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Abstract Among several well-known transition metal-based compounds, cleavable van der Waals (vdW) Fe_3-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 (T_C~154 K), and versatile magnetic character that is retained in the low-dimensional limit. While the T_Cremains 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. 

Abstract A new isolation protocol was recently reported for highly purified metallic FullertubesD_5h‐C₉₀,D_3d‐C₉₆, andD_5d‐C_100,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.