Technological research progress on CO2-CH4 replacement for hydrate exploitation and enhancement
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摘要: 天然气水合物具有资源储量大、分布范围广等特点，是一种潜力巨大的替代能源，经济、高效、安全地开发天然气水合物是目前研究的热点。CO2-CH4置换水合物开采法既可以置换出水合物储层中的甲烷，同时还将CO2封存其中以保持地层稳定，受到了广泛的关注。本文从CO2-CH4置换的可行性、实验模拟与数值模拟的角度综述了近些年CO2-CH4置换水合物开采法的最新研究进展，并针对置换过程效率低、速度慢等缺点，探讨了改变CO2注入相态、CO2协同小分子气体以及CO2置换联合开采法等强化置换技术，指出了不同强化方法的技术壁垒及应用局限，展望了CO2-CH4置换水合物开采技术的研究方向和发展前景。Abstract: Considering the huge reserve and wide distribution in nature, natural gas hydrates have a great potential to become an alternative energy resource in future. How to economically and safely recovery natural gas from hydrate reservoirs is the focus of current researches. The method by using carbon dioxide (CO2) to replace methane (CH4) within natural gas hydrates has drawn enormous interests due to its two-fold bonus: CH4 recovery for energy and CO2 sequestration for safety. The latest experimental and numerical research in technology on CO2-CH4 replacement for hydrate exploitation, and the feasibility as well as its challenges were summarized. For the challenges to the low efficiency and slow rate in the replacement process, various methods and technologies to enhance the replacement processes were analyzed on examples of the usage of different phase CO2, cooperation with small-molecule gas, and combination with other exploitation methods. Finally, technical barriers and application limitations of different enhancement technologies were pointed out, and the research direction and development prospect of CO2-CH4 replacement for hydrate exploitation were prospected.
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表 1 不同相态CO2的强化置换效果
Table 1 Enhanced displacement effect with CO2 in different states
CO2相态 检测手段 介质体系 温度/K 压力/MPa 甲烷回收效率 文献来源 液 GC 冰粒/纯水 263/275 9 14%/40.3% Lee等[56] 液 Raman 纯水 273.2 3.6/5.4/6 37.6%/27%/29% Ota等[62-63] 液 GC 纯水 283.5 4.5/5.0 20.60%/18.11% 张凤琦等[64] 液 GC 石英砂+水 282.15 6～8 13%～45.4% Zhang等[42] 液 GC 石英砂+盐水 275.2 4.19～4.21 26%～33% Yuan等[33] 液 GC 石英砂+盐水 280.2 4.2 35% Yuan等[33] 液 GC 石英砂+ SDS溶液 281.2 5 18.6% Zhou等[65] 液 GC 石英砂+盐水 273.2 4 26.4% Wang等[66] 液 Raman+SEM 纯水 277 6 11.4% Falenty等[67] 液 MRI 砂岩+盐水 273.2 8.3 59% Kvamme等[68] 乳液 GC 石英砂+ SDS溶液 281.2 5 17%/27.1% Zhou等[65,69] 乳液 GC 石英砂+水 281 5 27.1% 周锡堂等[70] 超临界 GC 石英砂+冰颗粒/盐水 275.2 7.5 37.5% Deusner等[71] 超临界 GC 石英砂+冰颗粒/盐水 275.2/281.2/283.2 13 3.4%/40.7%/10.7% Deusner等[71] 注：GC：气相色谱技术，Raman：拉曼光谱技术，SEM：扫描电子显微镜技术，MRI：核磁共振成像技术。 
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表 2 不同CO2/N2注气比的强化置换效果
Table 2 Enhanced displacement effect at different CO2/N2 injection ratios
气体成分(CO2/N2) 检测手段 介质体系 温度/K 压力/MPa 甲烷回收效率 文献来源 10%CO2+90%N2 NMR+DSC 多孔硅胶+水 274 11.54/14.59/18.59 77%/80%/79% Lee等[74] 10%CO2+90%N2 GC 纯水+SDS溶液 298.15 9.05 41% Pandey等[88] 14.6%CO2+85.4%N2 GC 硅砂+水 273.3 4.2 53.3% Yang等[89] 19%CO2+81%N2 GC 石英砂+冰粒 274.15 15.8 6.1% 王曦等[90] 20%CO2+80%N2 Raman+NMR 粉末冰颗粒 274.15 12 85% Park等[91] 20%CO2+80%N2 SEM 黏土+水 273.15 15 85% Koh等[92] 20%CO2+80%N2 NMR+GC 多孔硅胶+水 273 10 42% Cha等[93] 20%CO2+80%N2 GC 玻璃珠+水 275.15 9.8 49.2% Koh等[94] 20%CO2+80%N2 GC 玻璃珠+水 274 9.5 39.3% Youn等[95] 22%CO2+78%N2 GC 石英砂+盐水 273.2 5.0 36.9 Liu等[87] 23%CO2+77%N2 Raman+GC 石英砂+水 281 10 90% Schicks等[35] 25%CO2+75%N2 GC 砂土+水 274.2 10 25% Pan等[96] 25%CO2+75%N2 GC 高岭石+水 274.2 10 24.5% 潘栋彬等[97] 25%CO2+75%N2 GC 伊利石+水 274.2 10 25% 潘栋彬等[97] 25%CO2+75%N2 GC 蒙脱石+水 274.2 10 18.2% 潘栋彬等[97] 28%CO2+72%N2 GC+CCD 纯水+ SDS溶液 284.2 9.02 13.2% Niu等[98] 40%CO2+60%N2 NMR+GC 多孔硅胶+水 274 10 51% Seo等[99] 50%CO2+50%N2 Raman+CCD+GC 纯水 273.9 5/6.67 8.3%/17.7% Zhou等[100] 53%CO2+47%N2 GC 石英砂+冰粒 274.15 2.1/3.4 12.6%/19% 王曦等[90] 53%CO2+47%N2 GC 纯水 279.15 8.01 52.42% Ouyang等[101] 53%CO2+47%N2 GC 石英砂+热水 274.15 14 91.6% 操原[102] 59%CO2+41%N2 GC 石英砂+水 277.15 7 40.8% Yasue等[86] 60%CO2+40%N2 GC 石英砂+水 277.15/280.15 7 30% Masuda等[103] 60%CO2+40%N2 Raman+FTIR+GC 纯水 274 4.5 73.42% Xu等[41] 75%CO2+25%N2 GC 石英砂+冰粒 275.15 3 41.4% Li等[82] 75%CO2+25%N2 GC 石英砂+水 275.65 4.8 68.8% Tupsakhare等[104] 75%CO2+25%N2 Raman+CCD+GC 纯水 274 2.6/3.11/3.5 9.5%/12.6%/17.9% Zhou等[100] 87.6%CO2+12.4%N2 GC 石英砂+水 277.15 8.9 46.32% Mu等[75] 注：DSC：差式扫描量热技术，NMR：核磁共振技术，CCD：影像检测技术，FTIR：红外光谱技术。
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表 3 不同热激发方式的强化置换效果
Table 3 Enhanced replacement effects in different thermal excitation methods
热激发方式 介质体系 温度/K 压力/MPa 甲烷回收效率（无热激发） 甲烷回收效率（有热激发） 文献来源 热烟气(CO2/N2) 硅砂+水 273.3 4.2 15.9% 53.3% Yang等[89] 短暂升高温度 玻璃珠+水 273.7 3.69 11.55% 59.16% Zhang等[108] 重复注热+分阶段注热 石英砂+冰粒 271.15 3 28% 82% Stanwix等[109] 间歇式原位加热 纯水 280.15 8 35.64% 64.80% 欧阳潜[110] 间歇式原位加热+脉冲注热 纯水 275.15 4 19.83% 35.50% Ouyang等[101] 脉冲注热 纯水 279.15 8 40% 55% 张育诚[111] 热电偶原位加热 石英砂+水 275.65 3.3 24% 99% Tupsakhare等[112] 热电偶原位加热+注入CO2/N2 石英砂+水 275.65 4.8 50% 68.8% Tupsakhare等[104]
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表 4 不同强化方法对置换效率的影响对比
Table 4 Comparison of the effects in different strengthening methods on the replacement efficiency
强化方法类型 突出优势 主要影响因素 注液态CO2 特定成核位置的CO2浓度更高，有利于快速成核 水合物储层粒径 注CO2乳化液 具有更高的反应温度以及更好的传导性和扩散能力 乳化液的含量和种类 注CO2/N2混合气 降低CH4分压，置换出512小笼子中的CH4分子 不同气体比 与热激发法联合 缓解CH4水合物分解引起的局部热损 水合物储层饱和度 与降压法联合 CH4水合物的局部分解为CO2的渗透作用提供了更加丰富的孔隙通道 压降梯度 与注化学剂法联合 使相平衡条件向有利于CH4水合物分解和CO2水合物合成的方向移动 化学剂浓度
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