JP4533496B2 - Fuel production method from biomass - Google Patents
Fuel production method from biomass Download PDFInfo
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- JP4533496B2 JP4533496B2 JP2000072735A JP2000072735A JP4533496B2 JP 4533496 B2 JP4533496 B2 JP 4533496B2 JP 2000072735 A JP2000072735 A JP 2000072735A JP 2000072735 A JP2000072735 A JP 2000072735A JP 4533496 B2 JP4533496 B2 JP 4533496B2
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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
- Y02E50/30—Fuel from waste, e.g. synthetic alcohol or 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
- Y02P20/00—Technologies relating to chemical industry
- Y02P20/50—Improvements relating to the production of bulk chemicals
- Y02P20/54—Improvements relating to the production of bulk chemicals using solvents, e.g. supercritical solvents or ionic liquids
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Description
【０００１】
【発明の属する技術分野】
本発明はバイオマスから燃料を製造する方法、より詳しくは微細藻や草穀類を原料として超臨界水中で分解、低分子化した後、アルコール酵母等によるアルコール発酵やガス化菌によるメタン発酵を行い、エタノールやメタン等の燃料を製造する方法に関する。
【０００２】
【従来の技術】
従来エタノールは石炭、石油等の化石燃料を資源とし、エチレンを経由して化学合成する方法、あるいはトウモロコシ等の穀類のデンプン、微細藻の一部が細胞中に貯えるデンプン、グリコーゲン等（以下、デンプン等という）、又はサトウキビの廃糖蜜を原料として、カビ、酵母等の微生物等により製造されている。
【０００３】
これらのバイオマス資源、特にデンプン等を原料とするエタノールの製造は従来、次の方法で行われている。
(1) デンプン等を抽出分離するために、機械的な手段（超音破砕、爆砕等）、あるいは細胞壁を溶解させる酵素を用いてデンプンを細胞より露出させ、水や有機溶媒を用いて抽出分離する。
(2) 抽出分離したデンプン等は酵素糖化方法や酸による加水分解でブドウ糖まで分解する。
(3) 得られたブドウ糖にアルコール酵母を加えて発酵させ、エタノールに変換させる。
【０００４】
【発明が解決しようとする課題】
上記の従来方法では次のような問題があった。
(1) バイオマス資源の細胞内のデンプンを一旦抽出分離する必要があるが、一般に植物や藻類の細胞壁は強固なものが多く、機械的な破砕に多くの動力を消費したり、高価な細胞壁溶解酵素を必要とする。またデンプン抽出の過程では多量の有機溶媒や遠心分離の動力が必要であり、デンプン以外の残渣が大量に排出される。
(2) 抽出分離したデンプンは生の状態であるため、糖化酵素法等によりブドウ糖まで分解する前に加熱処理（糊化、αデンプン化と称する）を行う工程を要する。
【０００５】
これに対し、超臨界水〔ここでは、臨界点（３７３℃、２２．１ＭＰａ）以下の亜臨界条件から超臨界条件までを含めて広い範囲で超臨界と呼ぶことにする〕を利用すると、バイオマス中の酸素等のヘテロ原子を含むエーテル結合の部位が容易に開裂しブドウ糖レベルにまで低分子化されるため、この分解物を酵母や菌群によりアルコール発酵することでエタノールを得ることができることがこの度見出された。その結果、上述の如き抽出分離工程の負担は軽減され、しかも上述の加熱処理工程は省略される。
【０００６】
【課題を解決するための手段】
本発明は、上記課題の解決のために、以下の（１）、（２）の手段を提供する。
【０００７】
（１）その第１の手段として、バイオマスを収集し、粉砕する工程と、粉砕されたバイオマスに水を加えてスラリー化する工程と、当該スラリーを水の亜臨界状態乃至超臨界状態に保って当該バイオマスに含まれている多糖類を分解、糖化する工程と、しかる後に発酵を行う工程とによって燃料を製造するバイオマスからの燃料製造方法であって、さらに、製造された燃料を分離・濃縮する工程を有し、その残留水をリサイクルし、粉砕径を５ｍｍ以下に粉砕したバイオマスと混合してバイオマスと水のスラリー濃度が水とバイオマスの重量比で１〜１０となるようにスラリー化させた後、このスラリーを温度２５０〜４００℃、圧力１０〜３０ＭＰａの水の亜臨界状態乃至超臨界状態で５分〜１時間保持することによりバイオマス原料をブドウ糖レベルまで分解・低分子化させ、この分解液に任意的に酵母や菌を加えて発酵を行なうことを特徴とするバイオマスからの燃料製造方法を提供する。
（２）第２の手段として、前記発酵がアルコール発酵であり、製造される燃料がエタノールであるか、又は前記発酵がメタン発酵であり、製造される燃料がメタンである、上記（１）に記載のバイオマスからの燃料製造方法を提供する。
【０００８】
本発明の第一の態様は、微細藻や草穀類等のバイオマスを収集、粉砕してスラリーとした後、水の亜臨界状態乃至超臨界状態に保つことにより当該バイオマスに含まれている多糖類を分解、糖化した後、酵母によるアルコール発酵を行いエタノールを製造するプロセスに関する。かかるプロセスは次の工程を含んでなる：
(a) バイオマスを粉砕化する工程；
(b) 粉砕したバイオマスに水を加えスラリー化する工程；
(c) 前記スラリーを水の超臨界状態あるいは亜臨界状態に保ち、当該バイオマスに含まれている多糖類を分解・低分子化する工程；
(d) 分解液に酵母を加えアルコール発酵を行いエタノールを製造する工程；そして
(e) 生成したエタノールを分離・濃縮する工程。
【０００９】
上記プロセスでは、アルコール酵母等によりアルコール発酵を行うのに対して、超臨界水による処理後の分解液にガス化菌を加えてメタン発酵を行い、メタンガスを得ることも可能である。
【００１０】
従って、本発明の第二の態様は、微細藻や草穀類等のバイオマスを収集、粉砕してスラリーとした後、水の亜臨界状態乃至超臨界状態に保つことにより当該バイオマスに含まれている多糖類を分解、糖化した後、ガス化菌等によるメタン発酵を行いメタンを製造するプロセスに関する。かかるプロセスは次の工程を含んでなる：
(a) バイオマスを粉砕化する工程；
(b) 粉砕したバイオマスに水を加えスラリー化する工程；
(c) 前記スラリーを水の超臨界状態あるいは亜臨界状態に保ち、当該バイオマスに含まれている多糖類を分解・低分子化する工程；そして
(d) 分解液にガス化菌を加えメタン発酵を行いメタンを製造する工程。
【００１１】
メタン発酵を行う場合においてもアルコール発酵の場合と同様に燃料の収率を向上させるためにはバイオマスを分解、低分子化しておくことが必要であり、メタン発酵の前に超臨界水を用いてバイオマスを分解することでメタンの収率を向上及び残渣を低減することが可能である。
【００１２】
本発明の好適な態様において、水でスラリー化せしめた粉砕バイオマスを水の亜臨界状態乃至超臨界状態、即ち温度約２００〜５００℃、好ましくは約２５０〜４００℃、より好ましくは約３００〜３５０℃、特に約３００℃、圧力約１０〜４０ＭＰａ、好ましくは約１０〜３０ＭＰａ、より好ましくは約１５〜２５ＭＰａ、特に約２５ＭＰａに、このバイオマスに含まれるデンプン、グリコーゲン、セルロース等の多糖類が分解・低分子化するのに十分な時間、例えば約１分〜約１０時間、好ましくは約５分〜約１時間、より好ましくは約１０分〜約１５、特に約１０分保持する。
【００１３】
本発明におけるバイオマス原料には、微細藻や草穀類等、従来のアルコール発酵やメタン発酵の原料となり得る多糖類を含む様々な植物、微生物等が含まれる。微細藻としてはクロレラ（Ｃｈｌｏｒｅｌｌａ）、ドナリエラ（Ｄｕｎａｌｉｅｌｌａ）、クラミドモナス（Ｃｈｌａｍｙｄｏｍｏｎｕｓ）、セネデスムス、（Ｓｃｅｎｅｄｅｓｍｕｓ）スピルリーナ（Ｓｐｉｒｉｌｌｉｎａ）等が挙げられるが、それらに限定されない。草穀類としては、トウモロコシ、サトウキビ、テンサイ、コムギ、オオムギ、カラスムギ、バレイショ、サツマイモ等，様々な穀類が挙げられるが、それらに限定されない。
【００１４】
本発明におけるアルコール発酵に使用できる酵母には、サッカロマイセス（Ｓａｃｃｈａｒｏｍｙｃｅｓ）属に属する酵母等、アルコール発酵産業において通常使用される酵母が挙げられる。また、ザイモモナス（Ｚｙｍｏｍｏｎａｓ）属細菌も本発明のアルコール発酵に使用できる。ガス化菌としてはメタノコッカス属（Ｍｅｔｈａｎｏｃｏｃｃｃｕｓ）、メタノサルシナ属（Ｍｅｔｈａｎｏｓａｒｃｉｎａ）、メタノバクテリア（Ｍｅｔｈａｎｏｂａｃｔｅｒｉｕｍ）属等に属する代謝産物としてメタンを発生することで知られる様々なメタン細菌が挙げられる。
【００１５】
発酵時間は特に限定されないが、約１０〜１００時間、好ましくは約２０〜６０時間、特に約４０時間程度が好ましい。
【００１６】
本発明により製造される燃料は、発酵がアルコール発酵酵母等によるアルコール発酵の場合はエタノールであり、発酵がガス化菌によるメタン発酵の場合はメタンである。さらに、本発明はアセトンやブタノール発酵によりアセトンやブタノールを製造する場合にも適用され得る。即ち、本発明はバイオマスを原料とし、発酵工程を利用して製造されるあらゆる燃料の製造に有用である。
【００１７】
【発明の実施の形態】
以下に本発明の好適な実施の形態を説明する。
トウモロコシの穀粒をバイオマス原料とし、バイオマス粉砕工程において、ボールミル等の粉砕機で直径約５ｍｍまで粉砕、微細化する（図１：１バイオマス粉砕工程）。粉砕したバイオマスに水を加えてスラリー液とする必要があるが（図１：２スラリー化工程）、ここで水とバイオマスの重量比（水／バイオマス）は１〜１０程度の範囲、好ましくは１〜２程度の範囲が適当である。実験の結果、超臨界水中での分解によりヘキソース等のアルコール発酵の原料が、セルロース等のバイオマス原料に対して３０重量％の収率で得られる。一方、エタノール発酵を行う場合、ヘキソース濃度が高すぎると発酵が起こりにくくなりエタノールの生成速度が低下するため、ヘキソース濃度は１０重量％程度がアルコール発酵において好ましい。従って、超臨界水によるバイオマスの分解において適正な水／バイオマス重量比にする必要がある。
【００１８】
スラリー液を温度２００〜４００℃、圧力２５ＭＰａの条件下で所定時間保持させ、穀粒を分解し、ブドウ糖レベルまで低分子化する（図１：３分解・低分子化工程）。ここで反応時間は反応温度が３００℃において１０分程度とした場合、投入したバイオマスは１００％完全分解し、ブドウ糖レベルまで低分子化する。そして分解液にアルコール酵母を加え、発酵を行いエタノールを製造する（図１：４アルコール発酵工程）。分離・濃縮工程を経て（図１：５分離・濃縮工程）生成されたエタノールは、原料の１０〜３０重量％に相当する。
【００１９】
【実施例】
以下の実施例により本発明のプロセスを具体的に説明する。
バイオマス原料としてセルロース粉末を用い、内容積１０ｍｌのオートクレーブにセルロースを２ｇ、蒸留水を４ｇ充填して密栓して反応器内の温度を２００〜３００℃まで上げて所定時間保持した後、水冷にて強制冷却した。反応器から分解液を取り出し活性炭で濾過した後の分解液にペプトン、酵母エキス、ＭｇＳＯ4 ，ＫＨ2 ＰＯ4 をそれぞれ１．０、０．５、０．２、０．５、０．５重量％となるように添加し、ＮａＯＨでｐＨ８に調整した。これに１白金耳の酵母〔サッカロマイセス・セレビシェ（Ｓａｃｃｈａｒｏｍｙｃｅｓ ｃｅｒｅｖｉｓａｅ）〕（１×１０7 ｃｅｌｌ／ｍｌ）を加えて発酵を行った。生成物をＨＰＬＣで分析したところ、発酵時間２５〜４０時間でエタノールが生成し、最大エタノール濃度は１８．２重量％に達した。以下の表にその結果を示す。
【００２０】
【表１】
【発明の効果】
本発明のプロセスでスラリー化したバイオマスを超臨界水により分解することで、バイオマス資源の細胞内のデンプン等の抽出分離に伴う負担が軽減され、しかも従来技術において必要とされる糊化のための加熱処理工程を省略して、エタノールやメタン等の燃料の収率の向上及び残渣の低減を図ることができる。
【図面の簡単な説明】
【図１】本発明のエタノール製造プロセスのフロー。[0001]
BACKGROUND OF THE INVENTION
The present invention is a method for producing fuel from biomass, more specifically, after decomposing and reducing the molecular weight in supercritical water using microalgae and grass grains as raw materials, alcohol fermentation with alcohol yeast or the like, and methane fermentation with gasification bacteria, The present invention relates to a method for producing a fuel such as ethanol or methane.
[0002]
[Prior art]
Conventionally, ethanol is a method that uses fossil fuels such as coal and petroleum as resources and is chemically synthesized via ethylene, or starch of cereals such as corn, starch in which some microalgae are stored in cells, glycogen, etc. (hereinafter referred to as starch Etc.), or sugarcane waste molasses as a raw material, and is produced by microorganisms such as mold and yeast.
[0003]
The production of ethanol from these biomass resources, particularly starch and the like, has been conventionally performed by the following method.
(1) In order to extract and separate starch, etc., starch is exposed from the cells using mechanical means (sound crushing, explosion, etc.) or an enzyme that dissolves the cell wall, and then extracted and separated using water or an organic solvent. To do.
(2) Extracted and separated starch and the like are degraded to glucose by enzymatic saccharification and acid hydrolysis.
(3) Alcohol yeast is added to the obtained glucose and fermented to convert it to ethanol.
[0004]
[Problems to be solved by the invention]
The above conventional method has the following problems.
(1) It is necessary to extract and separate the starch in the cells of biomass resources, but in general, the cell walls of plants and algae are often strong, and they consume a lot of power for mechanical crushing or expensive cell wall lysis Requires an enzyme. In the starch extraction process, a large amount of organic solvent and centrifugal power are required, and a large amount of residue other than starch is discharged.
(2) Since the extracted and separated starch is in a raw state, it requires a step of performing a heat treatment (referred to as gelatinization or α-starchization) before degrading to glucose by a saccharification enzyme method or the like.
[0005]
On the other hand, if supercritical water (here, it is called supercritical in a wide range including subcritical conditions up to the critical point (373 ° C., 22.1 MPa) to supercritical conditions), biomass is used. Since the site of the ether bond containing a heteroatom such as oxygen is easily cleaved and the molecular weight is reduced to the glucose level, ethanol can be obtained by subjecting this decomposition product to alcohol fermentation with yeasts or fungi. It was discovered this time. As a result, the burden of the extraction and separation process as described above is reduced, and the above-described heat treatment process is omitted.
[0006]
[Means for Solving the Problems]
The present invention, in order to solve the above problems, the following (1), that provides a means (2).
[0007]
(1) As a first means, a step of collecting and pulverizing biomass, a step of adding water to the pulverized biomass to form a slurry, and maintaining the slurry in a subcritical or supercritical state of water A method for producing fuel from biomass in which a polysaccharide is contained in the biomass, which is decomposed and saccharified, and then fermented, and then the produced fuel is further separated and concentrated. The remaining water was recycled and mixed with the biomass pulverized to a pulverized diameter of 5 mm or less, and slurried so that the slurry concentration of biomass and water became 1 to 10 by weight ratio of water and biomass. Thereafter, the biomass raw material is blocked by holding the slurry in a subcritical or supercritical state of water at a temperature of 250 to 400 ° C. and a pressure of 10 to 30 MPa for 5 minutes to 1 hour. To c sugar level is decomposed and low molecular weight, to provide a fuel production process from optionally biomass and performing fermentation by adding yeast or bacteria to the decomposition solution.
(2) As a second means, in the above (1), the fermentation is alcohol fermentation, and the produced fuel is ethanol, or the fermentation is methane fermentation, and the produced fuel is methane. A method for producing fuel from the described biomass is provided.
[0008]
The first aspect of the present invention is a polysaccharide contained in the biomass by collecting and crushing biomass such as microalgae and cereals into a slurry, and then maintaining the water in a subcritical or supercritical state. It is related with the process which manufactures ethanol by carrying out alcoholic fermentation by yeast, after decomposing | disassembling and saccharifying. Such a process comprises the following steps:
(a) pulverizing biomass;
(b) adding water to the pulverized biomass to make a slurry;
(c) maintaining the slurry in a supercritical or subcritical state of water, and decomposing / reducing the polysaccharide contained in the biomass;
(d) adding yeast to the digestion solution to produce ethanol by alcohol fermentation; and
(e) A step of separating and concentrating the produced ethanol.
[0009]
In the above process, while alcoholic fermentation is performed using alcohol yeast or the like, methane gas can also be obtained by adding gasified bacteria to the decomposition solution after the treatment with supercritical water and performing methane fermentation.
[0010]
Therefore, the second aspect of the present invention is contained in the biomass by collecting and crushing biomass such as microalgae and grass grains into a slurry and then maintaining the water in a subcritical or supercritical state of water. The present invention relates to a process for producing methane by decomposing and saccharifying polysaccharides and then performing methane fermentation with gasifying bacteria. Such a process comprises the following steps:
(a) pulverizing biomass;
(b) adding water to the pulverized biomass to make a slurry;
(c) maintaining the slurry in a supercritical or subcritical state of water, decomposing / reducing the polysaccharide contained in the biomass; and
(d) A process of producing methane by adding gasifying bacteria to the decomposition solution and performing methane fermentation.
[0011]
In the case of methane fermentation, as in the case of alcoholic fermentation, it is necessary to decompose and lower the biomass in order to improve the fuel yield. Supercritical water is used before methane fermentation. It is possible to improve the yield of methane and reduce residues by decomposing biomass.
[0012]
In a preferred embodiment of the present invention, the pulverized biomass slurried with water is subcritical to supercritical in water, that is, a temperature of about 200-500 ° C, preferably about 250-400 ° C, more preferably about 300-350. The polysaccharides such as starch, glycogen, and cellulose contained in this biomass are decomposed and decomposed at ℃, particularly about 300 ℃, pressure of about 10 to 40 MPa, preferably about 10 to 30 MPa, more preferably about 15 to 25 MPa, particularly about 25 MPa. It is maintained for a time sufficient for molecular weight reduction, for example, about 1 minute to about 10 hours, preferably about 5 minutes to about 1 hour, more preferably about 10 minutes to about 15, especially about 10 minutes.
[0013]
The biomass raw material in the present invention includes various plants, microorganisms and the like including polysaccharides that can be used as raw materials for conventional alcohol fermentation and methane fermentation, such as microalgae and grass grains. Examples of the microalga include, but are not limited to, Chlorella, Dunaliella, Chlamydomonas, Senedesmus, and Spirulina. Examples of grass cereals include, but are not limited to, corn, sugar cane, sugar beet, wheat, barley, oats, potato, sweet potato, and the like.
[0014]
Examples of yeasts that can be used for alcohol fermentation in the present invention include yeasts commonly used in the alcohol fermentation industry, such as yeasts belonging to the genus Saccharomyces. Also, Zymomonas bacteria can be used for the alcohol fermentation of the present invention. Examples of gasifying bacteria include various methane bacteria known to generate methane as metabolites belonging to the genus Methanococcus, Methanosarcina, and Methanobacteria.
[0015]
The fermentation time is not particularly limited, but is preferably about 10 to 100 hours, preferably about 20 to 60 hours, particularly about 40 hours.
[0016]
The fuel produced according to the present invention is ethanol when fermentation is alcohol fermentation using alcohol-fermenting yeast or the like, and methane when fermentation is methane fermentation using gasification bacteria. Furthermore, the present invention can also be applied to the production of acetone or butanol by acetone or butanol fermentation. That is, the present invention is useful for the production of all fuels produced using biomass as a raw material and utilizing a fermentation process.
[0017]
DETAILED DESCRIPTION OF THE INVENTION
Hereinafter, preferred embodiments of the present invention will be described.
Corn grain is used as a biomass raw material, and is pulverized and refined to a diameter of about 5 mm with a pulverizer such as a ball mill in the biomass pulverization step (FIG. 1: 1 biomass pulverization step). Although it is necessary to add water to the pulverized biomass to form a slurry liquid (FIG. 1: 2 slurrying process), the weight ratio of water to biomass (water / biomass) is in the range of about 1 to 10, preferably 1. A range of about ~ 2 is appropriate. As a result of the experiment, a raw material for alcohol fermentation such as hexose is obtained in a yield of 30% by weight with respect to a biomass raw material such as cellulose by decomposition in supercritical water. On the other hand, when ethanol fermentation is carried out, if the hexose concentration is too high, fermentation hardly occurs and the production rate of ethanol decreases, so that the hexose concentration is preferably about 10% by weight in alcohol fermentation. Therefore, an appropriate water / biomass weight ratio is required in the decomposition of biomass with supercritical water.
[0018]
The slurry liquid is held for a predetermined time under conditions of a temperature of 200 to 400 ° C. and a pressure of 25 MPa to decompose the grain and reduce the molecular weight to the glucose level (FIG. 1: 3 decomposition / low molecularization step). Here, when the reaction time is about 10 minutes at a reaction temperature of 300 ° C., the input biomass is completely decomposed 100%, and the molecular weight is reduced to the glucose level. And alcohol yeast is added to a decomposition solution, and it ferments and manufactures ethanol (FIG. 1: 4 alcohol fermentation process). Ethanol produced through the separation / concentration step (FIG. 1: 5 separation / concentration step) corresponds to 10 to 30% by weight of the raw material.
[0019]
【Example】
The following examples illustrate the process of the present invention.
Cellulose powder is used as a biomass raw material, and 2 g of cellulose and 4 g of distilled water are filled in an autoclave having an internal volume of 10 ml, and the reactor is heated up to 200-300 ° C. and kept for a predetermined time, and then cooled with water. Forced cooling. Peptone, yeast extract, MgSO 4 , KH 2 PO 4 were added to the decomposition solution after taking out the decomposition solution from the reactor and filtering with activated carbon, respectively, 1.0, 0.5, 0.2, 0.5, 0.5 weight. % And adjusted to pH 8 with NaOH. 1 platinum ear yeast [Saccharomyces cerevisiae] (1 × 10 7 cells / ml) was added to this for fermentation. When the product was analyzed by HPLC, ethanol was produced in a fermentation time of 25 to 40 hours, and the maximum ethanol concentration reached 18.2% by weight. The results are shown in the following table.
[0020]
[Table 1]
【The invention's effect】
By decomposing biomass slurried by the process of the present invention with supercritical water, the burden associated with the extraction and separation of starch and the like of biomass resources in the cells is reduced, and for gelatinization required in the prior art By omitting the heat treatment step, it is possible to improve the yield of fuel such as ethanol and methane and reduce residues.
[Brief description of the drawings]
FIG. 1 shows the flow of the ethanol production process of the present invention.
Claims (2)
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