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金属学报  2018, Vol. 54 Issue (11): 1665-1682    DOI: 10.11900/0412.1961.2018.00423
  材料与工艺 本期目录 | 过刊浏览 |
金属催化剂控制生长单壁碳纳米管研究进展
吉忠海1,2, 张莉莉1,2, 汤代明1,2(), 刘畅1,2, 成会明1,3
1 中国科学院金属研究所 沈阳 110016
2 中国科学技术大学材料科学与工程学院 沈阳 110016
3 清华-伯克利深圳学院 深圳 518055
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
引用本文:

吉忠海, 张莉莉, 汤代明, 刘畅, 成会明. 金属催化剂控制生长单壁碳纳米管研究进展[J]. 金属学报, 2018, 54(11): 1665-1682.
Zhonghai JI, Lili ZHANG, Daiming TANG, Chang LIU, Huiming CHENG. A Review on the Controlled Growth of Single-Wall Carbon Nanotubes from Metal Catalysts[J]. Acta Metall Sin, 2018, 54(11): 1665-1682.

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摘要: 

单壁碳纳米管具有独特的一维管状结构和优异的电学、热学和力学性质。但其在微纳电子、传感器件等领域的应用,仍受限于高品质单壁碳纳米管的可控制备。大规模、高纯度、有序排列、特定手性和导电属性的单壁碳纳米管可控生长仍然是该研究领域的巨大挑战。取得突破的关键在于对单壁碳纳米管生长机理的深刻理解,核心在于对单壁碳纳米管在催化剂上形核与生长过程的有效调控。本文从金属催化剂的电子结构与催化活性、熔点与结构稳定性、碳溶解度和扩散率等角度阐述其对单壁碳纳米管产率、纯度、有序度和精细结构的影响,总结金属催化剂控制生长单壁碳纳米管的研究进展、现状和挑战,展望可控生长的研究策略、设计准则与发展趋势。

关键词 金属催化剂单壁碳纳米管结构控制生长机理    
Abstract

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 wordsmetal catalyst    single-wall carbon nanotube    structure control    growth mechanism
收稿日期: 2018-09-08     
基金资助:国家自然科学基金项目Nos.51522210、51802316、51521091和51625203,国家重点研发计划项目No.2016YFA0200101及中国科学院百人计划A类择优支持、“青年俊才” (C类)
作者简介: 作者简介 吉忠海,男,1991年生,博士生
图1  单壁碳纳米管的催化反应、输运、形核、生长过程示意图
图2  原位TEM观察碳纳米管在Co、Fe、Au、SiOx催化剂颗粒上的形核与生长[31,32,33]
图3  金属-碳二元相图理解碳纳米管生长过程[64,77]
图4  单壁碳纳米管金属催化剂分类[90]
Group Property
Periodic table group Tm
Te
C
%
Carbide Ef
eV
Ea
eV
Ed
eV
Feature
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
表1  金属催化剂体系与物理化学性质特点[35,68,71,91~94]
图5  Fe系金属催化生长和控制单壁碳纳米管[12,21,100,101]
图6  货币金属(Au、Cu)生长单壁碳纳米管[49,51,78]
图7  双金属催化剂生长单壁碳纳米管[27,145,146]
图8  金属化合物催化剂生长单壁碳纳米管[150,151]
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
90%S[151]
Oxide - 10[152] 196[152] 0.0083[149] 139[152] 80%M/ - Low growth rate
91%S[150]
表2  催化剂体系与碳纳米管结构控制进展[11,13,14,21,29,30,32,51,78,89,100,102,104,107,116,133,139,140,149~152,155~163]
图9  生长碳纳米管催化剂的物理化学性质与高效多元合金催化剂设计准则
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