Defect Etching in Carbon Nanotube Walls for Porous Carbon Nanoreactors: Implications for CO 2 Sorption and the Hydrosilylation of Phenylacetylene.

Autor: Astle MA; School of Chemistry and Nanoscale and Microscale Research Centre (nmRC), University of Nottingham, University Park, Nottingham NG7 2RD, United Kingdom., Weilhard A; School of Chemistry and Nanoscale and Microscale Research Centre (nmRC), University of Nottingham, University Park, Nottingham NG7 2RD, United Kingdom., Rance GA; School of Chemistry and Nanoscale and Microscale Research Centre (nmRC), University of Nottingham, University Park, Nottingham NG7 2RD, United Kingdom., LeMercier TM; School of Chemistry and Nanoscale and Microscale Research Centre (nmRC), University of Nottingham, University Park, Nottingham NG7 2RD, United Kingdom., Stoppiello CT; School of Chemistry and Nanoscale and Microscale Research Centre (nmRC), University of Nottingham, University Park, Nottingham NG7 2RD, United Kingdom., Norman LT; School of Chemistry and Nanoscale and Microscale Research Centre (nmRC), University of Nottingham, University Park, Nottingham NG7 2RD, United Kingdom., Fernandes JA; School of Chemistry and Nanoscale and Microscale Research Centre (nmRC), University of Nottingham, University Park, Nottingham NG7 2RD, United Kingdom., Khlobystov AN; School of Chemistry and Nanoscale and Microscale Research Centre (nmRC), University of Nottingham, University Park, Nottingham NG7 2RD, United Kingdom.
Jazyk: angličtina
Zdroj: ACS applied nano materials [ACS Appl Nano Mater] 2022 Feb 25; Vol. 5 (2), pp. 2075-2086. Date of Electronic Publication: 2022 Feb 07.
DOI: 10.1021/acsanm.1c03803
Abstrakt: A method of pore fabrication in the walls of carbon nanotubes has been developed, leading to porous nanotubes that have been filled with catalysts and utilized in liquid- and gas-phase reactions. Chromium oxide nanoparticles have been utilized as highly effective etchants of carbon nanotube sidewalls. Tuning the thermal profile and loading of this nanoscale oxidant, both of which influence the localized oxidation of the carbon, have allowed the controlled formation of defects and holes with openings of 40-60 nm, penetrating through several layers of the graphitic carbon nanotube sidewall, resulting in templated nanopore propagation. The porous carbon nanotubes have been demonstrated as catalytic nanoreactors, effectively stabilizing catalytic nanoparticles against agglomeration and modulating the reaction environment around active centers. CO 2 sorption on ruthenium nanoparticles (RuNPs) inside nanoreactors led to distinctive surface-bound intermediates (such as carbonate species), compared to RuNPs on amorphous carbon. Introducing pores in nanoreactors modulates the strength of absorption of these intermediates, as they bond more strongly on RuNPs in porous nanoreactors as compared to the nanoreactors without pores. In the liquid-phase hydrosilylation of phenylacetylene, the confinement of Rh 4 (CO) 12 catalyst centers within the porous nanoreactors changes the distribution of the products relative to those observed in the absence of the additional pores. These changes have been attributed to the enhanced local concentration of phenylacetylene and the environment in which the catalytic centers reside within the porous carbon host.
Competing Interests: The authors declare no competing financial interest.
(© 2022 American Chemical Society.)
Databáze: MEDLINE
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