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
Electrocatalytic hydrogenation (ECH) is a burgeoning strategy for the sustainable utilization of hydrogen. However, how to effectively suppress the competitive hydrogen evolution reaction (HER) is a big challenge to ECH catalysis. In this study, amine (NH2 R)-coordinated Pd nanoparticles loaded on carbon felt (Pd@CF) as a catalyst is successfully synthesized by a one-step solvothermal reduction method using oleylamine as the reducing agent. An exceptional ECH reactivity on benzaldehyde is achieved on the optimal Pd@CF catalyst in terms of a high conversion (89.7%) and selectivity toward benzyl alcohol (89.8%) at −0.4 V in 60 min. Notably, the Faradaic efficiency for producing benzyl alcohol is up to 90.2%, much higher than that catalyzed by Pd@CF-without N-group (41.1%) and thecommercial Pd/C (20.9%). The excellent ECH performance of Pd@CF can be attributed to the enriched electrons on Pd surface resulted from the introduction of NH2 R groups, which strengthens both the adsorption of benzaldehyde and the adsorbed hydrogen (Hads) on Pd, preventing the combination of Hads to form H2, that is, inhibiting the HER. This study gives a new insight into design principles of highly efficient electrocatalysts for the hydrogenation of unsaturated aldehydes molecules. 相似文献
Switchable passive radiative cooling (PRC) smart windows can modulate sunlight transmission and spontaneously emit heat to outer space through atmospheric transparent window, presenting great potential in building energy conservation. However, realizing stable and on-demand control of the cooling efficiency for PRC materials is still challenging. Herein, an electro-controlled polymer-dispersed liquid crystal (PDLC) smart window showing PRC property is designed and prepared by adding mid-infrared emitting reactive monomers into the conventional PDLC matrix. It is found that not only the electro-optical properties but also the PRC efficiency of PRC PDLC film are tunable by regulating the content of the mid-infrared emitting components, film thickness, and micromorphology. This advanced PRC PDLC material achieves a near/sub-ambient temperature when the solar irradiance is below 400 W m−2 and can dynamically manage daytime cooling efficiency. Importantly, its PRC efficiency is capable of being tuned in an on-demand and ultrafast millisecond-scale way, whose controllable transparency enables multistage heat regulation. This study is hoped to provide new inspiration in the preparation of advanced optical devices and energy-efficient equipment. 相似文献
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
Two novel transition metal-doped tungsten bronze oxides, Pb2.15Li0.85Nb4.85Ti0.15O15 (PLNT) and Pb2.15Li0.55Nb4.85W0.15O15 (PLNW), are synthesized by high-temperature solid-state reactions. The Rietveld method using the high-resolution synchrotron radiation indicates that PLNT and PLNW crystallize in the orthorhombic polar noncentrosymmetric space group, Pmn21 (no. 31). As a class of tungsten bronze oxide, PLNT and PLNW retain a unique rigid framework composed of d0 transition metal cation (Ti4+ or W6+)-doped highly distorted NbO6 octahedra along with the subsequently generated Pb/LiO12 and PbO15 polyhedra. Interestingly, the d0 transition metal-doped tungsten bronzes, PLNT and PLNW, exhibit extremely large second-harmonic generation (SHG) responses of 56 and 67 × KH2PO4, respectively. The observed immeasurably strong SHG is mainly attributed to a net polarization originating from the alignment of highly distorted NbO6 octahedra with doped transition metals in the frameworks. It is believed that doping transition metal cations at the B-site of the tungsten bronze structures should be an innovative strategy to develop novel high-performance nonlinear optical materials. 相似文献
Weather is a key factor affecting the control of air traffic. Accurate recognition and classification of similar weather scenes in the terminal area is helpful for rapid decision-making in air traffic flow management. Current researches mostly use traditional machine learning methods to extract features of weather scenes, and clustering algorithms to divide similar scenes. Inspired by the excellent performance of deep learning in image recognition, this paper proposes a terminal area similar weather scene classification method based on improved deep convolution embedded clustering (IDCEC), which uses the combination of the encoding layer and the decoding layer to reduce the dimensionality of the weather image, retaining useful information to the greatest extent, and then uses the combination of the pre-trained encoding layer and the clustering layer to train the clustering model of the similar scenes in the terminal area. Finally, terminal area of Guangzhou Airport is selected as the research object, the method proposed in this article is used to classify historical weather data in similar scenes, and the performance is compared with other state-of-the-art methods. The experimental results show that the proposed IDCEC method can identify similar scenes more accurately based on the spatial distribution characteristics and severity of weather; at the same time, compared with the actual flight volume in the Guangzhou terminal area, IDCEC's recognition results of similar weather scenes are consistent with the recognition of experts in the field. 相似文献
This paper provides an in-depth treatment of voltage-to-time converters (VTCs) for time-based signal processing with a nonlinearity emphasis. The need for VTCs in deployment of time-based techniques for high-speed or high-resolution analog-to-digital converters is investigated. It is followed with the classification of VTCs. A detailed treatment of the principle, topology, operation, and design consideration of variable-slope (VS) and constant-slope (CS) VTCs is provided. The nonlinearity of VS-VTCs and that of CS-VTCs are analyzed in detail analytically. It is shown that VS-VTCs is inherently nonlinear while CS-VTCs is intrinsically linear. Factors contributing to the nonlinearity of these VTCs are investigated. VS-VTCs and CS-VTCs studied are designed in TSMC 130 nm 1.2 V CMOS and analyzed using Spectre from Cadence Design Systems with BSIM3.3 device models. A good agreement between simulation and analytical results is obtained. The average gain of the VS-VTC is 4.4 times that of the CS-VTC. The 2nd and 3rd harmonics of the CS-VTC are significantly smaller as compared with those of the VS-VTC at the price of more power consumption.
The Journal of Supercomputing - In the literature, most previous studies on English implicit inter-sentence relation recognition only focused on semantic interactions, which could not exploit the... 相似文献