CN107488680A - A kind of method that biological methane gas is prepared with carbon raw material - Google Patents
A kind of method that biological methane gas is prepared with carbon raw material Download PDFInfo
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- C12P5/00—Preparation of hydrocarbons or halogenated hydrocarbons
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- C12P—FERMENTATION OR ENZYME-USING PROCESSES TO SYNTHESISE A DESIRED CHEMICAL COMPOUND OR COMPOSITION OR TO SEPARATE OPTICAL ISOMERS FROM A RACEMIC MIXTURE
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- C12P19/00—Preparation of compounds containing saccharide radicals
- C12P19/14—Preparation of compounds containing saccharide radicals produced by the action of a carbohydrase (EC 3.2.x), e.g. by alpha-amylase, e.g. by cellulase, hemicellulase
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Abstract
The present invention discloses a kind of method that biological methane gas is prepared with carbon raw material, this method utilizes sodium hydroxide/Urea treatment after crushing low-order coal such as peat, biomass, the processing of adding liquid cellulase, anaerobe fermentation generation methane is added, determines the content of methane in institute's aerogenesis body up to 50 68%.This method has simple and practical, the advantages that reagent price is cheap, reaction condition is gentle, process green non-pollution, suitable industrialized production are amplified, organic matter degradable in carbon raw material can be made to gas clean fuel biological methane or even hydrogen, platform chemicals, open peat, the new way of biomass such as agricultural crop straw, forestry processing waste comprehensive utilization of rich reserves.
Description
Technical field
The invention belongs to low-order coal, biomass as resources application field, is related to peat, the side of biomass production green energy resource
A kind of method, and in particular to method that biological methane gas is prepared with carbon raw material.
Background technology
Peat (also known as mud coal, turf, Peat), be plant residue under high humidity anaerobic environment and microbial action, do not divide
The organic matter for the tiering that solution part (chemical composition is cellulose, hemicellulose, lignin) is formed by long term accumulation
Ore body, it is minimus coal.Peat is formed through biodegradation under anoxic conditions into charcoal plant, peat is through diagenesis shape
Into lignite, it is transformed into bituminous coal until anthracite when temperature and pressure gradually increases, then through metamorphism.Peat main component is to have
Machine matter (average 53%) and humic acid (average 36%), fiber content enriches, loose porous, with more hole and huge
Internal surface area, adsorption moisture ability is strong, at present mainly as horticulture ground substance and organic fertilizer, Germany, Finland, Canada, Sweden,
The countries such as China are widely used in the fields such as flower gardening, proportion of crop planting, soil improvement, without performance resource valency to greatest extent
Value.It is a kind of waste that peat only is used for into horticulture ground substance and organic fertilizer, and peat should be positioned as to a kind of raw material, improve its economic valency
Value.
Into charcoal plant remains in the presence of microorganism, decompose, synthesize, assembling and be changed into peat, only having carried out one
Determine the decomposition of degree, contain a large amount of undecomposed plant roots, stem, the residuums of leaf in peat.Undressed peat is difficult to micro-
Biodegradation, during a large amount of peat trans-utilizations, pretreatment is indispensable step.Sambhunath Ghosh research hairs
Existing peat samples alkali (3% sodium hydroxide solution) or sour (8% hydrochloric acid solution) are located under 132 DEG C and 0.19MPa in a kettle
70min is managed, anaerobic digestion ability can be promoted.Forsberg etc. studies Steam explosion treatment peat, it is found that peat includes up to
31% hemicellulose and 25% cellulose, can be as a kind of carbohydrate source of microbial fermentation, by peat samples
Discharge, as a result show, the carbohydrate dissolved during steam explosion is with temperature after maintaining 5min Steam explosion treatments at 170 DEG C
Spend the growth with processing time and improve, the free sugar amount of steam blasting release also increases;Steam blasting causes up to 28%
Peat is discharged in the form of solable matter, wherein about 33% carbohydrate is free monose and disaccharide such as glucose, half
Lactose, xylose, cellobiose, 24% it is cellulose in steam explosion processing residue, it is impossible to as Bacteroides succinogenes
Bacteroides succinogenes or Clostridium thermocellum Clostridium thermocellum carbon source, disclose steam explosion and locate in advance
Comprehend and discharge fermentation inhibitor.The mechanochemistry conversion of the research liver moss high located peat water-soluble polysaccharide such as Vyacheslav Ivanov, 3%
In the presence of NaOH, high-order eriophorum peat is handled with star crushing mill, the composition of polysaccharide yield 1.6%, wherein polysaccharide is grape
Sugar, galactolipin, xylose, arabinose and fructose.
Because the essence of formtion of peat is exactly effective accumulation of plant organism and suppresses to decompose, the life of peat how is improved
Biodegradable, the biomethanation conversion for realizing its high methane yield are the general character of the mud and charcoal high level conversion of urgent need to resolve
Problem.
Existing patent (200910035462.6) discloses the new method for improving anaerobic gas generation property of wood fiber raw material, will
Mixed after lignocellulose raw material chopping with turf in ratio of the dry than 9: 11~3: 1, mixture is subjected to anaerobic fermentation production
Biogas.It is 1 that Zhang Xuecai etc., which reports peat and the proportioning of pig manure,:1 or 1:2 can produce containing methane under conditions of strictly anaerobic
65% or so biogas.(Zhang Xuecai, research [J] the coal gas and heating power of high wind coloured silk Generation of Marsh Gas from Peat, 2000,20 (1):3-5),
The former is that peat mixes with lignocellulose raw material, and the latter is that peat mixes with pig manure, all not individually using peat as raw material anaerobism
Ferment preparation of sludge gas, and realize the comprehensive utilization and multi-product conversion of peat.Therefore, for the reaction of peat raw material anaerobic fermentation
Feature improves the added value of peat, it is necessary to study the problem that corresponding method solves peat Degradation and Transformation.
Sodium hydroxide/urea dicyandiamide solution is applied to as a kind of more economical and environment amenable cellulose solvent
Cellulose dissolution, for the cellulose solution of stable performance to be made or prepares cellulose ether compound.Cellulose can dissolve quickly
In the urea dicyandiamide solution of -12 DEG C of 7% sodium hydroxides/12%.Regenerated fiber is successfully made by this dicyandiamide solution
Plain film, regenerated cellulose and the multifunctional fibre cellulosic material with improved performance.But sodium hydroxide/urea is used for mud
The fermented pretreatment of the low-order coals such as charcoal, the biomass such as carbon raw material such as agricultural crop straw maize straw, feces of livestock and poultry such as cow dung, mesh
Before there is no correlative study to report.Sodium hydroxide/urea mixed solution system forms stable hydrogen bond network bag by urea small molecule
The free cellulose macromolecule such as peat, stalk, cow dung is wrapped up in, is allowed to be combined with each other, so that sodium hydroxide is constantly opened
Between cellulosic molecule, intramolecular hydrogen bond, obtain more free-fiber element molecules, make free-fiber plain by adding cellulase
Molecule is degraded to glucose, for the production of the green energy resources such as biological methane, hydrogen or chemicals, passes through sodium hydroxide/urine
Element coupling cellulase pretreatment improves the biodegradability of peat, to realize the carbon raw materials such as peat, biomass low cost
High efficiency converts green energy resource biological methane and hydrogen lays the foundation.
The content of the invention
In order to overcome the biodegradability for how improving peat in the prior art, the biological first of its high methane yield is realized
Alkanisation is converted, while solves the problem of peat Degradation and Transformation, and biological methane gas is prepared with carbon raw material the invention provides one kind
The method of body, this method add anaerobism using sodium hydroxide/urea mixed solution, liquid cellulase processing peat, biomass
Activated sludge ferments as anaerobe source produces methane, can be gas by organic matter transformation degradable in carbon raw material
Clean fuel biological methane or even hydrogen, chemicals, reagent price is cheap, reaction condition is gentle, process green non-pollution, be adapted to
The advantages that industrialized production is amplified.
The technical solution adopted for the present invention to solve the technical problems is:
A kind of method that biological methane gas is prepared with carbon raw material, comprises the following steps:
1) sodium hydroxide solution and urea liquid are prepared respectively, and two kinds of solution are uniformly mixed afterwards, are prepared
Sodium hydroxide/urea mixed solution, stand;Cellulose macromolecule and sodium hydroxide in peat, biomass may carry out two kinds instead
Should, product is [C6H7O2(OH)3·NaOH]N[C6H7O2(OH)2ONa]N, between the two can mutual inversion of phases, cause in fibre
Between tieing up plain crystal region, or even also it is swelled inside cellulose crystallite area, causes cellulose dissolution, sodium hydroxide can be with
Peat fibre element intermolecular hydrogen bonding is destroyed, urea can be promoted fine in the presence of sodium hydroxide with hydrogen bond in saboteur
Tie up the dissolving of element, with the dissolving of cellulose in peat, biomass, the poly formed by cellulose, hemicellulose and lignin
Depolymerization, hemicellulose degradation, reduced sugar release occur for body.Stand, it is therefore an objective to be sufficiently mixed sodium hydroxide and urea.
2) carbon raw material added into step 1) after crushing, shake, stand, adjust pH, preheating.
3) sodium citrate buffer solution and liquid cellulase are sequentially added into step 2), is stirred, adds anaerobism activity
Sludge, anaerobic fermentation, you can methane gas is prepared.Cellulase refers to energy hydrocellulose β -1,4- glucoside bonds
Enzyme, it can make cellulose be changed into the reduced sugars such as cellobiose, glucose, have liquid cellulase and solid fine in the industrial production
Tie up plain two kinds of products of enzyme.Solid cellulase is to be produced on the basis of liquid cellulase by drying process with atomizing, more
One of process, thus price will costliness compared to liquid cellulase.In the present invention by add liquid cellulase make it is molten
Solution is degraded to glucose in the cellulosic molecule of sodium hydroxide/urea mixed solution.
Efficient, the stable operation of anaerobic fermentation generation methane system depend on anaerobic activated sludge, anaerobic activated sludge
Come from the activated sludge of secondary sedimentation tank of sewage treatment work, through anaerobic acclimation, rich in carbohydrate breakdown bacterium, acid-producing bacteria, production first
The microorganism species of alkane bacterium, each microorganism constitute micro- life of the syntrophism symbiosis of complexity by direct or indirect nutrition relationship
Thing flora, by adding anaerobic activated sludge in the present invention, microorganism species in anaerobic activated sludge are utilized to complete to decompose, production
Acid, methane phase process, make in the case where liquid cellulase acts on, be dissolved in the cellulosic molecule quilt of sodium hydroxide/urea mixed solution
Degraded obtains glucose (one kind of reduced sugar), and then in the case where anaerobe acts on, glucose is converted into biological methane gas.
Preferably, in step 1), sodium hydroxide solution mass percent concentration is 5-9%, urea solution mass percentage
Concentration is 10-14%, and the volume ratio of sodium hydroxide solution and urea liquid is (30 in sodium hydroxide/urea mixed solution:70)-
(50:50), within this range, cellulose discharges from the parcel of lignin, glycosidic bond fracture, discharges reduced sugar, measure is also
Raw sugar yield reaches highest, and highest yield is 7.698%.
Preferably, in step 1), the time that sodium hydroxide/urea mixed solution is stood is 1.5-3h, and the temperature of standing is 4-
20℃。
Preferably, in step 2), described carbon raw material is one kind in peat or biomass, per the carbon containing originals of 0.5-1.5g
0.5-1.5mL sodium hydroxides/urea mixed solution is added in material, concussion uses whirlpool mixed instrument, and the time of concussion is 2-10min,
20-30min is stood after concussion, the pH to 4.6-5.0 of hydrochloric acid solution regulation solution is added, is put into constant temperature water bath and is preheated to
40-60℃.Subsequent liquid cellulase play a role cellulose is thoroughly degraded to glucose optimum pH be 4.8, add
Hydrochloric acid solution adjusts the pH to 4.8 of solution, is put into constant temperature water bath pH value when being preheated to 40-60 DEG C and fluctuation occurs, subsequently
The pH in system is finely adjusted by adding sodium citrate buffer solution, stabilized it 4.8 so that cellulase plays maximum
Effect.
Preferably, described peat is one or more combinations in meadow peat, woody peat, moss peat.
Preferably, described biomass is the combination of one or both of agricultural crop straw, feces of livestock and poultry.
Preferably, the agricultural crop straw be maize straw, corncob, wheat stalk, rice straw, sunflower straw,
One or more combinations in cotton stalk, rape stalk.
Preferably, in step 3), the pH of described sodium citrate buffer solution is 4.6-5.0, per 0.5-1.5g carbon raw materials
The addition of middle sodium citrate buffer solution is 8-12mL;The addition of liquid cellulase is in per 0.5-1.5g carbon raw materials
0.1-0.3mL;The addition of described anaerobic activated sludge is 0.3-0.6 times of fermentation system volume;The time of stirring is 12-
36h.Liquid cellulase catalytic cellulose molecule be degraded to glucose, it is necessary to buffer solution maintenance system pH 4.8 condition
Lower progress, but buffer solution addition influences the volume of fermentation system, and then influence concentration of the glucose in fermentation system, experiment
Under conditions of the addition that data are shown in sodium citrate buffer solution in every 0.5-1.5g carbon raw materials is 8-12mL, it can play
Buffer solution buffer pH acts on, and does not produce impact to subsequent fermentation, reduces generation methane tolerance.And cellulase price is held high
It is expensive, it is contemplated that cost control, it is 0.1-0.3mL to control per the addition of liquid cellulase in 0.5-1.5g carbon raw materials, is
Cellulose is set to be degraded to the lowest dose level of glucose as far as possible.Within this range, cellulosic molecule glycosidic bond is broken, and discharges Portugal
Grape sugar (one kind of reduced sugar), measure Reducing sugar reach highest, and highest yield is 20.325%.Described anaerobism activity is dirty
Mud is the flora source of anaerobic fermentation generation methane, and equivalent to strain, addition is 0.3-0.6 times of fermentation system volume,
It can shorten fermentation period on the premise of gas production is ensured.The purpose of stirring is before anaerobic activated sludge is added, and passes through machinery
Stirring or magnetic agitation, promote cellulase that attachment and enzymolysis occurs with the cellulosic molecule in carbon raw material, improve cellulose
Molecular degradation is the yield of glucose, is at most stirred 36 hours, and cellulase hydrolysis is completed for sugar effect.
Preferably, in step 3), the time of described anaerobic fermentation is 30-40d, and fermentation temperature is 45-55 DEG C.In order to carry
The yield of high carbon raw material generation methane gas, carbon raw material is set to be converted into sugar as far as possible, sugar is converted into acid, and acid is converted into biology
Methane gas, time of anaerobic fermentation is most long to need 40d, and temperature is to regulate and control fermentative microflora, strengthen the important means of aerogenesis, anaerobism
Temperature needs to control at 28-35 DEG C or 45-55 DEG C in generation methane technology control parameter of fermenting, because temperature is higher, reaction
Speed is faster, considers that temperature maintains cost and gas production, fermentation temperature is defined as 45-55 DEG C by us.
It is an advantage of the invention that:
1) peat classified utilization, the main component of peat is organic matter and humic acid, by the cellulose in organic substance of peat
The green energy resources such as biological methane are converted into, undegradable hemicellulose, lignin and the humic acid of difficult degradation can subsequently prepare height
The products such as humic acid organic fertilizer material, make the polynary conversion of mud and charcoal high level, meet the industrial policy and energy policy of country, favorably
In Revising Products Structure For Enterprises, expand product category;
2) sodium hydroxide of the carbon raw material such as peat, biomass/urea coupled enzymatic processing method has simple and practical, examination
The advantages that agent is cheap, reaction condition is gentle, process green non-pollution, suitable industrialized production are amplified, can be by carbon raw material
In degradable organic matter gas clean fuel biological methane, hydrogen, chemicals is made, to the low-carbon of mud and charcoal using having
Important meaning.
Embodiment
The present invention is further illustrated below:
Embodiment 1
By the sodium hydroxide solution that mass percent concentration is 7%, the urea liquid that mass percent concentration is 12% is pressed
It is 30 according to volume ratio:70 mixing, sodium hydroxide/urea mixed solution stand 1.5h at 20 DEG C, take 40mL sodium hydroxides/urea to mix
Liquid is closed, addition is crushed to 150 mesh meadow peat 40g, stands 20min after whirlpool mixed instrument concussion 6min, determine Reducing sugar
For 6.432%, it is 4.8 to add hydrochloric acid solution regulation pH, is put into constant temperature water bath and is preheated to 50 DEG C, adds 400mL pH 4.8
Sodium citrate buffer solution, liquid cellulase 8mL is added, then magnetic agitation 12h, measure Reducing sugar is
17.055%, anaerobic activated sludge 220mL, material anaerobic fermentation residence time 35d are added, fermentation temperature is 50 DEG C, draining collection
Gas method collects biological methane gas, and fermentation group average aerogenesis 379mL, HPLC determine CH in biological methane gas4Content is 69%.
Embodiment 2
By the sodium hydroxide solution that mass percent concentration is 5%, the urea liquid that mass percent concentration is 10% is pressed
It is 40 according to volume ratio:60 mixing, sodium hydroxide/urea mixed solution stand 3h at 10 DEG C, take 220mL sodium hydroxides/urea to mix
Liquid is closed, addition is crushed to 150 mesh woody peat 110g, stands 30min after whirlpool mixed instrument concussion 4min, determine Reducing sugar
For 6.798%, it is 4.6 to add hydrochloric acid solution regulation pH, is put into constant temperature water bath and is preheated to 40 DEG C, adds 880mL pH 5.0
Sodium citrate buffer solution, liquid cellulase 20mL is added, then magnetic agitation 24h, measure Reducing sugar is
16.566%, anaerobic activated sludge 330mL, material anaerobic fermentation residence time 40d are added, fermentation temperature is 52 DEG C, draining collection
Gas method collects biological methane gas, and fermentation group average aerogenesis 380mL, HPLC determine CH in biological methane gas4Content is 66%.
Embodiment 3
By the sodium hydroxide solution that mass percent concentration is 9%, the urea liquid that mass percent concentration is 14% is pressed
It is 50 according to volume ratio:50 mixing, sodium hydroxide/urea mixed solution stand 2.5h at 4 DEG C, take 40mL sodium hydroxides/urea to mix
Liquid is closed, addition is crushed to 60 mesh moss peat 20g, 25min is stood after whirlpool mixed instrument concussion 8min, and measure Reducing sugar is
7.201%, it is 4.8 to add hydrochloric acid solution regulation pH, is put into constant temperature water bath and is preheated to 60 DEG C, adds the lemons of 220mL pH 4.8
Lemon acid sodium buffer solution, adds liquid cellulase 6mL, then magnetic agitation 36h, and measure Reducing sugar is 18.754%,
Anaerobic activated sludge 130mL, material anaerobic fermentation residence time 32d are added, fermentation temperature is 55 DEG C, and draining water gathering of gas law collects life
Thing methane gas, fermentation group average aerogenesis 361mL, HPLC determine CH in biological methane gas4Content is 63%.
Finally it should be noted that:Obviously, above-described embodiment is only intended to clearly illustrate example of the present invention, and simultaneously
The non-restriction to embodiment.For those of ordinary skill in the field, can also do on the basis of the above description
Go out other various forms of changes or variation.There is no necessity and possibility to exhaust all the enbodiments.And thus drawn
Among the obvious changes or variations that Shen goes out is still in protection scope of the present invention.
Claims (9)
- A kind of 1. method that biological methane gas is prepared with carbon raw material, it is characterised in that described method comprises the following steps:1) sodium hydroxide solution and urea liquid are prepared respectively, and two kinds of solution are uniformly mixed afterwards, hydrogen-oxygen is prepared Change sodium/urea mixed solution, stand;2) carbon raw material added into step 1) after crushing, shake, stand, adjust pH, preheating;3) sodium citrate buffer solution and liquid cellulase are sequentially added into step 2), stirs, adds anaerobic activated sludge, Anaerobic fermentation, you can methane gas is prepared.
- A kind of 2. method that biological methane gas is prepared with carbon raw material as claimed in claim 1, it is characterised in that step 1) In, sodium hydroxide solution mass percent concentration is 5-9%, and urea solution mass percent concentration is 10-14%, hydroxide The volume ratio of sodium hydroxide solution and urea liquid is (30 in sodium/urea mixed solution:70)-(50:50).
- A kind of 3. method that biological methane gas is prepared with carbon raw material as claimed in claim 1, it is characterised in that step 1) In, the time that sodium hydroxide/urea mixed solution is stood is 1.5-3h, and the temperature of standing is 4-20 DEG C.
- A kind of 4. method that biological methane gas is prepared with carbon raw material as claimed in claim 1, it is characterised in that step 2) In, described carbon raw material is one kind in peat or biomass, and 0.5-1.5mL hydrogen-oxygens are added in every 0.5-1.5g carbon raw materials Change sodium/urea mixed solution, concussion uses whirlpool mixed instrument, and the time of concussion is 2-10min, stands 20-30min after concussion, adds Enter the pH to 4.6-5.0 of hydrochloric acid solution regulation solution, be put into constant temperature water bath and be preheated to 40-60 DEG C.
- 5. a kind of method that biological methane gas is prepared with carbon raw material as claimed in claim 4, it is characterised in that described Peat is one or more combinations in meadow peat, woody peat, moss peat.
- 6. a kind of method that biological methane gas is prepared with carbon raw material as claimed in claim 4, it is characterised in that described Biomass is the combination of one or both of agricultural crop straw, feces of livestock and poultry.
- A kind of 7. method that biological methane gas is prepared with carbon raw material as claimed in claim 6, it is characterised in that the agriculture Crop material is in maize straw, corncob, wheat stalk, rice straw, sunflower straw, cotton stalk, rape stalk One or more combination.
- A kind of 8. method that biological methane gas is prepared with carbon raw material as claimed in claim 1, it is characterised in that step 3) In, the pH of described sodium citrate buffer solution is 4.6-5.0, the addition of sodium citrate buffer solution in every 0.5-1.5g carbon raw materials Measure as 8-12mL;The addition of liquid cellulase is 0.1-0.3mL in per 0.5-1.5g carbon raw materials;Described anaerobism activity The addition of sludge is 0.3-0.6 times of fermentation system volume;The time of stirring is 12-36h.
- A kind of 9. method that biological methane gas is prepared with carbon raw material as claimed in claim 1, it is characterised in that step 3) In, the time of described anaerobic fermentation is 30-40d, and fermentation temperature is 45-55 DEG C.
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CN108018319A (en) * | 2018-02-05 | 2018-05-11 | 内蒙古科技大学 | A kind of method of alkali process coupling microorganism conversion lignite production bio-fuel |
CN108998477A (en) * | 2018-07-20 | 2018-12-14 | 湖南和滨特种水产养殖有限公司 | A kind of kind of cultivation scrap concrete and the method utilized |
CN113527007A (en) * | 2021-08-05 | 2021-10-22 | 河北工程大学 | Saline-alkali soil improver modified by lignite and preparation method thereof |
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