CN104474890B - A kind of method of Engineering of Supported Metal Oxide Catalysts catalysis Direct Resolution NO denitration - Google Patents
A kind of method of Engineering of Supported Metal Oxide Catalysts catalysis Direct Resolution NO denitration Download PDFInfo
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Abstract
The present invention provides the method for a kind of Engineering of Supported Metal Oxide Catalysts catalysis Direct Resolution NO denitration, described method is carried out in microwave field, and described catalyst is support type O composite metallic oxide catalyst, described support type O composite metallic oxide catalyst is metal composite oxide MOxIt is supported on Al2O3On carrier, described M is two or three in selected from cerium, copper, manganese and nickel.The most described catalyst is selected from CeCuOx/Al2O3、CeMnOx/Al2O3、CeNiOx/Al2O3And CeCuMnOx/Al2O3.In the present invention, microwave catalysis Direct Resolution NO reaction does not has secondary pollution, and technique is simple, and easy to operate easily controllable, NO removal efficiency is high (NO conversion ratio is up to 95.1%), and antioxidant is strong, and operation temperature is low, and energy-conserving and environment-protective, operating cost is low.Flue gas or waste gas after using the inventive method to process can directly reach discharging standards.
Description
Technical field
The present invention relates to catalytic denitration field, be specifically related to a kind of Engineering of Supported Metal Oxide Catalysts catalysis Direct Resolution NO
The method of denitration.
Background technology
Nitrogen oxides is one of major pollutants of serious harm human health, and its more than 95% composition is NO.According to estimates,
China coal-burning power plant NO in 2015xDischarge capacity is up to 13,100,000 tons, it is seen that the discharge controlling NO is particularly important.
Along with improving constantly of human living standard, countries in the world all pay much attention to the research administered containing nitrogen oxides emissions,
Promotion and application.
The direct breakdown method of NO is because having economy, not consuming NH3、CO、CH4Deng reducing agent, do not produce secondary pollution
Feature is it is considered to be the method for most captivation.The reaction that NO decomposes isNO Direct Resolution is N2
And O2It is feasible for reaching 99% in the range of thermodynamics, but reaction activity is up to 364KJ/mol, therefore studies
The decomposition essence of NO is to inquire into its dynamic (dynamical) problem, namely finds suitable catalyst and the catalysis process of this reaction.
Numerous studies show, a lot of metal-oxides particularly catalyst of transition metal oxide all has certain urging to NO
Change degrading activity.Relative to noble metal, metal oxide catalyst cheap.But, the most at high temperature gold
Belong to oxide catalyst and just show the activity with direct catalytic decomposition NO；And this kind of catalyst nearly all exists strongly
Oxygen resistance phenomenon, the oxygen coexisted in actual waste gas makes NO conversion ratio seriously reduce.
Additionally, microwave energy has gained universal acceptance as one is high-effect.Huang Kama et al. has done long-time a series of grind
Study carefully, it is believed that microwave can change the interaction between molecule, significantly improve the speed of some chemical reaction and change reaction
Mechanism.Wei Shan makees catalyst and NH with Fe/Ga-5A4HCO3Make reducing agent selective reduction removing NO under microwave catalysis.
Zhang Tao et al. utilizes microwave discharge to process NO (without catalyst), achieves good effect.Tang Junwang is at microwave heating mould
Under formula and conventional heating pattern, carrying out denitration research with Fe/ZSM-5 catalyst, result shows that microwave heating can allow the most not
The reaction of energy catalytic decomposition there occurs really, and NO reaches the conversion ratio of 70%.
Although the studies above is all a lot, but from the point of view of disclosed data, best NO conversion ratio is about 70%, removing
Rate is the highest；And big by influence of oxygen content in waste gas, when oxygen content is bigger, the method does not reaches removing requirement.
Summary of the invention
The highest in order to solve NO removal efficiency present in prior art, that technics comparing is complicated problem, the present invention provides a kind of
Simple for process, removal of nitrogen oxide rate is high, the method for economical and practical removing nitrogen oxides of exhaust gas.
Based on above-mentioned prior art, the present inventor is in view of the most at high temperature metal oxide catalyst just table
Reveal the activity with direct catalytic decomposition NO；And this kind of catalyst nearly all exists strong oxygen resistance phenomenon, actual
The oxygen coexisted in waste gas makes NO conversion ratio seriously reduce.Therefore inventor attempts to find one and metal oxide catalyst
The efficient energy matched acts on the activation energy reducing reaction jointly so that the Direct Resolution of NO can be smoothed out.Examine
Consider and gained universal acceptance as one is high-effect to microwave energy.Therefore, inventor tries to carry out metal oxide catalyst
It is catalyzed the Direct Resolution of NO with mating of microwave energy.But microwave can not start all of metal-oxide at cryogenic conditions
Under the Direct Resolution reaction of NO in raw material is played efficient catalytic action, until the present inventor finds a kind of specific modified
Metal oxide catalyst so that this catalyst can form good coordinating with microwave in catalysis NO Direct Resolution reacts.
Therefore, the present invention provides the method for a kind of Engineering of Supported Metal Oxide Catalysts catalysis Direct Resolution NO denitration, described
Method is carried out in microwave field, and described catalyst is support type O composite metallic oxide catalyst, the compound gold of described support type
Belonging to oxide catalyst is metal composite oxide MOxIt is supported on Al2O3On carrier, described M is selected from cerium, copper, manganese
With two or three in nickel.In the present invention, described support type O composite metallic oxide catalyst is prepared for example with infusion process.
In a kind of specific embodiment, the M in described support type O composite metallic oxide catalyst includes at least cerium.Send out
A person of good sense finds, when in the metal composite oxide of catalyst containing cerium, the amplitude that catalyst performance improves further is clearly.
The most described catalyst is selected from CeCuOx/Al2O3、CeMnOx/Al2O3、CeNiOx/Al2O3And CeCuMnOx/Al2O3；
More preferably CeCuMnOx/Al2O3.Preferably, M and Al in described support type O composite metallic oxide catalyst2O3Carry
In body, the ratio of the amount of the material of aluminium element is 0.06～0.6:1, preferably 0.12～0.4:1.
In a kind of specific embodiment, the reaction tube of microwave catalysis reactor assembly is filled the compound gold of described support type
Belong to oxide catalyst and form microwave catalysis reaction bed, pending waste gas when by microwave catalysis reaction bed, at microwave and
The common effect of described catalyst issues raw gas-solid catalytic reaction, and the direct catalytic decomposition of NO therein becomes N2And O2.At this
In invention, the temperature of catalytic reaction for example, 100～300 DEG C, preferably 200～250 DEG C.
In the present invention, in described pending waste gas, the content of oxygen is 0.1～20%, preferably 1～15%, more preferably
7.5～10%.The waste gas that the catalysis process that the present invention provides is particularly suitable for oxygen content is higher processes, oxygen in waste gas
Content more Gao Yueneng embodies the inventive method advantage compared to existing technology.
In the present invention, the described pending waste gas time of staying for example, 0.5-10s in microwave catalysis reaction bed, preferably
1-3s.Microwave frequency of the present invention is 500～3000MHz.
When in the use present invention, specific support type O composite metallic oxide catalyst coordinates with microwave, can be at low temperature and height
Direct catalytic decomposition NO under the conditions of oxygen content.The present inventor is found through experiments, with this special in the present invention
When support type metal composite oxide is catalyst Direct Resolution NO denitration, described catalyst can absorb microwave.
The present invention correspondingly provides a kind of load metal oxide being catalyzed Direct Resolution NO denitration under microwave condition and urges
Agent, it is characterised in that described catalyst is support type O composite metallic oxide catalyst, described support type composition metal oxygen
Compound catalyst is metal composite oxide MOxIt is supported on Al2O3On carrier, described M is selected from cerium, copper, manganese and nickel
In two or three；The most described catalyst is CuMnOx/Al2O3、CeCuOx/Al2O3、CeMnOx/Al2O3、
CeNiOx/Al2O3And CeCuMnOx/Al2O3In one or more.
Compared with prior art, the invention have the advantages that microwave catalysis Direct Resolution NO reaction does not has secondary pollution,
And technique is simple, easy to operate easily controllable, NO removal efficiency is high (NO conversion ratio is up to 95.1%), and antioxidant is strong,
Operation temperature is low, and energy-conserving and environment-protective, operating cost is low.Flue gas or waste gas after using the inventive method to process can directly reach
Discharging standards.
Detailed description of the invention
It is described in further detail below in conjunction with embodiment.
Embodiment 1 and comparative example 1
Engineering of Supported Metal Oxide Catalysts uses equi-volume impregnating to prepare.First, activated alumina is 500 DEG C of roastings
2h, obtains Al2O3Carrier.Then Al2O3Carrier mixes, in room temperature with the metal-nitrate solutions equal-volume of variable concentrations
The lower ultrasonic 0.5h of elder generation, then impregnates 24h.Afterwards the dip compound obtained is dried 6h at 100 DEG C.Then at 500 DEG C
Roasting 2h, prepares a series of Al2O3Metal oxide supporting catalyst.The load capacity of metal-oxide is as shown in table 1.
Table 1
Embodiment 2 and comparative example 2
It is anti-that the method for the invention is included in catalyst filling formation microwave catalysis in the reaction tube of microwave catalysis reactor assembly
Answering bed, processed gas occurs gas-solid phase reaction to carry out denitration process when by microwave catalysis reaction bed.Described catalyst is
Prepare in embodiment 1 and comparative example 1 is metal oxide supported at Al2O3On carrier, consist of CuOx/Al2O3、
MnOx/Al2O3、NiOx/Al2O3、CuMnOx/Al2O3、CeCuOx/Al2O3、CeMnOx/Al2O3、CeNiOx/Al2O3
And CeCuMnOx/Al2O3Catalyst；Described catalyst is filled in the reaction tube of microwave catalysis reactor assembly, processed
Gas is through microwave catalysis reaction bed, and the NO in gas occurs the N that Direct Resolution reaction build environment is friendly2And O2,
To reach the purpose of direct denitration.
In this example, described waste gas for Dalian great Te gas company limited provide for N2The gaseous mixture formed with NO, wherein
NO concentration is 1000ppm.NOxAnalyser is Americanized 42C NO-NO2-NOx Analyzer。
Microwave power is at 0-1000w continuously adjustabe, and frequency is 2400-2500MHz.Quartz tube reactor is
WG1/2.45-Φ5.4×54.Quartzy pipe range 540mm, internal diameter 10mm used by this experiment.
Catalyst is filled in composition beds in quartz tube reactor, and the waste gas of above-mentioned test enters through beds
The reaction of row microwave catalysis Direct Resolution NO.Catalyst filling amount is 1.5g, and mesh number is 40-60 mesh.Air inlet NO concentration
For 1000ppm, oxygen content is 5%, and the gas time of staying in microwave catalysis reaction bed is 1s, and reaction pressure is normal pressure.
Regulation microwave power, changes the reaction bed temperature of catalyst, makes bed temperature be respectively maintained at 100 DEG C, 150 DEG C, 200 DEG C
With 250 DEG C, carry out the experiment of microwave catalysis Direct Resolution NO, experimental result is as shown in table 2.
Table 2
Catalyst CuO when reaction bed temperature is 100 DEG C, in comparative example 2x/Al2O3、MnOx/Al2O3With
NiOx/Al2O3Just showing the activity decomposing NO, its NO conversion ratio is respectively 58.3%, 68.7% and 74.3%.When urging
When agent bed temperature is 250 DEG C, on the catalyst in comparative example 2, NO conversion ratio is increased to 73.7%, 81.6% and respectively
82.7%.In the case of visible low temperature, Engineering of Supported Metal Oxide Catalysts just shows certain microwave catalysis and decomposes NO
Activity, but such NO rates of decomposing and transforming make use the method process after flue gas or waste gas be also difficult to directly reach state
Family's discharge standard.
But in the support type O composite metallic oxide catalyst shown in embodiment 2, when reaction bed temperature is 100 DEG C,
Catalyst just shows the activity of of a relatively high decomposition NO, CuMnOx/Al2O3、CeCuOx/Al2O3、
CeMnOx/Al2O3、CeNiOx/Al2O3And CeCuMnOx/Al2O3On catalyst NO conversion ratio be respectively 71.1%,
65.7%, 74.3%, 75.2% and 74.2%.When reaction bed temperature is 250 DEG C, NO conversion ratio on these catalyst
It is increased to 89.7%, 87.6%, 86.2%, 85.2% and 94.8% respectively.Compared with comparative example 2, it is seen that the compound gold of support type
The catalysis activity belonging to oxide catalyst is greatly improved.And at low temperature 250 DEG C, under the conditions of oxygen content is 5%,
CeCuMnOx/Al2O3The conversion ratio of upper microwave catalysis Direct Resolution NO may be up to 94.8%, illustrates to add modified the bearing of Ce
The catalytic performance of load type O composite metallic oxide catalyst is the most excellent.
Embodiment 3 and comparative example 3
Essentially identical with embodiment 2 and comparative example 2, except for the difference that changing the content of oxygen in air inlet is 0-10%.
Catalyst filling amount in embodiment 3 and comparative example 3 is respectively 1.5g, and mesh number is 40-60 mesh.Air inlet NO concentration
For 1000ppm, changing the content of oxygen in air inlet is 0%, 5%, 7.5%, 10%, and gas is in microwave catalysis reaction bed
The time of staying be 1s, reaction pressure is normal pressure.Regulation microwave power, makes reaction bed temperature be respectively maintained at 250 DEG C,
Investigate this catalyst antioxidant when microwave catalysis decomposes NO.Result is as shown in table 3.
Table 3
In the presence of oxygen, the conversion ratio of NO is not affected by oxygen concentration on each catalyst, shows comparative example and embodiment
In Engineering of Supported Metal Oxide Catalysts under microwave catalysis pattern, be respectively provided with good antioxidant.It addition, at oxygen content
Up to 10% and low temperature 250 DEG C under the conditions of, CeCuMnOx/Al2O3The conversion ratio of upper microwave catalysis Direct Resolution NO still can be high
Reach 95.1%.The flue gas after method processes in the present invention or waste gas is used easily to directly reach discharging standards.
Comparative example 4
Under as disclosed in prior art, data investigates popular response pattern, when 400 DEG C, metal composite oxide (includes
CuMnOx/Al2O3、CeCuOx/Al2O3、CeMnOx/Al2O3、CeNiOx/Al2O3And CeCuMnOx/Al2O3) catalysis
The performance of NO Direct Resolution.Experiment finds, composite metal oxide catalyst NO Direct Resolution reacts almost without activity.
Additionally, (500～600 DEG C) above-mentioned composite metal oxide catalyst Direct Resolution NO reaction is deposited under higher temperature conditions
Hinder at serious oxygen so that NO rates of decomposing and transforming drastically declines.
Claims (3)
1. the method for an Engineering of Supported Metal Oxide Catalysts catalysis Direct Resolution NO denitration, it is characterized in that, described method is carried out in microwave field, and described catalyst is support type O composite metallic oxide catalyst, and described support type O composite metallic oxide catalyst is metal composite oxide MOxIt is supported on Al2O3On carrier, and this catalyst is CeCuMnOx/Al2O3, M and Al in described support type O composite metallic oxide catalyst2O3In carrier, the ratio of the amount of the material of aluminium element is 0.12～0.4:1；Described method is included in the reaction tube of microwave catalysis reactor assembly fills described support type O composite metallic oxide catalyst formation microwave catalysis reaction bed, pending waste gas is when by microwave catalysis reaction bed, common effect at microwave and described catalyst issues raw gas-solid catalytic reaction, and the direct catalytic decomposition of NO therein becomes N2And O2, the temperature of catalytic reaction is 200～250 DEG C, and in pending waste gas, the content of oxygen is 1～15%, and the described pending waste gas time of staying in microwave catalysis reaction bed is 0.5-10s.
Method the most according to claim 1, it is characterised in that the described pending waste gas time of staying in microwave catalysis reaction bed is 1-3s.
Method the most according to claim 1, it is characterised in that described microwave frequency is 500～3000MHz.
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| CN104874394A (en) * | 2015-05-19 | 2015-09-02 | 大连理工大学 | Cheap low-temperature SCR catalyst with sulfur resistance and preparation method thereof |
| CN106345292A (en) * | 2016-10-10 | 2017-01-25 | 湘潭大学 | Method for directly decomposing NO by microwave catalysis and catalyst |
| CN106345488A (en) * | 2016-11-07 | 2017-01-25 | 北京石油化工学院 | Copper-manganese-cerium composite oxide FCC regenerated flue gas combustion-supporting denitration auxiliary agent and preparation method thereof |
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| CN109876657A (en) * | 2019-04-01 | 2019-06-14 | 萍乡市华星环保工程技术有限公司 | The method of integrated treatment volatile organic waste gas |
| CN113135552B (en) * | 2020-01-19 | 2023-02-07 | 中南大学 | Method for preparing chlorine by catalytic oxidation of hydrogen chloride |
| CN112452129B (en) * | 2020-12-14 | 2022-04-15 | 苏州大学 | Ternary NiO nanosheet @ bimetal CeCuOxMethod for low-temperature heat treatment of toluene by using microchip core-shell structure composite material |
| CN114653375A (en) * | 2020-12-23 | 2022-06-24 | 中国科学院江西稀土研究院 | Catalyst for removing CO in sintering flue gas and preparation method thereof |
| CN114643055B (en) * | 2022-04-08 | 2023-07-07 | 浙江大学 | Nano-gold-loaded nano cerium oxide for catalyzing direct decomposition of nitrogen oxides and preparation method thereof |
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