Journal
CCS CHEMISTRY
Volume 3, Issue 11, Pages 154-167Publisher
CHINESE CHEMICAL SOC
DOI: 10.31635/ccschem.020.202000595
Keywords
carbon nanotube; catalysts; chemical vapor deposition; structure evolution; aberration-corrected environmental transmission electron microscopy
Categories
Funding
- National Key Research and Development Program of China [2016YFA0201904, 2018YFA0703700]
- National Natural Science Foundation of China (NSFC) [21631002, 12034002, 51971025]
- Beijing National Laboratory for Molecular Sciences [BNLMS-CXTD202001]
- Shenzhen Basic Research Project [JCYJ20170817113121505]
- Shenzhen KQTD Project [KQTD20180411143400981]
- Fundamental Research Funds for the Central Universities [FRF-BD-18-004A]
- Science and Technology Innovation Committee Foundation of Shenzhen [KQTD2016022619565991, ZDSYS20141118160434515]
- NSFC [52002165]
- Beijing National Laboratory for Molecular Science [BNLMS202013]
- Guangdong Provincial Natural Science Foundation, Innovation Project for Guangdong Provincial Department of Education [2019KTSCX155]
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This study investigated the diffusion of carbon in transition metal catalysts at the atomic level using aberration-corrected environmental transmission electron microscopy and synchrotron X-ray absorption spectroscopy, revealing a cycle of carbon dissolving and precipitating in the catalysts near the nucleation site of single-walled carbon nanotubes. Understanding the dynamics of carbon atoms in catalysts provides deeper insights into the growth mechanisms of SWCNTs and other reactions. The developed methodologies have broad applications in studying catalytic and other processes.
When carbon-containing species are involved in reactions catalyzed by transition metals at high temperature, the diffusion of carbon on or in catalysts dramatically influences the catalytic performance. Acquiring information on the carbon-diffusioninvolved evolution of catalysts at the atomic level is crucial for understanding the reaction mechanism yet also challenging. For the chemical vapor deposition process of single-walled carbon nanotubes (SWCNTs), we recorded in situ the catalyst state (solid and molten) composition as well as near-surface structural and chemical evolution at the cobalt catalyst-tube interface with carbon permeation using aberration-corrected environmental transmission electron microscopy and synchrotron X-ray absorption spectroscopy. The nucleation of SWCNTs was linked with an alternating dissolving and precipitating cycle of carbon in catalysts close to the nucleation site. Understanding the dynamics of carbon atoms in catalysts brings deeper insight into the growth mechanism of SWCNTs and facilitates inferring mechanisms of other reactions. The methodologies developed here will find broad applications in studying catalytic and other processes. [GRAPHICS] .
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