CN107460211A - A kind of method for improving biological methane yield using hydrogen peroxide pretreatment coal - Google Patents

A kind of method for improving biological methane yield using hydrogen peroxide pretreatment coal Download PDF

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Publication number
CN107460211A
CN107460211A CN201710740239.6A CN201710740239A CN107460211A CN 107460211 A CN107460211 A CN 107460211A CN 201710740239 A CN201710740239 A CN 201710740239A CN 107460211 A CN107460211 A CN 107460211A
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coal
hydrogen peroxide
methane yield
biological methane
methane
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郭红光
韩青
梁卫国
张金龙
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Taiyuan University of Technology
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Taiyuan University of Technology
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    • C—CHEMISTRY; METALLURGY
    • C12—BIOCHEMISTRY; BEER; SPIRITS; WINE; VINEGAR; MICROBIOLOGY; ENZYMOLOGY; MUTATION OR GENETIC ENGINEERING
    • C12P—FERMENTATION OR ENZYME-USING PROCESSES TO SYNTHESISE A DESIRED CHEMICAL COMPOUND OR COMPOSITION OR TO SEPARATE OPTICAL ISOMERS FROM A RACEMIC MIXTURE
    • C12P5/00—Preparation of hydrocarbons or halogenated hydrocarbons
    • C12P5/02—Preparation of hydrocarbons or halogenated hydrocarbons acyclic
    • C12P5/023—Methane
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E50/00—Technologies for the production of fuel of non-fossil origin
    • Y02E50/30—Fuel from waste, e.g. synthetic alcohol or diesel

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Abstract

The invention discloses a kind of method for improving biological methane yield using hydrogen peroxide pretreatment coal, coal is pre-processed using hydrogen peroxide first, then adds microorganism fungus kind, realizes the process of biodegradable coal methane phase；In preprocessing process, the concentration of hydrogen peroxide is 5% ~ 30%, and processing time is 8 ~ 16 h.Using the inventive method, after being pre-processed to coal, by the oxidisability of pretreating agent, the degree of oxidation of coal is improved, and then improves the biological effectiveness of coal, effectively increases the yield of coal biological methane；When using hydrogen peroxide as pretreating agent, hydrogen peroxide has extremely strong oxidisability in itself, while final product is water after oxidation, has green characteristic.

Description

A kind of method for improving biological methane yield using hydrogen peroxide pretreatment coal
Technical field
The present invention relates to it is a kind of using hydrogen peroxide pretreatment coal improve biological methane yield method, belong to coal gasification, Improve the field of methane production.
Background technology
Compared in general larger molecular organicses, the molecular structure of coal is more complicated.Therefore, microorganism is difficult directly to act on In the macromolecular structure of coal, biological effectiveness is seriously reduced, directly affects the generation efficiency of biological methane.How coal knot is improved Structure, increase its biological effectiveness, it is extremely important to the biogasification process of coal so as to improve the yield of biological methane.Pre-process skill Art is handled coal with chemical method and physical method etc., changes the property of coal in itself, so as to improve the life of coal in itself Thing validity, increase its biological transformation ratio.Hydrogen peroxide has extraordinary oxidisability, can realize macromolecular by oxidation The fracture of part chemical bond in compound.And primary product of the hydrogen peroxide after redox reaction occurs is water, environmentally friendly valency Value is high.In addition, hydrogen peroxide can decompose under field conditions (factors), the place of remnant chemical reagents after pretreatment is efficiently solved Put problem.
The content of the invention
The present invention is intended to provide a kind of method for improving biological methane yield using hydrogen peroxide pretreatment coal, utilizes peroxide Change hydrogen pretreatment coal to strengthen the biological effectiveness of coal, improve biological methane yield.
The invention provides a kind of method for improving biological methane yield using hydrogen peroxide pretreatment coal, in biodegradation Before, the biological effectiveness of coal is strengthened by the preprocess method of hydrogen peroxide oxidation coal, improves the production of coal inverting biological methane Amount.
In the above method, hydrogen peroxide pretreatment is carried out before microorganism fungus kind is added, peroxidating in processing procedure The mass concentration of hydrogen is 5% ~ 30%, and processing time is 8 ~ 16 h.
In the above method, solid coal that feed coal obtains after hydrogen peroxide pre-processes, for producing biological methane.
The above method specifically includes following steps：
（1）Coal into powder and is sieved by crushing mechanism, the particle size range after coal sieving is 0.15 ~ 0.25 mm；
（2）Coal dust is mixed with hydrogen peroxide, 8 ~ 16 h are stirred at room temperature by magnetic stirring apparatus；
The ratio of coal dust and hydrogenperoxide steam generator is：4 ~ 5ml hydrogenperoxide steam generator is used per g coal dusts；Magnetic stirring apparatus Mixing speed is 600 ~ 800 rpm；
（3）By step（2）Gained mixed solution carries out separation of solid and liquid, obtains solid coal, obtains after being used for after solid coal drying Continuous biodegradable methane phase process；
In the step, separation of solid and liquid is realized by the method for being stored at room temperature or being filtered by vacuum；
（4）With step（1）Gained coal is substrate, under conditions of nutritional ingredient is provided, screened from coal bed gas product water or coal, The functional flora of enrichment degraded coal methane phase, including cellulose-degrading bacteria, aromatic compound degradation bacteria, methanogen etc..Institute Stating nutritional ingredient includes microorganism, especially the nutriment needed for methanogen growth in addition to carbon source, including basal nutrient, Trace element, vitamin etc..
（5）With step（3）Drying gained solid coal is substrate, utilizes step（4）The functional flora that enrichment obtains realizes life Thing degraded coal methane phase process, while in incubation, gas chromatographic detection methane production was utilized every 3-7 days.
The coal used in the present invention is the larger coal of the biodegradable difficulty such as anthracite, bituminous coal.
In the above method, step（3）The method of being stored at room temperature is specially：24h is stood under room temperature environment, makes to remain Hydrogen oxide consumes through autoxidation, while realizes that solid and liquid are sufficiently separated, and supernatant is removed, residual coal is dried.
In the above method, step（3）The vacuum filtration method is specially：Use Vacuum filtration device and supporting 0.22 μm filter membrane is filtered to mixed solution, and repeatedly washing is carried out to coal sample using distilled water in filter process was remained with removing Hydrogen oxide, residual coal is taken to be dried after washing.
The larger coal of the biodegradable difficulty such as anthracite, bituminous coal is employed herein, because anthracite, bituminous coal belong to The coal of high degree of metamorphism, it is more difficult to it is degraded by microorganisms, so, after being pre-processed by the inventive method to coal, by locating in advance The oxidisability of agent is managed, the degree of oxidation of coal is improved, enhances its biological effectiveness, and then improve biological methane yield.
Beneficial effects of the present invention：
（1）Using hydrogen peroxide to Coal pretreatment after, improve the biological effectiveness of coal, effectively increase coal biological methane Yield；
（2）When using hydrogen peroxide as pretreating agent, hydrogen peroxide has extremely strong oxidisability in itself, while in oxidation Final product is water afterwards, is easily separated with coal, has green characteristic.
Brief description of the drawings
Fig. 1 is coal biological methane yield versus time curve in embodiment 1 and comparative example 1；
Fig. 2 is coal biological methane yield versus time curve in embodiment 2 and comparative example 2.
Embodiment
The present invention is further illustrated below by embodiment, but is not limited to following examples.
Embodiment 1：
The hydrogen peroxide that mass concentration is 30% pre-processes the h of anthracite 8,12 h and 16 h, comprises the following steps：
The first step, after Qinshui basin target coal seam obtains anthracite coal sample, coal sample is crushed, sieved, choosing particle diameter is 0.15 ~ 0.25 mm fine coal is tested；
Second step, prepare the hydrogen peroxide that mass concentration is 30 %.
3rd step, the ml of 30 % hydrogen peroxide 25 and 5 g coals are separately added into 100 ml beakers.Lead under the conditions of 25 DEG C Magnetic stirring apparatus is crossed with 700 r/min speed, 8 h, 12 h and 16 h is continuously stirred respectively, mixed solution is obtained after stirring.
4th step, the separation of solid and liquid of mixed liquor are mainly carried out by the way of filtering, i.e., carried out using 0.22 μm of filter membrane Filter, fully wash coal with lot of pure water in filter process, the obtained coal of separation dries 6 h under the conditions of 45 DEG C, as life The substrate of produce Experiment of Methane.
5th step, coal bed gas product water is gathered from Qinshui basin, using anthracite as sole carbon source, in the bar of addition culture medium The mixed bacterial of degraded coal methane phase under part, is screened, is enriched with from output water.It is 35 DEG C to be enriched with temperature, quiescent culture.
Wherein, the enriched medium component of methanogen floras is：
1L enriched mediums include K2HPO40.4 g, MgCl22.0 g, KH2PO40.4g, yeast extract 1.0 g, NH4Cl 1.0 g, the g of resazurin 0.001, cysteine 0.5 g, Na2S 0.2 g, NaHCO30.2 g, sodium acetate 2.0 g, KCl 0.2 The g of g, NaCl 2.0, the ml of trace element solution 10.0, vitamin solution 10.0 ml, pH 7.0.
1L trace element solutions include：FeCl2·4H2O 1.5mg, AlK (SO4)210mg, ZnCl270mg, NiCl2· 6H2O 24mg, MnCl2·4H2O 100mg, NaMoO46mg, CuCl22mg, H3BO336mg, CoCl2·6H2The mg of O 190, 25% HCl 10 ml/L
1L vitamin solutions include：Biotin 2mg, folic acid 2mg, B6 10mg, B2 5mg, B1 5mg, nicotinic acid 5mg, B12 0.1mg, lipoic acid 5mg, p-aminobenzoic acid 5mg.
After 15 Secondary Cultures, the function Mixed Microbes based on Enterobacter and Methanosaeta are obtained Group.
6th step, in 140 ml serum bottles, using coals of 1 g after the drying of the 4th step as reaction substrate, utilize the The methane phase mixed bacterial that five steps obtain, continuous culture 40 days under the conditions of 35 DEG C, to realize the biodegradable methane phase of coal. Methane production is once monitored every 5 days during reaction.
Shown in coal biological methane yield as accompanying drawing 1.Methane production is in preceding 20 days rapid growths of culture, increasing in 20-40 days It is long slow.The average methane production of maximum after the h of 30% hydrogen peroxide treatment 8 is 214 μm of ol/g coals.30% hydrogen peroxide treatment 12 The average methane production of maximum after h is 232 μm of ol/g coals.Maximum after 30% hydrogen peroxide pretreatment anthracite 16 h is averagely produced Methane content is 230 μm of ol/g coals.
Comparative example 1：
In this example not plus hydrogen peroxide treatment coal, other process conditions are same as Example 1.Biological methane yield is shown in the institute of accompanying drawing 1 Show.In comparative example 1, the growth trend of methane production is similar to Example 1, but maximum average methane production is 204 μm of ol/g Coal.
By comparing embodiment 1 and comparative example 1, find：After the h of 30 % hydrogen peroxide treatments 8, biological methane yield Add 4.9 %；After the h of 30 % hydrogen peroxide treatments 12, biological methane yield adds 13.7 %；Through 30 % peroxidating After hydrogen handles 16 h, biological methane yield adds 12.7%.
Understood by Fig. 1 contrasts, after the present invention is pre-processed using hydrogen peroxide to coal, pass through the oxidation of pretreating agent Property improves the degree of oxidation of coal, its biological effectiveness is enhanced, so as to effectively increase the yield of coal biological methane.
Embodiment 2：
Mass concentration is that 5% hydrogen peroxide pre-processes the h of anthracite 12, is comprised the following steps：
The present embodiment is using anthracite similarly to Example 1.
The first step, after Qinshui basin target coal seam obtains anthracite coal sample, coal sample is crushed, sieved, choose grain Footpath for 0.15 ~ 0.25 mm's test；
Second step, prepare the hydrogen peroxide that mass concentration is 5 %.
3rd step, the ml of 5 % hydrogen peroxide 25 and 5 g coals are separately added into 100 ml beakers.Pass through under the conditions of 25 DEG C Magnetic stirring apparatus continuously stirs 12 h with 650 r/min speed, and mixed solution is obtained after stirring.
4th step, the separation of solid and liquid of mixed liquor stand 24h mainly using method progress is stored at room temperature under room temperature environment, Residual hydrogen dioxide is consumed through autoxidation, while realize that solid and liquid are sufficiently separated；Supernatant is gone using liquid-transfering gun Remove, residual coal dries 12 h to constant weight at 35 DEG C.
5th step, coal bed gas product water is gathered from Qinshui basin, using anthracite as sole carbon source, in the bar of addition culture medium The mixed bacterial of degraded coal methane phase under part, is screened, is enriched with from output water.It is 35 DEG C to be enriched with temperature, quiescent culture.
Wherein, the enriched medium component of methanogen floras is the same as embodiment 1.
After 30 Secondary Cultures, the functional flora of methanogen, bacterium and fungi mixing is obtained.
6th step, in 140 ml serum bottles, using coals of 1 g after the drying of the 4th step as reaction substrate, utilize the The methane phase mixed bacterial that five steps obtain, continuous culture 32 days under the conditions of 35 DEG C, to realize the biodegradable methane phase of coal. Periodic detection methane production during reaction.
Shown in coal biological methane yield as accompanying drawing 2.Methane production rapid growth since the 12nd day of culture, to culture 32 days, average methane production reaches 200.72 μm of ol/g coals.
Comparative example 2：
In this example not plus hydrogen peroxide treatment coal, other process conditions are same as Example 2.In comparative example 2, methane production is being trained Increases slowly, quickly increase before foster 20 days within 20-25 days；During by 32 days, average methane production reaches 31.3 μm of ol/g coals.
By comparing embodiment 2 and comparative example 2, find：After the h of 5 % hydrogen peroxide treatments 12, biological methane yield Add 541.27 %.
Understood by Fig. 2 contrasts, after the present invention is pre-processed using hydrogen peroxide to coal, significantly increase coal system biology The yield of methane.

Claims (10)

  1. A kind of 1. method for improving biological methane yield using hydrogen peroxide pretreatment coal, it is characterised in that：Peroxide is used first Change hydrogen solution to pre-process coal, then add microorganism fungus kind, realize the process of biodegradable coal methane phase.
  2. 2. the method according to claim 1 for improving biological methane yield using hydrogen peroxide pretreatment coal, its feature exist In：In preprocessing process, the mass concentration of hydrogenperoxide steam generator is 5% ~ 30%, and processing time is 8 ~ 16 h.
  3. 3. the method according to claim 1 for improving biological methane yield using hydrogen peroxide pretreatment coal, its feature exist In：Comprise the following steps：
    （1）Coal into powder and is sieved by crushing mechanism, the particle size range after coal sieving is 0.15 ~ 0.25 mm；
    （2）Coal dust is mixed with the hydrogenperoxide steam generator prepared, 8 ~ 16 h are stirred at room temperature by magnetic stirring apparatus；
    The ratio of coal dust and hydrogenperoxide steam generator is：4 ~ 5ml hydrogenperoxide steam generator is used per g coal dusts；Magnetic stirring apparatus stirs It is 600 ~ 800 rpm to mix speed；
    （3）By step（2）Gained mixed solution carries out separation of solid and liquid, obtains solid coal, and dry；
    （4）With step（1）Coal used is substrate, under conditions of nutritional ingredient is provided, screened from coal bed gas product water or coal, The functional flora of enrichment degraded coal methane phase；
    （5）With step（3）Drying gained solid coal is substrate, utilizes step（4）The functional flora that enrichment obtains realizes biology drop Coal methane phase process is solved, while in incubation, gas chromatographic detection methane production was utilized every 3-7 days.
  4. 4. the method according to claim 3 for improving biological methane yield using hydrogen peroxide pretreatment coal, its feature exist In：The coal is anthracite or bituminous coal.
  5. 5. the method according to claim 3 for improving biological methane yield using hydrogen peroxide pretreatment coal, its feature exist In：Step（3）In, separation of solid and liquid is realized by the method for being stored at room temperature or being filtered by vacuum.
  6. 6. the method according to claim 5 for improving biological methane yield using hydrogen peroxide pretreatment coal, its feature exist In：The method of being stored at room temperature is specially：24h is stood under room temperature environment, residual hydrogen dioxide is consumed through autoxidation, together Shi Shixian solids and liquid are sufficiently separated, and supernatant is removed, and residual coal is dried.
  7. 7. the method according to claim 5 for improving biological methane yield using hydrogen peroxide pretreatment coal, its feature exist In：The vacuum filtration method is specially：Mixed solution is filtered using Vacuum filtration device, made in Vacuum filtration device It is 0.22 μm of filter membrane, repeatedly washing is carried out to coal sample to remove residual hydrogen dioxide using distilled water in filter process, Residual coal is taken to be dried after washing.
  8. 8. the method according to claim 3 for improving biological methane yield using hydrogen peroxide pretreatment coal, its feature exist In：Step（3）In, drying temperature is 35 ~ 45 DEG C, and drying time is 6 ~ 12 h.
  9. 9. the method according to claim 3 for improving biological methane yield using hydrogen peroxide pretreatment coal, its feature exist In：Step（4）In, it is described degraded coal methane phase functional flora include cellulose-degrading bacteria, aromatic compound degradation bacteria or Methanogen.
  10. 10. the method according to claim 3 that biological methane yield is improved using NaOH pretreatment coal, its feature are existed In：Step（4）In, the nutritional ingredient includes basal nutrient, trace element or vitamin.
CN201710740239.6A 2017-08-25 2017-08-25 A kind of method for improving biological methane yield using hydrogen peroxide pretreatment coal Pending CN107460211A (en)

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Publication number Priority date Publication date Assignee Title
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CN102985514A (en) * 2010-04-21 2013-03-20 克里斯能量有限公司 Solubilization of carbonaceous materials and conversion to hydrocarbons and other useful products
CN102517368A (en) * 2011-12-15 2012-06-27 河南理工大学 Method for preparing biogas by degrading coal with microorganisms
CN104295276A (en) * 2014-07-29 2015-01-21 太原理工大学 Method for improving coalbed methane collection rate

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Application publication date: 20171212