[Germination et croissance des nanotubes monofeuillets : études par microscopie électronique en transmission du rôle du catalyseur]
This paper reviews transmission electron microscopy studies, combining high resolution imaging and electron energy loss spectroscopy, of the nucleation and growth of carbon single wall nanotubes with a particular emphasis on the nanotubes obtained from the evaporation-based elaboration techniques. Inspection of samples obtained from different synthesis routes shows that in all cases nanotubes are found to emerge from catalyst particles and that they have grown perpendicular or parallel to the surface according to whether they have been synthesized via evaporation-based methods or CCVD methods. Whereas the latter case corresponds to the well-known situation of carbon filaments growth, the former case strongly suggests another formation and growth process, which is described and its different steps discussed in detail. In this model, formation of the nanotubes proceeds via solvation of carbon into liquid metal droplets, followed by precipitation, at the surface of the particles, of excess carbon in the form of nanotubes through a nucleation and root growth process. It is argued that the nucleation of the nanotubes, which compete with the formation of graphene sheets wrapping the surface of the particle, necessarily results from a surface instability induced by the conditions of segregation. The nature and the origin of this instability was studied in the case of the class of catalyst Ni–R.E. (R.E.=Y, La, Ce, …) in order to identify the influence of the nature of the catalyst. The respective roles played by Ni and R.E. have been identified. It is shown that carbon and rear-earth co-segregate and self-assemble at the surface of the particle in order to form a surface layer destabilizing the formation of graphene sheets and providing nucleation sites for nanotubes growing perpendicular to the surface.
Cet article présente une revue des études, par microscopie électronique en transmission, couplant imagerie de haute résolution et spectroscopie de pertes d'énergie d'électrons, de la germination et de la croissance des nanotubes de carbone simple feuillet, avec un développement particulier pour les tubes obtenus par les techniques de synthèse mettant en jeu la vaporisation d'une cible. L'examen d'échantillons provenant de différentes voies de synthèse montre que, dans tous les cas, les nanotubes émergent de particules catalytiques et qu'ils ont crû perpendiculairement ou parallèlement à la surface selon qu'ils ont été synthétisés par des méthodes mettant en jeu la vaporisation d'une cible ou des méthodes de type CCVD. Alors que le dernier cas correspond à la situation bien connue de la croissance des filaments de carbone, le premier cas suggère fortement un autre procédé de formation et de croissance, qui est décrit et ces différentes étapes discutées en détail. Dans ce modèle, la formation des tubes s'effectue par dissolution de carbone dans des gouttes de métal liquide, suivie de la précipitation, à la surface des particules, du carbone en excès sous la forme de nanotubes par un mécanisme de nucléation et de croissance par le pied. Il est démontré que la nucléation des nanotubes, qui est en compétition avec la formation de feuillets de graphène couvrant la surface de la particule, provient nécessairement d'une instabilité de surface induite par les conditions de ségrégation. La nature et l'origine de cette instabilité a été étudiée dans le cas de la classe de catalyseurs Ni–R.E. (R.E.=Y, La, Ce…) afin d'identifier l'influence de la nature du catalyseur. Les rôles respectifs joués par le Ni et la terre rare ont été identifiés. Il est montré que le carbone et la terre rare co-ségrègent et s'auto-assemblent à la surface de la particule de façon à former une couche de surface qui déstabilise la formation de feuillets de graphène et qui est source de sites de nucléation pour des nanotubes croissant perpendiculairement à la surface.
Annick Loiseau 1 ; Julie Gavillet 1 ; François Ducastelle 1 ; Jany Thibault 2 ; Odile Stéphan 3 ; Patrick Bernier 4 ; Saı̈d Thair 4
@article{CRPHYS_2003__4_9_975_0,
author = {Annick Loiseau and Julie Gavillet and Fran\c{c}ois Ducastelle and Jany Thibault and Odile St\'ephan and Patrick Bernier and Sa{\i}\ensuremath{\ddot{}}d Thair},
title = {Nucleation and growth of {SWNT:} {TEM} studies of the role of the catalyst},
journal = {Comptes Rendus. Physique},
pages = {975--991},
publisher = {Elsevier},
volume = {4},
number = {9},
year = {2003},
doi = {10.1016/j.crhy.2003.10.022},
language = {en},
}
TY - JOUR AU - Annick Loiseau AU - Julie Gavillet AU - François Ducastelle AU - Jany Thibault AU - Odile Stéphan AU - Patrick Bernier AU - Saı̈d Thair TI - Nucleation and growth of SWNT: TEM studies of the role of the catalyst JO - Comptes Rendus. Physique PY - 2003 SP - 975 EP - 991 VL - 4 IS - 9 PB - Elsevier DO - 10.1016/j.crhy.2003.10.022 LA - en ID - CRPHYS_2003__4_9_975_0 ER -
%0 Journal Article %A Annick Loiseau %A Julie Gavillet %A François Ducastelle %A Jany Thibault %A Odile Stéphan %A Patrick Bernier %A Saı̈d Thair %T Nucleation and growth of SWNT: TEM studies of the role of the catalyst %J Comptes Rendus. Physique %D 2003 %P 975-991 %V 4 %N 9 %I Elsevier %R 10.1016/j.crhy.2003.10.022 %G en %F CRPHYS_2003__4_9_975_0
Annick Loiseau; Julie Gavillet; François Ducastelle; Jany Thibault; Odile Stéphan; Patrick Bernier; Saı̈d Thair. Nucleation and growth of SWNT: TEM studies of the role of the catalyst. Comptes Rendus. Physique, carbon nanotubes: state of the art and applications, Volume 4 (2003) no. 9, pp. 975-991. doi : 10.1016/j.crhy.2003.10.022. https://comptes-rendus.academie-sciences.fr/physique/articles/10.1016/j.crhy.2003.10.022/
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