The slow kinetics of oxygen evolution reaction (OER) causes high power consumption for electrochemical water splitting. Various strategies have been attempted to accelerate the OER rate, but there are few studies on regulating the transport of reactants especially under large current densities when the mass transfer factor dominates the evolution reactions. Herein, NixFe1–x alloy nanocones arrays (with ≈2 nm surface NiO/NiFe(OH)2 layer) are adopted to boost the transport of reactants. Finite element analysis suggests that the high‐curvature tips can enhance the local electric field, which induces an order of magnitude higher concentration of hydroxide ions (OH−) at the active sites and promotes intrinsic OER activity by 67% at 1.5 V. Experimental results show that a fabricated NiFe nanocone array electrode, with optimized alloy composition, has a small overpotential of 190 mV at 10 mA cm−2 and 255 mV at 500 mA cm−2. When calibrated by electrochemical surface area, the nanocones electrode outperforms the state‐of‐the‐art OER electrocatalysts. The positive effect of the tip‐enhanced local electric field in promoting mass transfer is also confirmed by comparing samples with different tip curvature radii. It is suggested that this local field enhanced OER kinetics is a generic effect to other OER catalysts.
Room-temperature phosphorescence (RTP) and thermally activated delayed fluorescence (TADF) materials with long afterglow lifetimes have aroused considerable interest. Here, we successfully achieve the modulation of RTP and TADF properties in a carbon dots (CDs)-in-zeolite system based on different organic templates via an in situ solvothermal synthetic method. Benefitting from the efficient stabilizing effect of triplet states of CDs by SBT zeolite matrix, CDs@SBT-1 with a larger singlet–triplet energy gap (ΔE ST) of 0.36 eV exhibits predominant RTP with a lifetime of 574 ms, while CDs@SBT-2 with a smaller ΔE ST value of 0.18 eV shows TADF with a lifetime of 153 ms. Further investigations reveal that different organic templates result in different CDs structures, thus modulating the ΔE ST values of CDs@zeolites. This work demonstrates a facile strategy to modulate the afterglow properties of CDs@zeolite composites, which opens the possibility of designing the novel afterglow materials desired for various advanced applications.
Abstract. Western China has experienced rapid industrialization and urbanization since the implementation of the National Western Development Strategies (the "Go West" movement) in 1999. This transition has affected the spatial and temporal characteristics of nitrogen dioxide (NO2) pollution. In this study, we analyze the trends and variability of tropospheric NO2 vertical column densities (VCDs) from 2005 to 2013 over Western China, based on a wavelet analysis on monthly mean NO2 data derived from the Ozone Monitoring Instrument (OMI) measurements. We focus on the anthropogenic NO2 by subtracting region-specific "background" values dominated by natural sources. After removing the background influences, we find significant anthropogenic NO2 growth over Western China between 2005 and 2013 (8.6 ± 0.9 % yr−1 on average, relative to 2005), with the largest increments (15 % yr−1 or more) over parts of several city clusters. The NO2 pollution in most provincial-level regions rose rapidly from 2005 to 2011 but stabilized or declined afterwards. The NO2 trends were driven mainly by changes in anthropogenic emissions, as confirmed by a nested GEOS-Chem model simulation and a comparison with Chinese official emission statistics. The rate of NO2 growth during 2005–2013 reaches 11.3 ± 1.0 % yr−1 over Northwestern China, exceeding the rates over Southwestern China (5.9 ± 0.6 % yr−1) and the three well-known polluted regions in the east (5.3 ± 0.8 % yr−1 over Beijing-Tianjin-Hebei, 4.0 ± 0.6 % yr−1 over the Yangtze River Delta, and −3.3 ± 0.3 % yr−1 over the Pearl River Delta). Subsequent socioeconomic analyses suggest that the rapid NO2 growth over Northwestern China is likely related to the fast developing resource- and pollution-intensive industries along with the "Go West" movement as well as relatively weak emission controls. Further efforts should be made to alleviate NOx pollution to achieve sustainable development in Western China.
A novel multifunctional drug delivery system has been constructed by assembling per-6-thio-β-cyclodextrin-modified ultrasmall CuS nanoparticles (CD-CuS) onto fluorescent AIEgen-containing mesoporous silica nanoparticles (FMSN). The CD-CuS nanoparticles are anchored on the surface of benzimidazole-grafted FMSN, acting as a gatekeeper and photothermal agent. The prepared blue-emitting nanocomposite (FMSN@CuS) exhibits good biocompatibility and cell imaging capability. Anticancer drug doxorubicin hydrochloride (DOX) molecules are loaded into FMSN@CuS, and zero prerelease at physiological pH (7.4) and on-demand drug release at an acidic environment can be achieved due to the pH-responsive gate-opening of CD-CuS only at an acidic condition. The FMSN@CuS nanocomposite can generate obvious thermal effect after the exposure of 808 nm laser, which can also accelerate the DOX release. Meanwhile, the fluorescence intensity of DOX-loaded FMSN@CuS increases with the release of DOX, and the intracellular drug release process can be tracked according to the change of luminescence intensity. More importantly, DOX-loaded FMSN@CuS displays efficient anticancer effects in vitro upon 808 nm laser irradiation, demonstrating a good synergistic therapeutic effect via combining enhanced chemotherapy and photothermal therapy.
A multifunctional porous N-rich polymer containing s-triazine and Tröger's base was synthesized. It shows selective adsorption for CO2, colorimetric performance for HCl and good catalytic activity in the Knoevenagel condensation.
Nitrogen dioxide (NO 2 ) at the ground level poses a serious threat to environmental quality and public health. This study developed a novel, artificial intelligence approach by integrating spatiotemporally weighted information into the missing extra-trees and deep forest models to first fill the satellite data gaps and increase data availability by 49% and then derive daily 1 km surface NO 2 concentrations over mainland China with full spatial coverage (100%) for the period 2019–2020 by combining surface NO 2 measurements, satellite tropospheric NO 2 columns derived from TROPOMI and OMI, atmospheric reanalysis, and model simulations. Our daily surface NO 2 estimates have an average out-of-sample (out-of-city) cross-validation coefficient of determination of 0.93 (0.71) and root-mean-square error of 4.89 (9.95) μg/m 3 . The daily seamless high-resolution and high-quality dataset “ChinaHighNO 2 ” allows us to examine spatial patterns at fine scales such as the urban–rural contrast. We observed systematic large differences between urban and rural areas (28% on average) in surface NO 2 , especially in provincial capitals. Strong holiday effects were found, with average declines of 22 and 14% during the Spring Festival and the National Day in China, respectively. Unlike North America and Europe, there is little difference between weekdays and weekends (within ±1 μg/m 3 ). During the COVID-19 pandemic, surface NO 2 concentrations decreased considerably and then gradually returned to normal levels around the 72nd day after the Lunar New Year in China, which is about 3 weeks longer than the tropospheric NO 2 column, implying that the former can better represent the changes in NO x emissions.
Conjugated microporous polymers based on biphenylene exhibit selective adsorption CO2 over CH4 and N2 and luminescence sensing for picric acid.
Ionic porous organic polymers have attracted much attention due to their broad applications in catalysis, energy storage/conversion, proton conduction, etc. In this paper, an ionic porous organic polymer, CMP-PM-Me, was synthesized through post-synthetic modification of a pyrimidine-based conjugated microporous polymer, CMP-PM, which was constructed by the palladium catalyzed Sonogashira reaction of 1,3,5-triethynylbenzen and 2,5-dibromopyrimidine. These two polymers are porous with Brunauer-Emmett-Teller surface areas of 416 and 241 m g for CMP-PM and CMP-PM-Me, respectively. Due to the cationic framework, CMP-PM-Me exhibits a much faster and more efficient adsorption performance to anionic dyes such as Congo red (CR) and methyl orange (MO) than that of CMP-PM with a neutral framework. The uptakes for CR are 400.0 mg g for CMP-PM-Me and 344.8 mg g for CMP-PM, respectively. Furthermore, CMP-PM-Me could quickly and drastically separate anionic dyes from the binary mixed solution of anionic and nonanionic dyes within a short time. This work not only enriches the family of ionic organic porous polymers and widens their synthetic utility, but also demonstrates their applications in the adsorption and separation of anionic dyes in water.
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