SCIENCE CHINA Information Sciences, Volume 62, Issue 12: 220403(2019) https://doi.org/10.1007/s11432-019-2676-x

All-carbon hybrids for high-performance electronics, optoelectronics and energy storage

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  • ReceivedAug 26, 2019
  • AcceptedOct 14, 2019
  • PublishedNov 11, 2019


The family of carbon allotropes such as carbon nanotubes (CNTs) and graphene, with their rich chemical and physical characteristics, has attracted intense attentions in the field of nanotechnology and enabled a number of disruptive devices and applications in electronics, optoelectronics and energy storage. Just as no individual 2D (two-dimensional) material can meet all technological requirements of various applications, combining carbon materials of different dimensionality into a hybrid form is a promising strategy to optimize properties and to build novel devices operating with new principles. In particular, the direct synthesis of 2D or 3D (three-dimensional) sp$^2$-hybridized all-carbon hybrids based on merging CNTs and graphene affords a great promise for future electronic, optoelectronic and energy storages. Here, we review the progress of all-carbon hybrids-based devices, covering material preparation, fabrication techniques as well as applied devices. Recent progress about large-scale synthesis and assembly techniques is highlighted, and with many intrinsic advantages, the all-carbon strategy opens up a highly promising approach to obtain high-performance integrated circuits. Moreover, this review will discuss the remaining challenges in the field and provide perspectives on future applications.


This work was supported in part by National Key R D Program of China (Grant Nos. 2018YFB22-00500, 2017YFA0206304), National Basic Research Program of China (Grant No. 2014CB921101), National Natural Science Foundation of China (Grant Nos. 61775093, 61427812), National Youth 1000-Talent Plan, `Jiangsu Shuangchuang Team' Program, and Jiangsu NSF (Grant No. BK20170012).


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  • Figure 1

    (Color online) Schematic of the electronic, opto-electronic devices and supercapacitors based on graphene/CNTs all-carbon materials. The main examples of the representative architecture and their main features are exhibited.

  • Figure 2

    (Color online) The structures of carbon nanotube and graphene. (a) The carbon atoms of graphene in a honeycomb lattice. A nanotube formed by rolling a strip of graphene along the chiral vector ($C_{h})$ [4]@Copyright 2007 Macmillan Publishers Ltd. (b) Bandgaps versus nanotube radius for several selected families CNTs with different chiral [n,~m] [18]@Copyright 2005 ACS. The electronic DOS for selected metallic (c) and semiconducting (d) nanotubes [30]@Copyright 2011, ACS. (e) The linear energy dispersion of graphene in the honeycomb lattice [3]@Copyright 2009 APS.

  • Figure 3

    (Color online) Growth separation and transfer of carbon nanotubes and graphene. (a) The typical SEM image of horizontally CNTs [34]@Copyright 2001 AIP. (b) The centrifuge tube loaded with as-received nanotubes with different diameters [35]@Copyright 2009 Macmillan Publishers Ltd. (c) Unzipping diagram from a carbon nanotube to a nanoribbon. Inset: a TEM image of formed nanoribbon [36]@Copyright 2009 Macmillan Publishers Ltd. (d) Graphene transferred from the Pt foil to a SiO$_{2}$ chip [37]@Copyright 2012 Macmillan Publishers Ltd. (e) Photograph of fast growth graphene transferred on the wafer [38]@Copyright 2016 Wiley. (f) Schematics of graphene growth by local fluorine. (g) SEM image of graphene domains growing at $\Delta~t$=5 s [39]@Copyright 2019 Macmillan Publishers Ltd.

  • Figure 4

    (Color online) Configuration models and fabrications of all-carbon hybrids. (a) Hybrids of graphene with horizontal CNTs and the typical synthesis process [69]@Copyright 2012 Macmillan Publishers Ltd. (b) Hybrids of graphene with vertical CNTs and the typical synthesis process [70] @Copyright 2014 ACS. (c) TEM and schematic of the vein-membrane-like hybrid [71]@Copyright 2013 Macmillan Publishers Ltd. (d) TEM image of interconnected SWCNT networks in rebar graphene sheets [70]@Copyright 2014 ACS. (e) Hybrid paper macroscopic appearance after thermal reduction [72] @Copyright 2013 ACS. (f) SEM of nanotube carpet [69]@Copyright 2012 Macmillan Publishers Ltd. (g) and (h) SEM images of the cross-section of all-carbon hybrid microfibers [73]@Copyright 2014 Macmillan Publishers Ltd.

  • Figure 5

    (Color online) All-carbon hybrids for electronic devices. (a) Transparent electrodes based on graphene/CNTs hybrid films compared with ITO films [113] @Copyright 2009 ACS. (b) The sheet resistances distribution of graphene/CNTs hybrids measured along parallel ($\vert~\vert~)$ and perpendicular ($~\bot )$ to CNT array. (c) Optical transmittance spectra of the flat electrochromic device [116]@Copyright 2015 Wiley. (d) Hysteresis of the device using graphene gate electrode [117]@Copyright 2011 ACS. (e) Current change of on/off states versus the duration time of gate pulse [118]@Copyright 2011 Wiley. (f) Output characteristics of an inverter [117]@Copyright 2011 ACS. (g) The current variations to the acoustic vibrations from different words [119]@Copyright 2017 Wiley. (h) Field emission current density as a function of applied field of graphene/CNTs hybrids with different CNT densities [120]@Copyright 2012 RSC. (i) Photograph of a field-emitting device [121]@Copyright 2010 Wiley.

  • Figure 6

    (Color online) All-carbon hybrids for optoelectronic devices. (a) Comparison of transport characteristics between graphene and metal CNT (m-CNT) and semiconducting CNT (s-CNT) [143]@Copyright 2011 AIP. (b) External quantum efficiency of all-carbon photodetector under 650 nm illumination. Inset shows the responsivities versus optical power of different illumination wavelengths [124]@Copyright 2015 Macmillan Publishers Ltd. (c) Images of folded photodetector and its photoresponse under a high strain of over 50%[144]Copyright 2017 Wiley. (d) Power conversion efficiency of the different solar cells [145]@Copyright 2015 IOP. (e) Electroluminescence (EL) spectra with the current in LED [146]@Copyright 2014 Macmillan Publishers Ltd. (f) Schematic illustrations of the synapse based on graphene/SWNT hybrids. (g) The change of PSC amplitudes triggered by a presynaptic light spike Insets: the typical IPSC and EPSC changes triggered by the light spike [147]@Copyright 2017 IOP. (h) Image of the integrated array based on graphene/C$_{60}$ all-carbon hybrids. (i) The corresponding spatial-light mapping for the devices [148]@Copyright 2019 ACS.

  • Figure 7

    (Color online) All-carbon hybrids with different dimensionalities for energy storages. (a) Illustration of 2D graphene/CNTs hybrids via self-assembly process [168]@Copyright 2009 ACS. (b) Cycling performance of all-carbon composite electrode [165]@Copyright 2011 RSC. (c) Vertical CNTs pillar height versus the nanotube deposition time. Inset is a SEM image of thermally expanded graphene layers intercalated with CNTs [170]@Copyright 2011 ACS. (d) The density, surface area of hybrid fibers as a function of SWNT fraction. Inset show a photograph of the as-prepared fibers collected in water. (e) Schematic of a self-powered nanosystem. Inset: SEM of an aligned TiO$_{2}$ nanorod array [73]@Copyright 2014 Macmillan Publishers Ltd. (f) Cyclic performance and high-rate capability of the vertically aligned CNT/graphene film in a lithium-ion battery [171]@Copyright 2011 Wiley. (g) Schematics of 3D graphene/CNT-Ni nanostructure as an anode material during the charging and discharging processes in lithium-ion batteries [172]@Copyright 2013 IOP.

  • Table 1   Comparison of technical features of all-carbon hybrids forelectronics, optoelectronics and energy storages
    Architecture Electronics Optoelectronics Energy storages
    Individual CNT High carrier mobility and Limited response time and High electrical
    small on/off ratio for responsivity from UV conductivity but tends
    metallic CNTs; to NIR to stack into bundles
    Larger on/off ratio and
    limited carrier mobility
    for semiconducting CNTs
    Individual graphene High carrier mobility but Ultrafast photoresponse High surface area,
    small on/off ratio (GHz) but limited chemically stable but
    responsivity from easily forms irreversible
    UV to THz agglomerates
    2D planar CNT/graphene High carrier mobility and Strong light absorption Well suited for
    limited on/off ratio and high carrier mobility; optoelectronics such
    due to graphene efficient exciton separation as photodetectors
    at interface; fast
    response time and
    high photoresponsivity
    3D vertical CNT/graphene Well suited for energy Strong light absorption High surface-to-volume
    storages such as and high carrier ratio; abundant mesoporosity
    Li-ion batteries mobility; improved and activation sites

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