用于复杂原油乳液的高效破乳剂开发及应用研究进展

doi:10.16085/j.issn.1000-6613.2022-1754

化工进展 ›› 2023, Vol. 42 ›› Issue (8): 4398-4413.DOI: 10.16085/j.issn.1000-6613.2022-1754

用于复杂原油乳液的高效破乳剂开发及应用研究进展

吴亚¹^,²(), 赵丹¹, 方荣苗¹, 李婧瑶¹, 常娜娜¹, 杜春保¹, 王文珍¹^,²(), 史俊¹()

^1.西安石油大学化学化工学院，陕西西安 710065
^2.陕西省绿色低碳能源材料与过程工程技术研究中心，陕西西安 710065

收稿日期:2022-09-20 修回日期:2023-01-19 出版日期:2023-08-15 发布日期:2023-09-19
通讯作者: 王文珍,史俊
作者简介:吴亚（1979—），女，博士，教授，研究方向为提高油田水质。E-mail：wuya@xsyu.edu.cn。
基金资助:
国家自然科学基金(22002117);陕西省重点研发计划工业领域(2022GY-162);陕西省重点研发计划国际科技合作与交流项目(2019KW-061)

Research progress on highly efficient demulsifiers for complex crude oil emulsions and their applications

WU Ya¹^,²(), ZHAO Dan¹, FANG Rongmiao¹, LI Jingyao¹, CHANG Nana¹, DU Chunbao¹, WANG Wenzhen¹^,²(), SHI Jun¹()

^1.College of Chemistry and Chemical Engineering, Xi’an Shiyou University, Xi’an 710065, Shaanxi, China
^2.Shaanxi Engineering Research Center of Green Low-carbon Energy Materials and Processes, Xi’an 710065, Shaanxi, China

Received:2022-09-20 Revised:2023-01-19 Online:2023-08-15 Published:2023-09-19
Contact: WANG Wenzhen, SHI Jun

摘要/Abstract

摘要：

石油生产中通常产生大量W/O、O/W或多重乳化的复杂原油乳液，造成生产效率大大降低以及严重的环境问题。目前所使用的破乳剂破乳效率低、普适性差、成本高、安全性不够等，开发高效、普适、绿色、安全破乳剂仍备受关注。本文基于原油乳液的特点及稳定机制分析，综述了不同原油乳液的破乳剂研究进展，主要围绕聚合物破乳剂、生物质基破乳剂、离子液体破乳剂和纳米材料破乳剂的特点、适用范围及其应用效果进行全面总结，对相应破乳剂的破乳机理进行针对性地分析研究，并指出破乳剂机理的研究方法。最后，本文对复杂原油乳液的高效破乳剂开发进行展望，提出破乳技术的未来发展趋势，以期为W/O、O/W或多重乳化的复杂原油乳液的破乳技术应用提供一定借鉴与参考。

关键词: 复杂原油乳液, 离子液体破乳剂, 生物质基破乳剂, 纳米材料破乳剂, 破乳机理

Abstract:

In petroleum production, a large number of W/O, O/W or multiple emulsified emulsions are usually produced, resulting in greatly reduced production efficiency and serious environmental problems. The demulsifiers used in production have low demulsification efficiency, high cost, poor universality and insufficient safety. There is still more attention to develop efficient, universal, green and safe demulsifiers. Based on the analysis of the characteristics and stability mechanism of crude oil emulsion, the research progress of demulsifiers for different crude oil lotion were summarized. It mainly included polymer demulsifiers, biomass based demulsifiers, ionic liquid demulsifiers and nano material demulsifiers. Finally, the development of efficient demulsifiers and the future development trend of demulsification technology were put forward. It laid a foundation for the demulsification technology application of W/O, O/W or complex crude oil emulsions.

Key words: complex crude oil emulsion, ionic liquid demulsifier, biomass-based demulsifier, nanogenic material demulsifier, demulsification mechanism

中图分类号:

TE39

吴亚, 赵丹, 方荣苗, 李婧瑶, 常娜娜, 杜春保, 王文珍, 史俊. 用于复杂原油乳液的高效破乳剂开发及应用研究进展[J]. 化工进展, 2023, 42(8): 4398-4413.

WU Ya, ZHAO Dan, FANG Rongmiao, LI Jingyao, CHANG Nana, DU Chunbao, WANG Wenzhen, SHI Jun. Research progress on highly efficient demulsifiers for complex crude oil emulsions and their applications[J]. Chemical Industry and Engineering Progress, 2023, 42(8): 4398-4413.

图/表 16

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破乳剂	适用油水体系类型	DE/%	最佳破乳环境	优点	缺点
BP系列^[25]	胜利油田	90以上	50℃，3h	脱水效果好	对分子量和破乳温度要求高，否则破乳效果不明显，对环境污染较大
AP系列^[23]	渤海油田、东海油田	90	1.25％的水分散体系破乳剂用量25mg/L	对海洋原油具有脱水速度快、油水界面齐、脱出水清
SD破乳剂^[26]	塔河油田重质原油	89	破乳剂用量100mg/L，温度为70℃	—
DS-06/DL11正反破乳剂复配^[27]	呼和浩特炼油厂含油污泥	95	180mg/L，30∶10复配	专一性强，工业应用效果明显
DS-1复配型^[24]	大庆油田北二联合站高机械杂质含量污油	97	4.5h，50℃	—

破乳剂	适用油水体系类型	DE/%	最佳破乳环境	优点	缺点
BP系列^[25]	胜利油田	90以上	50℃，3h	脱水效果好	对分子量和破乳温度要求高，否则破乳效果不明显，对环境污染较大
AP系列^[23]	渤海油田、东海油田	90	1.25％的水分散体系破乳剂用量25mg/L	对海洋原油具有脱水速度快、油水界面齐、脱出水清
SD破乳剂^[26]	塔河油田重质原油	89	破乳剂用量100mg/L，温度为70℃	—
DS-06/DL11正反破乳剂复配^[27]	呼和浩特炼油厂含油污泥	95	180mg/L，30∶10复配	专一性强，工业应用效果明显
DS-1复配型^[24]	大庆油田北二联合站高机械杂质含量污油	97	4.5h，50℃	—

生物质破乳剂原料	生物质破乳剂	适用乳液类型	DE/%	最佳破乳环境	优点	缺点
花青素^[39]	PC9015	渤海油田老化油乳液	84.6	70℃，2h，100mg/L	脱水性能好，实用性较强，适用于海上平台的原油和老化油破乳，以天然多酚为原料，更为经济、绿色油水界面清晰，无挂壁，取代了用于制备常规石油衍生的壬基酚表面活性剂	挂壁严重
表没食子儿茶素没食子酸酯^[41]	EGA603	渤海油田老化原油乳液	94.3	70℃，100min，100mg/L		挂壁较轻
单宁酸^[43]	TAPA9920	南海油田老化油乳液	97.9	70℃，40min，100mg/L		合成困难
腰果酚^[44]	DECA	阿拉伯重质原油	100	60℃，40min，100mg/L		合成困难，尚在实验室阶段
木质素^[49]	木质素和二氧化硅的高效膜	O/W体系	98.6	与滤纸表面完全接触。一旦有色油被完全过滤掉，分离过程就算作结束	效果明显，分离简单	合成困难，尚在实验室阶段
荷叶^[50]	HLLF	长庆油田	88.17	1000mg/L在70℃下持续90min	油水界面清晰，水质清亮	适用范围较窄，DEMLOCS较其他相似产品剂量颇高
稻壳^[51]	RHC	W/O体系	96.99	600mg/L，70℃，80min	具有较宽的pH范围和良好的耐盐性	适用范围较窄，DEMLOCS较其他相似产品剂量颇高
椰子提取物	DEMLOCS	老化油乳液	88	45℃，24h，2000mg/L	温度适宜，水热法合成步骤简单	适用范围较窄，DEMLOCS较其他相似产品剂量颇高

生物质破乳剂原料	生物质破乳剂	适用乳液类型	DE/%	最佳破乳环境	优点	缺点
花青素^[39]	PC9015	渤海油田老化油乳液	84.6	70℃，2h，100mg/L	脱水性能好，实用性较强，适用于海上平台的原油和老化油破乳，以天然多酚为原料，更为经济、绿色油水界面清晰，无挂壁，取代了用于制备常规石油衍生的壬基酚表面活性剂	挂壁严重
表没食子儿茶素没食子酸酯^[41]	EGA603	渤海油田老化原油乳液	94.3	70℃，100min，100mg/L		挂壁较轻
单宁酸^[43]	TAPA9920	南海油田老化油乳液	97.9	70℃，40min，100mg/L		合成困难
腰果酚^[44]	DECA	阿拉伯重质原油	100	60℃，40min，100mg/L		合成困难，尚在实验室阶段
木质素^[49]	木质素和二氧化硅的高效膜	O/W体系	98.6	与滤纸表面完全接触。一旦有色油被完全过滤掉，分离过程就算作结束	效果明显，分离简单	合成困难，尚在实验室阶段
荷叶^[50]	HLLF	长庆油田	88.17	1000mg/L在70℃下持续90min	油水界面清晰，水质清亮	适用范围较窄，DEMLOCS较其他相似产品剂量颇高
稻壳^[51]	RHC	W/O体系	96.99	600mg/L，70℃，80min	具有较宽的pH范围和良好的耐盐性	适用范围较窄，DEMLOCS较其他相似产品剂量颇高
椰子提取物	DEMLOCS	老化油乳液	88	45℃，24h，2000mg/L	温度适宜，水热法合成步骤简单	适用范围较窄，DEMLOCS较其他相似产品剂量颇高

性能	离子液体	传统破乳剂（表面活性剂）
界面张力	表面活性离子液体可以将界面张力降低到10^-2mN/m，有必要提高离子液体的表面活性，并注意界面张力与盐度的协同作用	可以降低IFT达到10^-4~10^-3mN/m，显示了它们在油水分离应用中的有效性
黏度	离子液体的黏度可以通过支化的变化来调节	在水溶液中，它们无法产生更高的黏度
稳定性	离子液体高温下是稳定的，可以长时间储存而不会分解	表面活性剂在高温下不稳定
毒性	离子液体毒性较小且环保	部分烷基酚表面活性剂毒性大，无法达到降解要求
可回收性	回收离子液体的方法有很多种，如液液萃取、蒸馏、吸附、结晶、力场分离和膜分离等^[53]	不可回收

用于复杂原油乳液的高效破乳剂开发及应用研究进展

Research progress on highly efficient demulsifiers for complex crude oil emulsions and their applications

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离子液体	阳离子	阴离子	乳液类型	剂量/mg·L^-1	DE/%	界面张力降低	结论
C _n mim NTf₂（n=10、12、14）	咪唑啉	双（三氟甲基磺酰基）亚胺	SW/O	100~3500	93.6~100	77~95	对于亲水性离子液体，增加离子液体的剂量和烷基阳离子链长度导致聚集并导致破乳不良以及增加IFT^[61]
C _n mim PF₆（n=10、12、14）		六氟磷酸		500~3500	71.25~86.25	54~81
C _n mim Cl（n=10、12、14）		氯离子		500~3500	76.25~93.75	64~80
三阳离子液体
TNPy	氨基吡啶	溴离子	W/O	250~1000	100	24	研究了烷基链长度、破乳剂剂量和RSN值对破乳活性的影响。结果表明，与含有十六烷基链的TCPyILs相比，壬基和十四烷基链的TCPyILs具有更好和更高的破乳效率。TNPy和TTPyIL对W/O（50/50、30/70和10/90，v/v）的破乳效率即使在低浓度下也达到100%^[62]
TTPy			W/O	250~1000	100	24
TTPy			W/O	250~1000	100	26.5
TCPy			W/O	250~1000	100	26.5
TCPy			W/O	500	100	26
绿色环保的ILs
海藻基	铵	溴离子	SW/O	1000	100	—	BH-ALG和BN-ALG都表现出良好的降低界面张力的能力。在这两种PIL中，BH-ALG的表面活性高于BN-ALG，这可能是由于与BN-ALG相比，其烷基链更长，因此具有更高的疏水性^[63]
松香酸（AA）	咪唑	碘离子	SW/O	250~1000	100	—	在原油与盐水体积比为90∶10时，两种AILs的脱水率均达到100%，这可以称为由于存在聚乙二酸酯环而增加其疏水性^[64]
废弃塑料^[65]	铵	氯离子	W/O	1000	94	34.5	PET废物的糖酵解产生BHET，其与氯化亚砜反应形成BCET，然后与HEOD和DOAD进行季铵化，分别形成相应的两亲性GIL、HEOD-IL和DOAD-IL。HEOD-IL的CMC低于DOAD-IL，两种两亲性GIL中烷基链的存在有助于它们在连续相中的扩散，以取代刚性沥青质薄膜
聚离子液体修饰的磁性纳米复合材料
	乙烯基咪唑	溴离子	W/O	1000	99.9±0.3	18±0.1	对于W/O乳液，1000μg/L的破乳剂，在70℃下2h后获得了(99.9±0.3)%的破乳效率。破乳后，破乳剂的界面张力从(20.0±0.1)mN/m降低到(1.9±0.1)mN/m，证明了其破乳率高。第一次破乳循环后，通破乳剂过外部磁铁从容器中取出，并重新用于下一个破乳循环。重复使用4个循环后，其破乳效率达到89%^[66]

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