Article(id=1320176229567807530, tenantId=1146029695717560320, journalId=1301849854269554754, issueId=1320176147946648091, articleNumber=null, orderNo=null, doi=10.11729/syltlx20250126, pmid=null, cstr=null, oa=null, hot=null, price=null, onlineType=0, articleFormat=0, articleType=null, articleTypeStr=null, receivedDate=1767110400000, receivedDateStr=2025-12-31, revisedDate=1770825600000, revisedDateStr=2026-02-12, acceptedDate=1772640000000, acceptedDateStr=2026-03-05, onlineDate=1792684140816, onlineDateStr=2026-10-22, pubDate=1787587200000, pubDateStr=2026-08-25, doiRegisterDate=null, doiRegisterDateStr=null, onlineIssueDate=1792684140816, onlineIssueDateStr=2026-10-22, onlineJustAcceptDate=null, onlineJustAcceptDateStr=null, onlineFirstDate=null, onlineFirstDateStr=null, sourceXml=null, magXml=null, createTime=1792684140816, creator=13701087609, updateTime=1792684140816, updator=13701087609, issue=Issue{id=1320176147946648091, tenantId=1146029695717560320, journalId=1301849854269554754, year='2026', volume='40', issue='4', pageStart='1', pageEnd='137', issueExtLink='null', onlineDate='null', pubDate='1787587200000', pubDateStr='2026-08-25', beforeIssueId=null, nextIssueId=null, price=null, status=1, issueComplete=1, articleOrder=1, issueType=1, specialIssue=null, createTime=1792684121357, creator='13701087609', updateTime=1792720571222, updator='13701087609', preIssue=null, nextIssue=null, articleTotal=null, ext={EN=IssueExt(id=1320329029853495708, tenantId=1146029695717560320, journalId=1301849854269554754, issueId=1320176147946648091, language=EN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=), CN=IssueExt(id=1320329029853495709, tenantId=1146029695717560320, journalId=1301849854269554754, issueId=1320176147946648091, language=CN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=)}, issueFiles=null, downloadFileDto=null}, startPage=105, endPage=116, ext={EN=ArticleExt(id=1320176231715291179, articleId=1320176229567807530, tenantId=1146029695717560320, journalId=1301849854269554754, language=EN, title=Electro–elasto–microfluidic precisely tuned manipulation of particles regulated by polymer chain length, columnId=1320176148672262684, journalTitle=Journal of Experiments in Fluid Mechanics, columnName=Special Issue on Microscale and Nanoscale Flows, runingTitle=null, highlight=null, articleAbstract=

Electro–elasto–microfluidic technology integrates the high controllability of electric fields with the viscoelasticity of non-Newtonian fluids, representing a frontier approach for precise manipulation of particles at the micro- and nanoscale. However, existing studies have predominantly focused on macroscopic rheological properties and particle size effects, while the influence of microscopic rheological parameters—such as polymer chain length—on particle migration behavior remains insufficiently understood. In particular, the coupling mechanism between the polymer chain length and slip-velocity-induced lift has yet to be elucidated. In this study, an electro–elasto–microfluidic system with tunable viscoelastic parameters was designed, and a control strategy incorporating polymer chain-scale parameters was established to systematically investigate the effects of polymer solutions with different chain lengths and concentrations on the migration of nano- and microparticles. Experimental results demonstrate that the polymer chain length plays a critical role in regulating the lift force balance in electro–elasto–coupled systems. Numerical simulations further reveal that the polymer chain length significantly influences the particle slip velocity. The particle slip velocity Us exhibits an approximately linear dependence on the ratio between the force acting on the particle and its radius, Fp/R. With increasing polymer chain length, the slip velocity Us decreases monotonically under identical Fp/R conditions. Theoretical analysis indicates that, as particle size decreases, the flow-induced elastic lift decays much more rapidly than the slip-induced lift, causing the latter to dominate nanoparticle manipulation. Based on these findings, efficient nanoparticle focusing at prescribed flow velocities, as well as high-throughput continuous separation of particles spanning the nano- to microscale, were achieved by appropriately matching polymer chain length and concentration. This work not only elucidates the microscopic regulatory role of the polymer chain length—a key microrheological parameter—on macroscopic particle dynamics, but also provides a new theoretical foundation and design strategy for electro–elasto–synergistically driven microfluidic sorting technologies.

, authors=Xinlei Qi, Shuhao Ma, Guoqing Hu*, authorsList=Xinlei Qi, Shuhao Ma, Guoqing Hu, authorCompany=null, correspAuthors=Guoqing Hu, authorNote=null, correspAuthorsNote=null, copyrightStatement=Copyright ©2026 Journal of Experiments in Fluid Mechanics. All rights reserved., copyrightOwner=null, extLink=null, articleAbsUrl=null, sourceXml=null, magXml=null, pdfUrl=null, pdf=null, pdfFileSize=null, pdfExtLink=null, richHtmlUrl=null, mobilePdfUrl=null, reviewReport=null, pdfFirstPage=null, abstractGraph=null, abstractGraphContent=null, abstractVideo=null, citation=null, cebUrl=null, magXmlContent=null, mapNumber=null, fund=null), CN=ArticleExt(id=1320176263554253013, articleId=1320176229567807530, tenantId=1146029695717560320, journalId=1301849854269554754, language=CN, title=聚合物链长调控的电场–弹性微流控颗粒精确操控机制研究, columnId=1320176148844229150, journalTitle=实验流体力学, columnName=微纳尺度流动专刊, runingTitle=null, highlight=null, articleAbstract=

电场–弹性微流控技术结合了电场的可控性与非牛顿流体的黏弹性,是微纳尺度颗粒精准操控的前沿方法。然而,现有研究多聚焦于宏观流变特性和颗粒尺寸效应,而聚合物链长等微观流变学参数对颗粒迁移行为的影响,特别是其与滑移速度诱导升力的耦合机制,尚不明确。本文设计了可调黏弹性参数的电场–弹性微流控系统,构建了包含聚合物链尺度参数的调控方案,研究了不同链长与质量分数的聚合物溶液对纳米及微米颗粒迁移行为的影响。实验结果显示,聚合物链长显著调控了电场–弹性耦合体系的升力平衡。结合数值模拟进一步表明,聚合物链长对颗粒滑移速度具有显著影响,颗粒滑移速度Us与施加在颗粒上的力和颗粒半径的比值Fp/R呈近似线性关系。随着聚合物链长的增加,在相同Fp/R条件下,滑移速度Us不断减小。理论分析表明,随着颗粒尺寸减小,流动诱导弹性升力的衰减速度远快于滑移诱导升力,使后者在纳米颗粒操控中占据主导地位。基于此规律,通过合理匹配聚合物链长与质量分数,实现了在特定流速下纳米颗粒的高效聚焦以及纳–微米尺度颗粒的高通量连续分离。该研究不仅揭示了微观流变学参数—聚合物链长对颗粒宏观动力学的微观调控机制,也为基于电场–弹性协同驱动的微流控分选技术提供了新的理论基础与设计策略。

, authors=綦新磊, 马淑浩, 胡国庆*, authorsList=綦新磊, 马淑浩, 胡国庆, authorCompany=null, correspAuthors=胡国庆, authorNote=

綦新磊(1996—),男,博士。研究方向:微纳流体力学。E-mail:

, correspAuthorsNote=
E-mail:
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綦新磊(1996—),男,博士。研究方向:微纳流体力学。E-mail:

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綦新磊(1996—),男,博士。研究方向:微纳流体力学。E-mail:

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Calculation of relaxation times for PEO solutions at different concentrations

, figureFileSmall=null, figureFileBig=null, tableContent=
PEO分子量/kDacc*/10−6c/c*λz/msλ/ms
6000.2%18771.10.0460.88
6000.6%18773.20.0461.76
20000.2%8582.30.33510.4
20000.6%8587.00.33521.4
40000.2%5473.71.05244.3
40000.6%54711.01.05290.0
), ArticleFig(id=1320176363068306072, tenantId=1146029695717560320, journalId=1301849854269554754, articleId=1320176229567807530, language=CN, label=表1, caption=

不同质量分数PEO溶液的松弛时间

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PEO分子量/kDacc*/10−6c/c*λz/msλ/ms
6000.2%18771.10.0460.88
6000.6%18773.20.0461.76
20000.2%8582.30.33510.4
20000.6%8587.00.33521.4
40000.2%5473.71.05244.3
40000.6%54711.01.05290.0
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聚合物链长调控的电场–弹性微流控颗粒精确操控机制研究
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綦新磊 , 马淑浩 , 胡国庆 *
实验流体力学 | 微纳尺度流动专刊 2026,40(4): 105-116
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实验流体力学 |微纳尺度流动专刊 2026 , 40 (4) : 105 -116
聚合物链长调控的电场–弹性微流控颗粒精确操控机制研究
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綦新磊 , 马淑浩, 胡国庆*
作者信息
  • 浙江大学 工程力学系 流体动力与机电系统国家重点实验室,杭州 310027
通讯作者:
作者简介:

綦新磊(1996—),男,博士。研究方向:微纳流体力学。E-mail:

Electro–elasto–microfluidic precisely tuned manipulation of particles regulated by polymer chain length
Xinlei Qi , Shuhao Ma, Guoqing Hu*
Affiliations
  • State Key Laboratory of Fluid Power and Mechatronic Systems, Department of Engineering Mechanics,Zhejiang University, Hangzhou 310027, China
出版时间: 2026-08-25 doi: 10.11729/syltlx20250126
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电场–弹性微流控技术结合了电场的可控性与非牛顿流体的黏弹性,是微纳尺度颗粒精准操控的前沿方法。然而,现有研究多聚焦于宏观流变特性和颗粒尺寸效应,而聚合物链长等微观流变学参数对颗粒迁移行为的影响,特别是其与滑移速度诱导升力的耦合机制,尚不明确。本文设计了可调黏弹性参数的电场–弹性微流控系统,构建了包含聚合物链尺度参数的调控方案,研究了不同链长与质量分数的聚合物溶液对纳米及微米颗粒迁移行为的影响。实验结果显示,聚合物链长显著调控了电场–弹性耦合体系的升力平衡。结合数值模拟进一步表明,聚合物链长对颗粒滑移速度具有显著影响,颗粒滑移速度Us与施加在颗粒上的力和颗粒半径的比值Fp/R呈近似线性关系。随着聚合物链长的增加,在相同Fp/R条件下,滑移速度Us不断减小。理论分析表明,随着颗粒尺寸减小,流动诱导弹性升力的衰减速度远快于滑移诱导升力,使后者在纳米颗粒操控中占据主导地位。基于此规律,通过合理匹配聚合物链长与质量分数,实现了在特定流速下纳米颗粒的高效聚焦以及纳–微米尺度颗粒的高通量连续分离。该研究不仅揭示了微观流变学参数—聚合物链长对颗粒宏观动力学的微观调控机制,也为基于电场–弹性协同驱动的微流控分选技术提供了新的理论基础与设计策略。

微流控  /  颗粒操控  /  非牛顿流体  /  微纳尺度流动

Electro–elasto–microfluidic technology integrates the high controllability of electric fields with the viscoelasticity of non-Newtonian fluids, representing a frontier approach for precise manipulation of particles at the micro- and nanoscale. However, existing studies have predominantly focused on macroscopic rheological properties and particle size effects, while the influence of microscopic rheological parameters—such as polymer chain length—on particle migration behavior remains insufficiently understood. In particular, the coupling mechanism between the polymer chain length and slip-velocity-induced lift has yet to be elucidated. In this study, an electro–elasto–microfluidic system with tunable viscoelastic parameters was designed, and a control strategy incorporating polymer chain-scale parameters was established to systematically investigate the effects of polymer solutions with different chain lengths and concentrations on the migration of nano- and microparticles. Experimental results demonstrate that the polymer chain length plays a critical role in regulating the lift force balance in electro–elasto–coupled systems. Numerical simulations further reveal that the polymer chain length significantly influences the particle slip velocity. The particle slip velocity Us exhibits an approximately linear dependence on the ratio between the force acting on the particle and its radius, Fp/R. With increasing polymer chain length, the slip velocity Us decreases monotonically under identical Fp/R conditions. Theoretical analysis indicates that, as particle size decreases, the flow-induced elastic lift decays much more rapidly than the slip-induced lift, causing the latter to dominate nanoparticle manipulation. Based on these findings, efficient nanoparticle focusing at prescribed flow velocities, as well as high-throughput continuous separation of particles spanning the nano- to microscale, were achieved by appropriately matching polymer chain length and concentration. This work not only elucidates the microscopic regulatory role of the polymer chain length—a key microrheological parameter—on macroscopic particle dynamics, but also provides a new theoretical foundation and design strategy for electro–elasto–synergistically driven microfluidic sorting technologies.

microfluidics  /  particle manipulation  /  non-Newtonian fluids  /  micro- and nanoscale flows
綦新磊, 马淑浩, 胡国庆. 聚合物链长调控的电场–弹性微流控颗粒精确操控机制研究. 实验流体力学, 2026 , 40 (4) : 105 -116 . DOI: 10.11729/syltlx20250126
Xinlei Qi, Shuhao Ma, Guoqing Hu. Electro–elasto–microfluidic precisely tuned manipulation of particles regulated by polymer chain length[J]. Journal of Experiments in Fluid Mechanics, 2026 , 40 (4) : 105 -116 . DOI: 10.11729/syltlx20250126
微纳尺度颗粒操控是近年来在微纳流体力学[1-3]、生物医学工程[4]、材料合成[5-6]与药物递送[7-8]等领域交叉发展起来的重要研究方向。鉴于多数生物流体(如血液、黏液)具有非牛顿特性[9-10],对其中外泌体、病毒等纳米尺度样本的高效分选开展研究具有重要的力学意义与应用价值[11]。微流控是研究微颗粒精细操控的重要方法,目前的微流控技术已发展出了惯性[12-13]、黏弹性微流控[14]等被动方法,以及利用外加物理场(声场[15]、光场[16]、电场[17-19]及振荡[20]等)的主动微流控方法。其中,电场具有可精确调控、即时响应且对颗粒损伤低的优势。电场–弹性微流控方法结合了电场的精确可控性与非牛顿流体的黏弹性,为微纳颗粒的高效聚焦与分离提供了新途径。浸入电解质溶液中的颗粒周围会形成一层薄薄的双电层[21]。当在溶液中施加直流电场时,颗粒会在电场作用下发生滑移,产生领先或滞后于周围流体的速度。滑移速度Us定义为U–Up,其中U是流体速度,Up是颗粒速度[22]。非牛顿流体在微通道内流动产生非均匀剪切梯度,通过施加直流电场,将颗粒滑移与微流体黏弹性流动相结合,可实现微米乃至纳米尺度颗粒在微通道内的可控横向迁移[23]。然而,现有电场–弹性微流控研究多集中于微米尺度及宏观流变特性[1],缺乏对纳米尺度下聚合物链长等微观参数与电场驱动滑移升力耦合机制的系统探讨。
聚合物在流体中的存在不仅影响整体的流变性质,其分子链长、质量分数及相互作用方式还可能显著改变流体内局部应力场的分布[24],从而对颗粒在电场作用下的运动轨迹产生潜在影响。微流控技术为观察颗粒在黏弹性流体中的动态行为提供了有力支持[14]。Li等[25]在颗粒的电场–弹性微流控实验中发现,不同方向直流电场的作用下,当颗粒领先或滞后于黏弹性聚氧化乙烯(Polyethylene Oxide, PEO)溶液流动时,颗粒会向矩形微通道的中心或壁角迁移。该迁移行为与聚合物的分子量和质量分数密切相关,在低质量分数下逐渐表现为牛顿流体特征,而随着质量分数从远低于聚合物重叠质量分数增加至高于该质量分数,颗粒迁移模式由牛顿型过渡到黏弹性型[26]。Serhatlioglu等[27]通过实验揭示了在微流控通道中同时施加压力驱动流与直流电场时,黏弹性非牛顿流体中颗粒的横向迁移由滑移、弹性、剪切梯度等多种因素导致的升力之间的相互耦合作用决定,并解释了牛顿流体与不同黏弹性流体中复杂的颗粒聚焦行为及横向不均匀黏弹性的形成机理。Bentor等[28]通过实验验证了聚合物溶液中颗粒电泳迁移率与颗粒粒径之间的关系,并且发现这种尺寸依赖性随聚合物质量分数或链长的增加而增强。以上文献中的实验和理论研究主要针对微米尺寸颗粒的电场–弹性迁移,连续介质流体力学理论在描述宏观流动时具有较高的准确性;但在纳米尺度下,由于更微观尺度的分子级相互作用以及电场作用的复杂耦合,传统理论往往难以给出精确解释。Liu等[29]在黏弹性微流控实验中比较了不同分子量黏弹性聚合物溶液中纳米颗粒的聚焦行为,结果表明采用低分子量、剪切变稀效应弱的黏弹性聚合物溶液,可实现更稳定的纳米颗粒聚焦与高效分离。然而,对于外加电场作用下的颗粒迁移,滑移速度作为本控制方法中诱导聚合物变形和升力产生的关键因素,其与聚合物链长等微观参数的耦合作用机制在以往的研究中并未得到详细的数值模拟与实验验证。
聚合物链长作为关键的微观流变参数,显著影响溶液的宏观流变特性及颗粒周围的局部应力分布,进而调控颗粒的滑移速度与升力。其中,一个非常重要但鲜有关注的问题是聚合物链长对颗粒迁移过程—特别是对纳米颗粒迁移的影响。本文采用实验与数值模拟相结合的方法,引入聚合物链长作为调控参数,定量表征不同尺寸颗粒的滑移速度变化及其诱导升力机理。进一步地,本文从理论上探讨电场与非牛顿流体在颗粒迁移过程中的耦合机制,引入聚合物链长作为调控参数,不仅丰富了电场–弹性微流控机制的物理表征,也为构建更符合实际情况的理论模型提供了依据。通过设计不同链长聚合物在滑移–流动联合诱导下的颗粒迁移微流控实验,研究微米及纳米颗粒在不同链长聚合物溶液中存在滑移速度时的迁移行为差异,证实纳米和微米颗粒迁移行为在一定流速范围内随聚合物链长的变化规律,并利用合适链长和质量分数的聚合物溶液,在特定流速范围内实现纳米颗粒的高效聚焦及纳–微米尺度颗粒的高通量分离。
电场–弹性微流控方法是在微流控实验系统的基础上,利用直流电场、流场和非牛顿流体黏弹性联合操控颗粒的方法。本文设计了具有矩形直通道结构的微流控芯片,以一定的入口速度注入具有特定黏弹性的非牛顿流体,同时在微流控芯片电极上施加直流电场,以操控分散在流体内的颗粒。具体而言,实验中通过信号发生器耦合高压放大器施加直流电场,并将电极置于微通道进、出口以形成恒定电场强度。在电场和黏弹性流场的共同作用下,颗粒受到复杂的升力并发生横向迁移。其中,非牛顿流体溶液中的聚合物链长、质量分数以及由于颗粒滑移导致的局部聚合物链变形,直接影响了颗粒所受的聚合物应力、颗粒的迁移与平衡位置。颗粒在不同链长聚合物溶液中的电场–弹性操控示意如图1所示,其中,图1(a)为颗粒在聚合物溶液中电场–弹性微流控示意图,图1(b)为不同链长聚合物示意图,图1(c)为颗粒在聚合物溶液中的滑移速度示意图。
为了系统探讨聚合物链长对纳米颗粒迁移的影响,本文设计了一系列实验,采用不同分子量的聚合物溶液作为工作介质,并在无外加电场和施加电场条件下进行对比机理实验,以探究颗粒在电场–弹性微流控实验中迁移的关键机制。本文所用实验系统的主要设备包括:Olympus公司的IX73显微镜,配套卤素灯光源与汞灯;高速成像采用Phantom的VEO1010L高速摄像机;直流电场由Tektronix的AFG31000信号发生器与Aigtek的ATA–7050高压放大器提供;流体通过微流控注射泵注入芯片入口;实验用水由Elga的Classic DI超纯水仪提供;微流控芯片利用聚二甲基硅氧烷(Poly dimethylsilox-ane, PDMS)通过软光刻法制备而成[30],键合处理通过等离子清洗器完成,并在入口和出口处插入金属空心电极。本研究所使用的主要试剂和材料包括:Thermo Fisher Scientific的100 nm聚苯乙烯微球,以及Huge Biotechnology提供的5和10 µm聚苯乙烯微球;将固体聚氧化乙烯在0.01 mmol/L磷酸盐缓冲液中完全溶解,制备不同质量分数的黏弹性流体。配制过程中,首先让溶液静置使聚氧化乙烯粉末溶解,然后置于摇床上振荡12 h以上,以确保溶液充分均匀。颗粒分散于配制好的聚合物溶液中,加入体积分数为0.1%的Tween 20,以减少颗粒的黏附和聚集。使用配备卤素和汞光源的倒置荧光显微镜观察颗粒迁移,并使用高速摄像机进行图像采集。在卤素光源下,采用亮场成像模式观察微米颗粒的运动;在荧光条件下,使用BrightLine BasicTM单带滤光片(Ex: 559 nm/34 > 90%;Em: 630 nm/69 > 90%;BS: 585 nm)对汞灯光进行过滤,以观察与采集荧光纳米颗粒的运动图像。使用ImageJ软件包对图像进行处理:对时间序列图像进行z-projection堆栈,荧光图像采用“sum slices”选项,亮场图像采用“standard deviation”选项进行处理。
研究中通过调节电场强度、流速以及聚合物链长(600、2000和4000 kDa聚氧化乙烯溶液),实现了对纳米颗粒运动状态的精确控制。其中,未施加电场时的颗粒迁移实验在长度为4.5 cm的矩形微通道中进行,施加电场时的颗粒操控实验在长度为2 cm的矩形微通道中进行。本文中,当直流电场方向与流动方向相同时,记为“+”;当方向相反时,记为“−”。2种通道横截面均为50 µm × 50 µm的正方形。采用流变仪(MCR 302, Anton Paar)在25 ℃下测量不同聚合物溶液的流变特性,实验测得的不同质量分数、不同链长聚合物溶液的剪切黏度见图2。
为了评估PEO溶液在不同质量分数下的弹性,可使用基于毛细管破裂扩展流变学(Capillary Breakup Extension Rheometry, CaBER)测量的经验公式计算溶液的松弛时间$\mathit{\lambda } $[31]:
$ \mathit{\lambda}=18\mathit{\lambda}_{\mathrm{Z}}\left(c/c^{\ast}\right)^{0.65} $
式中:λz为Zimm松弛时间,c为质量分数,$c^{\ast } $为重叠质量分数。
$ {c}^{\ast }=0.77/[\eta ] $
特征黏度[η]用Mark–Houwink关系[32]确定:
$ [\eta]=0.072M_{\mathrm{w}}^{0.65} $
式中:$M_{\mathrm{w}} $为聚合物分子量。$\mathit{\lambda }\mathrm{_Z} $可计算为:
$ \mathit{\lambda}\mathrm{_Z}=\mathit{\text{F}}[\eta]M_{\mathrm{w}}\eta\mathrm{_s}/(N_{\mathrm{A}}k_{\mathrm{B}}T) $
式中:前因子F = 0.463,T为温度,NA是Avogadro数,kB是Boltzmann常数[33],$\eta \mathrm{_s} $为溶剂的黏度。
$ \eta\mathrm{_s}=1\times10^{-3}\ \mathrm{Pa}\cdot\text{s} $
表1为不同质量分数PEO溶液的松弛时间。
滑移速度计算采用格子玻尔兹曼方法(Lattice Boltzmann Method, LBM),并耦合粗粒化分子动力学(Coarse-Grained Molecular Dynamics, CGMD)模拟聚合物链的力学行为。不可压缩流体遵循连续性方程和Navier–Stokes方程,可表述为:
$ \nabla \cdot {\boldsymbol{u}}=0 $
$ \rho \left(\frac{\partial {\boldsymbol{u}}}{\partial t} + {\boldsymbol{u}}\cdot \nabla {\boldsymbol{u}}\right)=\nabla \cdot \left(-p{\boldsymbol{I}} + {{\tau} }_{\upsilon } + {{\tau} }_{{\mathrm{e}}}\right) + {\boldsymbol{F}} $
式中:$\nabla $、u、ρ、p、$\boldsymbol{I} $、$ {{\tau} }_{\upsilon } $、$ {{\tau} }_{{\mathrm{e}}} $分别表示Nabla算子、流体的速度场、密度、压力、单位张量、黏性应力场和弹性应力场,η为流体的动力黏度,t为时间,F为外力项。微通道流动中,通道固体壁面需满足无滑移与不可渗透边界条件。与直接求解Navier–Stokes方程不同,本文采用LBM对流动过程进行模拟[34]。从介观角度来看,黏弹性流体可通过将弹性聚合物链溶解于牛顿流体中获得。采用结合LBM和CGMD的浸入边界法(Immersed Boundary Method, IBM)来模拟黏弹性流体与颗粒的耦合行为[35]。聚合物溶液通过将粗粒化(CG)链浸入牛顿流体中得到。在聚合物链中,每2个相邻珠子通过谐波键连接,势能为k(r – r0)2,其中r为珠子相对距离,k为键强度,r0为平衡键长。每条链由M + 1个珠子组成。当rij(第i和j个珠子的相对距离) < rc(珠子相对距离的截断半径)时,CG珠子间存在弱排斥力$ {\boldsymbol{F}}_{ij}= {a}_{ij}{\boldsymbol{\hat{r}}}_{ij} $,其中${a}_{ij} $为排斥力系数,${\boldsymbol{\hat{r}}}_{ij} $为珠子相对距离方向的单位矢量,以保持系统均匀性。通过IBM将CG珠子和LBM流体耦合,实现颗粒与流体间的无滑移。设定溶剂黏度为1.0 mPa·s,键强度为0.6 nJ,平衡键长为0.4 μm,单链珠子变量为20,阻塞比为0.1,排斥力系数为2.5,数密度为30,弹性数为0.78。为平衡计算效率与物理真实性,采用“珠–簧”模型来表征聚合物链。模拟中设定粗粒化聚合物链的珠子变量M 为主要变量,取值为5、10、15 和20,对应于相应的链长变量N。为了将模拟中的参数与实际物理链长对应,基于以下粗粒化映射逻辑进行表征:PEO单体的分子量约为44 Da,长度约为0.58 nm。对于600 kDa的PEO,其理论轮廓长度约为7.9 μm(600000/44 × 0.58 nm)。本CGMD模拟中,设定相邻珠子间的平衡键长为0.4 μm。当模拟参数取M = 20 时,模拟轮廓长度为20 × 0.4 μm = 8.0 μm,与600 kDa PEO 的实际轮廓长度7.9 μm吻合较好。
采用IBM方法将粗粒化模型与流体流动耦合。IBM确保结构与周围流体保持相同速度,且从粗粒化模型获得的力通过插值传播至邻近的欧拉流体网格,并作为外力项引入LBM。粗粒化模型粒子的运动可利用势函数计算结构的力密度$ {\boldsymbol{F}}({\boldsymbol{X}},t) $,并以如下形式将其作用传递至周围流体网格:
$ {\boldsymbol{f}}({\boldsymbol{x}},t)={\int}_{\varOmega }{{\boldsymbol{F}}}({{\boldsymbol{X}}},t)\delta [{{\boldsymbol{x}}}-{{\boldsymbol{x}}}({{\boldsymbol{X}}},t)]\text{d}\varOmega $
式中:${\boldsymbol{X}} $与${\boldsymbol{x}} $分别为拉格朗日坐标与欧拉坐标,$\delta $与$\varOmega $分别为狄拉克函数与积分区域。结构在移动边界上的速度可同样插值为:
$ {{\boldsymbol{u}}}({{\boldsymbol{X}}},t)={\int}_{\varOmega}{{\boldsymbol{u}}}({{\boldsymbol{x}}},t)\delta [{{\boldsymbol{x}}}-{{\boldsymbol{x}}}({{\boldsymbol{X}}},t)]\text{d}\varOmega $
本文采用4点插值方案。模拟中,管道壁同样被视为固定的浸入式边界。
颗粒带电量为q,在直流电场E下所受电力Fe为:
$ \mathbf{\mathit{\boldsymbol{F}}}\mathrm{_e}=q{{\boldsymbol{E}}} $
颗粒的电泳速度$ \boldsymbol{U}_{\mathrm{ep}} $可写为[21]:
$ \boldsymbol{U}_{\mathrm{ep}}=\mu_{\mathrm{ep}}\boldsymbol{E} $
式中:$ {\mu }_{{\mathrm{ep}}} $为颗粒的电泳迁移率。在满足薄双电层假设的情况下,悬浮于无界介质中的$\mu _{\mathrm{ep}} $可描述为:
$ \mu_{\mathrm{ep}}=\frac{\varepsilon_0\varepsilon_{\mathrm{f}}\zeta}{\eta} $
式中:ε0和εf分别为真空的绝对介电常数和流体的相对介电常数,$\zeta $为Zeta 电位。
颗粒为球形,直径为a,在低雷诺数黏性流体中,球形颗粒所受黏性阻力$ \boldsymbol{F}\mathrm{_D} $为:
$ \boldsymbol{F}\mathrm{_D}=3\pi a\eta K_{\text{d}}\left(\boldsymbol{U}-\boldsymbol{U}_{\mathrm{p}}\right) $
式中:U和Up分别为流体速度和颗粒速度,Kd为修正系数。结合电泳力公式,可得:
$ q\boldsymbol{E}=3\pi a\eta K_{\text{d}}\left(\boldsymbol{U}-\boldsymbol{U}_{\mathrm{p}}\right) $
综上:
$ \mu_{\mathrm{ep}}=\frac{\left(\boldsymbol{U}-\boldsymbol{U}_{\mathrm{p}}\right)}{\boldsymbol{E}}=\frac{q}{3\pi a\eta K_{\text{d}}} $
为研究电场和非牛顿流体流动条件下纳米颗粒黏弹性聚焦的机理,从弹性升力、电场升力和电场–黏弹性3个角度进行了力学实验和分析。在较低流速下,壁面和剪切梯度引起的惯性升力在操控小颗粒时开始失效[13]。
在纯压力驱动的黏弹性流动中,弹性升力占主导地位,其表达式为[36]:
$ {\boldsymbol{F}}_{{\mathrm{eL}}}={C}_{{\mathrm{eL}}}{a}^{3}\nabla {N}_{1} $
式中:CeL为无量纲弹性升力系数,N1为第1个法向应力差($ N_1=\tau_{11}-\tau_{22} $为沿流体流线产生额外张力,$\tau_{11} $、$\tau_{22} $分别为流动方向和速度梯度方向的法向应力)。黏弹性流体流动时,$ N_1 $产生的升力将悬浮颗粒导向剪切速率较小的区域。$ N_1 $在正方形通道的中心及4个角处最小。Oldroyd–B模型具有与剪切速率无关的剪切黏度和法向应力系数,能准确描述Boger流体[37],使流体黏弹性研究不受剪切变稀的影响。采用Oldroyd–B模型作为本构方程计算$ N_1 $:
$ N_1=2\eta_{\mathrm{p}}\lambda\dot{\gamma}^2 $
式中:ηp为聚合物黏度,$ \dot{\gamma } $为剪切速率。Weissenberg数Wi用于表征黏弹性,定义为:
$ W\mathrm{_i}=\mathit{\lambda}\dot{\gamma}=\mathit{\lambda}\frac{2\overline{U}}{W}=\frac{2\mathit{\lambda}Q}{W^2H} $
式中:$ \overline{U} $为平均流速, Q为流量,W和H分别为通道的宽度和高度。弹性升力FeL与$ N_1 $成正比,并随颗粒尺寸变化。因此,作用在纳米颗粒上的弹性升力随尺寸减小而急剧减小,导致仅靠压力驱动流动无法聚焦纳米颗粒。
在纯电场驱动的流动中,电场导致的升力占主导地位。颗粒的电泳速度如式(11)所示,作用在液体上的电场力为[21]:
$ {\boldsymbol{F}}_{{\mathrm{EOF}}}=-{\varepsilon }_{0}{\varepsilon }_{{\mathrm{f}}}({\nabla }^{2}\phi )\boldsymbol{E} $
式中:$ \phi $为流体中的电势。Maxwell应力M定义为[1, 38]:
$ \boldsymbol{M}=\nabla \phi \nabla \phi -\frac{1}{2}(\nabla \phi \cdot \nabla \phi )\boldsymbol{I} $
该应力由颗粒周围静电势分布的横向不对称引起,而该不对称性源于壁面的存在。
在直矩形微通道中,电场与黏弹性流场共同驱动下,滑移速度诱导的局部弹性应力Fsl在非均匀剪切流场中对颗粒迁移起到重要的作用。该应力由颗粒表面周围聚合物的不对称应变引起,而不对称应变源于颗粒电泳运动产生的滑移速度。即在压力驱动流引起的非均匀剪切速率场中,电场的加入引发颗粒滑移,这种耦合产生了很高的升力。在非均匀剪切速率场中,滑移速度引起的局部聚合物弹性应力不对称是导致纳米颗粒聚焦的主要因素。Li等[25]提出了黏弹性剪切流与颗粒电泳额外升力的非线性耦合公式:
$ {\boldsymbol{F}}_{{\mathrm{sl}}}={C}_{{\mathrm{sl}}}3\pi {\eta }_{{\mathrm{p}}}a\lambda \left(\frac{\partial U}{\partial y}{{\boldsymbol{j}}} + \frac{\partial U}{\partial z}{{\boldsymbol{k}}}\right){U}_{{\mathrm{s}}} $
式中:Csl为无量纲系数,Us为颗粒滑移速度, $ {\boldsymbol{j}} $和$ {\boldsymbol{k}} $分别为y和z方向上的单位矢量。
上述升力与作用在颗粒上的黏性阻力相平衡,黏性阻力表达式见式(13)。
假设电场施加的力${\boldsymbol{F}}_{{\mathrm{p}}} $与黏性阻力达到平衡,即$ {\boldsymbol{F}}_{{\mathrm{p}}}=-{\boldsymbol{F}}_{{\mathrm{D}}}=3\pi a\eta {K}_{\text{d}}{{\boldsymbol{U}}}_{{\mathrm{s}}}=6\pi R\eta {K}_{\text{d}}{{\boldsymbol{U}}}_{{\mathrm{s}}} $(其中R为颗粒半径),此时颗粒稳定运动。因此,Fp/R与滑移速度$ {{\boldsymbol{U}}}_{{\mathrm{s}}} $存在一定映射关系。本文对施加于颗粒上的力Fp与颗粒半径之比Fp/R与颗粒在特定链长聚合物溶液(黏弹性流体)中滑移速度的关系进行了数值模拟。图3为不同尺寸颗粒在链长N = 20条件下的滑移速度数值模拟结果,分别计算了半径R = 2.50、3.75、5.00及7.50 µm这4种工况下颗粒滑移速度与$ {{\boldsymbol{F}}}_{{\mathrm{p}}} $/R的关系。每种工况下,$ {{\boldsymbol{U}}}_{{\mathrm{s}}} $均与$ {{\boldsymbol{F}}}_{{\mathrm{p}}} $/R呈近似线性关系,随施加在颗粒上的力Fp增加,滑移速度不断提高。滑移速度Us与颗粒受力比值Fp/R呈近似线性相关,且斜率受聚合物链长N调制,随N增加,流体微观阻力增大,导致相同驱动力下的$ {{\boldsymbol{U}}}_{{\mathrm{s}}} $减小。模拟结果证实,在相同Fp/R下,颗粒尺寸对滑移速度的影响较小,这意味着滑移诱导升力Fsl与颗粒直径a近似成正比(据式(21)),而弹性升力FeL与a3成正比。这是纳米颗粒操控机制发生转变的力学本质。
根据弹性升力计算公式[26]:
$ \begin{split}& {\boldsymbol{F}}_{{\mathrm{eL}}}=2{C}_{{\mathrm{eL}}}{a}^{3}{\eta }_{{\mathrm{p}}}\lambda \nabla {{\dot{{\gamma} }}}^{2}=4{C}_{{\mathrm{eL}}}{a}^{3}{\eta }_{{\mathrm{p}}}\lambda ({\dot{{\gamma} }}\cdot \nabla {\dot{{\gamma} }})= \\&\qquad 4{C}_{{\mathrm{eL}}}{a}^{3}{\eta }_{{\mathrm{p}}}{W_\mathrm{i}}\frac{{\dot{{\gamma} }}\cdot \nabla {\dot{{\gamma} }}}{\overline{\dot{\gamma }}} \end{split} $
另外,根据滑移速度诱导的升力计算公式:
$ {\boldsymbol{F}}_{{\mathrm{sl}}}=3{C}_{{\mathrm{sl}}}\pi {\eta }_{{\mathrm{p}}}a\lambda {\dot{{\gamma} }}{U}_{\mathrm{s}}=3{C}_{{\mathrm{sl}}}\pi {\eta }_{{\mathrm{p}}}a{W_\mathrm{i}}\frac{\dot{{\gamma} }}{\overline{\dot{\gamma }}}{U}_{\mathrm{s}} $
两者之比为:
$ \frac{\left| {\boldsymbol{F}}_{{\mathrm{eL}}}\right| }{\left| {\boldsymbol{F}}_{{\mathrm{sl}}}\right| }=\frac{4{C}_{{\mathrm{eL}}}{a}^{2}|{\dot{{\gamma} }}\cdot \nabla {\dot{{\gamma} }}|}{3{C}_{{\mathrm{sl}}}\pi \left| {\dot{{\gamma} }}{U}_{\mathrm{s}}\right| } $
由式可知,随颗粒尺寸减小,弹性升力的衰减程度高于滑移速度诱导的升力。图4(a)展示了不同尺寸颗粒在低电场强度下的受力分析示意图,其中Fw为壁面诱导电升力。特征剪切速率可估算为$ \overline{\dot{\gamma}}=2 \overline {\boldsymbol{U}}/W $,剪切速率梯度通过$ \nabla\overline{\dot{\gamma}}\sim2\overline{\dot{\gamma}}/W= 4 \overline{\boldsymbol{U}}/W^2 $计算。在流体平均速度$ \overline{U} $ = 0.1 m/s,λ = 1.76 ms,ηp = 6 mPa·s,μep = −1.21 × 10−8 m2/(V·s) [26],电场强度50 V/cm条件下,对流动诱导的弹性升力和滑移速度诱导的升力进行求解和对比。取弹性升力系数CeL = 0.009[26],滑移诱导升力系数Csl = 0.5[26],根据升力计算式所得结果如图4(b)所示。据此关系,调节电场强度时,弹性升力与滑移速度诱导的升力变化在不同尺寸颗粒间不同步,适当调节可实现大尺寸与小尺寸颗粒的分离。
电场–弹性微流控方法控制颗粒迁移过程中,聚合物链尺度微观参数是决定黏弹性流变行为和颗粒宏观动力学的关键。图5计算了N = 5、10、15和20这4种链长聚合物黏弹性溶液中R = 2.50 μm颗粒的滑移速度。结果表明,每种工况下Us均与Fp/R呈近似线性关系,且随着聚合物链长的增加,相同Fp/R条件下,滑移速度Us不断减小。
首先,通过黏弹性微流控方法研究了微米及纳米颗粒在不同链长聚合物溶液中、无滑移速度条件下的迁移行为。该实验在尺寸为4.5 cm × 50 µm × 50 µm的直微通道中进行,以PEO溶液为工作流体,通过改变聚合物链长和流速,观察颗粒在不同黏弹性环境中的横向迁移与聚焦特性。图6展示了不同分子量(PEO质量分数均为0.2%)下,粒径为5 µm的颗粒在无滑移速度时的迁移行为差异。从图中可以看出,当链长较低(600 kDa)时,5 μm颗粒在低流速下一部分聚焦于通道中心位置,另一部分沿横向迁移至通道壁。这是因为在黏弹性流动条件下,通道中心部分和壁角位置处的弹性力最小。随着流动速度增加,颗粒的惯性效应愈发明显;在惯性造成的扰动下,壁角部分的颗粒迁移至通道中心,在5~20 cm/s的流速范围内,颗粒在通道中心汇聚成一条线。随着流速继续增加,惯性升力与流动导致的弹性升力相互竞争,颗粒聚焦为2条线,在这2个位置处颗粒所受的升力达到平衡。当聚合物链长增加时,5 μm颗粒在较低流速下即发生有效聚焦,这是因为相同质量分数的长链聚合物溶液具有更高的弹性;但随着流速继续提升,更显著的剪切变稀效应反而减弱了颗粒的聚焦效果。
纳米颗粒因尺寸较小,黏弹性流动导致的弹性与惯性作用均急剧减小。纳米颗粒在无滑移速度条件下、不同分子量(PEO质量分数均为0.2%)溶液中的实验结果如图7所示。从图中可以看出,仅靠纯流动导致的惯性升力与弹性升力无法使纳米颗粒发生聚焦,在3种链长的PEO溶液中均是如此。这是因为弹性升力和惯性升力随颗粒尺寸减小均急剧下降,而滑移速度诱导的升力虽有所下降,但下降速率较慢。因此,在小尺寸纳米颗粒的迁移过程中,滑移速度诱导的升力占主导。未施加外加电场时,颗粒无滑移速度,仅靠在非均匀剪切的黏弹性流场中无法对纳米尺度颗粒进行有效聚焦。实验表明,纳米尺度颗粒在3种链长的聚合物溶液中均未发生可见的横向迁移与聚焦。
这一对比结果表明,在纳米尺度下,颗粒迁移机制与微米尺度显著不同:惯性主导与弹性主导的聚焦机制已不再适用,滑移速度诱导的升力成为实现颗粒可控迁移的关键因素。因此,若要在纳米尺度下实现颗粒聚焦与分离,需引入额外的驱动力(如电场诱导滑移速度等),为小尺寸纳米颗粒提供有效的升力。
纳米颗粒在外加电场下的电场–弹性联合操控实验结果如图8所示,该实验在尺寸为2 cm × 50 µm × 50 µm的直微通道中进行,施加的直流电场强度为−800 V/cm。图中利用荧光强度分布的归一化曲线及半峰全宽(Full Width at Half Maxima, FWHM)量化表征聚焦效果。由图可见,施加电场后纳米颗粒获得了更好的聚焦效果。在低流速时,链长较长的PEO溶液因弹性效应更强,促进了纳米颗粒聚焦,产生了较好的聚焦效果。随着流速增加,长链PEO溶液中纳米颗粒的聚焦效果变差;在高速流动条件下,低链长PEO溶液表现出更稳定的聚焦特性,这主要归因于其较弱的剪切变稀效应且能维持足够的有效弹性。纳米颗粒所受流动导致的惯性升力和弹性升力并不明显;施加外加电场后,颗粒相对周围黏弹性流体产生滑移速度,该滑移速度导致的局部聚合物应力显著提升了纳米颗粒的横向迁移速率,使其获得了较好的聚焦效果,如图8所示。因此,滑移速度导致的聚合物应力是纳米颗粒横向迁移的主导升力。长链PEO溶液虽能提高弹性力,但其黏度高且剪切变稀效应明显,高黏度削弱了颗粒的滑移速度。在高流速下,颗粒在低链长PEO溶液中具有更高的滑移速度和较弱的剪切变稀效应,且低链长PEO溶液也能够维持足够的弹性,使纳米颗粒在宽流速范围内产生较好的聚焦效果。
微米颗粒在电场–黏弹性微流控实验中受流动导致的弹性升力和滑移导致的聚合物应力共同影响,这2种升力的竞争和协同效应可使微米颗粒产生不同的横向迁移。为使溶液具备足够的流动诱导弹性升力,并探究其在不同链长PEO溶液中与滑移速度诱导聚合物应力之间的竞争关系,本研究采用质量分数为0.6%的PEO溶液作为工作流体,该实验在尺寸为2 cm × 50 µm × 50 µm的直微通道中进行。在600 kDa的低链长PEO溶液中,5 μm颗粒在低速(1 cm/s)时一部分聚焦于通道中心位置,另一部分迁移至通道壁;高速下所有颗粒聚焦于通道中心,如图9(a)所示。在施加与流动方向相同的直流电场时,颗粒在滑移速度导致的聚合物应力作用下发生横向迁移:低速(1 cm/s)时仅需150 V/cm的电场强度即可使颗粒全部克服弹性升力并迁移至通道壁面。但随着流动速度增加,需要更高的电场强度才能使颗粒全部迁移至通道壁面。作为对比,在链长较高的实验中(图9(b)),所有颗粒均未发生较好聚焦。即使施加较高的电场强度(500 V/cm),颗粒也未能明显迁移至通道壁面。这表明,高链长、高质量分数PEO溶液的强烈剪切变稀效应会导致一定流速下对5 μm颗粒的操控失效。而在低链长PEO溶液中,由于流动诱导的惯性升力、弹性升力以及滑移速度诱导的聚合物应力三者的竞争与协同作用,微米颗粒在矩形通道中产生了更多的平衡位置,这种效应为微米颗粒的聚焦与分离创造了良好条件。
图8实验证明,低流速时长链PEO溶液具有较好的聚焦效果,而高流速时低链长聚合物溶液的聚焦效果更优。因此,可通过混合不同链长的PEO溶液,使其在特定流速下达到最佳聚焦效果。质量分数为0.6%的PEO混合溶液(600与4000 kDa链长的PEO质量比m600 kDa∶m4000 kDa = 5∶1)纳米颗粒在−800 V/cm的电场–弹性聚焦实验结果如图10所示。由图可见,混合溶液在低速和高速区域的聚焦效果均介于低链长与高链长PEO溶液之间,而在中间流速区域,混合溶液呈现出了较好的聚焦效果。因此,通过混合不同链长的PEO溶液,可在合适的流速下实现较好的聚焦效果。
微米级大颗粒在PEO溶液中受流动诱导的惯性升力、弹性升力及滑移速度导致的聚合物应力共同影响;而纳米颗粒仅滑移速度导致的聚合物应力能使其在50 μm × 50 μm的矩形通道中发生明显的横向迁移。利用该特性,可通过电场–弹性微流控方法实现10 μm颗粒与100 nm颗粒的高通量分离。图11展示了在50 V/cm电场强度条件下,100 nm颗粒与10 μm颗粒在分子量为600 kDa、质量分数为0.6%的PEO溶液中的高通量分离实验结果。在一定速度条件下,10 μm颗粒聚焦于通道中心,且低正电场强度下的低滑移速度诱导升力不足以使其迁移至壁面;而流动诱导的弹性升力随颗粒尺寸急剧降低,100 nm颗粒所受流动诱导的弹性升力不明显,在滑移诱导升力主导下聚集于通道两侧,从而实现了100 nm颗粒与10 μm颗粒的高通量分离。
本文系统阐明了关键微观流变学参数—聚合物链长在黏弹性流场中对滑移颗粒(尤其是纳米尺度颗粒)迁移行为的影响,揭示了聚合物链长对颗粒滑移速度及升力平衡的调控规律。通过实验证实了聚合物链长调控在提升流体弹性和颗粒聚焦方面的关键作用,并通过理论分析揭示了电场–弹性耦合作用下滑移颗粒的横向迁移机制。当颗粒尺寸减小时,流动诱导弹性升力的衰减速度快于滑移诱导升力,证实在纳米尺度下滑移诱导升力取代弹性升力成为颗粒迁移的主导升力。基于该规律,通过合理优化聚合物链长与质量分数,实现了特定流速条件下纳米颗粒的高效聚焦及微纳尺度颗粒的高通量连续分离。本研究揭示了聚合物链长及滑移速度等参数的微观调控对颗粒宏观动力学行为的影响机制,为电场–弹性协同驱动的微流控分选技术提供了新的理论依据与设计思路。这种多尺度、多因素耦合的研究方法,有助于揭示电场、流体力学与聚合物物理之间的复杂关系,从而推动纳米颗粒操控技术的理论发展与实验应用。电场–流体弹性协同驱动方法及聚合物应力的分析与调控,为不同应用场景下的系统参数优化提供了新的变量和调控策略,使得该技术在面对复杂颗粒体系时,能够根据需要定制参数,以应用于高通量分选。

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doi: 10.11729/syltlx20250126
  • 接收时间:2025-12-31
  • 首发时间:2026-10-22
  • 出版时间:2026-08-25
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  • 收稿日期:2025-12-31
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  • 录用日期:2026-03-05
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    浙江大学 工程力学系 流体动力与机电系统国家重点实验室,杭州 310027

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https://castjournals.cast.org.cn/joweb/syltlx/CN/10.11729/syltlx20250126
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2种不同金属材料的力学参数
科
Family
属数
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
species (%)
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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