重晶石螯合解堵剂作用机理及其评价方法研究

doi:10.13745/j.esf.sf.2023.6.4

地学前缘 ›› 2023, Vol. 30 ›› Issue (6): 451-462.DOI: 10.13745/j.esf.sf.2023.6.4

重晶石螯合解堵剂作用机理及其评价方法研究

张雄¹^,²(), 潘丽娟¹^,²^,^*(), 李亮¹^,², 方俊伟¹^,², 韦仲进³, 杨俊程³, 周风山³

1.中国石化碳酸盐岩缝洞型油藏提高采收率重点实验室, 新疆乌鲁木齐 830011
2.中国石化西北油田分公司, 新疆乌鲁木齐 830011
3.中国地质大学(北京) 材料科学与工程学院, 北京 100083

收稿日期:2022-10-11 修回日期:2023-05-09 出版日期:2023-11-25 发布日期:2023-11-25
通讯作者: * 潘丽娟(1983—),女,副研究员,长期从事油田化学领域的研究工作。E-mail: panlij.xbsj@sinopec.com
作者简介:张雄(1986—),男,副研究员,主要从事酸化压裂方面的研究工作。E-mail: zxiong.xbsj@sinopec.com
基金资助:
国家科技重大专项“海相碳酸盐岩超深油气井关键工程技术(2017ZX05005-005);中国石油化工股份有限公司科研项目“顺北一区采输关键技术研究与应用(P18022-001);顺北一区5号断裂带提质提速钻完井技术研究(P20002)

Mechanism of action and evaluation of chelating agents on barite removal

ZHANG Xiong¹^,²(), PAN Lijuan¹^,²^,^*(), LI Liang¹^,², FANG Junwei¹^,², WEI Zhongjin³, YANG Juncheng³, ZHOU Fengshan³

1. Key Laboratory of Enhanced Oil Recovery in Carbonate Fractured-vuggy Reservoirs, SINOPEC, ürümqi 830011, China
2. Northwest Oilfield Company, SINOPEC, ürümqi 830011, China
3. School of Materials Science and Technology, China University of Geosciences (Beijing), Beijing 100083, China

Received:2022-10-11 Revised:2023-05-09 Online:2023-11-25 Published:2023-11-25

摘要/Abstract

摘要：

以重晶石加重剂为主要成分的钻井液滤饼形成的重晶石堵塞是造成油气储层伤害、影响油气产量的主要因素之一。常规的酸化解堵措施难以溶解重晶石堵塞物,而研制高性价比的非酸螯合解堵剂并制定科学的解堵施工工艺是解决重晶石堵塞的有效工程手段。氨基多羧酸螯合剂通过与重晶石表面的钡离子形成强螯合物,促进重晶石的快速溶解,有助于解除重晶石滤饼堵塞。文章归纳了常见的氨基多羧酸螯合剂的结构特征,从螯合解堵机理角度认为 DTPA对重晶石堵塞的油气井解堵效果最佳;同时分析了常用的螯合解堵剂评价方法的优缺点,建立了一套准确、简单、快捷的重晶石螯合解堵剂性能的评价方法。相比于其他评价方法,高温动态溶解率评价方法具有实验耗时短、对实验器材要求低、实验结果直观等优点,推荐使用高温动态溶解率评价方法去评价螯合解堵剂的性能。

关键词: 钻井液, 重晶石滤饼, 油气堵塞, 螯合解堵剂

Abstract:

Barite blockage—a result of the formation of a drilling fluid filter cake with barite weighting agent as the main component—is one of the main contributing factors to reservoir damage and causes major problems in oil and gas production. As conventional acidification measures fail to remove the barite blockage, finding cost-effective, non-acid chelating agents and formulating a barite removal scheme are an effective engineering means to solve the barite blockage problem. Aminopolycarboxylic acids as chelating agents bind strongly with barium ions on the surface of barite promoting the rapid dissolution of the barite filter cake. The structural characteristics of common aminopolycarboxylic acids are summarized. From the mechanistic perspective of chelating, we consider DTPA to be most effective for the barite removal in oil and gas wells. In addition, the pros and cons of commonly used evaluation methods for chelating agents are considered, and an evaluation scheme for accurate, simple, fast performance evaluation of chelating agents is established. We recommend using the high-temperature dynamic dissolution-rate measurements to evaluate chelating reagents, as it has the advantages of short experiment time, low requirements on test equipment and intuitive test results.

Key words: drilling fluid, barite filter cake, oil and gas blockage, chelating removal agent

中图分类号:

TE254

张雄, 潘丽娟, 李亮, 方俊伟, 韦仲进, 杨俊程, 周风山. 重晶石螯合解堵剂作用机理及其评价方法研究[J]. 地学前缘, 2023, 30(6): 451-462.

ZHANG Xiong, PAN Lijuan, LI Liang, FANG Junwei, WEI Zhongjin, YANG Juncheng, ZHOU Fengshan. Mechanism of action and evaluation of chelating agents on barite removal[J]. Earth Science Frontiers, 2023, 30(6): 451-462.

图/表 15

参考文献 34

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中文名称	英文名称	分子式	分子量	缩写代号
氮川三乙酸	Nitrilotri-Acetic Acid	C₆H₉NO₆	191	NTA
乙二胺四乙酸	Ethylenediaminetetra-Acetic Acid	C₁₀H₁₆N₂O₈	292	EDTA
乙二胺四乙酸二钠盐	Ethylenediaminetetra-Acetic Acid Disodium Salt	C₁₀H₁₄N₂Na₂O₈	336	EDTA-2Na₂
环己烯二硝基乙酸	Cyclohexylenedinitrilotetra-Acetic Acid	C₁₄H₂₂N₂O₈	346	DOTA
二乙烯三胺五乙酸	Diethylene Triamine Penta-Acetic Acid	C₁₄H₂₃N₃O₁₀	393	DTPA
二氧辛烷乙基二硝基四乙酸	Dioxaoctane Ethylenedinitrilo Tetra-Acetic Acid	C₁₄H₂₄N₂O₁₀	380	DOCTA
环己二胺四乙酸	Trans-l,2-cyclohexylenediaminetetraacetic Acid	C₁₄H₂₂N₂O₈	389	CDTA
羟乙基乙二胺四乙酸酯	(Hydroxyethyl)-Ethylene-Diamine-Tetra-Acetate	C₁₀H₁₅Na₃N₂O₇	278	HEDTA
三乙烯四胺六乙酸	Triethylene-Theremin-Hexa-Acetic Acid	C₁₀H₃₀N₄O₁₂	494	TTHA
羟乙基亚氨基二乙酸	Hydroxyethyliminodiacetic Acid	C₆H₁₁NO₅	177	HEIDA
L-谷氨酸-N,N-二乙酸	L-Glutamic Acid N, N-Diacetic Acid	C₉H₁₃NO₈	263	GLDA
甲基甘氨酸二乙酸	Methylglycinediacetic Acid	C₇H₁₁NO₆	205	MGDA

中文名称	英文名称	分子式	分子量	缩写代号
氮川三乙酸	Nitrilotri-Acetic Acid	C₆H₉NO₆	191	NTA
乙二胺四乙酸	Ethylenediaminetetra-Acetic Acid	C₁₀H₁₆N₂O₈	292	EDTA
乙二胺四乙酸二钠盐	Ethylenediaminetetra-Acetic Acid Disodium Salt	C₁₀H₁₄N₂Na₂O₈	336	EDTA-2Na₂
环己烯二硝基乙酸	Cyclohexylenedinitrilotetra-Acetic Acid	C₁₄H₂₂N₂O₈	346	DOTA
二乙烯三胺五乙酸	Diethylene Triamine Penta-Acetic Acid	C₁₄H₂₃N₃O₁₀	393	DTPA
二氧辛烷乙基二硝基四乙酸	Dioxaoctane Ethylenedinitrilo Tetra-Acetic Acid	C₁₄H₂₄N₂O₁₀	380	DOCTA
环己二胺四乙酸	Trans-l,2-cyclohexylenediaminetetraacetic Acid	C₁₄H₂₂N₂O₈	389	CDTA
羟乙基乙二胺四乙酸酯	(Hydroxyethyl)-Ethylene-Diamine-Tetra-Acetate	C₁₀H₁₅Na₃N₂O₇	278	HEDTA
三乙烯四胺六乙酸	Triethylene-Theremin-Hexa-Acetic Acid	C₁₀H₃₀N₄O₁₂	494	TTHA
羟乙基亚氨基二乙酸	Hydroxyethyliminodiacetic Acid	C₆H₁₁NO₅	177	HEIDA
L-谷氨酸-N,N-二乙酸	L-Glutamic Acid N, N-Diacetic Acid	C₉H₁₃NO₈	263	GLDA
甲基甘氨酸二乙酸	Methylglycinediacetic Acid	C₇H₁₁NO₆	205	MGDA

逐级脱质子化学反应	氨基多羧酸螯合剂脱质子反应平衡常数
逐级脱质子化学反应	NTA	EDTA	HEDTA	DTPA	HEIDA	GLDA	DOTA	CDTA	MGDA
pK_a1	9.7	10.2	9.8	10.5	8.7	9.4	404	364	205
pK_a2	2.5	6.1	5.4	8.5	2.2	5.0	11.9	11.7	10.5
pK_a3	1.8	2.7	2.6	4.3		3.5	9.72	6.12	2.5
pK_a4	1.0	2.0		2.6		2.6	4.6	3.52	1.6
pK_a5		1.5		1.8			4.13	2.43

逐级脱质子化学反应	氨基多羧酸螯合剂脱质子反应平衡常数
逐级脱质子化学反应	NTA	EDTA	HEDTA	DTPA	HEIDA	GLDA	DOTA	CDTA	MGDA
pK_a1	9.7	10.2	9.8	10.5	8.7	9.4	404	364	205
pK_a2	2.5	6.1	5.4	8.5	2.2	5.0	11.9	11.7	10.5
pK_a3	1.8	2.7	2.6	4.3		3.5	9.72	6.12	2.5
pK_a4	1.0	2.0		2.6		2.6	4.6	3.52	1.6
pK_a5		1.5		1.8			4.13	2.43

金属离子	氨基多羧酸与金属离子配位形成的螯合物的稳定性常数
金属离子	NTA	EDTA	HEDTA	DTPA	HEIDA	GLDA	DOTA	CDTA	MGDA
Ca²⁺	6.4	10.7	8.4	10.9	4.8	5.9	17.2	12.5	7
Mg²⁺	5.4	8.7	7.0	9.3	3.46	5.2	11.85	10.32	5.8
Fe²⁺	8.8	14.3	12.2	16.5	6.8	8.7		16.27	8.1
Fe³⁺	15.8	25.7	19.8	28	11.6	15.2		28.05	16.5
Ba²⁺	4.8	7.7	6.2	8.6	2.8	3.5	12.87	8.69	4.9
Sr²⁺	5.0	8.6	6.92	9.7	3.8	4.1	15	10.54	5.2
Al³⁺	11.4	16.1	15.6	18.4	7.74	12.2

重晶石螯合解堵剂作用机理及其评价方法研究

Mechanism of action and evaluation of chelating agents on barite removal

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试验方法	优点	缺点	参考文献
滤饼溶蚀率	静态试验,结果直观	实验过程烦琐,不能直接反映重晶石的溶蚀特性,实验结果容易受泥饼制备方法的影响	[25]
滤饼元素组成变化	静态实验,结果直观	实验过程烦琐,实验器材昂贵,不能直接反映重晶石的溶蚀特性	[26-27]
重晶石表面微观形貌变化	静态实验,结果直观	实验器材昂贵,实验成本高,不能定量表述重晶石的溶蚀结果	[28]
岩心流动渗透率实验	动态实验,结果直观,实验器材标准	实验过程耗时长,实验成本高,人造岩心质量容易影响实验结果,不能直接提供重晶石的溶解效能	[29]
高温动态溶解率评价方法	动态实验,评价溶解潜力全面,实验器材标准、简单,实验方法快捷,实验成本低,实验结果直观	此实验方法未考虑不同商品化重晶石解堵剂的最佳适用范围可能有差别的情况	本文