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Positive and negative regulation of carbon nanotube catalysts through encapsulation within macrocycles

One of the most attractive applications of carbon nanomaterials is as catalysts, due to their extreme surface-to-volume ratio. The substitution of C with heteroatoms (typically B and N as p- and n-dopants) has been explored to enhance their catalytic activity. Here we show that encapsulation within...

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Published in:Nature communications 2018-07, Vol.9 (1), p.2671-7, Article 2671
Main Authors: Blanco, Matías, Nieto-Ortega, Belén, de Juan, Alberto, Vera-Hidalgo, Mariano, López-Moreno, Alejandro, Casado, Santiago, González, Luisa R., Sawada, Hidetaka, González-Calbet, José M., Pérez, Emilio M.
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Language:English
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Summary:One of the most attractive applications of carbon nanomaterials is as catalysts, due to their extreme surface-to-volume ratio. The substitution of C with heteroatoms (typically B and N as p- and n-dopants) has been explored to enhance their catalytic activity. Here we show that encapsulation within weakly doping macrocycles can be used to modify the catalytic properties of the nanotubes towards the reduction of nitroarenes, either enhancing it (n-doping) or slowing it down (p-doping). This artificial regulation strategy presents a unique combination of features found in the natural regulation of enzymes: binding of the effectors (the macrocycles) is noncovalent, yet stable thanks to the mechanical link, and their effect is remote, but not allosteric, since it does not affect the structure of the active site. By careful design of the macrocycles’ structure, we expect that this strategy will contribute to overcome the major hurdles in SWNT-based catalysts: activity, aggregation, and specificity. Doping carbon nanomaterials with heteroatoms is the most common way to change their catalytic activity. Here, the authors show that the catalytic properties of single-walled carbon nanotubes can be modified by non-covalently encapsulating them within electron-accepting or electron-donating macrocycles to form rotaxane-like structures.
ISSN:2041-1723
2041-1723
DOI:10.1038/s41467-018-05183-8