Issue 33, 2022

Mechanical interlocking of SWNTs with N-rich macrocycles for efficient ORR electrocatalysis

Abstract

Substitutional N-doping of single-walled carbon nanotubes is a common strategy to enhance their electrocatalytic properties in the oxygen-reduction reaction (ORR). Here, we explore the encapsulation of SWNTs within N-rich macrocycles as an alternative strategy to display electroactive sites on the surface of SWNTs. We design and synthesize four types of mechanically interlocked derivatives of SWNTs (MINTs) by combining two types of macrocycles and two types of SWNT samples. Comprehensive electrochemical characterization of these MINTs and their reference SWNTs allows us to establish structure–activity relationships. First, we show that all MINT samples are superior electrocatalysts compared to pristine SWNTs, which serves as general validation of our strategy. Secondly, we show that macrocycles displaying both N atoms and carbonyl groups perform better than those with N atoms only. Finally, we demonstrate that a tighter fit between macrocycles and SWNTs results in enhanced catalytic activity and stability, most likely due to a more effective charge-transfer between the SWNTs and the macrocycles. These results, focusing on the ORR as a testbed, show the possibility of understanding electrocatalytic performance of SWNTs at the molecular level and thus enable the design of more active and more stable catalysts in the future.

Graphical abstract: Mechanical interlocking of SWNTs with N-rich macrocycles for efficient ORR electrocatalysis

Supplementary files

Article information

Article type
Edge Article
Submitted
26 Apr 2022
Accepted
23 Jul 2022
First published
25 Jul 2022
This article is Open Access

All publication charges for this article have been paid for by the Royal Society of Chemistry
Creative Commons BY-NC license

Chem. Sci., 2022,13, 9706-9712

Mechanical interlocking of SWNTs with N-rich macrocycles for efficient ORR electrocatalysis

W. Zhang, M. Guillén-Soler, S. Moreno-Da Silva, A. López-Moreno, L. R. González, M. D. C. Giménez-López and E. M. Pérez, Chem. Sci., 2022, 13, 9706 DOI: 10.1039/D2SC02346F

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