Research progress of paper-based flexible conductive composite materials
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摘要: 伴随着现代电子科技领域的蓬勃发展，大量电子垃圾的产生给环境带来了巨大压力。以纤维素为主的柔性导电复合材料具有与传统石油基导电产品不可比拟的优点，如轻质、可降解、可再生、生物相容性好等。近年来，纸基柔性导电材料逐步成为该领域研究的热点。本文综述了近些年来国内外纸基柔性导电材料的研究进展，描述了柔性导电材料的工作原理，详细概述了纸基导电材料的制备方法与相关应用，对纸基柔性导电材料亟待解决的问题及未来发展趋势进行了总结和展望。Abstract: With the rapid development of modern electronic technology, a large amount of e-waste puts huge pressure on the environment. The cellulose-based flexible conductive composite material has incomparable advantages with traditional petroleum-based conductive products, such as lightweight, degradable, renewable, bio-compatible, and so on. In recent years, paper-based flexible conductive materials have gradually become a research focus in this field. This article reviews the research progress of paper-based flexible conductive materials at home and abroad in recent years, describes the working principle of flexible conductive materials, summarizes the preparation methods and related applications of paper-based flexible conductive materials in detail, and the paper-based flexible conductive materials urgently need to be solved and the future development trend is summarized and prospected.
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图 2 利用迈耶棒涂覆A4纸示意图 (a)、用薄层电阻变化来反映聚对苯二甲酸乙二醇酯(PET)与纸在洗涤前后活性材料附着情况 (b)、导电材料在不同弯曲半径下与电阻变化率R/R0曲线(c)[23]、利用聚偏氟乙烯(PVDF)与单壁碳纳米管(SWNT)制备导电材料的过程 (d)~(e)以及在2 500次循环下纸基超级电容器的电容保持性能曲线 (f)[24]
Figure 2. Schematic diagram of coating A4 paper with Meyer rod (a), change of sheet resistance to reflect the adhesion of the active material between polyethylene terephthalate (PET) and paper before and after washing (b), conductive material under different bending radius and the resistance change rate R/R0 curve (c)[23], process of preparing conductive materials using polyvinylidene fluoride (PVDF) and single-walled carbon nanotube (SWNT) (d)-(e), and capacitance retention performance curve of paper-based supercapacitors under 2 500 cycles (f)[24]
图 3 喷墨打印机打印超级电容器示意图及所用的喷墨打印机照片(a)、超级电容器与温度传感器连接制作智能温度感应杯 (b)[26]、利用丝网印刷技术制备氧化石墨烯(GO)湿度发电器件示意图 (c)、超级电容器供电示意图 (d)[28]
Figure 3. Schematic diagram of inkjet printer printing super capacitor and the photo of inkjet printer (a), connecting supercapacitors with temperature sensor to make intelligent temperature sensing cup (b)[26], schematic diagram of graphene oxide (GO) humidity power generation device prepared by screen printing technology (c), schematic diagram of super capacitors power supply for calculator (d)[28]
图 4 聚丙烯(PP)薄膜热压示意图及载旋涂法下的银镜反应 (a)、基于银/纸电极材料制备的有机太阳能电池(OSC)与有机发光二极管(OLED) (b)[29]、利用3D打印技术制备锂电池结构示意图 (c)[30]
Figure 4. Schematic diagram of polypropylene (PP) film hot pressing and silver mirror reaction under spin coating method (a), organic solar cells (OSC) and oganic light emitting diodes (OLED) based on silver/paper electrode material (b)[29], structure diagram of lithium battery prepared by 3D printing (c)[30]
图 5 石墨烯/纤维素纸超级电容器照片 (a)；在5 000次循环下超级电容器(SC)的电容保持率，嵌图显示的是SC的伏安曲线(b)[31]；柔性、超薄纤维素纤维/石墨阳极制备过程示意图 (c)；石墨(GP)/纤维/羧甲基纤维素(CMC)阳极的比电容与库仑效率曲线 (d)[32]；细菌纤维素(BC)/聚吡咯(PPy)/多壁碳纳米管(MWCNTs)复合膜制备过程示意图 (e)；电容保持率曲线 (f)[35]；PPy沉积过程示意图 (g)；在弯曲折叠下电压与电流密度曲线 (h)[39]
Figure 5. Photograph of graphene/cellulose paper supercapacitor (a); Capacitance retention of supercapacitor (SC) under 5000 cycles, the inset shows the CV curve under 1 and 5 000 cycles (b)[31]; Schematic diagram of the preparation process of flexible, ultra-thin cellulose fiber/graphite anode (c); Specific capacitance and coulombic efficiency profile of graphite (GP)/fiber/carboxymethylcellulose (CMC) anode (d)[32]; Preparation process of bacterial cellulose (BC)/polypyrrole (PPy)/multiwalled carbon nanotube (MWCNTs) composite membrane (e); Capacitance retention curve (f)[35]; Schematic diagram of PPy deposition process (g); Voltage and current density profile under bending and folding (h)[39]
RGO—Reduced graphene oxide; CMP—5'-cytidine acid
图 6 在不同吡咯(Py)/OH摩尔比下Py/纤维的电导率曲线，嵌图为导电纤维的TEM图像 (a)；不同参数下，超级电容器的电容曲线 (b)；超级电容器的充放电性能 (c)[44]；还原氧化石墨烯(RGO)/PPy/碳纤维纸电极制备示意图 (d)；三种复合材料电流密度对面积电容曲线 (e)；超级电容器的电容保持率 (f)[45]；BC/碳纳米管(CNT)超级电容器比电容变化曲线 (g)[48]；锂离子电池结构示意图 (h)[49]；锂离子电池电极电容保持率与库伦效率曲线 (i)[51]
Figure 6. Conductivity profile of pyrrole (Py)/fiber under different Py/OH molar ratio, inset shows the TEM image of conductive fiber (a); Capacitance profile of supercapacitor under different parameters (b); Supercapacitor charge and discharge performance (c)[44]; Schematic diagram of preparation of reduced graphene oxide (RGO)/PPy/carbon fiber paper electrode (d); Curves of current density versus area capacitance for three composite materials (e); Capacitance retention of supercapacitors (f)[45]; Specific capacitance change curves of BC/carbon nanotube (CNT) supercapacitors (g)[48]; Structure diagram of lithium ion battery (h)[49]; Curves of electrode capacitance retention and coulomb efficiency for lithium ion battery (i)[51]
LTO—Li4Ti5O12; LCO—LiCoO2; CB—Carbon black; CCFs—Chopped carbon fibers
图 7 纸基摩擦纳米发电机(P-TENG)示意图 (a)、不同堆叠层数产生的电荷数 (b)[54]、非接触式TENGs原理图(c)、不同距离下TENGs电压输出情况 (d)、TENGs为电容器充电 (e)[55]、TEGs电流与功率、电压曲线 ((f)、(g))[56]、不同基底下光透射雾度与透射率曲线 (h)[57]、电压与电流密度曲线 (i)[58]、CNP太阳能电池结构示意图 (j)、电流转换效率对比图 (k)[59]
Figure 7. Schematic diagram of P-nanogenerator (TENG) (a), number of charges generated by different stacking layers (b)[54], schematic diagram of noncontact TENGs (c), voltage output of Tengs at different distances (d), TENGs charges the capacitor (e)[55], curves of TEGs current versus power and voltage ((f), (g))[56], optical transmission haze versus transmittance for different substrates (h)[57], voltage versus current density curve (i)[58], structure diagram of CNP solar cell (j), comparison of current conversion efficiency (k)[59]
图 8 生物燃料电池工作原理 (a)、电压与电流密度曲线 (b)、葡萄糖测定可视化示意图 (c)[63]、酶基生物燃料电池纸基分析装置(µPAD-EBFC)制备过程示意图 (d)、不同葡萄糖浓度下电压与电流密度曲线 (e)、µPAD-EBFC串并联情况 (f)[64]
Figure 8. Schematic diagram of working principle of biofuel cells (a), voltage and current density curve (b), visualization of glucose determination (c)[63], schematic diagram of preparation process of paper-based analytical device for enzymatic biofuel cells (µPAD-EBFC) (d), voltage and current density curves under different glucose concentrations (e), voltage output of series and parallel connection of µPAD-EBFC (f)[64]
图 9 碳化钼/石墨烯(MCG)复合材料SEM图像 (a)；电磁屏蔽性能图，嵌图为3D结构示意图 (b)[66]；Ti3C2Tx/纳米纤维素纤维复合纸制备方法与材料结构示意图 (c)；材料拉伸应变曲线 (d)；电磁屏蔽性能曲线 (e)[67]；导电滤纸制备流程示意图 (f)；电磁屏蔽性能曲线 (g)；导电滤纸表观形貌SEM图像 (h)；电磁屏蔽过程示意图 (i)[68]
Figure 9. SEM image of molybdenum carbide/graphene(MCG)composites (a); Picture of electromagnetic shielding performance, the inset shows 3D structure of the MCG (b)[66]; Preparation method and material structure of Ti3C2Tx/cellulose nanofiber composite paper (c); Tensile strain curve of materials (d); Profile of electromagnetic shielding performance (e)[67]; Preparation process of conductive filter paper (f); Profile of electromagnetic shielding performance (g); SEM image of the surface morphology of conductive filter paper (h); Schematic diagram of electromagnetic shielding process (i)[68]
表 1 不同纸基复合材料制备方法分析
Table 1. Analysis of different preparation methods of paper-based conductive composites
Method Active material Substrate Index Parameter Application Reference Meyer rod coating EDOT Filter paper Conductivity 1.8 S/cm Electrode [22] Inkjet printing AgNWs, SWNTs, AC A4 paper Resistance 8 Ω/sq Supercapacitor [26] Screen printing GO A4 paper Voltage output 0.7 V Humidity generator [28] Spin coating Silver nanoparticles Cellulose paper Conductivity 1.2×107 S/m Electrode, solar cell substrate [29] Dehydration forming PPy, MWCNTs Bacterial cellulose paper Conductivity 7.78 S/cm Electrode, supercapacitor [35] Polymerization PPy, GO Cellulose paper Resistance 1.7 Ω/sq Electrode, supercapacitor [39] In-situ growth AuNP Cellulose paper Conductivity 1.15×10−5 Ω·cm Electrode [43] 
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