RESUMO
In this article, we report on video-rate identification of very low-cost tags in the terahertz (THz) domain. Contrary to barcodes, Radio Frequency Identification (RFID) tags, or even chipless RFID tags, operate in the Ultra-Wide Band (UWB). These THz labels are not based on a planar surface pattern but are instead embedded, thus hidden, in the volume of the product to identify. The tag is entirely made of dielectric materials and is based on a 1D photonic bandgap structure, made of a quasi-periodic stack of two different polyethylene-based materials presenting different refractive indices. The thickness of each layer is of the order of the THz wavelength, leading to an overall tag thickness in the millimetre range. More particularly, we show in this article that the binary information coded within these tags can be rapidly and reliably identified using a commercial terahertz Time Domain Spectroscopy (THz-TDS) system as a reader. More precisely, a bit error rate smaller than 1% is experimentally reached for a reading duration as short as a few tens of milliseconds on an 8 bits (~40 bits/cm2) THID tag. The performance limits of such a tag structure are explored in terms of both dielectric material properties (losses) and angular acceptance. Finally, realistic coding capacities of about 60 bits (~300 bits/cm2) can be envisaged with such tags.
RESUMO
Fabricating highly efficient and robust oxygen reduction reaction (ORR) electrocatalysts is challenging but desirable for practical Zn-air batteries. As an early transition-metal oxide, zirconium dioxide (ZrO2) has emerged as an interesting catalyst owing to its unique characteristics of high stability, anti-toxicity, good catalytic activity, and small oxygen adsorption enthalpies. However, its intrinsically poor electrical conductivity makes it difficult to serve as an ORR electrocatalyst. Herein, we report ultrafine N-doped ZrO2 nanoparticles embedded in an N-doped porous carbon matrix as an ORR electrocatalyst (N-ZrO2/NC). The N-ZrO2/NC catalyst displays excellent activity and long-term durability with a half-wave potential (E1/2) of 0.84 V and a selectivity for the four-electron reduction of oxygen in 0.1 M KOH. Upon employment in a Zn-air battery, N-ZrO2/NC presented an intriguing power density of 185.9 mW cm-2 and a high specific capacity of 797.9 mA h gZn -1, exceeding those of commercial Pt/C (122.1 mW cm-2 and 782.5 mA h gZn -1). This excellent performance is mainly attributed to the ultrafine ZrO2 nanoparticles, the conductive carbon substrate, and the modified electronic band structure of ZrO2 after N-doping. Density functional theory calculations demonstrated that N-doping can reduce the band-gap of ZrO2 from 3.96 eV to 3.33 eV through the hybridization of the p state of the N atom with the 2p state of the oxygen atom; this provides enhanced electrical conductivity and results in faster electron-transfer kinetics. This work provides a new approach for the design of other enhanced semiconductor and insulator materials.
RESUMO
Defect-mediated nonradiative recombination in traditional semiconductors, such as porous graphene, tremendously lowers the fluorescence emission, thus greatly restricting their applications in more extensive fields. Here, we report that the fluorescence emission of porous graphene with a high defect density has a giant enhancement (about two orders of magnitude) by a direct and simple fluorination strategy, showing a fine defect-tolerance characteristic. Meanwhile, the corresponding fluorocarbon bonds with excellent thermostability (over 500 °C in N2 even air) also bring about good stability. The photophysical origins during the whole photoluminescence evolution are further investigated. In the excitation process, the coexistence of fluorine and aromatic regions in fluorinated porous graphene (FPG) contributes to producing a new electronic band gap structure to match the maximum excitation wavelength, then numerous excitons generate, which is a precondition for strong fluorescence emission. In the emission process, weak electron-phonon interactions, large rigidity, and constrained electron at the defects in FPG greatly reduce nonradiative recombination loss. Moreover, fluorine at the defects also reduces interlayer interactions among FPG nanosheets and resists the influence of absorbed impurities, thereby further restricting nonradiative recombination pathway. Highly fluorescent FPG has been utilized as a fascinating tool to achieve sensitive and naked-eye detection of Fe3+ ions with a high selectivity. The fluorescence quenching efficiency reaches 24% even with an ultralow concentration of Fe3+ (0.06 µM), and that increases to 84% when the concentration of Fe3+ is 396 µM.