TWI576430B - 具高co質量轉移係數之合成氣發酵的方法和裝置 - Google Patents
具高co質量轉移係數之合成氣發酵的方法和裝置 Download PDFInfo
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- TWI576430B TWI576430B TW101121891A TW101121891A TWI576430B TW I576430 B TWI576430 B TW I576430B TW 101121891 A TW101121891 A TW 101121891A TW 101121891 A TW101121891 A TW 101121891A TW I576430 B TWI576430 B TW I576430B
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- clostridium
- gas
- reactor vessel
- syngas
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Description
本申請案係補充美國專利暫時申請案號61/571,564與61/571,565,二者皆於2011年6月30日提申,以及61/573,845,於2011年9月13日提申,這些案件皆在此併入本案以作為參考資料。
係提供一種方法與裝置,可增進一氧化碳(CO)之質量轉移。更特別的是,如合成氣品質、合成氣分散、反應器壓力與混合等因素皆經平衡,以提供增進之體積性CO質量轉移係數,在合成氣發酵過程中。
厭氧微生物可藉由使氣體受質發酵,而自一氧化碳(CO)製造乙醇。使用梭菌屬(Clostridium)厭氧微生物發酵法可產生乙醇以及其他有用的產物。例如,美國專利號5,173,429描述楊氏梭菌(Clostridium ljungdahlii)ATCC No.49587,一種可由合成氣製造乙醇與醋酸酯之厭氧菌。美國專利號5,807,722描述一種可使用楊氏梭菌(Clostridium ljungdahlii)ATCC No.55380將廢氣轉換為有機酸與醇類之方法與裝置。美國專利號6,136,577係描述一種可使用楊氏梭菌(Clostridium ljungdahlii)ATCC No.55988與55989a將廢棄物轉換為乙醇之方法與裝置。
CO通常可使用於發酵過程,作為合成氣氣體受質之一部分。含碳物質之氣化可製造生產氣或合成氣體或合成
氣,包括技術上已知之一氧化碳與氫。一般而言,此氣化過程涉及碳物質之部分氧化或空氣限制氧化作用,其中次化學計量之氧係提供於氣化過程中,以促進一氧化碳產生,如WO 2009/154788中所述。
氣相受質之發酵為一大挑戰,由於至少部分氣體受質需溶於水相發酵液中,之後受質才可由微生物培養物固定。提供微生物碳源與能量源之氣相受質發酵特別困難,這是由於需要大量之受質溶解於發酵液中,之後才能進行代謝。受質如CO,其在水相發酵液中溶解度相當低,需要高效率之質量轉移至水相發酵液中,如此CO才可提供作為厭氧發酵之碳源。如何增進CO之質量轉移係描述於美國專利號5,972,661與7,201,884,以及WO 2011/028137中。
係提供一種可在合成氣發酵過程中有效增進體積CO質量轉移係數之方法與裝置。在一觀點中,係提供一種合成氣發酵之方法,包含經由氣體分佈器或氣體分散器導入該合成氣至反應器容器中。該氣體分佈器位於反應器容器之液面下,該合成氣以可有效維持反應器容器內部壓力至少約1 psig,且在另一觀點中,至少約10 psig之流速導入。該合成氣具CO/CO2莫耳濃度比例至少約0.75。輸入約0.01至約12 kWatts/m3培養液之攪動能量至該反應器容器。該方法可有效提供STY至少約10 g乙醇/(L日),以及體積CO質量轉移係數約100至約1500每小時。
在另一觀點中,係提供一種合成氣發酵之方法,包含經由氣體分佈器導入該合成氣至反應器容器中。該氣體分佈器位於反應器容器之液面下,該合成氣以可有效維持反應器容器內部壓力至少約1 psig,且在另一觀點中,至少約10 psig之流速導入。該合成氣具CO/CO2莫耳濃度比例至少約0.75,以及在另一觀點中,該合成氣具CO含量至少約20莫耳%。該合成氣與位於氣體分佈器上方之至少一氣體分散葉輪接觸,並以位於氣體分散葉輪上方之至少一混合葉輪混合該合成氣與產乙酸菌。該氣體分散葉輪與混合葉輪係經由驅動軸操作性地聯結至攪拌器上。該攪拌器輸入約0.3至約12 kWatts/m3培養液之攪動能量,在另一觀點中,約0.7至約12 kWatts/m3,在另一觀點中,約0.9至約12 kWatts/m3培養液。該方法可有效提供體積CO質量轉移係數約100至約1500每小時。
在一觀點中,該氣體分佈器包括直徑為10 mm或更小之孔洞,在另一觀點中,該孔洞具2.5 mm或更小之直徑。合成氣亦可以25 m/秒或更高之氣體速率由該孔洞之出口導入該反應器中,及/或該合成氣越過分佈器後之壓力下降值為約0.5至約2.5 psi。
在另一觀點中,係提供一種增進體積CO質量轉移係數之方法。該方法包含經由氣體分佈器導入該合成氣至反應器容器中,該氣體分佈器位於反應器容器之液面下,該合成氣以可有效維持反應器容器內部壓力至少約1 psig,且在另一觀點中,至少約10 psig之流速導入。該合成氣具
CO/CO2莫耳濃度比例至少約0.75,在另一觀點中,該合成氣具CO含量至少約20莫耳%。該合成氣與至少一氣體分散葉輪與一混合葉輪接觸。該氣體分散葉輪與混合葉輪係經由驅動軸操作性地聯結至攪拌器上。該攪拌器輸入約0.3至約12 kWatts/m3培養液,在另一觀點中,約0.7至約12 kWatts/m3培養液,在又一觀點中,約0.9至約12 kWatts/m3培養液之攪動能量。該方法可有效提供體積CO質量轉移係數約100至約1500每小時。
係提供一種生物反應器,包含一定義出反應器容器之外殼,該反應器容器可有效維持壓力於至少約1 psig,在另一觀點中,至少約10 psig。一攪拌器,至少部分置於反應器容器中,且至少部分位於反應器容器液面下方。該攪拌器可操作性地與驅動軸聯結,該攪拌器可有效輸入約0.3至約12 kWatts/m3培養液,在另一觀點中,約0.7至約12 kWatts/m3培養液,在又一觀點中,約0.9至約12 kWatts/m3培養液之攪動能量。至少一混合葉輪,操作性地與驅動軸聯結,並置於培養液液面下方,且至少一氣體分散葉輪,操作性地與驅動軸聯結,並置於混合葉輪下方。一氣體分散器,位於氣體分散葉輪下方,該氣體分散器包括直徑為10 mm或更小之孔洞,可於該孔洞出口處有效提供氣體速率約25 m/秒或更高。該生物反應器可更包含位於反應器容器下方終端之靴形部位。
在另一觀點中,係提供一種生物反應器,包含一定義出反應器容器之外殼,該反應器容器可有效維持壓力於至
少約1 psig,在另一觀點中,至少約10 psig。一攪拌器,至少部分置於反應器容器中,且至少部分反應器容器液面下方。該攪拌器可操作性地與驅動軸聯結,該攪拌器可有效輸入約0.3至約12 kWatts/m3培養液,在另一觀點中,約0.7至約12 kWatts/m3培養液,在又一觀點中,約0.9至約12 kWatts/m3培養液之攪動能量。至少一混合葉輪,操作性地與驅動軸聯結,並置於培養液液面下方,且至少一氣體分散葉輪,操作性地與驅動軸聯結,並置於混合葉輪下方。一氣體分散器,位於氣體分散葉輪下方,該氣體分散器包括直徑為10 mm或更小之孔洞,可於該孔洞出口處有效提供氣體速率約25 m/秒或更高。該生物反應器可更包含位於反應器容器較低下方之靴形部位,該靴形部位包括一靴形部位分散器與靴形部位混合器。
在另一觀點中,係提供一種合成氣之發酵方法,包括將產乙酸菌植入位於反應器容器靴形部位位置之培養液中,該培養液可有效填充靴形部位總體積至少約75%。將該產乙酸菌與合成氣接觸一段時間,該段時間可有效提供細胞密度至少約5克每公升。加入培養液至該反應器容器中,以提供反應器容器液面。經由氣體分佈器導入該合成氣至反應器容器中,該氣體分佈器位於反應器容器之液面下,該合成氣以可有效維持反應器容器內部壓力至少約1 psig,在另一觀點中為約10 psig之流速導入。該合成氣具CO/CO2莫耳濃度比例至少約0.75,與位於氣體分佈器上方之至少一氣體分散葉輪接觸。以位於氣體分散葉輪上方之
至少一混合葉輪混合該合成氣與產乙酸菌。該氣體分散葉輪與混合葉輪係經由驅動軸操作性地聯結至攪拌器上。該攪動能量輸入約0.3至約12 kWatts/m3培養液。該方法可有效提供體積CO質量轉移係數約100至約1500每小時。
在另一觀點中,係提供一種合成氣之發酵方法,包括將產乙酸菌植入位於反應器容器靴形部位位置之培養液中,該培養液可有效填充靴形部位總體積至少約75%。將該產乙酸菌與合成氣接觸一段時間,該段時間可有效提供細胞密度至少約3克每公升。加入培養液至該反應器容器中,並維持細胞密度至少3克每公升。加入培養液直至達到反應器容器之液面。經由氣體分佈器導入該合成氣至反應器容器中。該氣體分佈器位於反應器容器之液面下。該合成氣以可有效維持反應器容器內部壓力至少約1 psig之流速導入,在另一觀點中為約10 psig。該合成氣具CO/CO2莫耳濃度比例至少約0.75,將該合成氣與位於氣體分佈器上方之至少一氣體分散葉輪接觸。以位於氣體分散葉輪上方之至少一混合葉輪混合該合成氣與產乙酸菌。其中該氣體分散葉輪與混合葉輪係經由驅動軸操作性地聯結至攪拌器上,該攪拌器提供約0.3至約12 kWatts/m3培養液之能量輸入。該方法可有效提供體積CO質量轉移係數約100至約1500每小時。
上述以及其他觀點、特徵與該方法數種態樣之優點,將由下列圖示更臻清楚。
第1圖為生物反應器之透視圖。
第2A與2B圖為氣體入口/分佈器之底部圖。
第3圖為氣體分佈器之橫截面圖。
第4A與4B圖為反應器容器之頂部橫截面圖,顯示不同之葉輪組合。
第5圖為生物反應器靴形部位之另一配置。
在各圖示中,相對應之參考字母代表相對應之元件。熟習此技術領域者應瞭解到圖示中之元件僅用於簡化且清楚說明,並不一定照實際規格畫出。例如,在圖示中某些元件尺寸可能被放大,相對於其他元件,以幫助瞭解本發明方法與裝置之各種態樣。同時,在工業上常見中可使用但非必須之常見但已知之元件,經常未被指出,這是為了使各觀點之透視圖較不複雜。
下列描述並非用於限制,僅用於描述示範實施例之一般原則。本發明之範疇應以申請專利範圍中所描述為準。
合成氣發酵效率可藉由增強可增加體積性CO質量轉移係數之條件而增進。於此係提供可有效提供體積性CO質量轉移係數達約100至約1500每小時,在另一觀點中,達約200至約1100每小時,在另一觀點中,達約200至約900每小時,在另一觀點中,達約300至約800每小時,在另一觀點中,達約400至約700每小時,在另一觀點中,約500至約600每小時之方法與裝置。影響CO質量轉移係數之變數包括合
成氣導入情況、反應器容器壓力、合成氣品質,以及氣體分散與混合情況。
於此描述之方法可有效提供高產能。在此觀點中,該方法可有效提供STY(空間時間產率)至少約10 g乙醇/(L.日)。可能之STY值包括約10 g乙醇/(L.日)至約200 g乙醇/(L.日),在另一觀點中,約10 g乙醇/(L.日)至約160 g乙醇/(L.日),在另一觀點中,約10 g乙醇/(L.日)至約120 g乙醇/(L.日),在另一觀點中,約10 g乙醇/(L.日)至約80 g乙醇/(L.日),在另一觀點中,約20 g乙醇/(L.日)至約140 g乙醇/(L.日),在另一觀點中,約20 g乙醇/(L.日)至約100 g乙醇/(L.日),在另一觀點中,約40 g乙醇/(L.日)至約140 g乙醇/(L.日),以及,在另一觀點中,約40 g乙醇/(L.日)至約100 g乙醇/(L.日)。
除非另有指出,下列於本發明說明書中全篇使用之術語係依據以下定義,並可包括該定義之單數與複數形式:
術語“約”係修飾任一數值,代表該數值在真實條件,如在實驗室、試驗工廠或生產工廠中之數量變異度。例如,當混合物中之某一成分或數量之測量值以“約”修飾時,包括在生產工廠或實驗室中測量時所使用之變異度與程度。例如,當產物中某一成分之含量以“約”修飾時,則包括在工廠或實驗室中,多次實驗之各批次間之變異度,以及該分析方法本身就有的變異度。不論是否以“約”修飾,該數量接包括這些數值之等效值。於此陳述與以“約”修飾之任何數量亦可使用於本發明揭示中,如同未經“約”修飾者。
“含碳材料”使用於此係指富含碳的材料,如煤炭與石化材料。然而,在本說明書中,含碳材料包括任何碳材料,不論為固體、液體、氣體或漿體狀態。在數種可考慮作為含碳材料之項目中,本發明揭示包含:含碳材料、含碳液體產物、含碳工業液體再循環物、含碳都市固體廢物(MSW或msw)、含碳城市廢液、含碳農業材料、含碳森林材料、含碳廢棄木材、含碳建築材料、含碳蔬菜材料、含碳工業廢料、含碳發酵廢料、含碳石化副產物、酒精製造過程之含碳副產物、含碳煤、輪胎、塑膠、廢棄塑膠、焦爐焦油、纖維柔軟物(fibersoft)、木質素、黑液、聚合物、廢聚合物、聚對苯二甲酸乙二醇酯(PETA)、聚苯乙烯(PS)、污水污泥、動物糞便、作物殘餘物、能源作物、森林加工殘餘物、木材加工殘餘物、禽畜糞便、家禽廢物、食品加工殘餘物、發酵過程中的廢物、乙醇副產物、糟粕、失效微生物(spent microorganisms),或其組合。
術語“纖維柔軟物”或“柔軟纖維”或“纖維軟布”或“纖維性軟布”係指一種含碳材料,由多種物質軟化與濃縮而製成;例如各種經由蒸汽高溫高壓滅菌製備之含碳材料。在另一範例中,纖維柔軟物可包括都市、工業、商用與醫療廢棄物之柔軟纖維之蒸汽高溫高壓滅菌物。
術語“都市固體廢棄物”或“MSW”或“msw”代表包括居家、商用、工業及/或殘餘廢棄物之廢棄物。
術語“合成氣”或“合成氣體”代表含有各種含量之一氧化碳與氫之氣體混合物之合成氣體。製造方法之範例包括
天然氣或碳氫化合物之蒸汽再形成、煤炭之氣化,以及某些廢棄物轉化能量之氣化設施。此名稱是由於它們作為產生合成天然氣(SNG),以及製造氨或甲醇之中間物之用途。合成氣包含作為製造用於燃料或潤滑劑之合成石油之中間物,經由Fischer-Tropsch合成法,以及先前之汽車甲醇轉化汽油之製程之中間物。合成氣主要是由氫、一氧化碳與某些二氧化碳組成,具有小於天然氣一半之能量密度(即BTU含量)。合成氣為可燃,且通常使用作為燃料來源或生產其他化學物質之中間物。
術語“發酵”、“發酵製程”或“發酵反應”及類似術語,係包含該製程之生長相與產物生合成相。在一觀點中,發酵係指CO轉化為醇類。
術語“質量轉移”使用於此係相關於將原子或分子,尤其是受質原子或分子由氣相轉移至水性溶液中。質量轉移係數可依據Younesi等人(Iranian Journal of Biotechnology,Vol.4,No.1,January 2006)描述之函數計算,在此併入本案以作為參考資料。下列函數代表CO生物轉換(XCO),以及體積質量轉移係數:
kLa:體積質量轉移係數
XCO:% CO生物轉換
R:常數
T:溫度
VL:液體體積
H:亨利常數(CO=1.226公升.atm.mmol-1)
vg:氣體體積
術語“增進效率”、“效率增加”以及類似術語,當與發酵製程相關時,係包括增加發酵時微生物之生長速率、消耗每單位體積或質量之受質(如一氧化碳)而產生之希望產物(如醇類)之體積或質量、希望產物之生產量或生產速率,以及希望產物與其他發酵副產物之相關比例。
第1圖為生物反應器裝置之透視圖。該生物反應器裝置包括一外殼105,定義出反應器容器100。反應器容器100實質上可為圓柱型,且反應器容器之橫截面可塑形為圓形,實質上為環狀,或其他可有效增進混合與質量轉移之形狀。外殼105可以任何可承受操作壓力,至少約1 psig至上限至少約250 psig,且可與培養液相容之材料製成。在各觀點中,可使用下列壓力,約5至約200 psig、約5至約100 psig、約5至約50 psig、約5至約25 psig、約10至約200 psig、約10至約100 psig、約10至約50 psig、約10至約25 psig、約15至約200 psig、約15至約100 psig、約15至約50 psig、約15至約25 psig、約20至約200 psig、約20至約100 psig、約20至約50 psig,以及約20至約25 psig。某些適合之材料範例包括不鏽鋼、具適當內襯之鋼板與玻璃。
如第1圖所示,合成氣經由氣體入口/分散器/分佈器120進入反應器容器100。藉由與驅動軸200連結之至少一氣體分散葉輪225與至少一混合葉輪220,來達成合成氣之散佈
與進一步混合。驅動軸200係由攪拌支撐板210支撐。氣體經排出閥170自反應器容器100排出。反應器容器100亦可包括檔板300,以增進混合效果。在此觀點中,檔板300可延伸約25%至未氣化液面115上方,以形成較高之操作液面,若系統發現有低發泡性。
在另一觀點中,反應器容器100可包括添加口230。添加口230可包括如一或多個酸添加口、一或多個鹼添加口,以及一或多個中性物添加口。在此觀點中,添加口可沿著反應器容器周圍等距分佈。各口可位於相同或不同水平面上。在一觀點中,反應器容器100包括至少4個等距之培養液添加口,鄰近於混合葉輪220。該口可沿著反應器容器100周圍等距分佈,角度為45°。
氣化液面110與未氣化液面115係維持於反應器容器100中。維持未氣化液面115於反應器容器100中,可使質量轉移更有效率,並可幫助控制發泡。在此觀點中,未氣化液面115係維持於反應器容器100中,可有效提供頂部空間至少約反應器容器100總體積之1%。在另一觀點中,未氣化液面115係提供頂部空間為反應器容器100總體積之約1至約75%。在各觀點中,該頂部空間可包括下列反應器總體積之百分比:約5至約50%、約10至約50%、約15至約50%、約20至約50%、約25至約50%、約30至約50%、約30至約40%,以及約30至約35%。反應器容器100亦可包括至少一液體入口130,其可幫助控制發泡,並可調整反應器之液體體積。該液體入口130可為噴嘴形式。反應器容器100
亦可包括添加口190。
如第1圖所示,反應器容器100亦可包括靴形部位400與位於靴形部位內部之震盪斷路器410,其位於培養液出口420上方。靴形部位400與震盪斷路器410可有效預防氣體經由培養液出口420排出。經由培養液出口420排出之培養液可送回培養液再循環迴圈450或培養液過濾迴圈460中。培養液再循環迴圈450中之培養液可送至冷卻/加熱交換器500中,經冷卻之培養液510可循環回反應器容器100中。
靴形部位400可有效使靴形部位400中產生之氣泡送回反應器容器100中。在此觀點中,靴形部位400中之液體應盡可能不要攪動,且氣體送出靴形部位400之速率應快於液體吸入靴形部位中之速率。在此觀點中,小於約2%之氣體經由培養液出口420吸至幫浦中。
來自培養液過濾迴圈460之培養液可送至再循環過濾器600中。經濃縮之細胞610返回反應器容器100中,經滲透作用620送出,進行進一步處理。進一步處理可包括分離出希望之產物如乙醇、醋酸與丁醇。
在另一觀點中,生物反應器可不配置葉輪。例如,生物反應器可配置為氣體上抬形式反應器,或氣泡管柱形式反應器。在這些反應器配置中,係提供約0.01至約12 kWatts/m3培養液之攪動能量。
合成氣經氣體入口/分佈器120引入生物反應器中。合成氣可自任何已知來源提供。在一觀點中,合成氣可來自
含碳材料氣化來源。氣化涉及生物物質在氧氣限制性供應中之部分燃燒。所得氣體主要包括CO與H2。在此觀點中,合成氣包含至少約20莫耳% CO,在一觀點中,約20至約100莫耳% CO,在另一觀點中,約30至約90莫耳% CO,在另一觀點中,約40至約80莫耳% CO,在另一觀點中,約50至約70莫耳% CO。該合成氣具有CO/CO2莫耳濃度比例至少約0.75。某些適當之氣化方法與裝置範例係提供於美國專利系列號61/516,667、61/516,704與61/516,646,這些文獻皆於2011年4月6日提申,並在此併入本案以作為參考資料。
該生物反應器可包括一CO濃度梯度,其中接近分佈器之CO濃度較反應器較高處之CO濃度高。在此觀點中,該生物反應器包括生物反應器底部(分佈器高度)之CO濃度比生物反應器上部之CO濃度比例約100:1至約10:1。
影響CO質量轉移至水性培養液中之轉移速率之一因素為包括CO之氣體受質之分壓。在此觀點中,該質量轉移速率可由於氣流中CO比例增加而增加,該比例增加係藉由濃縮或移除不希望之成分而達成。在此觀點中,該氣流具有小於約10 ppm之氧化或未氧化芳香族化合物。
第2A與2B圖為氣體入口/分佈器120之底視圖。在此觀點中,氣體入口/分佈器120可包括入口導管530,與分佈器組件540聯結。分佈器組件540一般可為環狀或圓形,如圖所示,或任何其他形狀,如直線、長方形或任意形狀。在此觀點中,當分佈器組件540為環狀時,該分佈器組件540之直徑為氣體分散葉輪225之約30至約100%,在多種其他
觀點中,約40至約90%、約40至約80%,以及約50至約70%。
分佈器組件540之底部部分包括複數個孔洞550。孔洞550之直徑可有效提供孔洞出口處之氣體速率為約25m/秒或更大,在另一觀點中,孔洞出口處之氣體速率為約25m/秒至約75m/秒。在多種觀點中,該氣體速率可包括下列範圍:約25至約75m/秒、約25至約50m/秒、約25至約40m/秒、約25至約30m/秒、約30至約75m/秒、約30至約50m/秒、約30至約40m/秒、約35至約75m/秒、約35至約50m/秒、約35至約40m/秒、約40至約75m/秒、約40至約50m/秒,以及約50至約75m/秒。在此觀點中,該孔洞之直徑為約10mm或更低,在另一觀點中,直徑約2.5mm至約1.0mm。
第3圖為分佈器組件540之橫截面圖。在此觀點中,點狀箭頭代表氣體通過孔洞550之流向。角度120°之直線指向分佈器組件中點(以α表示)。孔洞可以任何角度沿著分佈器組件配置。在一觀點中,該分佈器組件540包括約1至約5排平行孔洞550。孔洞550係間隔分開,並指向向下方向。如第3圖所示,分佈器組件540包括5排平行孔洞550,總共790個孔洞,分隔30°配置。孔洞方向向下可有效預防壅塞或堵塞,並使回流至分佈器組件540之情況降至最低。
請再次參照第1圖,反應器容器100更包括一混合組件,其包括一驅動軸200、至少一混合葉輪220,以及至少一氣體分散葉輪225。混合葉輪220一般位於液面110下方。
在一觀點中,反應器容器100包括二或多個混合葉輪220。氣體分散葉輪225位於混合葉輪220下方。反應器容器100可包括一或二或多個氣體分散葉輪225。
請參照第4A圖,每一混合與氣體分散葉輪組件包括輪轂500與葉輪組,沿著驅動軸200排列。每一葉輪包括臂510,聯結至輪轂500並支撐一或多個葉片520。葉片可為混合葉輪或氣體分散葉輪。混合葉輪組件包括至少2個葉片,至多6個葉片。混合葉輪之範例包括低動能葉輪,如船用葉輪或船用螺旋槳。在另一觀點中,氣體分散葉輪組件包括至少2個葉片,至多6個葉片。氣體分散葉輪之範例包括高動能葉輪如Rushton葉輪或凹型葉輪。第4B圖類似於第4A圖,除了葉片520直接聯結至輪轂500之外。
由於驅動軸200轉動,由氣體入口/分佈器導入之合成氣會被包入培養液之小泡泡中,並沿著反應器容器100之圓形橫截面移動。驅動軸係操作性地聯結至適當之攪拌器,如電動馬達、馬達與齒輪箱,或液壓馬達上並隨之轉動。在此觀點中,攪拌器係提供能量輸入約0.3至約12kWatts/m3,在另一觀點中,約0.7kWatts/m3至約12kWatts/m3,以及在一重要觀點中,0.9kWatts/m3至約12kWatts/m3培養液。
依據本發明之一觀點,該發酵過程係以加入適當培養液至反應器容器中而開始。反應器容器中所含之液體可包括任一形式之適當營養培養液或發酵液。營養培養液包括
維他命與礦物質,足夠使所使用之微生物生長。適用於使用CO作為碳源之乙醇發酵厭氧培養液為已知。適當之發酵培養液範例係描述於美國專利號7,285,402,在此併入本案以作為參考資料。
培養液係經滅菌移除不希望之微生物,反應器種入希望之微生物。在一觀點中,所使用之微生物包括產乙酸菌。可使用之產乙酸菌範例包括梭菌屬,如楊氏梭菌(Clostridium ljungdahlii菌株),包括描述於WO 2000/68407、EP 117309、美國專利號5,173,429、5,593,886與6,368,819、WO 1998/00558與WO 2002/08438中者,產乙醇梭菌(Clostridium autoethanogenum)菌株(DSM 10061與DSM 19630,DSMZ,德國),包括描述於WO 2007/117157與WO 2009/151342中者,以及Clostridium ragsdalei(P11,ATCC BAA-622)與巴氏鹼性桿菌(Alkalibaculum bacchi)(CP11,ATCC BAA-1772),包括分別描述於美國專利號7,704,723與“Biofuels and Bioproducts from Biomass-Generated Synthesis Gas”,Hasan Atiyeh,在2010年4月29日之Oklahoma EPSCoR年度會議上發表者,以及Clostridium carboxidivorans(ATCC PTA-7827),描述於美國專利申請案2007/0276447中者。其他適用之微生物包括穆爾氏菌(Moorella)屬,包括穆爾氏菌種(Moorella sp.)HUC22-1,以及氧化碳嗜熱菌(Carboxydothermus)屬。這些文獻每一者皆在此併入本案以作為參考資料。可使用二或多種微生物之混合培養物。
某些可使用之細菌範例包括凱伍產乙酸菌(Acetogenium kivui)、潮濕厭氧產乙酸菌(Acetoanaerobium noterae)、伍德乙酸桿菌(Acetobacterium woodii)、巴氏鹼性桿菌(Alkalibaculum bacchi)CP11(ATCC BAA-1772)、Blautia producta、食甲基丁酸桿菌(Butyribacterium methylotrophicum)、Caldanaerobacter subterraneous、Caldanaerobacter subterraneous pacificus、生氫氧化碳嗜熱菌(Carboxydothermus hydrogenoformans)、醋酸梭菌(Clostridium aceticum)、丙酮丁酸梭菌(Clostridium acetobutylicum)、丙酮丁酸梭菌(Clostridium acetobutylicum)P262(DSM 19630,DSMZ,德國)、產乙醇梭菌(Clostridium autoethanogenum)(DSM 19630,DSMZ德國)、產乙醇梭菌(Clostridium autoethanogenum)(DSM 10061,DSMZ德國)、產乙醇梭菌(Clostridium autoethanogenum)(DSM 23693,DSMZ德國)、產乙醇梭菌(Clostridium autoethanogenum)(DSM 24138,DSMZ德國)、氧化碳梭菌(Clostridium carboxidivorans)P7(ATCC PTA-7827)、柯氏梭菌(Clostridium coskatii)(ATCC PTA-10522)、卓氏梭菌(Clostridium drakei)、楊氏梭菌(Clostridium ljungdahlii)PETC(ATCC 49587)、楊氏梭菌(Clostridium ljungdahlii)ERI2(ATCC 55380)、楊氏梭菌(Clostridium ljungdahlii)C-01(ATCC 55988)、楊氏梭菌(Clostridium ljungdahlii)O-52(ATCC 55889)、大梭菌(Clostridium magnum)、巴斯德梭菌(Clostridium pasteurianum)(DSM 525,DSMZ,德國)、
拉氏梭菌(Clostridium ragsdali)P11(ATCC BAA-622)、臭氣梭菌(Clostridium scatologenes)、熱乙酸梭菌(Clostridium thermoaceticum)、烏氏梭菌(Clostridium ultunense)、庫氏脫硫腸狀菌(Desulfotomaculum kuznetsovii)、林氏真桿菌(Eubacterium limosum)、硫還原泥土桿菌(Geobacter sulfurreducens)、乙酸甲烷八疊球菌(Methanosarcina acetivorans)、巴氏甲烷八疊球菌(Methanosarcina barkeri)、熱乙酸穆爾氏菌(Morrella thermoacetica)、熱自養穆爾氏菌(Morrella thermoautotrophica)、芬氏氧菌(Oxobacter pfennigii)、產胜肽鏈球菌(Peptostreptococcus productus)、產硫胃球菌(Ruminococcus productus)、凱氏熱厭氧菌(Thermoanaerobacter kivui),及其混合物。
種菌後,初始之進料氣體供應速率係建立為可有效供應微生物初使群體存活。流出氣體經分析以測定流出氣體之含量。氣體分析之結果係用於控制進料氣體速率。一旦達到希望之含量,液相與細胞材料便由反應器中抽出,並填滿培養液。在此觀點中,該生物反應器係操作以維持細胞密度為至少約2克/公升,而在另一觀點中,約2至約50克/公升,在各式觀點中,約5至約40克/公升、約5至約30克/公升、約5至約20克/公升、約5至約15克/公升、約10至約40克/公升、約10至約30克/公升、約10至約20克/公升,以及約10至約15克/公升。細胞密度可經由再循環過濾器600控制。在一相關觀點中,該生物反應器係經操作以提供液體遲滯時間約10至約400小時,且在多種觀點中,約10至約300
小時、約10至約200小時、約10至約100小時、約10至約75小時、約10至約60小時、約10至約50小時、約10至約40小時、約10至約30小時,以及約10至約20小時。在此觀點中,液體遲滯時間(LRT)可以下式計算:
合成氣係以可有效維持生物反應器壓力於至少約1 psig之速率導入生物反應器中,而在另一觀點中,壓力為約10至約250 psig。在各式觀點中,壓力可為約10至約200 psig、約10至約100 psig、約10至約75 psig、約10至約50 psig、約10至約25 psig、約20至約250 psig、約20至約200 psig、約20至約100 psig、約20至約75 psig、約20至約50 psig、約20至約25 psig、約30至約250 psig、約30至約200 psig、約30至約100 psig、約30至約75 psig、約30至約50 psig、約40至約250 psig、約40至約200 psig、約40至約100 psig、約40至約75 psig、約40至約50 psig、約50至約250 psig、約50至約200 psig、約50至約100 psig,以及約50至約75 psig之速率導入生物反應器中。
在一觀點中,在某些尺寸之發酵槽中,合成氣經氣體入口/分佈器120導入之速率為約10至約50 ft3/秒,而在另一觀點中,速率為約25至約35 ft3/秒。壓力藉由控制合成氣之導入速率與氣體自反應器容器排出之速率而控制。壓力可於反應器頂部空間或反應器容器底部測量。
在一觀點中,分佈器孔洞550以及越過孔洞後之壓力下
降,對於增進CO之體積質量轉移速率相當重要。越過分佈器孔洞550之壓力下降值需要夠高,以確保分佈器組件540周圍之氣泡分佈。在此觀點中,分佈器可有效提供越過分佈器孔洞550之壓力下降值為約0.5 psi至約2.5 psi,而在另一觀點中,約1 psi至約2 psi。該分佈器孔洞550提供較其他噴灑形式更佳之優點。例如,分佈器孔洞550可有效防止壅塞,此情況常發生於燒結金屬分佈器。此外,分佈器孔洞550可有效提供一致的氣泡尺寸,幫助增進質量轉移。
另一可能會影響質量轉移速率之因素為氣體遲滯時間。在此觀點中,該生物反應器可有效提供氣體遲滯時間至少約2分鐘,以及,在另一觀點中,氣體遲滯時間約2分鐘至約15分鐘,以及在另一觀點中,約5至約10分鐘。氣體遲滯時間(GRT)可依據下式決定:
溫度與離子強度亦可能對於質量轉移速率有影響。在此觀點中,生物反應器之溫度為約30至約50℃。
另一靴形部位400之配置示於第5圖。在此觀點中,靴形部位400係於開始時使用作為成長反應器。該靴形部位配置為包括一靴形部位分佈器600。該靴形部位亦包括一靴形部位混合器。該靴形部位混合器可以任何已知之混合裝置組裝。例如,氣體混合可以葉輪(圖上未顯示)或氣體抬升形式之發酵器,裝配有通風管620而達成。如第5圖所示,氣體抬升形式之發酵器可有效循環氣泡610,以及靴形部位
400周圍之細胞。其他形式之反應器設計,包括氣泡式反應器,以及額外之氣體迴圈或噴射形式之反應器,皆可使用。
另一靴形部位配置為可種入產乙酸菌至反應器容器靴形部位之培養液中。靴形部位中之培養液佔靴形部位總體積至少約75%,在另一觀點中,至少約80%,在另一觀點中,至少約85%,在另一觀點中,至少約90%,以及在另一觀點中,至少約95%。靴形部位係導入合成氣,並混合一段可有效提供目標細胞密度之時間。在此觀點中,該目標細胞密度為約5至約40克/公升,且在各式觀點中,約5至約30克/公升、約5至約20克/公升、約5至約15克/公升、約10至約40克/公升、約10至約30克/公升、約10至約20克/公升,以及約10至約15克/公升。當達到目標細胞密度時,培養液含量可升高流出靴形部位,並流入反應器容器中至預定高度。在靴形部位中停止噴灑與混合,進行先前描述之發酵過程。
在另一觀點中,靴形部位中之細胞密度可到達至少約3克每公升或此述之任一細胞密度。當達到細胞密度至少約3克每公升,便以可有效將細胞密度維持於至少約3克每公升之速率加入培養液。當達到希望之培養液高度時,在靴形部位中停止噴灑與混合,進行先前描述之發酵過程。
遂進行試驗工廠規格之發酵,以測定kLa。kLa係以約60 g乙醇/(L.日)STY(空間時間產率)進行。kLa之預測係於質量轉移限制條件或零CO溶解濃度下進行。藉由暫時降低氣體
流速或攪拌速率,使得氣體中有過多的細胞而達成。在這些條件下,CO在溶解時便立即進行反應,使得該反應為質量轉移限制。溶解至溶液中之CO等於進料氣體之CO與產物之CO之差異值。在質量轉移限制系統中,此差異值為該反應條件下之質量轉移速率。
所使用之基本公式為kLa=Ckla(Pg/Vl)avb sg其中
kLa=體積質量轉移係數(m3氣體/s/m3液體)
Ckla=特定系統之常數
Pg=氣化攪拌器功率消耗(W)
Vl=液體體積(m3)
vsg=表面氣體速率(m/s)
a=比例增加常數
b=比例增加常數
每一回合係於6 psig(頂部壓力)下開始,測量係於60 g乙醇/(L.日)STY下進行。結果如下:
本發明於此已以各特定實施例、範例與應用進行詳細揭示,多種修飾與變化皆可由熟習此技術領域者依此進行,但仍不脫離本發明範疇,本發明範疇以後附申請專利範圍為準。
100‧‧‧反應器容器
105‧‧‧外殼
110‧‧‧氣化液面
115‧‧‧未氣化液面
120‧‧‧氣體入口/分散器/分佈器
130‧‧‧液體入口
170‧‧‧氣體排出閥
190‧‧‧添加口
200‧‧‧驅動軸
210‧‧‧攪拌支撐板
220‧‧‧混合葉輪
225‧‧‧氣體分散葉輪
230‧‧‧添加口
300‧‧‧檔板
400‧‧‧靴形部位
410‧‧‧震盪斷路器
420‧‧‧培養液出口
450‧‧‧培養液再循環迴圈
460‧‧‧培養液過濾迴圈
500‧‧‧冷卻/加熱交換器、輪轂
510‧‧‧培養液、臂
520‧‧‧葉片
530‧‧‧入口導管
540‧‧‧分佈器組件
550‧‧‧孔洞
600‧‧‧再循環過濾器
610‧‧‧經濃縮之細胞
620‧‧‧滲透作用
第1圖為生物反應器之透視圖。
第2A與2B圖為氣體入口/分佈器之底部圖。
第3圖為氣體分佈器之橫截面圖。
第4A與4B圖為反應器容器之頂部橫截面圖,顯示不同之葉輪組合。
第5圖為生物反應器靴形部位之另一配置。
100‧‧‧反應器容器
110‧‧‧氣化液面
115‧‧‧未氣化液面
120‧‧‧氣體入口/分散器/分佈器
130‧‧‧液體入口
170‧‧‧氣體排出閥
190‧‧‧添加口
200‧‧‧驅動軸
210‧‧‧攪拌支撐板
220‧‧‧混合葉輪
225‧‧‧氣體分散葉輪
230‧‧‧添加口
300‧‧‧檔板
400‧‧‧靴形部位
410‧‧‧震盪斷路器
420‧‧‧培養液出口
450‧‧‧培養液再循環迴圈
460‧‧‧培養液過濾迴圈
500‧‧‧冷卻/加熱交換器
510‧‧‧培養液
600‧‧‧再循環過濾器
610‧‧‧經濃縮之細胞
620‧‧‧滲透作用
Claims (10)
- 一種合成氣厭氧發酵之方法,該方法包含:經由氣體分佈器導入該合成氣至攪拌槽反應器容器中,該氣體分佈器位於該反應器容器之液面下,該合成氣係經由該氣體分佈器中之指向向下方向之孔洞以一流速被導入,該流速有效於提供約0.5至約2.5psi之越過該分佈器後之壓力下降值且有效將該反應器容器內部壓力維持在至少約1psig,其中該合成氣具有至少約0.75之CO/CO2莫耳濃度比;且該方法提供約5至約10分鐘之氣體遲滯時間以及每公升約5至約40克的細胞密度;該合成氣與位於該氣體分佈器上方之至少一氣體分散葉輪接觸;且以位於該氣體分散葉輪上方之至少一混合葉輪混合該合成氣與至少一產乙酸菌,其中該氣體分散葉輪及混合葉輪係經由驅動軸操作性地聯結至攪拌器上,該攪拌器提供約0.9至約12kWatts/m3培養液之攪動能量輸入,其中該方法可有效提供每小時約200至約1100之體積CO質量轉移係數及提供約20g至約140g乙醇/(L.日)之STY。
- 如申請專利範圍第1項之方法,其中於該氣體分佈器包括指向向下方向且直徑為10mm或10mm以下之孔洞。
- 如申請專利範圍第2項之方法,其中該氣體分佈器包括 直徑為2.5mm或2.5mm以下之孔洞。
- 如申請專利範圍第1項之方法,其中該合成氣係以25m/秒或25m/秒以上之氣體速率由該等孔洞之出口導入該反應器容器中。
- 如申請專利範圍第1項之方法,其中該合成氣係以可有效將該反應器容器內部壓力維持在至少約10psig之流速導入。
- 如申請專利範圍第1項之方法,其中該方法可有效提供每公升約10至約40克的細胞密度。
- 如申請專利範圍第1項之方法,其中該方法可有效提供約10至約400小時之液體遲滯時間。
- 如申請專利範圍第1項之方法,其中該合成氣具有至少約20莫耳%之CO含量。
- 如申請專利範圍第1項之方法,其中該合成氣包含小於約10ppm之含氧或不含氧之芳香族化合物。
- 如申請專利範圍第1項之方法,其中該產乙酸菌係選自於由以下所組成之組群:凱伍產乙酸菌(Acetogenium kivui)、潮濕厭氧產乙酸菌(Acetoanaerobium noterae)、伍德乙酸桿菌(Acetobacterium woodii)、巴氏鹼性桿菌(Alkalibaculum bacchi)CP11(ATCC BAA-1772)、Blautia producta、食甲基丁酸桿菌(Butyribacterium methylotrophicum)、Caldanaerobacter subterraneous、產氫氧化碳嗜熱菌(Carboxydothermus hydrogenoformans)、醋酸梭菌(Clostridium aceticum)、 丙酮丁酸梭菌(Clostridium acetobutylicum)、產乙醇梭菌(Clostridium autoethanogenum)(DSM 19630,DSMZ德國)、產乙醇梭菌(Clostridium autoethanogenum)(DSM 10061,DSMZ德國)、產乙醇梭菌(Clostridium autoethanogenum)(DSM 23693,DSMZ德國)、產乙醇梭菌(Clostridium autoethanogenum)(DSM 24138,DSMZ德國)、氧化碳梭菌(Clostridium carboxidivorans)P7(ATCC PTA-7827)、柯氏梭菌(Clostridium coskatii)(ATCC PTA-10522)、卓氏梭菌(Clostridium drakei)、楊氏梭菌(Clostridium ljungdahlii)PETC(ATCC 49587)、楊氏梭菌(Clostridium ljungdahlii)ERI2(ATCC 55380)、楊氏梭菌(Clostridium ljungdahlii)C-01(ATCC 55988)、楊氏梭菌(Clostridium ljungdahlii)O-52(ATCC 55889)、大梭菌(Clostridium magnum)、巴斯德梭菌(Clostridium pasteurianum)(DSM 525,DSMZ,德國)、拉氏梭菌(Clostridium ragsdali)P11(ATCC BAA-622)、臭氣梭菌(Clostridium scatologenes)、熱乙酸梭菌(Clostridium thermoaceticum)、烏氏梭菌(Clostridium ultunense)、庫氏脫硫腸狀菌(Desulfotomaculum kuznetsovii)、林氏真桿菌(Eubacterium limosum)、硫還原泥土桿菌(Geobacter sulfurreducens)、乙酸甲烷八疊球菌(Methanosarcina acetivorans)、巴氏甲烷八疊球菌(Methanosarcina barkeri)、熱乙酸穆爾氏菌(Morrella thermoacetica)、熱自養穆爾氏菌(Morrella thermoautotrophica)、芬氏氧菌 (Oxobacter pfennigii)、產胜肽鏈球菌(Peptostreptococcus productus)、產硫胃球菌(Ruminococcus productus)、凱氏熱厭氧菌(Thermoanaerobacter kivui),及其混合。
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