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Free, publicly-accessible full text available June 1, 2026
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Abstract Among several well-known transition metal-based compounds, cleavable van der Waals (vdW) Fe3-xGeTe2(FGT) magnet is a strong candidate for use in two-dimensional (2D) magnetic devices due to its strong perpendicular magnetic anisotropy, sizeable Curie temperature (TC~154 K), and versatile magnetic character that is retained in the low-dimensional limit. While the TCremains far too low for practical applications, there has been a successful push toward improving it via external driving forces such as pressure, irradiation, and doping. Here we present experimental evidence of a room temperature (RT) ferromagnetic phase induced by the electrochemical intercalation of common tetrabutylammonium cations (TBA+) into quasi-2D FGT. We obtained Curie temperatures as high as 350 K with chemical and physical stability of the intercalated compound. The temperature-dependent Raman measurements, in combination with vdW-corrected ab initio calculations, suggest that charge transfer (electron doping) upon intercalation could lead to the observation of RT ferromagnetism. This work demonstrates that molecular intercalation is a viable route in realizing high-temperature vdW magnets in an inexpensive and reliable manner, and has the potential to be extended to bilayer and few-layer vdW magnets.more » « less
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Considerable efforts are being made to find cheaper and more efficient alternatives to the currently commercially available catalysts based on precious metals for the Hydrogen Evolution Reaction (HER). In this context, fullerenes have started to gain attention due to their suitable electronic properties and relatively easy functionalization. We found that the covalent functionalization of C 60 , C 70 and Sc 3 N@ I h C 80 with diazonium salts endows the fullerene cages with ultra-active charge polarization centers, which are located near the carbon-diazonium bond and improve the efficiency towards the molecular generation of hydrogen. To support our findings, Electrochemical Impedance Spectroscopy (EIS), double layer capacitance ( C dl ) and Mott–Schottky approximation were performed. Among all the functionalized fullerenes, DPySc 3 N@ I h C 80 exhibited a very low onset potential (−0.025 V vs. RHE) value, which is due to the influence of the inner cluster on the extra improvement of the electronic density states of the catalytic sites. For the first time, the covalent assembly of fullerenes and diazonium groups was used as an electron polarization strategy to build superior molecular HER catalytic systems.more » « less
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Today, magnetic hyperthermia constitutes a complementary way to cancer treatment. This article reports a promising aspect of magnetic hyperthermia addressing superparamagnetic and highly Fe/Au core-shell nanoparticles. Those nanoparticles were prepared using a wet chemical approach at room temperature. We found that the as-synthesized core shells assembled with spherical morphology, including face-centered-cubic Fe cores coated and Au shells. The high-resolution transmission microscope images (HRTEM) revealed the formation of Fe/Au core/shell nanoparticles. The magnetic properties of the samples showed hysteresis loops with coercivity (HC) close to zero, revealing superparamagnetic-like behavior at room temperature. The saturation magnetization (MS) has the value of 165 emu/g for the as-synthesized sample with a Fe:Au ratio of 2:1. We also studied the feasibility of those core-shell particles for magnetic hyperthermia using different frequencies and different applied alternating magnetic fields. The Fe/Au core-shell nanoparticles achieved a specific absorption rate of 50 W/g under applied alternating magnetic field with amplitude 400 Oe and 304 kHz frequency. Based on our findings, the samples can be used as a promising candidate for magnetic hyperthermia for cancer therapy.more » « less
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Abstract A new isolation protocol was recently reported for highly purified metallic FullertubesD5h‐C90,D3d‐C96, andD5d‐C100,which exhibit unique electronic features. Here, we report the oxygen reduction electrocatalytic behavior of C60, C70(spheroidal fullerenes), and C90, C96, and C100(tubular fullerenes) using a combination of experimental and theoretical approaches. C96(a metal‐free catalyst) displayed remarkable oxygen reduction reaction (ORR) activity, with an onset potential of 0.85 V and a halfway potential of 0.75 V, which are close to the state‐of‐the‐art Pt/C benchmark catalyst values. We achieved an excellent power density of 0.75 W cm−2using C96as a modified cathode in a proton‐exchange membrane fuel cell, comparable to other recently reported efficient metal‐free catalysts. Combined band structure (experimentally calculated) and free‐energy (DFT) investigations show that both favorable energy‐level alignment active catalytic sites on the carbon cage are responsible for the superior activity of C96.more » « less
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