CN103614162B - Method for preparing biological oil-based syngas by utilizing biological oil produced by thermal cracking of agricultural and forestry wastes to gasify - Google Patents
Method for preparing biological oil-based syngas by utilizing biological oil produced by thermal cracking of agricultural and forestry wastes to gasify Download PDFInfo
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Abstract
The invention discloses a method for preparing biological oil-based syngas by utilizing biological oil produced by thermal cracking of agricultural and forestry wastes to gasify. The biological oil produced by thermal cracking of the agricultural and forestry wastes is taken as a raw material, the raw material is extensive in source and low in cost, the use of a catalyst is not required in gasification process, the pretreatment of the biological oil and water is not required, the gasification can be realized under the action of normal pressure and a conventional gasifying agent, the problem that the catalyst is easy to coke and inactivate is avoided, and the raw material cost and the equipment cost are reduced. The gasification raw material composition is changed by introducing the proper amount of waste hydrocarbon type liquid fuel into the biological oil, the technical difficult problem of coking in a biological oil gasification process is solved, the yield and the quality of the syngas are further improved, a new concept is provided for reforming of the syngas, a new method is created for preparing high-grade chemical products by taking waste biomass as raw material, and a new way is simultaneously provided for recycling of the waste hydrocarbon type liquid fuel.
Description
Technical field:
The present invention relates to a kind of biomass-making that utilizes for the method for synthetic gas, be specifically related to the method for a kind of bio oil vaporizing system utilizing agriculture and forestry organic waste material thermo-cracking to produce for biological oil base synthetic gas.
Background technology:
Synthetic gas is a kind of important basic chemical industry raw material, is rich in H
2, CO and a small amount of CO
2, it can be used for refining as intermediate or synthesize various high-quality liquid fuel and chemical, as hydrogen, methyl alcohol, low-carbon alcohol, dme and various Fischer Tropsch fuels etc.Through development for many years, being raw material with Sweet natural gas, coal at present, synthetic gas preparation technology is very ripe, take synthetic gas as the synthetic ammonia of raw material, oxygenatedchemicals, hydro carbons and carbon one chemical production technical put into commercial operation all.But produce the investment of production of synthetic gas by Sweet natural gas or coal and cost accounts for 50 ~ 60% of product cost usually, therefore the research of cheap syngas production technology is of crucial importance.At present, Sweet natural gas (methane) steam reforming technology is the most ripe, H
2/ CO(mol ratio, lower same) high, generally 2.5 ~ 3.0, but apparatus expensive; Methane self-heating recapitalization and catalyzing part oxidation preparing synthetic gas technology still under development; Coal Gasification Technology equipment is complicated, investment is large, it is heavy to pollute, H
2/ CO than on the low side, about 0.4 ~ 0.7.
Biomass are the reproducible carbon sources of unique carbon containing, have that sulphur content is low, resource extensively, forever can utilize and not increase earth's surface CO
2the features such as circulation total amount.It is be the heat treatment of high-grade clean gaseous fuel by low-grade solid biomass feedstock conversion that gasifying biomass prepares synthetic gas technology, can effectively reduce greenhouse gas emission problem, be a kind of continuable clean Energy Conversion Technology, in economy and technical elements, all there is potential advantage and huge application prospect.Gasifying biomass prepares synthetic gas two kinds of technological approaches: one is directly biomass gasified in vapourizing furnace, then carries out reformation conversion to the combustion gas produced and makes synthetic gas; Two is first carry out middle temperature fast pyrogenation to biomass to obtain bio oil, then bio oil is gasified, makes synthetic gas through reformation conversion.In the direct gasification process of biomass, can produce more tar (can be condensed into liquid organic compound under normal temperature, can block, corrosion pipeline), its energy accounts for 5% ~ 15% of gasifying biomass total energy, the small molecules inflammable gas (H simultaneously produced
2, CO) amount less, thus reduce integrated gasification efficiency, limit the application of biomass gasification technology.Compared with biomass direct gasification, preparing synthetic gas by gasifying biological oil has following advantage: the feature that (1) bio oil has easily collecting, easily stores, easily transports, a certain place can be focused on gasify, be which solved the problem of biomass material large scale collection, storage and transport; (2) continuously feeding with pressure can be realized by oil pump, reduce the energy consumption of the subsequent synthetic processes of synthetic gas; (3) biomass high-temperature can be avoided to gasify deslagging problem that grey fractional melting brings; (4) gas that bio oil vaporizing system is standby is pure, and the technical difficulty of subsequent gases conversion is less.
In recent years, the research of gasifying about bio oil has caused the great attention of Chinese scholars.Different by gasification mode, bio oil gasification can be divided into bio-oil steam reforming, pyrolytic gasification and supercritical water gasification etc.Be hydrogen, carbon monoxide, methane and carbon dioxide in the main component without the bio oil pyrolytic gasification gained crude synthesis gas under outside oxygen supply condition, volume fraction is respectively 31.5%, 37.7%, 16.9% and Zhu 9.4%(Xi Feng, Venderbosch R H, biomass pyrolysis oil Study on gasification experiment, chemistry of fuel journal, Vol.132, No.14,2004, Pages 510-512), H
2/ CO is lower, and CH
4and CO
2content is high, and being not suitable for, directly as the unstripped gas of higher alcohols synthesis, generally needs to carry out modulation through follow-up reforming process to its composition, thus obtain clean higher-grade biomass synthesis gas.The method that crude synthesis gas reformation adopts comprises the novel gasification of design or reforming reactor, introduce suitable vaporized chemical (as air, oxygen, CO, hydrogen, water vapour or wherein several gas mixtures), select suitable catalyzer and gasification reaction conditions, or improve reforming reaction temperature.
Holland biomass Technical Research Center (BTG) Venderbosch R.H. etc. at ambient pressure, using air as vaporized chemical, carry out gasification test to wooden bio oil, under having investigated 1000-1100 DEG C of condition respectively, different air equivalent coefficient (ER) is on the impact of gasification product.Result shows: in ER variation range (0.1 ~ 0.4), V (H
2)/V (CO) remains on 0.8 ~ 0.9, H substantially
2drop to 15.0% with the volume fraction of CO from 25.0%, gas Lower heat value is corresponding drops to 4MJ/kg from 8MJ/kg.Lanzhou Inst. of Chemical Physics, Chinese Academy of Sciences's oxo process and selective oxidation National Key Laboratory Lv Gong is fluffy etc. develops a kind of novel " Y " type reactor, and be applied to bio-oil steam reformation (SR), bio oil partial oxidation (POX) and bio oil oxidative steam reform (SOR) coupled biological oil CO 2 reformation (DR) prepare synthetic gas, its result shows, at 800 DEG C, under normal pressure, V (H in three kinds of coupling technique gained synthetic gas
2)/V (CO) is respectively 1.69,1.33 and 1.56, effectively reduces CO in gained synthetic gas
2content (Xun Hu, Gongxuan Lu, Bio-oil steam reforming, partial oxidation oroxidative steam reforming coupled with bio-oil dry reforming to eliminate CO
2emission, Vol.35,2010, Pages 7169-7176).These methods all rest on the desk study stage and deliver without any Patents.
Domestic patent CN 101214919A discloses a kind of employing pressurized entrained-bed, using one or more in air, oxygen, carbonic acid gas, overheated steam or oxygen-rich air as vaporized chemical, bio oil is carried out to the device of gasification reaction.This patent is intended to carry out pressurized gasification to bio oil, and adjusts the composition of synthetic gas by the combination of vaporized chemical, and the method is higher to equipment requirements, and pipeline needs particular design, adds the fund input to reaction unit.Domestic patent CN 101560413A discloses the device that a kind of biomass rough gas autothermal catalysis is reformed, and autothermal reaction technology is applied to the reformation scavenging process of biomass rough gas, makes the tar in biogas and CH
4, C
2, C
3, under honeycomb monolith nickel magnesium sosoloid catalyst action, be optionally converted into H
2and CO, effective modulation H
2/ CO ratio, but this device adopts biomass rough gas as unstripped gas, be not suitable for the gasification reaction carrying out bio oil, and the catalyzer used easily produces carbon distribution problem.With regard to biomass-based methanol, application number is that the domestic patent of 201010190095.X proposes after biomass cracking generates bio oil steam and biomass charcoal powder, and bio oil steam, by steam reforming reaction, obtains coarse biometric oil reformed syngas; Biomass charcoal powder then with NiO-Al
2o
3with HZSM-5 catalyzer, and one or both associating agent in kaolin or sesbania powder are by a certain percentage after ground and mixed, carry out coal gas reaction (CO to biological oil reforming synthetic gas
2+ C → 2CO) and reverse water-gas-shift reaction (CO
2+ H
2→ CO+H
2o), biological oil reforming-adjustment synthetic gas is obtained through condensation, drying.These two kinds of synthetic gas are at Cu/ZnO/Al
2o
3the synthesis of methyl alcohol is carried out under the effect of catalyzer, this technology is one of current domestic rare biological oil reforming synthetic gas patent report preparing oxygen-containing organic compound, but this technical matters is comparatively complicated, catalyzer used in synthetic gas reforming process easily causes coking and deactivation.Therefore, find new bio oil gasification synthesis gas reforming method, improve gasification efficiency and regulate H in synthetic gas
2the ratio of/CO is significant for the synthesis of follow-up liquid fuel.
China has a large amount of discarded liquid hydrocarbon fuels to result from the industries such as machinery, chemical industry and communications and transportation every year.According to statistics, by the end of the year 2009, national vehicle guaranteeding organic quantity, more than 1.86 hundred million, will produce used oil 7,000,000 about t, will cause very large pollution pressure to environment.At present, be used as fuel after most used oil reclaims, this not only causes the wasting of resources, and due to wherein containing heavy metal compound, enters in physical environment and cause very serious pollution after burning.Therefore, from the angle of energy saving standard, how discarded liquid hydrocarbon fuel is effectively recycled, become current urgent problem.
Summary of the invention:
The object of this invention is to provide the method for a kind of bio oil vaporizing system utilizing agriculture and forestry organic waste material thermo-cracking to produce for biological oil base synthetic gas, change gasified raw material composition by introducing appropriate discarded liquid hydrocarbon fuel in bio oil, thus realize H in biological oil base synthetic gas
2effective modulation of/CO ratio.
The present invention is achieved by the following technical programs:
The bio oil vaporizing system utilizing agriculture and forestry organic waste material thermo-cracking to produce is for a method for biological oil base synthetic gas, and the method comprises the following steps:
A, under violent stirring effect, in discarded liquid hydrocarbon fuel, slowly add hydrophilic emulsifier and lipophilic emulsifier, add moisture simultaneously and carry out emulsification, liquid hydrocarbon fuel is discarded in obtained emulsification;
B, the emulsification prepared by step a are discarded after liquid hydrocarbon fuel and agriculture and forestry organic waste material fast pyrolysis gained bio oil add uniform moisture mixing respectively, with air or oxygen or both gas mixtures (air mixes with arbitrary proportion with oxygen) as vaporized chemical, non-catalytic partial oxidation gasification is carried out at 500 ~ 1400 DEG C of temperature, gained gaseous product, after desulfurization, washing, dry removal sulfide, tar and moisture, obtains biological oil base synthetic gas; The mass ratio that liquid hydrocarbon fuel is discarded in described agriculture and forestry organic waste material fast pyrolysis gained bio oil and emulsification is 1:0.25 ~ 1:4.
Described agriculture and forestry organic waste material fast pyrolysis gained bio oil be prepared as prior art, reference literature [Zhu Xifeng, Guo Tao, Lu Qiang, Guo Qingxiang. bio oil spray burning testing of characteristic, China Science & Technology University's journal, 2005,35 (6): 856-860] disclosed preparation method's preparation.
Described agriculture and forestry organic waste material comprises various production estimation and processing waste, production of forestry and processing waste, municipal wastes etc.
Described discarded liquid hydrocarbon fuel is selected from one or more the mixture in the liquid fuels such as used oil, waste coal oil, waste diesel, waste lubricating oil, barren rock cerebrol, or contains the high ratio of carbon-hydrogen compound of a small amount of oxygen.
Described hydrophilic emulsifier selects one or more the mixture in polysorbas20, polysorbate60, tween 80, sodium oleate, potassium oleate or laurilsulfate sodium; Described lipophilic emulsifier selects one or more the mixture in oleic acid, class 20 of department, class 60 of department or class 80 of department.
Hydrophilic emulsifier addition in described step a is 1 ~ 8wt%, and lipophilic emulsifier addition is 1 ~ 4wt%, and the addition of moisture is 10 ~ 40wt%, and emulsification is Homogeneous phase mixing 5 ~ 60min under 10 ~ 80 DEG C of conditions.
Moisture addition in described step b is 10 ~ 40wt%, and interpolation moisture is intended to the C/H ratio in modulation gasified raw material, strengthens the water gas shift reaction (CO+H in gasification reaction process
2o → CO
2+ H
2), effectively improve the H in gained synthetic gas
2/ CO ratio.
Temperature of reaction in described step b is preferably 800 ~ 1100 DEG C, and at this temperature, the non-catalytic partial oxidation gasification reaction of bio oil reaches balance, achieves organism in bio oil to H
2, the micro-molecular gas such as CO maximum conversion.
Compared with prior art, the present invention has following beneficial effect:
(1) bio oil that the present invention adopts agriculture and forestry organic waste material thermo-cracking to produce is raw material, raw material sources are extensive and cheap, do not need in gasification to use catalyzer, do not need to carry out pre-treatment to bio oil and water, effective gasification can be realized under normal pressure and traditional gasification agent effect, thus avoid the problem of the easy coking and deactivation of catalyzer, greatly reduce the complicacy of bio oil gasification system, reduce raw material and equipment cost.
(2) bio oil oxygen level is high, and calorific value is lower than oil fuel, and Intermolecular Forces is large, and viscosity is large, and pH value is low, and intermolecular being heated is easy to polymerization, poor heat stability.Discarded liquid hydrocarbon fuel carbon content is high, boiling point is high, there is good heat conductivility, the present invention changes gasified raw material composition by introducing appropriate discarded liquid hydrocarbon fuel in bio oil, discarded liquid hydrocarbon fuel is used as the thermal conducting agent of bio oil gasification, then discarded liquid hydrocarbon fuel generation cracking and structural rearrangement is made through non-catalytic partial oxidation gasification, small molecule hydrocarbon is become by macromolecular cleavage, and then being converted into biological oil base synthetic gas, the recycling for discarded liquid hydrocarbon fuel provides a kind of new way.
(3) the present invention utilizes discarded liquid hydrocarbon fuel and bio oil two kinds of materials to carry out mixing gasifying, not only can improve the mass-and heat-transfer condition of bio oil gasification, solve the coking technical barrier in bio oil gasifying process, and productive rate and the quality of synthetic gas can be improved, effectively regulate the H in the biological oil base synthetic gas of gained
2/ CO ratio, reduces the CO in synthetic gas
2content, realize effective reformation of bio oil gasification synthesis gas, make it be suitable for the techniques such as follow-up F-T synthesis, methyl alcohol, higher alcohols synthesis, reforming for synthetic gas provides new approaches, and opening one with abandoned biomass is the novel method that higher-grade Chemicals prepared by raw material.
Accompanying drawing illustrates:
Fig. 1 is process flow sheet of the present invention.
Embodiment:
Below further illustrate of the present invention, instead of limitation of the present invention.
Embodiment 1: utilize bio oil and used oil mixing gasifying to prepare synthetic gas
Adopt the technical process shown in Fig. 1, under violent stirring effect, to the used oil (H through processed
2o≤0.5wt%) in slowly add the class of department 60 of the polysorbate60 of 8wt% and 4wt% and the mixture of class 80 of department, add the moisture of 40wt% simultaneously, obtain emulsification used oil at 80 DEG C of emulsified 5min.(it prepares reference literature [Zhu Xifeng to the bio oil obtained with discarded cornstalk fast pyrolysis, Guo Tao, Lu Qiang, Guo Qingxiang. bio oil spray burning testing of characteristic, China Science & Technology University's journal, 2005,35 (6): 856-860] disclosed preparation method) and emulsification used oil be gasified raw material, its physical parameter and element set prejudice table 1.
The physical parameter of table 1 bio oil and emulsification used oil and elementary composition
Bio oil and emulsification used oil 20wt% and 30wt% that add water respectively stirs, be that 1 ﹕ 1 squeezes into head tank by bio oil and emulsification used oil mass ratio, squeeze in vapourizing furnace with the flow velocity of 7.6kg/h after high-speed stirring in head tank, pass into air with the flow velocity of 12.4L/h simultaneously, gasification reaction is carried out at 500 ~ 1400 DEG C, gained gaseous product is again through desulfurization, washing, dry removal sulfide, after tar and moisture, obtain biological oil base synthetic gas, adopt its composition of chromatographic, calculate bio oil and emulsification used oil non-catalytic partial oxidation vaporizing system under different gasification temperature thus for total efficiency of carbon conversion of synthetic gas and H
2/ CO ratio, result is as shown in table 2.
At the different gasification reaction temperature of table 2, bio oil and emulsification used oil mixing gasifying prepare synthetic gas result
Bio oil and emulsification used oil 20wt% and 30wt% that add water respectively stirs, 1 ﹕ 0.25 is respectively by bio oil and emulsification used oil mass ratio, 1 ﹕ 0.33, 1 ﹕ 1, 1 ﹕ 3 and 1 ﹕ 4 squeezes into head tank, squeeze in vapourizing furnace with the flow velocity of 7kg/h after high-speed stirring in head tank, pass into air with the flow velocity of 12L/h simultaneously, gasification reaction is carried out at 1000 ~ 1100 DEG C, gained gaseous product is through desulfurization, washing, dry removal sulfide, after tar and moisture, obtain biological oil base synthetic gas, and adopt its composition of chromatographic, calculate total efficiency of carbon conversion and the H of gasified raw material thus
2/ CO ratio, result is as shown in table 3.
Bio oil and the emulsification used oil mixing gasifying of table 3 different mass ratio prepare synthetic gas result
Embodiment 2 utilizes bio oil and waste diesel mixing gasifying to prepare synthetic gas
Adopt the technical process shown in Fig. 1, under violent stirring effect, to waste diesel (H
2o≤0.1wt%) in slowly add tween 80 and the class of 1wt% department 80 of 1wt%, add the moisture of 10wt% simultaneously, obtain emulsification waste diesel at 10 DEG C of emulsified 60min.(it prepares reference literature [Zhu Xifeng to the bio oil obtained with discarded rice husk fast pyrolysis, Guo Tao, Lu Qiang, Guo Qingxiang. bio oil spray burning testing of characteristic, China Science & Technology University's journal, 2005,35 (6): 856-860] disclosed preparation method) and emulsification waste diesel be gasified raw material, its physical parameter and element set prejudice table 4.
The physical parameter of table 4 bio oil and emulsification waste diesel and elementary composition
Bio oil and emulsification waste diesel 10wt% and 40wt% that add water respectively stirs, be that 1 ﹕ 0.33 squeezes into head tank by bio oil and emulsification waste diesel mass ratio, squeeze in vapourizing furnace with the flow velocity of 9.3kg/h after high-speed stirring in head tank, pass into oxygen with the flow velocity of 2.7L/h simultaneously, gasification reaction is carried out at 500 ~ 1400 DEG C, gained gaseous product is through desulfurization, washing, dry removal sulfide, after tar and moisture, obtain biological oil base synthetic gas, and adopt its composition of chromatographic, calculate bio oil and emulsification waste diesel non-catalytic partial oxidation vaporizing system under different gasification temperature thus for total efficiency of carbon conversion of synthetic gas and H
2/ CO ratio, result is as shown in table 5.
At the different gasification reaction temperature of table 5, bio oil and emulsification waste diesel mixing gasifying prepare synthetic gas result
Bio oil and emulsification waste diesel 10wt% and 40wt% that add water respectively stirs, 1 ﹕ 0.25 is respectively by bio oil and emulsification waste diesel mass ratio, 1 ﹕ 0.33, 1 ﹕ 1, 1 ﹕ 3 and 1 ﹕ 4 squeezes into head tank, squeeze in vapourizing furnace with the flow velocity of 9kg/h after high-speed stirring in head tank, pass into air with the flow velocity of 12L/h simultaneously, gasification reaction is carried out at 1000 ~ 1100 DEG C, gained gaseous product is through desulfurization, washing, dry removal sulfide, after tar and moisture, obtain biological oil base synthetic gas, and adopt its composition of chromatographic, calculate total efficiency of carbon conversion and the H of gasified raw material thus
2/ CO ratio, result is as shown in table 6.
Bio oil and the emulsification waste diesel mixing gasifying of table 6 different mass ratio prepare synthetic gas result
Foregoing be only the present invention conceive under basic explanation, and according to any equivalent transformation that technical scheme of the present invention is done, all should protection scope of the present invention be belonged to.
Claims (4)
1. the bio oil vaporizing system utilizing agriculture and forestry organic waste material thermo-cracking to produce is for a method for biological oil base synthetic gas, and the method comprises the following steps:
A, under violent stirring effect, in discarded liquid hydrocarbon fuel, slowly add hydrophilic emulsifier and lipophilic emulsifier, add moisture simultaneously and carry out emulsification, liquid hydrocarbon fuel is discarded in obtained emulsification; Described hydrophilic emulsifier addition is 1 ~ 8wt%, and described lipophilic emulsifier addition is 1 ~ 4wt%, and the addition of described moisture is 10 ~ 40wt%, and described emulsification is at 10 ~ 80 DEG C of emulsified 5 ~ 60min of condition;
B, the emulsification prepared by step a are discarded after liquid hydrocarbon fuel and agriculture and forestry organic waste material fast pyrolysis gained bio oil add uniform moisture mixing respectively, with air or oxygen or both with arbitrary proportion mixing gas mixture be used as vaporized chemical, non-catalytic partial oxidation gasification is carried out at 500 ~ 1400 DEG C of temperature, gained gaseous product, after desulfurization, washing, dry removal sulfide, tar and moisture, obtains biological oil base synthetic gas; The mass ratio that liquid hydrocarbon fuel and agriculture and forestry organic waste material fast pyrolysis gained bio oil are discarded in described emulsification is 1:0.25 ~ 1:4; Described moisture addition is 10 ~ 40wt%.
2. the bio oil vaporizing system utilizing agriculture and forestry organic waste material thermo-cracking to produce according to claim 1 is for the method for biological oil base synthetic gas, it is characterized in that, described hydrophilic emulsifier selects one or more the mixture in polysorbas20, polysorbate60, tween 80, sodium oleate, potassium oleate or laurilsulfate sodium; Described lipophilic emulsifier selects one or more the mixture in oleic acid, class 20 of department, class 60 of department or class 80 of department.
3. the bio oil vaporizing system utilizing agriculture and forestry organic waste material thermo-cracking to produce according to claim 1 is for the method for biological oil base synthetic gas, it is characterized in that, described agriculture and forestry organic waste material is selected from production estimation and processing waste, production of forestry and processing waste, municipal wastes; Described discarded liquid hydrocarbon fuel is selected from one or more the mixture in discarded machine oil, kerosene, gasoline, diesel oil, lubricating oil, petroleum naphtha or liquefied petroleum gas (LPG), or contains the high ratio of carbon-hydrogen compound of a small amount of oxygen.
4. the bio oil vaporizing system utilizing agriculture and forestry organic waste material thermo-cracking to produce according to claim 1 is for the method for biological oil base synthetic gas, it is characterized in that, in described step b, temperature of reaction is 800 ~ 1100 DEG C.
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