RESUMO
Heusler alloys are a series of well-established intermetallic compounds with abundant structure and elemental substitutions, which are considered as potentially valuable catalysts for integrating multiple reactions owing to the features of ordered atomic arrangement and optimized electronic structure. Herein, a nanoporous copper titanium tin (np-Cu2TiSn) Heusler alloy is successfully prepared by the (electro)chemical dealloying transformation method, which exhibits high nitrate (NO3-) reduction performance with an NH3 Faradaic efficiency of 77.14 %, an NH3 yield rate of 11.90 mg h-1 mg-1cat, and a stability for 100 h under neutral condition. Significantly, we also convert NO3- to high-purity ammonium phosphomolybdate with NH4+ collection efficiency of 83.8 %, which suggests a practical approach to convert wastewater nitrate into value-added ammonia products. Experiments and theoretical calculations reveal that the electronic structure of Cu sites is modulated by the ligand effect of surrounding Ti and Sn atoms, which can simultaneously enhance the activation of NO3-, facilitate the desorption of NH3, and reduce the energy barriers, thereby boosting the electrochemical nitrate reduction reaction.
RESUMO
Due to their outstanding power density, long cycle life and low cost, supercapacitors have gained much interest. As for supercapacitor electrodes, molybdenum nitrides show promising potential. Molybdenum nitrides, however, are mainly prepared as nanopowders via a chemical route and require binders for the manufacture of electrodes. Such electrodes can impair the performance of supercapacitors. Herein, binder-free chromium (Cr)-doped molybdenum nitride (Mo2N) TFEs having different Cr concentrations are prepared via a reactive co-sputtering technique. The Cr-doped Mo2N films prepared have a cubic phase structure of γ-Mo2N with a minor shift in the (111) plane. While un-doped Mo2N films exhibit a spherical morphology, Cr-doped Mo2N films demonstrate a clear pyramid-like surface morphology. The developed Cr-doped Mo2N films contain 0-7.9 at.% of Cr in Mo2N lattice. A supercapacitor using a Cr-doped Mo2N electrode having the highest concentration of Cr reveals maximum areal capacity of 2780 mC/cm2, which is much higher than that of an un-doped Mo2N electrode (110 mC/cm2). Furthermore, the Cr-doped Mo2N electrode demonstrates excellent cycling stability, achieving ~ 94.6% capacity retention for about 2000 cycles. The reactive co-sputtering proves to be a suitable technique for fabrication of binder-free TFEs for high-performance energy storage device applications.
