CN103977680A - Room temperature catalytic oxidation-solid alkali absorption method for purifying nitrogen oxide of semi-closed space - Google Patents

Room temperature catalytic oxidation-solid alkali absorption method for purifying nitrogen oxide of semi-closed space Download PDF

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CN103977680A
CN103977680A CN201410210507.XA CN201410210507A CN103977680A CN 103977680 A CN103977680 A CN 103977680A CN 201410210507 A CN201410210507 A CN 201410210507A CN 103977680 A CN103977680 A CN 103977680A
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China
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pollutant
catalytic oxidation
solid base
hours
room
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CN201410210507.XA
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Chinese (zh)
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郭杨龙
王洁
卢冠忠
王爱勇
詹望成
郭耘
王丽
王筠松
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华东理工大学
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Abstract

The invention discloses a room temperature catalytic oxidation-solid alkali absorption technology for thoroughly removing low-concentration NOx pollutant emitted by a semi-closed space such as a road tunnel and an underground parking lot, belonging to the field of air pollution control. The technology concretely comprises the steps of oxidizing the NO part in the NOx pollutant into NO2 by taking O2 in the air as an oxidizing agent under the action of a high-performance NO room temperature oxidation catalyst, and enabling the NO2 to account for 50-60% of the NOx pollutant; thoroughly removing the NOx pollutant by a solid alkali absorbent. The room temperature catalytic oxidation-solid alkali absorption technology is high in waste gas treatment airspeed, has the NOx removal rate reaching up to 100%, is capable of avoiding the generation of a great deal of waste liquid, and is low in waste gas treatment cost, thus having better application prospect.

Description

Room-temperature catalytic oxidation-solid base absorption process purifies the nitrogen oxide of hemi-closure space

Technical field

The present invention relates to a kind of low concentration of NO for the discharge of the hemi-closure space such as roads and tunnels and underground parking xroom-temperature catalytic oxidation-solid base absorption techniques that pollutant is thoroughly eliminated, belongs to Air Pollution Control field.

Background technology

Along with the quick increase of through street and vehicle guaranteeding organic quantity, in order to solve the problem such as urban traffic blocking and parking difficulty of increasingly sharpening, the quantity of the hemi-closure space facilities such as roads and tunnels and underground parking also sharply increases.But in this class hemi-closure space, air flow property is poor, adds motor vehicle cold start or frequent starting, causes discharged pollutant constantly to accumulate, so that as particle (PM), carbon monoxide (CO), nitrogen oxide (NO x) and the pollutant load superstate secondary air far away quality standard such as hydrocarbon (HC).NO xenter the formation that can cause acid rain, photochemical fog in atmospheric environment, participate in the destruction of ozone layer, the mankind's healthy and living environment is caused to great harm.Therefore, the NO to the discharge of the hemi-closure space such as roads and tunnels and underground parking xthe improvement of pollutant is extremely urgent.

NO xthe conventional improvement technology of pollutant is mainly selective catalytic reduction (SCR) and absorption method.SCR method can be by the NO in dusty gas xconcentration drops to 100 ~ 200ppm, NO from 1000ppm left and right xstable removal efficiency can reach more than 80%, but the reaction temperature of SCR method is high, operating cost is large, cannot be applied to the NO of low concentration (≤200ppm) and low temperature (≤200 DEG C) xthe improvement of pollutant.And absorption method can only be served as NO xthe transition means of pollutant control, only plays enrichment of N O xeffect, do not change the existence of NO, can not be by NO xbe converted into N 2, the innoxious material such as nitrite, nitrate.Therefore, if will thoroughly solve NO xpollution problem, also need to adopt other technologies to be further processed.

Due to NO in dusty gas xbeing mainly NO(accounts for more than 90%), NO is supercritical fluid at normal temperatures, has low pole and stable physico-chemical property, is all difficult to reaction in water or in alkaline solution, therefore be difficult to be removed by conventional means.Than the stable physicochemical property of NO, NO 2be easy to and H 2o reacts and generates HNO by formula 1 3; And by equimolar NO and NO 2while passing into alkaline solution (as NaOH solution), can return middle reaction by formula 2 simultaneously, eliminate NO and NO simultaneously 2pollution.

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Formed room-temperature catalytic oxidation-solid base absorption process based on above-mentioned thinking, it is with airborne O 2for oxidant, under the effect of oxidation catalyst, by NO xnO partial oxidation in pollutant is NO 2, make NO 2account for all NO x50 ~ 60% of pollutant, then absorb with solid base absorbent, the products such as nitrite generated.Therefore, the key of room-temperature catalytic oxidation-solid base absorption process is to develop high performance NO normal temperature oxidation catalyst.

Chinese invention patent CN101279185A discloses NO in a kind of gas phase oxidation-liquid phase reduction absorbing and removing waste gas xmethod, utilize oxygen in waste gas as oxidant, by the NO of suboxides degree xwaste gas after the absorbent charcoal material catalytic oxidation of non-catalytic oxidation or aqueous slkali modification, after then fully reacting with alkaline reducing solution to remove NO xbut, the NO in waste gas xneed to pass through multi-stage oxidizing and Reducing and absorption, complex technical process, after treatment NO xremoval efficiency is the highest also only has 86.4%.

Chinese invention patent CN102527198A discloses a kind of liquid phase catalytic oxidation-alkali liquor absorption and has purified containing NO xthe method of flue gas, utilizes the NO in the acidic liquid catalysts catalytic oxidation flue gas of iron content, as NO in flue gas after oxidation 2volume fraction account for total NO x40 ~ 65% time, and then absorbed with ammonia spirit, effectively removed NO xpollution problem, but the NO of the method xremoval efficiency is up to 95%.

In above-mentioned two Chinese invention patents, exhaust-gas treatment air speed is little, NO xremoval efficiency is low, and finally all with alkaline solution to NO xpollutant carries out absorbing and removing, easily produces a large amount of waste liquids, increases processing cost.

Summary of the invention

The present invention seeks to little, the NO of exhaust-gas treatment air speed existing in order to overcome prior art xthe shortcomings such as the low and easy generation waste liquid of removal efficiency, provide a kind of low concentration of NO for the discharge of the hemi-closure space such as roads and tunnels and underground parking xroom-temperature catalytic oxidation-solid base absorption techniques that pollutant is thoroughly eliminated.

The object of the invention can be achieved through the following technical solutions: under the effect of high performance NO normal temperature oxidation catalyst, with airborne O 2for oxidant, by NO xnO partial oxidation in pollutant is NO 2, make NO 2account for all NO x50 ~ 60% of pollutant, then carry out absorbing and removing with solid base absorbent, generate the products such as nitrite.

Described high performance NO normal temperature oxidation catalyst is the catalyst of transition metal oxide loading on absorbent charcoal carrier, wherein transition metal oxide is one or more in lanthana, zirconia, iron oxide, chromium oxide, vanadium oxide, tungsten oxide, and the weight ratio of transition metal and absorbent charcoal carrier is 1 ~ 30%.

The preparation method of described high performance NO normal temperature oxidation catalyst, comprises the following steps: transition metal nitrate, ammonium vanadate or ammonium tungstate are dissolved in deionized water, constantly under stirring condition, are adding absorbent charcoal carrier, continue to stir 6 ~ 24 hours; Then successively 100 ~ 120 DEG C dry 12 ~ 24 hours, under nitrogen protection in 300 ~ 600 DEG C of roastings 4 ~ 8 hours.

Described solid base absorbent is NaOH or the potassium hydroxide loading on absorbent charcoal carrier, and wherein the percentage by weight load capacity of NaOH or potassium hydroxide is 5 ~ 30%.

Described solid base absorbent is prepared with equi-volume impregnating, comprise the following steps: NaOH or potassium hydroxide are dissolved in deionized water, constantly under stirring condition, add absorbent charcoal carrier, continuing to stir 12 ~ 24 hours, be then dried 12 ~ 24 hours at 100 ~ 120 DEG C.

Described NO room-temperature catalytic oxidation reaction condition is: NO concentration is 50 ~ 400ppm, and reaction velocity is 30000 ~ 60000h -1, reaction temperature is 0 ~ 50 DEG C.

One of remarkable advantage of the present invention is that exhaust-gas treatment air speed is large, NO xremoval efficiency can reach 100%.

Two of remarkable advantage of the present invention is the NO after to partial oxidation with activated carbon supported NaOH or potassium hydroxide solid base xpollutant carries out absorbing and removing, has avoided the generation of a large amount of waste liquids.

Brief description of the drawings

Fig. 1 is the NO of catalyst composition for NO normal temperature oxidation catalyst 2the impact of yield;

Fig. 2 is the NO of tungsten load amount for NO normal temperature oxidation catalyst 2the impact of yield;

Fig. 3 is the NO of NO concentration for NO normal temperature oxidation catalyst 2the impact of yield;

Fig. 4 is the NO of reaction velocity for NO normal temperature oxidation catalyst 2the impact of yield;

Fig. 5 is the NO of reaction temperature for NO normal temperature oxidation catalyst 2the impact of yield;

Fig. 6 is NO normal temperature autoxidation-solid base absorption process of not adding any catalyst;

Fig. 7 is 10%WO xnO room-temperature catalytic oxidation-solid base absorption process of/AC catalyst.

Detailed description of the invention

Below in conjunction with specific embodiment, the present invention is described in detail, but never limit the scope of the invention.

In following examples, the catalytic performance test condition of all NO normal temperature oxidation catalyst is: 0.1 gram of NO normal temperature oxidation catalyst is placed in to quartz fixed bed reactor, taking air as oxidant, is that 150ppm, reaction velocity are 45000h in NO concentration -1be to carry out the reaction of NO room-temperature catalytic oxidation under the reaction condition of 25 DEG C with reaction temperature, the Model 42i-LS type chemiluminescence NO-NO of Thermo Fisher Scientific company of the U.S. for nitrous oxides concentration 2-NO xanalyzer carries out on-line analysis.

Comparative example 1

0.1 gram of absorbent charcoal carrier is placed in to quartz fixed bed reactor, taking air as oxidant, is that 150ppm, reaction velocity are 45000h in NO concentration -1be to carry out the reaction of NO room-temperature catalytic oxidation under the reaction condition of 25 DEG C with reaction temperature, react the NO after 10 hours 2yield is 4.7%, NO 2the Changing Pattern of yield as shown in Figure 1.

Comparative example 2

Solid base absorbent is prepared with equi-volume impregnating: 42.9 grams of NaOH or potassium hydroxide are dissolved in 140 ml deionized water, constantly under stirring condition, adding 100 grams of absorbent charcoal carriers, continue to stir 24 hours, then be dried 24 hours, the solid base absorbent that the percentage by weight load capacity that can obtain NaOH or potassium hydroxide is 30% at 105 DEG C.

Using NO normal temperature autoxidation-solid base absorption process of not adding catalyst as blank assay, taking air as oxidant, be that 150ppm, reaction velocity are 45000h in NO concentration -1be under the reaction condition of 25 DEG C, to carry out the reaction of NO normal temperature autoxidation with reaction temperature, react the NO after 10 hours 2yield is only 0.87%, the exit gas of reactor is passed through to 1 gram of solid base absorbent simultaneously, the NO after 450 minutes solid bases absorb xelimination factor is only 46%, NO xthe Changing Pattern of concentration as shown in Figure 6.

Embodiment 1

2.8 grams of lanthanum nitrate hexahydrates are dissolved in 25 ml deionized water, constantly under stirring condition, are adding 3 grams of active carbons (AC) carrier, continue to stir 8 hours; Then be dried 24 hours at 105 DEG C successively, under nitrogen protection, in 500 DEG C of roastings 4 hours, can obtain La 2o 3/ AC catalyst (weight ratio of La and AC is 30%).

By 0.1 gram of La 2o 3/ AC catalyst is placed in quartz fixed bed reactor, taking air as oxidant, is that 150ppm, reaction velocity are 45000h in NO concentration -1be to carry out the reaction of NO room-temperature catalytic oxidation under the reaction condition of 25 DEG C with reaction temperature, react the NO after 10 hours 2yield is 33%, NO 2the Changing Pattern of yield as shown in Figure 1.

Embodiment 2

4.0 gram of five water zirconium nitrate is dissolved in 25 ml deionized water, constantly under stirring condition, adding 3 grams of active carbons (AC) carrier, continue to stir 6 hours; Then be dried 24 hours at 105 DEG C successively, under nitrogen protection, in 600 DEG C of roastings 6 hours, can obtain ZrO 2/ AC catalyst (weight ratio of Zr and AC is 30%).

ZrO 2the catalytic performance test condition of/AC catalyst is identical with embodiment 1, reacts the NO after 10 hours 2yield is 19%, NO 2the Changing Pattern of yield as shown in Figure 1.

Embodiment 3

6.5 gram of nine water ferric nitrate is dissolved in 25 ml deionized water, constantly under stirring condition, adding 3 grams of active carbons (AC) carrier, continue to stir 24 hours; Then be dried 24 hours at 105 DEG C successively, under nitrogen protection, in 500 DEG C of roastings 6 hours, can obtain FeO x/ AC catalyst (weight ratio of Fe and AC is 30%).

FeO xthe catalytic performance test condition of/AC catalyst is identical with embodiment 1, reacts the NO after 10 hours 2yield is 21%, NO 2the Changing Pattern of yield as shown in Figure 1.

Embodiment 4

2.1 grams of ammonium vanadate are dissolved in 25 ml deionized water, constantly under stirring condition, are adding 3 grams of active carbons (AC) carrier, continue to stir 24 hours; Then be dried 24 hours at 105 DEG C successively, under nitrogen protection, in 500 DEG C of roastings 6 hours, can obtain VO x/ AC catalyst (weight ratio of V and AC is 30%).

VO xthe catalytic performance test condition of/AC catalyst is identical with embodiment 1, reacts the NO after 10 hours 2yield is 35%, NO 2the Changing Pattern of yield as shown in Figure 1.

Embodiment 5

6.9 gram of nine water chromic nitrate is dissolved in 25 ml deionized water, constantly under stirring condition, adding 3 grams of active carbons (AC) carrier, continue to stir 12 hours; Then be dried 24 hours at 105 DEG C successively, under nitrogen protection, in 300 DEG C of roastings 5 hours, can obtain CrO x/ AC catalyst (weight ratio of Cr and AC is 30%).

CrO xthe catalytic performance test condition of/AC catalyst is identical with embodiment 1, reacts the NO after 10 hours 2yield is 30%, NO 2the Changing Pattern of yield as shown in Figure 1.

Embodiment 6

1.2 grams of ammonium tungstates are dissolved in 25 ml deionized water, constantly under stirring condition, are adding 3 grams of active carbons (AC) carrier, continue to stir 10 hours; Then be dried 24 hours at 105 DEG C successively, under nitrogen protection, in 450 DEG C of roastings 8 hours, can obtain WO x/ AC catalyst (weight ratio of W and AC is 30%).

WO xthe catalytic performance test condition of/AC catalyst is identical with embodiment 1, reacts the NO after 10 hours 2yield is 38%, NO 2the Changing Pattern of yield as shown in Figure 1.

Embodiment 7

The preparation process of catalyst is identical with embodiment 6, prepares the WO of different W load capacity by changing the addition of ammonium tungstate x/ AC catalyst (weight ratio of W and AC is respectively 1%, 5%, 10%, 15% and 30%).

The WO of different W load capacity xthe catalytic performance test condition of/AC catalyst is identical with embodiment 1, NO 2the Changing Pattern of yield as shown in Figure 2.

Embodiment 8

WO prepared by 0.1 gram of embodiment 7 x/aC catalyst (weight ratio of W and AC is 10%) is placed in quartz fixed bed reactor, taking air as oxidant, is 45000h at reaction velocity -1be to carry out the reaction of NO room-temperature catalytic oxidation under the reaction condition of 25 DEG C with reaction temperature, investigate different N O concentration (NO concentration is respectively 50ppm, 100ppm, 150ppm, 200ppm, 250ppm, 300ppm and 400ppm) for NO 2the impact of yield, experimental result as shown in Figure 3.

Embodiment 9

WO prepared by 0.1 gram of embodiment 7 x/aC catalyst (weight ratio of W and AC is 10%) is placed in quartz fixed bed reactor, taking air as oxidant, be that 150ppm and reaction temperature are to carry out the reaction of NO room-temperature catalytic oxidation under the reaction condition of 25 DEG C in NO concentration, (reaction velocity is respectively 30000 h to investigate differential responses air speed -1, 37500 h -1, 45000 h -1, 52500 h -1with 60000 h -1) for NO 2the impact of yield, experimental result as shown in Figure 4.

Embodiment 10

WO prepared by 0.1 gram of embodiment 7 x/aC catalyst (weight ratio of W and AC is 10%) is placed in quartz fixed bed reactor, taking air as oxidant, is that 150ppm and reaction velocity are 45000h in NO concentration -1reaction condition under carry out the reaction of NO room-temperature catalytic oxidation, investigate differential responses temperature (reaction temperature is respectively 0 DEG C, 20 DEG C, 25 DEG C, 30 DEG C, 40 DEG C and 50 DEG C) for NO 2the impact of yield, experimental result as shown in Figure 5.

Embodiment 11

WO prepared by 0.1 gram of embodiment 7 x/aC catalyst (weight ratio of W and AC is 10%) is placed in quartz fixed bed reactor, taking air as oxidant, is that 150ppm, reaction velocity are 45000h in NO concentration -1be to carry out the reaction of NO room-temperature catalytic oxidation under the reaction condition of 25 DEG C with reaction temperature, react the NO after 650 minutes 2yield is 50%, the solid base absorbent of simultaneously exit gas of reactor being prepared by 1 gram of comparative example 2, the NO in 400 minutes solid base absorption processes xelimination factor is all 100%, NO xthe Changing Pattern of concentration as shown in Figure 7.

Claims (6)

1. the low concentration of NO for the discharge of the hemi-closure space such as roads and tunnels and underground parking xroom-temperature catalytic oxidation-solid base absorption techniques that pollutant is thoroughly eliminated, is characterized in that, under the effect of high performance NO normal temperature oxidation catalyst, with airborne O 2for oxidant, by NO xnO partial oxidation in pollutant is NO 2, make NO 2account for all NO x50 ~ 60% of pollutant, then use solid base absorbent to NO xpollutant is thoroughly eliminated.
2. the low concentration of NO for the discharge of the hemi-closure space such as roads and tunnels and underground parking according to claim 1 xroom-temperature catalytic oxidation-solid base absorption techniques that pollutant is thoroughly eliminated, it is characterized in that, described high performance NO normal temperature oxidation catalyst is the catalyst of transition metal oxide loading on absorbent charcoal carrier, wherein transition metal oxide is one or more in lanthana, zirconia, iron oxide, chromium oxide, vanadium oxide, tungsten oxide, and the weight ratio of transition metal and absorbent charcoal carrier is 1～30%.
3. according to the low concentration of NO for the discharge of the hemi-closure space such as roads and tunnels and underground parking described in claim 1 and 2 xroom-temperature catalytic oxidation-solid base absorption techniques that pollutant is thoroughly eliminated, it is characterized in that, the preparation method of described high performance NO normal temperature oxidation catalyst, comprise the following steps: transition metal nitrate, ammonium vanadate or ammonium tungstate are dissolved in deionized water, constantly under stirring condition, adding absorbent charcoal carrier, continuing to stir 6 ~ 24 hours; Then successively 100 ~ 120 DEG C dry 12 ~ 24 hours, under nitrogen protection in 300 ~ 600 DEG C of roastings 4 ~ 8 hours.
4. the low concentration of NO for the discharge of the hemi-closure space such as roads and tunnels and underground parking according to claim 1 xroom-temperature catalytic oxidation-solid base absorption techniques that pollutant is thoroughly eliminated, it is characterized in that, described solid base absorbent is NaOH or the potassium hydroxide loading on absorbent charcoal carrier, and wherein the percentage by weight load capacity of NaOH or potassium hydroxide is 5 ~ 30%.
5. according to the low concentration of NO for the discharge of the hemi-closure space such as roads and tunnels and underground parking described in claim 1 and 4 xroom-temperature catalytic oxidation-solid base absorption techniques that pollutant is thoroughly eliminated, it is characterized in that, described solid base absorbent is prepared with equi-volume impregnating, comprise the following steps: NaOH or potassium hydroxide are dissolved in deionized water, constantly under stirring condition, adding absorbent charcoal carrier, continue to stir 12 ~ 24 hours, be then dried 12 ~ 24 hours at 100 ~ 120 DEG C.
6. the low concentration of NO for the discharge of the hemi-closure space such as roads and tunnels and underground parking according to claim 1 xroom-temperature catalytic oxidation-solid base absorption techniques that pollutant is thoroughly eliminated, is characterized in that, described NO room-temperature catalytic oxidation reaction condition is: NO concentration is 50 ~ 400ppm, and reaction velocity is 30000 ~ 60000h -1, reaction temperature is 0 ~ 50 DEG C.
CN201410210507.XA 2014-05-19 2014-05-19 Room temperature catalytic oxidation-solid alkali absorption method for purifying nitrogen oxide of semi-closed space CN103977680A (en)

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* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN108579368A (en) * 2018-03-13 2018-09-28 浙江工业大学 A kind of solid state chemistry absorption techniques purification nitrogen oxides

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Application publication date: 20140813