CN113231016A - Preparation process of renewable sulfur-doped mesoporous carbon adsorbent for flue gas demercuration - Google Patents
Preparation process of renewable sulfur-doped mesoporous carbon adsorbent for flue gas demercuration Download PDFInfo
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- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 title claims abstract description 57
- 239000003463 adsorbent Substances 0.000 title claims abstract description 55
- 239000003546 flue gas Substances 0.000 title claims abstract description 36
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 title claims abstract description 33
- 238000002360 preparation method Methods 0.000 title claims abstract description 23
- VMJOFTHFJMLIKL-UHFFFAOYSA-N 2-thiophen-2-ylethanol Chemical compound OCCC1=CC=CS1 VMJOFTHFJMLIKL-UHFFFAOYSA-N 0.000 claims abstract description 10
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims abstract description 9
- PRZSXZWFJHEZBJ-UHFFFAOYSA-N thymol blue Chemical compound C1=C(O)C(C(C)C)=CC(C2(C3=CC=CC=C3S(=O)(=O)O2)C=2C(=CC(O)=C(C(C)C)C=2)C)=C1C PRZSXZWFJHEZBJ-UHFFFAOYSA-N 0.000 claims abstract description 9
- 239000011259 mixed solution Substances 0.000 claims description 28
- 238000003756 stirring Methods 0.000 claims description 21
- 239000007787 solid Substances 0.000 claims description 19
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 16
- 238000000034 method Methods 0.000 claims description 14
- 229920000642 polymer Polymers 0.000 claims description 14
- 239000000843 powder Substances 0.000 claims description 13
- 238000010438 heat treatment Methods 0.000 claims description 11
- 229910052573 porcelain Inorganic materials 0.000 claims description 10
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 10
- 238000001035 drying Methods 0.000 claims description 9
- 239000000243 solution Substances 0.000 claims description 9
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- 239000007788 liquid Substances 0.000 claims description 7
- 238000001354 calcination Methods 0.000 claims description 6
- 238000005119 centrifugation Methods 0.000 claims description 5
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- 238000000227 grinding Methods 0.000 claims description 4
- 230000007935 neutral effect Effects 0.000 claims description 4
- 238000002156 mixing Methods 0.000 claims description 3
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 abstract description 14
- 229910052717 sulfur Inorganic materials 0.000 abstract description 8
- 239000011593 sulfur Substances 0.000 abstract description 8
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 abstract description 7
- 229910052799 carbon Inorganic materials 0.000 abstract description 5
- QSHDDOUJBYECFT-UHFFFAOYSA-N mercury Chemical compound [Hg] QSHDDOUJBYECFT-UHFFFAOYSA-N 0.000 description 35
- 229910052753 mercury Inorganic materials 0.000 description 34
- 230000008929 regeneration Effects 0.000 description 14
- 238000011069 regeneration method Methods 0.000 description 14
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- 238000002474 experimental method Methods 0.000 description 6
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- 238000001179 sorption measurement Methods 0.000 description 5
- 239000012298 atmosphere Substances 0.000 description 4
- 238000012986 modification Methods 0.000 description 4
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 description 3
- 238000009792 diffusion process Methods 0.000 description 3
- 230000004048 modification Effects 0.000 description 3
- 238000011160 research Methods 0.000 description 3
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 2
- 238000006243 chemical reaction Methods 0.000 description 2
- 125000004122 cyclic group Chemical group 0.000 description 2
- 239000008367 deionised water Substances 0.000 description 2
- 229910021641 deionized water Inorganic materials 0.000 description 2
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- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J20/00—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof
- B01J20/02—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material
- B01J20/20—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material comprising free carbon; comprising carbon obtained by carbonising processes
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
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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
- B01D53/02—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 by adsorption, e.g. preparative gas chromatography
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- B01J20/00—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof
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- B01J20/28054—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof characterised by their form or physical properties characterised by their surface properties or porosity
- B01J20/28069—Pore volume, e.g. total pore volume, mesopore volume, micropore volume
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- B01J20/00—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof
- B01J20/30—Processes for preparing, regenerating, or reactivating
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Abstract
The invention relates to a preparation process of a renewable sulfur-doped mesoporous carbon adsorbent for flue gas demercuration, which is characterized in that thymol blue and 2-thiopheneethanol are respectively used as a carbon source and a sulfur source, and MCM-41 is used as a template to prepare the sulfur-doped mesoporous carbon adsorbent which has excellent demercuration capacity, especially has high-quality reproducibility and SO resistance for flue gas demercuration of a coal-fired power plant, and simultaneously has high-quality reproducibility and SO resistance2Interference ability, can realize the high-efficient demercuration of coal-fired flue gas.
Description
Technical Field
The invention relates to a preparation process of a renewable sulfur-doped mesoporous carbon adsorbent for flue gas demercuration, belonging to the field of coal-fired flue gas demercuration.
Background
Mercury (Hg), colloquially known as mercury, is a highly toxic substance that can cause serious environmental pollution worldwide because it can be transported over long distances and settled over long distances through the atmosphere. The artificial emission of mercury is mainly from fuel combustion, and a thermal power station using coal as a main fuel is the largest artificial mercury emission source at present. In the coal-fired pollutants, mercury has become secondary dust and SO2And the fourth macrocontaminant after NOx.
The most mature and feasible technology suitable for coal-fired flue gas demercuration is flue adsorbent injection technology, and research aiming at the technology mainly focuses on development of a demercuration adsorbent which is cheap and efficient at present. Research shows that the demercuration efficiency of the adsorbent is easily affected by SO in flue gas2Is mainly due to SO2Will compete with Hg for the same adsorption active sites, while the sulfur-modified activated carbon adsorbent can be used at low SO concentrations2The maintenance of high mercury removal efficiency in the environment has received much attention. However, the existing commercial sulfur modified activated carbon is mainly prepared by post-modification impregnation modification, sulfur groups mainly stay in pore channels of the activated carbon to block the diffusion of mercury into the activated carbon, sulfur is easy to separate out at high temperature, the stability is poor, and the regeneration cost of the adsorbent is high.
Aiming at the current situation, the method for preparing the sulfur-doped ordered mesoporous carbon demercuration by adopting the template method has great advantages, for example, the sulfur-doped mesoporous carbon has a more regular pore channel structure, a larger specific surface area and pore volume, no sulfur group stays in the pore channel to block the diffusion of mercury, and meanwhile, the mesoporous carbon has higher graphitization degree after high-temperature calcination, and has good thermal stability and chemical stability after adsorbing pollutants such as heavy metals; the sulfur-doped mesoporous carbon is prepared by a template method, and sulfur functional groups can be doped into the mesoporous carbon at one time, so that a sulfur impregnation modification process of activated carbon is omitted. However, the related research reports of developing sulfur-doped mesoporous carbon by using a template method for the field of mercury removal of coal-fired flue gas are very limited, and based on the report, a renewable sulfur-doped mesoporous carbon preparation process needs to be researched, so that the prepared adsorbent cannot block the pore structure of the adsorbent, the stability of sulfur groups can be enhanced, the mercury removal and regeneration capacity of the adsorbent is obviously improved, and the regeneration cost of the adsorbent is reduced.
Disclosure of Invention
The invention provides a preparation process of a renewable sulfur-doped mesoporous carbon adsorbent for flue gas demercuration, and the sulfur-doped mesoporous carbon adsorbent prepared and obtained by the process has excellent demercuration capacity, high-quality reproducibility and SO resistance2Interference capability.
The technical scheme adopted by the invention for solving the technical problems is as follows:
a preparation process of a renewable sulfur-doped mesoporous carbon adsorbent for flue gas demercuration comprises the following steps:
firstly, mixing three components of MCM-41, thymol blue and 2-thiophene ethanol, uniformly stirring, and adding absolute ethyl alcohol to prepare a mixed solution A with the volume of 15 ml;
secondly, stirring the mixed solution A by using an electromagnetic stirrer at room temperature, naturally evaporating absolute ethyl alcohol in the mixed solution A to dryness in the stirring process to form a gel substance, placing the gel substance in a constant-temperature water bath kettle, and continuously evaporating the absolute ethyl alcohol to form a powder polymer;
thirdly, placing the powder polymer in a porcelain boat, and placing the porcelain boat in a horizontal tube furnace for heating and calcining;
fourthly, putting the calcined powder polymer into HF solution to obtain 100ml of mixed solution B, and stirring the mixed solution B by using an electromagnetic stirrer at room temperature;
fifthly, placing the stirred mixed solution B into a centrifugal tube, performing solid-liquid separation on the centrifugal tube through a centrifugal machine, and washing the separated wet solid until the pH value of the wet solid is neutral;
sixthly, placing the wet solid in a centrifugal tube, and then placing the centrifugal tube in an oven for drying;
grinding the dried solid to obtain a renewable sulfur-doped mesoporous carbon adsorbent for flue gas demercuration;
as further optimization of the invention, in the first step, the mass part ratio of the MCM-41, the thymol blue and the 2-thiophene ethanol is 3:1: 6;
as a further preferable aspect of the present invention, in the second step, the time for stirring the mixed solution a with the electromagnetic stirrer at room temperature is 18 to 24 hours;
the rotating speed is set to be 400 r/min;
the temperature of the constant-temperature water bath kettle is set to be 70 ℃;
as a further optimization of the invention, in the third step, the porcelain boat is placed in a horizontal tube furnace for heating and calcining, the heating rate is 3 ℃/min until the temperature in the horizontal tube furnace is increased to 900 ℃, and the temperature is kept for 2 hours;
as a further preference of the present invention, in the fourth step, the calcined powdery polymer is put into an HF solution at a concentration of 10%;
stirring the mixed solution B by using an electromagnetic stirrer for 24 hours, and setting the rotating speed of the electromagnetic stirrer to be 600 r/min;
further preferably, in the fifth step, the centrifuge rotation speed of the centrifuge for solid-liquid separation is set to 8000r/min, the centrifugation time is 5min, and the number of times of centrifugation is 5 to 6;
as a further preference of the present invention, in the sixth step, the temperature of the wet solid is set to 105 ℃ and the drying time is 12 hours while it is dried in the oven.
Through the technical scheme, compared with the prior art, the invention has the following beneficial effects:
1. according to the invention, thymol blue and 2-thiopheneethanol are used as a carbon source and a sulfur source, MCM-41 is used as a template to prepare the sulfur-doped mesoporous carbon adsorbent with a porous structure, so that the sulfur-doped mesoporous carbon adsorbent has excellent demercuration performance;
2. the demercuration product of the sulfur-doped mesoporous carbon adsorbent prepared by the invention is HgS which can be decomposed at 250-350 ℃, so that the sulfur-doped mesoporous carbon adsorbent after demercuration can be subjected to thermal regeneration treatment, the treated adsorbent can recover excellent demercuration performance to obtain regeneration, and the cyclic utilization of the adsorbent is realized;
3. the sulfur-doped mesoporous carbon prepared based on the template method has single chemical functional group on the surface, mainly takes the sulfur group as the main component, can selectively adsorb mercury, and can resist other flue gas components (SO) in the coal-fired flue gas under severe conditions2、H2O, etc.) on mercury removal, has superior SO resistance2Interference capability.
Drawings
The invention is further illustrated with reference to the following figures and examples.
FIG. 1 is a graphical representation of the results of an experiment conducted in a first instance in accordance with a preferred embodiment of the present invention;
FIG. 2 is a graphical representation of the results of an experiment conducted in a second instance in accordance with a preferred embodiment of the present invention;
FIG. 3 is a graphical representation of the results of an experiment conducted in a third scenario with a preferred embodiment of the present invention.
Detailed Description
The present invention will now be described in further detail with reference to the accompanying drawings. In the description of the present application, it is to be understood that the terms "left side", "right side", "upper part", "lower part", etc., indicate orientations or positional relationships based on those shown in the drawings, and are only for convenience of describing the present invention and simplifying the description, but do not indicate or imply that the referred device or element must have a specific orientation, be constructed in a specific orientation, and be operated, and that "first", "second", etc., do not represent an important degree of the component parts, and thus are not to be construed as limiting the present invention. The specific dimensions used in the present example are only for illustrating the technical solution and do not limit the scope of protection of the present invention.
At present, the technology for preparing sulfur-doped mesoporous carbon by adopting a template method for the field of mercury removal of coal-fired flue gas is very limited, the mercury removal efficiency of the existing sulfur-doped active carbon adsorbent is not high, the current situation of difficult regeneration is also faced, and meanwhile, sulfur simple substances and SO can also exist under the high-temperature condition2Precipitation, etc., aiming at the problemsThe application aims to provide a preparation process of a regenerable sulfur-doped mesoporous carbon adsorbent for flue gas demercuration.
Specifically, the method comprises the following specific steps:
firstly, mixing MCM-41, thymol blue and 2-thiophene ethanol in a mass part ratio of 3:1:6, uniformly stirring, and adding absolute ethyl alcohol to prepare a 15ml mixed solution A; according to the application, thymol blue and 2-thiophene ethanol are respectively used as a carbon source and a sulfur source, MCM-41 is used as a template to manufacture the sulfur-doped mesoporous carbon adsorbent with a porous structure, sulfur groups in the sulfur-doped mesoporous carbon adsorbent have extremely strong binding capacity with mercury in flue gas, and active sulfur is doped into the mesoporous carbon in a body-driving doping mode, so that no sulfur groups stay in pore channels to block the diffusion of mercury, and the sulfur-doped mesoporous carbon adsorbent has excellent demercuration performance.
And secondly, stirring the mixed solution A by using an electromagnetic stirrer at room temperature, setting the rotating speed of the stirrer to be 400r/min, setting the stirring time to be within 18-24 h, naturally evaporating absolute ethyl alcohol in the mixed solution A to dryness during the stirring process to form a gel substance, placing the gel substance in a constant-temperature water bath kettle at the temperature of 70 ℃, and continuously evaporating the absolute ethyl alcohol to form a powder polymer.
And thirdly, placing the powder polymer in a porcelain boat, placing the porcelain boat in a horizontal tubular furnace for heating and calcining at the heating rate of 3 ℃/min until the temperature in the horizontal tubular furnace is increased to 900 ℃, and keeping for 2 hours.
And fourthly, putting the calcined powder polymer into a 10% HF solution to obtain 100ml of a mixed solution B, and stirring the mixed solution B at room temperature for 24 hours by using an electromagnetic stirrer, wherein the rotating speed of the electromagnetic stirrer is set to 600 r/min.
And fifthly, placing the stirred mixed solution B into a centrifugal tube, carrying out solid-liquid separation on the centrifugal tube by a centrifugal machine, setting the centrifugal speed during separation to be 8000r/min, setting the centrifugal time to be 5min, setting the centrifugal times to be 5-6 times (wherein deionized water is used for 3 times, and absolute ethyl alcohol is used for 2-3 times), and washing the separated wet solid until the pH value of the wet solid is neutral.
Sixthly, placing the wet solid in a centrifugal tube, and then placing the centrifugal tube in an oven for drying, wherein when the wet solid is dried in the oven, the temperature is set to be 105 ℃, and the drying time is 12 hours; the dried demercuration product is HgS which can be decomposed at 250-350 ℃, so that the high-temperature thermal desorption method can be adopted to carry out thermal regeneration treatment on the sulfur-doped mesoporous carbon adsorbent after demercuration, the regenerated adsorbent can restore excellent demercuration performance, and the cyclic utilization of the adsorbent is realized.
And seventhly, grinding the dried solid to obtain the renewable sulfur-doped mesoporous carbon adsorbent for flue gas demercuration.
Next, in order to better verify the preparation process provided by the present application, a preferred embodiment is made, and the specific operation steps are as follows:
weighing 1g of MCM-41 and 0.33g of thymol blue by using an analytical balance for later use, extracting 2ml of 2-thiophene ethanol and 13ml of absolute ethanol by using a rubber head dropper, placing the extracted 2ml of 2-thiophene ethanol and 13ml of absolute ethanol into a beaker, adding the weighed medicines into the absolute ethanol, and uniformly stirring until no obvious fine particles exist to prepare a mixed solution A;
stirring the mixed solution A for 24h by using an electromagnetic stirrer, setting the rotating speed at 400r/min, basically evaporating absolute ethyl alcohol to dryness when stirring is finished to obtain a gelatinous substance, and completely evaporating the absolute ethyl alcohol from the gelatinous substance in a constant-temperature water bath kettle at 70 ℃ to obtain a powder polymer;
putting the powder polymer into a porcelain boat, then putting the porcelain boat into a horizontal tubular furnace for heating and calcining, controlling the heating rate to be 3 ℃/min, heating to 900 ℃ and keeping for 2 h;
putting the calcined powder polymer into a 10% HF solution to obtain 100ml of a mixed solution B, and stirring the mixed solution B for 24 hours at room temperature by using an electromagnetic stirrer, wherein the rotating speed is set at 600 r/min;
putting the stirred mixed solution B into a centrifuge tube, performing solid-liquid separation on the mixed solution B by using a centrifuge, and washing the obtained solid until the pH value of the solid is neutral, wherein the centrifugal speed is set to be 8000r/min, the centrifugal time is 5min, and the centrifugation times are 5-6 times (3 times of deionized water and 2-3 times of absolute ethyl alcohol washing);
putting the wet solid obtained after solid-liquid separation and a centrifuge tube into a drying oven at 105 ℃, and drying for 12 h;
and grinding the dried solid to prepare the renewable sulfur-doped mesoporous carbon adsorbent for flue gas demercuration.
The regenerative sulfur-doped mesoporous carbon adsorbent obtained by the preferred embodiment is verified to have demercuration and regeneration effects on a fixed bed mercury adsorption performance test device, and the experimental device and the setting are specifically as follows:
the mercury adsorption experimental device of the fixed bed comprises a gas distribution system (N)2、O2、SO2) The system comprises a mercury vapor generation system (a constant-temperature water bath kettle, a U-shaped high borosilicate glass tube and a mercury permeation tube), a fixed bed adsorption reaction system (Boyutong VTL1200 vertical tube furnace and a fixed bed reactor), a flue gas purification system (a sodium hydroxide solution and an ice water bath), a tail gas treatment system (an activated carbon column) and a data real-time acquisition system (a VM3000 mercury measuring instrument and a notebook computer). The total flow of the simulated flue gas is 2L/min, the flow of the mercury-carrying nitrogen is 300ml/min, and the mercury concentration at the inlet of the fixed bed laboratory is controlled to be 27.0 +/-0.5 mu g/m3The dosage of the sulfur-doped mesoporous carbon in the demercuration experiment is 200mg, and the adsorption reaction temperature is 150 ℃.
The main study item in the test is O2With SO2The influence on the demercuration of the reproducible sulfur-doped mesoporous carbon adsorbent in existence and the thermal reproducibility thereof are investigated, and the following points are obtained in summary:
in the first case, the flue gas temperature is 150 ℃ and is respectively in pure N2,N2/6%O2And N is2/10%O2A fixed bed demercuration experiment of the sulfur-doped mesoporous carbon adsorbent is carried out in the atmosphere of (1), and a mercury penetration rate curve shown in figure 1 is obtained:
by comparing the mercury penetration rate curves of the three, it can be seen that 6% of O exists in the flue gas2Or 10% O2When the penetration rate of the sulfur-doped mesoporous carbon is lower than that of the sulfur-doped mesoporous carbon10 percent, which indicates that the demercuration efficiency of the sulfur-doped mesoporous carbon can be kept above 90 percent in 150 min;
compared with pure N2Atmosphere, O2When existing, the mercury removal efficiency of the sulfur-doped mesoporous carbon is further improved mainly because of O2Can be adsorbed on the surface of the mesoporous carbon in the form of molecules or free radicals when Hg is contained0When the mercury is close to the adsorbent, the mercury is rapidly oxidized by O free radicals, and the mercury in an oxidized state is more easily combined with sulfur functional groups on the surface of the adsorbent, so that the mercury removal efficiency is improved.
In the second case, the flue gas temperature is 300 ℃ and pure N2Under the atmosphere, carrying out thermal regeneration on the sulfur-doped mesoporous carbon subjected to mercury removal, and observing the mercury removal performance of the regenerated sulfur-doped mesoporous carbon to obtain a mercury penetration rate curve shown in figure 2:
by comparing the demercuration efficiency of the sulfur-doped mesoporous carbon before and after regeneration, the sulfur-doped mesoporous carbon adsorbent still has strong demercuration capacity after thermal regeneration, and the demercuration rate after regeneration is still kept above 80%, which shows that the sulfur-doped mesoporous carbon adsorbent has good thermal regeneration performance.
In the third case, the flue gas temperature is 150 ℃ and N2/O2/SO2In the atmosphere, a demercuration experiment of the sulfur-doped mesoporous carbon adsorbent is carried out to obtain a mercury penetration rate curve shown in fig. 3:
by comparing the sulfur-doped mesoporous carbon adsorbent with different SO contents in the flue gas2The mercury penetration rate curve in concentration shows that the sulfur-doped mesoporous carbon adsorbent is applied to different SO2The mercury removal efficiency is kept high when the concentration is high, and can reach more than 85 percent, and the concentration is low and medium2Has certain promotion effect on the demercuration of the adsorbent, which shows that the sulfur-doped mesoporous carbon has good SO resistance2Interference capability.
In summary, the sulfur-doped mesoporous carbon adsorbent prepared by the preparation process of the regenerable sulfur-doped mesoporous carbon adsorbent for flue gas demercuration provided by the application has the advantages of high demercuration efficiency, good regenerability and excellent SO resistance2The interference ability improves the defects of the prior sulfur-doped active carbon that the demercuration efficiency is not high enough and the regeneration is difficult.
It will be understood by those skilled in the art that, unless otherwise defined, all terms (including technical and scientific terms) used herein have the same meaning as commonly understood by one of ordinary skill in the art to which this application belongs. It will be further understood that terms, such as those defined in commonly used dictionaries, should be interpreted as having a meaning that is consistent with their meaning in the context of the prior art and will not be interpreted in an idealized or overly formal sense unless expressly so defined herein.
The meaning of "and/or" as used herein is intended to include both the individual components or both.
The term "connected" as used herein may mean either a direct connection between components or an indirect connection between components via other components.
In light of the foregoing description of the preferred embodiment of the present invention, many modifications and variations will be apparent to those skilled in the art without departing from the spirit and scope of the invention. The technical scope of the present invention is not limited to the content of the specification, and must be determined according to the scope of the claims.
Claims (7)
1. A preparation process of a renewable sulfur-doped mesoporous carbon adsorbent for flue gas demercuration is characterized by comprising the following steps of: the method comprises the following steps:
firstly, mixing three components of MCM-41, thymol blue and 2-thiophene ethanol, uniformly stirring, and adding absolute ethyl alcohol to prepare a mixed solution A with the volume of 15 ml;
secondly, stirring the mixed solution A by using an electromagnetic stirrer at room temperature, naturally evaporating absolute ethyl alcohol in the mixed solution A to dryness in the stirring process to form a gel substance, placing the gel substance in a constant-temperature water bath kettle, and continuously evaporating the absolute ethyl alcohol to form a powder polymer;
thirdly, placing the powder polymer in a porcelain boat, and placing the porcelain boat in a horizontal tube furnace for heating and calcining;
fourthly, putting the calcined powder polymer into HF solution to obtain 100ml of mixed solution B, and stirring the mixed solution B by using an electromagnetic stirrer at room temperature;
fifthly, placing the stirred mixed solution B into a centrifugal tube, performing solid-liquid separation on the centrifugal tube through a centrifugal machine, and washing the separated wet solid until the pH value of the wet solid is neutral;
sixthly, placing the wet solid in a centrifugal tube, and then placing the centrifugal tube in an oven for drying;
and seventhly, grinding the dried solid to obtain the renewable sulfur-doped mesoporous carbon adsorbent for flue gas demercuration.
2. The preparation process of the regenerable sulfur-doped mesoporous carbon adsorbent for flue gas demercuration according to claim 1, wherein the preparation process comprises the following steps: in the first step, the mass part ratio of the MCM-41, the thymol blue and the 2-thiophene ethanol is 3:1: 6.
3. The preparation process of the regenerable sulfur-doped mesoporous carbon adsorbent for flue gas demercuration according to claim 1, wherein the preparation process comprises the following steps: in the second step, stirring the mixed solution A for 18-24 h at room temperature by using an electromagnetic stirrer;
the rotating speed is set to be 400 r/min;
the temperature of the constant temperature water bath was set to 70 ℃.
4. The preparation process of the regenerable sulfur-doped mesoporous carbon adsorbent for flue gas demercuration according to claim 1, wherein the preparation process comprises the following steps: in the third step, the porcelain boat is placed in a horizontal tube furnace for heating and calcining, the heating rate is 3 ℃/min until the temperature in the horizontal tube furnace is raised to 900 ℃, and the temperature is kept for 2 hours.
5. The preparation process of the regenerable sulfur-doped mesoporous carbon adsorbent for flue gas demercuration according to claim 1, wherein the preparation process comprises the following steps: in the fourth step, the calcined powder polymer is put into an HF solution, and the concentration of the HF solution is 10 percent;
the time for stirring the mixed solution B by using an electromagnetic stirrer is 24h, and the rotating speed of the electromagnetic stirrer is set to be 600 r/min.
6. The preparation process of the regenerable sulfur-doped mesoporous carbon adsorbent for flue gas demercuration according to claim 1, wherein the preparation process comprises the following steps: in the fifth step, the centrifugal rotation speed of the centrifuge for solid-liquid separation is set to 8000r/min, the centrifugation time is 5min, and the centrifugation times are 5-6.
7. The preparation process of the regenerable sulfur-doped mesoporous carbon adsorbent for flue gas demercuration according to claim 1, wherein the preparation process comprises the following steps: in the sixth step, the temperature of the wet solid is set to 105 ℃ and the drying time is 12h while drying in the oven.
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CN103172043A (en) * | 2011-12-20 | 2013-06-26 | 中国科学院大连化学物理研究所 | Sulfur functionalization meso pore carbon block material and preparation method |
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