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Article(id=1236323800766271647, tenantId=1146029695717560320, journalId=1210938733613449225, issueId=1236323797054312545, articleNumber=null, orderNo=null, doi=10.19666/j.rlfd.202411234, pmid=null, cstr=null, oa=null, hot=null, price=null, onlineType=0, articleFormat=0, articleType=null, articleTypeStr=null, receivedDate=1732464000000, receivedDateStr=2024-11-25, revisedDate=null, revisedDateStr=null, acceptedDate=null, acceptedDateStr=null, onlineDate=1772692163888, onlineDateStr=2026-03-05, pubDate=1758729600000, pubDateStr=2025-09-25, doiRegisterDate=null, doiRegisterDateStr=null, onlineIssueDate=1772692163888, onlineIssueDateStr=2026-03-05, onlineJustAcceptDate=null, onlineJustAcceptDateStr=null, onlineFirstDate=null, onlineFirstDateStr=null, sourceXml=null, magXml=null, createTime=1772692163888, creator=13701087609, updateTime=1772692163888, updator=13701087609, issue=Issue{id=1236323797054312545, tenantId=1146029695717560320, journalId=1210938733613449225, year='2025', volume='54', issue='9', pageStart='1', pageEnd='178', issueExtLink='null', onlineDate='null', pubDate='null', beforeIssueId=null, nextIssueId=null, price=null, status=1, issueComplete=1, articleOrder=1, issueType=-1, specialIssue=null, createTime=1772692163003, creator=13701087609, updateTime=1772692223569, updator=13701087609, preIssue=null, nextIssue=null, ext={EN=IssueExt(id=1236324051153646111, tenantId=1146029695717560320, journalId=1210938733613449225, issueId=1236323797054312545, language=EN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=), CN=IssueExt(id=1236324051153646112, tenantId=1146029695717560320, journalId=1210938733613449225, issueId=1236323797054312545, language=CN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=)}, issueFiles=null}, startPage=79, endPage=85, ext={EN=ArticleExt(id=1236323802209112274, articleId=1236323800766271647, tenantId=1146029695717560320, journalId=1210938733613449225, language=EN, title=Adsorption properties of modified silica gel on Fe3+ in wind turbine gear oil, columnId=1236323798149025895, journalTitle=Thermal Power Generation, columnName=Special topic on low carbon power technology, runingTitle=null, highlight=null, articleAbstract=

A comparative test was conducted on operating oil samples from wind turbine gear oil and a fresh oil sample, revealing that the Fe3+ content was the most rapidly deteriorating indicator. The SG-PEI adsorbent was prepared by loading polyethyleneimine (PEI) onto a silica gel material (SG) through impregnation modification, and its characteristics were evaluated. The adsorption isotherms and kinetics of Fe3+ on SG-PEI were thoroughly investigated. The results indicated that, the adsorption isotherm of Fe3+ on SG-PEI conforms to Langmuir model. The saturated adsorption capacity of SG-PEI for Fe3+ was 28.71 mg/g, representing a 39.2% improvement compared to SG (20.63 mg/g). The adsorption process of Fe3+ on SG-PEI adhered to the pseudo-second-order kinetic model, with adsorption process occurring as a spontaneous exothermic reaction. Under optimal conditions of an adsorption temperature of 60 ℃, an adsorption time of 120 min, and an oil-adsorbent ratio of 100:3, the removal rate of Fe3+ from wind turbine gear oil by SG-PEI reached 96.23%, which is 29.43 times higher than that of the 801 adsorbent (3.27%) and 185.06 times higher than that of Al2O3 (0.52%). The SG-PEI has a good prospect for applications due to its high adsorption capacity and selectivity for Fe3+.

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对风电机组齿轮油运行油样品和新油样品进行对比测试，发现Fe3+含量为劣化最快的指标。通过浸渍改性将聚乙烯亚胺（PEI）负载到硅胶材料（SG）上制备SG-PEI吸附剂并进行表征，研究了Fe3+在SG-PEI上的吸附等温线和动力学。结果表明：Fe3+在SG-PEI上的吸附等温线符合Langmuir吸附模型；SG-PEI对Fe3+饱和吸附量约为28.71 mg/g，相比SG（20.63 mg/g）提升39.2%；SG-PEI对Fe3+的吸附过程符合拟二级动力学模型，吸附过程为自发的放热反应；在吸附温度60 ℃，吸附时间120 min，油剂比100:3的条件下，SG-PEI对风电机组运行齿轮油中Fe3+脱除率达96.23%，是801吸附剂（3.27%）的29.43倍，也是Al2O3（0.52%）的185.06倍，其对齿轮油中Fe3+具有高吸附容量和选择性，具有良好的应用前景。

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夏启斌（1976），男，博士，研究员，主要研究方向为新型环境功能材料和碳基能源材料应用，。
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底广辉（1990），男，硕士，高级工程师，主要研究方向为电力用油监测、诊断、处理，。

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底广辉（1990），男，硕士，高级工程师，主要研究方向为电力用油监测、诊断、处理，。

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底广辉（1990），男，硕士，高级工程师，主要研究方向为电力用油监测、诊断、处理，。

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tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1236323800766271647, language=CN, orderNo=5, keyword=改性)], refs=[Reference(id=1236323816738181973, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1236323800766271647, doi=null, pmid=null, pmcid=null, year=2024, volume=40, issue=7, pageStart=70, pageEnd=72, url=null, language=null, rfNumber=［1］, rfOrder=0, authorNames=徐丹丹, journalName=清洗世界, refType=null, unstructuredReference=徐丹丹. 基于“双碳”目标的清洁能源发电现状及发展分析[J]. 清洗世界, 2024, 40(7): 70-72., articleTitle=基于“双碳”目标的清洁能源发电现状及发展分析, refAbstract=null), Reference(id=1236323816826262364, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1236323800766271647, doi=null, pmid=null, pmcid=null, year=2024, volume=40, issue=7, pageStart=70, pageEnd=72, url=null, language=null, rfNumber=［1］, rfOrder=1, authorNames=XU Dandan, journalName=Cleaning World, refType=null, unstructuredReference=XU Dandan. 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tableContent=null), ArticleFig(id=1236323815064654595, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1236323800766271647, language=EN, label=Tab.1, caption=

Basic properties of gear oil samples and the oil change indicators

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性质壳牌OMALA S2G新油（320号）风电机组运行油1（220号）风电机组运行油2（320号）NB/SH/T 0586—2010L-CKD
40 ℃运动黏度/(mm2·s–1)323.62229.78325.16变化率>15%
20 ℃油密度/(g·cm–3)0.879 90.874 30.873 8
水分/(mg·L–1)55.9(0.006%)182.2(0.02%)119.5(0.013%)>0.5%
酸值/(mgKOH·g–1)0.384 90.383 20.666 4酸值增加>1
Fe3+质量分数/(mg·g–1)<5.017.393.1>200.0
Cu2+质量分数/(mg·g–1)<5<5<5
), ArticleFig(id=1236323815148540680, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1236323800766271647, language=CN, label=表1, caption=

齿轮油样品基本性质以及换油指标

, figureFileSmall=null, figureFileBig=null, tableContent=
性质壳牌OMALA S2G新油（320号）风电机组运行油1（220号）风电机组运行油2（320号）NB/SH/T 0586—2010L-CKD
40 ℃运动黏度/(mm2·s–1)323.62229.78325.16变化率>15%
20 ℃油密度/(g·cm–3)0.879 90.874 30.873 8
水分/(mg·L–1)55.9(0.006%)182.2(0.02%)119.5(0.013%)>0.5%
酸值/(mgKOH·g–1)0.384 90.383 20.666 4酸值增加>1
Fe3+质量分数/(mg·g–1)<5.017.393.1>200.0
Cu2+质量分数/(mg·g–1)<5<5<5
), ArticleFig(id=1236323815257592590, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1236323800766271647, language=EN, label=Tab.2, caption=

Pore parameters of SG and SG-PEI

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材料BET比表面积/(m2·g–1)总孔容/(cm3·g–1)平均孔径/nm
SG312.5761.15811.002
SG-PEI262.5231.02410.318
), ArticleFig(id=1236323815370838803, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1236323800766271647, language=CN, label=表2, caption=

SG与SG-PEI的孔隙参数

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材料BET比表面积/(m2·g–1)总孔容/(cm3·g–1)平均孔径/nm
SG312.5761.15811.002
SG-PEI262.5231.02410.318
), ArticleFig(id=1236323815467307801, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1236323800766271647, language=EN, label=Tab.3, caption=

Mass fractions of element C, N, O and Si

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材料元素质量分数
CNOSi
SG7.67050.3441.99
SG-PEI16.681.5847.2634.48
), ArticleFig(id=1236323815609914146, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1236323800766271647, language=CN, label=表3, caption=

C、N、O、Si元素质量分数

, figureFileSmall=null, figureFileBig=null, tableContent=
材料元素质量分数
CNOSi
SG7.67050.3441.99
SG-PEI16.681.5847.2634.48
), ArticleFig(id=1236323815702188842, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1236323800766271647, language=EN, label=Tab.4, caption=

Fitting parameters of the kinetics models

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材料拟一级动力学模型拟二级动力学模型
qe/(mg·g–1)k1/h–1R2qe/(mg·g–1)k2/(g·mg–1·h–1)R2
SG7.2440.503 90.996 010.4800.177 80.998 99
SG-PEI3.3380.334 60.840 317.5930.588 50.999 97
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动力学模型拟合参数

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材料拟一级动力学模型拟二级动力学模型
qe/(mg·g–1)k1/h–1R2qe/(mg·g–1)k2/(g·mg–1·h–1)R2
SG7.2440.503 90.996 010.4800.177 80.998 99
SG-PEI3.3380.334 60.840 317.5930.588 50.999 97
), ArticleFig(id=1236323815937069876, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1236323800766271647, language=EN, label=Tab.5, caption=

Adsorption thermodynamic parameters

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T/Kk2/(g∙(mg∙h)–1)ΔG0/(kJ∙mol–1)ΔS0/(J∙(mol∙K)–1)ΔH0/(kJ∙mol–1)Ea/(kJ∙mol–1)
3080.539–17.0496.896–14.86215.884
3180.749–16.919
3280.784–17.195
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吸附热力学参数

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T/Kk2/(g∙(mg∙h)–1)ΔG0/(kJ∙mol–1)ΔS0/(J∙(mol∙K)–1)ΔH0/(kJ∙mol–1)Ea/(kJ∙mol–1)
3080.539–17.0496.896–14.86215.884
3180.749–16.919
3280.784–17.195
), ArticleFig(id=1236323816180339518, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1236323800766271647, language=EN, label=Tab.6, caption=

Fitting parameters of the adsorption isotherm equations

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材料Langmuir方程Freundlich方程
qm/(mg∙g–1)KLR2nKFR2
SG26.4961.770.822 62.081.670.739 1
SG-PEI29.818.900.997 04.459.340.829 0
), ArticleFig(id=1236323816289391428, tenantId=1146029695717560320, journalId=1210938733613449225, articleId=1236323800766271647, language=CN, label=表6, caption=

吸附等温方程拟合参数

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材料Langmuir方程Freundlich方程
qm/(mg∙g–1)KLR2nKFR2
SG26.4961.770.822 62.081.670.739 1
SG-PEI29.818.900.997 04.459.340.829 0
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改性硅胶对风电齿轮油中Fe3+的吸附性能
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底广辉 1 , 李师圆 1 , 黄泽宇 2 , 夏启斌 2
热力发电 | 低碳电力技术研究专题 2025,54(9): 79-85
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热力发电 | 低碳电力技术研究专题 2025, 54(9): 79-85
改性硅胶对风电齿轮油中Fe3+的吸附性能
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底广辉1 , 李师圆1, 黄泽宇2, 夏启斌2
作者信息
  • 1.华北电力科学研究院有限责任公司，北京　100045
  • 2.华南理工大学化学与化工学院，广东　广州　510640

    • 底广辉（1990），男，硕士，高级工程师，主要研究方向为电力用油监测、诊断、处理，。

通讯作者:

夏启斌（1976），男，博士，研究员，主要研究方向为新型环境功能材料和碳基能源材料应用，。
Adsorption properties of modified silica gel on Fe3+ in wind turbine gear oil
Guanghui DI1 , Shiyuan LI1, Zeyu HUANG2, Qibin XIA2
Affiliations
  • 1.North China Electric Power Research Institute Co., Ltd., Beijing 100045, China
  • 2.School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou 510640, China
出版时间: 2025-09-25 doi: 10.19666/j.rlfd.202411234
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摘要
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对风电机组齿轮油运行油样品和新油样品进行对比测试，发现Fe3+含量为劣化最快的指标。通过浸渍改性将聚乙烯亚胺（PEI）负载到硅胶材料（SG）上制备SG-PEI吸附剂并进行表征，研究了Fe3+在SG-PEI上的吸附等温线和动力学。结果表明：Fe3+在SG-PEI上的吸附等温线符合Langmuir吸附模型；SG-PEI对Fe3+饱和吸附量约为28.71 mg/g，相比SG（20.63 mg/g）提升39.2%；SG-PEI对Fe3+的吸附过程符合拟二级动力学模型，吸附过程为自发的放热反应；在吸附温度60 ℃，吸附时间120 min，油剂比100:3的条件下，SG-PEI对风电机组运行齿轮油中Fe3+脱除率达96.23%，是801吸附剂（3.27%）的29.43倍，也是Al2O3（0.52%）的185.06倍，其对齿轮油中Fe3+具有高吸附容量和选择性，具有良好的应用前景。

齿轮油  /  吸附再生  /  金属脱除  /  硅胶  /  改性

A comparative test was conducted on operating oil samples from wind turbine gear oil and a fresh oil sample, revealing that the Fe3+ content was the most rapidly deteriorating indicator. The SG-PEI adsorbent was prepared by loading polyethyleneimine (PEI) onto a silica gel material (SG) through impregnation modification, and its characteristics were evaluated. The adsorption isotherms and kinetics of Fe3+ on SG-PEI were thoroughly investigated. The results indicated that, the adsorption isotherm of Fe3+ on SG-PEI conforms to Langmuir model. The saturated adsorption capacity of SG-PEI for Fe3+ was 28.71 mg/g, representing a 39.2% improvement compared to SG (20.63 mg/g). The adsorption process of Fe3+ on SG-PEI adhered to the pseudo-second-order kinetic model, with adsorption process occurring as a spontaneous exothermic reaction. Under optimal conditions of an adsorption temperature of 60 ℃, an adsorption time of 120 min, and an oil-adsorbent ratio of 100:3, the removal rate of Fe3+ from wind turbine gear oil by SG-PEI reached 96.23%, which is 29.43 times higher than that of the 801 adsorbent (3.27%) and 185.06 times higher than that of Al2O3 (0.52%). The SG-PEI has a good prospect for applications due to its high adsorption capacity and selectivity for Fe3+.

gear oil  /  adsorption regeneration  /  metal removal  /  silica gel  /  modification
底广辉, 李师圆, 黄泽宇, 夏启斌. 改性硅胶对风电齿轮油中Fe3+的吸附性能. 热力发电, 2025 , 54 (9) : 79 -85 . DOI: 10.19666/j.rlfd.202411234
Guanghui DI, Shiyuan LI, Zeyu HUANG, Qibin XIA. Adsorption properties of modified silica gel on Fe3+ in wind turbine gear oil[J]. Thermal Power Generation, 2025 , 54 (9) : 79 -85 . DOI: 10.19666/j.rlfd.202411234
正文
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作为世界上最大的能源消费国，我国十分重视清洁能源发电技术的研发和应用，积极推动新能源行业发展，力争实现“碳达峰、碳中和”[1]。风能作为一种清洁无公害的可再生能源，与传统火力发电相比，风力发电具有零排放、污染小、成本低等优点，因此成为目前全球发展最快的新能源之一[2]。
风电增速齿轮箱是双馈型风力发电机组的核心部件，它将低转速的风轮所携带的功率转换为与发电机匹配的高转速低扭矩功率，它的运转性能决定着风力发电整机的发电量[3]。造成风电齿轮箱失效的原因有设计、安装、环境和齿轮油等，其中齿轮油为风电齿轮箱提供主要的润滑作用，但在工作过程中可能会受到恶劣环境的影响，造成齿轮油的劣化，出现性能下降、润滑不良等问题，影响风电齿轮箱的稳定运行并产生大量废润滑油[4-5]。大量的废油直接丢弃会造成极大的环境污染，因此废油再生与循环利用具有重要意义[6]。
风电齿轮油油品劣化故障案例中统计较多的为黏度超标（34%）与Fe磨损元素超标（27%）[7]。若油液中出现磨损元素异常增加，反映出齿轮异常磨损状态，会导致润滑油劣化，影响油品使用寿命。Fe元素是摩擦副材质的最主要物质，在风机运行中，Fe元素含量也是判断齿轮箱内部磨损情况的主要指标，《工业闭式齿轮油换油指标》（NB/SH/T 0586—2010）中指出油品Fe3+质量分数高于200 μg/g时需换油处理。目前，关于废油吸附再生常以色度、酸值、黏度、密度等常规性质作为指标[8-11]，对于油品中金属离子的脱除研究较少[12-13]。因此，开发出一种针对风电机组齿轮油中Fe3+脱除的技术具有重要研究价值。
吸附技术是一种广泛用于废油再生的重要手段，吸附剂是吸附技术的核心[8]。本研究对常用吸附材料进行了初步筛选，并对筛选出的最优吸附材料进行改性，使其对于油中Fe3+具有高效吸附脱除性能。
1　实验内容
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1.1　试剂及仪器
本文齿轮油运行油样品采集于两处风电机组，其与壳牌OMALA S2G新油的物化参数列于表1。氢氧化钾、无水乙醇、甲醇、酚酞、甲酚红、聚乙烯亚胺（分子量为600）均为分析纯试剂，VHG-21磨损元素标油（Fe，1 000 μg/g）购于英国LGC公司，硅胶细砂购于青岛硕远硅胶科技有限公司，白油购于广州穗欣化工有限公司、溶剂油购于广东文天环保清洗液科技有限公司。主要测试仪器包括石油产品运动黏度测定仪、石油产品微量水分测定仪、安捷伦240FS AA火焰原子吸收光谱仪。
1.2　实验部分
1.2.1　改性材料的制备
通过在硅胶（SG）表面修饰聚乙烯亚胺（PEI）合成吸附剂（SG-PEI）。硅胶使用前进行酸洗活化除杂[14]，称取一定活化后的硅胶，加入30 mL 5%的PEI-甲醇溶液，室温下浸渍搅拌24 h，用去离子水、甲醇洗涤后，放入60 ℃烘箱干燥过夜，得到SG-PEI吸附剂。
1.2.2　改性材料的表征测试
改性材料XRD测试在Bruker D8 ADVANCE多晶衍射仪上进行。N2吸脱附测试在Micromeritics ASAP 2460全自动比表面与孔径分析仪上进行，材料测试前要在150 ℃真空脱气12 h，采用BET方程和BJH模型计算材料比表面积、孔容和平均孔径。在Thermo Nicolet IS50红外光谱仪上进行FTIR测试。SEM/EDS测试在HITACH SU8600超高分辨场发射扫描电子显微镜上进行，加速电压15 kV。
1.2.3　Fe3+吸附实验
由于齿轮油体系复杂，为了消除各类添加剂对实验的干扰，更好地分析材料的吸附行为，本实验通过白油添加VHG-21磨损标油配制模拟油进行吸附实验。配置Fe3+初始质量分数为100 μg/g的模拟油，加入一定量的SG-PEI，在室温和不同温度下，分别以5、10、20、40、60 min及2、5、10、24 h作为取样时间点，完成吸附动力学与热力学测试。配置不同Fe3+初始质量分数（70、120、180、260、290、380 μg/g）的模拟油，加入一定量的SG-PEI，吸附平衡后静置取上清油样过滤测定Fe3+质量分数，完成等温吸附实验。
1.2.4　运行油样品吸附对比实验
选用风电机组运行油2（ULO2）进行吸附材料筛选实验。具体操作为：ULO2自然沉降24 h后，取50 g上清油样，与1.5 g SG-PEI混合，在60 ℃下恒温搅拌120 min，静置分层，取上清液油样过滤后进行分析。油样黏度通过石油产品运动黏度测定仪测试，水分通过石油产品微量水分测定仪测试，酸值按照GB/T 264标准进行测试，Fe3+含量按照SH/T 0077—1991标准进行测试。
2　结果与讨论
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2.1　新油及运行油样品分析
油样基本性质与《工业闭式齿轮油换油指标》（NB/SH/T 0586—2010）标准见表1。从表1可以看出，2种运行油运动黏度与密度未发生明显降低，说明其油膜强度、接触面隔离能力并未损失较多[7]，水分、酸值与Fe3+质量分数均有不同程度增加。值得注意的是，运行油2的Fe3+质量分数为93.1 μg/g，相比其他性质更接近换油指标。
新油与2种风电机组运行油的红外光谱如图1所示。2 958~2 854 cm–1代表CH3和CH2的伸缩振动，1 463、1 377 cm–1是CH3和CH2的变形振动。 2种运行油在1 734 cm–1附近出现了强的C=O吸收峰[15]，在1 162 cm–1处出现了C-O吸收峰[16]，说明运行油中产生了一定量的酸、醛、酮等氧化产物[11,17-18]。
2.2　改性硅胶的表征
2.2.1　比表面及孔径分析
77 K下N2在PEI改性SG前后材料上的吸脱附曲线如图2所示。由图2可见，N2在SG与SG-PEI上的吸脱附曲线均属于介孔材料特有的IV型等温线[19]，存在明显H2型回滞环，其孔径参数列于表2。由表2可知，SG与SG-PEI的BET比表面积为312.576 m2/g和262.523 m2/g，改性后材料的孔容、孔径等均略有下降，这可能是由于材料吸附了PEI使得表面官能团增加[20]，部分孔道被PEI占据所致。
图3为SG与SG-PEI的孔径分布。由图3可以看出，PEI改性前后材料均以5~20 nm介孔为主，利于吸附扩散。
2.2.2　FTIR表征
SG与SG-PEI材料的FTIR光谱如图4所示。其中，波数3 454、1 639 cm–1处的峰对应于样品中的O-H振动，1 100 cm–1处的大包峰对应于Si-O-Si的拉伸振动[19,21]，804、484 cm–1处的峰对应于硅胶中Si-O-Si的弯曲振动[22]。对于改性后的材料， 3 454 cm–1处的峰宽、峰高均有减小，可能是硅胶表面-OH基团参与反应[23]。改性后的材料出现了许多PEI的特征峰：2 855 cm–1处的峰归因于C-H键的振动，1 540 cm–1处的峰归因于N-H的弯曲振动[24]，1 470 cm–1处的峰归因于C-N键的伸缩振动[19]。这说明浸渍改性后PEI成功涂覆在硅胶材料表面。
2.2.3　XRD表征
SG与SG-PEI材料XRD谱图如图5所示。硅胶为无定形材料，衍射峰强度均较低，且衍射峰位置接近，无新增特征峰出现。
2.2.4　SEM/EDS表征
使用扫描电子显微镜观察改性前后材料的表面形貌和元素分布情况，结果如图6所示。材料改性前后并未出现典型外观，均为不规则结构。
EDS mapping元素含量测试结果见表3。改性前SG样品N元素质量分数为0，改性后SG-PEI样品中的C与N元素质量分数均有上升，证明了PEI的有效负载。
2.3　改性硅胶吸附油中Fe3+的动力学分析
图7为SG与SG-PEI的qt-t曲线。由图7中可以看出：SG吸附Fe3+的吸附速率缓慢上升，5 h后吸附基本平衡；SG-PEI在初始阶段吸附速率极快，1 h后吸附速率放缓，同样在5 h左右基本达到平衡；SG-PEI对Fe3+吸附量（17.54 mg/g）显著高于SG（10.28 mg/g）。
采用拟一级动力学模型、拟二级动力学模型对SG与SG-PEI吸附油中Fe3+的动力学过程进行拟合分析。所采用的动力学方程如下。
拟一级动力学模型：
ln(qe−qt)=lnqe−k1t
拟二级动力学模型：
tqt=1qe⋅t+1k2qe2
式中：qe为平衡吸附量，mg/g；qt为时间t时的吸附量，mg/g；t为吸附时间，h；k1为拟一级吸附速率常数，h–1；k2为拟二级吸附速率常数，g/(mg∙h)。
拟一级动力学模型和拟二级动力学模型，拟合参数结果见表4。拟合结果显示：SG与SG-PEI拟二级动力学模型计算得到的平衡吸附量更接近实验值，而拟一级动力学模型计算平衡吸附量远低于实验值；另外，SG-PEI拟二级动力学模型得到的相关系数R2为0.999 97。因此，拟二级动力学模型能更好地解释其吸附行为，进一步说明了吸附过程由化学吸附主导[25]，存在化学键的断裂和产生，可能是N、O等原子与Fe3+配位的过程。
2.4　改性硅胶吸附油中Fe3+的热力学分析
图8为308、318、328 K下吸附材料的qt-t曲线。由图8可见，SG-PEI对Fe3+的吸附量随温度升高略有减小，说明吸附过程可能是放热反应。为了更好分析吸附过程与温度的关系，通过式(3)—式(5)对测试结果进行拟合分析，拟合结果见表5。
lnK0=ΔS0R−ΔH0RT
ΔG0=ΔH0−TΔS0
lnk2=lnA−EaRT
式中：K0为无因次热力学平衡常数；ΔS0为标准熵变，J/(mol∙K)；ΔH0为标准焓变，kJ/mol；ΔG0为吉布斯自由能变，kJ/mol；Ea为表观活化能，kJ/mol；k2为速率常数，g/(mg∙h)；A为常数；R为摩尔气体常数，8.314 J/(mol∙K)。
表5为吸附热力学参数。由表5中拟合结果可知，随着温度升高，速率常数k2值有所增加，说明温度升高有利于提升吸附速率。反应的标准焓变ΔH0=–14.862 kJ/mol，说明其为放热反应，升高温度不利于吸附进行，对应于图8曲线中吸附量的降低。反应标准熵变ΔS0>0，表明吸附过程中体系的无序度增加。在不同温度下ΔG0值均小于0，说明吸附过程为自发过程，并且随着温度的升高，ΔG0绝对值先减小后增加，这可能是由于反应为放热反应，温度升高抑制吸附进行，另一方面温度升高会降低油相的黏度[7]，固液两相接触更充分，在一定程度上促进了吸附的进行，因此，该体系下吸附过程的难易程度与温度并非简单的线性关系。
2.5　改性硅胶对油中Fe3+的吸附等温线
SG与SG-PEI的吸附等温线如图9所示。由图9可知，存在明显平台区，SG-PEI对Fe3+的饱和吸附量约为28.71 mg/g，而SG平衡吸附量约为20.63 mg/g。SG-PEI相比SG对Fe3+吸附量提升了39.2%。这是由于PEI中具有丰富的氨基基团（图10），其中的N原子能够提供电子，形成空腔，与Fe3+配位络合形成螯合环，从而有效吸附Fe3+[19,25-26]。
使用Langmuir和Freundlich模型对吸附等温线进行拟合，拟合参数见表6，方程表达式如下。
Langmuir方程：
Ceqe=Ceqm+KLqm
Freundlich方程：
lnqe=1n⋅lnCe+lnKF
式中：Ce为平衡质量分数，mg/kg；qm为饱和吸附量，mg/g；KL为Langmuir常数；n与KF为Freundlich常数。
由表6中参数可知，Langmuir方程的R2大于Freundlich方程R2，说明相对于Freundlich模型，Langmuir模型能够更好描述吸附过程，且吸附过程具有单层吸附的特征。
2.6　运行油样品吸附净化对比实验
在吸附温度60 ℃，吸附时间120 min，油剂比100:3的条件下测试了SG-PEI与其他常规吸附剂对风电机组运行油2（320号）的净化效果，结果如图11所示。吸附处理后上清油液样品Fe3+质量分数为3.51 μg/g，油样酸值为0.263 mgKOH/g，水分为65 mg/L，Fe3+脱除率为96.23%，是801吸附剂（Fe3+脱除率3.27%）的29.43倍，是Al2O3吸附剂（Fe3+脱除率0.52%）的185.06倍。
3　结论
收起
1）对运行油样品进行对比测试发现Fe3+含量相比其他基础指标劣化更快。
2）采用浸渍法制备了SG-PEI材料，PEI成功负载并且材料介孔结构保持良好。SG-PEI对油中Fe3+具有高吸附容量（28.71 mg/g），吸附过程为单层吸附，符合拟二级动力学模型，为自发的放热反应。
3）SG-PEI对齿轮油样品中Fe3+的脱除能力远高于801、Al2O3等常规吸附剂，并且能够有效降低酸值、水分等指标。这表明SG-PEI是一种优良的齿轮油再生吸附剂，同时浸渍合成简单，具有良好的应用前景。
基金
收起
  • 华北电力科学研究院有限责任公司科研项目(KJZ2023119)
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doi: 10.19666/j.rlfd.202411234
  • 接收时间：2024-11-25
  • 首发时间：2026-03-05
  • 出版时间：2025-09-25
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  • 收稿日期：2024-11-25
基金
Scientific Research Project of North China Electric Power Research Institute Co., Ltd.(KJZ2023119)
华北电力科学研究院有限责任公司科研项目(KJZ2023119)
作者信息
    1.华北电力科学研究院有限责任公司，北京　100045
    2.华南理工大学化学与化工学院，广东　广州　510640

通讯作者:

夏启斌（1976），男，博士，研究员，主要研究方向为新型环境功能材料和碳基能源材料应用，。
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2种不同金属材料的力学参数
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Number of
genus		 种数
Number of
species		 占总种数比例
Percentage of
total species (%)		 属
Genus		 种数
Number of
species		 占总种数比例
Percentage of total
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鹅膏菌科Amanitaceae 2 11 5.26 鹅膏菌属 Amanita 10 4.78
小菇科 Mycenaceae 2 12 5.74 丝盖伞属 Inocybe 5 2.39
多孔菌科 Polyporaceae 8 14 6.70 蜡蘑属 Laccaria 5 2.39
红菇科 Russulaceae 3 23 11.00 小皮伞属 Marasmius 6 2.87
小菇属 Mycena 11 5.26
光柄菇属 Pluteus 5 2.39
红菇属 Russula 17 8.13
栓菌属 Trametes 5 2.39
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