CN112156630A - Denitration synergistic method for 500-DEG C and 900 DEG C - Google Patents

Denitration synergistic method for 500-DEG C and 900 DEG C Download PDF

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CN112156630A
CN112156630A CN202011081409.2A CN202011081409A CN112156630A CN 112156630 A CN112156630 A CN 112156630A CN 202011081409 A CN202011081409 A CN 202011081409A CN 112156630 A CN112156630 A CN 112156630A
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denitration
molecular sieve
reducing agent
temperature
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CN112156630B (en
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由长福
刘涵子
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Tsinghua University
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    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • 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
    • B01D53/46—Removing components of defined structure
    • B01D53/54—Nitrogen compounds
    • B01D53/56—Nitrogen oxides
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • 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
    • B01D53/80—Semi-solid phase processes, i.e. by using slurries
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2251/00—Reactants
    • B01D2251/20—Reductants
    • B01D2251/206—Ammonium compounds
    • B01D2251/2062—Ammonia
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2251/00—Reactants
    • B01D2251/20—Reductants
    • B01D2251/206—Ammonium compounds
    • B01D2251/2067—Urea
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2258/00—Sources of waste gases
    • B01D2258/02—Other waste gases
    • B01D2258/0283—Flue gases

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  • Chemical & Material Sciences (AREA)
  • Environmental & Geological Engineering (AREA)
  • Health & Medical Sciences (AREA)
  • Biomedical Technology (AREA)
  • Analytical Chemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Oil, Petroleum & Natural Gas (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Exhaust Gas Treatment By Means Of Catalyst (AREA)
  • Treating Waste Gases (AREA)

Abstract

The invention discloses a denitration synergistic method at 500-900 ℃ and relates to the technical field of pollution control. Adding a molecular sieve into the denitration reducing agent solution to uniformly disperse the molecular sieve in the denitration reducing agent solution to form mixed slurry; the mixed slurry is sprayed into flue gas at the temperature of 500-900 ℃, the denitration reducing agent reduces nitric oxide into nitrogen, and the denitration synergistic effect is realized under the action of the molecular sieve. The invention aims to provide a reduction denitration synergistic method for 500-plus-900 ℃ flue gas, which is convenient, efficient and simple in process. The molecular sieve raw material is dispersed in the denitration reducing agent solution, so that new construction or modification engineering is convenient, and the industrial realization is easy.

Description

Denitration synergistic method for 500-DEG C and 900 DEG C
Technical Field
The invention belongs to the technical field of pollution control, and particularly relates to a 500-DEG C900-DEG C denitration synergistic method.
Background
The denitration reducing agent can be used for converting nitrogen oxides in the flue gas into nitrogen under the medium-high temperature condition, so that the aim of denitration is fulfilled. When the temperature of the flue gas is about 400 ℃, a V/W/Ti catalyst can be adopted to catalyze the process of reducing nitrogen oxides by reducing agents such as ammonia or urea. When the temperature of the flue gas is 850-1100 ℃, reducing agents such as ammonia or urea can be directly adopted to reduce the nitrogen oxide, and a catalyst is not needed, so that the aim of high denitration can be fulfilled. In an actual system, due to the influence of process design, load variation and the like, the temperature of the injection point of the reducing agent is always in the range of 500-900 ℃, and a large amount of ammonia or urea needs to be injected to meet the requirements of pollution emission regulations. Therefore, research on the denitration synergy method at 500-900 ℃ needs to be carried out.
Disclosure of Invention
The invention aims to provide a reduction denitration synergistic method for 500-plus-900 ℃ flue gas, which is convenient, efficient and simple in process.
The invention is realized by the following technical scheme:
A500-DEG C and 900-DEG C denitration synergistic method is characterized by comprising the following steps:
adding the particle size d of the raw material particles into the denitration reducing agent solution50The molecular sieve with the particle size less than 5 microns is uniformly dispersed in the denitration reducing agent solution to form mixed slurry;
the mixed slurry is sprayed into flue gas at the temperature of 500-900 ℃, the denitration reducing agent reduces nitric oxide into nitrogen, and the denitration synergistic effect is realized under the action of the molecular sieve.
In the above technical scheme, the denitration reducing agent solution is ammonia or urea aqueous solution.
In the above technical scheme, the molecular sieve is an H-type molecular sieve.
In the technical scheme, the mass ratio of the molecular sieve to the effective components in the denitration reducing agent solution is less than or equal to 3: 1.
In the technical scheme, the inorganic high-temperature-resistant glue is added into the mixed slurry and uniformly dispersed in the slurry. The mass ratio of the inorganic high-temperature-resistant glue to the mixed slurry is 1: 10-1: 1000.
In the technical scheme, the inorganic high-temperature-resistant glue can resist the temperature of more than or equal to 500 ℃.
In the technical scheme, the effective component of the inorganic high-temperature-resistant glue is one or a mixture of two materials of silica sol and aluminum sol.
Compared with the prior art, the invention has the following advantages and prominent effects:
high efficiency: by adopting the specific molecular shape-selective filtration of the molecular sieve and the function of carrying an acid site per se, small molecules such as reducing agents of ammonia, nitrogen oxide and nitrogen can be separated from complex flue gas, combined and converted into an intermediate product in a temperature-resistant silicon-aluminum tetrahedral framework, and a superior selective reduction atmosphere is created; h introduced on the surface of the hydrogen type molecular sieve due to unsaturated potential of Al atom+The group can obviously relieve the conversion of the reducing agent to the nitrogen oxide and is beneficial to the conversion process to the nitrogen; the hydrogen type ZSM-5 type molecular sieve has a specific mesopore structure which can be in the same silica-alumina ratioUnder the condition, more stable acid sites are effectively loaded, and the method has more advantages in the aspects of selectivity and improvement of reduction denitration efficiency by surface groups; inorganic high temperature glue can realize that molecular sieve high strength loads on the particle surface in the flue gas, alleviates the wearing and tearing that the granule collision caused, prolongs dwell time, further promotes denitration increase effect.
② the cooperativity: molecular sieves, especially hydrogen-type molecular sieves, often employ an ammonia exchange link to enhance surface acidic site groups during the preparation process. The method mixes the molecular sieve in ammonia or urea aqueous solution to ensure that the [ AlO ] in the molecular sieve4]-H in ionic and ammonia solutions+The ions are fully combined, and the original ions can be further enriched
Figure BDA0002718497260000021
Acid site group, the purpose of denitration and efficiency improvement is realized. In addition, the existing ammonia spraying denitration reaction mainly belongs to the gas phase interaction of reducing agent ammonia and nitrogen oxide, and the mixed addition of the molecular sieve only promotes the gas-solid heterogeneous catalysis process, so that the original reaction is not negatively influenced.
Convenience: the molecular sieve raw material is dispersed in the denitration reducing agent solution through aqueous solution or particles, so that the new construction or modification is convenient, and the industrial implementation is easy.
Detailed Description
The following will further describe the specific implementation and operation of the present invention with reference to the following examples.
The invention provides a denitration synergistic method at 500-900 ℃. The method comprises the following steps:
adding the particle size d of the raw material particles into the denitration reducing agent solution50And (3) uniformly dispersing the molecular sieve with the particle size less than 5 microns in the denitration reducing agent solution to form mixed slurry. The denitration reducing agent solution is ammonia or urea aqueous solution. The molecular sieve is an H-type molecular sieve. The mass ratio of the molecular sieve to the effective components in the denitration reducing agent solution is less than or equal to 3: 1. The particle size of the raw material particles of the molecular sieve is less than 5 microns, so that the dispersibility of the particles in the reducing agent solution can be improved, and the problem of blockage of a mixed solution spraying device can be avoided.
The mixed slurry is sprayed into flue gas at the temperature of 500-900 ℃, the denitration reducing agent reduces nitric oxide into nitrogen, and the denitration synergistic effect is realized under the action of the molecular sieve.
And adding inorganic high-temperature-resistant glue into the mixed slurry, and uniformly dispersing the inorganic high-temperature-resistant glue into the slurry. The mass ratio of the inorganic high-temperature-resistant glue to the mixed slurry is 1: 10-1: 1000. The inorganic high-temperature-resistant glue can resist the temperature of more than or equal to 500 ℃. The effective component of the inorganic high-temperature-resistant glue is one or a mixture of two materials of silica sol and aluminum sol.
The principle of the invention is as follows:
by adopting the specific molecular shape-selective filtration of the molecular sieve and the function of carrying an acid site per se, small molecules such as reducing agents of ammonia, nitrogen oxide and nitrogen can be separated from complex flue gas, combined and converted into an intermediate product in a temperature-resistant silicon-aluminum tetrahedral framework, and a superior selective reduction atmosphere is created; h introduced on the surface of the hydrogen type molecular sieve due to unsaturated potential of Al atom+The group can obviously relieve the conversion of the reducing agent to the nitrogen oxide and is beneficial to the conversion process to the nitrogen; the hydrogen type ZSM-5 molecular sieve can effectively load more stable acid sites under the condition of the same silica-alumina ratio due to the specific mesoporous structure, and has more advantages in the aspects of improving the reduction denitration efficiency by selectivity and surface groups; inorganic high temperature glue can realize that molecular sieve high strength loads on the particle surface in the flue gas, alleviates the wearing and tearing that the granule collision caused, prolongs dwell time, further promotes denitration increase effect.
Molecular sieves, especially hydrogen-type molecular sieves, often employ an ammonia exchange link to enhance surface acidic site groups during the preparation process. The method mixes the molecular sieve in ammonia or urea aqueous solution to ensure that the [ AlO ] in the molecular sieve4]-H in ionic and ammonia solutions+The ions are fully combined, and the original ions can be further enriched
Figure BDA0002718497260000031
Acid site group, the purpose of denitration and efficiency improvement is realized. In addition, the existing ammonia spraying denitration reaction mainly belongs to the gas phase interaction of reducing agent ammonia and nitric oxide, and the molecular sieveThe mixed addition only promotes the gas-solid heterogeneous catalysis process, and has no negative effect on the original reaction.
The molecular sieve raw material is dispersed in the denitration reducing agent solution through aqueous solution or particles, the new construction or the modification engineering is convenient, and the industrial realization is easy.
The present invention will be further described below by way of specific examples.
Example 1:
will d50Directly adding 2-micron hydrogen type ZSM-5 molecular sieve particles into a denitration reducing agent ammonia water container, wherein the mass ratio of the molecular sieve to ammonia in the ammonia water is 1:1, and uniformly spraying the mixed solution into flue gas at 850 ℃ for 1 s. And (3) comparing the results: by adopting the method, the denitration efficiency is improved by 30 percent.
Example 2:
will d50Preparing slurry with the solid content of 10% from 2-micron hydrogen type ZSM-5 molecular sieve particles, adding the slurry into an ammonia water conveying main pipeline of a denitration reducing agent, wherein the mass ratio of the molecular sieve to ammonia in ammonia water is 1:1, and uniformly spraying the mixed solution into smoke at 850 ℃ for 1 s. And (3) comparing the results: by adopting the method, the denitration efficiency is improved by 28 percent.
Example 3:
will d50Preparing slurry with the solid content of 10% from hydrogen type ZSM-5 molecular sieve particles of 2 microns, adding silica sol high-temperature resistant glue, adding the formed slurry into an ammonia water conveying main pipeline of a denitration reducing agent, wherein the mass ratio of the molecular sieve to ammonia in ammonia water is 1:1, and the mass ratio of inorganic high-temperature resistant glue to mixed slurry is 1: 50. And uniformly spraying the mixed solution into the flue gas at 850 ℃ in a direction countercurrent to the flue gas, wherein the volume fraction of particulate matters in the flue gas is 0.1, and the retention time is 1 s. And (3) comparing the results: by adopting the method, the denitration efficiency is improved by 33 percentage points.
The above description is only a preferred embodiment of the present invention and is not intended to limit the present invention, and various modifications and changes may be made by those skilled in the art. Any modification, equivalent replacement, or improvement made within the spirit and principle of the present invention should be included in the protection scope of the present invention.

Claims (7)

1. A500-DEG C and 900-DEG C denitration synergistic method is characterized by comprising the following steps:
adding the particle size d of the raw material particles into the denitration reducing agent solution50The molecular sieve with the particle size less than 5 microns is uniformly dispersed in the denitration reducing agent solution to form mixed slurry;
the mixed slurry is sprayed into flue gas at the temperature of 500-900 ℃, the denitration reducing agent reduces nitric oxide into nitrogen, and the denitration synergistic effect is realized under the action of the molecular sieve.
2. The method as claimed in claim 1, wherein the denitration efficiency enhancement method comprises the following steps: the denitration reducing agent solution is ammonia or urea aqueous solution.
3. The method as claimed in claim 1, wherein the denitration efficiency enhancement method comprises the following steps: the molecular sieve is an H-type molecular sieve.
4. The method as claimed in claim 1, wherein the denitration efficiency enhancement method comprises the following steps: the mass ratio of the molecular sieve to the effective components in the denitration reducing agent solution is less than or equal to 3: 1.
5. The method as claimed in claim 1, wherein the denitration efficiency enhancement method comprises the following steps: and adding inorganic high-temperature-resistant glue into the mixed slurry, and uniformly dispersing the inorganic high-temperature-resistant glue into the slurry. The mass ratio of the inorganic high-temperature-resistant glue to the mixed slurry is 1: 10-1: 1000.
6. The method as claimed in claim 5, wherein the denitration efficiency enhancement method comprises the following steps: the inorganic high-temperature-resistant glue can resist the temperature of more than or equal to 500 ℃.
7. The method as claimed in claim 5, wherein the denitration efficiency enhancement method comprises the following steps: the effective component of the inorganic high-temperature-resistant glue is one or a mixture of two materials of silica sol and aluminum sol.
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Cited By (1)

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CN113440992A (en) * 2021-07-29 2021-09-28 清华大学 Composite additive for medium-high temperature denitration and preparation method and application thereof

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Publication number Priority date Publication date Assignee Title
CN113440992A (en) * 2021-07-29 2021-09-28 清华大学 Composite additive for medium-high temperature denitration and preparation method and application thereof

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