Integrated electrocatalysts derived from metal organic frameworks for gas-involved reactions

Integrated electrocatalysts(IECs)containing well-defined functional materials directly grown on the current collector have sparked increasing interest in the fields of electrocatalysis owing to efficient activity,high stability and the fact that they are easily assembled into devices.Recently,metal organic frameworks(MOFs)provide a promising platform for constructing advanced IECs because of their properties of low cost,large surface area and efficient structural tunability.In this review,the design principles of state-of-the-art IECs based on MOFs are presented,including by hydrothermal/solvothermal,template-directed,electrospinning,electrodeposition and other methods.The high performance of MOF-derived IECs has also been demonstrated in electrocatalytic gasinvolved reactions.This is promising for green energy storage and conversion.The structure-activity relationship and performance improvement mechanism of IECs are uncovered by discussing some in situ technologies for IECs.Finally,we provide an outlook on the challenges and prospects in this booming field.

MEC环境下增强ABR视频缓存传输

提出移动边缘计算环境下增强自适应比特流视频缓存传输方案。首先针对网络效用最大化问题提出基于改进的Kmeans算法对移动用户进行动态分组,解决码率分配子问题;然后将缓存策略和无线资源联合分配归纳为一个多对多匹配问题,同时通过等效带宽,用户可以根据时变信道选择无线链路,灵活地调整实际传输比特率版本。仿真实验结果表明,MECABR方案与其他方案相比,能够同时提高缓存命中率和吞吐量。

云机器人系统研究综述

随着云计算、大数据和其他新兴技术的发展,云技术和多机器人系统的集成使得能够设计出具有改进能源效率、实时性高、成本低的多机器人系统。为了解决云增强系统中机器人的潜力,介绍了云机器人的起源、发展过程以及有关云机器人的研究项目。介绍了云机器人系统的整体架构,然后从开源源码、云计算、雾计算、网络切换管理、机器人即服务(Raa S)、大数据等方面分析了云机器人系统中各层的主要发展驱动力。详细阐述了当前云机器人系统中的关键技术,并给出了一些可能的解决方案。最后,对云机器人系统的未来发展进行了讨论。

车载边缘计算环境中的任务卸载决策和优化

车载云计算卸载存在高网络延迟、核心网负载严重等问题,本文提出了一种计算切换策略来降低车载边缘计算环境下的任务完成时间.基于Matlab R2016a平台对最小执行时间算法和最小完成时间算法进行了2组仿真实验,结果表明:通过本文提出的计算切换策略能改良任务卸载效率,缩短任务的完成时间.

Advances in efficient electrocatalysts based on layered double hydroxides and their derivatives

The explore and development of electrocatalysts have gained significant attention due to their indispensable status in energy storage and conversion systems, such as fuel cells, metal–air batteries and solar water splitting cells. Layered double hydroxides（LDHs） and their derivatives（e.g., transition metal alloys, oxides, sulfides, nitrides and phosphides） have been adopted as catalysts for various electrochemical reactions, such as oxygen reduction, oxygen evolution, hydrogen evolution, and COreduction, which show excellent activity and remarkable durability in electrocatalytic process. In this review, the synthesis strategies, structural characters and electrochemical performances for the LDHs and their derivatives are described. In addition, we also discussed the effect of electronic and geometry structures to their electrocatalytic activity. The further development of high-performance electrocatalysts based on LDHs and their derivatives is covered by both a short summary and future outlook from the viewpoint of the material design and practical application.

基于深度学习的农作物病虫害识别方法

传统的农作物病虫害识别方法具有鲁棒性差、识别准确率低等问题,而卷积神经网络具有自动提取图像特征、泛化能力强、识别准确率高等特点。快速准确地识别出农作物病虫害类型不仅可以减少病害给农民带来的损失,还可以降低农药对生态环境带来的影响。因此找到一种简单易行的检测方法来快速检测农作物病虫害类型很有意义。基于此,笔者在实验中采用了一种基于残差网络改进的卷积神经网络,并以公开的植物数据集影像作为实验的数据集来训练神经网络,且引入了Xception、VGG-16网络模型进行比较,实验结果证明:笔者所提出的神经网络模型识别准确率达到了98.6%,高于xception的93%、VGG-16的95%。

Layered double hydroxides:Scale production and application in soil remediation as super-stable mineralizer

Soil contamination by heavy metals has presented severe risks to human health through food chain.As one of the most promising remediation technologies,in-situ immobilization strategy has been widely adopted in practice.However,considering the large quantities of contaminated soil,it is still a huge challenge to design low-cost amendments with strong and long-term immobilization ability.Layered double hydroxides(LDHs)have drawn tremendous attention in fundamental research and practical application because of their unique properties.Moreover,owing to its super-stable mineralization effect to heavy metal ions,LDHs have exhibited great potential in the field of soil remediation.In this work,we mainly focused on the scale production strategy of LDHs with low-cost,and its application in soil remediation.Besides,several key challenges in using LDHs as amendments for immobilization of heavy metal ions are presented.We hope that this mini-review could shed light on the sustainable development of LDHs as amendment for heavy metals in future research directions.

基于神经网络的农作物产量预测方法

准确预测农作物的产量对指导农业生产、保障粮食安全以及维持农业可持续发展具有重要意义。传统的农作物产量预测模型通常对输入数据进行统计和拟合,从而实现农作物产量预测,这些模型一般需要人工选取特征且拟合的方法是线性拟合的,而实际中大多要处理的是非线性问题。研究小组采用深度学习方法,并用已公开的农作物遥感图像数据来训练神经网络。由实验结果可以明显地发现研究小组所提出的神经网络模型识别误差率为5.5左右,优于传统的方法,而且鲁棒性也高于传统方法。

Co-thermal in-situ reduction of inorganic carbonates to reduce carbon-dioxide emission

Thermal decomposition of inorganic metal carbonates is the main path to prepare metal oxides;nonetheless,it is always accompanied by the emission of large amounts of CO_(2) as one of the gas products.This study reports a concept of co-thermal insitu reduction of inorganic carbonates by using the energy released by carbonate decomposition under pure hydrogen atmosphere,which reduces the decarboxylation temperature and significantly inhibits the CO_(2) emissions.A combination of hydrogen–deuterium exchange,isotope experiment,and density functional theory calculations demonstrates that the CO results from the selective cleavage of Ca–O bonds at the surface of CaCO_(3) via the direct hydrogenation mechanism at relatively low temperature.However,it undergoes the reverse water–gas shift reaction path at high temperature,i.e.,CO being produced by the reduction of CO_(2) released by the decomposition of carbonates.This study sheds light on the potential of green hydrogen technology for inorganic carbonate valorization toward high value-added products,which can facilitate the large-scale industrial applications.

Cation effects in electrocatalytic reduction reactions:Recent advances

Electrocatalytic reduction reactions,powered by clean energy sources such as solar energy and wind,offer a sustainable method for converting inexpensive feedstocks(e.g.,CO_(2),N_(2)/NO_(x),organics,and O_(2))into high-value-added chemicals or fuels.The design and modification of electrocatalysts have been widely implemented to improve their performance in these reactions.However,bottle-necks are encountered,making it challenging to further improve performance through catalyst development alone.Recently,cations in the electrolyte have emerged as critical factors for tuning both the activity and product selectivity of reduction reactions.This review summarizes recent advances in understanding the role of cation effects in electrocatalytic reduction reactions.First,we introduce the mechanisms underlying cation effects.We then provide a comprehensive overview of their application in electroreduction reactions.Characterization techniques and theoretical calcula-tion methods for studying cation effects are also discussed.Finally,we address remaining challeng-es and future perspectives in this field.We hope that this review offers fundamental insights and design guidance for utilizing cation effects,thereby advancing their development.

Ternary NiCoP nanosheet arrays： An excellent bifunctional catalyst for alkaline overall water splitting

Exploring bifunctional catalysts for the hydrogen and oxygen evolution reactions （HER and OER） with high efficiency, low cost, and easy integration is extremely crucial for future renewable energy systems. Herein, ternary NiCoP nanosheet arrays （NSAs） were fabricated on 3D Ni foam by a facile hydrothermal method followed by phosphorization. These arrays serve as bifunctional alkaline catalysts, exhibiting excellent electrocatalytic performance and good working stability for both the HER and OER. The overpotentials of the NiCoP NSA electrode required to drive a current density of 50 mA/cm2 for the HER and OER are as low as 133 and 308 mV, respectively, which is ascribed to excellent intrinsic electrocatalytic activity, fast electron transport, and a unique superaerophobic structure. When NiCoP was integrated as both anodic and cathodic material, the electrolyzer required a potential as low as -1.77 V to drive a current density of 50 mA/cm2 for overall water splitting, which is much smaller than a reported electrolyzer using the same kind of phosphide-based material and is even better than the combination of Pt/C and Ir/C, the best known noble metal-based electrodes. Combining satisfactory working stability and high activity, this NiCoP electrode paves the way for exploring overall water splitting catalysts.

Phosphorus oxoanion-intercalated layered double hydroxides for high-performance oxygen evolution

Rational design and controlled fabrication of efficient and cost-effective electrodes for the oxygen evolution reaction （OER） are critical for addressing the unpre- cedented energy crisis. Nickel-iron layered double hydroxides （NiFe-LDHs） with specific interlayer anions （i.e. phosphate, phosphite, and hypophosphite） were fabricated by a co-predpitation method and investigated as oxygen evolution electrocatalysts. Intercalation of the phosphorus oxoanion enhanced the OER activity in an alkaline solution; the optimal performance （i.e., a low onset potential of 215 mV, a small Tafel slope of 37.7 mV/dec, and stable electrochemical behavior） was achieved with the hypophosphite-intercalated NiFe-LDH catalyst, demonstrating dramatic enhancement over the traditional carbonate-intercalated NiFe-LDH in terms of activity and durability. This enhanced performance is attributed to the interaction between the intercalated phosphorous oxoanions and the edge-sharing MO6 （M = Ni, Fe） layers, which modifies the surface electronic structure of the Ni sites. This concept should be inspiring for the design of more effective LDH-based oxygen evolution electrocatalvsts.

Layer-by-layer assembly of long-afterglow self-supporting thin films with dual-stimuli-responsive phosphorescence and antiforgery applications

The assembly of thin films （TFs） having long-lasting luminescence can be expected to play an important role in the development of new-generation smart sensors, anti-counterfeiting materials, and information-encryption systems. However, such films are limited compared with their powder and solution counterparts. In this study, by exploiting the self-organization of phosphors in the two-dimensional （2D） galleries between clay nanosheets, we developed a method for the ordered assembly of long-afterglow TFs by utilizing a hydrogen-bonding layer-by-layer （LBL） process. Compared with the pristine powder, the TFs exhibit high polarization and up-conversion room-temperature phosphorescence （RTP）, as well as enhanced quantum yields and luminescence lifetimes, allowing them to be used as room-temperature phosphorescent sensors for humidity and oxygen. Moreover, modified clay-based hybrids with multicolor RTP can serve as anti-counterfeiting marks and triple-mode 2D barcode displays. We anticipate that the LBL assembly process can be extended to the fabrication of other inorganic--organic room-temperature phosphorescent hybrids with smart luminescent sensor and antiforgery applications.

Effects of redox-active interlayer anions on the oxygen evolution reactivity of NiFe-layered double hydroxide nanosheets

Nickel-iron layered double hydroxide （NiFe-LDH） nanosheets have shown optimal oxygen evolution reaction （OER） performance; however, the role of the intercalated ions in the OER activity remains unclear. In this work, we show that the activity of the NiFe-LDHs can be tailored by the intercalated anions with different redox potentials. The intercalation of anions with low redox potential （high reducing ability）, such as hypophosphites, leads to NiFe-LDHs with low OER overpotential of 240 mV and a small Tafel slope of 36.9 mV/dec, whereas NiFe-LDHs intercalated with anions of high redox potential （low reducing ability）, such as fluorion, show a high overpotential of 370 mV and a Tafel slope of 80.8 mV/dec. The OER activity shows a surprising linear correlation with the standard redox potential. Density functional theory calculations and X-ray photoelectron spectroscopy analysis indicate that the intercalated anions alter the electronic structure of metal atoms which exposed at the surface. Anions with low standard redox potential and strong reducing ability transfer more electrons to the hydroxide layers. This increases the electron density of the surface metal sites and stabilizes their high-valence states, whose formation is known as the critical step prior to the OER process.

A Co-N/C hollow-sphere electrocatalyst derived from a metanilic CoAl layered double hydroxide for the oxygen reduction reaction, and its active sites in various pH media

Transition-metal-coordinating nitrogen-doped carbon catalysts （M-N/C, M = Co, Fe, Mn, Ni, etc.） are considered one of the most promising nonprecious-metal electrocatalysts for the oxygen reduction reaction （ORR）. However, they suffer from low ORR catalytic activity, and their active sites have not been fully identified. Herein, we report the synthesis of a porous Co-N/C hollow-sphere electrocatalyst by carbonization of metanilic anions between the layers of a Co-A1 layered double hydroxide. The as-prepared Co-N/C catalyst exhibited excellent ORR catalytic activity with a high half-wave potential and a large diffusion-limited current in alkaline and neutral solutions. The performance of the catalyst was comparable to those of commercial Pt/C electrocatalysts. Through investigating the effects of mask ions （SCN- and F-） on the ORR activity of the Co-N/C catalyst, and comparing the ORR activity before and after the destruction of Co-Nx sites in different pH media, we concluded that the Co-Nx sites act directly as the ORR active sites in acidic and neutral solutions, but have a negligible effect on the ORR activity in alkaline conditions.

A highly-efficient oxygen evolution electrode based on defective nickel-iron layered double hydroxide

Exploring efficient and cost-effective electro- catalysts for oxygen evolution reaction （OER） is critical to water splitting. While nickel-iron layered double hydroxide （NiFe LDH） has been long recognized as a promising non- precious electrocatalyst for OER, its intrinsic activity needs further improvement. Herein, we design a highly-efficient oxygen evolution electrode based on defective NiFe LDH na- noarray. By combing the merits of the modulated electronic structure, more exposed active sites, and the conductive elec- trode, the defective NiFe LDH electrocatalysts show a low onset potential of 1.40 V （vs. RHE）. An overpotential of only 200 mV is required for 10 mA cm-2, which is 48 mV lower than that of pristine NiFe-LDH. Density functional theory plus U （DFT＋U） calculations are further employed for the origin of this OER activity enhancement. We find the introduction of oxygen vacancies leads to a lower valance state of Fe and the narrowed bandgap, which means the electrons tend to be ea- sily excited into the conduction band, resulting in the lowered reaction overpotential and enhanced OER performance.

Multi-dimensional, light-controlled switch of fluorescence resonance energy transfer based on orderly assembly of 0D dye@micro-micelles and 2D ultrathin-layered nanosheets

Fluorescence resonance energy transfer （FRET） systems have broad applications in visual detection, intelligent materials, and biological imaging, all of which favor the transmission of light through multiple dimensions and in diverse directions. Herein, we have demonstrated multi-dimensional （0D and 2D） FRET within a multi-layer ultrathin film （UTF） by employing a layer-by-layer （LBL） assembly technique. The anionic block copolymer micelle poly（tert-butyl acrylate- co-ethyl acrylate-co-methacrylic acid） （PTBEM） is chosen as a molecular carrier for the incorporation of bis（8-hydroxyquinolate） zinc （Znq2） and open-ring merocyanine （MC） （denoted as （Znq2/MC）@PTBEM）. Alternatively, electrostatic assembly is performed with cationic layered double hydroxide （LDH） nanosheets （denoted as [（Znq2/MC）@PTBEM/LDH]n）. This [（Znq2/MC）@PTBEM/ LDH]n system offers a multi-dimensional propagation medium and ensures that the FRET donor and acceptor are located within their F6rster radii in each direction. The system demonstrates a FRET process that can be switched via alternating ultraviolet/visible （UV/vis） irradiation, with tunable blue-green/red fluorescence, resulting in a FRET efficiency as high as 81.7%. It is expected that this assembly method, which uses 0D micelles on a 2D layered material, can be extended to other systems for further development of multi-dimensional FRET.

Exchange-Biased NiFe_(2)O_(4)/NiO Nanocomposites Derived from NiFe-Layered Double Hydroxides as a Single Precursor

NiFe_(2)O_(4) nanoparticles(<10 nm)embedded in a NiO matrix have been fabricated by calcining the corresponding Ni^(Ⅱ)Fe^(Ⅲ)-layered double hydroxide(LDH)precursors at high temperature(500℃).Compared with the NiFe_(2)O_(4)/NiO nanocomposite obtained by calcination of a precursor prepared by a traditional chemical coprecipitation method,those derived from NiFe-LDH precursors show much higher blocking temperatures(TB)(~380 K).The enhanced magnetic stability can be ascribed to the much stronger interfacial interaction between NiFe_(2)O_(4) and NiO phases due to the topotactic nature of the transformation of the LDH precursor to the NiFe_(2)O_(4)/NiO composite material.Through tuning the Ni^(Ⅱ)/Fe^(Ⅲ) molar ratio of the NiFe-LDH precursor,the NiFe_(2)O_(4) concentration can be precisely controlled,and the TB value as well as the magnetic properties of the final material can also be regulated.This work represents a successful example of the fabrication of ferro(ferri)magnetic(FM)/antiferrimagnetic(AFM)systems with high magnetic stability from LDH precursors.This method is general and may be readily extended to other FM/AFM systems due to the wide range of available LDH precursors.

Layered double hydroxide monolayers for controlled loading and targeted delivery of anticancer drugs

Two-dimensional （2D） nanomaterials have gained tremendous attention in the field of biomedicine because of their high specific surface areas and fascinating physicochemical properties. Herein, 2D monolayered double hydroxide （MLDH） nanosheets were employed to localize doxorubicin （DOX）, an anticancer drug, with a loading capacity of as high as 3.6 mg.mg-1 （w/w）. Structural characterizations and theoretical calculations indicate that the DOX molecule is uniformly arranged and oriented at the surface of the MLDHs with a binding energy of 15.90 eV, showing significant electrostatic interaction. With the assistance of the targeting agent folic acid （FA）, DOX-FA/MLDHs demonstrate targeted cellular uptake and superior anticancer behavior based on in vitro tests performed with cancer cells. In addition, this composite material exhibits a selective release toward cancer cells and good biocompatibility with normal cells, which would guarantee its practical applications in cancer therapy.

Sandwich layered double hydroxides with graphene oxide for enhanced water desalination

Layered double hydroxides(LDHs)are a class of two-dimensional(2D)clay compounds that consist of positively charged host layers and exchangeable interlayer anions.The stability of their assemblies in aqueous environment is a challenge due to the extremely high hydrophilicity,which limits their use in membrane-based technologies.Here,we propose a graphene oxide(GO)armour protection strategy to substantially improve the stability of LDH membranes in aqueous solution.The sandwich structured GO/LDH/GO membranes(GLGMs)possess a negative-positive-negative charge heterojunction in the vertical direction that effectively blocks the transport of both cations and anions,i.e.,NaCl,but allows the permeation of water molecules.Following this mechanism,the GLGMs are used for desalination in a forward osmosis mode.A high rejection rate of over 95.2% for NaCl and water flux of over 2.1 Lm^(-2)h^(-1) are achieved with simulated seawater.