehyde.All Pt/Fe/AlOOH catalyst are urged
Change reactivity to increase with the raising of reaction temperature.When 25 DEG C at room temperature of temperature, Pt1.2/Fe3.8/AlOOH
Catalyst shows highest catalytic performance, and it is 80% that formaldehyde, which converts formaldehyde conversion,.When temperature is increased to 45 DEG C, Pt1.2/
Fe3.8The upper formaldehyde of/AlOOH catalyst is converted into carbon dioxide CO completely2。
The Pt that preparation method according to the present invention obtains1.2/Fe3.8/ AlOOH integration catalyst is applied to indoor strong wind
Amount, high pressure drop, circulated air and low-methoxyl aldehyde concentration true indoor environment in, the Pt for being 200 × 200 × 0.4mm by size1.2/
Fe3.8/ AlOOH single layer netted catalyst is applied in 3m3In cube cabin.The result shows that room temperature is unglazed, relative humidity 55%
Air in, circulated air volume flow GHSV be 8m3/ s, under conditions of wind speed is 1.30m/s, which can be in 25 minute
Formaldehyde is decomposed into safety value 0.08ppm from 1ppm.Catalytic effect is as shown in Figure 4.
Vigorous nurse body (AlOOH) carrier of the integration that preparation method according to the present invention obtains and Pt1.2/Fe3.8/ AlOOH mono-
The X-ray diffractogram (XRD) of body catalyst is as shown in figure 5, Pt therein1.2/Fe3.8/ AlOOH integration catalyst in addition to
Except the characteristic peak of AlOOH, there are also FeOOH (Ferrihydrite) characteristic peaks to return, and exposes two kinds of crystal faces of AlOOH and FeOOH,
A kind of two kinds of hydroxyl groups of carrier carrying, the hydroxyl groups that this crystal plane structure exposes facilitate formaldehyde in catalyst surface
Adsorpting aggregation, improve catalysis reaction efficiency.
The Pt that preparation method according to the present invention obtains1.2/Fe3.8The thermogravimetric analysis figure (TG) of/AlOOH integration catalyst
As shown in fig. 6, there are three weightless peaks for its tool.The 1st peak that temperature occurs at 90-100 DEG C or so is that physical absorption water is heated de-
It is attached.2nd weightless peak is FeOOH by the weightless peak for thermally decomposing to generate ferriferous oxide at 200-320 DEG C or so；3rd weightless peak
It is the weightless peak that the hydroxyl groups on the surface AlOOH are thermally decomposed at 330-450 DEG C or so.This result confirms Pt1.2/Fe3.8/
AlOOH catalyst surface exposes two kinds of hydroxyl groups, respectively FeOOH and Al-OH.
Above-described, only presently preferred embodiments of the present invention, the range being not intended to limit the invention, of the invention is upper
Stating embodiment can also make a variety of changes.Made by i.e. all claims applied according to the present invention and description
Simply, equivalent changes and modifications fall within the claims of the invention patent.The not detailed description of the present invention is
Routine techniques content.
Claims (10)
1. a kind of preparation method of the structural catalyst of catalysis oxidation formaldehyde, which comprises the steps of:
S1 provides integrated vigorous nurse body carrier；And
Integrated vigorous nurse body carrier is placed in Fe (NO by S23)3Precursor solution in impregnate, be dried to obtain load Fe Bo Mu
Body；The vigorous nurse body for loading Fe is placed in H2PtCl6It is impregnated in solution, is dried to obtain the vigorous nurse body of load Fe and Pt；Also using liquid phase
Former method restores the vigorous nurse body of load Fe and Pt, is dried to obtain structural catalyst.
2. preparation method according to claim 1, which is characterized in that the step S1 is specifically included:
S11 carries out pre-treatment to aluminium net or aluminium sheet with highly basic and strong acid and obtains pre-treatment aluminium net or pre-treatment aluminium sheet；
S12, pre-treatment aluminium net or pre-treatment aluminium sheet are immersed in anodizing tank and carry out anodic oxidation to form one layer of oxygen on surface
Change aluminium film, obtains oxidation aluminium net or alumina plate；And
S13 aoxidizes aluminium net or alumina plate by being hydrated to form the vigorous nurse body carrier of integration rich in hydroxyl after roasting.
3. preparation method according to claim 2, which is characterized in that in the step S12, by pre-treatment aluminium net or preceding
Processing aluminium sheet is placed in 2-10wt% oxalic acid solution Anodic Oxidation.
4. preparation method according to claim 2, which is characterized in that in the step S13, the roasting is in 100-400
It is carried out at DEG C, which carries out in 60-100 DEG C of hot water.
5. preparation method according to claim 1, which is characterized in that in the step S2, the precursor solution is
Fe (the NO of 0.1-0.8g/L3)3Precursor solution.
6. preparation method according to claim 1, which is characterized in that in the step S2, the H2PtCl6Solution is
The H of 0.1-0.8g/L2PtCl6Solution.
7. preparation method according to claim 1, which is characterized in that in the step S2, the vigorous of Fe and Pt will be loaded
Nurse body is placed in the sodium borohydride solution of 0.01-0.05mol/L and restores.
8. a kind of structural catalyst that preparation method described in any one of -7 obtains according to claim 1, which is characterized in that
The structural catalyst has the FeOOH hydroxyl from the Al-OH hydroxyl of vigorous nurse body and from Fe.
9. structural catalyst according to claim 8, which is characterized in that the structural catalyst loads 1.5-
The Pt of the Fe and 0.3-2.4wt% of 5.5wt%.
10. a kind of application of the structural catalyst according to any one of claim 8-9, which is characterized in that apply ring
The content of formaldehyde in border is greater than 0.08ppm.
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| CN111905758A (en) * | 2020-08-18 | 2020-11-10 | 厦门大学 | Gold-based catalyst, preparation method and application thereof |
| CN112742417A (en) * | 2021-01-15 | 2021-05-04 | 华东理工大学 | Noble metal catalyst and preparation method and application thereof |
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| CN112742417A (en) * | 2021-01-15 | 2021-05-04 | 华东理工大学 | Noble metal catalyst and preparation method and application thereof |
| CN112742417B (en) * | 2021-01-15 | 2022-08-09 | 华东理工大学 | Noble metal catalyst and preparation method and application thereof |
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