Herein, we developed a partially controlled pyrolysis strategy to create evenly distributed NiO nanoparticles within NiFe‐MOF nanosheets (MOF NSs) for electrochemical synthesis of H2O2 by a ...two‐electron oxygen reduction reaction (ORR). The elemental Ni can be partially transformed to NiO and uniformly distributed on the surface of the MOF NSs, which is crucial for the formation of the particular structure. The optimized MOF NSs‐300 exhibits the highest activity for ORR with near‐zero overpotential and excellent H2O2 selectivity (ca. 99 %) in 0.1 m KOH solution. A high‐yield H2O2 production rate of 6.5 mol gcat−1 h−1 has also been achieved by MOF NSs‐300 in 0.1 m KOH and at 0.6 V (vs. RHE). In contrast to completely pyrolyzed products, the enhanced catalytic activities of partially pyrolyzed MOF NSs‐300 originates mainly from the retained MOF structure and the newly generated NiO nanoparticles, forming the coordinatively unsaturated Ni atoms and tuning the performance towards electrochemical H2O2 synthesis.
A new class of partially pyrolyzed NiFe metal–organic framework nanosheets (MOF NSs) was created for the electrochemical synthesis of H2O2 by two‐electron oxygen reduction reaction (ORR) for the first time. The optimized MOF NSs‐300 exhibits the highest activity for ORR with near‐zero overpotential and excellent H2O2 selectivity (ca. 99 %) in 0.1 m KOH, outperforming most electrocatalysts reported to date.
Heterojunction nanostructures usually exhibit enhanced properties in compariosn with their building blocks and are promising catalyst candidates due to their combined surface and unique interface. ...Here, for the first time we realized the oriented growth of ultrasmall metal nanoparticles (NPs) on metal–organic framework nanosheets (MOF NSs) by precisely regulating the reduction kinetics of metal ions with solvents. In particular, a rapid reduction of metal ions leads to the random distribution of metal NPs on the surface of MOF NSs, while a slow reduction of metal ions results in the oriented growth of NPs on the edge of MOF NSs. Impressively, the strong synergy between Pt NPs and MOF NSs significantly enhances the hydrogen evolution reaction (HER) performance, and the optimal catalyst displays HER activities superior to those of a composite with a random growth of Pt NPs and commercial Pt/C under both acidic and alkaline conditions. Moreover, the versatility of such oriented growth has been extended to other metal NPs, such as Pd, Ag, and Au. We believe this work will promote research interest in material design for many potential applications.
Two‐dimensional (2D) metal–organic framework nanosheets (MOF NSs) play a vital role in catalysis, but the most preparation is ultrasonication or solvothermal. Herein, a liquid–liquid interfacial ...synthesis method has been developed for the efficient fabrication of a series of 2D Ni MOF NSs. The active sites could be modulated by readily tuning the ratios of metal precursors and organic linkers (RM/L). The Ni MOF NSs display highly RM/L dependent activities towards 2e oxygen reduction reaction (ORR) to hydrogen peroxide (H2O2), where the Ni MOF NSs with the RM/L of 6 exhibit the optimal near‐zero overpotential, ca. 98 % H2O2 selectivity and production rate of ca. 80 mmol gcat−1 h−1 in 0.1 M KOH. As evidenced by X‐ray absorption fine structure spectroscopy, the coordination environment of active sites changed from saturation to unsaturation, and the partially unsaturated metal atoms are crucial to create optimal sites for enhancing the electrocatalysis.
2D Ni metal–organic framework nanosheets (MOF NSs) with controlled coordination mode were carefully created through a liquid‐liquid interfacial synthesis strategy for the first time and adopted as efficient electrocatalysts for hydrogen peroxide (H2O2) synthesis. The optimized partially unsaturated Ni MOF NSs‐6 exhibits near‐zero overpotential as well as ca. 98 % H2O2 selectivity in 0.1 M KOH, exceeding most electrocatalysts up to date.
In this paper, based on outdoor microcellular channel measurements at 32 GHz for 5G radio systems, a comprehensive channel modeling, simulation, and validation are performed. The ...directional-scan-sounding measurements using a horn antenna rotated with an angular step at the receiver are carried out, which constitutes a virtual array to form a single-input multiple-output radio channel. The directional- and omni-directional path-loss models are developed by using close-in and floating-intercept methods. Non-parametric and parametric methods are applied to extract large-scale channel parameters (LSPs). The non-parametric method is based on the definition of a channel parameter, whereas the parametric method is derived by the space-alternating generalized expectation-maximization (SAGE) algorithm, which can de-embed an antenna pattern. It is found that the LSPs in the angular domain are significantly different by using the two methods; however, the LSPs in the delay domain almost stay the same. By comparing the LSPs with the parameter table at 32 GHz with 3GPP standard, it is found that 3GPP LSPs should be corrected at the International Telecommunications Union-assigned millimeter wave (mmWave) frequencies for 5G. In this paper, the channel simulation is implemented by using the quasi-deterministic radio channel generator (QuaDRiGa) platform recommended by 3GPP. By comparing the LSPs with the simulated and measured results, it is found that QuaDRiGa is a good platform at the mmWave band, even if it is originally developed for channel simulation below 6 GHz. The results of this paper are important and useful in the simulations and design of future 5G radio systems at 32 GHz.
A pair of tri-band multiple-input-multiple-output (MIMO) antennas with high isolation is investigated in this paper. The proposed antenna consists of two monopole antenna elements with an edge to ...edge spacing of 4 mm (0.03~\lambda _{0} at 2.3 GHz). The monopole antenna element chose the bending line structure that can operate in tri-band and realize miniaturization. To achieve compact dimension and high isolation, symmetrical distribution layout is adopted to decouple the low frequency band, the U-shaped neutralization line (NL) contacting with two microstrip lines, and it can to improve the isolation in high frequency band, and the inverted U-shaped NL contacting with two radiation patch can decoupling in the middle frequency band. And then study the envelope correlation coefficient is lower, and the radiation pattern in operation bands is quasi-omnidirectional. It indicates that the antenna has obtained a satisfactory diversity performance within the whole operation bands which can be a good candidate for some portable MIMO applications.
The Sustainable Livelihoods Framework (SLF) serves as an integrated method and instrument that discerns the primary constraints and associated connections pertaining to the sustainable development of ...community residents. In this study, this framework has been enhanced through field investigations of the inhabitants within the “Three Parallel Rivers” World Heritage Site. Through these investigations, an empirical exploration of their livelihood capital was undertaken. It revealed that the collective livelihood capital of these residents within the World Heritage site was notably fragile, and characterized by a low degree of social integration.In the context of preserving the World Heritage Site, it was crucial for community residents to utilize ecological protection policies and compensation mechanisms to optimize and transform their livelihood capital. Additionally, it was important to focus on nurturing sustainable livelihood development, particularly in terms of human capital. This would lay the foundation for transitioning towards a sustainable livelihood model.
•Sensor devices based on a configuration of HZSM-5 zeolite films printed Pd-WO3 sensing film were prepared.•The selectivity of Pd-WO3 sensors is considerably improved by the printing of HZSM-5 ...zeolite films.•Selective detection of CO and methanol is achieved by printing with HZSM-5 and Pt/HZSM-5 films on the top of sensing layers.
In the present study, gas sensors based on Pd-loaded WO3 sensor layers were prepared and coated with zeolite films to improve the selectivity. The sensing behavior of such sensors was characterized using different single gases and mixtures to assess their selectivity. We observed that the selectivity of sensors based on Pd-WO3 can be significantly tailored towards specific target gases by adding a printed zeolite film. The use of an HZSM-5 zeolite film made the Pd-loaded WO3 sensor highly sensitive to CO, with a response of around 10 at 100 ppm CO. When Pt-modified HZSM-5 zeolite film was used, same sensor became sensitive to methanol, with a detection limit of 0.5 ppm even in the presence of high concentration of CO. Interestingly, the Pt-modified HZSM-5 film caused the catalytic conversion of CO, which resulted in a p-type response to CO. In addition, in the presence of methanol such a p-type response to CO was also observed in pure WO3 sensor. Based on the power-law response to oxygen, it is proposed that the resistive responses of all tested sensors were highly dependent on the oxygen content, indicating that oxygen adsorbates on the surface were involved in the fundamental sensing mechanism, which is the same process as conventional gas sensors. The present study showed that the configuration of Pd-WO3 sensing layers coated with zeolite films is viable for tailoring the selectivity of gas sensors.
Computational fluid dynamics (CFD) simulation is used to test two body design methods which use negative pressure gradient to suppress laminar flow separation and drag reduction. The steady-state ...model of the Transition SST model is used to calculate the pressure distribution, wall shear stress, and drag coefficient under zero angle of attack at different velocities. Four bodies designed by two different methods are considered. Our results show the first method is superior to the body of Hansen in drag reduction and the body designed by the first method is more likely to obtain the characteristics of suppressing or eliminating separation, which can effectively improve laminar flow coverage to achieve drag reduction under higher Reynolds number conditions. The results show that the negative pressure gradient method can suppress separation and drag reduction better than the second method. This successful design method is expected to open a promising prospect for its application in the design of small drag, small noise subsonic hydrodynamic hull and underwater weapons.
Hepatocellular carcinoma (HCC) remains as the fifth most common cancer in the world and accounts for more than 700,000 deaths annually. Changes in serum glycosylation have long been associated with ...this cancer but the source of that material is unknown and direct glycan analysis of HCC tissues has been limited. Our laboratory previously developed a method of in situ tissue based N-linked glycan imaging that bypasses the need for microdissection and solubilization of tissue prior to analysis. We used this methodology in the analysis of 138 HCC tissue samples and compared the N-linked glycans in cancer tissue with either adjacent untransformed or tissue from patients with liver cirrhosis but no cancer. Ten glycans were found significantly elevated in HCC tissues as compared to cirrhotic or adjacent tissue. These glycans fell into two major classes, those with increased levels of fucosylation and those with increased levels of branching with or without any fucose modifications. In addition, increased levels of fucosylated glycoforms were associated with a reduction in survival time. This work supports the hypothesis that the increased levels of fucosylated N-linked glycans in HCC serum are produced directly from the cancer tissue.
•Monodisperse and spherical AgNPs were successfully prepared by UILM method.•The formation process of AgNPs was affected by fluid dynamics and chemical effects.•Uncontrolled secondary nucleation and ...particle growth processes could be inhibited.•Machine learning approach was available for quick evaluation.
Due to the high reactivity of Ag+ and uncontrolled growth process, the AgNPs produced by conventional Lee-Meisel method always exhibited larger particle size (30–200 nm) and polydisperse morphology (including spherical, triangular, and rod-like shape). An ultrasound-intensified Lee-Meisel (UILM) method is developed in this study to environmental-friendly and controllable synthesize monodisperse spherical AgNPs (~3.7 nm). Effects of Ag:citrate ratio (1:3 or 5:4), ultrasound power (300 to 1200 W) and reaction time (4 to 24 min) on the physical–chemical properties of AgNPs are investigated systematically. The transmission electron microscope (TEM) images, UV–Vis spectra, average particle size, zeta potential and pH value all demonstrate that crystallization and digestive ripening processes are facilitated in the presence of ultrasound irradiation. Therefore, both chemical reaction rate and mass transfer rate are enhanced to accelerate primary nucleation and inhibit uncontrolled particle growth, leading to the formation of monodisperse spherical AgNPs. Moreover, a machine learning approach - Decision Tree Regressor in conjunction with Shapley value analysis reveal the concentration of reactants is a more important feature affecting the particle.
PDF
