低密度陶粒支撑剂的水敏老化机理研究

硅酸盐通报 ›› 2023, Vol. 42 ›› Issue (9): 3334-3341.

低密度陶粒支撑剂的水敏老化机理研究

陈佳宁¹, 郝建英¹, 王升昌¹, 梁天成^2,3

1.太原科技大学材料科学与工程学院,太原 030024;
2.中国石油勘探开发研究院,北京 100083;
3.中国石油天然气集团有限公司油气藏改造重点实验室,廊坊 065007

收稿日期:2023-05-05 修订日期:2023-06-12 出版日期:2023-09-15 发布日期:2023-09-14
通信作者: 郝建英,博士,副教授。E-mail:jianyinghao@tyust.edu.cn
作者简介:陈佳宁(1998—),女,硕士研究生。主要从事先进陶瓷材料方面的研究。E-mail:2995167829@qq.com
基金资助:
山西省基础研究计划(202203021211186);山西省重点研发项目(201903D121101);中国石油前瞻性基础工程项目(2021DJ1805)

Water-Sensitive Aging Mechanism of Low-Density Ceramic Proppant

CHEN Jianing¹, HAO Jianying¹, WANG Shengchang¹, LIANG Tiancheng^2,3

1. School of Materials Science and Engineering, Taiyuan University of Science and Technology, Taiyuan 030024, China;
2. PetroChina Research Institute of Petroleum Exploration & Development, Beijing 100083, China;
3. CNPC Key Laboratory of Oil & Gas Reservoir Stimulation, Langfang 065007, China

Received:2023-05-05 Revised:2023-06-12 Online:2023-09-15 Published:2023-09-14

摘要/Abstract

摘要： 低密度陶粒支撑剂良好的性能在非常规能源开采工作中显得十分重要。针对低密度陶粒支撑剂在地层水服役期间性能退化的现象,本文选取两种不同规格的支撑剂,在地层水中浸泡不同时间后取出,采用XRF、XPS、XRD、SEM、TEM对浸泡前后的支撑剂进行表征,探索支撑剂老化机理。结果显示:支撑剂中ClO₂含量增加,Al₂O₃、SiO₂含量减少,地层水中Cl^-、HCO^-₃含量减少;XPS检测出Cl 2p峰和Cl 2s峰;XRD检测出新相SiCl₄。以上结果证实,地层水中的Cl^-扩散到支撑剂表面与SiO₂反应生成SiCl₄,SiCl₄进一步水化生成硅凝胶或硅酸凝胶包覆在支撑剂表面。支撑剂中Al₂O₃会与地层水中H⁺(酸性环境)反应生成Al³⁺,Al³⁺再与HCO^-₃反应生成Al(OH)₃沉淀进入地层水中。地层水中大量的Cl^-和H⁺共同作用,使支撑剂从表面开始侵蚀,导致支撑剂内部结构致密化程度降低,结构松散,从而使支撑剂的抗破碎能力降低,性能退化。

关键词: 低密度陶粒支撑剂, 地层水, 硅凝胶, 老化机理, Cl^-侵蚀, 酸性环境

Abstract: Good performance of low-density ceramic proppant is particularly important during the exploration of unconventional energy. In view of the performance degradation of low-density ceramic proppant upon serving in the formation water, two specifications of proppant were selected to be soaked in the formation water for different time. The proppant before and after soaking was characterized by XRF, XPS, XRD, SEM and TEM, and its aging mechanism was explored. The results show that the content of ClO₂ in the proppant increases, while the content of Al₂O₃ and SiO₂ decreases, and the content of Cl^- and HCO^-₃ in the formation water decreases. The peaks of Cl 2p and Cl 2s appear by XPS, and the new phase SiCl₄ is detected by XRD. These results confirm that Cl^- in the formation water diffuses to the proppant surface and reacts with SiO₂ to form SiCl₄, which further hydrates to generate silicone gel or silicic acid gel and coats the proppant surface. Al₂O₃ in the proppant can react with H⁺ (acidic environment) of the formation water to form Al³⁺, and then Al³⁺ reacts with HCO^-₃ to form Al(OH)₃ precipitating into the formation water. A large amount of Cl^- and H⁺ in the formation water erode the proppant from the surface, reducing the densification within the structure and making the structure loose, which reduces the proppant crushing resistance and degrades its performance.

Key words: low-density ceramic proppant, formation water, silicon gel, aging mechanism, Cl^- erosion, acidic environment

中图分类号:

TQ174.1

陈佳宁, 郝建英, 王升昌, 梁天成. 低密度陶粒支撑剂的水敏老化机理研究[J]. 硅酸盐通报, 2023, 42(9): 3334-3341.

CHEN Jianing, HAO Jianying, WANG Shengchang, LIANG Tiancheng. Water-Sensitive Aging Mechanism of Low-Density Ceramic Proppant[J]. BULLETIN OF THE CHINESE CERAMIC SOCIETY, 2023, 42(9): 3334-3341.

参考文献

[1] 毛昭元, 高凯强, 史晓琪. 水力压裂陶粒支撑剂的研究现状[J]. 佛山陶瓷, 2022, 32(7): 1-5+8.
MAO Z Y, GAO K Q, SHI X Q. Research status of hydro-fracturing ceramic proppant[J]. Foshan Ceramics, 2022, 32(7): 1-5+8 (in Chinese).
[2] 关舒文. 水力裂缝内支撑剂多孔介质导流能力的影响机制[D]. 太原: 太原理工大学, 2021.
GUAN S W. Influence mechanism of proppant porous media conductivity in hydraulic fractures[D]. Taiyuan: Taiyuan University of Technology, 2021 (in Chinese).
[3] 毕思峰, 曾永明, 杨沛鹏. 石油压裂支撑剂的研究现状[J]. 山东化工, 2023, 52(6): 76-78.
BI S F, ZENG Y M, YANG P P. Research progress of petroleum fracturing proppants[J]. Shandong Chemical Industry, 2023, 52(6): 76-78 (in Chinese).
[4] 沈渭滨, 赵之晗. 支撑剂嵌入对致密砂岩储层裂缝导流能力的影响[J]. 能源化工, 2022, 43(1): 48-51.
SHEN W B, ZHAO Z H. Influence of proppant embedment on fracture conductivity of tight sandstone reservoirs[J]. Energy Chemical Industry, 2022, 43(1): 48-51 (in Chinese).
[5] 雷俊雄, 陈锦风, 林泽钦, 等. 低密度支撑剂技术及研究现状[J]. 化工管理, 2020(26): 46-47.
LEI J X, CHEN J F, LIN Z Q, et al. Low density proppant technology and its research status[J]. Chemical Enterprise Management, 2020(26): 46-47 (in Chinese).
[6] KUMAR G S, PATWARDHAN S D, GUNAJI R G. Impact of proppant diagenesis on shale gas productivity[J]. International Journal of Oil, Gas and Coal Technology, 2017, 14(1/2): 147.
[7] ELSARAWY A M, NASR EL DIN H A. Proppant diagenesis in carbonate-rich eagle ford shale fractures[J]. SPE Drilling & Completion, 2020: 35(3): 465-477.
[8] MITTAL A, RAI C, SONDERGELD C. Proppant-conductivity testing under simulated reservoir conditions: impact of crushing, embedment, and diagenesis on long-term production in shales[J]. SPE Journal, 2018, 23(4): 1304-1315.
[9] GUPTA A K, RAI C S, SONDERGELD C H. Experimental investigation of propped fracture conductivity and proppant diagenesis[C]//Proceedings of the 7th Unconventional Resources Technology Conference. Amsterdam: Elsevier, 2019.
[10] RAYSONI N, WEAVER J. Long-term proppant performance[C]//SPE International Symposium on Formation Damage Control. Amsterdam: Elsevier, 2012(1): 162-177.
[11] AVEN N K, WEAVER J, LOGHRY R, et al. Long-term dynamic flow testing of proppants and effect of coatings[C]//SPE-European Formation Damage Conference. Amsterdam: Elsevier, 2013(1): 344-365.
[12] YU J Y, WANG J H, WANG S G, et al. Conductivity evolution in propped fractures during reservoir drawdown[J]. Rock Mechanics and Rock Engineering, 2022, 55(6): 3583-3597.
[13] PATWARDHAN S D. Shale gas productivity: a geo-chemical diagenesis perspective[C]//Proceedings-SPE Annual Technical Conference and Exhibition, Amsterdam: Elsevier, 2015: 6860-6878.
[14] Interaational Organization for Standardization. Measurement of properties of proppants used in hydraulic fracturing and gravel-packing operations: ISO 13503-2—2006[S]. Switzerland: International Organization for Standardization, 2006: 21-23.
[15] 国家能源局. 水力压裂和砾石充填作业用支撑剂性能测试方法: SY/T 5108—2014[S]. 北京: 石油工业出版社, 2015.
National Energy Administration. Proppant performance test method for hydraulic fracturing and gravel packing operations: SY/T 5108—2014[S]. Bejing: Petroleum Industry Press, 2015 (in Chinese).
[16] 邱镁钫, 张青艳, 郑宇轩. 氧化铝陶瓷压缩破坏过程离散元数值模拟[J]. 硅酸盐通报, 2022, 41(9): 3296-3303.
QIU M F, ZHANG Q Y, ZHENG Y X. Discrete element simulations on compressive fragmentation of alumina ceramics[J]. Bulletin of the Chinese Ceramic Society, 2022, 41(9): 3296-3303 (in Chinese).
[17] 付绿平, 黄奥, 顾华志, 等. 纳米氧化铝超塑性及其对轻量刚玉材料微结构的影响[J]. 陶瓷学报, 2018, 39(1): 20-23.
FU L P, HUANG A, GU H Z, et al. Superplasticity of nano-alumina and its effect on the microstructure of microporous alumina[J]. Journal of Ceramics, 2018, 39(1): 20-23 (in Chinese).
[18] 郭会师, 陈文亮, 李文凤, 等. 烧结温度对莫来石多孔陶瓷结构与性能的影响[J]. 耐火材料, 2023, 57(1): 10-14.
GUO H S, CHEN W L, LI W F, et al. Effects of sintering temperatures on microstructure and properties of mullite porous ceramics[J]. Refractories, 2023, 57(1): 10-14 (in Chinese).
[19] 梁天成, 严玉忠, 蒙传幼, 等. 水力压裂用支撑剂破碎率的影响因素分析[J]. 重庆科技学院学报(自然科学版), 2021, 23(3): 10-14+44.
LIANG T C, YAN Y Z, MENG C Y, et al. Analysis of influence factor of the proppants crush resistance in hydraulic fracturing[J]. Journal of Chongqing University of Science and Technology (Natural Sciences Edition), 2021, 23(3): 10-14+44 (in Chinese).
[20] 王丽萍, 郭昭华, 池君洲, 等. 氧化铝多用途开发研究进展[J]. 无机盐工业, 2015, 47(6): 11-15+62.
WANG L P, GUO Z H, CHI J Z, et al. Progress in multipurpose research and development of multiform alumina[J]. Inorganic Chemicals Industry, 2015, 47(6): 11-15+62 (in Chinese).