Demonstrated here is the correlation between atomic configuration induced electronic density of single‐atom Co active sites and oxygen reduction reaction (ORR) performance by combining density‐functional theory (DFT) calculations and electrochemical analysis. Guided by DFT calculations, a MOF‐derived Co single‐atom catalyst with the optimal Co1‐N3PS active moiety incorporated in a hollow carbon polyhedron (Co1‐N3PS/HC) was designed and synthesized. Co1‐N3PS/HC exhibits outstanding alkaline ORR activity with a half‐wave potential of 0.920 V and superior ORR kinetics with record‐level kinetic current density and an ultralow Tafel slope of 31 mV dec−1, exceeding that of Pt/C and almost all non‐precious ORR electrocatalysts. In acidic media the ORR kinetics of Co1‐N3PS/HC still surpasses that of Pt/C. This work offers atomic‐level insight into the relationship between electronic density of the active site and catalytic properties, promoting rational design of efficient catalysts.
Stretchable micropower sources with high energy density and stability under repeated tensile deformation are key components of flexible/wearable microelectronics. Herein, through the combination of strain engineering and modulation of the interlayer spacing, freestanding and lightweight MXene/bacterial cellulose (BC) composite papers with excellent mechanical stability and a high electrochemical performance are first designed and prepared via a facile all‐solution‐based paper‐making process. Following a simple laser‐cutting kirigami patterning process, bendable, twistable, and stretchable all‐solid‐state micro‐supercapacitor arrays (MSCAs) are further fabricated. As expected, benefiting from the high‐performance MXene/BC composite electrodes and rational sectional structural design, the resulting kirigami MSCAs exhibit a high areal capacitance of 111.5 mF cm
−2
, and are stable upon stretching of up to 100% elongation, and in bent or twisted states. The demonstrated combination of an all‐solution‐based MXene/BC composite paper‐making method and an easily manipulated laser‐cutting kirigami patterning technique enables the fabrication of MXene‐based deformable all‐solid‐state planar MSCAs in a simple and efficient manner while achieving excellent areal performance metrics and high stretchability, making them promising micropower sources that are compatible with flexible/wearable microelectronics.
The modulation effect has been widely investigated to tune the electronic state of single‐atomic M‐N‐C catalysts to enhance the activity of oxygen reduction reaction (ORR). However, the in‐depth study of modulation effect is rarely reported for the isolated dual‐atomic metal sites. Now, the catalytic activities of Fe‐N4 moiety can be enhanced by the adjacent Pt‐N4 moiety through the modulation effect, in which the Pt‐N4 acts as the modulator to tune the 3d electronic orbitals of Fe‐N4 active site and optimize ORR activity. Inspired by this principle, we design and synthesize the electrocatalyst that comprises isolated Fe‐N4/Pt‐N4 moieties dispersed in the nitrogen‐doped carbon matrix (Fe‐N4/Pt‐N4@NC) and exhibits a half‐wave potential of 0.93 V vs. RHE and negligible activity degradation (ΔE1/2=8 mV) after 10000 cycles in 0.1 M KOH. We also demonstrate that the modulation effect is not effective for optimizing the ORR performances of Co‐N4/Pt‐N4 and Mn‐N4/Pt‐N4 systems.
Ag nanoparticles with average sizes of 20 nm were well-dispersed on the surfaces of Fe3O4@SiO2 composite microspheres through a simple wet-chemical method employing the Ag-mirror reaction. The as-synthesized Ag-coated Fe3O4@SiO2 three-ply composite microspheres are monodisperse and bifunctional, with ferromagnetic and surface-enhanced Raman scattering (SERS) properties. The products were characterized by means of X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), and energy dispersive X-ray analysis (EDX). SERS signals of typical analytes such as rhodamine 6G (Rh 6G) were observed on Ag nanoparticles from the Ag-coated Fe3O4@SiO2 microspheres, even though the concentration of the analyte was as low as 1 × 10−15 M (Rh 6G). The Ag-coated Fe3O4@SiO2 microspheres were applied to detecting melamine, and strong SERS signals were obtained with melamine concentration of 1 × 10−6 M. This work may provide a potential and unique technique to detect melamine.
Herein, based on the recently developed magnetic-induced self-assembly techniques, we designed a novel, simple and low-cost method to fabricate a special class of photonic crystals with double photonic band-gap hetero-structures, and eventually achieved the purpose of modulating the optical diffraction color of the structural colors. The method greatly simplifies the fabrication of photonic crystals with multiple photonic band-gap hetero-structures and extends the modulation means of the optical diffraction color of structural colors. Furthermore, it is worth noting that due to the resulting structural colors that are derived from the double photonic band-gap hetero-structures consisting of double diffraction peaks and presenting a magnetic switching effect through the application and withdrawal of the magnetic fields (0.05 T), which is more difficult to be imitated by those of chemical dyes and pigments, a kind of novel photonic anti-counterfeiting label has been prepared with these structural colors. Due to the widespread counterfeiting of various commercial objects and the urgent requirements of forgery protection, the photonic anti-counterfeiting label demonstrated in our work will undoubtedly find applications in meeting the growing anticounterfeiting needs.
Invisible photonic printing, an emerging printing technique, is particularly useful for steganography and watermarking for anti-counterfeiting purposes. However, many challenges exist in order to realize this technique. Herein, we describe a novel photonic printing strategy targeting to overcome these challenges and realize fast and convenient fabrication of invisible photonic prints with good tenability and reproducibility. With this novel photonic printing technique, a variety of graphics with brilliant colors can be perfectly hidden in a soft and waterproof photonic-paper. The showing and hiding of the latent photonic prints are instantaneous with magnet as the only required instrument. In addition, this strategy has excellent practicality and allows end-user control of the structural design utilizing simple software on a PC.
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