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Varied morphology carbon nanotubes

a carbon nanotube and morphology technology, applied in the field of varied morphology carbon nanotubes, can solve the problems of large quantity, cost-effective production methods, and only providing a uniform flat surface, and achieve the effects of increasing the yield of cnt products, promoting the activity of catalytic substrates, and rapid carbon deposition and cnt growth

Inactive Publication Date: 2008-05-22
TRUSTEES OF BOSTON COLLEGE THE
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Benefits of technology

This approach enables the production of CNTs with controlled morphology and structure in high yields, making them suitable for applications in materials reinforcement, energy storage, and electronic devices, while reducing production costs and overcoming previous synthesis limitations.

Problems solved by technology

A major limitation to their large-scale commercialization however, has remained the need for large quantity, cost-effective production methods.
They however, require relatively expensive and complex reactor apparatus, and typically require a high vacuum (10−5 to 10−7 torr) environment.
Furthermore, such methods are only capable of providing a uniform flat surface layer of the metal catalyst on the substrate on which CNT formation and growth can occur.
Since CNT yield is directly related to surface area of the catalytic surface, substantially large areas of metal coated substrate is required to synthesize large quantities of CNTs, which is impractical in terms of existing limitations of the reaction apparatus.
According to Li et al., preparation of such large area catalytic substrate is hampered by the inherent tendency to shrink, crack and shatter during their preparation.
Imperfect catalyst preparation can severely limit yields of CNT product.
Also, CNT synthesis by the process of Li et al. requires a reaction temperature of 700° C., which is impractical for substrates such as flat panel glass.
Such methods however, require high vacuum conditions, which is difficult to achieve in large reactors in a commercially viable CNT manufacturing processes.
Although such methods are capable of providing highly pure, aligned CNTs, they are not best suited for large-scale production due to low volume (typically several milligrams to grams per batch), low yields based on amount of catalyst and high manufacturing cost.
Furthermore, existing methods do not allow control of nanotube morphology, tubule diameter, tubule wall thickness and other structural elements that are important in achieving desired material properties that may required for specific applications.
Such drawbacks are limiting factors that restrict the widespread use of CNTs in potential applications.
Although it is theoretically possible to introduce a wide range of structural defects with useful electronic properties in CNTs, synthetic limitations have precluded such introduction of systematic structural defects.
Furthermore, currently available methods do not allow controlled alteration of linear tubule structures during their growth.
Post growth modifications of CNTs have been difficult to implement and are prone to uncontrolled and random defects.
The branched Y-shaped CNTs obtained by the method however, are not symmetrical with respect to arm length, straightness and angles between arms, since their shape and symmetry is determined by limitations in fabrication of the aluminum mold in which they are formed.
Such processes are also not suited for large scale manufacture of CNTs and are, therefore, not economically viable for use in a commercial process.

Method used

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Examples

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example 1

Preparation of Catalyst Substrate for Synthesis of Linear CNTs

[0058]Mesoporous silica containing iron nanoparticles were prepared by a sol-gel process by hydrolysis of tetraethoxysilane (TEOS) in the presence of iron nitrate in aqueous solution following the method described by Li et al. (Science, (1996), Vol. 274, 1701-3) with the following modification. The catalyst gel was dried to remove excess water and solvents and calcined for 10 hours at 450° C. and 10−2 torr to give a silica network with substantially uniform pores containing iron oxide nanoparticles that are distributed within. The catalyst gel is then ground into a fine, micro-particulate powder either mechanically using a ball mill or manually with a pestle and mortar. The ground catalyst particles provide particle sizes that range between 0.1 and 100 μM under the grinding conditions.

example 2

Preparation of Catalyst Substrate for Synthesis of Branched CNTs

[0059]Magnesium oxide (MgO) supported cobalt (Co) catalysts were prepared by dissolving 0.246 g of cobalt nitrate hexahydrate (Co(NO3)2.6H2O, 98%) in 40 ml ethyl alcohol, following which immersing 2 g of particulate MgO powder (−325 mesh) were added to the solution with sonication for 50 minutes. The solid residue was filtered, dried and calcined at 130° C. for 14 hours.

example 3

General Synthetic Procedure for Linear CNTs

[0060]The synthesis of CNTs is carried out in a quartz tube reactor of a chemical vapor deposition (CVD) apparatus. For each synthetic run, 100 mg of the micro-particulate catalyst substrate was spread onto a molybdenum boat (40×100 mm2) either mechanically with a spreader or by spraying. The reactor chamber was then evacuated to 10−2 torr, following which the temperature of the chamber was raised to 750° C. Gaseous ammonia was introduced into the chamber at a flow rate of 80 sccm and maintained for 10 minutes, following which acetylene at a flow rate of 20 sccm was introduced for initiate CNT growth. The total gas pressure within the reaction chamber was maintained at a fixed value that ranged from 0.6 torr to 760 torr (depending on desired morphology for the CNTs). The reaction time was maintained constant at 2 hours for each run. The catalytic substrate containing attached CNTs were washed with hydrofluoric acid, dried and weighed prior ...

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Abstract

The present invention describes the preparation of carbon nanotubes of varied morphology, catalyst materials for their synthesis. The present invention also describes reactor apparatus and methods of optimizing and controlling process parameters for the manufacture carbon nanotubes with pre-determined morphologies in relatively high purity and in high yields. In particular, the present invention provides methods for the preparation of non-aligned carbon nanotubes with controllable morphologies, catalyst materials and methods for their manufacture.

Description

RELATED APPLICATIONS[0001]This application is a divisional of U.S. application Ser. No. 10 / 151,382, filed May 20, 2002, which claims priority to U.S. Provisional Application Ser. No. 60 / 292,486, filed on May 21, 2001, and the entirety of these applications are hereby incorporated herein by reference for the teachings therein.STATEMENT AS TO FEDERALLY SPONSORED RESEARCH[0002]The present invention was made with partial support from The US Army Natick Soldier Systems Center (DAAD, Grant Number 16-00-C-9227), Department of Energy (Grant Number DE-FG02-00ER45805) and The National Science Foundation (Grant Number DMR-9996289)FIELD OF THE INVENTION[0003]The present invention relates generally to carbon nanotubes of varied morphology, catalyst materials for their synthesis, and apparatus and methods for controllably manufacturing carbon nanotubes with pre-determined morphologies. More particularly, the present invention concerns non-aligned carbon nanotubes with controllable morphologies, c...

Claims

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Application Information

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Patent Type & Authority Applications(United States)
IPC IPC(8): D01F9/12B01J23/745B01J23/75B01J37/03C01B31/02D01F9/127
CPCB01J23/745B01J23/75B01J37/036Y10S977/843B82Y40/00C01B31/0233D01F9/127B82Y30/00C01B32/162
Inventor LI, WENZHIWEN, JIAN GUOREN, ZHIFENG
Owner TRUSTEES OF BOSTON COLLEGE THE
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