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

Zhang, Wanzheng; Guillen-Soler, Melanie; Silva, Sara Moreno-Da; López‐Moreno, Alejandro; Ruiz‐González, M. Luisa; Giménez, Maria; Lara, David Pérez de

doi:10.1039/d2sc02346f

Cited by 6 publications

(6 citation statements)

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“…In our case, we use a U‐shape precursor constituted by two recognition motifs for SWNT and two terminal alkene functionalities that react forming a structure around the SWNT through a ring‐closing metathesis reaction. Different recognition motifs have been explored by our group, including exTTF, [20a] anthraquinone, [22] pyrene, [23] NDIs, [24] porphyrins, [25] benzophenones and diphenylmethane [26] . These MINTs have demonstrated improved properties with respect to pristine SWNTs or the supramolecular modified SWNTs in different fields such as catalysis, [22,26–27] or, directly related to the present work reinforcing polymers (Figure 1).…”

Section: Introductionmentioning

confidence: 94%

“…Different recognition motifs have been explored by our group, including exTTF, [20a] anthraquinone, [22] pyrene, [23] NDIs, [24] porphyrins, [25] benzophenones and diphenylmethane [26] . These MINTs have demonstrated improved properties with respect to pristine SWNTs or the supramolecular modified SWNTs in different fields such as catalysis, [22,26–27] or, directly related to the present work reinforcing polymers (Figure 1). [28] The mechanical bond exerts an important influence on the mechanical properties of SWNT‐based composites.…”

Section: Introductionmentioning

confidence: 94%

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Mechanical Interlocking to Unlock the Reinforcing Potential of Carbon Nanotubes

Mena-Hernando

Eaton

Fernandéz‐Blázquez

et al. 2023

Chemistry A European J

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Single‐walled carbon nanotubes (SWNTs) present extraordinary mechanical properties, with Youngs’ modulus > 1 TPa and tensile strength > 50 GPa which makes them ideal candidates as fillers for the reinforcement of polymers. However, the performance of SWNTs in this field has fallen behind expectations. This is due to a combination of imperfect individualization of the SWNTs and poor load transfer from the polymer to the SWNTs. Here, we study the reinforcement of polymers of different chemical nature using mechanically interlocked derivatives of single‐walled carbon nanotubes (MINTs). We compare the mechanical properties of fibers made of poly (methyl methacrylate) (PMMA) and polysulfone (PSU) and their composites made with pristine SWNTs, MINTs, and the corresponding supramolecular models. With very low loading of MINTs (0.01% w/w), improvements of more than 100% on Youngs Modulus and the tensile strength are observed for both the nonpolar aliphatic PMMA and the very polar aromatic PSU polymers, while pristine carbon nanotubes and the supramolecular nanofillers showed smaller reinforcement. These data, together with our previous report on the reinforcement of polystyrene (nonpolar and aromatic), indicate that derivatization of SWNTs as MINTs is a valid general strategy to optimize the interaction between SWNT fillers and the polymer matrix.

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Section: Introductionmentioning

confidence: 94%

Section: Introductionmentioning

confidence: 94%

Mechanical Interlocking to Unlock the Reinforcing Potential of Carbon Nanotubes

Mena-Hernando

Eaton

Fernandéz‐Blázquez

et al. 2023

Chemistry A European J

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“…More recently, we have used N-rich macrocycles to wrap SWNTs and enhance their electrocatalytic performance towards ORR. 79…”

Section: Mints As Spectator Linksmentioning

confidence: 99%

Mechanically interlocked derivatives of carbon nanotubes: synthesis and potential applications

2022

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“…These favorable features concerning the various aspects of catalysis thus pave a way to the development of mechanical interlocking as a new paradigm in designing transition metal catalysts. In fact, catenanes and related MIMs are promising scaffolds for catalyst developments, − and other aspects of MIMs such as large-amplitude (co)conformational change and mechanostereochemistry have also been exploited in switchable and stereoselective catalysis. − …”

Section: Introductionmentioning

confidence: 99%

Mechanical Interlocking Enhances the Electrocatalytic Oxygen Reduction Activity and Selectivity of Molecular Copper Complexes

Deng

Lai

et al. 2023

J. Am. Chem. Soc.

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Efficient O2 reduction reaction (ORR) for selective H2O generation enables advanced fuel cell technology. Nonprecious metal catalysts are viable and attractive alternatives to state-of-the-art Pt-based materials that are expensive. Cu complexes inspired by Cu-containing O2 reduction enzymes in nature are yet to reach their desired ORR catalytic performance. Here, the concept of mechanical interlocking is introduced to the ligand architecture to enforce dynamic spatial restriction on the Cu coordination site. Interlocked catenane ligands could govern O2 binding mode, promote electron transfer, and facilitate product elimination. Our results show that ligand interlocking as a catenane steers the ORR selectivity to H2O as the major product via the 4e– pathway, rivaling the selectivity of Pt, and boosts the onset potential by 130 mV, the mass activity by 1.8 times, and the turnover frequency by 1.5 fold as compared to the noninterlocked counterpart. Our Cu catenane complex represents one of the first examples to take advantage of mechanical interlocking to afford electrocatalysts with enhanced activity and selectivity. The mechanistic insights gained through this integrated experimental and theoretical study are envisioned to be valuable not just to the area of ORR energy catalysis but also with broad implications on interlocked metal complexes that are of critical importance to the general fields in redox reactions involving proton-coupled electron transfer steps.

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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...

Cited by 6 publications

References 53 publications

Mechanical Interlocking to Unlock the Reinforcing Potential of Carbon Nanotubes

Mechanical Interlocking to Unlock the Reinforcing Potential of Carbon Nanotubes

Mechanically interlocked derivatives of carbon nanotubes: synthesis and potential applications

Mechanical Interlocking Enhances the Electrocatalytic Oxygen Reduction Activity and Selectivity of Molecular Copper Complexes

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