碳纳米管受限空间对共轭高分子聚(9,9-二辛基芴-2,7-二基)链段运动行为的影响

李灵栋; 叶安娜; 周胜林; 张晓华; 杨朝晖

doi:10.7498/aps.68.20182008

摘要

在纳米受限空间中, 高分子往往会表现出与本体状态不同的性质, 如异常的链段运动特性及晶相间转变行为等, 这些性质对于研究和开发新型高分子材料具有重要的意义, 因此针对受限环境下高分子的物理化学特性研究也一直是高分子界关注的焦点. 本文通过化学气相沉积法制备垂直取向排列的多壁碳纳米管阵列, 借助溶剂润湿–收缩法获得规整的高密度阵列结构, 其取向排列的碳纳米管间隙形成了准一维的纳米受限空间, 尺寸在5—50 nm尺度下可调. 进一步将共轭高分子聚(9,9-二辛基芴-2,7-二基)(PFO)填充到碳管间隙的纳米空间中, 制备PFO与取向多壁碳纳米管阵列复合膜. 结果发现在碳纳米管形成的纳米受限空间中, PFO的链段热运动行为与本征态PFO薄膜相比受到了明显的抑制, 不同晶型间转变速度大大减缓, 提高了$\beta $构象的热稳定性, 同时取向排列的碳纳米管对PFO分子链取向排列分布具有明显的诱导作用, 有利于获得高性能的PFO晶体. 这种高密度取向排列的碳纳米管阵列结构未来可以用于制备优良发光性能及高稳定性的PFO光电器件.

关键词:

Abstract

The conjugated polymer polyflourene has been well studied for its strong blue light emission ability and high quantum efficiency behavior. It has wide applications for light emitting diodes, sensors as well as photo-detectors. Therein the $ \beta $ conformation of PFO crystals is more attractive due to its longer conjugation length, higher carrier mobility and better luminous efficiency. Therefore it is great essential to control the formation and stability of $ \beta $ conformation of PFO crystals to develop new kind of photo-electronic devices. As is known, polymeric materials confined in a nanometer-sized space often exhibit unique properties compared with their bulk state, such as abnormal chain mobility, molecular assembly and phase transition behavior. These factors are of great significance to develop new kind of material and applications. Generally the confined condition includes quantum dot (zero-dimensional, 0D), nanowire or nanotube (1D), ultrathin film (2D) and nanoparticle (3D). In this paper, we design a unique 1D nanoconfined environment based on vertically aligned carbon nanotube (CNT) array structure. An ultra-high CNT density is achieved through a solvent-induced contraction process. The adjacent narrow carbon nanotube gap thus forms a quasi-1 confined nano-space with the tunable size ranging from 5 to 50 nm. Then we infiltrate the conjugated polymer poly(9,9-dioctylfluorene-2,7-diyl) (PFO) into those nano-gaps of carbon nanotube arrays through a solvent evaporation method to obtain the PFO infilled CNT array composite film. It is found that the chain mobility of PFO molecules in such a 1D nano-confined space of carbon nanotubes is significantly suppressed compared with the scenario of the spin-coated PFO film. The transition speed between different crystal forms of PFO declines greatly, which meanwhile improves the thermal stability of the $ \beta $ conformation of PFO crystal. Additionally, the aligned carbon nanotubes have great effects on the orientation and distribution of PFO chains. The PFO crystals are confirmed to grow preferentially along the longitudinal direction of CNT array, which is potential to grow PFO crystals with high quality and excellent performance. Thus, such a PFO/CNT array composite film can have great potential to prepare PFO photovoltaic devices with excellent luminescent properties and high stability in the future.

Keywords:

carbon nanotube arrays /
polymer poly(9,9-dioctylfluorene-2,7-diyl) /
confined space /
chain mobility

作者及机构信息

苏州大学物理科学与技术学院, 软凝聚态物理及交叉研究中心, 江苏省薄膜材料重点实验室, 苏州　215006

通信作者: 杨朝晖, yangzhaohui@suda.edu.cn

基金项目: 国家自然科学基金(批准号: 21204059)、江苏省特聘教授计划(批准号: SR10800215, SR10800312)和江苏省自然科学基金(批准号: BK20181430)资助的课题.

Authors and contacts

Jiangsu Key Laboratory of Thin Films,Center for Soft Condensed Matter Physics and Interdisciplinary Research, School of Physical Science and Technology, Soochow University, Suzhou 215006, China

Corresponding author: Yang Zhao-Hui, yangzhaohui@suda.edu.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant No. 21204059), the Specially-Appointed Professor Plan in Jiangsu Province, China (Grant Nos. SR10800215, SR10800312), and the Natural Science Foundation of Jiangsu Province, China (Grant No. BK20181430).

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参考文献

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施引文献

图 1 PFO的化学结构式及三种不同的构象结构及其特征内扭角的示意图 (a) R=(CH₂)₇CH₃; (b) $\alpha$构象; (c) $\gamma $构象; (d) $\beta $构象

Fig. 1. Chemical structure of PFO and Schematic illustration of three distinct conformational structures and their characteristic intrachain torsional angles: (a) R=(CH₂)₇CH₃; (b) $\alpha$-phase; (c) $\gamma $-phase; (d) $\beta $-phase.

下载: 全尺寸图片幻灯片

图 2 (a) PFO/S-ACNTs样品制备流程图; (b) ACNTs阵列收缩前后的对照图; (c) ACNTs的SEM和TEM图 (插图); (d), (e), (f) 相同放大倍数ACNTs、S-ACNTs和PFO/S-ACNTs的SEM图

Fig. 2. (a) Schematic preparation of PFO/S-ACNTs; (b) photographs of ACNTs before and after the densification; (c) SEM and TEM (insets) images of as-grown ACNTs; (d), (e), (f) SEM cross-section images of ACNTs、S-ACNTs and PFO/S-ACNTs in the same magnification.

下载: 全尺寸图片幻灯片

图 3 (a) PFO薄膜的吸收光谱 (蓝色) 与荧光光谱 (红色); (b), (c), (d) 分别对应PFO薄膜、PFO/S-ACNTs和PFO&RCNTs薄膜随退火温度变化的荧光光谱图 (激发波长为380 nm); (e) 三种PFO样品0—0发射峰峰位随退火温度的变化

Fig. 3. (a) UV-vis absorption spectra (blue) and PL spectra (red) of PFO film; PL spectra of PFO film, PFO/S-ACNTs and PFO&RCNTs film with different annealing conditions corresponding to (b), (c) and (d), respectively (the excitation wavelength is 380 nm); (e) annealing temperature dependence of the 0—0 emission peak of three PFO based samples.

下载: 全尺寸图片幻灯片

图 4 三种薄膜样品在不同温度下退火后的XRD衍射图 (所有样品在氮气氛围下退火1 h) (a) PFO滴膜样品; (b) PFO/S-ACNTs样品; (c) PFO & RCNTs

Fig. 4. XRD diffraction pattern of (a) PFO drop film, (b) PFO/S-ACNTs, and (c) PFO & RCNTs at different annealing temperature (all samples are annealed in nitrogen atmosphere for 1 h).

下载: 全尺寸图片幻灯片

[1]	Cook J H, Santos J, Li H, Al-Attar H A, Bryce M R, Monkman A P 2014 J. Mater. Chem. C 2 5587 Google Scholar
[2]	Schelkle K M, Bender M, Jeltsch K, Buckup T, Mullen K, Hamburger M, Bunz U H 2015 Angew. Chem. Int. Ed. 54 14545 Google Scholar
[3]	Luo J, Zhou Y, Niu Z Q, Zhou Q F, Ma Y G, Pei J 2007 J. Am. Chem. Soc. 129 11314 Google Scholar
[4]	Zhong C, Duan C, Huang F, Wu H, Cao Y 2011 Chem. Mater. 23 326 Google Scholar
[5]	Cingil H E, Storm I M, Yorulmaz Y, Te B D W, De V R, Cohen S M A, Sprakel J 2015 J. Am. Chem. Soc. 137 9800 Google Scholar
[6]	Lv F T, Qiu T, Liu L B, Ying J M, Wang S 2016 Small 12 696 Google Scholar
[7]	Inganas O, Zhang F, Andersson M R 2009 Acc. Chem. Res. 42 1731 Google Scholar
[8]	Wu H, Ying L, Yang W, Cao Y 2009 Chem. Soc. Rev. 38 3391 Google Scholar
[9]	Scherf U, List E J W 2002 Adv. Mater. 14 477 Google Scholar
[10]	Chen S H, Su A C, Su C H, Chen S A 2005 Macromolecules 38 379 Google Scholar
[11]	Chen S H, Chou H L, Su A C, Chen S A 2004 Macromolecules 37 6833 Google Scholar
[12]	Grell M, Bradley D D C, Ungar G, Hill J, Whitehead K S 1999 Macromolecules 32 5810 Google Scholar
[13]	Lee C C, Lai S Y, Su W B, Chen H L, Chung C L, Chen J H 2013 J. Phys. Chem. C 117 20387 Google Scholar
[14]	Chunwaschirasiri W, Tanto B, Huber D L, Winokur M J 2005 Phys. Rev. Lett. 94 107402 Google Scholar
[15]	Arif M, Volz C, Guha S 2006 Phys. Rev. Lett. 96 025503 Google Scholar
[16]	Cadby A J 2000 Phys. Rev. B 62 15604 Google Scholar
[17]	Lu H H, Liu C Y, Chang C H, Chen S A 2007 Adv. Mater. 19 2574 Google Scholar
[18]	Peet J, Brocker E, Xu Y, Bazan G C 2008 Adv. Mater. 20 1882 Google Scholar
[19]	Asada K, Kobayasi T, Naito H 2006 Japanese Journal of Applied Physics Part 2-Letters and Express Letters 45 L247 Google Scholar
[20]	Zhang Q, Chi L, Hai G, Fang Y, Li X, Xia R, Huang W, Gu E 2017 Molecules 22 315 Google Scholar
[21]	Huang L, Huang X, Sun G, Gu C, Lu D, Ma Y 2012 J. Phys. Chem. C 116 7993 Google Scholar
[22]	Li T, Liu B, Zhang H, Ren J, Bai Z, Li X, Ma T, Lu D 2016 Polymer 103 299 Google Scholar
[23]	Li T, Huang L, Bai Z, Li X, Liu B, Lu D 2016 Polymer 88 71 Google Scholar
[24]	O'Carroll D, Lieberwirth I, Redmond G 2007 Nat. Nanotechnol. 2 180 Google Scholar
[25]	Grimm S, Martín J, Rodriguez G, Fernández-Gutierrez M, Mathwig K, Wehrspohn R B, Gösele U, San Roman J, Mijangos C, Steinhart M 2010 J. Mater. Chem. 20 3171 Google Scholar
[26]	Liu C L, Chen H L 2018 Soft Matter 14 5461 Google Scholar
[27]	Li M, Wu H, Huang Y, Su Z 2012 Macromolecules 45 5196 Google Scholar
[28]	Shin K, Woo E, Jeong Y G, Kim C, Huh J, Kim K W 2007 Macromolecules 40 6617 Google Scholar
[29]	Garcia G M C, Linares A, Hernandez J J, Rueda D R, Ezquerra T A, Poza P, Davies R J 2010 Nano Lett. 10 1472 Google Scholar
[30]	Steinhart M, Goring P, Dernaika H, Prabhukaran M, Gosele U, Hempel E, Thurn A T 2006 Phys. Rev. Lett. 97 027801 Google Scholar
[31]	Hui W, Wei W, Huixian Yang A, Su Z 2007 Macromolecules 40 4244 Google Scholar
[32]	Wu H, Wang W, Huang Y, Su Z 2009 Macromol Rapid Commun. 30 194 Google Scholar
[33]	Wu Y, Gu Q, Ding G, Tong F, Hu Z, Jonas A M 2013 ACS Macro Lett. 2 535 Google Scholar
[34]	Ding G, Wu Y, Weng Y, Zhang W, Hu Z 2013 Macromolecules 46 8638 Google Scholar
[35]	O'Brien G A, Quinn A J, Tanner D A, Redmond G 2006 Adv. Mater. 18 2379 Google Scholar
[36]	O'Carroll D, Iacopino D, O'Riordan A, Lovera P, O'Connor É, O'Brien G A, Redmond G 2008 Adv. Mater. 20 42 Google Scholar
[37]	Steinhart M, Wendorff J H, Greiner A, Wehrspohn R B, Nielsch K, Schilling J, Choi J, Gösele U 2002 Science 296 1997 Google Scholar
[38]	Ding G, Li C, Li X, Wu Y, Liu J, Li Y, Hu Z, Li Y 2015 Nanoscale 7 11024 Google Scholar
[39]	Wei S, Zhang Y, Liu J, Li X, Wu Y, Wei H, Weng Y, Gao X, Li Y, Wang S D, Hu Z 2015 Adv. Mater. Interfaces 2 1500153 Google Scholar
[40]	Zhang P, Huang H, He T, Hu Z 2012 ACS Macro Lett. 1 1007 Google Scholar
[41]	Li X H, Shen X Z, Gao X, Weng Y Y 2017 RSC Adv. 7 55885 Google Scholar
[42]	Ajayan P M, Lijima S 1993 Nature 361 333 Google Scholar
[43]	Ugarte D, Stöckli T, Bonard J M, Châtelain A, Heer W A D 1998 Appl. Phys. A 67 101
[44]	Nakamura A, Koyama T, Miyata Y, Shinohara H 2016 J. Phys. Chem. C 120 4647 Google Scholar
[45]	Liu Z, Liao G, Li S, Pan Y, Wang X, Weng Y, Zhang X, Yang Z 2013 J. Mater. Chem. A 1 13321 Google Scholar
[46]	Bai Z, Liu Y, Li T, Li X, Liu B, Liu B, Lu D 2016 J. Phys. Chem. C 120 27820 Google Scholar
[47]	Futaba D N, Hata K, Yamada T, Hiraoka T, Hayamizu Y, Kakudate Y, Tanaike O, Hatori H, Yumura M, Iijima S 2006 Nat. Mater. 5 987 Google Scholar
[48]	Zhou S, Sheng J, Yang Z, Zhang X 2018 J. Mater. Chem. A 6 8763 Google Scholar
[49]	Li X, Bai Z, Liu B, Li T, Lu D 2017 J. Phys. Chem. C 121 14443 Google Scholar
[50]	Jen T H, Wang K K , Chen S A 2012 Polymer 53 5850 Google Scholar
[51]	Chen S H, Su A C, Chen S A 2005 J. Phys. Chem. B 109 10067 Google Scholar
[52]	Torkkeli M, Galbrecht F, Scherf U, Knaapila M 2015 Macromolecules 48 5244 Google Scholar
[53]	Sheng J, Zhou S, Yang Z, Zhang X 2018 Langmuir 34 3678 Google Scholar
[54]	Wang M, Li L, Zhou S, Tang R, Yang Z, Zhang X 2018 Langmuir 34 10702 Google Scholar

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[18]	陈传盛, 陈小华, 李学谦, 张　刚, 易国军, 张　华, 胡　静. 碳纳米管增强镍磷基复合镀层研究. 物理学报, 2004, 53(2): 531-536. doi: 10.7498/aps.53.531
[19]	宋教花, 张耿民, 张兆祥, 孙明岩, 薛增泉. 多壁碳纳米管阵列场发射研究. 物理学报, 2004, 53(12): 4392-4397. doi: 10.7498/aps.53.4392
[20]	朱亚波, 王万录, 廖克俊. 对碳纳米管阵列的场发射电场增强因子以及最佳阵列密度的研究. 物理学报, 2002, 51(10): 2335-2339. doi: 10.7498/aps.51.2335

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碳纳米管受限空间对共轭高分子聚(9,9-二辛基芴-2,7-二基)链段运动行为的影响