RESUMEN
NO3RR synthesis of ammonia is a complex eight-electron reaction involving multiple steps and intermediates, in which NO3- adsorption and NH3 desorption are crucial. The Cu-based high entropy quinary alloy catalyst has good surface adsorption and desorption ability for the reduction of nitric acid to ammonia. Here, the catalytic sites were coordinated by constructing CuNiCoZnMn alloys to adjust the electronic structure of the catalytic sites to facilitate the reaction of the substrate and thus optimize the whole reaction path. Based on the ternary alloy CuNiCo, the introduction of the Zn element continues to reduce the desorption energy barrier, and the introduction of the Mn element continues to enhance the initial adsorption energy so that the target product can be quickly held and released to accelerate the production of ammonia. The NH3 yield and Faraday efficiency obtained for the quinary CuNiCoZnMn alloy catalyst reached 723.7 µmol h-1 cm-2 and 96.6%, respectively, at -0.35 V vs RHE potential. The density functional theory calculations showed that the quinary CuNiCoZnMn alloy (NO3- to *NO3-) initial adsorption-free energy change and (*NH3 to NH3) NH3 desorption-free energy change are -2.50, 0.072 eV, respectively, which are significantly better than those of the ternary CuNiC and quaternary CuNiCoZn of -2.02, 0.544 eV and -1.97, 0.217 eV.
RESUMEN
It is an ideal way to use triboelectric nanogenerators (TENGs) to capture energy from the environment for the degradation of organic contaminants in water as a zero-carbon pathway. However, there is an urgent need to further develop TENGs with a simple structure and high output power. Herein, a novel TENG with a vortex-like flexible self-recovery blades of inner stator (denoted as VFR-TENG) is designed and manufactured with the assistance of a fused deposition modeling 3D printing technology. With the rotation of the outer rotor, a facile rotating contact-separation mode is achieved by the alternating arrangement of the flexible self-recovery blades. The contact tightness of the friction layer, a key factor for the transfer of charge density, can be easily adjusted by the thickness and arrangement style of the flexible self-recovery blades. The regulation of material elasticity and rotational frequency on the output characteristics is further investigated based on the special flexible structure. The VFR-TENG exhibits an instantaneous short-circuit current of 350 µA, an open-circuit voltage of 650 V, a transferred charge of 1.1 µC, and an optimum output power density of 4.4 W·m-2. This high-performance VFR-TENG is used for electrochemical degradation systems, which achieves excellent degradation efficiencies of 88.9, 91.7, and 94.1% for methylene blue, methyl orange, and malachite green within 150 min, respectively. This work provides a new idea for the design of flexible self-recovery contact-separation TENGs, which is of great inspiration for the exploitation of TENGs with both the high peak current and high-frequency characteristics for efficient water treatment.
