湖北宜昌产气页岩氧化溶蚀增渗的地球化学影响

余奇; 刘丹青; 刘方; 张泽星

doi:10.19509/j.cnki.dzkq.tb20230204

湖北宜昌产气页岩氧化溶蚀增渗的地球化学影响

doi: 10.19509/j.cnki.dzkq.tb20230204

余奇^a,,
刘丹青^{a, b, ,},
刘方^a,
张泽星^a

a.
中国地质大学(武汉)环境学院, 武汉 430078
b.
中国地质大学(武汉)生物地质与环境地质国家重点实验室, 武汉 430078

基金项目:

国家自然科学基金青年基金项目“产气页岩氧化溶蚀增渗过程中黄铁矿的影响机理研究” 41902253

详细信息

作者简介:
余奇, E-mail: yuqi@cug.edu.cn

通讯作者:
刘丹青, E-mail: liudq@cug.edu.cn

中图分类号: TE37
计量
- 文章访问数: 259
- PDF下载量: 74
- 被引次数: 0
出版历程
- 收稿日期: 2023-04-17
- 录用日期: 2023-07-19
- 修回日期: 2023-07-12

Geochemical factors affecting oxidation dissolution and permeability enhancement of Yichang gas-producing shale in Hubei Province

YU Qi^a
,,
LIU Danqing^{a, b
, ,},
LIU Fang^a,
ZHANG Zexing^a

a.
School of Environment Studies, China University of Geosciences(Wuhan), Wuhan 430078, China
b.
State Key Laboratory of Biogeology and Environmental Geology, China University of Geosciences(Wuhan), Wuhan 430078, China

More Information

Author Bio:
YU Qi, E-mail: yuqi@cug.edu.cn

Corresponding author: LIU Danqing, E-mail: liudq@cug.edu.cn

摘要

摘要:
为探究湖北宜昌地区产气页岩氧化溶蚀增渗的地球化学影响因素, 以宜昌地区陡山沱组页岩为研究对象, 选取了H₂O₂(w_B=15%)和Na₂S₂O₈(c_B=0.5 mol/L)2种氧化剂开展了氧化溶蚀实验, 探究了不同pH值、温度、地下水水化学离子浓度对氧化溶蚀效果的影响。研究结果表明, Na₂S₂O₈氧化溶蚀效果优于H₂O₂, H₂O₂和Na₂S₂O₈在酸性条件下氧化溶蚀效果均优于碱性条件, 碱性环境不利于2种氧化剂的氧化; 升温会促进Na₂S₂O₈和H₂O₂的热分解, 分别产生H₂SO₄和O₂, 对页岩的氧化溶蚀有积极影响。外源Na⁺(氯化物)的添加能促进页岩在Na₂S₂O₈和H₂O₂氧化过程下Ca²⁺和Mg²⁺的释放, 增强氧化溶蚀效果; 而外源Ca²⁺、SO₄^2-的添加, 容易与碳酸盐酸蚀产生的SO₄^2-、Ca²⁺形成石膏沉淀, 从而引起页岩孔隙堵塞, 降低页岩渗透性; 同时, 外源Mg²⁺易在弱碱性环境下生成硅酸镁沉淀, 对页岩的氧化溶蚀产生负面影响。建议今后在页岩气氧化压裂开采过程中, 预先调查开采地层的水化学参数, 根据地层温度、pH值和阴阳离子来选择氧化液和开采方式。
- 页岩 /
- H₂O₂ /
- Na₂S₂O₈ /
- 氧化溶蚀 /
- 湖北宜昌
Abstract: Objective
Chemical oxidation and infiltration technology has become a mature method for shale gas exploitation. This study aims to investigate the influence of geochemical factors on the exploitation process.
Methods
In this study, the Doushantuo Formation shale in Yichang, Hubei Province, which exhibits significant potential for shale gas exploitation and contains a high organic matter content along with pyrite, was selected as the research object. Two commonly used oxidants, 15% H₂O₂ and 0.5 mol/L Na₂S₂O₈, were selected for oxidation corrosion experiments conducted at normal temperature and pressure. Post-reaction measurements included cation concentration, pH, Eh, mass loss and XRD analysis.
Results
The results show that Na₂S₂O₈ outperforms H₂O₂, and the advanced oxidation process driven by pyrite and the erosion effect of carbonate under acid production make the acidic environment more suitable for the dissolution of carbonate-rich shale. An increase in temperature enhances the thermal decomposition of Na₂S₂O₈ and H₂O₂. The thermal decomposition of H₂O₂ produces O₂, and Na₂S₂O₈ produces H₂SO₄, O₂ and SO₄^- with strong oxidation. Thus, the temperature's enhancement effect on Na₂S₂O₈ is greater than that on H₂O₂. Sodium ions (chloride) can promote the release of Ca²⁺ and Mg²⁺ during Na₂S₂O₈ and H₂O₂ oxidation, indicating that a high concentration of NaCl in groundwater plays a positive role in the oxidation and dissolution of shale. Both calcium ions and sulfate ions can cause gypsum precipitation by influencing the interactions between the reactions, thus affecting the oxidative dissolution of shale. Low concentrations of exogenous calcium ions reduce the buffering effect of carbonate and promote its dissolution, while high concentrations of exogenous calcium ions cause secondary mineral precipitation, block shale pores and hinder the oxidation and dissolution of shale. However, the effect of sulfate ions on the oxidative corrosion of shale differs from that of calcium ions. A low concentration of exogenous sulfate ions inhibits the oxidative corrosion of shale by generating secondary ore and impeding the oxidation of pyrite.
Conclusion
Therefore, in the future process of shale gas oxidative fracturing for extraction, it is necessary to preassess the water chemical parameters of the exploitation formation in advance and select the oxidation liquid and mining modes based on the temperature, pH and cationions.
- shale /
- H₂O₂ /
- Na₂S₂O₈ /
- oxidation dissolution /
- Yichang area, Hubei Province
注释:

所有作者声明不存在利益冲突。

HTML全文

图 1 湖北宜昌地区地质构造简图^[31]

Nh.南华系; Z.震旦系; ∈.寒武系; O.奥陶系; S.志留系; D.泥盆系; P.二叠系; T.三叠系; J.侏罗系; K.白垩系; E.古近系

Figure 1. Sketch map of tectonics in the Yichang area, Hubei Province

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图 2 不同氧化剂处理页岩后质量损失(a)和离子质量浓度(b)随初始pH值的变化

Figure 2. Mass loss(a) and ion concentration(b) with initial pH after shale treatment with different oxidants

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图 3 不同氧化剂氧化页岩后质量损失(a)、pH(b)、Ca²⁺(c)及Mg²⁺质量浓度(d)随温度的变化

Figure 3. Mass loss(a), pH(b), Ca²⁺ concentration(c), Mg²⁺ concentration(d) changes with temperature after shale oxidation with different oxidants

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图 4 不同氧化剂氧化页岩后质量损失(a)、Eh值(b)、Fe²⁺(c)、Ca²⁺和Mg²⁺质量浓度(d)随外源Na⁺质量浓度的变化

Figure 4. Mass loss(a), Eh(b), Fe²⁺ concentration(c), Ca²⁺ concentration and Mg²⁺ concentration(d) changes with the exogenous Na⁺ concentration after shale oxidation with different oxidants

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图 5 不同氧化剂氧化页岩后质量损失(a)、Eh值和pH值(b)、Fe²⁺(c)、Ca²⁺和Mg²⁺质量浓度(d)随外源Ca²⁺质量浓度的变化

Figure 5. Mass loss(a), Eh and pH(b), Fe²⁺ concentration(c), Ca²⁺ concentration and Mg²⁺ concentration(d) changes with the exogenous Ca²⁺ concentration after shale oxidation with different oxidants

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图 6 不同氧化剂氧化页岩后质量损失(a)、Ca²⁺和Mg²⁺质量浓度(b)随外源Mg²⁺质量浓度的变化

Figure 6. Mass loss(a), Ca²⁺ concentration and Mg²⁺ concentration(b) changes with the exogenous Mg²⁺ concentration after shale oxidation with different oxidants

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图 7 不同氧化剂氧化页岩后质量损失(a)、Ca²⁺和Mg²⁺质量浓度(b)随外源SO₄^2-质量浓度的变化

Figure 7. Mass loss(a), Ca²⁺ concentration and Mg²⁺ concentration(b) changes with the exogenous SO₄^2- concentration after shale oxidation with different oxidants

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图 8 原岩及氧化后固体产物XRD分析图

Q.石英; D.白云石; P.黄铁矿; A.钠长石; I.伊利石; Ch.绿泥石; G.石膏

Figure 8. XRD analysis of original rock and oxidized solid products

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图 9 酸性条件下产气页岩氧化溶蚀增渗机理作用图

Figure 9. Oxidation dissolution and permeability mechanism action diagram of gas producing shale under acidic conditions

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图 10 碱性条件下产气页岩氧化溶蚀增渗机理作用图

Figure 10. Oxidation dissolution and permeability mechanism action diagram of gas producing shale under alkaline conditions

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图 11 高温下产气页岩氧化溶蚀增渗机理作用图(仅考虑分解产物造成的一次反应)

Figure 11. Oxidation dissolution and permeability mechanism diagram of gas producing shale at high temperature(only considering the first reaction caused by decomposition products)

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表 1 湘鄂西区海相地层水化学参数统计

Table 1. Statistical table of chemical parameters in marine formation water in western Hunan and Hubei Provinces ρ_B/(mg·L^-1)

储层	井号	Na⁺	Ca²⁺	Mg²⁺	Cl^-	SO₄^2-	HCO₃^-	矿化度	水型
震旦系	宜3	1 597.90	568.45	201.98	1 156.11	3 786.30	166.43	7 460.50	SO₄-Na
	宜4	1 746.16	534.93	179.88	1 138.98	3 954.10	175.95	7 730.27	SO₄-Na
	宜7	1 590.27	538.69	194.54	1 083.88	3 783.06	153.77	7 348.37	SO₄-Na
	宜8	1 675.00	550.00	203.00	1 238.00	3 749.00	245.00	7 660.00	SO₄-Na
均值(ρ)		1 652.33	548.02	194.85	1 154.24	3 818.12	185.29	7 549.79	SO₄-Na

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表 2 实验设计

Table 2. Experimental design

组别	pH值	温度/℃	阴阳离子	质量浓度ρ_B
A	1，2，3，7，9，11	25	—	—
B	—	25，45，60	—	—
C	—	25	Na⁺	0，0.5ρ，ρ，1.5ρ，2ρ
			Ca²⁺
			Mg²⁺
			SO₄^2-

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