WO2015055072A1 - 活化油藏中产甲烷菌转化二氧化碳生产甲烷的方法 - Google Patents

活化油藏中产甲烷菌转化二氧化碳生产甲烷的方法 Download PDF

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WO2015055072A1
WO2015055072A1 PCT/CN2014/087046 CN2014087046W WO2015055072A1 WO 2015055072 A1 WO2015055072 A1 WO 2015055072A1 CN 2014087046 W CN2014087046 W CN 2014087046W WO 2015055072 A1 WO2015055072 A1 WO 2015055072A1
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reservoir
carbon dioxide
methane
acetate
oil reservoir
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牟伯中
刘金峰
杨世忠
王立影
孙晓博
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华东理工大学
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    • C12P5/00—Preparation of hydrocarbons or halogenated hydrocarbons
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    • C12P5/023—Methane
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    • Y02E50/30—Fuel from waste, e.g. synthetic alcohol or diesel

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  • the invention relates to the technical field of reservoir microbial development and utilization, and particularly relates to a technical method for converting CO 2 to methane by using a reservoir microorganism.
  • the reservoir is a basic gathering of several hundred meters to several kilometers underground, with crude oil having the same pressure system in a single trap.
  • the microorganisms in this environment are characterized by many species, many types of metabolism, interrelated, and relatively stable structure. For a particular reservoir, the microorganisms formed a relatively stable community after a long period of evolution.
  • methane-producing bacteria and methane biosynthesis in water-driven reservoirs has become a universally accepted fact.
  • Methanobacterium thermaggregans which has been isolated from undeveloped reservoirs, has the same thermophilic and salt-tolerant properties as the isolated reservoir environment, indicating that methanogens are typical indigenous bacteria in the reservoir.
  • the analysis determines that at least one of the following species of Syntrophomonadaceae or Thermotogaceae exists in the target reservoir fluid, and at least one of the following bacteria is present: Methanobacterium, Methanothermobacter, Methanolinea, Methanospirillum, Methanoculleus;
  • the present invention utilizes the original microorganisms in the reservoir to reduce CO 2 to CH 4 , which is a complex biological reaction process involving multiple organisms, which requires a plurality of microorganisms to work together, and is most likely in the downstream reaction process.
  • the reaction pathway is that acetic acid is oxidized by acetic acid oxidizing bacteria to produce H 2 , and the hydrogen trophic methanogenic bacteria reproduces methane by using H 2 and CO 2 , and the chain reaction is equivalent to the food chain structure of the microorganism.
  • the study found that the limiting step of the chain reaction is mainly the oxidative hydrogen production process of Syntrophus.

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Abstract

一种活化油藏中产甲烷菌转化二氧化碳生产甲烷的方法，该方法包括如下步骤：（1）分析确定目标油藏流体中至少存在互营单胞菌或热袍菌中的一种菌，同时存在下列菌中的至少一种：甲烷杆菌，嗜热甲烷杆菌，甲烷绳菌，甲烷螺菌，甲烷囊菌；（2）向油藏中注入乙酸或乙酸盐，使油藏水中乙酸或乙酸盐浓度为5.0~10.0mM；（3）收获甲烷。该方法可以大大提高二氧化碳还原型产甲烷速率，具有经济、简便可行等优点。

Description

活化油藏中产甲烷菌转化二氧化碳生产甲烷的方法 技术领域
本发明涉及油藏微生物开发及利用技术领域，具体涉及利用油藏微生物转化CO2产甲烷的技术方法。
背景技术
油藏是位于地下几百米至数千米、原油在单一圈闭中具有同一压力系统的基本聚集。这种环境中孕育的微生物具有物种多、代谢类型多、互相关联、结构相对稳定等特点。对于特定油藏，经长时间的演化适应，其中的微生物形成了较为稳定的群落。目前，水驱油藏中存在着甲烷生成菌和甲烷生物合成已成为普遍接受的事实。从未开发油藏分离到的产甲烷菌Methanobacterium thermaggregans具有的嗜热和耐盐等特性与所分离的油藏环境具有很好的一致性，说明产甲烷菌是油藏中典型的土著菌。
研究证实，CO2地质埋存是减少CO2排放的有效途径。CO2埋存对环境产生的影响小、成本较低，与国际、国内相关政策、法规具有一致性。研究和实践证明，油气藏，特别是濒临枯竭的油气藏是CO2地质埋存最有利的场所。
研究证实，油藏中具有将CO2转化为甲烷的潜力。油藏发育着多种多样的微生物并形成了相对稳定的微生物群落。油田地层水中一般可分离出不同生理群的微生物如好氧的化能异养菌(如烃氧化菌)和厌氧的发酵菌、硫酸盐还原菌、硝酸盐还原菌和产甲烷菌等。本实验室用克隆文库法分析了中国陆上高温(75℃)水驱油藏产出水样中微生物的群落结构，发现高温油藏中存在丰富的微生物，主要为厚壁菌门(Firmicutes)、热袍菌门(Thermotogae)的细菌，氢营养型(Methanomicrobiales，Methanococcale，Methanobacteriales)和乙酸营养型产甲烷菌(Methanosarcinales)等古菌。油藏中发现的产甲烷菌主要包括甲烷杆菌和甲烷八叠球菌，甲烷杆菌中典型菌为布氏甲烷杆菌(M.bryantii)和甲酸甲烷杆菌(M.formicicum)，两者均能利用CO2/H2产甲烷。
油藏中微生物活性低，自然状态下CO2生物转化为甲烷的速率较低。由 于油藏中营养物质匮乏，微生物数量一般较低。Knapp等对Oklahoma州Payne县SEVVSU油田单元油藏中的微生物进行了研究，发现其中产甲烷菌数量仅为2～46个细胞/ml。同样，在Romashkino油田302单元地层中发酵菌浓度约为102～104个细胞/ml，甲烷生成菌浓度约为1～102个细胞/ml。Romashkino油田甲烷主要由重碳酸盐产生，速率为0.0126～0.2786ml CH4·L-1·天-1。西伯利亚Mamontovskoe高温油田在注水井井底区域，甲烷通过HCO3 -和乙酸盐合成，速率为0.0327～5.3130ml CH4·L-1·天-1；在与生产井相连的区域，甲烷主要通过乙酸盐合成，速率为0.0041～0.1291ml CH4·L-1·天-1。由上可见，无论地下油藏条件还是实验室条件，油藏中微生物均具有将CO2生物转化为甲烷的能力，但由于自然条件下油藏微生物浓度低、代谢活性低，CO2生物转化的速率很低，不能满足实际需求。
发明内容
本发明的目的就是为了克服上述现有技术存在的缺陷而提供一种可以大大提高二氧化碳还原型产甲烷速率、经济简便可行的活化油藏中产甲烷菌转化二氧化碳生产甲烷的方法。
本发明的目的可以通过以下技术方案来实现：一种活化油藏中产甲烷菌转化二氧化碳生产甲烷的方法，其特征在于，该方法包括如下步骤：
(1)分析确定目标油藏流体中至少存在互营单胞菌(Syntrophomonadaceae)或热袍菌(Thermotogaceae)中的一种菌，同时存在下列菌中的至少一种：甲烷杆菌(Methanobacterium),嗜热甲烷杆菌(Methanothermobacter)，甲烷绳菌(Methanolinea)，甲烷螺菌(Methanospirillum)，甲烷囊菌(Methanoculleus)；
(2)向油藏中注入乙酸或乙酸盐，使油藏水中乙酸或乙酸盐浓度为5.0～10.0mM；
(3)收获甲烷。
步骤(2)所述的乙酸盐浓度较佳为6.8mM，所述的乙酸盐包括但不限于乙酸盐钠、乙酸钾。
步骤(3)所述的收获甲烷由注入井收获或从采油井收获。
步骤(1)分析确定目标油藏流体中互营单胞菌(Syntrophomonadaceae) 或热袍菌(Thermotogaceae)、甲烷杆菌(Methanobacterium),嗜热甲烷杆菌(Methanothermobacter)，甲烷绳菌(Methanolinea)，甲烷螺菌(Methanospirillum)，甲烷囊菌(Methanoculleus)，可采用文献[International Biodeterioration&Biodegradation]2011年第65期444-450页报道的16S rDNA方法进行分析鉴定。
与现有技术相比，本发明利用油藏中的本源微生物将CO2还原成CH4是多生物参与的复杂生物反应过程，需要多种微生物共同作用才能完成，在下游反应过程中，最可能的反应途径是乙酸被乙酸氧化菌类氧化产生H2，氢营养型的产甲烷菌再利用H2和CO2产生甲烷，此种链式反应情况相当于微生物的食物链结构。研究发现，该链式反应的限制性步骤主要是共生菌(Syntrophus)氧化产氢过程。本发明通过注入短链有机酸盐，刺激互营单胞菌(Syntrophomonadaceae)或/和热袍菌(Thermotogaceae)生长代谢，进而激活下游二氧化碳还原型产甲烷菌，由此提高了还原CO2产甲烷的速率。本发明可以大大提高二氧化碳还原型产甲烷速率，具有经济、简便可行等优点。
附图说明
图1为乙酸钠对产甲烷上游细菌菌群的影响；
图2为乙酸钠对产甲烷菌组成的影响。
具体实施方式
下面结合附图和具体实施例对本发明进行详细说明。
实施例1
分析大庆油田某区块产出液中含有互营单胞菌(Syntrophomonadaceae)和热袍菌(Thermotogaceae)以及嗜热甲烷杆菌(Methanothermobacter)，以该产出液配制2个培养体系(体系组成见表1～3)，55℃下培养180天，体系都没有检测到CH4，表明体系中产甲烷菌活性很低。然后，其中一个体系保持不变，另外一个体系加入0.41g(5mM)乙酸钠，培养12天，在两体系中均检测到了CH4，培养120天后两体系中CH4含量分别为18.3mmol/L(添加乙酸钠)和2.7mmol/L(未添加乙酸钠)。2个体系群落分析见图1和图2。由图1可见，互营单胞菌(Syntrophomonadaceae)丰度由20％(未添加乙酸 钠体系)提高到57％(添加乙酸钠体系)。由图2可见，产甲烷菌Methanothermobacter丰度由52％(未添加乙酸钠体系)提高到98％(添加乙酸钠体系)。表明加入乙酸钠后参与CO2转化产CH4过程或与之密切相关的微生物被激活了或丰度增大了，菌群向有利于还原CO2产甲烷方向演变，同时甲烷产率提高近7倍。
实施例2
分析华北油田某区块产出液中含有9.5％互营单胞菌(Syntrophomonadaceae)及18.3％甲烷杆菌(Methanobacterium)和10.8％甲烷绳菌(Methanolinea)，以该产出液配制2个培养体系(体系组成见表1～3)，38℃下培养100天，两个体系都没有检测到CH4，表明体系中产甲烷菌活性很低。然后保持一个体系不变，在另一个体系中加入0.56g(6.8mM)乙酸钠，继续培养33天后在两体系中检测到了CH4，培养75天后两体系中CH4含量分别为4.7mmol/L(未添加乙酸钠)和22.4mmol/L(添加乙酸钠)。体系中互营单胞菌(Syntrophomonadaceae)丰度由20％(未添加乙酸钠体系)提高到57％(添加乙酸钠体系)，甲烷杆菌(Methanobacterium)和甲烷绳菌(Methanolinea)分别由未添加乙酸钠体系的18.3％和10.8％提高至添加乙酸钠体系的33.7％和12.2％。
实施例3
分析新疆油田某区块产出液中含有15.7％的互营单胞菌(Syntrophomonadaceae)和9.6％的热袍菌(Thermotogaceae)以及23.2％的嗜热甲烷杆菌(Methanobacterium)和13.7％的甲烷囊菌(Methanoculleus)，以该产出液配制2个培养体系(体系组成见表1～3)，21℃下培养64天，两个体系都没有检测到CH4，表明体系中产甲烷菌活性很低。然后保持一个体系不变，在另一个体系中加入0.98g(10mM)乙酸钾，继续培养23天，在两体系中均检测到了CH4，培养143天后两体系中CH4含量分别为3.2mmol/L(未添加乙酸钾体系)和37.2mmol/L(添加乙酸钾体系)。体系中互营单胞菌(Syntrophomonadaceae)丰度由15.7％(未添加乙酸钾体系)提高到37.6％(添加乙酸钾体系),热袍菌(Thermotogaceae)分别为9.6％(未添加乙酸钾体系)和10.2％(添加乙酸钾体系)。嗜热甲烷杆菌(Methanobacterium)由23.2％(未添加乙酸钾体系)提高至45.0％(添加乙酸钾体系)，甲烷囊菌(Methanoculleus) 由13.7％(未添加乙酸钾体系)提高至28.6％(添加乙酸钾体系)。
表1 培养体系组成
Figure PCTCN2014087046-appb-000001
表2 维生素
Figure PCTCN2014087046-appb-000002
表3 微量元素
Figure PCTCN2014087046-appb-000003

Claims (4)

  1. 一种活化油藏中产甲烷菌转化二氧化碳生产甲烷的方法，其特征在于，该方法包括如下步骤：
    (1)分析确定目标油藏流体中至少存在互营单胞菌(Syntrophomonadaceae)或热袍菌(Thermotogaceae)中的一种菌，同时存在下列菌中的至少一种：甲烷杆菌(Methanobacterium),嗜热甲烷杆菌(Methanothermobacter)，甲烷绳菌(Methanolinea)，甲烷螺菌(Methanospirillum)，甲烷囊菌(Methanoculleus)；
    (2)向油藏中注入乙酸或乙酸盐，使油藏水中乙酸或乙酸盐浓度为5.0～10.0mM；
    (3)收获甲烷。
  2. 根据权利要求1所述的活化油藏中产甲烷菌转化二氧化碳生产甲烷的方法，其特征在于，步骤(2)所述的乙酸盐浓度为6.8mM，所述的乙酸盐包括但不限于乙酸盐钠、乙酸钾。
  3. 根据权利要求1所述的活化油藏中产甲烷菌转化二氧化碳生产甲烷的方法，其特征在于，步骤(3)所述的收获甲烷由注入井收获或从采油井收获。
  4. 根据权利要求1所述的活化油藏中产甲烷菌转化二氧化碳生产甲烷的方法，其特征在于，步骤(1)分析确定目标油藏流体中互营单胞菌(Syntrophomonadaceae)或热袍菌(Thermotogaceae)、甲烷杆菌(Methanobacterium),嗜热甲烷杆菌(Methanothermobacter)，甲烷绳菌(Methanolinea)，甲烷螺菌(Methanospirillum)，甲烷囊菌(Methanoculleus)，采用文献[International Biodeterioration&Biodegradation]2011年第65期444-450页报道的16S rDNA方法进行分析鉴定。
PCT/CN2014/087046 2013-10-14 2014-09-22 活化油藏中产甲烷菌转化二氧化碳生产甲烷的方法 WO2015055072A1 (zh)

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