可拉伸导体的最新进展

何文倩; 周湘; 刘遵峰

doi:10.7498/aps.69.20200632

摘要

可拉伸导体因能够适应较大的变形以及与三维不规则表面实现无缝接触, 受到了广泛关注, 在信息、能源、医疗、国防等领域具有广阔的应用前景. 在过去的几十年中, 人们开发出了很多性能优异的导电纳米材料, 如金属纳米线、碳纳米管、石墨烯和导电聚合物等. 将导电纳米填料均匀分散到聚合物基质中是制备弹性导体的一种有效方法, 可以实现导电性和拉伸性; 另一种方法则是对导电复合物进行结构设计, 引入可拉伸结构(如褶皱, 网型, 蛇形等), 实现大形变下的性能稳定. 本文主要总结了近五年来在弹性导体领域的最新进展, 并指出了当前弹性导体领域存在的挑战. 另外还讨论了一些柔性电子器件, 如发光二极管、传感器、加热器等的研究现状, 指明了柔性电子器件的发展趋势.

关键词:

Abstract

Flexible stretchable conductors have attracted wide attention due to their promising applications in information, energy, medical, national defense and other fields, where elastic conductors undergo large deformation and form intimate contact with three-dimensional irregular surfaces. Many conductive nanomaterials with excellent properties have been developed over the past decades, such as metal nanowires, carbon nanotubes, graphene and conductive polymers. One efficient method to prepare stretchable conductor is to disperse conductive materials into elastic matrix to form a conductive network, showing stretchability and conductivity. As an alternative way, elastic conductors show stable resistance change during stretch by use of buckled or serpentine structural design for rigid conductors. This review summarizes recent advances in flexible elastic conductors in the past five years. In addition, some flexible electronic devices such as light-emitting diodes, sensors, heaters, etc. are also discussed and the development direction in the field of flexible electronic devices is also suggested.

Keywords:

作者及机构信息

1.
南开大学化学学院, 南开大学药学院, 药物化学生物学国家重点实验室, 功能高分子材料教育部重点实验室, 天津　300071

2.
中国药科大学, 天然药物国家重点实验室, 生物活性天然产物研究江苏省重点实验室, 南京　210009

通信作者: 周湘, zhouxiang@cpu.edu.cn ; 刘遵峰, liuzunfeng@nankai.edu.cn

Authors and contacts

1.
Key Laboratory of Functional Polymer Materials, Ministry of Education, State Key Laboratory of Medicinal Chemical Biology, College of Chemistry, College of Pharmacy, Nankai University, Tianjin 300071, China

2.
Jiangsu Key Laboratory of Bioactive Natural Product Research, State Key Laboratory of Natural Medicines, Pharmaceutical University, Nanjing 210009, China

Corresponding author: Zhou Xiang, zhouxiang@cpu.edu.cn ; Liu Zun-Feng, liuzunfeng@nankai.edu.cn

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施引文献

图 1 (a) AgNW-PUU-PDMS薄膜被玻璃棒挤压的光学照片; (b) AgNW-PUU-PDMS薄膜放置在拉伸装置上以及拉伸50%应变的光学照片^[14]; (c) AgNW-poly(TBA-co-AA)复合物的制备过程; (d) AgNW-poly (TBA-co-AA) 复合物的截面扫描电镜 (SEM) 图; (e) AgNW-poly (TBA-co-AA) 复合物热驱动的示意图, 展示了68%的面积变化^[34]

Fig. 1. (a) Stretched area created by pressing AgNW-PUU-PDMS (silver nanowires-polyurethane-urea poly(dimethylsiloxane)) film with the end of a glass rod; (b) photographs of sample mounted on a stretching tester and sample after 50% increase in film length^[14]; (c) schematic illustration of the fabrication process of AgNW-polymer composites; (d) scanning electron microscope (SEM) image of the conductive cross-section surface of a AgNW-poly(TBA-co-AA) (poly(tert-butylacrylate-co-acrylic acid)) composite; (e) photographs of deformed circular active area of actuator in response to electric fields with different amplitude^[34].

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图 2 (a)银片/橡胶复合物的光学照片和示意图; (b)导电复合物作为皮肤电极检测皮肤拉伸压缩时的心电信号, 插图描述了拉伸和压缩时电极-皮肤界面的保形接触^[38]; (c)由模板印刷工艺制备可拉伸天线的示意图^[37]

Fig. 2. (a) Optical photographs and schematic illustration of the formation process of Ag-PDMS/Ecoflex; (b) effect of skin deformation on electrocardiogram signals collected by electrically conductive composites electrode. The insets show the conformal contact at the skin-electrode interface during compression and stretch^[38]; (c) stencil printing process to fabricate a stretchable antenna^[37].

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图 3 (a) Mxene水凝胶制备过程示意图; (b), (c) 3D Mxene泡沫和3D Mxene干凝胶的光学图片; (d) Mxene水凝胶, MXene /氧化石墨烯杂化膜和MXene膜在电流密度0.2—1000 A/g的速率性能; (e)在1000 mV/s下的循环伏安图^[43]

Fig. 3. (a) Schematic illustration of the formation process of MXene hydrogel; (b), (c) optical photographs of the 3D MXene foam and 3D MXene xerogel; (d) rate performance of the the Mxene hydrogel, Mxene/ reduced graphene oxide film, and MXene film electrodes at current densities ranging from 0.2 to 1000 A/g; (e) cyclic voltammetry profiles collected at 1000 mV/s^[43].

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图 4 (a)带有内部导电路径的液态金属复合物被拉伸和加捻的光学照片, 左边的插图展示了未变形的液态金属复合物, 右边的插图为复合物被拉伸50%的光学照片; (b)自修复的软体机器人; (c)从软机器人的自上而下视图穿越平滑地形的电影帧序列^[46]

Fig. 4. (a) A liquid metal (LM)-elastomer composite being stretched and twisted with an intricate design of electrically conductive traces. The lower left inset shows the undeformed sample and lower right inset is an optical micrograph showing the LM microdroplets in the elastomer at ϕ = 50%; (b) a soft quadruped with autonomously self-healing soft-matter electronics; (c) movie frame sequence from the top-down view of the soft robot traversing smooth terrain^[46].

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图 5 (a)磁流变弹性体的SEM图, 标尺为10 μm; (b) LMMRE电阻与应变的关系; (c)LMMRE作为传感器监测手指运动过程中的电阻变化; (d)手持式加热装置的分解示意图和红外热图像, 标尺为1 cm^[47]

Fig. 5. (a) SEM images of the liquid metal-filled magnetorheological elastomer (LMMRE). Scale bars are 10 µm; (b) resistance-strain curve of the LMMRE; (c) resistance-strain curve of the LMMRE as a sensor. Inset are finger with different gestures; (d) exploded schematics and thermal images of the hand-held heating column. Scale bars are 1 cm^[47].

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图 6 (a) Graphene-AgNW薄膜在PET基底上的实物照片, 标尺为2 cm, 插图为复合物的SEM图, 标尺为5 μm; Graphene-AgNW-PDMS在弯曲(b)、拉伸(c)过程中的电阻变化; (d)单像素隐形眼镜显示器的示意图; (e)隐形眼镜装置的实物照片, 标尺为5 mm, 插图为混合电极和隐形眼镜表面略微凹陷的无机发光二极管的光学显微图像, 标尺为300 μm; (f)人体模型眼睛上的无机发光二极管混合电极隐形眼镜装置的照片, 标尺为5 mm^[27]

Fig. 6. (a) Photograph of graphene-AgNW hybrid film on a polyethylene terephthalate (PET) substrate. The scale bar indicates 2 cm. The inset shows a SEM image of this hybrid (scale bar: 5 μm); (b), (c) relative difference in resistance as a function of radius of curvature and tensile strain; (d) schematic illustration of the device layout; (e) photograph of the contact lens device (scale bar: 5 mm). (Inset: optical microscopic image of slightly sunken inorganic light-emitting diode (ILED) on the surface of hybrid electrode and contact lens. Scale bar is300 μm); (f) a photograph of the ILED-hybrid electrode-contact lens device on an eye of a mannequin. Scale bar is 5 mm^[27].

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图 7 (a)在PDMS上印刷弹性导体, 左插图显示SWNT呈浓稠糊状, 右插图为线宽为100 µm的印刷弹性导体的显微镜照片; (b) SWNT复合物的SEM图像^[19]; (c) CNT/AgNW纳米复合物中AgNW和CNT含量与透明度的关系; (d) CNT/AgNW纳米复合物与只含有AgNW的复合物在拉伸过程中的电阻变化^[57]

Fig. 7. (a) Printed elastic conductors on a PDMS sheet. The insets show single walled carbon nanotubes (SWNTs) dispersed in paste and a micrograph of printed elastic conductors with a line width of 100 µm; (b) SEM image of the elastic conductor^[19]; (c) surface plot of transparency for various AgNW and carbon nanotubes (CNT) concentration; (d) stretchability comparison of AgNW only percolation network and hierarchical multiscale AgNW/CNT hybrid nanocomposite^[57].

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图 8 (a)从CNT森林中拉出的取向CNT薄膜的SEM图, 箭头代表拉伸方向; (b) CNT-PDMS薄膜在第一次、第二次拉伸-释放过程中的电阻变化^[58]; (c)三种CNT薄膜堆叠排列的示意图; (d)两层CNT交叉排列的SEM图; (e) CNT呈(45°, 45°)交叉排列的CNT-PDMS薄膜在第一次拉伸后的连续三次拉伸30%的电阻变化^[59]; (f)由CNT纤维制备的电子皮肤在拉伸状态的光学照片^[60]

Fig. 8. (a) SEM images of CNT ribbons directly drawn from CNT forest (arrow shows the drawing direction), and magnified CNT ribbons; (b) resistance of a CNT/PDMS film as a function of tensile strains in the 1 st stretching, 1 st releasing and 2 nd stretching cycles^[58]; (c) illustration of strips of cross-stacked films with three typical directions; (d) SEM image of a 2-layer cross-stacked CNT film; (e) change of resistance of a (45°, 45°) SACNT/PDMS film during three sequential stretch processes after the first stretch process^[59]; (f) photographs of a fully fabricated e-skin device under stretching conditions^[60].

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图 9 (a) PEDOT:PSS和离子增强剂的分子结构式; (b) PEDOT:PSS薄膜加入STEC后的示意图; (c) PEDOT/STEC薄膜的应力应变曲线; (d)加入不同离子增强剂的PEDOT:PSS复合物在拉伸过程中的电导率变化, 插图为PEDOT/STEC薄膜在拉伸状态下的照片^[67]

Fig. 9. (a) Chemical structures of poly(3, 4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) and representative ionic additives–assisted stretchability and electrical conductivity (STEC) enhancers; (b) schematic diagram representing the morphology of a stretchable PEDOT film with STEC enhancers; (c) stress/strain of freestanding PEDOT/STEC films; (d) conductivity under various strains for PEDOT with different STEC enhancers. Inset: photograph showing a freestanding PEDOT/STEC film being stretched^[67].

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图 10 (a)具有不同CVD沉积时间的聚乙烯醇(PVA)涂覆的平面和褶皱石墨烯片的电阻对拉伸应变的依赖性^[68]; (b) PET薄膜上铜纳米粒子的SEM图; (c)铜纳米粒子复合物在弯曲过程中的电阻变化, 下面插图展示了薄膜在最大最小弯曲半径下的状态, 右边插图展现了薄膜在折叠(破坏)状态下仍然导电^[69]

Fig. 10. (a) Dependency of resistance of the polyvinyl alcohol (PVA)-coated planar and wrinkled graphene sheets with different chemical vapor deposition (CVD) deposition times on the tensile strain ^[68]; (b) SEM image of transferred Cu nanoparticle random network on a PET film; (c) resistance change against bending radius. Bottom inset pictures show the digital image at maximum and minimum bending radius. Right inset pictures show permanently damaged (folded) transparent conductor at maximum bending radius, yet electrically conductive^[69].

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图 11 (a)蛇纹石结构的Ag-PDMS弹性导体的制备过程; (b)弹性导体透明度与片层电阻的关系; (c) Ag-PDMS弹性导体在拉伸过程中的电阻变化^[74]

Fig. 11. (a) Fabrication of the serpentine transparent conductors; (b) the relationship between the transmittance and sheet resistance of the composites; (c) the resistance of composites plotted as a function of the applied strain percentage^[74].

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图 12 (a) NTS_m@fiber制备过程示意图; (b) SEM图展现了施加100%应变时NTS₁₈₀ @fiber的多级褶皱^[70]; (c)熔融-拉丝法制备微米级纤维的示意图; (d)纤维拉伸过程中的电导率变化(插图为小应变下的电导率变化)^[75]

Fig. 12. (a) Steps in the fabrication of an NTS_m@fiber; (b) SEM images showing long- and short-period buckles for an NTS₁₈₀@fiber at 100% applied strain ^[70]; (c) schematic illustration of the melt-draw method used for the preparation of micrometer-size rubber fibers; (d) fiber electrical conductivity versus applied strain (with an inset for small applied strains)^[75].

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图 13 (a)面内褶皱的CNT的SEM图; (b) CNT-PDMS在拉伸过程中的电阻变化^[77]; (c)褶皱的AgNW网络透明电极的制备过程示意图; (d), (e)水面漂浮的AgNW网络压缩前后的光学显微镜图^[78]

Fig. 13. (a) SEM image showing the lateral buckling of CNTs; (b) resistance change of a typical CNT-PDMS film as a function of applied strain^[77]; (c) schematic for the preparation of AgNW networks with wavy configurations; (d), (e) optical microscope images of AgNW networks floated on water (d) before and (e) after compression^[78].

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图 14 (a)使用不同收集器制备不同取向的PVA纤维的示意图; (b)图案化电极的工艺流程图, 包括金属化、纳米纤维转移、图案化和包装; (c)不同取向PVA纤维的SEM, 标尺为10 μm; (d)柔性AgNW电极的光学照片^[86]

Fig. 14. (a) Schematic illustration of the electrospinning with different collectors to obtain various PVA NFs with controlled fiber orientation; (b) technological flow chart of the patterned electrode, including metallization, nanofibers (NFs) transfer, patterning, and packaging; (c) SEM images of different oriented PVA NFs. Scale bar is10 μm; (d) optical photographs of a fabricated stretchable transparent AgNWs electrode^[86].

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图 15 (a) CNT-rGO-CNF气凝胶的制备过程示意图^[90]; (b) CuNW-PVA气凝胶在第一次和第二次拉伸-释放60%应变过程中的电阻变化; (c) CuNW-PVA气凝胶在拉伸应变60%下循环1000次的电阻变化, 插图为拉伸至60%应变5次、100次、1000次的电阻变化^[91]

Fig. 15. (a) Schematic illustration of the fabrication of the CNT/rGO/CNF (carbon nanotubes-reduced grapheme oxide-cellulose fibers) aerogel^[90]; (b) variation of the resistance of the copper nanowires-polyvinyl alcohol (CuNW-PVA) as a function of tensile strain up to 60% in the first two stretch-release cycles; (c) variation of the resistance of the CuNW-PVA as a function of stretching cycles at a strain of 60%. The inset showed the resistance changes for the 5th, 100th, and 1000th stretching cycles, respectively^[91].

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图 16 (a) Agar-PAM双网络水凝胶呈花瓣状、打结及拉伸状态下的光学照片; (b) Agar-PAM双网络水凝胶作为传感器在拉伸-释放过程中的电阻和影响因子变化^[92]; (c)在人体模型上自粘水凝胶后, 通过LED灯演示人体模型上的水凝胶传感器; (d) PNIPAM/L/CNT水凝胶作为应变传感器的应用, 在不同部位电阻呈现可重复的规律性变化^[93]

Fig. 16. (a) Photograph of transparent flower-shaped, knotting and stretching Agar-PAM (polyacrylamide) hydrogel; (b) resistance change and gauge factor variations of the Agar-PAM hydrogel as sensors on applied tension^[92]; (c) demonstration of hydrogels as sensor on a wooden mannequin and pressure-dependent conductivity by LED bulb after the hydrogels self-adhered on a wooden mannequin model; (d) the application of (poly-N-isopropylacrylamide) PNIPAM/L/CNT hydrogel as a strain sensor, showing repeatable regular resistance changes in different parts^[93].

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图 17 (a)制备CNT/rGO-PDMS复合物的示意图; (b) CNT/rGO-PDMS复合物在拉伸过程中的电导率变化, 插图为2 wt.% CNT/rGO的复合物在不同拉伸应变下对应的电导率^[13]; (c) CNT/rGO-PDMS导体作为电气互联连接LED灯, 在拉伸弯曲过程中LED灯亮度不变^[98]

Fig. 17. (a) Schematic illustration of the CNT/rGO-PDMS preparation; (b) conductivity of the composite as a function of tensile strain, inset curve shows the electrical conductivity of the CNT/rGO-PDMS with 2 wt.% graphene/CNT loading under stretching ^[13]; (c) the brightness of LED lamps depending on the strains and bends^[98].

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图 18 (a) PUS-AgNW-PDMS双网络制备过程示意图^[101]; (b)褶皱的SWNT/PP泡沫在拉伸过程中的SEM截面图; (c)不同预应变的SWNT/PP泡沫在拉伸过程中的电阻变化^[25]

Fig. 18. (a) Fabrication procedure for PUS-AgNW-PDMS stretchable conductors^[101]; (b) SEM images for cross-sections of 35% biaxial pre-strain SWNT/PP (polypropylene foam) at applied strains; (c) resistance change as a function of applied strain for SWNT/PP with different biaxial fabrication strains^[25].

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图 19 (a)基于GO-AgNW/PUA制备的可拉伸OLED的结构示意图; (b) OLED在不同拉伸应变下的光学照片^[25]; (c)基于PAM-LiCl和ZnS制备的OLED的结构示意图; (d) OLED在不同拉伸应变下的光学照片^[104]

Fig. 19. (a) Schematic drawing of a fully stretchable OLED using GO-AgNW/PUA composite electrode; (b) optical photographs of an OLED stretched to specified strains^[25]; (c) schematic drawing of OLED using PAM-LiCl-ZnS composite electrode; (d) optical photographs of an OLED stretched to specified strains^[104].

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图 20 (a)基于丝网印刷的AgNW源/漏电极的全印刷FET的配置示意图; (b)柔性10 × 6 FET阵列的光学照片^[105]; (c)附着在织物上的FET拉伸30%的光学照片^[106]

Fig. 20. (a) Schematic illustration of the configuration of a fully printed FET based on screen-printed AgNW source/drain electrodes; (b) optical image of a fully printed stretchable 10 × 6 FET array^[105]; (c) FET adhered to a textile and stretched to 30%^[106].

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图 21 (a)基于Ag-Au核壳结构制备的超级电容器在循环拉伸过程中的相对电容变化^[107]; (b) Ag/Au/PPy核壳纳米网络薄膜的制备过程示意图; (c)基于Ag/Au/PPy核壳结构制备的超级电容器在不同拉伸应变下的CV曲线, 扫描速率为50 mV/s. 插图为电容器在拉伸状态下的示意图^[108]

Fig. 21. (a) The relative capacitance change of the Ag-Au core-shell NW-based supercapacitor during the repeated stretching cycles^[107]; (b) fabrication step of Ag/Au/PPy core-shell NW network mesh film; (c) CV curves of the supercapacitor based on Ag/Au/PPy coreshell NW mesh at a scan rate of 50 mV/s at indicated strain rates. Insets are schematic illustration of transparent and stretchable supercapacitor on strain condition^[108].

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图 22 (a)加捻的矩形夹芯纤维的示意图, 该纤维包括一个Ecoflex橡胶芯和两个对称的、褶皱的CNT电极; (b)纤维厚度方向的电容和分数变化与拉伸应变的关系, 插图为纤维侧视图的照片^[109]; (c)裂纹传感器的示意图^[115]; (d)基于褶皱的碳纳米管制备的传感器对手臂运动的响应^[112]

Fig. 22. (a) Schematic illustration of a twist-inserted rectangular sandwich fiber, which comprises an Ecoflex rubber core and two symmetric, buckled CNT electrodes; (b) capacitance and fractional change in fiber thickness versus tensile strain. Inset: photograph showing a side view of the sandwich fiber^[109]; (c) Illustration of the crack-based sensor^[115]; (d) response of the sensor to motions of arm muscle with different gestures^[112].

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图 23 (a)基于AgNW-PDMS渗透网络复合物制备的透明可拉伸加热器的示意图; (b)施加不同电压, AgNW-PDMS在0−30%应变下的温度变化, 插图为在不同拉伸应变下的红外图^[22]

Fig. 23. (a) Schematic illustration of the stretchable and transparent heater composed of Ag NW-PDMS composites; (b) transient temperature evolution of heater under stepwise application of 0−30% strain at a constant voltage. Insets are temperature field at each strain^[22].

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