油气田压裂返排液高级氧化工艺研究进展

doi:10.16085/j.issn.1000-6613.2025-0399

化工进展 ›› 2025, Vol. 44 ›› Issue (S1): 441-450.DOI: 10.16085/j.issn.1000-6613.2025-0399

• 资源与环境化工 • 上一篇

油气田压裂返排液高级氧化工艺研究进展

马云¹^,²(), 崔家豪¹^,², 杜杰³, 张帆³, 单巧利³, 牛瑞泽¹^,², 白海涛¹^,²()

^1.西安石油大学石油工程学院，陕西省油气田特种增产技术重点实验室，陕西西安 710065
^2.西部低渗-特低渗油藏开发与治理教育部工程研究中心，陕西西安 710065
^3.长庆工程设计有限公司，陕西西安 710018

收稿日期:2025-03-17 修回日期:2025-04-11 出版日期:2025-10-25 发布日期:2025-11-24
通讯作者: 白海涛
作者简介:马云（1975—），女，教授，博士生导师，研究方向为油气田水污染控制技术。E-mail：mayun9401@xsyu.edu.cn。
基金资助:
低渗透油气田勘探开发国家工程实验室开放课题;西安石油大学青年科研创新团队项目(2019QNKYCXTD04)

Prospect of research on advanced oxidation processes for fracturing flowback fluids in oil and gas fields

MA Yun¹^,²(), CUI Jiahao¹^,², DU Jie³, ZHANG Fan³, SHAN Qiaoli³, NIU Ruize¹^,², BAI Haitao¹^,²()

^1.Shaanxi Key Laboratory of Advanced Stimulation Technology for Oil & Gas Reservoirs, Institute of Petroleum Engineering, Xi’an Shiyou University, Xi’an 710065, Shaanxi, China
^2.Engineering Research Center of the Ministry of Education for the Development and Treatment of Western Low Permeability-Ultra-Low Permeability Reservoirs, Xi’an 710065, Shaanxi, China
^3.Changqing Engineering Design Co. , Ltd. , Xi’an 710018, Shaanxi, China

Received:2025-03-17 Revised:2025-04-11 Online:2025-10-25 Published:2025-11-24
Contact: BAI Haitao

摘要/Abstract

摘要：

油气田压裂返排液含大量难降解污染物，传统物理、化学、生物处理技术各有优缺点，但这些技术存在实际应用条件不适宜、有机物去除不全等问题。高级氧化技术可高效降解污染物，提高后续流程的水质适应性。国内外学者进行了大量研究并取得了较大进展，但鲜少有针对油气田压裂返排液处理的归纳总结。因此，本文在分析油气田压裂返排液成分与污染源的基础上，列举了化学剂氧化、电化学氧化、光催化氧化、催化湿式空气氧化等多种高级氧化技术处理典型油气田压裂返排液的反应条件、效果等相关研究进展并进行了对比分析，提出了一系列该领域的发展需求与方向，诸如通过技术创新与工程化集成、开发低成本的非均相催化剂、结合智能化控制，实现深度氧化-膜分离联用等多技术耦合处理模式，以期为该领域的后续研究与实践提供参考。

关键词: 压裂返排液, 高级氧化技术, 氧化, 资源化, 水处理

Abstract:

The fracturing flowback fluids in oil and gas fields contain a large number of refractory pollutants. Traditional physical, chemical and biological treatment technologies have their own advantages and disadvantages, but there are limitations such as inappropriate practical application conditions and incomplete removal of organic matter. The advanced oxidation processes can efficiently degrade pollutants and improve the water quality adaptability of the subsequent process. The domestic and foreign scholars have carried out a lot of researches and made great progress, but the treatment of the fracturing flowback fluids are rarely systematically summarized. Therefore, based on the analysis of the composition and pollution sources of the fracturing flowback fluids, this paper listed and compared the research progress of chemical agent oxidation, electrochemical oxidation, photocatalytic oxidation, catalytic wet air oxidation and other advanced oxidation processes in dealing with the reaction conditions and effects of typical fracturing flowback fluids, and put forward a series of development needs and directions in this field, such as the integration of technological innovation and engineering, the development of low-cost heterogeneous catalysts, combined with intelligent control, the realization of deep oxidation-membrane separation and other multi-technology coupling treatment modes, in order to provide reference for the follow-up research and practice in this field.

Key words: fracturing flowback fluids, advanced oxidation processes (AOPs), oxidation, resource utilization, water treatment

中图分类号:

TE992.2

马云, 崔家豪, 杜杰, 张帆, 单巧利, 牛瑞泽, 白海涛. 油气田压裂返排液高级氧化工艺研究进展[J]. 化工进展, 2025, 44(S1): 441-450.

MA Yun, CUI Jiahao, DU Jie, ZHANG Fan, SHAN Qiaoli, NIU Ruize, BAI Haitao. Prospect of research on advanced oxidation processes for fracturing flowback fluids in oil and gas fields[J]. Chemical Industry and Engineering Progress, 2025, 44(S1): 441-450.

图/表 13

参考文献 64

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参数	巴肯	巴奈特	马塞勒斯	四川盆地	苏里格气田	煤层气
一般理化参数
pH	5.5~8.0	6.5~8.0	3.9~11.8	6.7~8.2	6.4~6.6	5.6~6.6
电导率/μs·cm^-1	259000	11300~179000	61.9~763000	11290~23600	5~50	70~128
总有机碳（TOC）/mg·L^-1	1804~4523	6.2~99.1	1.2~5804	78~1975	—	919~1442
COD/mg·L^-1	20000~79000	850~10520	18.7~51000	358~3477	2000~8000	1400~6100
TSS/mg·L^-1	3134	36.8~253	2~7600	70~455	54~230	35~498
TDS/mg·L^-1	1755~357527	3600~98900	2.8~394600	6906~28900	14000~53000	35000~300000
碱度(以CaCO₃计)/mg·L^-1	2000	215~1630	6.1~1100	600	260~15499	61~1409
硬度(以CaCO₃计)/mg·L^-1	—	840~21000	196~95000	283~1334	5158~36084	7708~48318
有机物
油和脂/mg·L^-1	—	5.6~1720	3.0~1500	17.3	50~120	4~150
苯/mg·L^-1	—	0.049~5.3	0.001~1.3	—	—	—
甲苯/mg·L^-1	—	0.079~8.1	0.000097~2.45	—	—	—
乙苯/mg·L^-1	—	0.0022~0.67	0~0.235	—	—	—

参数	巴肯	巴奈特	马塞勒斯	四川盆地	苏里格气田	煤层气
一般理化参数
pH	5.5~8.0	6.5~8.0	3.9~11.8	6.7~8.2	6.4~6.6	5.6~6.6
电导率/μs·cm^-1	259000	11300~179000	61.9~763000	11290~23600	5~50	70~128
总有机碳（TOC）/mg·L^-1	1804~4523	6.2~99.1	1.2~5804	78~1975	—	919~1442
COD/mg·L^-1	20000~79000	850~10520	18.7~51000	358~3477	2000~8000	1400~6100
TSS/mg·L^-1	3134	36.8~253	2~7600	70~455	54~230	35~498
TDS/mg·L^-1	1755~357527	3600~98900	2.8~394600	6906~28900	14000~53000	35000~300000
碱度(以CaCO₃计)/mg·L^-1	2000	215~1630	6.1~1100	600	260~15499	61~1409
硬度(以CaCO₃计)/mg·L^-1	—	840~21000	196~95000	283~1334	5158~36084	7708~48318
有机物
油和脂/mg·L^-1	—	5.6~1720	3.0~1500	17.3	50~120	4~150
苯/mg·L^-1	—	0.049~5.3	0.001~1.3	—	—	—
甲苯/mg·L^-1	—	0.079~8.1	0.000097~2.45	—	—	—
乙苯/mg·L^-1	—	0.0022~0.67	0~0.235	—	—	—

来源	方式	Fenton试剂用量	反应条件	去除率	优点	缺点
川西某气田^[28]	Fenton	H₂O₂浓度为10mL/L Fe²⁺浓度为9g/L	pH=3.5，反应1h	COD去除率为70.3%	反应相对简单，对设备要求低	反应pH范围较窄，H₂O₂利用率较低，会产生大量含铁污泥
PotiguarBasin油田^[29]	P-Fenton	H₂O₂浓度为10mmol/L Fe²⁺浓度为0.44mmol/L	高压400W汞蒸气灯 T=20℃，反应45min	油去除率为99%	降解效率高，除油效果好，Fe²⁺可循环利用	对光照条件要求高，设备能耗较大，水样必须透明，增加了预处理难度
涪陵焦石坝页岩气开采井^[30]	E-Fenton	H₂O₂浓度为80mL/h	pH=6~7，极板间距为2.5cm，电流密度135mA/cm²，90min后取上清液进行二次反应60min	COD去除率为97.65%	电极反应持续产生H₂O₂，污泥产量少	电极材料选择有限且易腐蚀
黄海模拟压裂返排液^[27]	S-Fenton	H₂O₂浓度为80mmol/L Fe²⁺浓度为5mmol/L	pH=3，超声功率180W，频率20~25kHz，T=39℃，反应30min	COD去除率为81.15%	传质效果好，加快反应进程；自由基产量大，提高矿化效率	超声设备成本较高，能耗较大，对设备稳定性和维护要求高

来源	方式	Fenton试剂用量	反应条件	去除率	优点	缺点
川西某气田^[28]	Fenton	H₂O₂浓度为10mL/L Fe²⁺浓度为9g/L	pH=3.5，反应1h	COD去除率为70.3%	反应相对简单，对设备要求低	反应pH范围较窄，H₂O₂利用率较低，会产生大量含铁污泥
PotiguarBasin油田^[29]	P-Fenton	H₂O₂浓度为10mmol/L Fe²⁺浓度为0.44mmol/L	高压400W汞蒸气灯 T=20℃，反应45min	油去除率为99%	降解效率高，除油效果好，Fe²⁺可循环利用	对光照条件要求高，设备能耗较大，水样必须透明，增加了预处理难度
涪陵焦石坝页岩气开采井^[30]	E-Fenton	H₂O₂浓度为80mL/h	pH=6~7，极板间距为2.5cm，电流密度135mA/cm²，90min后取上清液进行二次反应60min	COD去除率为97.65%	电极反应持续产生H₂O₂，污泥产量少	电极材料选择有限且易腐蚀
黄海模拟压裂返排液^[27]	S-Fenton	H₂O₂浓度为80mmol/L Fe²⁺浓度为5mmol/L	pH=3，超声功率180W，频率20~25kHz，T=39℃，反应30min	COD去除率为81.15%	传质效果好，加快反应进程；自由基产量大，提高矿化效率	超声设备成本较高，能耗较大，对设备稳定性和维护要求高

来源	联用方式	臭氧浓度	反应条件	去除率	优点	缺点
页岩气^[34]	超声波-臭氧	42mg/L	pH=2.5，超声（US）功率800W， 1.5h后加入450mg/L MnO₂	COD去除率为68.17%	空化效应产生局域高温高压，促使臭氧分解产生更多·OH；粉碎作用使臭氧气泡粉碎成微气泡，提高臭氧溶解速度和浓度	能量消耗大，工程化难度大
胜利油田^[35]	活性炭三维电极耦合臭氧（3D/O₃）	80mg/L	电流1A，气体流速0.5L/min，活性炭30g，反应3h	COD去除率为78.00%	活性炭吸附富集污染物；通过电化学氧化技术实现原位再生；多周期运行稳定性好	处理高盐度、高有机物浓度返排液时受限
重庆涪陵某油气田^[36]	高压脉冲-臭氧-Fenton	10mg/L	pH=9，高压脉冲放电电压35kV，放电频率80Hz，脉宽60ns，反应30min；pH=3，H₂O₂浓度为6mL/L，Fe²⁺浓度为5mmol/L，反应60min	COD去除率为99.55%	液电空化效应增大臭氧与返排液的接触面积；碱性条件更有利于产生·OH	对设备、操作要求高，系统较为复杂
四川页岩气^[37]	MFe₂O₄（M=Cu、Ni、Co、Zn）多相耦合臭氧	1440mg/L	催化剂投加量150mg/L 气体流速0.8L/min	COD去除率为66.7%	有效提高返排液的可生化性，大幅降低生物毒性；具有较好的回收性能	制备过程复杂

油气田压裂返排液高级氧化工艺研究进展

Prospect of research on advanced oxidation processes for fracturing flowback fluids in oil and gas fields

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来源	阳极材料	反应条件	去除率	优点	缺点
玛湖油田^[48]	镀钌铱钛板	单向脉冲电源，电流密度25mA/cm²，极板间距为4cm，电源脉冲频率4000Hz、占空比65%，电解时间90min	COD去除率为92.2%，TSS去除率为91.8%，氨氮去除率为91.4%	具有优异的电化学稳定性和较高的析氧电位；镀钌铱层能够保护钛基板不被腐蚀，延长寿命	钌铱涂层成本较高，长期运行经济性较差；脉冲电源设备复杂，维护难度大
长庆油田Z293井^[49]	IrO₂-RuO₂/Ti	直接电化学氧化时，极板间距0.5cm，反应电流0.7A，电解时间120min；预处理-电化学氧化时，极板间距0.5cm，反应电流0.7A，电解时间120min；药剂强化-电化学氧化时，极板间距0.5cm，反应电流0.8A，电解时间180min	直接电化学氧化时，COD去除率为76.1%，TSS去除率为82.5%，氨氮去除率为99.0%，预处理-电化学氧化时，COD去除率为78.0%，TSS去除率为91.8%，氨氮去除率为99.2%，药剂强化-电化学氧化时，COD去除率为87.0%，TSS去除率为93.0%，氨氮去除率为100.0%	具有优异的电催化活性和稳定的化学性质	电极制备工艺复杂，成本较高；对反应条件控制要求严格
某页岩气区块^[50]	PbO₂/Ti	电流密度35mA/cm²，极板间距3cm，脉冲频率1500Hz、占空比50%	COD去除率为91.2%	钛基作为支撑材料，机械强度高；在酸性、高盐环境中耐用	PbO₂易出现析氧反应，电极表面产生钝化膜与杂质沉淀
新疆油田^[51]	IrO₂-RuO₂/Ti	电流密度8.66mA/cm²，极板间距为2.81cm	COD去除率为100.0%	结合了钛基板的耐腐蚀性和RuO₂、IrO₂的高电催化活性；石墨作为阴极材料，具有良好的导电性和化学稳定性，能够承受较高的电流密度	复杂的电极制备工艺导致成本上升；对水质适应性有一定限制，需要预处理
川庆钻探某区块平台^[52]	钛基极板	反应电流60A，电解时间10min	COD去除率为92.0% TSS去除率为95.0%	具有良好的耐腐蚀性和较长的使用寿命；减少副反应的发生，提高电解效率	在高盐度或强酸碱条件下，电化学性能可能受影响；初期投资成本较高

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