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Arai, S. Fabrication of Metal/Carbon Nanotube Composites by Electrochemical Deposition. Encyclopedia. Available online: https://encyclopedia.pub/entry/16223 (accessed on 25 April 2024).
Arai S. Fabrication of Metal/Carbon Nanotube Composites by Electrochemical Deposition. Encyclopedia. Available at: https://encyclopedia.pub/entry/16223. Accessed April 25, 2024.
Arai, Susumu. "Fabrication of Metal/Carbon Nanotube Composites by Electrochemical Deposition" Encyclopedia, https://encyclopedia.pub/entry/16223 (accessed April 25, 2024).
Arai, S. (2021, November 21). Fabrication of Metal/Carbon Nanotube Composites by Electrochemical Deposition. In Encyclopedia. https://encyclopedia.pub/entry/16223
Arai, Susumu. "Fabrication of Metal/Carbon Nanotube Composites by Electrochemical Deposition." Encyclopedia. Web. 21 November, 2021.
Fabrication of Metal/Carbon Nanotube Composites by Electrochemical Deposition
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This entry is adapted from the peer-reviewed paper 10.3390/electrochem2040036

Metal/carbon nanotube (CNT) composites are promising functional materials due to the various superior properties of CNTs in addition to the characteristics of metals. Electrochemical deposition can be classified into three types: (1) composite plating by electrodeposition or electroless deposition, (2) metal coating on CNT by electroless deposition, and (3) electrodeposition using CNT templates, such as CNT sheets and CNT yarns. 

metal/carbon nanotube composite electrochemical deposition electrodeposition electroless deposition composite plating carbon nanotube sheet carbon nanotube yarn

1. Introduction

Carbon nanotubes (CNTs) [1][2] have excellent mechanical characteristics such as high tensile strength and high elastic modulus, and also possess high thermal and electrical conductivity. Therefore, research into the practical applications of carbon nanotubes has been expanding into wide field, and composite materials of such nano-sized filler materials, such as polymer/CNT composites, have been studied expecting their innovative functions. Metal/CNT composites also have been investigated to enhance properties of metals and/or to give new innovative functions to metals. However, in general, the wettability of molten metals against CNTs is poor, resulting in difficulties of controlling the interface between the filler and matrix. In addition, since CNTs are nanosized fibrous materials and easily form aggregates, it is very difficult to form a metal/CNT composite with well-distributed CNTs in the metal matrix.
Electrochemical deposition is roughly classified into electrodeposition and electroless deposition, and the fabrication processes of metal/CNT composites by the electrochemical deposition can be categorized into three types: (1) composite plating by electrodeposition or electroless deposition, (2) CNT coating by electroless deposition, and (3) electrodeposition using CNT templates (Figure 1). “Composite plating” is one of the electrochemical deposition techniques. CNTs are incorporated in deposited metal matrix during plating. In the case of “metal coating on CNTs by electroless deposition”, the prepared metal-coated CNTs are mainly used as filler of composites, such as resin composites. In the case of “electrodeposition on CNT templates”, CNT yarns or CNT sheets are used as CNT templates. The electrochemical deposition is a nano-scale or atomic scale process to fabricate metal materials and hence is effective to form atomic scall boundary between metals and CNTs. Moreover, this method is a wet process and consequently is likely advantageous to form metal/CNT composites with well-distributed CNTs in the metal matrix, especially in the case of the composite plating.
Electrochem 02 00036 g001 550
Figure 1. Classification of fabrication process for metal/CNT composites by electrochemical deposition.

2. Fabrication of Metal/CNT Composites Using Composite Plating by Electrodeposition or Electro Less Deposition

2.1. Composite Plating

Rough schematics of composite plating by electrodeposition and electroless deposition are displayed in Figure 2 and Figure 3, respectively. In the case of electrodeposition, inert particles are dispersed homogeneously in a plating bath. When a voltage is applied, metal is electrodeposited on a cathode and the particles adsorb on the surface of the deposited metal. Then, the particles are embedded in depositing metal, resulting in a metal composite (Figure 2). In the case of CNT composite plating by electrodeposition, inert particles are dispersed homogeneously in a plating bath containing a reducing agent. When a substrate is soaked in the bath, metal is reductively deposited on the substrate accepting electrons from the reducing agent and, at the same time, the particles adsorb on the surface of the deposited metal. The particles are then embedded in depositing metal, resulting in a metal composite (Figure 3). In general, the substrate is pre-treated and catalyst particles, such as Pd particles, are fixed on the surface of the substrate before soaking into the plating bath. As far as was searched, the first article of the composite plating is on Cu/graphite composites by electrodeposition and was reported in 1928 [3]. Regarding the mechanism of the composite plating, several models have been proposed [4][5][6][7][8].

Electrochem 02 00036 g003 550
Figure 2. Schematic of composite plating by electrodeposition.
Electrochem 02 00036 g004 550
Figure 3. Schematic of composite plating by electroless deposition.

2.2. Preparation of Plating Bath for Metal/CNT Composite Plating

To fabricate metal/CNT composites with uniform distribution of CNTs, the preparation of plating baths with homogeneous dispersion of CNTs is important. In general, plating baths are aqueous solutions, while CNTs are hydrophobic. Therefore, hydrophilization of CNTs have been examined by the addition of surfactants or the direct introduction of hydrophilic groups on the surfaces of CNTs (Figure 4). The addition of surfactants in plating baths is a common method. Various kinds of surfactants [9][10][11][12][13][14][15][16][17][18][19][20][21][22][23][24][25][26], such as sodium dodecylbenzene sulfonate and sodium deoxycholate, have been examined for the homogeneous dispersion of CNTs in a pure water. However, effective surfactants for the dispersion in a pure water are not always effective in plating baths which contain great amounts of ions. Moreover, even if the surfactant is effective for the dispersion of CNTs in a plating bath, CNTs are not always co-deposited by electrochemical deposition. Therefore, the selection of appropriate surfactants is essential. Since the surfactants are likely incorporated in deposited metal matrix during electrochemical deposition, the concentration of surfactants should be examined. On the contrary, the direct introduction of hydrophilic groups, such as -COOH, onto the surfaces of CNTs has been examined using a chemical treatment [27], a plasma treatment [28], a heat treatment [29], and so on. These methods destroy the sp2 carbon bonding of the surfaces of CNTs. Therefore, the conditions of the treatments should be examined.

Electrochem 02 00036 g005 550
Figure 4. Schematic of hydrophilization of CNTs.
On the contrary, CNTs are nanosized fibrous material and consequently tend to aggregate. In particular, SWCNTs have the thinnest (ca. 1–4 nm in diameter) among the various types of CNTs and can thus easily form aggregates referred to as bundles (Figure 5).
Electrochem 02 00036 g006 550
Figure 5. TEM image of SWCNT bundle.

2.3. Unique Feature of Composite Plating Using CNTs as Inert Particles

Since a single CNT, especially multi-walled CNT (MWCNT) has a fibrous shape with large aspect ratio in addition to a high electrical conductivity in the axis direction. Therefore, composite plating using CNTs as inert particles often shows a unique feature unlike other composite plating using insulation particles such as Al2O3 particles. The schematic of the unique feature is showed in Figure 6 [30]. When a part of a MWCNT is incorporated in the deposited metal matrix during electrodeposition, the metal can be electrodeposited not only on the deposited metal but also on the protruding edge (a defect site) of the MWCNT. If the defect sites exist on the sidewall of the MWCNT, the metal can also be electrodeposited on the defect sites.

Electrochem 02 00036 g007 550
Figure 6. Schematic of unique phenomenon of composite plating using MWCNTs as inert particles. (Figure 6 is adapted from reference [30]).
Using this unique phenomena, powder Cu/MWCNT composites could be obtained [31]. Figure 7a displays the surface morphology of Cu/MWCNT composites just after the electrodeposition. Many Cu/MWCNT composites particles are seen. These particles are fixed loosely on the cathode substrate and can be separated easily by ultrasonification. Figure 7b displays the morphology of the Cu/MWCNT composite powder after the separation from the substrate by ultrasonification. A large number of MWCNTs stick out from the Cu particles, resulting in a sea urchin shape. The size of the Cu spheres is 2–15 μm.
Electrochem 02 00036 g008 550
Figure 7. SEM images of (a) Cu/MWCNT composite immediately after electrodeposition and (b) Cu/MWCNT composite powder separated by ultrasonification. (Figure 8 is adapted from reference [31]).

2.4. Fabrication of Metal/CNT Composites Using Composite Plating by Electrodeposition

Fabrication conditions in these articles are listed in Table 1.

Table 1. Fabrication conditions of metal/CNT composites using composite plating by electrodeposition.
Metal CNT Treatment of CNT Base Plating Bath Surfactant Remarks Year Ref.
Ni MWCNT Chemical treatment Dull Watts bath Sodium lauryl sulfate Corrosion behavior 2020 [32]
Ni MWCNT Chemical treatment Dull Watts bath Sodium lauryl sulfate Corrosion protection 2020 [33]
Ni MWCNT Wrapped by polydopamine Dull Watts bath Non Wear and corrosion resistance 2019 [34]
Ni MWCNT Non Ionic liquid (choline chloride/carbamide) Non Non-aqueous solvent 2017 [35]
Ni MWCNT Non Sulfamate bath Cationic surfactant, compound name is unknown Improvement in tool life 2014 [36]
Ni MWCNT Non NiSO4+NaCl Polyvinylpyrrolidone Cyclic voltametric route 2011 [37]
Ni MWCNT Ball milling Bright Watts bath Sodium lauryl sulfate and
Hydroxypropylcellulose		 Corrosion behavior 2011 [38]
Ni MWCNT Chemical treatment Choline chloride/urea Non Non-aqueous solvent 2010 [39]
Ni MWCNT Non Bright Watts bath Polyacrylic acid Solid lubrication 2008 [40]
Ni MWCNT Ball milling Watts type bath Sodium lauryl sulfate, Cetyltrimethylammonium bromide Effects of surfactants 2008 [41]
Ni MWCNT Chemical treatment Dull Watts bath Non Effects of current density 2008 [42]
Ni MWCNT Ball milling Bright Watts bath Sodium lauryl sulfate and
Hydroxypropylcellulose		 Mechanical properties 2008 [43]
Ni MWCNT Non Bright Watts bath Non Mechanical properties 2008 [44]
Ni MWCNT Non Bright Sulfamate bath Polyacrylic acid Low internal stress 2007 [45]
Ni MWCNT Non Dull Watts bath Non Pulse-reverse parameter 2007 [46]
Ni MWCNT Non Bright Watts bath Polyacrylic acid Thermal conductivity 2006 [47]
Ni MWCNT Non Dull Watts bath Poly(diallyldimethylammonium chrolide) Pulse-reverse electrodeposition 2005 [48]
Ni MWCNT Chemical treatment Dull Watts bath Cetyltrimethylammonium bromide Corrosion behavior 2005 [49]
Ni MWCNT Non Dull Watts bath Polyacrylic acid Ni deposition on incorporated CNT 2004 [30]
Ni MWCNT Ball milling Dull Watts bath Non CNT content 2002 [50]
Ni MWCNT Ball milling Dull Watts bath Non Tribological property 2001 [51]
Ni-Co MWCNT Chemical treatment Dull Watts bath
+ Co salt		 Non Corrosion behavior 2019 [52]
Ni-P MWCNT Non Dull Watts bath + citric acid + P compound Polyacrylic acid Tribological properties 2010 [53]
Ni-Co MWCNT Non Dull Watts bath + Co salt Compound name is
unknown		 Mechanical and tribological properties 2006 [54]
Ni-P MWCNT Non Ni salts + citric acid + P compounds Compound name is
unknown		 Corrosion properties 2004 [55]
Cu MWCNT Chemical treatment Citric bath Non Corrosion behavior 2021 [56]
Cu MWCNT Chemical treatment Sulfate bath Non Pulse reverse, electrical conductivity 2020 [57]
Cu MWCNT Chemical treatment? Sulfate bath Non-ionic surfactants, Compound name is unknown Mechanical properties, Microlaminated structure 2020 [58]
Cu SWCNT Non Sulfate bath Stearyltrimethylammonium chloride Mechanical properties 2020 [59]
Cu SWCNT Non Sulfate bath Non Microstructure 2019 [60]
Cu MWCNT Non Sulfate bath Sodium lauryl sulfate Jet electrodeposition,
Tribological properties		 2019 [61]
Cu MWCNT Non Sulfate bath Polyacrylic acid Current collector for LIB anode 2019 [62]
Cu MWCNT Chemical treatment Sulfate bath Stearyltrimethylammonium bromide Electrical conductivity, Corrosion resistance 2018 [63]
Cu MWCNT Non Sulfate bath Non-ionic surfactants, Compound name is unknown Mechanical properties, Laminated structure 2018 [64]
Cu MWCNT Chemical treatment Sulfate bath Non Cu/CNT powder + powder metallurgy 2018 [65]
Cu MWCNT Chemical treatment Sulfate bath Non Cu/CNT powder + powder metallurgy 2018 [66]
Cu MWCNT Chemical treatment Sulfate bath Non Cu/CNT powder + powder metallurgy 2017 [67]
Cu MWCNT Chemical treatment Commercially available Nano diamond Periodic pulse reverse electrodeposition 2016 [68]
Cu MWCNT Non Sulfate bath Polyacrylic acid Current collector for LIB anode 2016 [69]
Cu MWCNT Non Sulfate bath Polyacrylic acid Co-deposition mechanism of CNT 2013 [70]
Cu MWCNT Non Sulfate bath Non Electrochemical reduction behavior 2011 [71]
Cu MWCNT Non Sulfate bath Polyacrylic acid Pulse-reverse 2011 [72]
Cu MWCNT Non Sulfate bath Polyacrylic acid Surface morphology, Hardness, Internal stress 2010 [73]
Cu MWCNT Non Sulfate bath Polyacrylic acid Patterned field emitter 2008 [74]
Cu SWCNT Non Sulfate bath Commercial products Mechanical properties 2008 [75]
Cu SWCNT Chemical treatment Sulfate bath Cetyltrimethylammonium chloride Mechanical properties 2008 [76]
Cu Cup-stacked CNT Non Sulfate bath Polyacrylic acid Various CNTs 2005 [77]
Cu MWCNT Non Sulfate bath Polyacrylic acid Microstructure 2004 [78]
Cu MWCNT Non Sulfate bath Polyacrylic acid Cu/MWCNT composite powder 2003 [31]
Zn MWCNT Chemical treatment Sulfate bath Cetyltrimethylammonium bromide Corrosion resistance 2021 [79]
Zn MWCNT Non Zincate bath Unknown Pulse electrodeposition, Corrosion resistance 2020 [80]
Zn MWCNT Chemical treatment Sulfate bath Cetyltrimethylammonium bromide Corrosion resistance 2007 [81]
Zn-Ni MWCNT Non Chloride bath Non Pulse reverse, Tribological and Corrosion properties 2016 [82]
Cr MWCNT Non Trivalent Cr bath Sodium lauryl sulfate Tribological properties,
Corrosion resistance		 2020 [83]
Cr MWCNT Non Trivalent Cr bath Sodium lauryl sulfate Tribological properties 2018 [84]
Cr MWCNT Non Trivalent Cr bath Non Mechanical properties 2009 [85]
Co MWCNT Non Choline chloride/urea Non Non-aqueous solvent 2017 [86]
Co MWCNT Non Sulfate bath Polyacrylic acid Field emission properties 2013 [87]
Co MWCNT Non Sulfate bath Polyacrylic acid Tribological properties 2013 [88]
Co MWCNT Acid-treatment Sulfate bath + citrate Sodium lauryl sulfate Tribological properties, Corrosion properties 2013 [89]
Co-W MWCNT Non Co salt + Tungstate + Citrate Polyacrylic acid Tribological properties
Corrosion properties		 2015 [90]
Co-W MWCNT Non Co salt + Tungstate + Citrate Polyacrylic acid Tribological properties 2013 [91]
Au MWCNT Non Sulfite bath Stearyltrimethylammonium chloride Electrical conductivity, Tribological properties 2009 [92]
Ag MWCNT Non Choline chloride + glycerol Poly (N-vinyl pyrrolidone) Pulse reverse electrodeposition 2021 [93]
Ag MWCNT Non Iodide bath Non Electrical contact resistance against H2S gas 2021 [94]
Ag MWCNT Non Iodide bath Non Hardness, Electrical and Tribological properties 2020 [95]
Ag MWCNT Non Cyanide bath Unknown Electrical contact resistance against H2S gas 2010 [96]
Al MWCNT Acid treatment Diethylene glycol dimethyl ether Non Hardness 2020 [97]
Al MWCNT Non 1-ethyl-3-methylimidazolium chloride Non Hardness 2006 [98]
Sn MWCNT Non Choline chloride + ethylene glycole Non Nucleation study 2019 [99]
Pb-Sn MWCNT Acid treatment Fluoroborate bath Polyacrylic acid Corrosion resistance 2010 [100]

2.5. Fabrication of Metal/CNT Composites Using Composite Plating by Electroless Deposition

Regarding the number of published articles on metal/CNT composite plating using electroless deposition, those on the Ni-P alloy/CNT is large. In the case of electroless deposition of Ni, phosphorous compounds such as sodium hypophosphite (NaH2PO2) are usually used as the reducing agent and the P derived from the NaH2PO2 is co-deposited with Ni, resulting in Ni-P alloy deposit. Most of the purpose of the fabrication of Ni-P alloy/CNT composites is the improvement of tribological properties. Fabrication conditions in these articles are listed in Table 2.

Table 2. Fabrication conditions of metal/CNT composites by electroless deposition.
Metal CNT Pre-Treatment of CNT Reducing Agent Surfactant Remarks Year Ref.
Ni-P MWCNT Non NaH2PO2 Sodium lauryl sulfate Tribological properties,
Corrosion resistance		 2021 [101]
Ni-P MWCNT Ball milling NaH2PO2 Cetyltrimethylammonium bromide Tribological properties 2012 [102]
Ni-P MWCNT Ball milling,
Chemical treatment		 NaH2PO2 Commercial product Tribological properties,
Corrosion resistance		 2012 [103]
Ni-P MWCNT Chemical treatment Ball milling NaH2PO2 Sodium lauryl sulfate Mechanical attrition, Tribological properties 2012 [104]
Ni-P MWCNT HNO3 Commercial product Commercial product Substrate: Mg powder 2011 [105]
Ni-P MWCNT Non NaH2PO2 Stearyltrimethylammonium chloride Substrate: ABS resin
Tribological properties		 2011 [106]
Ni-P MWCNT Non NaH2PO2 Stearyltrimethylammonium chloride Various P content,
Tribological properties		 2010 [107]
Ni-P MWCNT Chemical treatment NaH2PO2 Unknown Effects on solder joint 2009 [108]
Ni-P MWCNT Chemical treatment NaH2PO2 Cetyltrimethylammonium bromide Tribological properties 2009 [109]
Ni-P MWCNT Chemical treatment NaH2PO2 unknown Tribological properties 2006 [110]
Ni-P MWCNT Ball milling NaH2PO2 Compound name is unknown Hardness,
Corrosion resistance		 2005 [111]
Ni-P SWCNT Heat treatment NaH2PO2 Compound name is unknown Tribological properties 2004 [112]
Ni-P MWCNT Ball milling NaH2PO2 Cetyltrimethylammonium bromide Tribological properties 2003 [113]
Ni-P MWCNT Ball milling NaH2PO2 Cetyltrimethylammonium bromide Tribological properties 2003 [114]
Ni-P MWCNT Ball milling NaH2PO2 Cetyltrimethylammonium bromide Tribological properties 2002 [115]
Cu SWCNT Non CHOCOOH Sodium lauryl sulfate
Hydroxypropylcellulose		 Mechanical disintegration, 2016 [116]
Cu MWCNT Non CHOCOOH Sodium lauryl sulfate
Hydroxypropylcellulose		 Various CNTs
Tribological properties		 2014 [117]
Co-P MWCNT Non NaH2PO2 Non Magnetic properties 2016 [118]

3. Metal-Coated CNTs by Electroless Deposition

3.1. Fabrication Process

A fabrication process of metal-coated CNTs by an autocatalytic electroless deposition is schematically showed in Figure 13. Even in the case of electroless deposition, homogeneous dispersion of CNTs in the plating bath is important. The introduction of functional groups on the surface of CNTs likely effective to increase deposition sites, resulting in CNTs coated by metal films and not metal particles.

3.2. Metal-Coated CNTs

Fabrication conditions in these articles are listed in Table 3.

Table 3. Fabrication conditions of metal-coated CNTs by electroless deposition.
Metal CNT Pre-Treatment of CNT Reducing Agent Surfactant Remarks Year Ref.
Ni-P MWCNT Sn2+sensitization +
Pd2+activation		 NaH2PO2 Non Microstructure, Co-coated CNTs 2020 [119]
Ni-P MWCNT Introduction of -COOH on CNT + Pd2+ NaH2PO2 Non EMI properties, Cotton fabric substrate 2020 [120]
Ni-P MWCNT Sn2+sensitization +
Pd2+activation		 NaH2PO2 Non Arc discharge synthesized CNTs 2015 [121]
Ni-P MWCNT Sn2+/Pd2+ commercial product NaH2PO2 Non Fe-50Co composites, magnetic properties 2014 [122]
Au/Ni-P MWCNT Sn2+sensitization +
Pd2+activation		 NaH2PO2 Polyacrylic acid
(Pre-treatment)		 Improved wettability with molten Al 2012 [123]
Fe-B/Ni-P MWCNT Sn2+sensitization +
Pd2+activation		 NaH2PO2, KBH4 Non Microwave absorbing properties 2011 [124]
Ni-P SWCNT Sn2+sensitization +
Pd2+activation		 NaH2PO2 Non Microstructure of Ni-layer 2011 [125]
Ni-B MWCNT Sn2+sensitization +
Pd2+activation		 (CH3)2NH·BH3 Polyacrylic acid
(Pre-treatment)		 Graphitized MWCNTs
Heat treatment		 2011 [126]
Ni MWCNT Sn2+sensitization +
Pd2+activation		 N2H4 Polyacrylic acid
(Pre-treatment)		 Graphitized MWCNTs
Magnetic properties		 2010 [127]
Ni-P MWCNT K2Cr2O7+H2SO4
Sn2+sensitization +
Pd2+activation		 NaH2PO2 Non Microwave absorbing properties, Ni-N alloy 2008 [128]
Ni-P MWCNT HNO3
Sn2+sensitization +
Pd2+activation		 NaH2PO2 Diallyl-dimethylammonium chloride Graphitized MWCNTs 2005 [129]
Ni-P MWCNT Sn2+sensitization +
Pd2+activation		 NaH2PO2 Polyacrylic acid
(Pre-treatment)		 Graphitized MWCNTs 2004 [130]
Ni-P MWCNT Sn2+sensitization +
Pd2+activation		 NaH2PO2 Non Continuous Ni-layer 2002 [131]
Ni-P MWCNT Mixed Pd2+/Sn2+ NaH2PO2 Non Pd-coated CNTs 1999 [132]
Ni-P MWCNT Sn2+sensitization +
Pd2+activation		 NaH2PO2 Non Magnetic property 1997 [133]
Al MWCNT Sn2+/Pd2+ commercial product LiAlH4 Non Non-aqueous bath: AlCl3-urea 2020 [134]
Ag MWCNT H2SO4 + HNO3
Sn2+sensitization +
Pd2+activation		 HCHO Non Interfacial adhesion of composites 2004 [135]
Cu MWCNT Sulphoric acid + HNO3
Sn2+sensitization +
Cu2+activation		 HCHO Non Electrical and mechanical properties 2009 [136]
Cu MWCNT HNO3
Sn2+sensitization +
Pd2+activation HNO3		 CHOCOOH Diallyl-dimethylammonium chloride Graphitized MWCNTs 2004 [137]
Co-P MWCNT K2Cr2O7+H2SO4
Sn2+sensitization +
Pd2+activation		 NaH2PO2 Non Heat-treatment 2000 [138]

4. Metal/CNT Composites by Electrodeposition Using CNT Templates (Sheet, Yarn)

CNT templates, such as CNT sheets [139][140][141][142] and CNT yarns or fibers [143][144][145][146], have been developed and their various practical applications have been researched. Although a single CNT has a high electrical conductivity, electrical conductivities of those templates are far less than metals such as Cu, due to the contact resistance between each CNT of which they consist. Therefore, metallization of the CNT templates is a promising process to give them enough electrical conductivity. On the contrary, CNTs have strong anisotropy in electrical and thermal properties [147]. Therefore, the orientation of CNTs which make up the templates is also important in order to achieve the expected properties of metal/CNT composites. Fabrication conditions in these articles are listed in Table 4.

Table 4. Fabrication conditions of Metal/CNT Composites by Electrodeposition using CNT Template.
CNT Template Feature of CNT
Template		 Metal Plating Bath Remarks Year Ref.
MWCNT film Super-aligned Cu, Ni Acid sulfuric bath + glucose
Dull Watts Bath		 Improved mechanical and electrical properties 2019 [148]
MWCNT film Super-aligned Ni Dull Watts Bath Improved mechanical properties 2019 [149]
SWCNT paper
(Bucky paper)		 Orientation: in-plane direction Cu Acid sulfate bath + polyethylene glycol + Cl− + bis(3-sulfopropyl) disulfide + Janus green B One-step electrodeposition by a combination of additives 2017 [150]
MWCNT paper Super-aligned Cu Acid sulfuric bath + glucose + polyethylene glycol + Cl−
Alkaline bath (EDTA, Citrate)		 Electrical conductivity 2017 [151]
MWCNT film Super-aligned Cu Acid sulfuric bath + glucose Improved mechanical properties 2016 [152]
MWCNT film Super-aligned Cu Acid sulfuric bath + glucose Improved mechanical properties 2015 [153]
SWCNT yarn Straight Cu Acid sulfate bath Graphen growth on the surface of electrodeposited Cu 2021 [154]
MWCNT yarn Twisted Cu Acid sulfate bath + polyethylene glycol + Cl− + bis(3-sulfopropyl) disulfide + Janus green B One-step electrodeposition by a combination of additives 2020 [155]
CNT yarn Straight Cu Acid sulfate bath Superior current carrying capacity 2018 [156]
MWCNT yarn Twisted Cu (CH3COO)2 + CH3CN
Acid sulfuric bath		 Effect of CNT yarn density 2018 [157]
MWCNT yarn Twisted Cu Cu (CH3COO)2 + CH3CN
Acid sulfuric bath		 Two-step electrodeposition
Uniform composite wire		 2017 [158]
MWCNT yarn Twisted Cu (CH3COO)2 + CH3CN
Acid sulfuric bath		 Two-step electrodeposition
Electrical properties, Solderability,		 2017 [159]
MWCNT yarn Straight Cu Acid sulfuric bath Electrodeposition of Cu interior of CNT yarn 2016 [160]
MWCNT yarn Twisted Ag, Pt KNO3+AgNO3
H2SO4 + H2Pt6Cl6		 Improved tensile strength and electrical conductivity 2013 [161]
MWCNT yarn Twisted Cu Acid sulfuric bath + octyl phenyl poly (ethylene gylcol) ether Continuous process: fiber spinning, anodization, electrodeposition 2011 [162]
MWCNT yarn Twisted Au, Pd, Pt, Cu, Ag, Ni Metal salt solution Self-fueled electrodeposition
Improved electrical conductivity		 2010 [163]

5. Conclusions

The fabrication process can be classified into three types: (1) composite plating by electrodeposition and electroless deposition, (2) metal coating on CNTs by electroless deposition, and (3) electrodeposition using CNT templates. In the composite plating, homogeneous dispersion of CNTs in plating baths is essential and, consequently, various processes, such as the addition of dispersants and introduction of hydrophilic groups on CNTs, have been studied. Numerous articles on Ni/CNT or Ni-P alloy/CNT composites by composite plating have been published and their excellent tribological properties and improved corrosion resistances have been reported. Many papers on Cu/CNT composites have also been published and their properties, such as electrical conductivity, have been investigated. The further elucidation of the mechanism of CNT composite plating process is expected. In the metal coating on CNTs by electroless deposition, the pre-treatments, such as sensitization and activation, are important. Oxidization of CNTs is useful for coating CNTs perfectly. A lot of articles on Ni-P alloy-coated CNTs have been published. In the electrodeposition using CNT templates, many papers on Cu/CNT composites using CNT sheets and CNT yarns have been published and their electrical properties have been reported. The preparation process to deposit Cu not only on the surfaces but also on the interior of CNT templates is likely the key technical point.
The practical applications of these technologies are expected in future work.

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Susumu Arai
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