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Photoredox catalysis is a green solution for organics transformation and CO2 conversion into valuable fuels, meeting the challenges of sustainable energy and environmental concerns. However, the regulation of single-atomic active sites in organic framework not only influences the photoredox performance, but also limits the understanding of the relationship for photocatalytic selective organic conversion with CO2 valorization into one reaction system. As a prototype, different single-atomic metal (M) sites (M2+ = Fe2+, Co2+, Ni2+, Cu2+, and Zn2+) in hydrogen-bonded organic frameworks (M-HOF) backbone with bridging structure of metal-nitrogen are constructed by a typical “two-in-one” strategy for superior photocatalytic C N coupling reactions integrated with CO2 valorization. Remarkably, Zn-HOF achieves 100% conversion of benzylamine oxidative coupling reactions, 91% selectivity of N-benzylidenebenzylamine and CO2 conversion in one photoredox cycle. From X-ray absorption fine structure analysis and density functional theory calculations, the superior photocatalytic performance is attributed to synergic effect of atomically dispersed metal sites and HOF host, decreasing the reaction energy barriers, enhancing CO2 adsorption and forming benzylcarbamic acid intermediate to promote the redox recycle. This work not only affords the rational design strategy of single-atom active sites in functional HOF, but also facilitates the fundamental insights upon the mechanism of versatile photoredox coupling reaction systems.  相似文献   
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Semitransparent organic solar cells (ST-OSCs) have attracted increasing attention due to their promising prospect in building-integrated photovoltaics. Generally, efficient ST-OSCs with good average visible transmittance (AVT) can be realized by developing active layer materials with light absorption far from the visible light range. Herein, the development of ultrawide bandgap polymer donors with near-ultraviolet absorption, paired with near-infrared acceptors, is proposed to achieve high-performance ST-OSCs. The key points for the design of ultrawide bandgap polymers include constructing donor–donor type conjugated skeleton, suppressing the quinoidal resonance effect, and minimizing the twist of conjugated skeleton via noncovalent conformational locks. As a proof of concept, a polymer named PBOF with an optical bandgap of 2.20 eV is synthesized, which exhibited largely reduced overlap with the human eye photopic response spectrum and afforded a power conversion efficiency (PCE) of 16.40% in opaque device. As a result, ST-OSCs with a PCE over 10% and an AVT over 30% are achieved without optical modulation. Moreover, colorful ST-OSCs with visual aesthetics can be achieved by tuning the donor/acceptor weight ratio in active layer benefiting from the ultrawide bandgap nature of PBOF. This study demonstrates the great potential of ultrawide bandgap polymers for efficient colorful ST-OSCs.  相似文献   
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In this paper, a finite-time optimal tracking control scheme based on integral reinforcement learning is developed for partially unknown nonlinear systems. In order to realize the prescribed performance, the original system is transformed into an equivalent unconstrained system so as to a composite system is constructed. Subsequently, a modified nonlinear quadratic performance function containing the auxiliary tracking error is designed. Furthermore, the technique of experience replay is used to update the critic neural network, which eliminates the persistent of excitation condition in traditional optimal methods. By combining the prescribed performance control with the finite-time optimization control technique, the tracking error is driven to a desired performance in finite time. Consequently, it has been shown that all signals in the partially unknown nonlinear system are semiglobally practical finite-time stable by stability analysis. Finally, the provided comparative simulation results verify the effectiveness of the developed control scheme.  相似文献   
45.
Zhu  Ting  Qu  Wen  Cao  Wenliang 《The Journal of supercomputing》2022,78(1):222-237
The Journal of Supercomputing - With the wide spread of image information, it is an urgent problem to protect image property rights and crack down on piracy. Watermarking algorithm is an effective...  相似文献   
46.
In this study, we report the results of an investigation into the sintering temperature dependence of magnetic and transport properties for GdBaCo2 O 5 + δ synthesized through a sol-gel method. The lowering of sintering temperature leads to the increase of oxygen content and the reduction of grain size. The increase of oxygen content results in the enhancement of magnetic interactions and the weakening of Coulomb repulsion effect, while the reduction of grain size improves the magnetoresistance effect. Metal-insulator transition accompanied with spin-state transition is observed in all samples.  相似文献   
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Spina bifida aperta are complex congenital malformations resulting from failure of fusion in the spinal neural tube during embryogenesis. Despite surgical repair of the defect, most patients who survive with spina bifida aperta have a multiple system handicap due to neuron deficiency of the defective spinal cord. Tissue engineering has emerged as a novel treatment for replacement of lost tissue. This study evaluated the prenatal surgical approach of transplanting a chitosan–gelatin scaffold seeded with bone marrow mesenchymal stem cells (BMSCs) in the healing the defective spinal cord of rat fetuses with retinoic acid induced spina bifida aperta. Scaffold characterisation revealed the porous structure, organic and amorphous content. This biomaterial promoted the adhesion, spreading and in vitro viability of the BMSCs. After transplantation of the scaffold combined with BMSCs, the defective region of spinal cord in rat fetuses with spina bifida aperta at E20 decreased obviously under stereomicroscopy, and the skin defect almost closed in many fetuses. The transplanted BMSCs in chitosan–gelatin scaffold survived, grew and expressed markers of neural stem cells and neurons in the defective spinal cord. In addition, the biomaterial presented high biocompatibility and slow biodegradation in vivo. In conclusion, prenatal transplantation of the scaffold combined with BMSCs could treat spinal cord defect in fetuses with spina bifida aperta by the regeneration of neurons and repairmen of defective region.  相似文献   
50.
The corrosion behavior of 2A02 Al alloy under simulated marine atmospheric environment has been studied using mass-gain, scanning electron microscope/energy dispersive spectroscopy (SEM/EDS), laser scanning confocal microscopy, X-ray diffraction spectroscopy and localized electrochemical methods. The results demonstrate that the relationship between the corrosion induced mass-gain and the corrosion time is in accordance with the power rule. The mass-gain increases gradually during the corrosion time, while the corrosion rate decreases. With ongoing of the corrosion, corrosion products film changed from a porous to a compact structure. The various spectroscopic data show that the corrosion products films composed mainly of Al(OH)3, Al2O3 and AlCl3. The electrochemical corrosion behavior of the 2A02 Al alloy was studied by electrochemical impedance spectroscopy (EIS).  相似文献   
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