Nonradical-based advanced oxidation processes for pollutant removal have attracted much attention due to their inherent advantages. Herein we report that magnesium oxides (MgO) in CuOMgO/Fe3O4 not only enhanced the catalytic properties but also switched the free radical peroxymonosulfate (PMS)-activated process into the 1O2 based nonradical process. CuOMgO/Fe3O4 catalyst exhibited consistent performance in a wide pH range from 5.0 to 10.0, and the degradation kinetics were not inhibited by the common free radical scavengers, anions, or natural organic matter. Quantitative structure–activity relationships (QSARs) revealed the relationship between the degradation rate constant of 14 substituted phenols and their conventional descriptor variables (i.e., Hammett constants σ, σ–, σ+), half-wave oxidation potential (E 1/2), and pK a values. QSARs together with the kinetic isotopic effect (KIE) recognized the electron transfer as the dominant oxidation process. Characterizations and DFT calculation indicated that the incorporated MgO alters the copper sites to highly oxidized metal centers, offering a more suitable platform for PMS to generate metastable copper intermediates. These highly oxidized metals centers of copper played the key role in producing O2 •– after accepting an electron from another PMS molecule, and finally 1O2 as sole reactive species was generated from the direct oxidation of O2 •– through thermodynamically feasible reactions.
Near‐infrared (NIR) luminescence materials with broadband emissions are necessary for the development of light‐emitting diodes (LEDs) based light sources. However, most known NIR‐emitting materials are limited by their low external quantum efficiency. This work demonstrates how the photoluminescence quantum efficiency of europium‐activated calcium oxide (CaO:Eu) NIR phosphor can be significantly improved and stabilized at operating temperatures of LEDs. A carbon paper wrapping technology is innovatively developed and used during the solid‐state sintering to promote the reduction of Eu3+ into Eu2+. In parallel, the oxygen vacancies in the CaO lattice are repaired utilizing GeO2 decomposition. Through this process, a record‐high external quantum efficiency of 54.7% at 740 nm is obtained with a thermal stability greatly improved from 57% to 90% at 125 °C. The as‐fabricated NIR‐LEDs reach record photoelectric efficiency (100 mA@23.4%) and output power (100 mA @ 319.5 mW). This discovery of high‐performance phosphors will open new research avenues for broadband NIR LED light sources in a variety of photonics applications.
The structure and function of the soil microbiome of urban greenspaces remain largely undetermined. We conducted a global field survey in urban greenspaces and neighboring natural ecosystems across 56 cities from six continents, and found that urban soils are important hotspots for soil bacterial, protist and functional gene diversity, but support highly homogenized microbial communities worldwide. Urban greenspaces had a greater proportion of fast-growing bacteria, algae, amoebae, and fungal pathogens, but a lower proportion of ectomycorrhizal fungi than natural ecosystems. These urban ecosystems also showed higher proportions of genes associated with human pathogens, greenhouse gas emissions, faster nutrient cycling, and more intense abiotic stress than natural environments. City affluence, management practices, and climate were fundamental drivers of urban soil communities. Our work paves the way toward a more comprehensive global-scale perspective on urban greenspaces, which is integral to managing the health of these ecosystems and the well-being of human populations.
These flat-panel X-ray detectors present high sensitivity and low detection limit, but suffer from high cost, complex configuration, and are not applicable to directly image irregular objects. [3] Accordingly, it is urgent to develop largearea, flexible structure with simple configuration, low cost, and high sensitivity detectors for advanced X-ray imaging. Among them, flexible detectors consisting of X-ray storage materials are emerging as one of promising candidates owing to their simple configuration, convenient readout processes, and abilities to enable X-ray imaging in less accessible situations. [3b,4] X-ray storage phosphors show X-rayactivated persistent luminescence (X-PersL) that can store excitation energy and give a sustained release of photon emissions with a duration of few seconds to days. [5] X-PersL materials (e.g., BaFCl:Eu 2+ ) were first used in imaging plates for commercial computed radiography (CR) by Fujifilm in 1983. [6] However, the development of these materials for X-ray imaging has made very little progress since then. [7] Recently, Ou et al. renovated the existing X-ray imaging technology via embedding X-PersL nanoparticles into silicone polymer as a flexible and stretchable detector. [3b] Their photophysical characteristics of excitation and emission separation allow time-lapse and convenient imaging, enabling simplification of the X-ray imaging system and visualization of X-ray imaging free from dangerous radiation. [4] Generally, X-ray storage materials should have excellent X-ray absorption capacity, low-temperature formation of crystalline, and energy traps with controllable properties. Defects play the crucial role in regulation of trap properties, which determine the storage capacities for X-ray imaging. [4,8] In the past few decades, researchers have made great efforts to develop inorganic oxidebased storage phosphors. Nevertheless, low X-ray sensitivity and high synthetic temperature as well as harsh conditions for generating appropriate energy traps limit their further applications. By contrast, halide perovskites are emerging as next-generation optoelectronic materials in recent years, which have the advantages of X-ray sensitivity, processable at low temperature, low-cost, and superior photophysical properties. [9] Despite some metal halide perovskite compounds show PersL, such as Cs 2 AgInCl 6 :Mn 2+ , [10] Cs 3 In 2 Cl 9 , [11] it remains a challenge to realize 3D X-ray imaging by using these materials due to their low storage capacities.In this work, we report the rational design and controlled synthesis of X-ray storage phosphor CsCdCl 3 :xMn 2+ , yR 4+ X-ray imaging has received sustained attention for healthcare diagnostics and nondestructive inspection. To develop photonic materials with tunable photophysical properties in principle accelerates radiation detection technologies. Here the rational design and synthesis of doped halide perovskite CsCdCl 3 :Mn 2+ , R 4+ (R = Ti, Zr, Hf, and Sn) are reported as next generation X-ray storage phosphors, and the capa...
Understanding the structure–property relationship of inorganic solids has emerged as a prevailing strategy to provide guidelines for predicting and designing desired functional materials. Keeping an eye on the mineral structure-chemical composition–property paradigm, such structure-related design methodologies toward new luminescence materials for light-emitting diodes (LEDs) applications have been proposed, extensively utilized, and demonstrated potentials herein. In this review, we summarized several important design principles in the discovery of new inorganic phosphors by the following aspects: (1) constructing or evolving new phases toward novel phosphors from the existing natural mineral prototypes, and several mineral models have been discussed and exemplified by some phosphors; (2) modifying mineral structures via different substitution strategies based on known phosphors to tune the photoluminescence; (3) tuning local structures toward unprecedented emissions, including the state-of-the-art narrow-band emission and the near-infrared emission. Lastly, we discussed some future challenges and opportunities for mineral structure-related investigations in the hopes of directing the discovery and development of the new phosphor materials for LEDs applications.
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