Mechanism of action and evaluation of chelating agents on barite removal

doi:10.13745/j.esf.sf.2023.6.4

Abstract

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

CLC Number:

TE254

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.

Figures/Tables 15

References 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