飞秒激光微纳制造水下气体浸润性表面 下载: 1833次特邀综述
1 引言
浸润现象在自然界中起着非常重要的作用,受到学术界的广泛关注[1-10]。随着科学技术的不断发展,各种研究的不断深入,固/液二相界面间的浸润现象已不再满足各国科学家的研究需求,气/固/液三相界面间的浸润现象亟需探索[11-16]。作为气/固/液三相界面的典型代表之一,水下气体浸润性界面的研究进入了人们的视野并获得了广泛的关注,这主要由于其在许多领域具有潜在的研究价值与广阔的实际应用前景,如电催化[17-19]、细胞工程[20-22]、减阻[23-25]、气体运输[26-27]等。近年来,关于水下气体浸润性界面的研究已成为了学术界的一个研究热点。研究表明,这种浸润现象的产生受固体材料表面的化学成分与微观几何形貌的共同作用所致[28-30]。基于浸润性原理,人们采用不同的方法制备了各种各样的水下气体浸润性界面[31-33]。然而,这些方法普遍存在一定的局限性,如制备工艺复杂、制造周期长或污染环境等。更重要的是这些方法难以对材料表面进行精细化的加工,与当前的精确调控水下气体浸润性界面的研究趋势相矛盾[34-36]。
飞秒激光加工作为一种全新的非接触式制造手段,具有简单快捷、精确可控、材料适用性广和环境友好等优势,是当前具有很大潜力的一种表面微纳结构的制备技术[37-43]。近年来,利用飞秒激光能够精密调控表面微小结构的特性,人们成功地将飞秒激光微纳加工技术用于调控材料表面的浸润性,并受到学术界的广泛关注。随着研究的不断进展,飞秒激光微纳加工调控界面浸润性的技术逐渐完善,从最初的加工材料单一扩展到适用于各种材料的处理,从功能应用单一发展到具有多功能应用。飞秒激光微纳加工技术发展迅猛,逐渐成为构建浸润性界面材料的重要技术手段之一[44-51]。
本文系统总结了近年来利用飞秒激光微纳加工技术制备水下气体浸润性界面的相关研究。以水下气体浸润性模型与飞秒激光微纳加工技术的介绍作为研究背景,从水下超疏气表面、水下超亲气表面、水下超疏气-超亲气转换以及水下气体运输四个方面进行了系统的归纳概述。最后结合当前的研究现状对该领域所面临的挑战与前景进行总结与展望。
2 研究背景
2.1 水下气体浸润性模型
在理想情况下,即固体表面完全平滑时,其在水下对气泡的浸润性与在空气中对水滴的浸润性具有很大的相关性[52] ,如
式中:θw是水接触角;γSV,γSL和γLV分别是固/气界面、固/水界面和水/气界面的表面自由能。由此可知,理想状态下的水接触角受三相界面间的表面自由能的共同影响。而水下气泡在固体表面的浸润性可以类比为一种特殊的空气环境中水滴的浸润性,因此其处于平衡时的气泡接触角(θb)同样可由Young式方程推导得出,即
结合以上两个公式可得
根据(3)式,推断出理想情况下气泡在水中于平滑固体表面的接触角与水滴在空气中于相同基底上的接触角的相关性:两者大小互补(实际情况中会有偏差)。固体表面的静态浸润性可根据其对水滴/气泡接触角的不同分为以下几种情况:当接触角大于90°时为疏水/气性,小于90°时为亲水/气性;在极端情况下,接触角大于150°时为超疏水/气性,接触角小于10°时为超亲水/气性。因此,理想情况下,亲水界面在水中表现出疏气性,而疏水界面在水中表现出亲气性。
非理想状态下,即固体表面具有微小的粗糙结构时,将具有超疏水性的材料浸入水中,水分子无法填充其表面的微纳结构,其表面剩余的空气会形成一层气膜[54-55]。当气泡在水中与超疏水材料表面接触时,能够轻易地被气膜吸收,与表面完全结合,对外表现出超亲气性[56-59],如
然而,实际情况中,有时根据水滴在固体表面的浸润情况无法准确判断出相应气泡的浸润性。该现象的产生原因是接触角滞后。以水中气泡为例,所谓接触角滞后,就是当固体基底倾斜一个特定的角度时,气泡达到最小(θmin)和最大(θmax)静态接触角时的余弦之差,如
图 1. 固体基质在空气和水中的浸润性关系。(a)空气中水接触角(θw)和水中气泡接触角(θb)的示意图;(b)超疏水/超亲气表面;(c)超亲水/超疏气表面
Fig. 1. Relationship between wettability of solid substrates in air and water. (a) Schematic of water contact angle (θw) in air and the bubble contact angle (θb) in water; (b) superhydrophobic/superaerophilic surface; (c) superhydrophilic/superaerophobic surface
图 2. 最大和最小水下气泡静态接触角示意图
Fig. 2. Schematic diagram of maximum (θmax) and minimum (θmin) static underwater bubble contact angles
水下超疏气的,与之相反,具有较小气泡接触角(小于10°)与较大接触角滞后的表面通常具有水下超亲气性[61]。
2.2 飞秒激光微纳加工
随着科学技术的不断发展,人们对精密器件的需求量不断增大,同时其加工精度指标也在不断提升。面对这些严峻挑战,传统的微纳加工技术逐渐难以满足新时代的需求,寻求新的微纳加工方式成为必然的选择。经过科学家们的不断探索,飞秒激光以其极高的能量峰值、超短脉冲宽度、超高的聚焦力等特点在微纳制造领域中展现出极高的潜力,成为当前微纳加工领域有力工具之一[62-63]。作为一种先进的微纳制造手段,飞秒激光微纳加工技术不仅仅被用于制造精密器件,还因其物理加工的特点能够与各种领域相结合,直接或间接带动各方面的研究步入超微超快领域,充分展现出其旺盛的“活力”。
飞秒激光微纳加工系统当前主要分为两种,都包括飞秒激光器、光路系统、三维移动平台三个组成部分。其中飞秒激光器用于产生飞秒脉冲激光;光路系统由反射镜、透镜、光闸等光学器件组成,用于调控激光路线与激光出射的角度等;而三维移动平台则用于样品的固定以及位置的调整。其中一种加工系统为激光进入扫描振镜系统,由相应控制程序设定激光加工的路径以及速度等参数,从而将光束聚焦到三维移动平台上的样品表面进行加工。而另一种是通过透镜或物镜将激光束聚焦到三维移动平台上的样品表面,再通过控制器驱动平台移动进行扫描加工,加工过程利用CCD进行实时监控[51]。
近几年来,研究者们成功地将飞秒激光微纳制造技术应用于水下气体浸润性界面的调控[64-66]。利用飞秒激光的高功率、超短脉冲等特点,只需直接扫描烧蚀材料便可在其表面精确地构建出各种不同的微纳图案,而不会像普通激光烧蚀一般出现无规则的表面形貌。又因为表面浸润性的产生受固体材料表面的化学成分与微观几何形貌的共同作用,这些通过飞秒激光构建的微小图案能够使材料表面展现出不同的水下气体浸润性。同时,飞秒激光微纳加工的适用范围相当广泛,包括金属、纺织物、塑料、有机物在内的众多材料均可通过飞秒激光烧蚀改变其表面浸润性[67-69]。相较于某些局限于特定材料的加工方式,其在浸润性调控方面具有更大的应用价值。因此,研究通过飞秒激光微纳制造技术调控水下气体浸润性界面具有重要意义。
3 水下气体浸润性表面
3.1 水下超疏气表面
气体无处不在,它以空气的形式存在于人们生活的环境中,是人类生存不可缺少的一部分。在水中,它以气泡的状态存在,使水下的世界更加绚丽多彩[70-72]。然而,在某些情况下,水中气泡的存在也会产生负面影响[73-74]。例如:在输送液体的管道中,气泡的存在会腐蚀管道,降低设备的使用寿命,造成不必要的财产损失;潜水时,潜水镜上的气泡会阻碍视线,增加潜水员在水底的危险系数;做化学实验时,气泡的产生会影响实验,尤其是固体材料间的反应,气泡的堆积会严重影响反应速率。因此,研究者们为解决水下气泡附着固体表面的问题付出许多努力。其中,通过飞秒激光制备具有水下超疏气性的表面便是热门的研究方向之一[75-77]。
为制备水下气泡低黏附的材料,基于飞秒激光加工的方法,Yang等[75]以铜为基底在其表面烧蚀形成了一层微/纳米级的复合结构。飞秒激光加工后,所制备的粗糙表面具有三维周期性的条纹结构,内部包含大量随机排列的纳米结构,影响了该金属表面的水下气泡浸润性。对加工后铜样品的浸润性能进行测试,发现其表面具备良好的水下超疏气性。作为浸润性的重要参数,加工前后铜片表面的水下气泡接触角发生了较大变化:加工前铜片在水中对气泡的接触角约为120°,气泡依附在铜片表面呈半球状;加工后气泡的接触角提高至159°,气泡在样品表面能够近似维持球形。在水下将气泡与经飞秒激光处理的铜片表面轻轻接触再离开的整个过程中,气泡并未附着铜片且很容易分离,这表明激光处理后的铜片表面对气泡的黏附性很低。由此可知,通过飞秒激光直接扫描制备的微纳复合铜片表面具有良好的水下抗气泡的能力。
相比于纯金属材料,合金材料在实际生活中具有更广泛的应用。Jiao等[76]通过飞秒激光烧蚀的方法在铝合金薄片表面加工出粗糙的沟槽结构。加工后的表面有规律地分布着微小的凹槽,而在其上还附着了一些微纳米级别的颗粒。飞秒激光诱导出粗糙结构后,铝合金表面的水下抗气泡能力增强:加工前其水下气泡接触角为111°,表现为水下疏气性,如
图 3. 飞秒激光制备的水下超疏气表面。(a)(b)铝合金表面[76];(c)~(f)硅表面[77]
Fig. 3. Different underwater superaerophobic surfaces fabricated by femtosecond laser. (a)(b) Aluminium alloy surface[76];(c)-(f) silicon surface[77]
图 4. 飞秒激光制备水下超亲气表面。(a)~(c) PDMS表面[77];(d)~(h)铝表面及相应浮力装置[82];(i)(j) PTFE表面[83]
Fig. 4. Different underwater superaerophilic surfaces fabricated by femtosecond laser. (a)-(c) PDMS surface[77]; (d)-(h) aluminum surface and corresponding buoyancy device[82]; (i)(j) PTFE surface[83]
同样是制备水下超疏气材料,Yong等[77]使用本身便具有水下疏气性的硅材料作为基底。为加强硅的水下疏气能力,通过飞秒激光一步直接扫描的方案在其表面烧蚀出分层的微观结构,成功将其浸润性进一步极化,制备出具有水下超疏气性的粗糙界面。如
3.2 水下超亲气表面
为解决水下气泡引发的各类问题,除制备能够防止水下气泡附着的表面外,主动收集水中的气泡也是解决问题的一种有效手段[78-81]。研究表明,水下超亲气材料能够有效地吸附并聚集水中的气泡,达到清除以及利用水中气泡的效果,是当前研究的热点之一。Yong等[77]通过飞秒激光微纳加工技术,在聚二甲基硅氧烷(PDMS)表面烧蚀出微纳米级别的粗糙结构,如
与之类似,为了制备出具有水下超亲气性的表面,Zhan等[82]以铝作为基底,通过调整飞秒激光加工参数调控铝片表面的微观形貌,令其表面变得粗糙,如
基于飞秒激光微纳加工的方式,Hu等[83]在PTFE表面进行烧蚀以进一步提高其粗糙度,使其成为水下超亲气表面。加工后的超亲气表面被微/纳米级的层次结构所覆盖,具有较高的粗糙度,与未加工的光滑表面形成明显对比。对激光烧蚀前后表面的水下气泡接触角进行测量,加工前水下气泡接触角为78°,气泡在其表面呈半球形,如
无论是水下超疏气或是水下超亲气的界面材料,均可通过飞秒激光微纳制造技术调控相应材料的表面微观结构得到,由此展现了该技术在制造不同水下气体浸润性界面领域的潜力。
3.3 水下超疏气-超亲气转换
水下超疏气与水下超亲气材料均具有广泛的实用性,因而受到了国内外许多研究人员的关注[84-86]。同时,近年来能够实现可切换浸润性的表面,因其应用方便,功能多样,适用性广等特点吸引了众多的目光。因此,能够可逆地转换水下超疏气与超亲气状态的材料或方法便成了水下气泡浸润性界面领域的研究热点之一。能够实现可切换浸润性的材料或方案通常是依靠不同的外部刺激或直接的物理化学处理所获得,如温度、湿度、光线、pH值、真空、等离子体处理、电势和磁场等[87-95]。基于以上观点,研究者们在水下超疏气-超亲气转换领域取得了众多的成果[96-100]。
聚四氟乙烯(PTFE)是一种化学物理性质极其稳定的材料,传统的加工方法难以精确调控其表面的微观结构,因而想要改变PTFE表面的浸润性便成为一个较为困难的任务[51]。然而,飞秒激光可以轻易地在PTFE表面烧蚀出微纳米级的精密图案,从而影响其表面浸润性。基于飞秒激光微纳加工技术,Huo等[96]在PTFE表面构建出微纳米级别的微观结构,表现为大量微小凸起与孔隙形成的类珊瑚丛状形貌,获得粗糙的水下超亲气PTFE表面,如
图 5. 飞秒激光制备的可切换水下超亲/疏气PTFE表面[96]。(a)(b)表面微观结构;(c)(d)水下超亲气与超疏气的可逆转换
Fig. 5. Switchable underwater superaerophilic/superaerophobic PTFE surfaces fabricated by femtosecond laser[96]. (a)(b) Surface microstructure; (c)(d) reversible switching between underwater superaerophilicity and superaerophobicity
与PTFE类似,同为聚合物的聚二甲基硅氧烷(PDMS)表面亦可实现水下气泡浸润性的可逆转换。Yong等[97]首先通过飞秒激光一步直接扫描处理获得了具有水下超亲气性的PDMS表面。激光烧蚀后,获得的粗糙PDMS表面随机分布着许多微纳米级别的爆米花状凸起,凸起的直径范围在400 nm~1.6 μm之间,同时每个凸起的表面还进一步覆盖了大量的纳米级颗粒,直径仅为60~140 nm,如
图 6. 飞秒激光制备的可切换水下超亲/疏气PDMS表面[97]。(a)~(c)表面微观结构;(d)~(g)水下超亲气与超疏气之间的转换
Fig. 6. Switchable underwater superaerophilic/superaerophobic PDMS surface fabricated by femtosecond laser[97].(a)-(c) Surface microstructure; (d)-(g) switching between underwater superaerophilicity and superaerophobicity
图 7. 飞秒激光制备的可切换水下超亲/疏气钛表面。(a)~(d) Jiao等[98]制备的样品;(e)~(i) Jiao等[99]制备的样品
Fig. 7. Switchable underwater superaerophilic/superaerophobic titanium surface fabricated by femtosecond laser.(a)-(d) Sample treated by Jiao et al.[98]; (e)-(i) sample fabricated by Jiao et al.[99]
除PTFE与PDMS两种聚合物材料之外,金属钛在水下气泡浸润性可逆转换方面同样有一定的研究进展。Jiao等[98]采用飞秒激光垂直交叉扫描的方式在钛表面加工出粗糙微观结构。如
基于非原位调控水下气泡浸润性的局限性,如复杂的转换过程、较长的转换时间以及额外的设备使用等,Jiao等[99]提出了一种通过控制水溶液中乙醇的含量来实现原位可调气泡浸润性的简单方案。以钛作为加工材料,利用飞秒激光烧蚀的方法,在其表面制备出以TiO2为主的城堡状微纳结构,如
虽然目前已经制备出大量可切换的浸润性表面,涉及各种材料各种特殊方法,但这些表面大部分都是依靠其基底的性质来实现浸润性的可逆切换,即功能的实现受限于材料。为解决该问题,Yong等[100]提出一种能够可逆转化众多材料表面水下气泡浸润性的策略。飞秒激光微纳加工是调控水下气泡浸润性的重要手段。包括铝、不锈钢、铜、镍、PTFE、PDMS在内的一系列材料,经过飞秒激光扫描处理形成表面微纳结构后,都在水中表现出超亲气/亲气性,在空气中表现出超疏水性,而该转换方案便是以此种材料为基础来实现的。以铝为例,飞秒激光在其表面诱导出微纳结构后,将其浸入水中,气泡与粗糙铝表面接触时迅速扩散,表现出水下超亲气性,相应地样品表面在空气中表现为超疏水性。若预先用乙醇溶液将铝表面润湿,再浸入水中,其表面则表现出水下超疏气性,水下气泡浸润状态发生完全相反的转换,而恢复样品表面的水下超亲气性也十分简单,只需将其进行干燥即可,如
图 8. 在飞秒激光处理过的铝表面进行水下超亲气和超疏气间的可逆切换[100]
Fig. 8. Reversible switching between underwater superaerophilicity and superaerophobicity on the femtosecond laser treated aluminum surface[100]
图 9. 飞秒激光制备的具有形状梯度的水下超亲气PTFE表面。(a)~(d) Yin等[104]制备的样品;(e)~(h) Duan等[105]制备的样品
Fig. 9. Underwater superaerophilic PTFE surfaces with shape gradient fabricated by femtosecond laser. (a)-(d) Sample treated by Yin et al.[104]; (e)-(h) sample treated by Duan et al.[105]
3.3 水下气体运输
水下气体在自然界中普遍存在,对人们的生活造成许多或积极或消极的影响,是工业生产与日常生活中的重要元素。为了能够对其进行有效利用,关于水下气体运输的研究获得了学术界的广泛关注,取得了重要进展[101-103]。其中,通过具有水下特殊浸润性的界面操控水下气泡行为,是研究水下气体运输的一个重要方案,吸引了众多研究者的目光[104-108]。
基于飞秒激光加工技术,Yin等[104]使用飞秒激光将矩形的PTFE片切割成梯形,再经过飞秒激光逐行直接扫描,获得表面粗糙的梯形PTFE样品,如
利用具有形状梯度的水下超亲气表面的拉普拉斯压力是实现水下气体运输的有效手段之一,除此之外,具有非对称浸润性的表面同样能够实现水下气体的定向运输。Yin等[106]通过飞秒激光直接扫描技术,在PTFE网膜表面的一侧加工出粗糙的微纳结构,使其两侧具有不同的表面微观形貌,成功获得具有非对称上下表面的样品,如
图 10. 飞秒激光制备的具有水下非对称浸润性PTFE表面[106]。(a)激光烧蚀过程示意图;(b)(c)表面微观结构;(d)(e)两侧的水下气泡接触角
Fig. 10. PTFE surfaces with underwater asymmetric wettability fabricated by femtosecond laser[106]. (a) Schematic of the laser ablation process; (b)(c) surface microstructure; (d)(e) underwater bubble contact angle on both sides
同样是利用表面的非对称性,Yan等[107]以铝作为加工材料,经过飞秒激光钻孔、表面氟化和氟化去除操作,制备出一种能够单向运输水下气体的Janus铝膜,如
通常被认知的气泡运输都发生在水下,即气泡在竖直方向运输,目前的研究大部分都是如此,而关于气泡在水平面上运输行为的探索较少。Chen等[108]基于飞秒激光垂直交叉扫描的方法,制备出一种由硅油和Fe3O4/PDMS膜组合而成的光响应界面,其中Fe3O4/PDMS膜表面分布着具有水下亲气性的微柱阵列,如
图 11. 飞秒激光制备的气泡运输表面。(a)~(c) Janus铝膜[107];(d)光响应界面[108]
Fig. 11. Bubble transportation surface fabricated by femtosecond laser. (a)-(c) Janus aluminum membrane[107]; (d) light-responsive interface[108]
4 结束语
水下气体浸润性界面在许多领域具有广阔的应用前景。而飞秒激光微纳加工技术相比于传统的微加工方案具有更高的加工精度,且能够适用于更广泛的加工材料,更重要的是其作为完全的物理加工技术,对环境不造成任何污染,因此当前已成为构建水下气体浸润性界面的重要手段之一。此外,飞秒激光对表面结构的精确设计同样符合了当前精密加工的研究趋势。本文系统总结了近年来利用飞秒激光微纳加工技术调控水下气体浸润性界面的研究进展。介绍了相应的研究背景,对水下超疏气表面、水下超亲气表面、水下超疏气-超亲气转换以及水下气体运输四个方面的应用进行了归纳阐述。
迄今为止,飞秒激光微纳加工技术仍处于起步阶段,离工业化应用还有很长一段距离,虽然目前在调控水下气体浸润性界面领域展现出巨大的潜力,但依然面临着许多挑战,许多关键的科学与技术问题亟待解决。1)飞秒激光微纳加工技术目前仍停留在实验研究阶段,虽然能够制备出各种具有水下特殊浸润性的界面,但制备出的表面中具有实际应用价值的并不多,该技术的潜力还有待开发。2)与大多数传统微纳加工方式相比,采用大功率高重复频率飞秒激光器与扫描振镜相结合的微纳加工技术在效率方面取得极大提升,但目前飞秒激光加工设备昂贵,其相对成本仍然很高。3)飞秒激光能够在材料表面制备出微纳结构进而调控其浸润性,然而加工出的粗糙结构会因材料和环境等因素的差异而出现不同的结果,其内在机理依旧不明朗。4)稳定性是实际应用中无法避免的问题。然而,目前通过飞秒激光制备的部分功能性材料无法维持长期稳定,浸润性会随放置时间的增加而逐渐发生变化,其在空气或水下等环境中的浸润性演化过程仍需探究。5)能够用于飞秒激光加工的材料相当广泛,理论上几乎所有的已知材料都能使用该技术加工。然而,目前用于制备浸润性界面的材料普遍硬度不高,对于金刚石、碳化硅等高硬度材料的研究较少。关于飞秒激光对这些高硬度材料表面浸润性的影响有待探索。
同其他正在发展中的工艺类似,飞秒激光微纳制造技术同样受到许多瓶颈的困扰,致使当前在调控水下气体浸润性表面方面表现并不理想,但其在精密制造领域相比于其他大部分微加工技术仍具备较大的优势,进行一些复杂精细的表面图案构建时该技术更加灵活,且相应的加工控制系统十分智能化,操作简便,无需经过复杂的培训便可熟练运用,这些都为其将来真正投入市场奠定了良好的基础。而随着研究的不断深入,对飞秒激光加工内在原理的理解不断加深,当前存在的科学技术问题终将会被解决。因此,可以肯定:通过飞秒激光微纳制造技术来制备水下气体浸润性表面,在将来必定会成为一个重要的发展方向。
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Article Outline
吴志鹏, 银恺, 吴俊瑞, 杨帅, 朱卓. 飞秒激光微纳制造水下气体浸润性表面[J]. 激光与光电子学进展, 2020, 57(11): 111418. Zhipeng Wu, Kai Yin, Junrui Wu, Shuai Yang, Zhuo Zhu. Femtosecond Laser Micro-Nano Fabrication of Underwater Gas Wettable Surface[J]. Laser & Optoelectronics Progress, 2020, 57(11): 111418.