二氧化碳置换法开采天然气水合物研究进展

doi:10.11743/ogg20240218

Abstract

Abstract:

The application of CO₂ replacement method to develop natural gas hydrates （NGHs） is considered a highly promising technology for enhancing both CH₄ recovery and CO₂ sequestration. This study presents a review of the replacement mechanisms with CO₂ and its mixed gas for NGH exploitation， as well as technological advances in the replacement with CO₂ mixed with N₂/H₂ and geothermal-assisted CO₂ replacement for enhancing CH₄ recovery from NGHs. Key findings are as follows：（1） To replace NGHs with pure CO₂ yields a low CH₄ recovery. In contrast， injecting CO₂ mixed with N₂/H₂ at varying ratios into NGH reservoirs proves effective in enhancing CH₄ recovery. （2） Injecting CO₂ mixed with N₂ or H₂ into NGH reservoirs can reduce the Van der Waals’ forces between CH₄ molecules and NGHs’ molecular cages through the competitive adsorption among various gas molecules. Furthermore， it can decrease the partial pressure on the CO₂ phase in the mixed gas， resulting in an upward shift in the phase equilibrium curve of NGHs. Such shift can inhibit the generation rate of CO₂ hydrates during the replacement process and mitigate the adverse effects of hydrate encapsulation， thus enhancing CH₄ recovery. （3） Injecting CO₂ mixed with N₂ for NGH exploitation can reduce the adverse effects of hydrate encapsulation. However， the newly formed N₂ hydrates can block the pathways through which CO₂ molecules enter the molecular cages of NGHs， thus leading to limited performance in enhancing CH₄ recovery. （4） Unlike CO₂ and N₂， H₂ does not form new hydrates under the conditions of hydrate reservoirs. Furthermore， competitive adsorption will occur between H₂ and N₂ when a minor amount of H₂ is injected， further curbing the formation of N₂ hydrates. Therefore， introducing H₂ of low concentration to mixed CO₂-N₂ gas can further increase the displacement rate of CH₄ in NGHs， thus boosting the CH₄ recovery， establishing it as a crucial method to enhance the performance of CO₂ replacement for NGH exploitation. （5） Cyclic injection of mixed gas can significantly enhance both the CH₄ recovery from NGHs and the sequestration rate of CO₂ hydrates. （6） Geothermal-assisted CO₂ replacement for NGH exploitation can not only reduce the encapsulation effect of newly formed CO₂ hydrates but also facilitate CO₂ sequestration in geothermal and hydrate reservoirs， thereby markedly increasing subsurface CO₂ sequestration rate while simultaneously enhancing CH₄ recovery.

Key words: phase equilibrium, encapsulation, sequestration rate, recovery, replacement with a mixture of CO₂ and N₂/H₂, CO₂ replacement method, natural gas hydrate （NGH）

CLC Number:

TE53

Mingxing BAI, Zhichao ZHANG, Qiaozhen CHEN, Long XU, Siyu DU, Yexin LIU. Advances in research on CO₂ replacement for natural gas hydrate exploitation[J]. Oil & Gas Geology, 2024, 45(2): 553-564.

Figures/Tables 10

Fig.1

Table 1

Fig.2

Table 2

Fig.3

Table 3

Performance of mixed CO2+N2 replacement in enhancing CH4 recovery from NGHs［1，27］"

混合气比例	分析技术	水合物介质	温度/K	压力/MPa	CH₄采收率/%	文献来源
10 %CO₂+90 %N₂	NMR+DSC	多孔硅胶+水	274.00	11.5/14.6/18.6	77.0/80.0/79.0	Lee等^［49］
10 %CO₂+90 %N₂	GC	纯水+SDS溶液	298.20	9.1	41.0	Pandey等^［50］
14.6 %CO₂+85.4 %N₂	GC	硅砂+水	273.30	4.2	53.3	Yang等^［51］
19 %CO₂+81 %N₂	GC	石英砂+冰粒	274.20	15.8	6.1	王曦等^［52］
20 %CO₂+80 %N₂	Raman+NMR	粉末冰颗粒	274.20	12.0	85.0	Park等^［46］
20 %CO₂+80 %N₂	SEM	黏土+水	273.20	15.0	85.0	Koh等^［53］
20 %CO₂+80 %N₂	NMR+GC	多孔硅胶+水	273.00	10.0	42.0	Cha等^［54］
20 %CO₂+80 %N₂	GC	玻璃珠+水	275.20	9.8	49.2	Koh等^［47］
20 %CO₂+80 %N₂	GC	玻璃珠+水	274.00	9.5	39.3	Youn等^［56］
22 %CO₂+78 %N₂	GC	石英砂+盐水	273.20	5.0	36.9	Liu等^［57］
23 %CO₂+77 %N₂	Raman+GC	石英砂+水	281.00	10.0	90.0	Schicks等^［58］
25 %CO₂+75 %N₂	GC	砂土+水	274.20	10.0	25.0	Liu等^［57］
25 %CO₂+75 %N₂	GC	高岭石+水	274.20	10.0	24.5	潘栋彬等^［59］
25 %CO₂+75 %N₂	GC	伊利石+水	274.20	10.0	25.0	潘栋彬等^［59］
25 %CO₂+75 %N₂	GC	蒙脱石+水	274.20	10.0	18.2	潘栋彬等^［59］
28 %CO₂+72 %N₂	GC+CCD	纯水+SDS溶液	284.20	9.0	13.2	Niu等^［48］
40 %CO₂+60 %N₂	NMR+GC	多孔硅胶+水	274.00	10.0	51.0	Mok等^［25］
50 %CO₂+50 %N₂	Raman+CCD+GC	纯水	273.90	5.0/6.7	8.3/17.7	Zhou等^［36］
53 %CO₂+47 %N₂	GC	石英砂+冰粒	274.15	2.1/3.4	12.6/19.0	王曦等^［52］
53 %CO₂+47 %N₂	GC	纯水	279.15	8.0	52.4	Ouyang等^［60］
53 %CO₂+47 %N₂	GC	石英砂+热水	274.15	14.0	91.6	操原^［61］
59 %CO₂+41 %N₂	GC	石英砂+水	277.15	7.0	40.8	Yasue等^［62］
60 %CO₂+40 %N₂	GC	石英砂+水	277.15/280.15	7.0	30.0	Masuda等^［63］
60 %CO₂+40 %N₂	Raman+FTIR+GC	纯水	274.00	4.5	73.4	Xu等^［44］
75 %CO₂+25 %N₂	GC	石英砂+冰粒	275.15	3.0	41.4	Li等^［64］
75 %CO₂+25 %N₂	GC	石英砂+水	275.65	4.8	68.8	Tupsakhare等^［65］
75 %CO₂+25 %N₂	Raman+CCD+GC	纯水	274.00	2.6/3.1/3.5	9.5/12.6/17.9	Zhou等^［36］
87.6 %CO₂+12.4 %N₂	GC	石英砂+水	277.15	8.9	46.3	Mu等^［66］

Table 3

Fig.4

Fig.5

Fig.6

Table 4

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74	SCHODERBEK D， MARTIN K L， HOWARD J， et al. North slope hydrate fieldtrial： CO₂/CH₄ exchange［C］//OTC Arctic Technology Conference， Houston， 2012. Red Hook： Curran Associates， Inc.， 2012： OTC-23725-MS.
75	BOSWELL R， SCHODERBEK D， COLLETT T S， et al. The Iġnik Sikumi field experiment， Alaska north slope： Design， operations， and implications for CO₂-CH₄ exchange in gas hydrate reservoirs［J］. Energy & Fuels， 2016， 31（1）： 140-153.
76	LEE H， SEO Y， SEO Y T， et al. Recovering methane from solid methane hydrate with carbon dioxide［J］. Angewandte Chemie International Edition， 2003， 42（41）： 5048-5051.

相态类型	分析技术	水合物介质	温度/K	压力/MPa	CH₄采收率/%	文献来源
液态CO₂	GC	冰粒/纯水	263.0/275.0	9.0	14.0/40.3	Lee等^［23］
液态CO₂	Raman	纯水	273.2	3.6/5.4/6.0	37.6/27.0/29.0	Ota等^［28-29］
液态CO₂	GC	纯水	283.5	4.5/5.0	20.6/18.1	张凤琦等^［30］
液态CO₂	GC	石英砂+水	282.2	6.0 ~ 8.0	13.0 ~ 45.0	Zhang等^［31］
液态CO₂	GC	石英砂+盐水	275.2	4.1 ~ 4.2	26.0 ~ 33.0	Yuan等^［32］
液态CO₂	GC	石英砂+盐水	280.2	4.2	35.0	Yuan等^［32］
液态CO₂	GC	石英砂+SDS溶液	281.2	5.0	18.6	Zhou等^［33］
液态CO₂	GC	石英砂+盐水	273.2	4.0	26.4	Wang^［9］
液态CO₂	Raman+SEM	纯水	277.0	6.0	11.4	Falenty等^［34］
液态CO₂	NMR	砂岩+盐水	273.2	8.3	59.0	Kvamme等^［35］
CO₂乳液	GC	石英砂+SDS溶液	281.2	5.0	27.1	Zhou等^［36］
CO₂乳液	GC	石英砂+水	281.0	5.0	27.1	周锡堂等^［37］
超临界CO₂	GC	石英砂+冰颗粒/盐水	275.2	7.5	37.5	Deusner等^［38］
超临CO₂	GC	石英砂+冰颗粒/盐水	275.2/281.2/283.2	13.0	3.4/40.7/10.7	Deusner等^［38］

混合气比例	分析技术	水合物介质	温度/K	压力/MPa	CH₄采收率/%	文献来源
72 %CO₂ + 28 %H₂	GC	砂岩+咸水	275.6	5.0	28.0	Wang等^［8］
55 %CO₂+ 45 %H₂	GC	砂岩+咸水	275.6	5.0	47.0	Wang等^［8］
36 %CO₂ + 64 %H₂	GC	砂岩+咸水	275.6	5.0	25.0	Wang等^［8］
18 %CO₂ + 82 %H₂	GC	砂岩+咸水	275.6	5.0	70.0	Xu等^［44］
40 %CO₂ + 60 %H₂	Raman+GC	纯水	274.0	4.5	78.0	Xu等^［44］
40 %CO₂ + 60 %H₂	Raman+GC	纯水	274.0	4.5	48.1	Ding等^{［27，40］}
60.1 %CO₂ + 39.9 %H₂	Raman+GC	纯水	274.2	4.5	71.0	Ding等^{［27，40］}
60.1 %CO₂ + 39.9 %H₂	Raman+GC	纯水	274.2	6.0	32.0	Sun等^［43］
74 %CO₂ + 26 %H₂	GC	石英岩+咸水	276.0	3.6	52.4	Sun等^［43］
74 %CO₂ + 26 %H₂	GC	石英岩+咸水	276.0	3.6	46.0	Sun等^［43］
74 %CO₂ + 26 %H₂	GC	石英岩+咸水	276.0	3.6	41.4	Sun等^［43］
43 %CO₂+ 57 %H₂	GC	石英岩+咸水	276.0	3.7	61.0	Sun等^［43］
20 %CO₂+ 80 %H₂	GC	石英岩+咸水	276.0	3.7	58.0	Sun等^［43］
100 %H₂	GC	石英岩+咸水	276.0	3.7	63.0	Sun等^［43］
74 %CO₂+ 26 %H₂	GC	石英砂+咸水	276.0	3.7	30.0 ~ 50.0	Sun等^［43］
40 %CO₂ + 60 %H₂	GC	石英砂+咸水	276.0	3.7	40.0 ~ 75.0	Sun等^［43］
22 %CO₂ + 78 %H₂	GC	石英砂+咸水	276.0	3.7	12.0 ~ 88.0	Sun等^［43］
22 %CO₂ + 78 %H₂	GC	石英砂+咸水	276.0	3.7	15.0 ~ 95.0	Sun等^［43］

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Advances in research on CO₂ replacement for natural gas hydrate exploitation

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开采方式	分析技术	水合物介质	温度/K	压力/MPa	甲烷采收率/%	文献来源
热烟气（CO₂/N₂）	数值模拟	硅砂+水	273.3	4.2	53.3	Yang等^［49］
热电偶原位加热+CO₂/N₂	数值模拟	石英砂+水	275.7	4.8	68.8	Tupsakhare等^［65］
CO₂+地热	数值模拟	石英砂+水	274.2	10.0	59.0	Liu^［70］

Advances in research on CO2 replacement for natural gas hydrate exploitation

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Advances in research on CO₂ replacement for natural gas hydrate exploitation