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1.
Nanoscale ; 16(4): 2048-2059, 2024 Jan 25.
Artigo em Inglês | MEDLINE | ID: mdl-38204411

RESUMO

Both at the academic and the industrial level, material scientists are exploring routes for mass production and functionalization of graphene, carbon nanotubes (CNT), carbon dots, 2D materials, and heterostructures of these. Proper application of the novel materials requires fast and thorough characterization of the samples. Raman spectroscopy stands out as a standard non-invasive technique capable of giving key information on the structure and electronic properties of nanomaterials, including the presence of defects, degree of functionalization, diameter (in the case of CNT), different polytypes, doping, etc. Here, we present a computational tool to automatically analyze the Raman spectral features of nanomaterials, which we illustrate with the example of CNT and graphene. The algorithm manages hundreds of spectra simultaneously and provides statistical information (distribution of Raman shifts, average values of shifts and relative intensities, standard deviations, correlation between different peaks, etc.) of the main spectral features defining the structure and electronic properties of the samples, as well as publication-ready graphical material.

2.
Chem Sci ; 13(33): 9706-9712, 2022 Aug 24.
Artigo em Inglês | MEDLINE | ID: mdl-36091908

RESUMO

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.

3.
Front Pharmacol ; 13: 920379, 2022.
Artigo em Inglês | MEDLINE | ID: mdl-36034868

RESUMO

In this study, we present the synthesis, kinetic studies of inhibitory activity toward aldo-keto reductase 1C (AKR1C) enzymes, and anticancer potential toward chemoresistant ovarian cancer of 10 organoruthenium compounds bearing diketonate (1-6) and hydroxyquinolinate (7-10) chelating ligands with the general formula [(η6-p-cymene)Ru(chel)(X)]n+ where chel represents the chelating ligand and X the chlorido or pta ligand. Our studies show that these compounds are potent inhibitors of the AKR enzymes with an uncommon inhibitory mechanism, where two inhibitor molecules bind to the enzyme in a first fast and reversible step and a second slower and irreversible step. The binding potency of each step is dependent on the chemical structure of the monodentate ligands in the metalloinhibitors with the chlorido complexes generally acting as reversible inhibitors and pta complexes as irreversible inhibitors. Our study also shows that compounds 1-9 have a moderate yet better anti-proliferative and anti-migration action on the chemoresistant ovarian cancer cell line COV362 compared to carboplatin and similar effects to cisplatin.

4.
Angew Chem Int Ed Engl ; 61(35): e202208189, 2022 Aug 26.
Artigo em Inglês | MEDLINE | ID: mdl-35789180

RESUMO

Mechanically interlocked derivatives of carbon nanotubes (MINTs) are interesting nanotube products since they show high stability without altering the carbon nanotube structure. So far, MINTs have been synthesized using ring-closing metathesis, disulfide exchange reaction, H-bonding or direct threading with macrocycles. Here, we describe the encapsulation of single-walled carbon nanotubes within a palladium-based metallosquare. The formation of MINTs was confirmed by a variety of techniques, including high-resolution transmission electron microscopy. We find the making of these MINTs is remarkably sensitive to structural variations of the metallo-assemblies. When a metallosquare with a cavity of appropriate shape and size is used, the formation of the MINT proceeds successfully by both templated clipping and direct threading. Our studies also show indications on how supramolecular coordination complexes can help expand the potential applications of MINTs.

5.
J Am Chem Soc ; 143(50): 21286-21293, 2021 Dec 22.
Artigo em Inglês | MEDLINE | ID: mdl-34825564

RESUMO

Atomic-scale reproducibility and tunability endorse magnetic molecules as candidates for spin qubits and spintronics. A major challenge is to implant those molecular spins into circuit geometries that may allow one, two, or a few spins to be addressed in a controlled way. Here, the formation of mechanically bonded, magnetic porphyrin dimeric rings around carbon nanotubes (mMINTs) is presented. The mechanical bond places the porphyrin magnetic cores in close contact with the carbon nanotube without disturbing their structures. A combination of spectroscopic techniques shows that the magnetic geometry of the dimers is preserved upon formation of the macrocycle and the mMINT. Moreover, the metallic core selection determines the spin location in the mMINT. The suitability of mMINTs as qubits is explored by measuring their quantum coherence times (Tm). Formation of the dimeric ring preserves the Tm found in the monomer, which remains in the µs scale for mMINTs. The carbon nanotube is used as vessel to place the molecules in complex circuits. This strategy can be extended to other families of magnetic molecules. The size and composition of the macrocycle can be tailored to modulate magnetic interactions between the cores and to introduce magnetic asymmetries (heterometallic dimers) for more complex molecule-based qubits.

6.
Nanoscale Horiz ; 6(7): 551-558, 2021 Jun 28.
Artigo em Inglês | MEDLINE | ID: mdl-33889898

RESUMO

The building of van der Waals heterostructures and the decoration of 2D materials with organic molecules share a common goal: to obtain ultrathin materials with tailored properties. Performing controlled chemistry on van der Waals heterostructures would add an extra level of complexity, providing a pathway towards 2D-2D-0D mixed-dimensional heterostructures. Here we show that thiol-ene-like "click" chemistry can be used to decorate franckeite, a naturally occurring van der Waals heterostructure with maleimide reagents. ATR-IR and NMR analyses corroborate the Michael addition mechanism via the formation of a S-C covalent bond, while Raman and HR-TEM show that the SnS2-PbS alternating structure of franckeite is preserved, and suggest that SnS2 reacts preferentially, which is confirmed through XPS. We illustrate how this methodology can be used to add functional molecular moieties by decorating franckeite with porphyrins. UV-vis-NIR spectroscopy confirms that the chromophore ground state remains operative, showing negligible ground-state interactions with the franckeite. Excited-state interactions across the hybrid interface are revealed. Time-resolved photoluminescence confirms the presence of excited-state deactivation in the linked porphyrin ascribed to energy transfer to the franckeite.

7.
RSC Adv ; 11(58): 36719-36725, 2021 Nov 10.
Artigo em Inglês | MEDLINE | ID: mdl-35494398

RESUMO

Functionalized epoxies show unique advantages in some special applications. Herein, a fluorescent and UV-shielding dual-functional epoxy resin, epoxy-EAn, is prepared via synthesizing and incorporating a reactive additive, 9-anthracenemethoxyl glycidyl ether (EAn), into the resin system. The results show that EAn performs an outstanding migration resistance. The addition of a small amount of EAn (0.1%) enables epoxy-EAn to emit bright blue-violet fluorescence under UV light, making epoxy-EAn a feasible fluorescent adhesive for reconstruction and repair. The fluorescence emission intensity is adjustable by the treatment with UV light and heat. Correspondingly, the epoxy-EAn can serve as an information storage material to realize information input and decryption. In addition, epoxy-EAn also possesses the ability to shield UV radiation, and transmittance in the near ultraviolet and middle ultraviolet region (200-400 nm) can decrease to zero when the EAn concentration is 0.8%. Meanwhile, epoxy-EAn also shows excellent mechanical properties similar to that of the pure epoxy. This work paves a facile way to fabricate a multi-functional epoxy suitable for various occasions.

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