CN117883964A - Method for purifying NOx-containing flue gas by utilizing microalgae - Google Patents
Method for purifying NOx-containing flue gas by utilizing microalgae Download PDFInfo
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- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 title claims abstract description 51
- 239000003546 flue gas Substances 0.000 title claims abstract description 51
- 238000000034 method Methods 0.000 title claims abstract description 34
- 239000007789 gas Substances 0.000 claims abstract description 36
- 239000001963 growth medium Substances 0.000 claims abstract description 27
- 241000894006 Bacteria Species 0.000 claims abstract description 23
- 238000012258 culturing Methods 0.000 claims abstract description 17
- 238000007599 discharging Methods 0.000 claims abstract description 3
- 239000007788 liquid Substances 0.000 claims description 22
- 241000195649 Chlorella <Chlorellales> Species 0.000 claims description 15
- 238000004321 preservation Methods 0.000 claims description 15
- 241000195663 Scenedesmus Species 0.000 claims description 13
- 238000005286 illumination Methods 0.000 claims description 11
- 229910052799 carbon Inorganic materials 0.000 claims description 6
- 238000002360 preparation method Methods 0.000 claims description 5
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 claims description 4
- 239000000463 material Substances 0.000 claims description 4
- 230000001580 bacterial effect Effects 0.000 claims description 3
- 241000589565 Flavobacterium Species 0.000 claims description 2
- JVMRPSJZNHXORP-UHFFFAOYSA-N ON=O.ON=O.ON=O.N Chemical compound ON=O.ON=O.ON=O.N JVMRPSJZNHXORP-UHFFFAOYSA-N 0.000 claims description 2
- MMDJDBSEMBIJBB-UHFFFAOYSA-N [O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O.[NH6+3] Chemical compound [O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O.[NH6+3] MMDJDBSEMBIJBB-UHFFFAOYSA-N 0.000 claims description 2
- 230000003698 anagen phase Effects 0.000 claims description 2
- 229910052757 nitrogen Inorganic materials 0.000 claims description 2
- 239000000779 smoke Substances 0.000 claims description 2
- 239000004519 grease Substances 0.000 abstract description 13
- 244000005700 microbiome Species 0.000 abstract description 6
- 230000002195 synergetic effect Effects 0.000 abstract description 3
- 230000008878 coupling Effects 0.000 abstract description 2
- 238000010168 coupling process Methods 0.000 abstract description 2
- 238000005859 coupling reaction Methods 0.000 abstract description 2
- MWUXSHHQAYIFBG-UHFFFAOYSA-N nitrogen oxide Inorganic materials O=[N] MWUXSHHQAYIFBG-UHFFFAOYSA-N 0.000 description 87
- 238000001514 detection method Methods 0.000 description 11
- 239000000243 solution Substances 0.000 description 10
- 239000002028 Biomass Substances 0.000 description 7
- 238000006477 desulfuration reaction Methods 0.000 description 7
- 230000023556 desulfurization Effects 0.000 description 7
- 241000186063 Arthrobacter Species 0.000 description 6
- 241000195493 Cryptophyta Species 0.000 description 5
- 238000005516 engineering process Methods 0.000 description 5
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 description 4
- 241000401308 Flavobacterium aquaticum Species 0.000 description 4
- 239000000706 filtrate Substances 0.000 description 4
- 238000009629 microbiological culture Methods 0.000 description 4
- 239000007787 solid Substances 0.000 description 4
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 3
- 238000010521 absorption reaction Methods 0.000 description 3
- 239000003054 catalyst Substances 0.000 description 3
- 238000010531 catalytic reduction reaction Methods 0.000 description 3
- 238000005119 centrifugation Methods 0.000 description 3
- 238000006243 chemical reaction Methods 0.000 description 3
- KRKNYBCHXYNGOX-UHFFFAOYSA-N citric acid Chemical compound OC(=O)CC(O)(C(O)=O)CC(O)=O KRKNYBCHXYNGOX-UHFFFAOYSA-N 0.000 description 3
- 230000000052 comparative effect Effects 0.000 description 3
- 230000000694 effects Effects 0.000 description 3
- OAYLNYINCPYISS-UHFFFAOYSA-N ethyl acetate;hexane Chemical compound CCCCCC.CCOC(C)=O OAYLNYINCPYISS-UHFFFAOYSA-N 0.000 description 3
- 239000002609 medium Substances 0.000 description 3
- 239000000203 mixture Substances 0.000 description 3
- 239000000843 powder Substances 0.000 description 3
- 230000008569 process Effects 0.000 description 3
- 230000004083 survival effect Effects 0.000 description 3
- 238000009777 vacuum freeze-drying Methods 0.000 description 3
- 229920001817 Agar Polymers 0.000 description 2
- 241000589597 Paracoccus denitrificans Species 0.000 description 2
- 239000008272 agar Substances 0.000 description 2
- 229910021529 ammonia Inorganic materials 0.000 description 2
- 239000003814 drug Substances 0.000 description 2
- 239000003344 environmental pollutant Substances 0.000 description 2
- 230000012010 growth Effects 0.000 description 2
- 230000003647 oxidation Effects 0.000 description 2
- 238000007254 oxidation reaction Methods 0.000 description 2
- 231100000719 pollutant Toxicity 0.000 description 2
- FGIUAXJPYTZDNR-UHFFFAOYSA-N potassium nitrate Chemical compound [K+].[O-][N+]([O-])=O FGIUAXJPYTZDNR-UHFFFAOYSA-N 0.000 description 2
- 230000009467 reduction Effects 0.000 description 2
- 238000006722 reduction reaction Methods 0.000 description 2
- 239000011734 sodium Substances 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- 239000012855 volatile organic compound Substances 0.000 description 2
- 241001489705 Aquarius Species 0.000 description 1
- KCXVZYZYPLLWCC-UHFFFAOYSA-N EDTA Chemical compound OC(=O)CN(CC(O)=O)CCN(CC(O)=O)CC(O)=O KCXVZYZYPLLWCC-UHFFFAOYSA-N 0.000 description 1
- 241000233866 Fungi Species 0.000 description 1
- 206010019233 Headaches Diseases 0.000 description 1
- 239000007836 KH2PO4 Substances 0.000 description 1
- 239000001888 Peptone Substances 0.000 description 1
- 108010080698 Peptones Proteins 0.000 description 1
- 239000002253 acid Substances 0.000 description 1
- 150000007513 acids Chemical class 0.000 description 1
- 230000009471 action Effects 0.000 description 1
- 230000004913 activation Effects 0.000 description 1
- FRHBOQMZUOWXQL-UHFFFAOYSA-L ammonium ferric citrate Chemical compound [NH4+].[Fe+3].[O-]C(=O)CC(O)(CC([O-])=O)C([O-])=O FRHBOQMZUOWXQL-UHFFFAOYSA-L 0.000 description 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
- 235000015278 beef Nutrition 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 239000003225 biodiesel Substances 0.000 description 1
- 239000002551 biofuel Substances 0.000 description 1
- 239000003153 chemical reaction reagent Substances 0.000 description 1
- 239000003638 chemical reducing agent Substances 0.000 description 1
- 239000003795 chemical substances by application Substances 0.000 description 1
- 239000003245 coal Substances 0.000 description 1
- 239000000356 contaminant Substances 0.000 description 1
- 238000007796 conventional method Methods 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 239000012153 distilled water Substances 0.000 description 1
- 229940079593 drug Drugs 0.000 description 1
- 239000000428 dust Substances 0.000 description 1
- 238000010894 electron beam technology Methods 0.000 description 1
- 238000004134 energy conservation Methods 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 238000002474 experimental method Methods 0.000 description 1
- 235000019387 fatty acid methyl ester Nutrition 0.000 description 1
- 229960004642 ferric ammonium citrate Drugs 0.000 description 1
- 239000012847 fine chemical Substances 0.000 description 1
- 239000000446 fuel Substances 0.000 description 1
- 238000010574 gas phase reaction Methods 0.000 description 1
- 238000003306 harvesting Methods 0.000 description 1
- 231100000869 headache Toxicity 0.000 description 1
- 230000002401 inhibitory effect Effects 0.000 description 1
- 239000004313 iron ammonium citrate Substances 0.000 description 1
- 235000000011 iron ammonium citrate Nutrition 0.000 description 1
- 230000007794 irritation Effects 0.000 description 1
- 230000002906 microbiologic effect Effects 0.000 description 1
- 238000002156 mixing Methods 0.000 description 1
- 229910000402 monopotassium phosphate Inorganic materials 0.000 description 1
- 235000019796 monopotassium phosphate Nutrition 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
- 229910052760 oxygen Inorganic materials 0.000 description 1
- 235000019319 peptone Nutrition 0.000 description 1
- 230000029553 photosynthesis Effects 0.000 description 1
- 238000010672 photosynthesis Methods 0.000 description 1
- GNSKLFRGEWLPPA-UHFFFAOYSA-M potassium dihydrogen phosphate Chemical compound [K+].OP(O)([O-])=O GNSKLFRGEWLPPA-UHFFFAOYSA-M 0.000 description 1
- 235000010333 potassium nitrate Nutrition 0.000 description 1
- 239000000047 product Substances 0.000 description 1
- 238000000746 purification Methods 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
- 208000023504 respiratory system disease Diseases 0.000 description 1
- PFUVRDFDKPNGAV-UHFFFAOYSA-N sodium peroxide Chemical compound [Na+].[Na+].[O-][O-] PFUVRDFDKPNGAV-UHFFFAOYSA-N 0.000 description 1
- 229940074404 sodium succinate Drugs 0.000 description 1
- ZDQYSKICYIVCPN-UHFFFAOYSA-L sodium succinate (anhydrous) Chemical compound [Na+].[Na+].[O-]C(=O)CCC([O-])=O ZDQYSKICYIVCPN-UHFFFAOYSA-L 0.000 description 1
- 238000001179 sorption measurement Methods 0.000 description 1
- 231100000331 toxic Toxicity 0.000 description 1
- 230000002588 toxic effect Effects 0.000 description 1
- 239000002912 waste gas Substances 0.000 description 1
- 239000002351 wastewater Substances 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 1
- 239000012224 working solution Substances 0.000 description 1
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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
- B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
- B01D53/84—Biological processes
-
- 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
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- C12N1/00—Microorganisms, e.g. protozoa; Compositions thereof; Processes of propagating, maintaining or preserving microorganisms or compositions thereof; Processes of preparing or isolating a composition containing a microorganism; Culture media therefor
- C12N1/12—Unicellular algae; Culture media therefor
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- C12N1/00—Microorganisms, e.g. protozoa; Compositions thereof; Processes of propagating, maintaining or preserving microorganisms or compositions thereof; Processes of preparing or isolating a composition containing a microorganism; Culture media therefor
- C12N1/20—Bacteria; Culture media therefor
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2251/00—Reactants
- B01D2251/95—Specific microorganisms
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2257/00—Components to be removed
- B01D2257/40—Nitrogen compounds
- B01D2257/404—Nitrogen oxides other than dinitrogen oxide
-
- 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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- C12R2001/00—Microorganisms ; Processes using microorganisms
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Abstract
The invention relates to a method for purifying NOx-containing flue gas by utilizing microalgae, which comprises the steps of adding a microalgae culture medium into a photobioreactor, inoculating the microalgae, and introducing CO-containing gas 2 Culturing the gas for a period of time, inoculating aerobic denitrifying bacteria for a period of time, introducing NOx-containing flue gas for treatment, and discharging purified gas; the microalgae are microalgae with a NOx removal rate of not less than 50%. The invention is advantageous inThe functional microalgae and aerobic denitrifying bacteria are used for coupling and purifying the flue gas, and through the synergistic effect of the two microorganisms, the high-efficiency removal of NOx in the flue gas is realized, and the microalgae cells with high grease content are obtained.
Description
Technical Field
The invention belongs to the technical field of biomass energy, and particularly relates to a method for purifying NOx-containing flue gas by utilizing microalgae.
Background
Nitrogen oxides (NOx) are mainly N 2 O、NO、NO 2 Various forms of the medicine can cause various damages, such as photochemical smog generated by Volatile Organic Compounds (VOC) in the atmosphere, thereby causing strong irritation to eyes and throat, headache, respiratory diseases and the like, and death can be caused by serious people. The NOx emission in China exceeds 2000 ten thousand tons for many years, and the pollution is still serious although the continuous trend of reduction is shown since 2012. 2014 issues about issues<Coal power energy conservation, emission reduction, upgrade and reformation action plan (2014-2020)>The notification of (1) requires that the flue gas of the coal-fired boiler be subjected to ultra-clean emission, namely smoke dust and SO 2 And NOx emission concentration levels of 10mg/Nm, respectively 3 、35mg/Nm 3 And 50mg/Nm 3 。
The prior flue gas denitration technology mainly comprises the following steps: SCR (selective catalytic reduction) and SNCR (selective non-catalytic reduction) of gas phase reaction, liquid absorption method, solid adsorption method, high-energy electron activated oxidation method (EBA electron beam irradiation method and PPCP pulse corona plasma method), and the like. Among the flue gas denitration treatment technologies, the SCR technology has the advantages of high denitration efficiency, mature technology and the like, and is the technology most applied to the flue gas denitration engineering at home and abroad at present. SCR method refers to using NH at a reaction temperature of 200-400 DEG C 3 Catalytic reduction of NOx to N as a reductant 2 The oxygen in the waste gas is little reacted, and the heat release amount is small. However, this reaction still needs to be carried out at a relatively high temperature in the presence of a catalyst, and there are problems such as ammonia slip.
Microalgae can utilize CO 2 Long autotrophy and high carbon fixation efficiency are carried out, and the problem of greenhouse effect brought by the current industrial society is relieved. Microalgae are important renewable resources among many biomass energy sources. They have the characteristics of wide distribution, large biomass, high photosynthesis efficiency, strong environment adaptability, short growth cycle, high biomass output and the like. The solar energy conversion efficiency of the microalgae can reach 3.5%, and the microalgae is a potential resource for producing medicines, fine chemicals and novel fuels, and is obtained from the microalgaeFatty acids can be converted to fatty acid methyl esters, i.e., biodiesel, and microalgae are therefore often considered ideal raw materials for third generation biofuels.
The flue gas contains high concentration of CO 2 But contains harmful substances such as SOx, NOx and the like, and has inhibiting effect on carbon fixation and growth of microalgae. Researchers find that, in practical use, when CO is in the environment 2 When the volume fraction is more than 5v%, most microalgae are inhibited from growing, and the carbon fixation efficiency is low; and CO in industrially discharged gas 2 The concentration is generally 10-20%, and the agent also contains SOx, NOx and other substances which have toxic effects on microalgae. Therefore, microalgae are utilized to purify flue gas, microalgae which can tolerate or remove pollutants of the type need to be bred, and the tolerance concentration of a single strain of microalgae is often not high.
CN109939548A discloses a flue gas desulfurization and denitration method, wherein flue gas is introduced into a desulfurization reactor for ammonia desulfurization to obtain an absorption liquid; introducing the desulfurization flue gas into a photobioreactor for culturing microalgae, and collecting exhaust gas, wherein the microalgae are NOx-tolerant microalgae; separating solid and liquid of the microalgae culture system, and respectively harvesting microalgae cells and filtrate; adding sodium peroxide into the filtrate, and introducing the collected exhaust gas into the filtrate to obtain purified gas; mixing the filtrate obtained by oxidation with desulfurization absorption liquid, and performing anaerobic ammoxidation treatment. The method combines wet desulfurization with microalgae culture process to treat the wastewater containing CO 2 、SO 2 、NO x The flue gas of the utility model realizes the high-efficiency treatment of the flue gas without using a catalyst, and has the advantages of good removal effect, low treatment cost, economy, environmental protection and the like. However, it is necessary to control the NOx content in each stage of photobioreactor to be less than 0.08v%.
Disclosure of Invention
Aiming at the defects of the prior art, the invention provides a method for purifying NOx-containing flue gas by utilizing microalgae. According to the invention, the functional microalgae and the aerobic denitrifying bacteria are utilized to couple and purify the flue gas, and through the synergistic effect of the two microorganisms, the high-efficiency removal of NOx in the flue gas is realized, and the microalgae cells with high grease content are obtained.
The invention provides a method for purifying NOx-containing flue gas by utilizing microalgae, which comprises the following steps:adding microalgae culture medium into a photobioreactor, inoculating microalgae, and introducing CO-containing material 2 Culturing the gas for a period of time, inoculating aerobic denitrifying bacteria for a period of time, introducing NOx-containing flue gas for treatment, and discharging purified gas; the microalgae are microalgae with a NOx removal rate of not less than 50%.
In the invention, the microalgae are microalgae with a NOx removal rate of not less than 50%, preferably more than 80%, for example, the microalgae can be at least one of chlorella SF-B1, scenedesmus TMJ-D3, scenedesmus SZLSi-3 and the like, and the scenedesmus SZLSi-3 is preferred. The preservation numbers of the chlorella SF-B1, the scenedesmus TMJ-D3 and the scenedesmus SZLSi-3 are as follows: CGMCC No. 11005, CGMCC No. 15299, CGMCC No. 22392. Among them, chlorella SF-B1 and Scenedesmus TMJ-D3 have been disclosed in CN109576158A, CN114507602A, and have been submitted for preservation and survival demonstration. The oil-ball algae isGraesiella emersonii) SZLSI-3 has been deposited at China general microbiological culture Collection center, china Committee for culture Collection of microorganisms, at April 04, 23; the preservation number is CGMCC No. 22392; preservation address: the institute of microorganisms of national academy of sciences of China, no. 1, no.3, north Chen West Lu, the Korean region of Beijing.
In the invention, the photobioreactor is a reactor for culturing microalgae conventionally, and can perform light-dark alternate culture.
In the invention, microalgae in the photobioreactor are inoculated according to the volume ratio of the microalgae seed liquid to the microalgae culture medium of 1:20-1:5.
In the invention, the microalgae culture medium adopts any one of BG11 culture medium, SE culture medium, D1 culture medium and the like. Specifically, the preparation of the culture medium and the seed solution of the microalgae is determined according to the types of the microalgae, and the conventional method is the same. Preferably, the preparation method of the seed liquid of the microalgae comprises the following steps: inoculating microalgae into a microalgae culture medium, and carrying out shake culture until the microalgae seed liquid is in a logarithmic growth phase under the conditions that the pH value is 6-9, the temperature is 20-35 ℃, the illumination period is 24 hours, the light-dark time ratio is 14:10-10:14 and the illumination intensity is 2000-20000 Lux, thereby obtaining the microalgae seed liquid.
In the present invention, the catalyst contains CO 2 In the gas, CO 2 The volume content is 5-45%, preferably 5-25%, and the product does not contain SO 2 Contaminants such as NOx.
In the invention, CO-containing material is introduced 2 The cultivation time of the gas is 24-72h.
In the invention, the aerobic denitrifying bacteria are bacterial strains capable of converting nitrate nitrogen and/or nitrite nitrogen into nitrogen under aerobic conditions. For example, arthrobacter can be usedArthrobacter creatinolyticus) FDN-1 and Flavobacterium aquaticumFlavobacterium mizutaii) At least one of the FDN-2 has the preservation numbers of CGMCC No.3657 and CGMCC No.3659 respectively. Arthrobacter FDN-1 and Flavobacterium aquaticum FDN-2 have been disclosed in CN102465105 and CN102465106 and submitted for preservation and survival demonstration.
In the invention, the aerobic denitrifying bacteria are inoculated in the form of seed liquid, and the volume ratio of the aerobic denitrifying bacteria seed liquid to the microalgae culture system is 1:50-1:100. The preparation method of the seed liquid comprises the following steps: the strain on the plate is inoculated in a culture medium by a strain inoculating loop, and is cultured to the logarithmic phase at the temperature of 20-30 ℃ and at the speed of 100-150 rpm.
In the invention, after aerobic denitrifying bacteria are inoculated, the culture is carried out for 12-24 hours, and then flue gas is introduced.
In the invention, the NOx-containing flue gas is derived from at least one of FCC regenerated flue gas, coal-fired flue gas and the like, wherein the concentration of NOx is less than or equal to 0.15% by volume and CO is 2 The concentration is less than or equal to 40v percent, preferably the concentration of NOx is 0.05 to 0.15v percent, and the concentration of CO is as follows 2 The concentration is 5-20 v%.
In the invention, the conditions for culturing in the photobioreactor are as follows: the illumination intensity is 1500-20000 Lux, the pH value is 6-9, the temperature is 20-35 ℃, the light-dark period is 24 hours, and the light-dark time ratio is 14:10-10:14.
Compared with the prior art, the invention has the following beneficial effects:
(1) Aiming at the characteristic of the flue gas containing NOx, the invention utilizes the coupling purification of the functional microalgae and the aerobic denitrifying bacteria to realize the efficient removal of NOx in the flue gas by the synergistic effect of the two microorganisms, and obtains microalgae cells with high grease content.
(2) The SZLSI-3 of the invention is more suitable for mixed culture with aerobic denitrifying bacteria, not only can effectively remove NOx, but also can remarkably improve the grease content.
Detailed Description
The technical scheme and effects of the present invention are further described in detail below with reference to specific examples. The embodiment is implemented on the premise of the technical scheme of the invention, and detailed implementation modes and specific operation processes are given, but the protection scope of the invention is not limited to the following embodiment.
The experimental methods in the following examples, unless otherwise specified, are all conventional in the art. The experimental materials used in the examples described below, unless otherwise specified, were purchased from conventional biochemical reagent stores. In the present invention, v% is the volume fraction.
The flue gas adopted by the invention contains NOx and CO 2 NOx is mainly NO and/or NO 2 . The pollutant content in the flue gas is detected by a flue gas analyzer.
In the present invention, the removal rate= (inlet gas content-outlet gas content)/inlet gas content.
The chlorella SF-B1, the scenedesmus TMJ-D3 and the oleaginous chlorella SZLSI-3 adopted by the embodiment of the invention are functional microalgae which are bred and preserved by the inventor and can remove NOx, wherein the oleaginous chlorella SZLSI-3 is a microalgae which is not disclosed yet. The chlorella is characterized in thatChlorella sp.) SF-B1 has been preserved in China general microbiological culture Collection center (CGMCC) at 7 and 6 of 2015 with a preservation number of CGMCC No. 11005. The scenedesmus is a kind of scenedesmusScenedesmus sp.) TMJ-D3 has been preserved in China general microbiological culture Collection center (CGMCC) with a preservation number of CGMCC No. 15299 in the 2 nd month 5 of 2018. The oil-ball algae isGraesiella emersonii) SZLSI-3 has been deposited at China general microbiological culture Collection center, china Committee for culture Collection of microorganisms, at April 04, 23; the preservation number is CGMCC No. 22392. The preservation addresses of the microalgae are the microbiological institute of China academy of sciences of national academy of sciences of No. 1 and No.3 of North West Lu of the Chaoyang area of Beijing city.
The microalgae culture medium adopted in the embodiment of the invention is BG11 culture medium, and the formula is shown in Table 1 and Table 2. BG11 liquid media were first prepared according to tables 1 and 2, the pH of the media was adjusted to 8.0, and then microalgae were inoculated into the media, respectively. Culturing in a constant temperature illumination shaking table at 25deg.C for 24 hr with a light-dark time ratio of 14:10 and illumination intensity of 5000Lux at 120rpm to logarithmic phase to obtain microalgae seed liquid.
TABLE 1 BG11 Medium
| Composition of the components | Working solution[g/L] |
| NaNO 3 | 1.5 |
| K 2 HPO 4 ·3H 2 O | 0.04 |
| MgSO 4 ·7H 2 O | 0.075 |
| CaCl 2 ·2H 2 O | 0.036 |
| Citric acid | 0.006 |
| Ferric ammonium citrate | 0.006 |
| EDTA | 0.001 |
| Na 2 CO 3 | 0.02 |
| A5+Co solution* | 1mL |
| Distilled water | 919 |
* Table 2 composition of A5+Co solution in Table 1
| Composition of the components | Content (g/L) |
| H 3 BO 3 | 2.86 |
| MnCl 2 ·H 2 O | 1.81 |
| ZnSO 4 ·7H 2 O | 0.222 |
| CuSO 4 ·5H 2 O | 0.079 |
| Na 2 MoO 4 ·2H 2 O | 0.390 |
| Co(NO 3 ) ·6H 2 O | 0.049 |
In the invention, the culture medium formula for the bacterial activation and seed solution culture of the Arthrobacter FDN-1 and the Flavobacterium aquaticum FDN-2 is as follows: beef extract 5g/L, peptone 10g/L, naNO 2 1g/L, and 2% agar was added to the solid medium. Inoculating aerobic denitrifying bacteria on a plate to a culture medium by a bacteria inoculating loop, and shake culturing for 48 hours at the temperature of 30 ℃ and at the speed of 150rpm to obtain aerobic denitrifying bacteria seed liquid.
The flue gas in the invention is derived from regenerated flue gas of FCC device in a certain refinery, after desulfurization treatment, the concentration of NOx is 0.05-0.15 v%, and the concentration of CO is as follows 2 The concentration is 5-20 v%.
Example 1
Adding 8L microalgae culture medium and 1L Chlorella SF-B1 seed solution into a 20L photobioreactor, and introducing CO 2 Culturing 5% by volume of gas alternately in light and dark for 48 hr, inoculating 100mL of Arthrobacter FDN-1 seed solution, culturing for 18 hr, introducing NOx-containing flue gas for treatment, wherein the content of NOx in the flue gas is 0.12v%, and CO is contained in the flue gas 2 The content was 20v%. The treatment conditions are as follows: the light-dark period is 24 hours, the light-dark time ratio is 14:10, the illumination intensity is 5000Lux, the culture temperature is 25 ℃, and the pH value is 8.0. Collecting purified gas for detection and analysis, wherein the NOx removal rate in the exhaust gas is 85.9%.
After the treatment is finished, microalgae cells are harvested by centrifugation, and the dry weight and the grease content of the cells are measured. And (3) vacuum freeze-drying at-60 ℃ to constant weight, measuring the dry weight of the algae powder, calculating the biomass yield, and measuring the total fat content by adopting an n-hexane-ethyl acetate method. The detection shows that the dry weight of the cells is 11.1g/L, and the oil content is 51.25% of the dry weight of the cells.
Example 2
Adding 8L microalgae culture medium and 800mL chlorella SF-B1 into a 20L photobioreactor, and introducing CO 2 Culturing 15% by volume of gas alternately in light and dark for 36h, inoculating 80mL of Arthrobacter FDN-1 seed solution, culturing for 12h, introducing NOx-containing flue gas for treatment, wherein the content of NOx in the flue gas is 0.15% by volume, and CO is contained in the flue gas 2 The content was 25v%. The treatment conditions are as follows: the light-dark period is 24h, and the light-dark time ratio is 14:10, the illumination intensity is 5000Lux, the culture temperature is 25 ℃, and the pH value is 8.0. And collecting purified gas for detection and analysis, wherein the NOx removal rate in the exhaust gas is 86.6%.
After the treatment is finished, microalgae cells are harvested by centrifugation, and the dry weight and the grease content of the cells are measured. And (3) vacuum freeze-drying at-60 ℃ to constant weight, measuring the dry weight of the algae powder, calculating the biomass yield, and measuring the total fat content by adopting an n-hexane-ethyl acetate method. The detection shows that the dry cell weight is 10.9g/L and the grease content is 50.47% of the dry cell weight.
Example 3
Adding 8L microalgae culture medium and 1.2L scenedesmus TMJ-D3 into a 20L photobioreactor, and introducing CO 2 Culturing gas with volume content of 10% alternately in light and dark for 60 hr, inoculating F.aquarius FDN-2 seed solution 120mL, culturing for 20 hr, introducing NOx-containing flue gas for treatment, wherein the content of NOx in the flue gas is 0.10v%, and CO is contained in the flue gas 2 The content was 20v%. The treatment conditions are as follows: the light-dark period is 24 hours, the light-dark time ratio is 14:10, the illumination intensity is 5000Lux, the culture temperature is 25 ℃, and the pH value is 8.0. The purified gas was collected for detection and analysis, and the NOx removal rate in the exhaust gas was 84.6%.
After the treatment is finished, microalgae cells are harvested by centrifugation, and the dry weight and the grease content of the cells are measured. And (3) vacuum freeze-drying at-60 ℃ to constant weight, measuring the dry weight of the algae powder, calculating the biomass yield, and measuring the total fat content by adopting an n-hexane-ethyl acetate method. The detection shows that the dry weight of the cells is 10.8g/L, and the grease content is 50.96% of the dry weight of the cells.
Example 4
The difference from example 2 is that: the microalgae adopts the oil chlorella SZLSi-3. The NOx removal rate in the exhaust gas was 90.2%. The detection shows that the dry cell weight is 9.6g/L and the grease content is 52.63% of the dry cell weight.
Example 5
The difference from example 2 is that: the microalgae adopts chlorella SF-B1, scenedesmus TMJ-D3 and YZLSi-3 seed liquid, and the volume ratio of the seed liquid to the seed liquid is 1:1:1. The NOx removal rate in the exhaust gas was 85.2%. The detection shows that the dry weight of the cells is 10.2g/L, and the grease content is 51.63% of the dry weight of the cells.
Example 6
The difference from example 2 is that: the aerobic denitrifying bacteria adopts Arthrobacter FDN-1 and Flavobacterium aquaticum FDN-2, and the volume ratio of the seed solution to the seed solution is 1:1. The NOx removal rate in the exhaust gas was 84.8%. The dry cell weight was found to be 11.3g/L and the oil content was found to be 50.88% of the dry cell weight.
Example 7
The difference from example 2 is that: the aerobic denitrifying bacteria adopts Flavobacterium aquaticum FDN-2. The NOx removal rate in the exhaust gas was 85.3%. The detection shows that the dry cell weight is 11.6g/L and the grease content is 51.33% of the dry cell weight.
Example 8
The difference from example 1 is that: the aerobic denitrifying bacteria inoculated in the culture process is paracoccus denitrificans DN-3, the preservation number is CGMCC No.3658, and the strain is disclosed in CN102465104A and submitted for preservation and survival demonstration. The formula of the culture medium is as follows: KNO3 1g/L, sodium succinate 8g/L, KH2PO4 1g/L, feCl2 0.5g/L; the solid medium was added with 20g/L agar. The paracoccus denitrificans DN-3 on the plate is inoculated in the culture medium by a fungus inoculating loop, and shake culture is carried out for 48 hours under the condition of 30 ℃ and 150rpm, thus obtaining seed liquid. After the cultivation is finished, the NOx removal rate in the exhaust gas is 72.8% through detection and analysis. The dry cell weight was found to be 11.0g/L and the fat content was found to be 49.67% of the dry cell weight.
Comparative example 1
The difference from example 1 is that: the microalgae adopts the chain belt alga HCS-BY1 disclosed in CN 114437935A, and the preservation number is CGMCC No. 19982. The NOx removal rate in the exhaust gas was 30.9%. The detection shows that the dry cell weight is 10.9g/L and the grease content is 50.34% of the dry cell weight.
Comparative example 2
The difference from example 1 is that: microalgae and aerobic denitrifying bacteria are directly mixed for treating flue gas. The NOx removal rate in the exhaust gas was 69.8%. The dry cell weight was found to be 11.0g/L and the oil content was found to be 48.84% of the dry cell weight.
Comparative example 3
The difference from example 1 is that: the microalgae do not contain CO 2 And (3) culturing the gas for a period of time, and directly treating the flue gas. NO in the exhaust gasThe x removal rate was 72.9%. The dry cell weight was found to be 10.8g/L and the fat content was found to be 49.26% of the dry cell weight.
Claims (14)
1. A method for purifying flue gas containing NOx by utilizing microalgae, which is characterized by comprising the following steps: adding microalgae culture medium into a photobioreactor, inoculating microalgae, and introducing CO-containing material 2 Culturing the gas for a period of time, inoculating aerobic denitrifying bacteria for a period of time, introducing NOx-containing flue gas for treatment, and discharging purified gas; the microalgae are microalgae with a NOx removal rate of not less than 50%.
2. The method according to claim 1, characterized in that: the microalgae are microalgae with a NOx removal rate of not less than 80%.
3. The method according to claim 1 or 2, characterized in that: the microalgae is at least one of Chlorella SF-B1, scenedesmus TMJ-D3 and Chlorella SZLSi-3, preferably Chlorella SZLSi-3; the preservation numbers of the chlorella SF-B1, the scenedesmus TMJ-D3 and the scenedesmus SZLSi-3 are as follows: CGMCC No. 11005, CGMCC No. 15299, CGMCC No. 22392.
4. The method according to claim 1, characterized in that: the microalgae culture medium adopts any one of BG11 culture medium, SE culture medium and D1 culture medium.
5. The method according to claim 1 or 4, characterized in that: the microalgae in the photobioreactor are inoculated according to the volume ratio of the microalgae seed liquid to the microalgae culture medium of 1:20-1:5.
6. The method according to claim 1 or 5, characterized in that: the preparation method of the seed liquid of the microalgae comprises the following steps: inoculating microalgae into a microalgae culture medium, and carrying out shake culture to a logarithmic growth phase under the conditions that the pH value is 6-9, the temperature is 20-35 ℃, the illumination period is 24 hours, the light-dark time ratio is 14:10-10:14 and the illumination intensity is 2000-20000 Lux, so as to obtain the seed liquid of the microalgae.
7. The method according to claim 1, characterized in that: said CO-containing 2 In the gas, CO 2 The volume content is 5-45%, preferably 5-25%, and the product does not contain SO 2 、NOx。
8. The method according to claim 1 or 7, characterized in that: introducing CO-containing gas 2 The cultivation time of the gas is 24-72h.
9. The method according to claim 1, characterized in that: the aerobic denitrifying bacteria are bacterial strains capable of converting nitrate nitrogen and/or nitrite nitrogen into nitrogen under aerobic conditions, and preferably adopting Arthrobacter @ aArthrobacter creatinolyticus) FDN-1 and Flavobacterium aquaticumFlavobacterium mizutaii) At least one of the FDN-2 has the preservation numbers of CGMCC No.3657 and CGMCC No.3659 respectively.
10. The method according to claim 1 or 9, characterized in that: the aerobic denitrifying bacteria are inoculated according to the volume ratio of the seed solution of the aerobic denitrifying bacteria to the microalgae culture system of 1:50-1:100.
11. The method according to claim 1 or 10, characterized in that: the preparation method of the seed liquid of the aerobic denitrifying bacteria comprises the following steps: the strain on the plate is inoculated in a culture medium by a strain inoculating loop, and is cultured to the logarithmic phase at the temperature of 20-30 ℃ and at the speed of 100-150 rpm.
12. The method according to claim 1 or 9, characterized in that: and (5) inoculating aerobic denitrifying bacteria, culturing for 12-24 hours, and then introducing smoke.
13. The method according to claim 1, characterized in that: the NOx-containing flue gas is derived from at least one of FCC regenerated flue gas and coal-fired flue gas, wherein the concentration of NOx is less than or equal to 0.15v%, and CO is contained in the flue gas 2 The concentration is less than or equal to 40v percent, preferably the concentration of NOx is 0.05 to 0.15v percent, and the concentration of CO is as follows 2 The concentration is 5-20 v%.
14. The method according to claim 1, characterized in that: the conditions for culturing in the photobioreactor are as follows: the illumination intensity is 1500-20000 Lux, the pH value is 6-9, the temperature is 20-35 ℃, the light-dark period is 24 hours, and the light-dark time ratio is 14:10-10:14.
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