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Acta Metall Sin  2018, Vol. 54 Issue (11): 1665-1682    DOI: 10.11900/0412.1961.2018.00423
Materials and Processes Current Issue | Archive | Adv Search |
A Review on the Controlled Growth of Single-Wall Carbon Nanotubes from Metal Catalysts
Zhonghai JI1,2, Lili ZHANG1,2, Daiming TANG1,2(), Chang LIU1,2, Huiming CHENG1,3
1 Institute of Metal Research, Chinese Academy of Sciences, Shenyang 110016, China
2 School of Materials Science and Engineering, University of Science and Technology of China, Shenyang 110016, China
3 Tsinghua-Berkeley Shenzhen Institute, Shenzhen 518055, China
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Single-wall carbon nanotubes (SWCNTs) with a unique tubular structure have exhibited excellent electrical, thermal and mechanical properties. However, their attractive applications in microelectronic devices and sensors are still pending due to the lack of high-quality, structure-defined SWCNTs. It is still a great challenge to grow pure and ordered SWCNTs with designated structures and properties. The key of breakthrough is to understand the fundamental nucleation and growth mechanism of SWCNTs under reaction conditions. In this article, we analyze the influences of physical and chemical properties, such as electronic structure, melting point, carbon solubility, and diffusivity, of catalyst nanoparticles on the productivity, purity, and fine structures of grown SWCNTs. The progress, current situation, and challenges on the controlled growth of SWCNTs are summarized. Finally, perspectives on future directions are presented and a strategy of structure-controlled production of SWCNTs is proposed.

Key words:  metal catalyst      single-wall carbon nanotube      structure control      growth mechanism     
Received:  08 September 2018     
Fund: Supported by National Natural Science Foundation of China (Nos.51522210, 51802316, 51521091, 51625203), National Key Research and Development Program of China (No.2016YFA0200101) and Hundred Talents Program of Chinese Academy of Sciences

Cite this article: 

Zhonghai JI, Lili ZHANG, Daiming TANG, Chang LIU, Huiming CHENG. A Review on the Controlled Growth of Single-Wall Carbon Nanotubes from Metal Catalysts. Acta Metall Sin, 2018, 54(11): 1665-1682.

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Fig.1  A schematic showing the catalytic reaction, transport, nucleation and growth process of single-wall carbon nanotubes (SWCNTs)
Fig.2  In-situ TEM observations of the nucleation and growth of individual CNTs from Co (a), Fe (b), Au (c) and SiOx (d) catalyst nanoparticles (DWCNT—double-wall carbon nanotube, C'sup(t)—active carbon supply rate, C'inc(t)—carbon incorporation rate, t—time)[31,32,33]
Fig.3  Metal-carbon phase diagrams (T—temperature)[64,77]
(a) Ni-C eutectic phase diagram, red arrows represent vapor-liquid-solid (VLS) growth mechanism; green arrows represent vapor-solid-solid (VSS) growth mechanism
(b) nanoscale Ni-C phase diagram. The melting and eutectic points are dramatically lowered. The carbon solubility is increased and a new phase with fluctuation surface structures appears (xc—atomic fraction of carbon)
(c) Cu-C phase diagram. Carbon solubility is almost 0% in the solid phase
(d) W-C phase diagram, including stable W2C and WC phases. The melting and eutectic points are higher than 2500 ℃, much higher than the growth temperature of CNTs
Fig.4  Types of metal catalysts for SWCNT growth. The melting points are represented by the filled color of the blocks, with blue and red for low and high melting points, respectively. The types of the catalyst are marked by the colors of the frames: Fe group metals (green), Pt group metals (blue), coin metals (red), carbide formation metals (black) and oxide formation metals (purple)[90]
Group Property
Periodic table group Tm
Carbide Ef
Fe-group 8~10 1455~ 1148~ 4~8 Metastable 0.08~0.27[91] -1.4[35] 0.83~1.57[93] High active
(Fe, Co, Ni) 1538 1327 carbon solubility
Pt-group 8~10 1555~ 1400~ <3 Unstable >>0[91] -1.8[35] ~1.37[71] High catalytic
(Ru, Rh, Pt) 2334 1900 activity
Coin-group 11 961~ No ~0.01 Unstable >>0[91] -(0.04~0.6)[35] ~0.9[94] High diffusion
(Cu, Ag, Au) 1084 rate
Carbide-forming 4~7 2600~ 2300~ ~1 Stable -(0.6~1.8) [91] -0.3[92] ~3.0[68] High melting point
group (W, Mo) 3400 2800
Table 1  Property and Characteristics of Metal Catalyst for SWCNTs[35,68,71,91~94]
Fig.5  SWCNTs grown from Fe group metals catalysts[12,21,100,101]
(a) vertical array
(b) horizontal array
(c) semiconductor-enriched SWCNTs
(d) isolated SWCNTs films
Fig.6  SWCNTs grown by coin metals (Au, Cu)[49,51,78]
(a) TEM and SEM images of Au nanoparticles and grown SWCNTs, and PL spectra of SWCNTs grown at different temperatures
(b) growth of SWCNTs network and horizontal array from Cu nanoparticles
Fig.7  SWCNTs grown from bi-metallic catalysts[27,145,146]
(a) growth rates of metallic nanotubes on Ni, Cu and Ni-Cu catalysts
(b) selective growth of (6, 5) and (7, 5) SWCNTs from Co-Mo catalyst
(c) chirality-specific growth of SWCNTs from Co-W catalyst
Fig.8  SWCNTs grown from metal compound catalysts[150,151]
(a) selective growth of metallic or semiconducting SWCNTs by SiOx catalyst. (a1, b1) heating SiOx thin films to form nanoparticles; (c1, d1) relationship between O/Si ratios of SiOx nanoparticles and percentage of grown semiconducting or metallic SWCNTs; (e1, f1) Raman spectra and transistor performance based on metallic and semiconducting SWCNTs
(b) growth of semiconducting SWCNTs by Mo2C (a2), SEM image, Raman spectra, AFM analysis and diameter distribution of Mo2C catalyzed SWCNT arrays (b2~e2)
Group Property
Height Density tubes·μm-1 Length Growth rate μm·s-1 IG/ID Conductivity Chirality richness Feature
μm μm richness
Fe-group 10000[100] 130[102] 100000[157] 22.4[158] 200[11] 91%M[107]/95%S[21]/99.9%S[14] 53%(6, 5)[104] High yield
Pt-group - 5[156] 120[156] 0.13[156] 60[159] 90%S[161] (6, 5)/(7, 5)/(8, 4)[32] High activity
Coin metal - 60[116] 10000[78] 11.11[78] 45[160] 95%S[160, 162] (6, 5)[51] Nonmagnetic
Bimetal-group 36[155] 160[11] 185000[133] 40[133] 141[11] 96%S[13]/95%S[163] 97%(14, 4)[140]/ Chirality
92%(12, 6)[29]/ enriched
80%(16, 0)[139]
Carbide - 20[30] 185[30] 1.54[30] 22[30] 95%S[89]/ 80%(8, 4)/90%(12, 6)[30] Specific symmetry
Oxide - 10[152] 196[152] 0.0083[149] 139[152] 80%M/ - Low growth rate
Table 2  Structure controlled growth of SWCNTs from different catalysts[11,13,14,21,29,30,32,51,78,89,100,102,104,107,116,133,139,140,149~152,155~163]
Fig.9  Properties of metal catalysts: melting points, catalytic activity, carbon solubility and diffusion rate
(a) comparison of properties of different catalyst systems
(b) comparison of the properties of Co and Co alloys. Design strategy of multiple alloy catalyst for optimized growth yield, quality and structural control
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