CN116059956A - EVS-10-based cerium-loaded catalytic adsorbent for flue gas mercury removal and denitration, and preparation method and application thereof - Google Patents
EVS-10-based cerium-loaded catalytic adsorbent for flue gas mercury removal and denitration, and preparation method and application thereof Download PDFInfo
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- 239000003463 adsorbent Substances 0.000 title claims abstract description 54
- QSHDDOUJBYECFT-UHFFFAOYSA-N mercury Chemical compound [Hg] QSHDDOUJBYECFT-UHFFFAOYSA-N 0.000 title claims abstract description 52
- 230000003197 catalytic effect Effects 0.000 title claims abstract description 45
- 229910052753 mercury Inorganic materials 0.000 title claims abstract description 40
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 title claims abstract description 29
- 239000003546 flue gas Substances 0.000 title claims abstract description 29
- 229910052684 Cerium Inorganic materials 0.000 title claims abstract description 26
- GWXLDORMOJMVQZ-UHFFFAOYSA-N cerium Chemical compound [Ce] GWXLDORMOJMVQZ-UHFFFAOYSA-N 0.000 title claims abstract description 25
- 238000002360 preparation method Methods 0.000 title abstract description 10
- 239000002808 molecular sieve Substances 0.000 claims abstract description 49
- URGAHOPLAPQHLN-UHFFFAOYSA-N sodium aluminosilicate Chemical compound [Na+].[Al+3].[O-][Si]([O-])=O.[O-][Si]([O-])=O URGAHOPLAPQHLN-UHFFFAOYSA-N 0.000 claims abstract description 49
- 238000000034 method Methods 0.000 claims description 24
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 20
- 239000000203 mixture Substances 0.000 claims description 17
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 17
- 239000002994 raw material Substances 0.000 claims description 15
- 238000009210 therapy by ultrasound Methods 0.000 claims description 14
- 239000000084 colloidal system Substances 0.000 claims description 11
- 239000002243 precursor Substances 0.000 claims description 11
- VHUUQVKOLVNVRT-UHFFFAOYSA-N Ammonium hydroxide Chemical compound [NH4+].[OH-] VHUUQVKOLVNVRT-UHFFFAOYSA-N 0.000 claims description 10
- 229920002845 Poly(methacrylic acid) Polymers 0.000 claims description 10
- 239000012670 alkaline solution Substances 0.000 claims description 10
- QGZKDVFQNNGYKY-UHFFFAOYSA-N ammonia Natural products N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 claims description 9
- HSJPMRKMPBAUAU-UHFFFAOYSA-N cerium(3+);trinitrate Chemical compound [Ce+3].[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O HSJPMRKMPBAUAU-UHFFFAOYSA-N 0.000 claims description 6
- 238000001816 cooling Methods 0.000 claims description 6
- 238000002156 mixing Methods 0.000 claims description 6
- 238000007873 sieving Methods 0.000 claims description 6
- 229920002125 Sokalan® Polymers 0.000 claims description 4
- 229920000141 poly(maleic anhydride) Polymers 0.000 claims description 4
- 239000004584 polyacrylic acid Substances 0.000 claims description 4
- 150000000703 Cerium Chemical class 0.000 claims description 3
- VYLVYHXQOHJDJL-UHFFFAOYSA-K cerium trichloride Chemical compound Cl[Ce](Cl)Cl VYLVYHXQOHJDJL-UHFFFAOYSA-K 0.000 claims description 3
- VGBWDOLBWVJTRZ-UHFFFAOYSA-K cerium(3+);triacetate Chemical compound [Ce+3].CC([O-])=O.CC([O-])=O.CC([O-])=O VGBWDOLBWVJTRZ-UHFFFAOYSA-K 0.000 claims description 3
- 238000001354 calcination Methods 0.000 claims description 2
- MWUXSHHQAYIFBG-UHFFFAOYSA-N nitrogen oxide Inorganic materials O=[N] MWUXSHHQAYIFBG-UHFFFAOYSA-N 0.000 abstract description 53
- 239000003054 catalyst Substances 0.000 abstract description 22
- 230000000694 effects Effects 0.000 abstract description 5
- 239000006185 dispersion Substances 0.000 abstract description 3
- 238000009776 industrial production Methods 0.000 abstract description 3
- 238000009434 installation Methods 0.000 abstract description 3
- 239000004973 liquid crystal related substance Substances 0.000 abstract 2
- 230000000052 comparative effect Effects 0.000 description 10
- 239000002245 particle Substances 0.000 description 9
- 235000011114 ammonium hydroxide Nutrition 0.000 description 8
- 239000000428 dust Substances 0.000 description 8
- 239000008367 deionised water Substances 0.000 description 7
- 229910021641 deionized water Inorganic materials 0.000 description 7
- 239000000243 solution Substances 0.000 description 7
- 238000012360 testing method Methods 0.000 description 5
- 238000006477 desulfuration reaction Methods 0.000 description 4
- 230000023556 desulfurization Effects 0.000 description 4
- 230000003647 oxidation Effects 0.000 description 4
- 238000007254 oxidation reaction Methods 0.000 description 4
- 230000008569 process Effects 0.000 description 4
- 230000002195 synergetic effect Effects 0.000 description 4
- FOIXSVOLVBLSDH-UHFFFAOYSA-N Silver ion Chemical compound [Ag+] FOIXSVOLVBLSDH-UHFFFAOYSA-N 0.000 description 3
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 description 3
- 239000003344 environmental pollutant Substances 0.000 description 3
- 150000002500 ions Chemical class 0.000 description 3
- 239000000463 material Substances 0.000 description 3
- 231100000572 poisoning Toxicity 0.000 description 3
- 230000000607 poisoning effect Effects 0.000 description 3
- 231100000719 pollutant Toxicity 0.000 description 3
- 238000000527 sonication Methods 0.000 description 3
- 229910052717 sulfur Inorganic materials 0.000 description 3
- 239000011593 sulfur Substances 0.000 description 3
- FAPWRFPIFSIZLT-UHFFFAOYSA-M Sodium chloride Chemical compound [Na+].[Cl-] FAPWRFPIFSIZLT-UHFFFAOYSA-M 0.000 description 2
- -1 V 2 O 5 Chemical class 0.000 description 2
- 238000006243 chemical reaction Methods 0.000 description 2
- 238000001035 drying Methods 0.000 description 2
- 238000005516 engineering process Methods 0.000 description 2
- 238000001704 evaporation Methods 0.000 description 2
- 239000000383 hazardous chemical Substances 0.000 description 2
- 230000036541 health Effects 0.000 description 2
- 238000011068 loading method Methods 0.000 description 2
- 230000004048 modification Effects 0.000 description 2
- 238000012986 modification Methods 0.000 description 2
- 229920000642 polymer Polymers 0.000 description 2
- 238000004064 recycling Methods 0.000 description 2
- 239000000779 smoke Substances 0.000 description 2
- 239000002594 sorbent Substances 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- 229910052720 vanadium Inorganic materials 0.000 description 2
- LEONUFNNVUYDNQ-UHFFFAOYSA-N vanadium atom Chemical compound [V] LEONUFNNVUYDNQ-UHFFFAOYSA-N 0.000 description 2
- ISIHFYYBOXJLTM-UHFFFAOYSA-N vanadium;pentasilicate Chemical compound [V].[V].[V].[V].[O-][Si]([O-])([O-])[O-].[O-][Si]([O-])([O-])[O-].[O-][Si]([O-])([O-])[O-].[O-][Si]([O-])([O-])[O-].[O-][Si]([O-])([O-])[O-] ISIHFYYBOXJLTM-UHFFFAOYSA-N 0.000 description 2
- 239000012855 volatile organic compound Substances 0.000 description 2
- 101710134784 Agnoprotein Proteins 0.000 description 1
- 229910018072 Al 2 O 3 Inorganic materials 0.000 description 1
- 229910016978 MnOx Inorganic materials 0.000 description 1
- 229910004298 SiO 2 Inorganic materials 0.000 description 1
- 239000004115 Sodium Silicate Substances 0.000 description 1
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 description 1
- 229910010413 TiO 2 Inorganic materials 0.000 description 1
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 description 1
- OBNDGIHQAIXEAO-UHFFFAOYSA-N [O].[Si] Chemical compound [O].[Si] OBNDGIHQAIXEAO-UHFFFAOYSA-N 0.000 description 1
- 238000003916 acid precipitation Methods 0.000 description 1
- 238000005054 agglomeration Methods 0.000 description 1
- 230000002776 aggregation Effects 0.000 description 1
- 230000032683 aging Effects 0.000 description 1
- 239000000809 air pollutant Substances 0.000 description 1
- 231100001243 air pollutant Toxicity 0.000 description 1
- 238000003915 air pollution Methods 0.000 description 1
- 229910021529 ammonia Inorganic materials 0.000 description 1
- 239000012298 atmosphere Substances 0.000 description 1
- 230000002238 attenuated effect Effects 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 229910002091 carbon monoxide Inorganic materials 0.000 description 1
- 239000003575 carbonaceous material Substances 0.000 description 1
- 239000000969 carrier Substances 0.000 description 1
- 238000010531 catalytic reduction reaction Methods 0.000 description 1
- 239000003245 coal Substances 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 238000003912 environmental pollution Methods 0.000 description 1
- 239000004744 fabric Substances 0.000 description 1
- 238000010304 firing Methods 0.000 description 1
- 238000011010 flushing procedure Methods 0.000 description 1
- 239000010881 fly ash Substances 0.000 description 1
- 239000007789 gas Substances 0.000 description 1
- 229910001385 heavy metal Inorganic materials 0.000 description 1
- 238000001027 hydrothermal synthesis Methods 0.000 description 1
- 238000011835 investigation Methods 0.000 description 1
- 229910000474 mercury oxide Inorganic materials 0.000 description 1
- 229910044991 metal oxide Inorganic materials 0.000 description 1
- 150000004706 metal oxides Chemical class 0.000 description 1
- 239000012299 nitrogen atmosphere Substances 0.000 description 1
- 229910052760 oxygen Inorganic materials 0.000 description 1
- 125000004430 oxygen atom Chemical group O* 0.000 description 1
- 239000013618 particulate matter Substances 0.000 description 1
- 238000011056 performance test Methods 0.000 description 1
- 239000000376 reactant Substances 0.000 description 1
- 238000011160 research Methods 0.000 description 1
- 239000011780 sodium chloride Substances 0.000 description 1
- NTHWMYGWWRZVTN-UHFFFAOYSA-N sodium silicate Chemical compound [Na+].[Na+].[O-][Si]([O-])=O NTHWMYGWWRZVTN-UHFFFAOYSA-N 0.000 description 1
- 229910052911 sodium silicate Inorganic materials 0.000 description 1
- 238000003756 stirring Methods 0.000 description 1
- 238000001308 synthesis method Methods 0.000 description 1
- 239000010936 titanium Substances 0.000 description 1
- 229910052719 titanium Inorganic materials 0.000 description 1
- 231100000331 toxic Toxicity 0.000 description 1
- 230000002588 toxic effect Effects 0.000 description 1
- 238000012546 transfer Methods 0.000 description 1
- IBYSTTGVDIFUAY-UHFFFAOYSA-N vanadium monoxide Chemical compound [V]=O IBYSTTGVDIFUAY-UHFFFAOYSA-N 0.000 description 1
- 238000005406 washing Methods 0.000 description 1
- 238000004846 x-ray emission Methods 0.000 description 1
Classifications
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- 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
- B01J20/10—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material comprising silica or silicate
-
- 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
- B01D53/02—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
-
- 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
- B01D53/86—Catalytic processes
- B01D53/8621—Removing nitrogen compounds
- B01D53/8625—Nitrogen oxides
- B01D53/8628—Processes characterised by a specific catalyst
-
- 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
- B01D53/86—Catalytic processes
- B01D53/8665—Removing heavy metals or compounds thereof, e.g. mercury
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- 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
- B01J20/06—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material comprising oxides or hydroxides of metals not provided for in group B01J20/04
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J29/00—Catalysts comprising molecular sieves
- B01J29/04—Catalysts comprising molecular sieves having base-exchange properties, e.g. crystalline zeolites
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2257/00—Components to be removed
- B01D2257/60—Heavy metals or heavy metal compounds
- B01D2257/602—Mercury or mercury compounds
-
- 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
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J2229/00—Aspects of molecular sieve catalysts not covered by B01J29/00
- B01J2229/10—After treatment, characterised by the effect to be obtained
- B01J2229/18—After treatment, characterised by the effect to be obtained to introduce other elements into or onto the molecular sieve itself
- B01J2229/186—After treatment, characterised by the effect to be obtained to introduce other elements into or onto the molecular sieve itself not in framework positions
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02A—TECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE
- Y02A50/00—TECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE in human health protection, e.g. against extreme weather
- Y02A50/20—Air quality improvement or preservation, e.g. vehicle emission control or emission reduction by using catalytic converters
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- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Analytical Chemistry (AREA)
- Environmental & Geological Engineering (AREA)
- Organic Chemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Oil, Petroleum & Natural Gas (AREA)
- Inorganic Chemistry (AREA)
- Health & Medical Sciences (AREA)
- Biomedical Technology (AREA)
- Crystallography & Structural Chemistry (AREA)
- Materials Engineering (AREA)
- Catalysts (AREA)
- Exhaust Gas Treatment By Means Of Catalyst (AREA)
- Solid-Sorbent Or Filter-Aiding Compositions (AREA)
Abstract
The present disclosure relates to an EVS-10-based cerium-loaded catalytic adsorbent for flue gas mercury removal and denitration, and a preparation method and an application thereof. The catalytic adsorbent comprises a carrier and an active component loaded on the carrier; wherein, the liquid crystal display device comprises a liquid crystal display device,the carrier comprises EVS-10 molecular sieve, and the active component comprises CeO 2 . The present disclosure successfully loads CeO-containing molecular sieves on EVS-10 2 Is carried by CeO of the catalyst adsorbent 2 The dispersion degree is high, the mercury removal efficiency and the denitration efficiency are excellent, the application effect is good in the aspect of cooperatively removing the elemental mercury and the nitrogen oxides in the coal-fired flue gas, and the equipment installation and the use cost are reduced; the catalyst adsorbent is relatively simple to synthesize, can be recycled, greatly reduces the comprehensive cost, and is suitable for industrial production.
Description
Technical Field
The invention relates to the technical field of environmental protection and air pollution control, in particular to an EVS-10-based cerium-loaded catalytic adsorbent for flue gas mercury removal and denitration, and a preparation method and application thereof.
Background
The flue gas discharged by the coal-fired power plant contains mercury, the mercury is a toxic heavy metal, serious harm is caused to human health and ecological environment, and the coal-fired power plant is considered as the largest global artificial mercury discharge source and also considered as one of the most important artificial mercury discharge sources. The mercury contained in the flue gas of the coal-fired power plant mainly comprises Hg 2+ 、Hg p And Hg of 0 Three forms. Wherein Hg is 2+ Is dissolved in water, so that the pollutant can be efficiently removed by adopting a wet desulphurization device of pollutant control equipment; hg in flue gas p The dust can be easily combined with fly ash, so that the dust can be removed by particulate matter control equipment, such as a cloth bag dust remover or an electrostatic dust remover; and Hg is 0 The water-insoluble and volatile organic compound is relatively strong, and is quite stable at low temperature, and is difficult to remove by the existing pollutant control equipment, so that the water-insoluble and volatile organic compound is directly discharged into the atmosphere in the flue gas discharge process to cause environmental pollution and harm to human health. Therefore, the key to removing mercury from flue gas of coal-fired power plants is to control Hg 0 Is arranged in the air.
The two main research directions of mercury removal at present are mercury removal by an adsorbent method and mercury removal by a catalytic oxidation method respectively. The mercury removal by the adsorbent method is to remove Hg 0 Is physically or chemically adsorbed on the surface of the adsorbent and then removed by the particle control equipment; catalyst catalysisThe Hg is removed by oxidation 0 High-efficiency oxidation to Hg 2+ And then is removed by a wet desulphurization device. The EVS-10 molecular sieve is a molecular sieve which is formed by completely replacing titanium in the titanosilicate molecular sieve ETS-10 and mainly comprises vanadium-oxygen octahedra and silicon-oxygen tetrahedra, and is linked through common angle oxygen atoms, and finally a three-dimensional network structure is formed, and the molecular sieve is similar to an industrial vanadium-carrying catalyst, and can catalyze and oxidize elemental mercury. However, experimental test results show that the material has low mercury catalytic oxidation efficiency of about 48%.
In addition to elemental mercury, nitrogen oxides are also a common air pollutant from coal burning, which can cause acid rain and the greenhouse effect. Nitrogen Oxides (NO) x ) The NO ratio in the catalyst is higher and more than 95 percent. Therefore, the efficient removal of NO is a key to the realization of removal of nitrogen oxides. The most effective and widely used technology for removing NO in coal-fired flue gas at present is NH 3 Selective Catalytic Reduction (SCR) technology. SCR catalysts currently under investigation are mainly based on metal oxides such as V 2 O 5 、CuO、Cr 2 O 3 、CeO 2 、Fe 2 O 3 、MnOx、Co 2 O 3 Equal load on Al 2 O 3 、SiO 2 、TiO 2 、ZrO 2 And the carbon material, molecular sieve and other carriers. However, the existing EVS-10 molecular sieve has certain mercury removal capability, but has poor catalytic denitration performance, and only has 14 percent of removal efficiency, so that the effects of high-efficiency mercury removal and denitration cannot be achieved at the same time; and the particles are easy to agglomerate into larger particles in the repeated recycling process, which is not beneficial to the repeated recycling of the molecular sieve.
Disclosure of Invention
The invention aims to provide an EVS-10-based cerium-loaded catalytic adsorbent for flue gas mercury removal and denitration, a preparation method and application thereof, and the catalytic adsorbent can realize the synergistic removal of mercury and nitrogen oxides.
In order to achieve the above object, a first aspect of the present disclosure provides an EVS-10-based cerium-supported catalytic adsorbent for flue gas mercury removal and denitration, the catalytic adsorbent comprising a support and an active component supported on the support; wherein the carrier comprises EVS-10 molecular sieve, and the active groupIncludes CeO 2 。
Optionally, the mass fraction of the carrier is 85-99 wt% and the mass fraction of the active component is 1-15 wt% based on the total weight of the catalytic adsorbent.
A second aspect of the present disclosure provides a method of preparing the catalytic adsorbent for mercury removal and denitration according to the first aspect of the present disclosure, comprising the steps of: (1) Mixing an EVS-10 molecular sieve, a cerium source and water to obtain a raw material mixture; (2) adding an alkaline solution to the raw material mixture; then adding alcohol to obtain a colloid precursor; (3) calcining the colloid precursor.
Optionally, in the step (1), the weight ratio of the EVS-10 molecular sieve to the cerium source to the water is (90-95): (13-18);
optionally, the cerium source is a soluble cerium salt, preferably one or more selected from cerium acetate, cerium chloride and cerium nitrate.
Optionally, step (1) further comprises: carrying out ultrasonic treatment on the EVS-10 molecular sieve in water for 5-30 minutes, and then adding the cerium source and an optional dispersing auxiliary for mixing to obtain the raw material mixture; preferably, the dispersing aid is selected from one or more of polymethacrylic acid, polyacrylic acid and hydrolyzed polymaleic anhydride, and more preferably polymethacrylic acid.
Optionally, the weight ratio of the dispersing aid to the cerium source is (34-68): (13-18).
Optionally, in step (2), the alkaline solution comprises aqueous ammonia; the alcohol comprises ethanol; further preferably, the addition volume ratio (4 to 8) of the aqueous ammonia to the alcohol is: (60-70).
Optionally, step (2) further comprises:
adding the alkaline solution into the raw material mixture obtained in the step (1), and performing ultrasonic treatment for 5-30 minutes; and
before the roasting treatment, the colloid precursor is subjected to ultrasonic treatment for 5-30 minutes, and then is evaporated at 70-100 ℃.
Optionally, in step (3), the conditions of the baking treatment include: the roasting temperature is 350-600 ℃ and the roasting time is 1-4 hours;
optionally, step (3) further comprises: and cooling the roasting treatment product, sieving, and taking the undersize product to obtain the catalytic adsorbent.
A third aspect of the disclosure provides an application of the catalytic adsorbent for mercury removal and denitration in the field of mercury removal and denitration in flue gas of coal-fired power plants.
Through the technical scheme, the disclosure provides the EVS-10-based cerium-loaded catalytic adsorbent for flue gas mercury removal and denitration, and the preparation method and application thereof, wherein the EVS-10 molecular sieve is loaded with the high-dispersity CeO-containing catalyst 2 The active components of the catalyst adsorbent have good mercury removal efficiency and higher denitration efficiency, and have good application effects in the aspect of cooperatively removing elemental mercury and nitrogen oxides in the coal-fired flue gas; the catalytic adsorbent is relatively simple to synthesize and can be recycled, so that the comprehensive cost is greatly reduced, and the catalytic adsorbent is suitable for industrial production; the sulfur poisoning resistance of the catalyst adsorbent is improved, the process adaptability and compatibility are good, the catalyst adsorbent is suitable for being used in series with dust removal and desulfurization equipment, is particularly suitable for upgrading and reconstruction of mercury removal by expanding enterprises with the desulfurization and dust removal equipment, reduces equipment installation and use cost, and has industrial application prospect.
Additional features and advantages of the present disclosure will be set forth in the detailed description which follows.
Detailed Description
The following describes specific embodiments of the present disclosure in detail. It should be understood that the detailed description and specific examples, while indicating and illustrating the disclosure, are not intended to limit the disclosure.
The inventors of the present disclosure found in the study that loading an EVS-10 molecular sieve with a catalyst comprising CeO 2 The active component of the catalyst not only can greatly improve the mercury removal efficiency of the EVS-10 molecular sieve (about 48 percent to 97 percent), but also can load CeO 2 The molecular sieve of the catalyst has better performance of removing nitrogen oxides (about 86 percent); the inventors further carried CeO 2 Active component molecular sieve in SO 2 Long-time test is carried out in complex smoke environment, the performance is not obviously attenuated, and the CeO loading is indicated 2 The sulfur poisoning resistance and the service life of the active component molecular sieve are improved.
The first aspect of the present disclosure provides an EVS-10-based cerium-loaded catalytic adsorbent for flue gas mercury removal and denitration, the catalytic adsorbent comprising a carrier and an active component loaded on the carrier; wherein the carrier comprises an EVS-10 molecular sieve, and the active component comprises CeO 2 。
The present disclosure supports CeO-containing high dispersity on EVS-10 molecular sieves 2 The active components of the catalyst adsorbent have good mercury removal efficiency and higher denitration efficiency, and have good application effects in the aspect of cooperatively removing elemental mercury and nitrogen oxides in the coal-fired flue gas; the catalytic adsorbent is relatively simple to synthesize and can be recycled, so that the comprehensive cost is greatly reduced, and the catalytic adsorbent is suitable for industrial production; the sulfur poisoning resistance of the catalyst adsorbent is improved, the process adaptability and compatibility are good, the catalyst adsorbent is suitable for being used in series with dust removal and desulfurization equipment, is particularly suitable for upgrading and reconstruction of mercury removal by expanding enterprises with the desulfurization and dust removal equipment, reduces equipment installation and use cost, and has industrial application prospect.
In the present disclosure, the EVS-10 molecular sieve has high hydrothermal stability, large specific surface area and fast heat and mass transfer, and is an excellent catalyst and carrier. The present disclosure provides for the use of CeO 2 The catalyst is loaded on an EVS-10 molecular sieve to obtain a catalytic adsorbent, wherein the molecular sieve framework contains vanadium, and part of elemental mercury can be catalytically oxidized; and CeO 2 Has good denitration performance, can catalyze and oxidize elemental mercury, vanadium in a framework and loaded CeO 2 Can realize the synergistic mercury removal and denitration.
In one embodiment, the mass fraction of the support is 85 to 99 wt% and the mass fraction of the active component is 1 to 15 wt%, based on the total weight of the catalytic adsorbent. When the content of each component in the catalytic adsorbent is within the range of the embodiment, the catalytic adsorbent can achieve a better synergistic effect of removing elemental mercury and nitrogen oxides.
In one embodiment, the support is an EVS-10 molecular sieve; in terms of element mole, si in the EVS-10 molecular sieve: na: k: the molar ratio of V is 3.92:1.39:0.48:1. specifically, XRF spectroscopy can be used to determine the chemical composition of the EVS-10 molecular sieve.
A second aspect of the present disclosure provides a method of preparing the catalytic adsorbent for mercury removal and denitration according to the first aspect of the present disclosure, comprising the steps of:
(1) Mixing an EVS-10 molecular sieve, a cerium source and water to obtain a raw material mixture;
(2) Adding an alkaline solution into the raw material mixture, and then adding alcohol to obtain a colloid precursor;
(3) And roasting the colloid precursor.
The synthesis method provided by the disclosure is stable and reliable, the comprehensive use cost of the catalytic adsorbent is low, and the method has good industrial application prospect.
Specifically, the addition amount of the raw materials or the weight ratio between different raw materials, such as the addition amount or the weight ratio of the EVS-10 molecular sieve and the cerium source, in the present disclosure is adjusted to obtain the mass fraction of each component in the catalytic adsorbent provided according to the first aspect of the present disclosure. The EVS-10 molecular sieves can be prepared according to existing methods, for example, as disclosed in the literature Zijian Zhou, tintian Cao, et al, "Vanadium silicate (EVS) -supported silver nanoparticles: A novel catalytic sorbent for elemental mercury removal from flue gas". Journal of Hazardous Materials,375 (2019) 1-8.
The EVS-10 molecular sieve adopted in the disclosure can be prepared by a hydrothermal method, and in a specific embodiment, the method comprises the following steps: dissolving sodium silicate in deionized water; naOH, KCl, naF and NaCl were then added to the solution to give solution A. Then VOSO is carried out 4 Dissolving in deionized water to obtain solution B. Solution a and solution B were mixed and stirred and aged at room temperature. The aged mixture was transferred to an autoclave for continued aging. And washing the synthesized product with deionized water and drying to obtain the EVS-10 molecular sieve. The amount of each reactant and the reaction in the preparation processThe conditions can be adjusted according to actual requirements.
In one embodiment, in the step (1), the weight ratio of the EVS-10 molecular sieve, the cerium source and the water is (90-95): (13-18); optionally, the cerium source is a soluble cerium salt, preferably one or more of cerium acetate, cerium chloride and cerium nitrate.
In a preferred embodiment, step (1) further comprises: carrying out ultrasonic treatment on the EVS-10 molecular sieve in water for 5-30 minutes, and then adding the cerium source and an optional dispersing auxiliary for mixing to obtain the raw material mixture; preferably, the weight ratio of the dispersing aid to the cerium source is (34 to 68): (13-18).
In a preferred embodiment, the dispersing aid is selected from one or more of polymethacrylic acid, polyacrylic acid and hydrolyzed polymaleic anhydride, and more preferably polymethacrylic acid. The inventors of the present disclosure have found in the study that, when cerium is introduced into an EVS-10 molecular sieve, one or more of polymethacrylic acid, polyacrylic acid and hydrolyzed polymaleic anhydride are added to the raw material mixture, the dispersity of cerium ions can be improved and the mercury removal and denitration performance of the finally prepared catalyst adsorbent can be further improved.
The present disclosure employs a dispersing aid to form a complex with Ce ions in solution, such that Ce ions are uniformly dispersed in the system in the form of a complex. When alkaline solution (such as ammonia water) is added subsequently, the Ce (OH) can be evenly dispersed 4 The complex further avoids agglomeration; after the alcohol is added, the complex in the system forms dispersion auxiliary agent-Ce polymer particles (such as PMAA-Ce polymer particles) on the surface of the EVS-10 molecular sieve, electrostatic repulsion among the particles ensures stable system, ensures the dispersity of Ce ions in the preparation system, and further ensures CeO loaded in the finally synthesized catalytic adsorbent 2 Is smaller and uniformly distributed.
In one embodiment, in step (2), the alkaline solution comprises aqueous ammonia; the alcohol comprises ethanol; further preferably, the addition volume ratio (4 to 8) of the aqueous ammonia to the alcohol is: (60-70).
In one embodiment, step (2) further comprises: adding the alkaline solution into the raw material mixture obtained in the step (1), and performing ultrasonic treatment for 5-30 minutes; and
before the roasting treatment, the colloid precursor is subjected to ultrasonic treatment for 5-30 minutes and then evaporated at 70-100 ℃. Sonication in the present disclosure means sonication using conventional ultrasonic equipment to more uniformly mix or disperse materials.
In one embodiment, in step (3), the conditions of the firing treatment include: the roasting temperature is 350-600 ℃ and the roasting time is 1-4 hours;
optionally, step (3) further comprises: and cooling the roasting treatment product, sieving, and taking the undersize product to obtain the catalytic adsorbent. For example, after cooling to room temperature, sieving with a 100 mesh sieve, and taking the undersize as the final catalytic adsorbent.
A third aspect of the disclosure provides an application of the catalytic adsorbent according to the first aspect of the disclosure in the field of flue gas mercury removal and denitration; optionally, the flue gas is flue gas of a coal-fired power plant.
The invention is further illustrated below in connection with specific embodiments, but the scope of the invention as claimed is not limited to the examples described.
The chemicals used in each example were commercially available from public sources.
The EVS-10 molecular sieves used in the examples and comparative examples below were prepared according to the methods disclosed in the documents Zijian Zhou, tintian Cao, et al, "Vanadium silicate (EVS) -supported silver nanoparticles: A novel catalytic sorbent for elemental mercury removal from flue gas". Journal of Hazardous Materials,375 (2019) 1-8.
The 25% aqueous ammonia used in the following examples, comparative examples and comparative examples was NH 3 ·H 2 Ammonia with an O content of 25 wt%.
The ultrasonic treatment uses conventional ultrasonic equipment to more uniformly mix or disperse the materials.
Example 1
(1) 9.0g EVS was preparedThe-10 molecular sieves were dispersed in 50mL deionized water and after 15 minutes of sonication 1.8g (CH) were added 3 CO 2 ) 3 Ce hydrate and 6.8g polymethacrylic acid;
(2) Adding 8mL of 25% ammonia water, performing ultrasonic treatment for 15 min, adding 70mL of ethanol to form a colloid precursor, performing ultrasonic treatment for 30 min, evaporating the sample at 80 ℃, finally roasting the sample in a muffle furnace at 500 ℃ for 2 h, cooling to room temperature, sieving with a 100-mesh sieve, and removing particles to obtain the loaded CeO 2 Is designated as sample 1.
Comparative example 1
A catalytic adsorbent was prepared by a procedure similar to example 1, except that in example 1: the EVS-10 molecular sieve was replaced with a commercially available ETS-10 molecular sieve. Other preparation procedures were the same as in example 1 to obtain CeO-supported particles 2 Is designated as sample D-1.
Example 2
(1) 9.5g of EVS-10 molecular sieve was dispersed in 60mL of deionized water, sonicated for 15 minutes, and 1.3g of Ce (NO) was added 3 ) 3 ·6H 2 O and 3.4g of polymethacrylic acid;
(2) Adding 4mL of 25% ammonia water, performing ultrasonic treatment for 15 min, adding 60mL of ethanol to form a colloid precursor, performing ultrasonic treatment for 30 min, evaporating the sample at 80 ℃, finally roasting the sample in a muffle furnace at 600 ℃ for 2 h, cooling to room temperature, sieving with a 100-mesh sieve, and removing particles to obtain the loaded CeO 2 Is designated as sample 2.
Example 3
A catalytic adsorbent was prepared by a procedure similar to example 1, except that in example 1: in the step (1), the polymethacrylic acid dispersing aid was not added, and the other preparation process and reaction conditions were the same as in example 1. Obtaining the loaded CeO 2 Is designated as sample 3.
Comparative example 2
Weigh 4.3g AgNO 3 Dissolving in 100ml deionized water, adding 10g EVS-10 molecular sieve, magnetically stirring in dark environment for 6 hr, andfiltering, repeatedly flushing with deionized water, drying at 80 ℃, and roasting in a tube furnace at 250 ℃ under nitrogen atmosphere for 1 hour. The catalyst adsorbent carrying only silver nanoparticles was obtained and was designated as sample D-2.
The samples obtained in the above examples and comparative examples were subjected to carrier molecular sieves, ceO 2 The mass fractions of (2) are listed in Table 1.
TABLE 1
Simulated smoke test case
The samples synthesized in the examples and the comparative examples are placed on an experimental system for simulating flue gas to perform mercury removal and denitration performance test. The simulated flue gas conditions were as follows: 5% O 2 ,12％CO 2 ,400ppm NO,400ppm NH 3 ,600ppm SO 2 ,30ppm HCl，Hg 0 The concentration is 110 mug/m 3 The balance gas is N 2 The flow rate was 500mL/min and the test temperature was 250 ℃. The results of the mercury removal and denitration test are shown in table 2 below.
TABLE 2
| Sample of | Hg 0 Removal efficiency (%) | NO x Removal efficiency (%) |
| 1 | 97 | 86 |
| D-1 | 74 | 67 |
| 2 | 93 | 84 |
| 3 | 83 | 67 |
| D-2 | 100 | 21 |
As can be seen from Table 2 above, hg of the catalyst prepared using the EVS-10 molecular sieve in example 1 of the present disclosure is higher than that of the commercial ETS-10 molecular sieve in comparative example 1 0 Removal efficiency and NO x The removal efficiency is better.
Comparing examples 1-3 of the present disclosure with comparative example 2, comparative example 2 can achieve better elemental mercury removal efficiency, but the nitrogen oxide removal efficiency is extremely low, only 21%. The catalytic adsorbent samples prepared by the method provided by the disclosure in examples 1-3 have higher elemental mercury removal efficiency and nitrogen oxide removal efficiency, and realize synergistic Hg removal 0 And NO x 。
Further comparing examples 1 to 3, it is understood that the catalyst adsorbents obtained in examples 1 to 2 have higher Hg when the dispersion aid is added 0 Removal efficiency and NO x And (5) removing efficiency.
The preferred embodiments of the present disclosure have been described in detail above, but the present disclosure is not limited to the specific details of the above embodiments, and various simple modifications may be made to the technical solutions of the present disclosure within the scope of the technical concept of the present disclosure, and all the simple modifications belong to the protection scope of the present disclosure.
In addition, the specific features described in the above embodiments may be combined in any suitable manner without contradiction. The various possible combinations are not described further in this disclosure in order to avoid unnecessary repetition.
Moreover, any combination between the various embodiments of the present disclosure is possible as long as it does not depart from the spirit of the present disclosure, which should also be construed as the disclosure of the present disclosure.
Claims (10)
1. The EVS-10-based cerium-loaded catalytic adsorbent for flue gas mercury removal and denitration is characterized by comprising a carrier and an active component loaded on the carrier; wherein the carrier comprises an EVS-10 molecular sieve, and the active component comprises CeO 2 。
2. The catalytic adsorbent of claim 1 wherein the mass fraction of the support is 85 to 99 wt% and the mass fraction of the active component is 1 to 15 wt%, based on the total weight of the catalytic adsorbent.
3. A method for preparing the mercury removal and denitration EVS-10 based cerium-supported catalytic adsorbent as claimed in claim 1 or 2, which comprises the following steps:
(1) Mixing an EVS-10 molecular sieve, a cerium source and water to obtain a raw material mixture;
(2) Adding an alkaline solution to the raw material mixture; then adding alcohol to obtain a colloid precursor;
(3) And roasting the colloid precursor.
4. A method according to claim 3, wherein in step (1), the weight ratio of EVS-10 molecular sieve, cerium source and water is (90 to 95): (13-18);
optionally, the cerium source is a soluble cerium salt, preferably one or more selected from cerium acetate, cerium chloride and cerium nitrate.
5. A method according to claim 3, wherein step (1) further comprises: carrying out ultrasonic treatment on the EVS-10 molecular sieve in water for 5-30 minutes, and then adding the cerium source and an optional dispersing auxiliary for mixing to obtain the raw material mixture; preferably, the dispersing aid is selected from one or more of polymethacrylic acid, polyacrylic acid and hydrolyzed polymaleic anhydride, and more preferably polymethacrylic acid.
6. The method of claim 5, wherein the weight ratio of the dispersing aid to the cerium source is (34-68): (13-18).
7. A method according to claim 3, wherein in step (2), the alkaline solution comprises aqueous ammonia; the alcohol comprises ethanol; further preferably, the addition volume ratio (4 to 8) of the aqueous ammonia to the alcohol is: (60-70).
8. A method according to claim 3, wherein step (2) further comprises:
adding the alkaline solution into the raw material mixture obtained in the step (1), and performing ultrasonic treatment for 5-30 minutes; and
before the roasting treatment, the colloid precursor is subjected to ultrasonic treatment for 5-30 minutes, and then is evaporated at 70-100 ℃.
9. A method according to claim 3, wherein in step (3), the conditions of the calcination treatment include: the roasting temperature is 350-600 ℃ and the roasting time is 1-4 hours;
optionally, step (3) further comprises: and cooling the roasting treatment product, sieving, and taking the undersize product to obtain the catalytic adsorbent.
10. Use of the catalytic adsorbent of claim 1 or 2 in the field of flue gas mercury removal and denitration; optionally, the flue gas is flue gas of a coal-fired power plant.
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