Effect of mesopore spatial distribution of HZSM-5 catalyst on zinc state and product distribution in 1-hexene aromatization

1-hexene aromatization is a promising technology to convert excess olefin in fluid catalytic cracking(FCC)gasoline to high-value benzene(B),toluene(T),and xylene.Besides,the increasing market demand of xylene has put forward higher requirements for new generation of catalyst.For increasing xylene yield in 1-hexene aromatization,the effect of mesopore structure and spatial distribution on product distribution and Zn loading was studied.Catalysts with different mesopore spatial distribution were prepared by post-treatment of parent HZSM-5 zeolite,including NaOH treatment,tetra-propylammonium hydroxide(TPAOH)treatment,and recrystallization.It was found the evenly distributed mesopore mainly prolongs the catalyst lifetime by enhancing diffusion properties but reduces the aromatics selectivity,as a result of damage of micropores close to the catalyst surface.While the selectivity of high-value xylene can be highly promoted when the mesopore is mainly distributed interior the catalyst.Besides,the state of loaded Zn was also affected by mesopores spatial distribution.On the optimized catalyst,the xylene selectivity was enhanced by 12.4%compared with conventional Zn-loaded parent HZSM-5 catalyst at conversion over 99%.It was attributed to the synergy effect of mesopores spatial distribution and optimized acid properties.This work reveals the role of mesopores in different spatial positions of 1-hexene aromatization catalysts in the reaction process and the influence on metal distribution,as well as their synergistic effect two on the improvement of xylene selectivity,which can improve our understanding of catalyst pore structure and be helpful for the rational design of high-efficient catalyst.

基于MIC特征提取与BO-CatBoost的航空发动机RUL预测

针对航空发动机传感器监测的退化参数提取困难,易受噪声干扰及发动机剩余使用寿命预测精度不足等问题,利用最大信息系数、贝叶斯优化算法和类别特征梯度提升算法,提出了一种新的发动机剩余使用寿命预测模型。首先,为有效解决特征提取不足的问题,对采集的传感器历史监测特征进行最大信息系数相关性计算,提取出对发动机寿命运行周期影响较大的关键退化特征。其次,为解决剩余使用寿命预测中的梯度偏差及预测偏移问题,使用基于贝叶斯优化的类别特征梯度提升方法对航空发动机进行剩余使用寿命预测。最后,在美国航空航天局提供的商用模块化航空推进系统仿真数据集上进行实验,结果表明所提预测方法的性能较好,验证了该方法的有效性。

弓形虫MIC1蛋白在杆状病毒系统中的表达及活性分析

为构建可溶性表达弓形虫MIC1蛋白质的重组杆状病毒株并分析重组蛋白质的活性,通过PCR扩增弓形虫mic1基因的编码序列并连接到pFastBac 1质粒中,将重组的转移质粒转化DH10Bac感受态细胞,通过蓝白斑筛选获得重组杆粒,转染Sf9细胞后连续培养3代获得重组杆状病毒株。结果显示,Sf9细胞在感染后的第3天出现典型的细胞病变;间接免疫荧光和Western blot试验结果表明MIC1重组蛋白质在感染的Sf9细胞中成功可溶性表达;纯化的MIC1重组蛋白质不仅具有结合唾液酸乳糖的能力,同时能够刺激Balb/c小鼠产生较高水平的特异性抗体(>1∶25600)。以上结果表明,通过杆状病毒表达系统可获得具有生物学活性的弓形虫MIC1重组蛋白质。

金属诱导晶化(MIC)模式非晶晶化的原位透射电子显微学研究

非晶晶化作为一种制备晶体材料的有效方法已得到广泛应用,近年来,采用金属诱导晶化(metal induced crystallization,MIC)法显著降低材料的晶化温度引起了研究者们的兴趣。为探究MIC模式下温度对金属催化剂扩散行为及晶化过程中材料结构变化的本征影响,本研究以金属Pt诱导非晶硅晶化为例,采用透射电镜结合原位热学研究方法,在原子尺度上直接观察MIC模式下非晶硅的晶化过程。结果显示在550℃下Pt/Si界面处产生了硅化物Pt_(2)Si等化合物,使得材料界面处出现明显的结构变化。而当温度升高至650℃时,Pt会以颗粒移动的形式发生扩散,且扩散过程中会发生明显的几何结构变化。Pt与非晶硅不同的扩散速度会导致界面处出现柯肯达尔孔洞而阻碍界面处两种材料的进一步扩散。当温度升高至700℃时,非晶硅发生晶化,且在此过程中Pt对非晶硅的晶化起了促进作用。

基于量子点@有序介孔复合材料的Micro⁃LED色转换特性

量子点(Quantum dots)由于具有优异的光电特性,广泛应用于发光与显示、太阳能电池、光催化等领域,它的发现和合成获得了2023年诺贝尔化学奖。采用量子点色转换的Micro-LED全彩化显示技术无需巨量转移,有望实现大规模量产,然而,量子点在高强度Micro-LED出光激发下的性能和寿命仍存在局限。基于此,本文研究了基于量子点@有序介孔(QDs@SBA-15)复合材料的Micro-LED色转换技术及其特性,有序介孔分子筛载体独特的孔道结构不仅能够有效提升Micro-LED色转换和光提取效率,且致密的有序介孔材料也一定程度上保障了量子点的稳定性。首先,通过时域有限差分方法(FDTD)建立了Micro-LED仿真模型,探究量子点粒径和有序介孔材料的孔径对光提取效率的影响;基于仿真结果指导,进一步采用物理共混法制备了QDs@SBA-15复合材料,通过透射光谱、荧光激发光谱、紫外-可见光吸收谱等手段对其进行表征并确定浓度配比;最后,将该复合材料与聚二甲基硅氧烷(PDMS)混合固化成膜,并研究了其光致发光性能。实验结果发现,量子点粒径和介孔材料孔径的匹配度以及量子点和有序介孔材料的比例浓度是影响QDs@SBA-15复合材料发光效率及Micro-LED色转换性能的关键因素;通过优化,所得复合材料可获得优异的发光性能以及良好的环境稳定性,相比于纯量子点色转换层,复合材料的光提取效率提升了81.73%,复合材料的环境稳定性提升了14.33%,以Micro-LED作为蓝光光源组成的三基色发光器件工作色域达到了104.52%NTSC。本研究为量子点色转换Micro-LED显示技术提供了理论指导,为实现Micro-LED全彩化开辟了新路径。

Electrochemical hydrogen evolution efficiently boosted by interfacial charge redistribution in Ru/MoSe_(2) embedded mesoporous hollow carbon spheres

The strong metal-support interaction inducing combined effect plays a crucial role in the catalysis reaction. Herein, we revealed that the combined advantages of MoSe_(2), Ru, and hollow carbon spheres in the form of Ru nanoparticles(NPs) anchored on a two-dimensionally ordered MoSe_(2) nanosheet-embedded mesoporous hollow carbon spheres surface(Ru/MoSe_(2)@MHCS) for the largely boosted hydrogen evolution reaction(HER) performance. The combined advantages from the conductive support, oxyphilic MoSe_(2), and Ru active sites imparted a strong synergistic effect and charge redistribution in the Ru periphery which induced high catalytic activity, stability, and kinetics for HER. Specifically, the obtained Ru/MoSe_(2)@MHCS required a small overpotential of 25.5 and 38.4 mV to drive the kinetic current density of 10 mA cm^(-2)both in acid and alkaline media, respectively, which was comparable to that of the Pt/C catalyst. Experimental and theoretical results demonstrated that the charge transfer from MoSe_(2) to Ru NPs enriched the electronic density of Ru sites and thus facilitated hydrogen adsorption and water dissociation. The current work showed the significant interfacial engineering in Ru-based catalysts development and catalysis promotion effect understanding via the metal-support interaction.

Thick free-standing electrode based on carbon-carbon nitride microspheres with large mesopores for high-energy-density lithium-sulfur batteries

The development of sulfur cathodes with high areal capacity and high energy density is crucial for the practical application of lithium-sulfur batteries(LSBs).LSBs can be built by employing(ultra)high-loading sulfur cathodes,which have rarely been realized due to massive passivation and shuttling.Herein,microspheres of a carbon-carbon nitride composite(C@CN)with large mesopores are fabricated via molecular cooperative assembly.Using the C@CN-based electrodes,the effects of the large mesopores and N-functional groups on the electrochemical behavior of sulfur in LSB cells are thoroughly investigated under ultrahigh sulfur-loading conditions(>15 mgS cm^(-2)).Furthermore,for high-energy-density LSBs,the C@CN powders are pelletized into a thick free-standing electrode(thickness:500^m;diameter:11 mm)via a simple briquette process;here,the total amount of energy stored by the LSB cells is 39 mWh,corresponding to a volumetric energy density of 440 Wh L-1 with an areal capacity of 24.9 and 17.5 mAh cm^(-2) at 0.47 and 4.7 mA cm^(-2),respectively(at 24mgS cm^(-2)).These results have significantly surpassed most recent records due to the synergy among the large mesopores,(poly)sulfide-philic surfaces,and thick electrodes.The developed strategy with its potential for scale-up successfully fills the gap between laboratory-scale cells and practical cells without sacrificing the high areal capacity and high energy density,providing a solid foundation for the development of practical LSBs.

Electrochemically-induced highly reactive PdO^(*) interface on modulated mesoporous MOF-derived Co_(3)O_(4) support for selective ethanol electro-oxidation

Herein,Pd nanoparticles loaded Co_(3)O_(4)catalysts(Pd@Co_(3)O_(4))are constructed from zeolitic imidazolate framework-67(ZIF-67)for the ethanol oxidation reaction(EOR).It is demonstrated for the first time that the electrochemical conversion of Co_(3)O_(4)support would result in the charge distribution alignment at the Pd/Co_(3)O_(4)interface and induce the formation of highly reactive Pd-O species(PdO^(*)),which can further catalyze the consequent reactions of the intermediates of the ethanol oxidation.The catalyst,Pd@Co_(3)O_(4)-450,obtained under the optimized conditions exhibits excellent EOR performance with a high mass activity of 590 mA mg-1,prominent operational stability,and extraordinary capability for the electro-oxidation of acetaldehyde intermediates.Importantly,the detailed mechanism investigation reveals that Pd@Co_(3)O_(4)-450 could be benefit to the C-C bond cleavage to promote the desirable C1 pathway for the ethanol oxidation reaction.The present strategy based on the metal-support interaction of the catalyst might provide valuable inspiration for the design of high-performing catalysts for the ethanol oxidation reaction.

Size Determination of Ultramicropores and Small Mesopores Using a Calculation Procedure Based on the Tangents of Comparison Plot

Pore size distribution（PSD） curves of synthesized hollow silica spheres with ultrmicropores and small mesopores were obtained from calculations based on the BJH,KJS,SF,MP,NLDFT models and Prof.Zhu＇s method.Comparisons indicate that Zhu＇s method not only gives reasonable small mesopore size but also could be further extended to the ultramicropores region for the PSD evaluation.

一种MICS频段小型化可植入天线的设计

提出了一款MICS频段的新型柔性植入天线。天线的介质板材料为柔性聚酰亚胺,辐射部分为回形金属带线,接地面为具有圆弧拐角的矩形,天线采用共面波导馈电,整体尺寸为12×7×0.24 mm^(3)。同时,本文还分析了绝缘材料、人体器官组织、天线植入深度、介质板厚度、辐射单元线长及线宽等因素对天线性能的影响。最后测得天线带宽为270~420 MHz,能够覆盖MICS频段,可应用于小型植入式医疗设备。

Core-shell mesoporous carbon hollow spheres as Se hosts for advanced Al-Se batteries

Incorporating a selenium(Se)positive electrode into aluminum(Al)-ion batteries is an effective strategy for improving the overall battery performance.However,the cycling stability of Se positive electrodes has challenges due to the dissolution of intermediate reaction products.In this work,we aim to harness the advantages of Se while reducing its limitations by preparing a core-shell mesoporous carbon hollow sphere with a titanium nitride(C@TiN)host to load 63.9wt%Se as the positive electrode material for Al-Se batteries.Using the physical and chemical confinement offered by the hollow mesoporous carbon and TiN,the obtained core-shell mesoporous carbon hollow spheres coated with Se(Se@C@TiN)display superior utilization of the active material and remarkable cycling stability.As a result,Al-Se batteries equipped with the as-prepared Se@C@TiN composite positive electrodes show an initial discharge specific capacity of 377 mAh·g^(-1)at a current density of 1000 mA·g^(-1)while maintaining a discharge specific capacity of 86.0 mAh·g^(-1)over 200 cycles.This improved cycling performance is ascribed to the high electrical conductivity of the core-shell mesoporous carbon hollow spheres and the unique three-dimensional hierarchical architecture of Se@C@TiN.

Atomically dispersed Fe sites on hierarchically porous carbon nanoplates for oxygen reduction reaction

Developing cost-effective,robust and stable non-precious metal catalysts for oxygen reduction reaction(ORR) is of paramount importance for electrochemical energy conversion devices such as fuel cells and metal-air batteries.Although Fe-N-C single atom catalysts(SACs) have been hailed as the most promising candidate due to the optimal binding strength of ORR intermediates on the Fe-N_(4) sites,they suffer from serious mass transport limitations as microporous templates/substrates,i.e.,zeolitic imidazolate frameworks(ZIFs),are usually employed to host the active sites.Motivated by this challenge,we herein develop a hydrogen-bonded organic framework(HOF)-assisted pyrolysis strategy to construct hierarchical micro/mesoporous carbon nanoplates for the deposition of atomically dispersed Fe-N_(4) sites.Such a design is accomplished by employing HOF nanoplates assembled from 2-aminoterephthalic acid(NH_(2)-BDC) and p-phenylenediamine(PDA) as both soft templates and C,N precursors.Benefitting from the structural merits inherited from HOF templates,the optimized catalyst(denoted as Fe-N-C SAC-950) displays outstanding ORR activity with a high half-wave potential of 0.895 V(vs.reversible hydrogen electrode(RHE)) and a small overpotential of 356 mV at 10 mA cm^(-2) for the oxygen evolution reaction(OER).More excitingly,its application potential is further verified by delivering superb rechargeability and cycling stability with a nearly unfading charge-discharge gap of 0.72 V after 160 h.Molecular dynamics(MD) simulations reveal that micro/mesoporous structure is conducive to the rapid mass transfer of O_(2),thus enhancing the ORR performance.In situ Raman results further indicate that the conversion of O_(2) to~*O_(2)-the rate-determining step(RDS) for Fe-N-C SAC-950.This work will provide a versatile strategy to construct single atom catalysts with desirable catalytic properties.

Enhanced activation of peroxymonosulfate by Fe/N co-doped ordered mesoporous carbon with dual active sites for efficient removal of m-cresol

The novel Fe-N co-doped ordered mesoporous carbon with high catalytic activity in m-cresol removal was prepared by urea-assisted impregnation and simple pyrolysis method.During the preparation of the Fe-NC catalyst,the complexation of N elements in urea could anchor Fe,and the formation of C3N4during urea pyrolysis could also prevent migration and aggregation of Fe species,which jointly improve the dispersion and stability of Fe.The FeN4sites and highly dispersed Fe nanoparticles synergistically trigger the dual-site peroxymonosulfate (PMS) activation for highly efficient m-cresol degradation,while the ordered mesoporous structure of the catalyst could improve the mass transfer rate of the catalytic process,which together promote catalytic degradation of m-cresol by PMS activation.Reactive oxygen species (ROS) analytic experiments demonstrate that the system degrades m-cresol by free radical pathway mainly based on SO_(4)^(-)·and·OH,and partially based on·OH as the active components,and a possible PMS activation mechanism by 5Fe-50 for m-cresol degradation was proposed.This study can provide theoretical guidance for the preparation of efficient and stable catalysts for the degradation of organic pollutants by activated PMS.

Hard-carbon hybrid Li-ion/metal anode enabled by preferred mesoporous uniform lithium growth mechanism

To achieve high energy density in lithium batteries,the construction of lithium-ion/metal hybrid anodes is a promising strategy.In particular,because of the anisotropy of graphite,hybrid anode formed by graphite/Li metal has low transport kinetics and is easy to causes the growth of lithium dendrites and accumulation of dead Li,which seriously affects the cycle life of batteries and even causes safety problems.Here,by comparing graphite with two types of hard carbon,it was found that hybrid anode formed by hard carbon and lithium metal,possessing more disordered mesoporous structure and lithophilic groups,presents better performance.Results indicate that the mesoporous structure provides abundant active site and storage space for dead lithium.With the synergistic effect of this structure and lithophilic functional groups(–COOH),the reversibility of hard carbon/lithium metal hybrid anode is maintained,promoting uniform deposition of lithium metal and alleviating formation of lithium dendrites.The hybrid anode maintains a 99.5%Coulombic efficiency(CE)after 260 cycles at a specific capacity of 500 m Ah/g.This work provides new insights into the hybrid anodes formed by carbon-based materials and lithium metal with high specific energy and fast charging ability.

模块化建筑(MiC)技术的研究综述与进展

装配式建筑作为重要抓手,推动着建筑工业化和行业转型升级的持续深化。高度符合“标准化设计、工厂化生产、低碳绿色建造、集成化装修”理念与特点的模块化建筑(MiC),正成为当下国内发展装配式建筑的又一重要方向,现已逐步在实际工程中推广应用。本文对模块化建筑的研究历程与进展进行梳理和总结,包括模块间连接安装技术,混凝土MiC物流运输、吊重设备布置规划及智能建造等施工技术方面的研究进展。最后,搜集了相关混凝土MiC项目发展历程与应用案例,总结模块化建筑现有研究的不足和发展趋势。

研华MIC-713系列NVIDIA Jetson Orin平台新品上市!

研华基于NVIDIAJetson Orin^(TM)平台开发的边缘AI推理BOxMIC-713系列,外形小巧,性能强大,接口丰富,灵活扩展。MIC-713版本与轻量级MIC-711系列相比,具有更多灵活的1/0扩展能力。适用于小型低功耗自主机器,例如小型化机器人开发,也适用于制造、物流、零售、农业、医疗和生命科学领域的先进应用。

Microwave-assisted conversion of biomass wastes to pseudocapacitive mesoporous carbon for high-performance supercapacitor

Developing an efficient approach of transforming biomass waste to functional carbon-based electrode materials applied in supercapacitor offers an important and high value-added practical application due to the abundance and considerable low price of biomass wastes.Herein,a hierarchical carbon functionalized with electrochemical-active oxygen-containing groups was fabricated by microwave treatment from the biomass waste of camellia oleifera.The obtained mesoporous carbon(MAC)owns nanosheet morphology,rich mesoporosity,large surface area(1726 m2/g)and very high oxygenic functionalities(16.2 wt%)with pseudocapacitive activity.Prepared electrode of supercapacitor and tested in 2.0 M H2 SO4,the MAC exhibits an obvious pseudocapacitive activity and achieved a superior supercapacitive performance to that of directly activated carbon(DAC-800)including high specific capacitance(367 F/g vs.298 F/g)and better rate performance(66%vs.44%).The symmetrical supercapacitor based on MAC shows a high capacity of275 F/g,large energy density of 9.55 Wh/kg(at power density of 478 W/kg)and excellent cycling stability with 99%capacitance retention after 10000 continuous charge-discharge,endowing the obtained MAC a promising functional material for electrochemical energy storage.

Fabrication of a nano-sized ZSM-5 zeolite with intercrystalline mesopores for conversion of methanol to gasoline

Carbon deposition during methanol to hydrocarbons leads to the quick deactivation of ZSM-5 catalyst and it is one of the major problems for this technology. Decreasing the crystal size or introducing mesopores into ZSM-5 zeolites can improve its diffusion property and decrease the coke formation. In this paper, nano-sized ZSM-5 zeolite with intercrystalline mesopores combining the mesoporous and nano sized structure was fabricated. For comparison, the mesoporous ZSM-5 and nano-sized ZSM-5 were also prepared. These catalyst samples were characterized by XRD, BET, NH3-TPD, TEM, Py-IR and TG techniques and used on the conversion of methanol to gasoline in a fixed-bed reactor at T=405 degrees C, WHSV =4.74 h(-1) and P=1.0 MPa. It was found that the external surface area of the nano-sized ZSM-5 zeolite with intercrystalline mesopores reached 104 m(2)/g, larger than that of mesoporous ZSM-5 (66 m(2)/g) and nano sized ZSM-5 (76 m(2)/g). Catalytic lifetime of the nano-sized ZSM-5 zeolite with intercrystalline mesopores was 93 h, which was only longer than that of mesoporous ZSM-5 (86 h), but shorter than that of nano sized ZSM-5 (104 h). Strong acidity promoted the coke formation and thus decreased the catalytic lifetime of the nano-sized ZSM-5 zeolite with intercrystalline mesopores though it presented large external surface that could improve the diffusion property. The special zeolite catalyst was further dealuminated to decrease the strong acidity. After this, its coke formation rate was slowed and catalytic lifetime was prolonged to 106 h because of the large external surface area and decreased weak acidity. This special structural zeolite is a potential catalyst for methanol to gasoline reaction. (C) 2016 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. and Science Press. All rights reserved.

Synthesis and Characterization of Y-Doped Mesoporous CeO_2 Using A Chemical Precipitation Method

Using cetyltrimethylammonium bromide （CTAB） as the template agent, cerium nitrate as the cerium resource, yttrium nitrate as the yttrium resource, and ammonium carbonate as the precipitating agent, mesoporous CeO2 powders doped with different yttrium contents were successfully synthesized using a chemical precipitation method, under an alkalescent condition. Properties of the obtained samples were characterized and analyzed with X-ray diffraction （XRD）, energy dispersive analysis of X-rays （EDAX）, transmission electron microscopy （TEM）, infrared （IR） absorbance, and the BET method. For the prepared samples with 20% （molar ratio） Y-doped content, a BET specific surface area of 106. 6 m^2 · g^- 1, with an average pore size of3~27 nm were obtained. XRD patterns showed that the doped samples were with a cubic fluorite structure. TEM micrographs revealed that the doped samples showed a spherical morphology with a diameter ranging from 20 to 30 nm and a round pore shape. IR results indicated that the Ce-O-Ce vibration intensity decreased as the Y-doped content increased. N2 adsorption-desorption isotherms showed that the samples possessed typical mesopore characteristics. The average pore size of the samples decreased alter mesoporous CeO2 was doped with yttrium, and the average pore size decreased largely as the Y-doped content increased.

Research on a New Process of Preparation for Nano-SiO_2 with High Activity and Mesopores

Nano-SiO_2 with high activity and mesopores was prepared through sol-gel synthesis followed by low-temperatureheat treatment and ball milling firstly in our experiments. TEM was performed to measure particle sizes. Nitrogenadsorption experiments were carried out to estimate specific surface area, porous distribution and porous ratio by BETand BJH methods. The content of Si-OH in SiO_2 surface was calculated by analysis of the results of hydrogen-oxygencontent mensuration (HOCM). As a result, appropriate heat treatment system and ball milling time are important topreparation for nano-SiO_2 with high activity and mesopores, which are 5～50 nm particles, 5～6 nm average aperture,85%～93% porous ratio, and 51%～55% Si-OH content in surface. Nano-SiO_2 with that structure has high surfaceenergy and activity. This process, which has simple facilities and operation rules, is a new way of preparation fornano-SiO_2 with high activity and mesopores.