CN104630065A - Combined method of microalgae culture and waste gas denitration - Google Patents
Combined method of microalgae culture and waste gas denitration Download PDFInfo
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- CN104630065A CN104630065A CN201310567259.XA CN201310567259A CN104630065A CN 104630065 A CN104630065 A CN 104630065A CN 201310567259 A CN201310567259 A CN 201310567259A CN 104630065 A CN104630065 A CN 104630065A
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- C—CHEMISTRY; METALLURGY
- C12—BIOCHEMISTRY; BEER; SPIRITS; WINE; VINEGAR; MICROBIOLOGY; ENZYMOLOGY; MUTATION OR GENETIC ENGINEERING
- C12N—MICROORGANISMS OR ENZYMES; COMPOSITIONS THEREOF; PROPAGATING, PRESERVING, OR MAINTAINING MICROORGANISMS; MUTATION OR GENETIC ENGINEERING; CULTURE MEDIA
- 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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- 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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- 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
- B01D53/77—Liquid phase processes
- B01D53/78—Liquid phase processes with gas-liquid contact
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2251/00—Reactants
- B01D2251/10—Oxidants
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2251/00—Reactants
- B01D2251/10—Oxidants
- B01D2251/102—Oxygen
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2251/00—Reactants
- B01D2251/10—Oxidants
- B01D2251/106—Peroxides
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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
Abstract
The invention discloses a combined method of microalgae culture and waste gas denitration. The method comprises: (1) providing part of a carbon source for the microalgae culture process by using gas containing CO2 at least; keeping the algae liquid alkali when the culture is finished by means of microalgae metabolism; separating out microalgae from the harvested algae liquid to obtain microalgae and alkali residue; (2) transforming NOx in industrial smoke into nitric acid and/or nitrous acid; and (3) contacting the alkali residue obtained in the step (1) with the nitric acid and/or nitrous acid obtained in the step (2) to obtain a nitrogen-containing neutralized liquid, which provides a nitrogen source for the microalgae culture process. According to the method, 'microalgae culture' and 'waste gas denitration' can be combined reasonably, the microalgae can grow normally with NOx in the waste gas, the NOx can be effectively removed from the waste gas, and mutual influence of 'microalgae culture' and 'waste gas denitration' can be further avoided, so that the two processes can run stably and reliably.
Description
Technical field
The present invention relates to the integrated processes of a kind of both culturing microalgae and exhaust gas denitration.
Background technology
" energy " and " environment " are the major issues that new millennium human society in Sustainable development faces, and on the one hand, the fossil energy supporting mankind's modern civilization is non-renewable, and thus exploitation substitute energy technology is being stepped up in countries in the world; On the other hand, the mankind inevitably produce serious waste gas and the emission problem of sewage when processing and use fossil energy, have caused serious impact to the living environment of weather and the mankind.These problems need the solution made overall plans and coordinate.
Micro-algae is " chemical plant of living " that driven by sunlight of ultrahigh in efficiency, by the efficient photosynthesis of microalgae cell, is the chemical energy of the carbohydrate such as fat or starch, and releases O by light energy conversion
2.Utilize micro-algae production bioenergy and chemical can reach the dual purpose of " substitute fossil energy and reduce industrial gas emission " simultaneously.Micro-algae is the Biological resources that a class is very original, does not have Organ Differentiation, so have the advantages that growth is fast, output is high, environmental compatibility is strong, and compared with higher plant, the content of the effective constituents such as their lipid, starch and protein is higher.The traditional commerce application of micro-algae comprises the raw material they being used as foodstuff additive, feed in agricultural and culture fishery and chemical industry.In addition, some algae possess oleaginousness high, be easy to cultivate, yield per unit greatly, with agricultural do not strive etc. advantage, be regarded as a new generation, or even uniquely can realize the biodiesel raw material of substitute fossil fuels.
Micro-algae can be divided into protokaryon algae and Eukaryotic Algae, and protokaryon algae is based on blue-green algae, and containing chlorophyll a, do not form organoid, can carry out photosynthesis, in cell, protein content is high, and can reach 70% of dry weight, lipid content is low, is about 5%; Eukaryotic Algae kind is many, is the source of main biofuel algae kind.Common micro-algae is mainly attributed to following eight classes: Bacillariophyta (Bacillariophyta), Chlorophyta (Chlorophyta), Chrysophyta (Chrysophyta), Cyanophyta (Cyanophyta), Pyrrophyta (Pyrroptata), Euglenophyta (Rhodophyta), Cryptophyta (Cryptophyta) and Xanthophyta (Xanthophyta).Wherein, Bacillariophyta, Chlorophyta and Chrysophyta are the biofuel algae kind sources of most potentiality.
Oxynitride (NO
x) be important pollutent contained in fossil oil flue gas, comprise multiple compounds, as Nitrous Oxide (N
2o), nitrogen protoxide (NO), nitrogen peroxide (NO
2), nitrous anhydride (N
2o
3), nitrogen tetroxide (N
2o
4) and nitrogen pentoxide (N
2o
5) etc.Wherein, nitrogen protoxide (NO) is NO
xmain component, it generates nitrogen peroxide (NO with the oxygen in air
2), then cause photo-chemical smog and acid rain.Meanwhile, NO
xalso be one of main greenhouse gases, if with CO
2count 1 as benchmark, then the warming effect of oxynitride is 310.And at present, the quantity discharged rapid development of the oxynitride of China, reaches 1797.7 ten thousand tons 2007 years, be cause China's big city content of nitrogen dioxide general higher and in the one of the main reasons progressively increasing trend.Therefore, country will in the control dynamics of " 12 " period increasing to discharged nitrous oxides, and exhaust gas denitration will become the emphasis of air contaminant treatment.But traditional exhaust gas denitration technology is because mostly existing, and some are as large in energy consumption, initial cost is high, poor stability and cause the problem of secondary pollution etc., are difficult to reach efficient, economy, low consumption requirement.Alkali absorption method is that people study class denitrations maximum the earliest and (remove the NO in waste gas
x) method, technical process and the equipment of the method are fairly simple, mature technical route, can by NO
xchange into marketable nitrite and/or nitrate products, therefore contain NO
xwaste gas pollution control and treatment in be widely used.In alkali absorption method, concentration of lye can not be too high, otherwise crystallization can be there is in the process generating nitrite and/or nitrate, cause the blocking on absorption tower, concentration of lye in commercial run generally needs to control below 16%, otherwise easily there is crystallization, but under so low concentration of lye, greatly can increase again energy consumption when extracting nitrite and/or nitrate.Nitric acid oxidation absorption process is the exhaust gas denitration method of another kind of industrial application, and the method is generally with the HNO of mass concentration 40 ~ 65%
3the aqueous solution, as absorption agent, absorbs the NO in waste gas at 0 ~ 60 DEG C
x, higher NO can be reached
xdecreasing ratio.
Both culturing microalgae is combined with off gas treatment, both can reduce the toxigenic capacity of algae, the reduction of discharging of pollutent can be realized again.Increasingly extensive along with cultivating microalgae, in the nineties in last century, some investigators consider that micro-algae absorbs the CO in fossil oil flue gas
2time, the pollution substance in flue gas can be removed, as NO simultaneously
x.If micro-algae in process of growth by NO
xalso absorb in a large number, both can meet self needs to N, again can flue, reduce NO
xdischarge, reduce further the toxigenic capacity of algae and produce more overall situation benefit.The report of Yoshihara etc. gives (YOSHIHARA K certainly to this, NAGASE H, EGUCHI K, et al.Miyamoto, biological elimination of nitric oxide and carbon dioxide from flue gas by marine microalga NOA-113cultivated in a long tubular photobioreactor [J] .J Ferment Bioeng, 1996,82 (4): 351-354).
Micro-algae removes NO by assimilation under photosynthesis
x, there is not the problem of material expensive and corrosion and pollution relative to conventional physical chemical process, again more general biological process fast growth and do not need supply organic, and can with CO
2fixing synchronously to carry out, can also produce the product of high economic worth, more meet changing waste into resources and innoxious thought, economy is also better.So remove NO by both culturing microalgae method
x(micro-algae denitration) is recently considered to a kind of and reduces NO in flue gas
xattractive selection, be a kind of potential NO
xremoval scheme.Prior art has many reports directly flue gas passed into both culturing microalgae device and realize method of denitration, the method described in CN1668185A.But, directly pass into flue gas cultivating microalgae can be with and serve insoluble problem, one, micro-algae denitration must solve some problems limiting its commercialization process, such as: the cultivation of micro-algae needs illumination and warm weather condition, and weather is change, so the efficiency that micro-algae absorbs fixed-contamination thing is also change, " directly pass into flue gas " and coupling denitration operating mode and both culturing microalgae operating mode will be difficult to, thus cause two-stage process to influence each other, the reduction of discharging requirement of the extensive waste gas to continuous blow-down in actual production cannot be met; Its two, NO solvability in water is extremely low, and " directly passing into flue gas " cannot solve NO
xin a large amount of NO water insoluble and be difficult to the problem that absorbs; Its three, most of micro-algaes are difficult to the NO of enduring high-concentration
x, therefore utilize micro-algae to absorb the NO of fixing high density
xbe very easy to cause microdisk electrode failure, the cultivation of micro-algae is also easily collapsed because of disease and pest, thus has a strong impact on the steady running of denitration.
No matter be absorb NO with water
x, or absorb NO with salpeter solution, alkaline solution
x, in absorption liquid, all will inevitably there is a large amount of NO
2 -.NO
3 -the main existence form of known occurring in nature inorganic nitrogen, almost can by all micro-algae assimilation, but occurring in nature NO
2 -content normally very low, and be known poisonous substance, most micro-algae can not metabolism NO
2 -.By NO
xchanging into suitable existence form is a kind of solution considered, as Chinese patent CN102061261B discloses a kind of method utilizing coal-fired plant flue gas cultivating microalgae, by by cultivating microalgae after the purification of coal-fired plant flue gas ultra-clean, realize reducing smoke pollution and carbon emission.Concrete steps are as follows: first flue gas is passed into de-CO tower by (1), make wherein trace amounts of CO and NO, under the effect of active carbocoal catalyst, catalyzed oxidation occur, and generate CO
2and N
2; (2) enter thionizer again from de-CO tower flue gas out, utilize contained O in flue gas
2by the SO in flue gas
xsO is oxidized under the effect of active carbocoal catalyst
3, and be adsorbed onto on catalyzer; (3) flue gas after thionizer enters denitrating tower, utilizes O contained in flue gas
2under the effect of active carbocoal catalyst, the NO in flue gas is oxidized to NO
2, and absorption is on a catalyst; (4) flue gas after purification passes into both culturing microalgae device, is fixed the CO in flue gas by oil-containing micro-algae
2, finally will remain fume emission.In described thionizer and denitrating tower, inactivation char catalyst is regenerated by ammonia scrubbing, obtains sulphur ammonium and ammonium nitrate solution simultaneously, and is inputted both culturing microalgae device.The method is by NO
xchange into ammonium nitrate and it can be used as nitrogenous fertilizer to be supplied to micro-algae, but most of micro-algae can not adapt to the ammonium salt solution of high density, as sulphur ammonium is usually used as the inhibitor of micro-algae in the prior art, therefore the application of the method can be subject to certain restrictions.
In sum, a kind of by the method for " both culturing microalgae " and " exhaust gas denitration " reasonable combination in the urgent need to developing, the NO in waste gas can either be utilized
xmake micro-algae normal growth, again can NO in effective elimination waste gas
x, influencing each other of " both culturing microalgae " and " exhaust gas denitration " can also be avoided, make two processes all can stablize, run reliably.
Summary of the invention
The object of the invention is, in order to provide a kind of by the method for " both culturing microalgae " and " exhaust gas denitration " reasonable combination, the NO in waste gas can either be utilized
xmake micro-algae normal growth, again can NO in effective elimination waste gas
x, influencing each other of " both culturing microalgae " and " exhaust gas denitration " can also be avoided, make two processes all can stablize, run reliably.
To achieve these goals, the invention provides the integrated processes of a kind of both culturing microalgae and exhaust gas denitration, the method comprises:
(1) at least with containing CO
2gas provide part carbon source for microalga cultivation process; Algae liquid at the end of relying on micro-algae metabolism to make cultivation is in alkalescence; From the algae liquid of results, isolate micro-algae, obtain micro-algae and alkaline residue;
(2) by the NO in the flue gas of industrial discharge
xbe converted into nitric acid and/or nitrous acid;
(3) nitric acid that alkaline residue step (1) obtained and step (2) obtain and/or nitrous acid contacts, obtain nitrogenous neutralizer, with described nitrogenous neutralizer for microalga cultivation process provides nitrogenous source.
Preferably, the algae liquid at the end of relying on micro-algae metabolism to make cultivation comprises in the method for alkalescence: make in micro algae culturing liquid containing at least one in base metal nitrate, alkali metal nitrites salts, alkaline carbonate, alkali metal hydrocarbonate, alkali metal phosphate, alkali metal hydrogen phosphate.Basic metal is preferably sodium or potassium.
Preferably, in microalga cultivation process, the pH value regulating algae liquid is 7-11.
Preferably, in step (1), at the end of relying on micro-algae metabolism to make cultivation, the pH value >8 of algae liquid, is more preferably 9-11.
" both culturing microalgae " and " exhaust gas denitration " can reasonably combine by the inventive method, can either utilize the NO in waste gas
xmake micro-algae normal growth, again can NO in effective elimination waste gas
x, influencing each other of " both culturing microalgae " and " exhaust gas denitration " can also be avoided, make two processes all can stablize, run reliably.
Other features and advantages of the present invention are described in detail in embodiment part subsequently.
Accompanying drawing explanation
Fig. 1 is the process flow sheet of the inventive method.
Fig. 2 is the growth curve that embodiment 1 cultivates chlorella.
Fig. 3 is the growth curve that embodiment 2 cultivates grid algae.
Fig. 4 is the growth curve that embodiment 3 cultivates single needle algae.
Embodiment
Below the specific embodiment of the present invention is described in detail.Should be understood that, embodiment described herein, only for instruction and explanation of the present invention, is not limited to the present invention.
The invention provides the integrated processes of a kind of both culturing microalgae and exhaust gas denitration, the method comprises:
(1) at least with containing CO
2gas provide part carbon source for microalga cultivation process; Algae liquid at the end of relying on micro-algae metabolism to make cultivation is in alkalescence; From the algae liquid of results, isolate micro-algae, obtain micro-algae and alkaline residue;
(2) by the NO in the flue gas of industrial discharge
xbe converted into nitric acid and/or nitrous acid;
(3) nitric acid that alkaline residue step (1) obtained and step (2) obtain and/or nitrous acid contacts, obtain nitrogenous neutralizer, with described nitrogenous neutralizer for microalga cultivation process provides nitrogenous source.
The technical process of the inventive method as shown in Figure 1.
According to the present invention, by the NO in the flue gas of fixing industrial discharge
xfor cultivating microalgae provides required nitrogenous source.Except nitrogenous source, also need to maintain other prerequisite required for micro-algae normal growth in the process of cultivating micro-algae, as provided suitable illumination, temperature, and the necessary nutrition of other micro algae growth, dissolved oxygen, water, necessary nutrient matter, pH value etc. in regulation and control algae liquid are in suitable scope, make the quick growth and reproduction of its suitable micro-algae, these are conventionally known to one of skill in the art, do not repeat them here.
The present inventor is found by lot of experiments research: along with some nutritive substance is absorbed by micro-algae, and the phenomenon risen can occur the pH value of algae liquid.Contriver is by studying discovery further, when containing at least one in base metal nitrate, alkali metal nitrites salts, alkaline carbonate, alkali metal hydrocarbonate, alkali metal phosphate, alkali metal hydrogen phosphate in micro algae culturing liquid, if do not pass into CO in algae liquid in the breeding process of micro-algae
2, then the pH value of algae liquid presents ascendant trend; Especially when containing at least one in base metal nitrate, alkali metal nitrites salts, alkaline carbonate and alkali metal hydrocarbonate in nutrient solution, then the pH value of algae liquid presents ascendant trend faster; Particularly when containing base metal nitrate and/or alkali metal nitrites salts in nutrient solution, the pH value of algae liquid presents ascendant trend faster.The present invention at least adopts containing CO
2gas be micro-algae breeding process provides part carbon source, by controlling containing CO
2the intake of gas, can easily the pH value of algae liquid be controlled in suitable scope.
As mentioned above, when containing at least one in base metal nitrate, alkali metal nitrites salts, alkaline carbonate, alkali metal hydrocarbonate, alkali metal phosphate, alkali metal hydrogen phosphate in micro algae culturing liquid, if in the breeding process of micro-algae, do not pass into or pass into CO less
2, then the pH value of algae liquid presents the trend of rising.Utilize this phenomenon, in the cultivating microalgae later stage, can not pass into or pass into CO less
2, the algae liquid at the end of relying on micro-algae metabolism to make cultivation is in alkalescence.Therefore, algae liquid at the end of relying on micro-algae metabolism to make cultivation preferably includes in the method for alkalescence: make in micro algae culturing liquid containing at least one in base metal nitrate, alkali metal nitrites salts, alkaline carbonate, alkali metal hydrocarbonate, alkali metal phosphate, alkali metal hydrogen phosphate, namely rely at least one in micro-algae metabolism base metal nitrate, alkali metal nitrites salts, alkaline carbonate, alkali metal hydrocarbonate, alkali metal phosphate, alkali metal hydrogen phosphate, the algae liquid at the end of making cultivation is in alkalescence; More preferably rely at least one in micro-algae metabolism base metal nitrate, alkali metal nitrites salts, alkaline carbonate and alkali metal hydrocarbonate, the algae liquid at the end of making cultivation is in alkalescence; Further preferably rely on micro-algae metabolism base metal nitrate and/or alkali metal nitrites salts, the algae liquid at the end of making cultivation is in alkalescence.
In the present invention, basic metal is preferably sodium and/or potassium, more preferably potassium.Because the present invention is a kind of denitration pattern capable of circulation, therefore potassium ion can be selected as NO under the adaptable prerequisite of micro-algae
3 -and NO
2 -counterion, both can reach better denitration effect, not increase reagent cost again.
It will be understood by those skilled in the art that, only in suitable pH value range, micro-algae can grow fast.Generally speaking, in the process of cultivating microalgae, suitable pH value is 7-11.Therefore, in preferred microalga cultivation process, the pH value regulating algae liquid is 7-11.As mentioned above, can by controlling containing CO
2the intake of gas regulate.
NO in the flue gas of industrial discharge
xnitric acid and nitrous acid can be generated with water or salpeter solution generation chemical reaction as a kind of sour gas, be shown below:
（i）2NO
2+H
2O→HNO
2+HNO
3
（ii）3NO
2+H
2O→2HNO
2+NO
（iii）2NO+O
2→2NO
2
（iv）NO+NO2→N
2O
3
（v）N
2O
3+H
2O→2HNO
2
NO can be converted into NO by oxidation
2, thus react with water further.Oxygenant have the generation being beneficial to reaction, conventional oxygenant has air, O
2, O
3or H
2o
2deng.If containing nitric acid in absorption liquid, then due to the oxidisability of nitric acid and its make absorption liquid to NO to the binding ability of NO
xreceptivity greatly strengthen.
The present invention can adopt existing known mode by the NO in industrial discharge flue gas
xbe converted into nitric acid and/or nitrous acid, such as can at NO
xwill containing NO in fixed cell
xindustrial gaseous waste under the existence of oxygenant, fill part contact with absorption liquid, remove NO
xand obtain nitric acid, nitrous acid or its mixture.Preferably in containing the absorption liquid of nitric acid, absorb NO
x, NO
xfixed cell can be such as bubbling reactor or packed absorber.In order to improve NO further
xremoval efficiency, the present invention can at described NO
xfixed cell downstream installs alkali liquor absorption NO additional
xdevice, such as installs one section of alkali lye spray equipment additional.Described alkali liquor absorption NO
xin device, the alkaline residue obtained after being preferably separated with described algae liquid is as described alkali liquor absorption NO
xthe absorption agent of device, described alkaline residue absorbs the NO in fixing waste gas
xafter, obtain containing NO
3 -and NO
2 -solution, this solution can be microalga cultivation process equally and provides nitrogenous source.
Contriver finds, utilizing both culturing microalgae unit to isolate the alkaline residue after micro-algae can by the NO in the flue gas of industrial discharge
xthe neutralization of the nitric acid transformed, nitrous acid becomes nitrogenous neutralizer, and nitrogenous neutralizer can easily for next batch both culturing microalgae provides nitrogenous source, the circulation closed can be realized between both culturing microalgae nutrient solution and exhaust gas denitration absorption liquid by a kind of like this pattern, thus " both culturing microalgae " and " exhaust gas denitration " are organically connected, not only can utilize micro-algae that nitrogen pollutant is changed into useful biomass expeditiously, and make " both culturing microalgae " and " exhaust gas denitration " become two relatively independent processes, avoid influencing each other of the two.In addition, nitrogenous neutralizer is used as the nutrient solution of cultivating microalgae in step (1), nitrite and/or the nitrate leaching process of conventional alkali absorb method can also be exempted, and then greatly save the energy consumption of exhaust gas denitration process.
In step of the present invention (1), the pH value >8 of algae liquid at the end of preferably relying on micro-algae metabolism to make cultivation, at the end of more preferably relying on micro-algae metabolism to make cultivation, the pH value of algae liquid is 9-11.Under above-mentioned preferable case, the nitric acid that the alkaline residue that step (1) can be made to obtain obtains with step (2) more expeditiously and/or nitrous acid contacts are obtained by reacting nitrogenous neutralizer.
In the present invention, in the nutrient solution of cultivating microalgae, in nitrogen-atoms, the content of nitrogenous compound is preferably 0.1-400mmol/L, is more preferably 5-50mmol/L, is further preferably 10-20mmol/L.
In the present invention, existing known micro-algae culture medium can be adopted to cultivate micro-algae, such as substratum BG11.
In the present invention, owing to there being algae slightly can not metabolism NO
2 -, therefore, the inventive method can be selected can the NO of metabolism simultaneously
3 -and NO
2 -micro-algae, also can before providing nitrogenous source with described nitrogenous neutralizer for microalga cultivation process, by the NO contained in nitrogenous neutralizer
2 -be converted into NO
3 -.Therefore, before the inventive method preferably includes the nutrient solution nitrogenous neutralizer being used as the middle cultivating microalgae of step (1), by the NO contained in nitrogenous neutralizer
2 -be converted into NO
3 -.The NO that the present invention both can adopt chemical process will to contain in nitrogenous neutralizer
2 -be converted into NO
3 -, also can adopt the NO that biological method will contain in this solution
2 -be converted into NO
3 -.Chemical process can adopt and comprise the oxygenant such as oxygen-containing gas, hydrogen peroxide by NO
2 -be oxidized to NO
3 -; Biological method comprises employing nitrifier by nitrification by NO
2 -be converted into NO
3 -.The present invention preferably by nitrifier by NO
2 -be converted into NO
3 -.
The kind of the present invention to micro-algae has no particular limits, as long as can the NO of metabolism simultaneously
3 -and NO
2 -, be preferably oil-producing microalgae, be more preferably the produce oil engineering microalgae with larger industrial utilization, such as, be preferably at least one in chlorella, single needle algae, grid algae and spirulina.
In the present invention, preferably can tolerate micro-algae of high alkali environment, cultivate this slightly algae can improve the pH value of alkaline residue further, and then to improve and the efficiency of nitric acid and/or nitrite reaction.Contriver through lot of experiments, filter out following can micro-algae of resistance to high alkali environment, as chlorella, single needle algae, grid algae or spirulina, this slightly algae can under pH is the environment of 9-11 healthy growth.
In the present invention, preferably can tolerate micro-algae of high nitrogen concentration environment, cultivate this slightly algae can improve the efficiency of cultivating microalgae process and exhaust gas denitration process simultaneously.Contriver is through lot of experiments, filter out following micro-algae that can tolerate high nitrogen concentration environment, as chlorella, single needle algae, grid algae or spirulina, above-mentioned micro-algae can grow fast in the solution of the NO3-N and NO2-N of more than nitrogen concentration 15mmol/L, and NO3-N and NO2-N metabolism is become the protein in frustule.
In the present invention, preferably those are not passing into CO
2when own metabolism can be relied on to improve rapidly micro-algae of algae liquid pH value, cultivate this slightly algae can improve the efficiency of cultivating microalgae process further.Contriver is through lot of experiments, filter out the following micro-algae can improving rapidly algae liquid pH value, as chlorella, single needle algae, grid algae or spirulina, the pH value of algae liquid can be brought up to 9-11 by above-mentioned micro-algae in 1-24 hour, made the requirement of algae hydroful foot efficient and nitric acid and/or nitrite reaction.
Therefore, in the present invention, micro-algae is preferably at least one in chlorella, single needle algae, grid algae and spirulina.
The flue gas of industrial discharge is except containing NO
xoutward, also other pollutents such as SO may be contained
x, those skilled in the art are tested (as by mensuration NO by simple
xthe reduction degree of specific absorption and the reduction degree of mensuration micro algae growth speed), just can confirm whether contain in waste gas or excessively contain the pollutent that integrated processes of the present invention is made a significant impact.Contriver finds, the SO in the flue gas of industrial discharge
xwhen content is higher, the SO of high density in nitrogenous neutralizer, can be contained
4 2-, and most of micro-algae is at the SO of high density
4 2-there is lower poor growth.As required, those skilled in the art also can pass through conventional known technique means, by the SO in waste gas
xbe reduced to the level that not remarkably influenced integrated processes of the present invention is implemented.The flue gas of general industry discharge, especially contains a large amount of SO in coal-fired flue-gas
x, therefore for these industrial smokes, need before exhaust gas denitration of the present invention, the SO contained
xremove.Therefore, in the present invention, the flue gas of industrial discharge (removes the SO in waste gas preferably past desulfurization process
x) industrial smoke.
Should be understood that, " both culturing microalgae " and " exhaust gas denitration " in the present invention is two relatively independent processes, containing CO
2the major function of gas be for micro algae growth provides carbon source.Therefore, in the present invention, containing CO
2gas (remove the SO in waste gas preferably past purifying treatment
xand NO
x) containing CO
2industrial smoke, or be not containing SO
xand NO
xindustrial smoke.
In the present invention, SO
xnamely the oxysulfide contained in industrial smoke is referred to, such as SO
2, SO
3deng.
In the present invention, both can adopt the mode of light autotrophy, also can adopt the mode cultivating microalgae of nutrition heterotrophism.When adopting the mode cultivating microalgae of light autotrophy, intensity of illumination is generally 1000-200000 lux.Light autotrophy is cultivated and is utilized free sunlight to produce valuable microalgae biomass, the alkaline residue simultaneously obtained and the NO absorbed in the flue gas of fixing industrial discharge
xthe nitric acid obtained and/or nitrite reaction obtain the nutrient solution that nitrogenous neutralizer is used as cultivating microalgae, significant.Utilize the cultivating microalgaes such as glucose to belong to mature technology, although cost is higher, efficiency is also higher.
The present invention has constructed a kind of exhaust gas emission reduction pollutent and the Mode of Circular producing micro-algae bioenergy.Utilize the NO in the flue gas of industrial discharge
xbe used as the nitrogenous source in nutrient solution, while pollutant emission reduction, obtain valuable microalgae biomass, microalgae biomass returns refinery can further processing biofuel by biorefinery.In the pattern of such recycling economy, administer the departmental cost of waste gas for cultivating micro-algae, thus counteract the departmental cost of cultivating microalgae.Factory decreases waste gas, discharge of wastewater and the pollution to environment, can produce again micro-algae bioenergy simultaneously, define closed circulation, and outlet only has clean fuel.
Embodiment
The present invention is further illustrated for following embodiment, but therefore do not limit the present invention.
Algae liquid optical density value (OD value) measures: optical density value spectrophotometric determination, compares with distilled water, measures the light absorption value of algae liquid at wavelength 680nm place, as the index of micro-concentration of algae.
The mensuration of nitrogen content in liquid:
Employing ICS3000 type ion chromatograph (Dionex company of the U.S.) measures the NO in the aqueous solution
3-content or NO
2 -content, instrument is furnished with EG40 leacheate automatic generator, electrical conductivity detector and chameleon chromatographic working station; IonPac AS11-HC type separator column (250mm × 4mm i.d.); IonPac AG11 type guard column (50mm × 4mm i.d.); Self suppressor of ASRS-ULTRA negatively charged ion.Leacheate: KOH solution; Flow velocity is 1mL/min; Eluent concentration: 30mmol/L; Sample size is 60 μ L; Column temperature is 30 DEG C; Suppress electric current 100mA; External standard method peak area quantification.
The mensuration of nitrogen content in simulated flue gas: adopt TESTO350 flue gas analyzing apparatus to measure the gas concentrations such as the oxynitride in simulated flue gas.
BG11 substratum: Media Components in Table 1-2, NaNO in BG11 substratum
3for nitrogenous source.
Table 1BG11 substratum
| Component | Content, mg/L |
| K 2HPO 4·3H 2O | 40 |
| NaNO 3 | 1500 |
| Na 2CO 3 | 20 |
| MgSO 4·7H 2O | 75 |
| CaCl 2·2H 2O | 36 |
| Citric acid | 6 |
| Ferric ammonium citrate | 6 |
| EDETATE SODIUM | 1 |
| Trace element A5 | 1 |
The micro-A5 of table 2
| Component | Composition, mg/L |
| H 3BO 3 | 2860 |
| MnCl 2·4H 2O | 1810 |
| ZnSO 4·7H 2O | 222 |
| CuSO 4·5H 2O | 79 |
| NaMoO 4·5H 2O | 390 |
| Co(NO 3) 2·6H 2O | 50 |
Embodiment 1
With BG11 culture medium culturing chlorella (being purchased from hydrobiont institute of the Chinese Academy of Sciences), in nitrogen-atoms, in BG11 substratum, the content of nitrogenous compound is 17.6mmol/L, and control temperature is between 20-30 DEG C, algae kind initial concentration OD
680be 0.5, pass into pressurized air and CO
2gas mixture carry out cultivating (CO
2concentration is at 2-5v%).Adopt natural daylight to cultivate in culturing process, daylight intensity reaches as high as 60000lux, by control CO
2intake controls algae liquid pH between 7-9, detects the OD value of algae liquid every day, and growth curve is shown in Fig. 2 example 1-1.Cultured continuously was gathered in the crops after 14 days, cultivated and terminated within first 1 day, to stop passing into CO
2gas, when terminating to cultivate, algae liquid pH is elevated to 9.8 naturally, and then, centrifugation obtains algae mud and alkalescence supports algae raffinate.
Simulated flue gas carries out NO in packing tower
xabsorb, the salpeter solution that concentration is 50% is housed in tower, at the bottom of tower, pass into packing tower after simulated flue gas is disperseed very well fill after part contacts with salpeter solution and flow out packing tower.NO in simulated flue gas
xconcentration is 800ppm, and oxygen concentration is 5%, and all the other are N
2, total gas couette is 1.5L/min, measures outlet NO
xconcentration is 160ppm, and denitration rate is 80%.After running for some time, in tower, concentration of nitric acid raises, and absorption liquid in tower is released 10%, and proceeds denitration operation after mending suitable quantity of water.
The acid solution of releasing and alkalescence are supported algae raffinate contact, control the amount of acid solution reaction is generated nitrogenous neutralizer that pH value is 7.Nitrogenous neutralizer is added the nutrient solution obtaining cultivating microalgae in the BG11 substratum in nonnitrogenous source, the consumption of nitrogenous neutralizer makes in the nutrient solution of the cultivating microalgae obtained, in nitrogen-atoms, the content of nitrogenous compound is 17.6mmol/L, for the cultivation of next batch chlorella, cultural method is the same, detects the OD value of algae liquid every day, and the growth curve of chlorella is shown in Fig. 2 example 1-2.
Embodiment 2
KNO is added in the BG11 substratum in nonnitrogenous source
3obtain the nutrient solution of cultivating microalgae, be used for cultivating grid algae (being purchased from hydrobiont institute of the Chinese Academy of Sciences), KNO
3add-on make in the nutrient solution of the cultivating microalgae obtained, in nitrogen-atoms, the content of nitrogenous compound is 10mmol/L, and control temperature is between 20-30 DEG C, and algae kind initial concentration OD is 0.5, passes into pressurized air and CO
2gas mixture carry out cultivating (CO
2concentration is at 2-5v%).Adopt natural daylight to cultivate in culturing process, daylight intensity reaches as high as 60000lux, by control CO
2intake controls algae liquid pH between 7-9, detects the OD value of algae liquid every day, and growth curve is shown in Fig. 3 example 2-1.Cultured continuously was gathered in the crops after 10 days, cultivated and terminated within first 2 days, to stop passing into CO
2gas, when terminating to cultivate, algae liquid pH is elevated to 9.1 naturally, and then, centrifugation obtains algae mud and alkalescence supports algae raffinate.
Simulated flue gas carries out NO in packing tower
xabsorb, the salpeter solution that concentration is 55% is housed in tower, at the bottom of tower, pass into packing tower after simulated flue gas is disperseed very well fill after part contacts with salpeter solution and flow out packing tower.NO in simulated flue gas
xconcentration is 500ppm, and oxygen concentration is 8%, and all the other are N
2, total gas couette is 1.5L/min, measures outlet NO
xconcentration is 125ppm, and denitration rate is 75%.After running for some time, in tower, concentration of nitric acid raises, and absorption liquid in tower is released 10%, and proceeds denitration operation after mending suitable quantity of water.
The acid solution of releasing and alkalescence are supported algae raffinate contact, control the amount of acid solution reaction is generated nitrogenous neutralizer that pH value is 7.3.Nitrogenous neutralizer is added the nutrient solution obtaining cultivating microalgae in the BG11 substratum in nonnitrogenous source, the consumption of nitrogenous neutralizer makes in the nutrient solution of the cultivating microalgae obtained, in nitrogen-atoms, the content of nitrogenous compound is 10mmol/L, for the cultivation of next batch grid algae, cultural method is the same, detects the OD value of algae liquid every day, and the growth curve of grid algae is shown in Fig. 3 example 2-2.
Embodiment 3
NaNO is added in the BG11 substratum in nonnitrogenous source
3and sodium bicarbonate, obtain the nutrient solution of cultivating microalgae, be used for cultivating single needle algae (being purchased from hydrobiont institute of the Chinese Academy of Sciences), the add-on of sodium bicarbonate makes the concentration of sodium bicarbonate in nutrient solution be 100mmol/L, NaNO
3add-on make in the nutrient solution of the cultivating microalgae obtained, in nitrogen, the content of nitrogenous compound is 20mmol/L, and control temperature is between 20-30 DEG C, algae kind initial concentration OD
680be 0.3, pass into pressurized air and CO
2gas mixture carry out cultivating (CO
2concentration is at 2-5v%).Adopt natural daylight to cultivate in culturing process, daylight intensity reaches as high as 60000lux, by control CO
2intake controls algae liquid pH between 7-9, detects the OD value of algae liquid every day, and growth curve is shown in Fig. 4 example 3-1.Cultured continuously was gathered in the crops after 12 days, cultivated and terminated within first 3 days, to stop passing into CO
2gas, when terminating to cultivate, algae liquid pH is elevated to 10.5 naturally, and then, centrifugation obtains algae mud and alkalescence supports algae raffinate.
Simulated flue gas carries out NO in packing tower
xabsorb, the salpeter solution that concentration is 53% is housed in tower, at the bottom of tower, pass into packing tower after simulated flue gas is disperseed very well fill after part contacts with salpeter solution and flow out packing tower.NO in simulated flue gas
xconcentration is 600ppm, and oxygen concentration is 7%, and all the other are N
2, total gas couette is 1.5L/min, measures outlet NO
xconcentration is 120ppm, and denitration rate is 80%.After running for some time, in tower, concentration of nitric acid raises, and absorption liquid in tower is released 10%, and proceeds denitration operation after mending suitable quantity of water.
The acid solution of releasing and alkalescence are supported algae raffinate contact, control the amount of acid solution reaction is generated nitrogenous neutralizer that pH value is 8.0.Nitrogenous neutralizer is added the nutrient solution obtaining cultivating microalgae in the BG11 substratum in nonnitrogenous source, the consumption of nitrogenous neutralizer makes in the nutrient solution of the cultivating microalgae obtained, in nitrogen-atoms, the content of nitrogenous compound is 20mmol/L, for the cultivation of next batch single needle algae, cultural method is the same, detects the OD value of algae liquid every day, and the growth curve of single needle algae is shown in Fig. 4 example 3-2.
As can be seen from Fig. 2-4, adopt method of the present invention, both can NO in effective elimination waste gas
x, can utilize again and absorb NO
xafter acid absorption liquid and alkalescence support algae raffinate and react the nitrogenous neutralizer generated and provide nitrogenous source for microalga cultivation process, carry out normally cultivating fast to micro-algae.
" both culturing microalgae " and " exhaust gas denitration " can reasonably combine by the inventive method, can either utilize the NO in waste gas
xmake micro-algae normal growth, again can NO in effective elimination waste gas
x, influencing each other of " both culturing microalgae " and " exhaust gas denitration " can also be avoided, make two processes all can stablize, run reliably.
Below the preferred embodiment of the present invention is described in detail by reference to the accompanying drawings; but; the present invention is not limited to the detail in above-mentioned embodiment; within the scope of technical conceive of the present invention; can carry out multiple simple variant to technical scheme of the present invention, these simple variant all belong to protection scope of the present invention.
It should be noted that in addition, each concrete technical characteristic described in above-mentioned embodiment, in reconcilable situation, can be combined by any suitable mode, in order to avoid unnecessary repetition, the present invention illustrates no longer separately to various possible array mode.
In addition, also can carry out arbitrary combination between various different embodiment of the present invention, as long as it is without prejudice to thought of the present invention, it should be considered as content disclosed in this invention equally.
Claims (14)
1. an integrated processes for both culturing microalgae and exhaust gas denitration, the method comprises:
(1) at least with containing CO
2gas provide part carbon source for microalga cultivation process; Algae liquid at the end of relying on micro-algae metabolism to make cultivation is in alkalescence; From the algae liquid of results, isolate micro-algae, obtain micro-algae and alkaline residue;
(2) by the NO in the flue gas of industrial discharge
xbe converted into nitric acid and/or nitrous acid;
(3) nitric acid that alkaline residue step (1) obtained and step (2) obtain and/or nitrous acid contacts, obtain nitrogenous neutralizer, with described nitrogenous neutralizer for microalga cultivation process provides nitrogenous source.
2. method according to claim 1, wherein, the algae liquid at the end of relying on micro-algae metabolism to make cultivation comprises in the method for alkalescence: make in micro algae culturing liquid containing at least one in base metal nitrate, alkali metal nitrites salts, alkaline carbonate, alkali metal hydrocarbonate, alkali metal phosphate, alkali metal hydrogen phosphate.
3. method according to claim 2, wherein, described basic metal is sodium or potassium.
4., according to the method in claim 1-3 described in any one, wherein, in microalga cultivation process, the pH value regulating algae liquid is 7-11.
5. according to the method in claim 1-3 described in any one, wherein, in step (1), the pH value >8 of algae liquid at the end of relying on micro-algae metabolism to make cultivation.
6. method according to claim 5, wherein, in step (1), at the end of relying on micro-algae metabolism to make cultivation, the pH value of algae liquid is 9-11.
7., according to the method in claim 1-3 described in any one, wherein, in the nutrient solution of cultivating microalgae, in nitrogen-atoms, the content of nitrogenous compound is 0.1-400mmol/L.
8. method according to claim 7, wherein, in the nutrient solution of cultivating microalgae, in nitrogen-atoms, the content of nitrogenous compound is 5-50mmol/L.
9. according to the method in claim 1-3 described in any one, wherein, described micro-algae is at least one in chlorella, single needle algae, grid algae and spirulina.
10. according to the method in claim 1-3 described in any one, wherein, the flue gas of described industrial discharge is the industrial smoke through desulfurization process.
11. according to the method in claim 1-3 described in any one, wherein, described containing CO
2gas be through purifying treatment containing CO
2industrial smoke, or be not containing SO
xand NO
xindustrial smoke.
12. according to the method in claim 1-3 described in any one, and wherein, in step (1), adopt the mode cultivating microalgae of light autotrophy, intensity of illumination is 1000-200000 lux.
13. according to the method in claim 1-3 described in any one, wherein, in step (1), adopts the mode cultivating microalgae of nutrition heterotrophism.
14. according to the method in claim 1-3 described in any one, wherein, with described nitrogenous neutralizer for before microalga cultivation process provides nitrogenous source, also comprises the NO will contained in described nitrogenous neutralizer
2 -be converted into NO
3 -step.
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