CN101255348B - Method for preparing bio-diesel by immobilized lipase-alcohol penetrating membrane bioreactor - Google Patents
Method for preparing bio-diesel by immobilized lipase-alcohol penetrating membrane bioreactor Download PDFInfo
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- CN101255348B CN101255348B CN200810060548XA CN200810060548A CN101255348B CN 101255348 B CN101255348 B CN 101255348B CN 200810060548X A CN200810060548X A CN 200810060548XA CN 200810060548 A CN200810060548 A CN 200810060548A CN 101255348 B CN101255348 B CN 101255348B
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- C—CHEMISTRY; METALLURGY
- C12—BIOCHEMISTRY; BEER; SPIRITS; WINE; VINEGAR; MICROBIOLOGY; ENZYMOLOGY; MUTATION OR GENETIC ENGINEERING
- C12M—APPARATUS FOR ENZYMOLOGY OR MICROBIOLOGY; APPARATUS FOR CULTURING MICROORGANISMS FOR PRODUCING BIOMASS, FOR GROWING CELLS OR FOR OBTAINING FERMENTATION OR METABOLIC PRODUCTS, i.e. BIOREACTORS OR FERMENTERS
- C12M29/00—Means for introduction, extraction or recirculation of materials, e.g. pumps
- C12M29/04—Filters; Permeable or porous membranes or plates, e.g. dialysis
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- C—CHEMISTRY; METALLURGY
- C12—BIOCHEMISTRY; BEER; SPIRITS; WINE; VINEGAR; MICROBIOLOGY; ENZYMOLOGY; MUTATION OR GENETIC ENGINEERING
- C12M—APPARATUS FOR ENZYMOLOGY OR MICROBIOLOGY; APPARATUS FOR CULTURING MICROORGANISMS FOR PRODUCING BIOMASS, FOR GROWING CELLS OR FOR OBTAINING FERMENTATION OR METABOLIC PRODUCTS, i.e. BIOREACTORS OR FERMENTERS
- C12M21/00—Bioreactors or fermenters specially adapted for specific uses
- C12M21/12—Bioreactors or fermenters specially adapted for specific uses for producing fuels or solvents
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- C—CHEMISTRY; METALLURGY
- C12—BIOCHEMISTRY; BEER; SPIRITS; WINE; VINEGAR; MICROBIOLOGY; ENZYMOLOGY; MUTATION OR GENETIC ENGINEERING
- C12M—APPARATUS FOR ENZYMOLOGY OR MICROBIOLOGY; APPARATUS FOR CULTURING MICROORGANISMS FOR PRODUCING BIOMASS, FOR GROWING CELLS OR FOR OBTAINING FERMENTATION OR METABOLIC PRODUCTS, i.e. BIOREACTORS OR FERMENTERS
- C12M21/00—Bioreactors or fermenters specially adapted for specific uses
- C12M21/18—Apparatus specially designed for the use of free, immobilized or carrier-bound enzymes
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- C—CHEMISTRY; METALLURGY
- C12—BIOCHEMISTRY; BEER; SPIRITS; WINE; VINEGAR; MICROBIOLOGY; ENZYMOLOGY; MUTATION OR GENETIC ENGINEERING
- C12M—APPARATUS FOR ENZYMOLOGY OR MICROBIOLOGY; APPARATUS FOR CULTURING MICROORGANISMS FOR PRODUCING BIOMASS, FOR GROWING CELLS OR FOR OBTAINING FERMENTATION OR METABOLIC PRODUCTS, i.e. BIOREACTORS OR FERMENTERS
- C12M29/00—Means for introduction, extraction or recirculation of materials, e.g. pumps
- C12M29/02—Percolation
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- 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
- Y02E50/10—Biofuels, e.g. bio-diesel
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- 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
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P30/00—Technologies relating to oil refining and petrochemical industry
- Y02P30/20—Technologies relating to oil refining and petrochemical industry using bio-feedstock
Abstract
The invention discloses a biological preparation by immobilized lipase-alcohol permeable membrane biological reactor. The process is that lipase is immobilized on surface of alcohol permeable membrane made of hollow fiber by physical absorption, membrane member of immobilized lipase is prepared, then assembled into enzyme-membrane reactor. Oil passes through shell side of membrane member, and low carbon alcohol passes through tube pass of the same, then fatifies them into biological diesel under catalysis of immobilized lipase. Low carbon alcohol selectively permeates hollow fibers to provide low carbon alcohol needed in preparation of biological diesel, so that inhibitory action towards enzyme activity caused by bottom articles is effectively avoided, and biological diesel is efficiently prepared. Moreover, solvent washing and batchwise charging is avoided, which meets the need of green chemistry, and reduces cost, simplify process, realizes continuous production.
Description
Technical field
The invention belongs to the bioenergy technical field.The immobilized lipase polymeric film and the bio-reactor thereof that are specifically related to a kind of energy selective permeation low-carbon alcohol are used to prepare method of bio-diesel oil.
Background technology
Biofuel be by reproducible glyceride stock through transesterify institute synthetic longer chain fatty acid methyl esters (or ethyl ester etc.), be a kind of environment Friendly fuel oil that replaces diesel oil.Immobilized enzyme method prepares that biofuel has efficient height, energy consumption low (reaction conditions gentleness), good, the pure consumption of selectivity is little, by product is few, environmental friendliness advantages such as (need not to carry out liquid waste disposal).Lipase can efficient catalytic alcohol carry out transesterification reaction with glycerin fatty acid ester, but the hydrogen bond system that immobilized enzyme method exists again to be shortened in lipase is on the high side, the absorption of by-product glycerin on the enzyme surface makes enzyme stability decreases and work-ing life, substrate methyl alcohol or ethanol (being low-carbon alcohol) can be deprived the necessary water of lipase and then destruction is kept the zymoprotein functional conformation and cause enzymic activity to descend and even a series of problems such as inactivation.
Patent disclosures such as CN1181161C, CN1325606C, CN1190471C utilize short-chain aliphatic ester to prepare method of bio-diesel oil as acyl acceptor.Patent US6398707B1 then discloses a kind of employing and has been no less than next " cleaning " immobilized enzyme of alcohol of three carbon atoms to recover the method that enzyme is lived.Lipase is carried out methods such as pre-treatment and portion-wise addition methyl alcohol and also obtains adopting, this Huang is reached the clouds wait people's description to some extent in " the fixed lipase catalyzed biodiesel synthesis of pre-treatment " literary composition (" Chinese oil) ", 2007,32 (7): 47-50).Directly more help biodiesel manufacture as acyl acceptor, but enzyme is carried out pre-treatment or clean expending a large amount of solvents, increased production cost and actually operating difficulty, be unfavorable for environment protection simultaneously with low-carbon alcohol.
The report that relevant polymer separation film is used for biodiesel manufacture seldom.People such as Guerreiro have reported application (the Transesterification of soybean oil oversulfonic acid functionalised polymeric membranes of polymeric film in the biodiesel manufacture process, Catalysis Today, 2006,118:166-171), but their employed polymeric film mainly is as solid acid catalyst, belongs to chemical catalysis.It is the method that two process couplings of propylene glycol are got up by membrane filtration technique with biodiesel manufacture and transformation of glycerol that CN1276962C discloses a kind of, but the main purpose of this method is the coupling production propylene glycol, and biological enzyme prepares the mode that methyl alcohol required in the biofuel process still adopts batch charging or dropping.This shows that reduce aspects such as realizing serialization production and simplification production technique when enzyme is lived avoiding substrate to suppress, existing technology exists obviously not enough.
Summary of the invention
The purpose of this invention is to provide a kind of preparation method of bio-diesel oil, lipase is fixed in pure hollow-fibre membrane surface by physical adsorption, the membrane module of preparation immobilized lipase, be assembled into enzyme-film bioreactor then, grease is walked the shell side of membrane module through pump, flow velocity is 1~5L/h, the while flow velocity is the tube side that the low-carbon alcohol of 2~100L/h is walked membrane module, and see through hollow-fibre membrane and enter the membrane module shell side, under catalytic action of immobilized lipase, promptly be converted into biofuel behind grease and the low-carbon alcohol circulating reaction 2~10h.Because adopt the selectivity alcohol permselective membrane that low-carbon alcohol is provided continuously, low-carbon alcohol is lower at the grease phase concentration, the activity of immobilized enzyme significantly improves.
A kind of preparation method of bio-diesel oil comprises the steps:
(1) lipase is fixed in pure hollow-fibre membrane surface by physical adsorption, the membrane module of preparation immobilized lipase is assembled into enzyme-film bioreactor then.
Described pure hollow-fibre membrane is polypropylene, polyethylene, polyvinylidene difluoride (PVDF).
Described lipase can be the general lipase in this area, for example derives from the lipase of Candida antarctica, Rhizomucor miehei, Thermomyces lanuginosus, Burkholderia acepacia, Pesudomonas fluorescens, Aspergillus niger, Mucor miehei or Candida rugosa.
(2) the 5L grease is injected grease storage tank 1, walk membrane module 3 shell sides through pump 2, flow velocity is 1~5L/h.Wherein grease is a bio-oil, comprises fish oil, lard, Viscotrol C, rapeseed oil, soybean oil, peanut oil, Semen Maydis oil, Oleum Gossypii semen, Rice pollard oil, algae grease, waste edible oil and oil refining pin material etc.
(3) methyl alcohol or the ethanol in the low-carbon alcohol storage tank 9 is walked membrane module 3 tube sides by pump 8, and enters shell side through hollow-fibre membrane, and the grease with shell side under the katalysis of immobilized enzyme reacts.The flow velocity of low-carbon alcohol is 2~100L/h, constantly circulation.
(4) after skimmer 5 separates, be collected in biofuel storage tank 6 by valve 4 behind grease circulation 2~10h, promptly obtain biofuel; Glycerine enters glycerine storage tank 7 through skimmer 5.
Effect of the present invention and benefit are to utilize low-carbon alcohol selective permeation hollow-fibre membrane that low-carbon alcohol required in the biodiesel manufacture process is provided, thereby have effectively avoided the enzyme that caused by the substrate low-carbon alcohol restraining effect of living, can the efficient production biofuel.And, avoided solvent cleaning and batch charging, meet the developing direction of Green Chemistry, can reduce cost, simplify technology, realize serialization production.
Description of drawings
Fig. 1 prepares biofuel apparatus structure synoptic diagram for the present invention.
Embodiment
Embodiment with reference to the description of drawings technical solution of the present invention, wherein the grease in the raw material storage tank 1 is walked the shell side of immobilized enzyme membrane module 3 through pump 2, the circulating reaction certain hour is after valve 4 enters skimmer 5, and separatory artifact diesel oil enters biofuel storage tank 6, and glycerine enters glycerine storage tank 7; Low-carbon alcohol is walked the tube side of immobilized enzyme membrane module 3 by low-carbon alcohol storage tank 9 through pump 8, recycles.Wherein shell side refers between the hollow-fibre membrane of immobilized enzyme membrane module 3 or the space between hollow-fibre membrane and the housing; Tube side refers to the hollow-fibre membrane internal space of immobilized enzyme membrane module 3.
Following examples are done more detailed description to the present invention, but described example is not construed as limiting the invention.
Embodiment 1
The lipase that derives from Candida antarctica is fixed in polydimethylsiloxane hollow-fibre membrane surface by physical adsorption, makes membrane module, link enzyme-film bioreactor.5L fish oil is injected grease storage tank 1, walk membrane module 3 shell sides through pump 2, flow velocity is 4L/h; Methyl alcohol in the low-carbon alcohol storage tank 9 is walked membrane module 3 tube sides by pump 8, and flow velocity is 20L/h.Circulation 2h artifact diesel oil yield is about 95%.
Embodiment 2
The lipase that derives from Rhizomucor miehei is fixed in poly-trimethyl silicane propine hollow-fibre membrane surface by physical adsorption, makes membrane module, link enzyme-film bioreactor.5L lard is injected grease storage tank 1, walk membrane module 3 shell sides through pump 2, flow velocity is 4L/h; Methyl alcohol in the low-carbon alcohol storage tank 9 is walked membrane module 3 tube sides by pump 8, and flow velocity is 20L/h.Circulation 4h artifact diesel oil yield is about 96%.
The lipase that derives from Thermomyces lanuginosus is fixed in chitosan hollow-fibre membrane surface by physical adsorption, makes membrane module, link enzyme-film bioreactor.The 5L Viscotrol C is injected grease storage tank 1, walk membrane module 3 shell sides through pump 2, flow velocity is 5L/h; Ethanol in the low-carbon alcohol storage tank 9 is walked membrane module 3 tube sides by pump 7, and flow velocity is 100L/h.Circulation 10h artifact diesel oil yield is about 100%.
It is that basement membrane and chitosan are the composite hollow fiber membrane surface on pure top layer that the lipase that derives from Burkholderia acepacia is fixed in the polyester by physical adsorption, makes membrane module, links enzyme-film bioreactor.The 5L rapeseed oil is injected grease storage tank 1, walk membrane module 3 shell sides through pump 2, flow velocity is 4L/h; Methyl alcohol in the low-carbon alcohol storage tank 9 is walked membrane module 3 tube sides by pump 8, and flow velocity is 40L/h.Circulation 6h artifact diesel oil yield is about 100%.
Embodiment 5
It is that basement membrane and polydimethylsiloxane are the composite hollow fiber membrane surface on pure top layer that the lipase that derives from Pesudomonas fluorescens is fixed in the polypropylene by physical adsorption, makes membrane module, links enzyme mebrane reactor.The 5L soybean oil is injected grease storage tank 1, walk membrane module 3 shell sides through pump 2, flow velocity is 4L/h; Methyl alcohol in the low-carbon alcohol storage tank 9 is walked membrane module 3 tube sides by pump 8, and flow velocity is 40L/h.Circulation 6h artifact diesel oil yield is about 99%.
It is that basement membrane and polydimethylsiloxane are the composite hollow fiber membrane surface on pure top layer that the lipase that derives from Aspergillus niger is fixed in the polyethylene by physical adsorption, makes membrane module, links enzyme mebrane reactor.5L peanut oil is injected grease storage tank 1, walk membrane module 3 shell sides through pump 2, flow velocity is 4L/h; Methyl alcohol in the low-carbon alcohol storage tank 9 is walked membrane module 3 tube sides by pump 8, and flow velocity is 20L/h.Circulation 4h artifact diesel oil yield is about 96%.
It is that basement membrane and poly-trimethyl silicane propine are the composite hollow fiber membrane surface on pure top layer that the lipase that derives from Mucor miehei is fixed in the polyvinylidene difluoride (PVDF) by physical adsorption, makes membrane module, links enzyme mebrane reactor.5L Semen Maydis oil is injected grease storage tank 1, walk membrane module 3 shell sides through pump 2, flow velocity is 4L/h; Methyl alcohol in the low-carbon alcohol storage tank 9 is walked membrane module 3 tube sides by pump 8, and flow velocity is 40L/h.Circulation 6h artifact diesel oil yield is about 99%.
Embodiment 8
It is that basement membrane and polydimethylsiloxane are the composite hollow fiber membrane surface on pure top layer that the lipase that derives from Candida rugosa is fixed in the polyacrylonitrile by physical adsorption, makes membrane module, links enzyme mebrane reactor.The 5L Oleum Gossypii semen is injected grease storage tank 1, walk membrane module 3 shell sides through pump 2, flow velocity is 4L/h; Methyl alcohol in the low-carbon alcohol storage tank 9 is walked membrane module 3 tube sides by pump 8, and flow velocity is 20L/h.Circulation 6h artifact diesel oil yield is about 98%.
Embodiment 9
It is that basement membrane and polydimethylsiloxane are the composite hollow fiber membrane surface on pure top layer that the lipase that derives from Candida antarctica is fixed in the polyethersulfone by physical adsorption, makes membrane module, links enzyme mebrane reactor.The 5L Rice pollard oil is injected grease storage tank 1, walk membrane module 3 shell sides through pump 2, flow velocity is 4L/h; Methyl alcohol in the low-carbon alcohol storage tank 9 is walked membrane module 3 tube sides by pump 8, and flow velocity is 20L/h.Circulation 6h artifact diesel oil yield is about 98%.
Embodiment 10
It is that basement membrane and polydimethylsiloxane are the composite hollow fiber membrane surface on pure top layer that the lipase that derives from Candida antarctica is fixed in the polyvinyl alcohol by physical adsorption, makes membrane module, links enzyme mebrane reactor.5L algae grease is injected grease storage tank 1, walk membrane module 3 shell sides through pump 2, flow velocity is 4L/h; Methyl alcohol in the low-carbon alcohol storage tank 9 is walked membrane module 3 tube sides by pump 8, and flow velocity is 20L/h.Circulation 6h artifact diesel oil yield is about 97%.
Embodiment 11
The lipase that derives from Candida antarctica is fixed in the Mierocrystalline cellulose by physical adsorption to be that basement membrane and polydimethylsiloxane are compound make membrane module for the hollow-fibre membrane surface on saturating pure top layer, links enzyme mebrane reactor.The 5L waste edible oil is injected grease storage tank 1, walk membrane module 3 shell sides through pump 2, flow velocity is 4L/h; Methyl alcohol in the low-carbon alcohol storage tank 9 is walked membrane module 3 tube sides by pump 8, and flow velocity is 20L/h.Circulation 10h artifact diesel oil yield is about 95%.
Embodiment 12
It is that basement membrane and polydimethylsiloxane are the composite hollow fiber membrane surface on pure top layer that the lipase that derives from Candida antarctica is fixed in the polyimide by physical adsorption, makes membrane module, links enzyme mebrane reactor.0.5L is refined oil the pin material inject grease storage tank 1, walk membrane module 3 shell sides through pump 2, flow velocity is 1L/h; Methyl alcohol in the low-carbon alcohol storage tank 9 is walked membrane module 3 tube sides by pump 8, and flow velocity is 2L/h.Circulation 10h artifact diesel oil yield is about 95%.
Embodiment 13
It is that basement membrane and polydimethylsiloxane are the composite hollow fiber membrane surface on pure top layer that the lipase that derives from Candida antarctica is fixed in the polyvinylidene difluoride (PVDF) by physical adsorption, makes membrane module, links enzyme mebrane reactor.The mixture of 2L rapeseed oil and 3L soybean oil is injected grease storage tank 1, walk membrane module 3 shell sides through pump 2, flow velocity is 4L/h; Methyl alcohol in the low-carbon alcohol storage tank 9 is walked membrane module 3 tube sides by pump 8, and flow velocity is 20L/h.Circulation 6h artifact diesel oil yield is about 96%.
Claims (5)
1. one kind prepares method of bio-diesel oil by immobilized lipase-alcohol permselective membrane bio-reactor, it is characterized in that: lipase is fixed in pure hollow-fibre membrane surface by physical adsorption, the membrane module of preparation immobilized lipase, be assembled into enzyme-film bioreactor then, grease is walked the shell side of membrane module through pump, flow velocity is 1~5L/h, the while flow velocity is the tube side that the low-carbon alcohol of 2~100L/h is walked membrane module, and see through hollow-fibre membrane and enter the membrane module shell side, under catalytic action of immobilized lipase, promptly be converted into biofuel behind grease and the low-carbon alcohol circulating reaction 2~10h.
2. prepare method of bio-diesel oil by claim 1 is described by immobilized lipase-alcohol permselective membrane bio-reactor, it is characterized in that described lipase is the lipase that derives from Candida antarctica, Rhizomucor miehei, Thermomyces lanuginosus, Burkholderia acepacia, Pesudomonas fluorescens, Aspergillus niger, Mucor miehei or Candida rugosa.
3. prepare method of bio-diesel oil by claim 1 is described by immobilized lipase-alcohol permselective membrane bio-reactor, it is characterized in that described pure hollow-fibre membrane for can selective permeation methyl alcohol or alcoholic acid silicone rubber membrane or chitosan film, or be the composite membrane on top layer with silicone rubber membrane or chitosan film; Described silicone rubber membrane is polydimethylsiloxane or poly-trimethyl silicane propine, and the basement membrane of described composite membrane is polyester, polypropylene, polyethylene, polyvinylidene difluoride (PVDF), polyacrylonitrile, polyethersulfone, polyvinyl alcohol, Mierocrystalline cellulose or polyimide.
4. prepare method of bio-diesel oil by claim 1 is described by immobilized lipase-alcohol permselective membrane bio-reactor, it is characterized in that described grease is a kind of or mixture in fish oil, lard, Viscotrol C, rapeseed oil, soybean oil, peanut oil, Semen Maydis oil, Oleum Gossypii semen, Rice pollard oil, algae grease, waste edible oil and the oil refining pin material.
5. prepare method of bio-diesel oil by claim 1 is described by immobilized lipase-alcohol permselective membrane bio-reactor, it is characterized in that described low-carbon alcohol is methyl alcohol or ethanol or their mixture.
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US10526299B2 (en) | 2004-12-22 | 2020-01-07 | Chemtor, Lp | Fiber conduit reactor with a heat exchange medium inlet and a heat exchange medium outlet |
US9168469B2 (en) | 2004-12-22 | 2015-10-27 | Chemtor, Lp | Method and system for production of a chemical commodity using a fiber conduit reactor |
US8128825B2 (en) * | 2004-12-22 | 2012-03-06 | Chemtor, Lp | Method and system for production of biofuels using a fiber conduit reactor |
CN101747923A (en) * | 2008-12-09 | 2010-06-23 | 上海华阜科技发展有限公司 | Process method for preparing biodiesel |
CN101418322B (en) * | 2008-12-11 | 2011-09-14 | 清华大学 | Method for preparing biodiesel through catalysis of renewable lipin by lipase recovered by membrane |
US8865950B2 (en) * | 2011-08-10 | 2014-10-21 | Saudi Arabian Oil Company | Olefin hydration process with an integrated membrane reactor |
CA2924459C (en) | 2012-09-18 | 2021-04-06 | Chemtor, Lp | Use of a fiber conduit contactor for metal and/or metalloid extraction |
CN104705422B (en) * | 2013-12-16 | 2020-10-30 | 丰益(上海)生物技术研发中心有限公司 | Method for preparing grease by enzyme method |
CN109569469A (en) * | 2019-01-30 | 2019-04-05 | 北京今大禹环境技术股份有限公司 | A kind of chemistry micro-reaction device and its application method |
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