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

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          Abstract

          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.

          Abstract

          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.

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          Most cited references26

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          Hydrogen Peroxide Synthesis: An Outlook beyond the Anthraquinone Process

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            Self-consistent molecular orbital methods. 21. Small split-valence basis sets for first-row elements

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              Can boron and nitrogen co-doping improve oxygen reduction reaction activity of carbon nanotubes?

              Two kinds of boron and nitrogen co-doped carbon nanotubes (CNTs) dominated by bonded or separated B and N are intentionally prepared, which present distinct oxygen reduction reaction (ORR) performances. The experimental and theoretical results indicate that the bonded case cannot, while the separated one can, turn the inert CNTs into ORR electrocatalysts. This progress demonstrates the crucial role of the doping microstructure on ORR performance, which is of significance in exploring the advanced C-based metal-free electrocatalysts.
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                Author and article information

                Contributors
                emilio.perez@imdea.org
                Journal
                Nat Commun
                Nat Commun
                Nature Communications
                Nature Publishing Group UK (London )
                2041-1723
                10 July 2018
                10 July 2018
                2018
                : 9
                : 2671
                Affiliations
                [1 ]IMDEA Nanociencia, Ciudad Universitaria de Cantoblanco, c/Faraday 9, 28049 Madrid, Spain
                [2 ]ISNI 0000 0001 2157 7667, GRID grid.4795.f, Departamento de Química Inorgánica, , Universidad Complutense de Madrid, ; 28040 Madrid, Spain
                [3 ]ISNI 0000 0001 2284 8430, GRID grid.410892.6, JEOL Ltd, 3-1-2 Musashino, ; Akishima, Tokyo 196-8558 Japan
                Author information
                http://orcid.org/0000-0001-5620-6129
                http://orcid.org/0000-0002-8739-2777
                Article
                5183
                10.1038/s41467-018-05183-8
                6039438
                29991679
                37e7b26b-0f74-48ea-980f-e8cd1805e8f6
                © The Author(s) 2018

                Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/.

                History
                : 18 January 2018
                : 20 June 2018
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