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1.
Angew Chem Int Ed Engl ; 55(17): 5238-42, 2016 Apr 18.
Artigo em Inglês | MEDLINE | ID: mdl-26990927

RESUMO

Construction of a molecular system in which the magnetic lattice exhibits long-range order is one of the fundamental goals in materials science. In this study, we demonstrate the artificial construction of a ferrimagnetic lattice by doping electrons into acceptor sites of a neutral donor/acceptor metal-organic framework (D/A-MOF). This doping was achieved by the insertion of Li-ions into the D/A-MOF, which was used as the cathode of a Li-ion battery cell. The neutral D/A-MOF is a layered system composed of a carboxylate-bridged paddlewheel-type diruthenium(II,II) complex as the donor and a TCNQ derivative as the acceptor. The ground state of the neutral form was a magnetically disordered paramagnetic state. Upon discharge of the cell, spontaneous magnetization was induced; the transition temperature was variable. The stability of the magnetically ordered lattice depended on the equilibrium electric potential of the D/A-MOF cathode, which reflected the electron-filling level.

3.
ACS Sustain Chem Eng ; 11(28): 10242-10251, 2023 Jul 17.
Artigo em Inglês | MEDLINE | ID: mdl-37476420

RESUMO

This work presents a mechanistic understanding of the synthesis of small (<3 nm) gold nanoparticles in a nontoxic, eco-friendly, and biodegradable eutectic mixture of choline chloride and urea (reline) without the addition of external reducing or stabilization agents. Reline acts as a reducing agent by releasing ammonia (via urea hydrolysis), forming gold nanoparticles even at trace ammonia concentration levels. Reline also affects the speciation of the gold precursor forming gold chloro-complexes, stabilizing Au+ species, leading to an easier reduction and avoiding the otherwise fast disproportionation reaction. Such a capability is however lost in the presence of large amounts of water, where water replaces the chloride ligands in the precursor speciation. In addition, reline acts as a weak stabilizing agent, leading to small particles (<3 nm) and narrow distributions although agglomerates quickly form. Such properties are maintained in the presence of water, indicating that it is linked to the urea stabilization rather than the hydrogen-bonding network. This work has important implications in the field of green synthesis of nanoparticles with small sizes, especially for biomedical and health care applications, due to the nontoxic nature of the components of deep eutectic solvents in contrast to the conventional routes.

4.
Nanomaterials (Basel) ; 9(9)2019 Aug 25.
Artigo em Inglês | MEDLINE | ID: mdl-31450701

RESUMO

Electronic systems and telecommunication devices based on low-power microwaves, ranging from 2 to 40 GHz, have massively developed in the last decades. Their extensive use has contributed to the emergence of diverse electromagnetic interference (EMI) phenomena. Consequently, EMI shielding has become a ubiquitous necessity and, in certain countries, a legal requirement. Broadband absorption is considered the only convincing EMI shielding solution when the complete disappearance of the unwanted microwave is required. In this study, a new type of microwave absorber materials (MAMs) based on reduced graphene oxide (rGO) decorated with zero-valent Fe@γ-Fe2O3 and Fe/Co/Ni carbon-protected alloy nanoparticles (NPs) were synthesized using the Pechini sol-gel method. Synthetic parameters were varied to determine their influence on the deposited NPs size and spatial distribution. The deposited superparamagnetic nanoparticles were found to induce a ferromagnetic resonance (FMR) absorption process in all cases. Furthermore, a direct relationship between the nanocomposites' natural FMR frequency and their composition-dependent saturation magnetization (Ms) was established. Finally, the microwave absorption efficiency (0.4 MHz to 20 GHz) of these new materials was found to range from 60% to 100%, depending on the nature of the metallic particles grafted onto rGO.

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