CN103721710A - Supported Pt catalyst as well as preparation method and application of supported Pt catalyst - Google Patents
Supported Pt catalyst as well as preparation method and application of supported Pt catalyst Download PDFInfo
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- CN103721710A CN103721710A CN201410006189.5A CN201410006189A CN103721710A CN 103721710 A CN103721710 A CN 103721710A CN 201410006189 A CN201410006189 A CN 201410006189A CN 103721710 A CN103721710 A CN 103721710A
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
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- Y02A50/20—Air quality improvement or preservation, e.g. vehicle emission control or emission reduction by using catalytic converters
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Abstract
The invention relates to a supported Pt catalyst as well as a preparation method and application of the supported Pt catalyst. The preparation method comprises the following steps of firstly supporting a Pt nano particle onto a TiO2 semiconductor oxide carrier with light absorption and CeO2 with strong low-temperature catalytic activity and oxygen storage capacity to prepare the supported Pt catalyst; and then introducing ultraviolet irradiation to a reaction system for catalyzing CO/NO by the catalyst. Compared with a conventional thermal catalytic reaction (without ultraviolet irradiation), the catalyst has the advantages that ultraviolet irradiation is capable of remarkably promoting catalysis of a Pt supported thermal catalyst to remove CO/NO. By using an optothermal coupling method, the use temperature of the catalyst is greatly reduced the optothermal coupling method is simple and easy to operate and is favorably applied to removal of NO and CO in automobile exhaust purification.
Description
Technical field
The invention belongs to catalytic elimination CO/NO reaction field, specifically relate to a kind of method that improves Pt catalyst removal CO/NO performance by photo-thermal coupling.
Background technology
Along with increasing sharply of city automobile, motor vehicle exhaust emission has become one of main air pollution source in city.The discharge of vehicle exhaust has caused great harm not only to our life, environment, is also a kind of very important injury to the health of human body simultaneously.The atmosphere oneself detergent power vehicle exhaust of can not having degraded, so solve automobile exhaust pollution, also clean environment of the mankind has been extremely urgent.
Scientific analysis shows, contains hundreds of different compound in vehicle exhaust, and pollutant wherein has Solid Suspension particulate, carbon monoxide, carbon dioxide, hydrocarbon, oxynitrides, lead and oxygen sulfur compound etc.For the control of motor vehicle exhaust emission amount, in the policy of various countries, experienced a series of change, from the initial discharge that only limits CO, to the discharge that is discharged into last integrated CO, HCs and nitrogen oxide NO of restriction CO and HCs; Simultaneously in scientific research, people attempt controlling the especially content carbon monoxide CO to the more serious gas of atmosphere pollution vehicle exhaust, hydrocarbon HCs and nitrogen oxide NOx from each side such as chemical fuel, engine combustion efficiency, catalyst always.
The technological means of administering automobile gas emission pollution mainly can be divided three classes: the one, and emission controls by improving combustion technology; as fuel qualities is improved. PCV system; EVAP recovery system; the transformation of combustion system, oil supply system and ignition system; EGR; in blast pipe, spray auxiliary air, high-energy ignition and lean burn etc.; The 2nd, external purification; mainly to carry out outward processing to reach the object that reduces motor vehicle exhaust emission aspect some at engine body; with regard to the development of current external purification technology; the direction of main research is to be generally mounted in automobile exhaust system to the arrangement for catalytic purification of the research vehicle exhaust of the catalytic purification of vehicle exhaust; adopt Catalysis Principles to carry out the exhaust gas processing device of the harmful substances such as carbon monoxide in purifying automobile tail gas, oxynitrides, hydrocarbon, this is a kind of device of integrated treatment on the whole that can carry out vehicle exhaust; The 3rd, use clean alternative fuel, as natural gas, liquefied petroleum gas or electric energy etc.
At emission controls by improving combustion technical research, run into bottleneck and green energy resource temporarily can not replace fossil fuel now, cleaning catalyst for tail gases of automobiles is just obtaining increasingly extensive application as environmental protection with catalyst.Three-way catalyst is the catalyst using in vehicle exhaust three-way catalytic converter, it has high activity, high selectivity, high thermal stability, good physical behavior, can remove the pollutants such as CO, HC in vehicle exhaust and NOx, be comparatively desirable auto-exhaust catalyst simultaneously.Three-way catalyst mainly comprises carrier and active component, and carrier is generally cellular an aromatic plant metioned in ancient books green stone, and active component research more be precious metals pt, Pd, Rh.
The main chemical reactions of three-way catalyst
Oxidation reaction CO+1/2 O of CO, HC
2→ CO
2
CxHy+（x+1/2y）O
2?→xCO
2+?1/2yH
2O
Reduction reaction NO+CO → 1/2N of NO
2+ CO
2
Especially the reduction reaction with NO is difficult to carry out, and this is also a difficult point in three-way catalyst research.
The research catalytic elimination CO/NO of relevant three-way catalyst reaches its maturity, wherein Pt, Pd, Rh are the active metal components of studying at most, particularly the catalyst of relevant Pt has occurred that more patent emerges in an endless stream especially, but also it should be noted that some limitation of thermocatalytic removal CO/NO simultaneously: three-way catalyst poison deactivation, the inactivation main Types of three-way catalyst has: mechanical inactivation, heat inactivation and chemical inactivation; Life-span is short, operation temperature area is narrow; Precious Metals Resources is deficient, cost is high; Nitrous oxides selectivity under lean-burn condition.
Therefore, how to improve the conversion ratio that low temperature is removed CO/NO reactivity, CO and NO, N
2selectively for purifying vehicle exhaust, have great significance.
Summary of the invention
The invention provides by photo-thermal coupling and improve the method that Pt catalyst is removed CO/NO performance, its object is to overcome the deficiency that above-mentioned simple thermocatalytic is removed CO/NO, improves low temperature active and the N of this type of catalyst
2selectively.The present invention is directed to conventional Pt loaded catalyst need be under higher temperature could catalysis CO and N
2selective low problem, selection has the conductor oxidate of optical excitation activity and prepares Pt loaded catalyst as carrier, and add according to NO+CO reaction characteristics the Ce that oxygen storage capacity is strong, strengthen contacting between Pt and carrier, in course of reaction, introduce ultraviolet lighting, thereby significantly improve the performance of its catalytic elimination CO/NO, greatly reduce the reaction temperature of catalyst, reduced energy consumption, and this method for preparing catalyst is simple, is conducive to apply.
The present invention implements by following technical solution:
First make supported Pt catalysts, then in the reaction system of supported Pt catalysts catalysis CO/NO, introduce ultraviolet lighting.
Above-mentioned reaction system is normal pressure continuous-flow device, this normal pressure continuous-flow device comprises the thermocouple interface with quartz glass reactor and the detected temperatures of air inlet and gas outlet, the inner chamber of described quartz glass reactor is filled with supported Pt catalysts, the all sides of described quartz glass reactor are provided with heater and for exciting the catalyst carrier of supported Pt catalysts to produce the UV-light luminous device of photoresponse, the ultraviolet light that described UV-light luminous device sends can see through quartz glass reactor and arrive supported Pt catalysts surface.
Described supported Pt catalysts is with TiO
2and the strong CeO of oxygen storage capacity
2for carrier, the Pt nano particle high-dispersion loading type catalyst that is active component, and in described supported Pt catalysts, the content of active component Pt is 0.2-2.0wt%, CeO
2for 5-20wt%, all the other are TiO
2carrier.Concrete preparation process is as follows:
Step (1): ethylene glycol adds acetone and deionized water after reacting 5-10h with tetra-n-butyl titanate, being deposited at 60-80 ℃ of obtaining is dry, then adds the CeCl of proportional quantity
3and urea is transferred in water heating kettle hydro-thermal 4-10h at 150-180 ℃ and is obtained TiO
2-CeO
2carrier;
Step (2): the carrier making in step (1) adds H
2ptCl
6solution, stirs 30min-1h, and ultrasonic 15-30min, adds the NaBH containing NaOH at turbid solution
4in solution, under room temperature, stir 2 ~ 6h, centrifugal, deionized water washes away after unnecessary ion, and vacuum drying at 60-80 ℃, makes Pt loaded catalyst;
Wherein, H
2ptCl
6molar concentration containing Pt in solution is 0.01-0.1mol/L, the described NaBH containing NaOH
4in solution, NaBH
4the concentration of solution is 0.01-0.1mol/L, and the concentration of NaOH is 0.01-0.1mol/L.
Described supported Pt catalysts is for the conversion of the NO+CO of vehicle exhaust and fuel vent.
Remarkable advantage of the present invention is:
(1) the present invention is with TiO
2-CeO
2oxide, as carrier, has not only been brought into play CeO
2the feature that cryogenic effect is strong and oxygen storage capacity is large in vehicle exhaust is processed, more take full advantage of semiconductor and can excite the feature that produces electron hole pair under the illumination of certain wavelength, when Pt is carried in examples of such carriers, light induced electron can be transferred to the Pt metal that fermi level is low from the high semiconductor of fermi level, thereby improve the electric surface density of active metal Pt, simultaneously CeO
2and TiO
2between interaction improved the efficiency in active component Pt transmission electronic and hole, be beneficial to absorption and the activation of CO and NO, and then promote the carrying out of CO/NO reaction, CO conversion ratio and N
2selectively all very high.Compare with simple heat catalysis, photo-thermal coupled reaction of the present invention can reduce reaction temperature, thereby has the effect of the energy consumption of minimizing.
(2) preparation method of the present invention and application operating method are simple, are conducive to apply.
Accompanying drawing explanation
Fig. 1 is embodiment 1 gained 1wt%Pt/CeO
2-TiO
2scanning electron microscope (SEM) photograph.
Fig. 2 is embodiment 1 gained 1wt%Pt/CeO
2-TiO
2bET figure.
Fig. 3 is embodiment 1 gained 1wt%Pt/CeO
2-TiO
2xRD figure.
Fig. 4 is embodiment 1 gained 1wt%Pt/CeO
2-TiO
2ultraviolet-spectrogram diffuses.
Fig. 5 is catalyst performance evaluation reaction system sketch.1. being air inlet, is 2. gas outlet, is 3. heater, is 4. quartz reactor, is 5. catalyst granules, is 6. ultraviolet source.
The specific embodiment
For above-mentioned feature and advantage of the present invention can be become apparent, special embodiment below, and coordinate accompanying drawing, be described in detail below, but the present invention is not limited to this.
Embodiment 1
Pt/CeO
2-TiO
2the preparation of catalyst
By 200mL ethylene glycol and 8 mL tetra-n-butyl titanate mix and blend 6h, then add 300mL acetone and 8mL deionized water, continue to stir 1h centrifugal after precipitation is complete, deionized water is washed rear 80 ℃ of dry TiO
2presoma.At TiO
2in presoma, add 0.2gCeCl
3with 1g urea, and add 60mL deionized water, be transferred to hydro-thermal reaction 10h at 150 ℃ of water heating kettles and obtain TiO
2-CeO
2carrier.Take 1.0g TiO
2-CeO
2carrier, measuring 8 mL concentration is the H between 0.05mol/L
2ptCl
6solution joins in carrier, and introduces 100mL deionized water, stirs 30min, ultrasonic 15min, and pH value to 10 left and right of regulator solution, slowly drips the NaBH that contains 0.1mol/L
4can be reduced completely to the excessive Pt made from the solution of 0.1mol/L NaOH, centrifugal, deionized water is washed to ion concentration lower than 11ppm, dries at 80 ℃, obtains Pt content and is about 1wt%, CeO
2content is about Pt/CeO of 10wt%
2-TiO
2catalyst.
Embodiment 2
The performance evaluation of catalyst
The prepared catalyst of embodiment 1 is removed the performance evaluation of CO/NO and is carried out on the normal pressure continuous-flow reaction unit with panel heater one.About 0.6g Catalyst packing is in the dull and stereotyped reactor of quartz (the high 1mm of the wide 15mm* of long 30mm*), catalyst particle size is about 0.2 ~ 0.3mm(60 ~ 80 order), in reaction gas, the content of CO and NO is fixed as respectively 0.5V% and 0.5V%, He gas supplements gas, the about 100mL/min of reaction gas overall flow rate as balance.Reaction temperature is regulated and controled by temperature programming temperature controller.Adopt CO, NO, CO in AIDE-OW/AI300 on-line analysis atmosphere
2concentration, the result that negate is answered 2 hours is calculated CO conversion ratio and N
2selective.
CO conversion ratio calculates with following formula: C1=(V
inCO-V
outCO)/V
inCO* 100%
NO conversion ratio calculates with following formula: C2=
(v
inNO-V
outNO )/ V
inNO* 100%
N
2the following formula of selective use calculates: S=2V
outN2/ (V
inNO-V
outNO) * 100%
In formula, the conversion ratio that C1 is CO, the conversion ratio that C2 is NO, S is N
2selectively; V
inCOand V
outCObe respectively air inlet and give vent to anger in CO content (V%), V
inNOand V
outNObe respectively air inlet and give vent to anger in NO content (V%), V
outN2for the N in effluent gases
2content (V%).
In this way, evaluated respectively the performance of the catalytic elimination CO/NO of various catalyst, its result is as shown in the table:
Pt/CeO before and after table 1 ultraviolet lighting
2-TiO
2the performance of catalytic elimination CO/NO
In upper table, result shows, for each catalyst, than the reaction condition of pure heat, under light+heat effect, the conversion ratio of CO all improves a lot, and N
2selective also purer thermal rection condition under selective height.Visible, illumination effect can improve performance and the N of the catalytic elimination CO/NO of this type of catalyst
2selectively.
From Fig. 1 and Fig. 2, can find out Pt/CeO
2-TiO2 catalyst has unique nucleocapsid solid microsphere structure to allow it have larger specific area, and melt and less aperture in larger hole, for the absorption of NO and CO, has very large facilitation; As can be seen from Figure 3,, because Pt content is low, in the XRD spectra of catalyst, only there is TiO
2diffraction cutting edge of a knife or a sword, this has also illustrated being uniformly dispersed of Pt particle in catalyst; As can be seen from Figure 4 except there is TiO in this catalyst,
2light absorption outside, at whole light absorption wave band absorption region, become wider, be conducive to the absorption for light, bring into play the short effect of better light; In Fig. 5 reactor feed gas by 1. enter catalyst granules is housed reactor 4. in, by the heater of being controlled by temperature programming temperature controller, 3. to reactor, provide temperature required, and 6. reactor imposed to ultraviolet lighting.
The foregoing is only preferred embodiment of the present invention, all equalizations of doing according to the present patent application the scope of the claims change and modify, and all should belong to covering scope of the present invention.
Claims (7)
1. a supported Pt catalysts, is characterized in that: described supported Pt catalysts is with CeO
2-TiO
2for carrier, the high-dispersion loading type catalyst that Pt nano particle is active component.
2. supported Pt catalysts according to claim 1, is characterized in that: in described supported Pt catalysts, the content of active component Pt is 0.2-2.0wt%, CeO
2content 5-20wt%, all the other are TiO
2carrier.
3. a method of preparing supported Pt catalysts as claimed in claim 1, is characterized in that: comprise the following steps:
(1) utilize hydro-thermal method to make solid microsphere CeO
2-TiO
2carrier;
(2) utilize load active component Pt on the carrier that deposition-precipitation method makes in step (1).
4. the preparation method of supported Pt catalysts according to claim 3, is characterized in that: with CeCl
37H
2o and butyl titanate are presoma, centrifugal after 150-180 ℃ of common hydro-thermal 4-10h, deionized water washing, and 60-80 ℃ of dry 6-10h obtains CeO
2-TiO
2carrier; The CeO making
2-TiO
2in carrier, add H
2ptCl
6solution and deionized water, stir 30min-1h, and ultrasonic 15-30min, adds the NaBH containing NaOH
4solution, stirs 2-5h under room temperature, centrifugal, deionized water washing, and 60～80 ℃ of vacuum drying, make CeO
2-TiO
2supported Pt catalysts.
5. the preparation method of supported Pt catalysts according to claim 4, is characterized in that: described H
2ptCl
6the concentration of solution is 0.01-0.1mol/L, the described NaBH containing NaOH
4in solution, NaBH
4the concentration of solution is 0.01-0.1mol/L, and the concentration of NaOH is 0.01-0.1mol/L.
6. an application for supported Pt catalysts as claimed in claim 1, is characterized in that: described supported Pt catalysts is applied to the removal of CO and NO in vehicle exhaust.
7. the application of supported Pt catalysts according to claim 6, is characterized in that: in the reaction system of supported Pt catalysts catalysis CO/NO, introduce ultraviolet lighting.
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Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN107020138A (en) * | 2017-05-09 | 2017-08-08 | 福州大学 | A kind of Supported Pd-Catalyst and its preparation method and application |
| CN113786842A (en) * | 2021-09-13 | 2021-12-14 | 福州大学 | Catalyst for synthesizing ammonia from NO oxide and preparation method and application thereof |
| CN114950402A (en) * | 2022-06-28 | 2022-08-30 | 苏州金宏气体股份有限公司 | TiO 2 /CeO 2 Heterojunction photocatalyst and preparation method thereof |
| CN116510510A (en) * | 2023-06-11 | 2023-08-01 | 连云港中星能源有限公司 | Efficient energy-saving denitration process based on electric heating assistance |
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| EP1053778A1 (en) * | 1999-05-19 | 2000-11-22 | Ford Global Technologies, Inc. | Method for manufacturing a three-way catalyst |
| CN101574648A (en) * | 2009-05-18 | 2009-11-11 | 刘光文 | Rare transition-metal catalyst for catalytic purification of CO, Nox and HC |
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Cited By (7)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN107020138A (en) * | 2017-05-09 | 2017-08-08 | 福州大学 | A kind of Supported Pd-Catalyst and its preparation method and application |
| CN107020138B (en) * | 2017-05-09 | 2019-06-07 | 福州大学 | A kind of Supported Pd-Catalyst and its preparation method and application |
| CN113786842A (en) * | 2021-09-13 | 2021-12-14 | 福州大学 | Catalyst for synthesizing ammonia from NO oxide and preparation method and application thereof |
| CN113786842B (en) * | 2021-09-13 | 2023-08-04 | 福州大学 | Catalyst for synthesizing ammonia from NO oxide, preparation method and application thereof |
| CN114950402A (en) * | 2022-06-28 | 2022-08-30 | 苏州金宏气体股份有限公司 | TiO 2 /CeO 2 Heterojunction photocatalyst and preparation method thereof |
| CN116510510A (en) * | 2023-06-11 | 2023-08-01 | 连云港中星能源有限公司 | Efficient energy-saving denitration process based on electric heating assistance |
| CN116510510B (en) * | 2023-06-11 | 2023-09-26 | 连云港中星能源有限公司 | Efficient energy-saving denitration process based on electric heating assistance |
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| CN103721710B (en) | 2015-08-12 |
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