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基于超构表面等离激元透镜的高速并行近场直写纳米光刻系统 Article

胡跃强, 李苓, 王榕, 宋剑, 王鸿栋, 段辉高, 纪佳馨, 孟永钢

《工程（英文）》 2021年 第7卷 第11期   页码 1623-1630 doi: 10.1016/j.eng.2020.08.019

摘要：

具有简单、高效、低成本和高灵活性等特点的纳米加工技术在纳米尺度基础研究和原型验证中不可或缺。研究已证明，采用表面等离激元的近场光刻技术（即等离激元光刻）是一种有前景的解决方案。基于高速旋转基底上高刚度被动纳米间隙控制的加工系统是其中一种高效率加工方案。但是，为了研发出新一代具有高分辨率且可靠高效的纳米加工技术，需要探索一种更小更稳定的纳米间隙和新型等离激元透镜及其并行加工方案。因此，本文设计了一套并行等离激元直写纳米光刻系统。该系统应用了新型等离子浮动磁头，当转速为8~18 m⋅s−1时，其最小飞行高度可实现15 nm并且具有高平行度。本文还研制了一种多级的基于超构表面的偏振不敏感等离激元透镜。与传统的等离激元透镜相比，该透镜耦合的功率更大，焦点的范围更集中。该原型系统实现了约26 nm最小线宽的纳米结构并行光刻。该系统有望应用于高自由级、低成本的纳米加工技术，如平面光学元件和纳米机电系统。

 

关键词： 纳米加工     表面等离激元     光刻     等离子体飞行头     超构表面    

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Recent advances in cycloaddition of CO with epoxides: halogen-free catalysis and mechanistic insights

《化学科学与工程前沿（英文）》 2023年 第17卷 第12期   页码 1879-1894 doi: 10.1007/s11705-023-2354-4

摘要： The atom-economical cycloaddition of CO2 with epoxides to synthesize cyclic carbonates is a promising route for valuable utilization of CO2. Halogenide such as alkali metal halides and quaternary ammonium salt have been developed as the efficient catalysts. However, the spilled halogen causes equipment corrosion and affects the product purity. To address these concerns, the halogen-free cycloaddition of CO2 with epoxides has always been desired. In this review, we systematically discussed the halogen-free catalysis for cycloaddition of CO2 with epoxides from the mechanistic insights, aiming to promote the development of efficient halogen-free catalysts. Two types of catalysts, i.e., alternatives of halogen nucleophiles for epoxide activation, and bifunctional catalysts with Lewis acid-base sites for synergistic activation of CO2 and epoxides are summarized and emphasized. Specially, metal oxides as the potential halogen-free catalysts are highlighted due to their flexible acid-base sites for synergistic activation of CO2 and epoxides, facile preparation, and low cost.

关键词： carbon dioxide     halogen-free catalysis     cyclic carbonate     mechanistic insight    

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Plasmonic Au nanoparticles supported on both sides of TiO2 hollow spheres for maximising photocatalytic

Jianwei Lu, Lan Lan, Xiaoteng Terence Liu, Na Wang, Xiaolei Fan

《化学科学与工程前沿（英文）》 2019年 第13卷 第4期   页码 665-671 doi: 10.1007/s11705-019-1815-2

摘要： A strategy of intensifying the visible light harvesting ability of anatase TiO hollow spheres (HSs) was developed, in which both sides of TiO HSs were utilised for stabilising Au nanoparticles (NPs) through the sacrificial templating method and convex surface-induced confinement. The composite structure of single Au NP yolk-TiO shell-Au NPs, denoted as Au@Au(TiO , was rendered and confirmed by the transmission electron microscopy analysis. Au@Au(TiO showed enhanced photocatalytic activity in the degradation of methylene blue and phenol in aqueous phase under visible light surpassing that of other reference materials such as Au(TiO by 77% and Au@P25 by 52%, respectively, in phenol degradation.

关键词： TiO2 hollow spheres     plasmonic Au nanoparticles     confinement     visible light     photocatalytic degradation    

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Magnetic-porous microspheres with synergistic catalytic activity of small-sized gold nanoparticles and titania matrix

Kadriye Özlem Hamaloğlu, Ebru Sağ, Çiğdem Kip, Erhan Şenlik, Berna Saraçoğlu Kaya, Ali Tuncel

《化学科学与工程前沿（英文）》 2019年 第13卷 第3期   页码 574-585 doi: 10.1007/s11705-019-1799-y

摘要： Fe O nanoparticles immobilized on porous titania in micron-size range were decorated with small-sized gold nanoparticles and used as a plasmonic catalyst for the reduction of 4-nitrophenol. Monodisperse-porous magnetic titania microspheres were synthesized with bimodal pore-size distribution by the sol-gel templating method. Small-sized gold nanoparticles obtained by the Martin method were attached onto the aminated form of the magnetic titania microspheres. A significant enhancement in the catalytic activity was observed using the gold nanoparticle-decorated magnetic titania microspheres compared to gold nanoparticle-decorated magnetic silica microspheres because of the synergistic effect between small-sized gold nanoparticles and titania. The synergistic effect for gold nanoparticle-attached magnetic titania microspheres could be explained by surface plasmon resonance-induced transfer of hot electrons from gold nanoparticles to the conduction band of titania. Using the proposed catalyst, 4-nitrophenol could be converted to 4-aminophenol in an aqueous solution within 0.5 min. The 4-nitrophenol reduction rates were 2.5–79.3 times higher than those obtained with similar plasmonic catalysts. The selection of micron-size, magnetic, and porous titania microspheres as a support material for the immobilization of small-sized gold nanoparticles provided a recoverable plasmonic catalyst with high reduction ability.

关键词： small-sized gold nanoparticles     magnetic titania microspheres     sol-gel template synthesis     plasmonic catalysis     4-nitrophenol    

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Application of heterogeneous catalysis to biodiesel synthesis using microalgae oil

《环境科学与工程前沿（英文）》 2021年 第15卷 第5期 doi: 10.1007/s11783-020-1343-9

摘要：

• Microalgae oil application for biodiesel synthesis is discussed.

关键词： Biodiesel     Heterogeneous catalysis     Transesterification     Microalgae oil    

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Plasma-catalysis: Is it just a question of scale?

J. Christopher Whitehead

《化学科学与工程前沿（英文）》 2019年 第13卷 第2期   页码 264-273 doi: 10.1007/s11705-019-1794-3

摘要： The issues of describing and understanding the changes in performance that result when a catalyst is placed into plasma are discussed. The different chemical and physical interactions that result and how their combination might produce beneficial results for the plasma-catalytic processing of different gas streams are outlined with particular emphasis being placed on the different range of spatial and temporal scales that must be considered both in experiment and modelling. The focus is on non-thermal plasma where the lack of thermal equilibrium creates a range of temperature scales that must be considered. This contributes in part to a wide range of inhomogeneity in different properties such as species concentrations and electric fields that must be determined experimentally by methods and be incorporated into modelling. It is concluded that plasma-catalysis is best regarded as conventional catalysis perturbed by the presence of a discharge, which modifies its operating conditions, properties and outcomes often in a very localised way. The sometimes used description “plasma-activated catalysis” is an apt one.

关键词： plasma catalysis     plasma-activated catalysis     non-thermal plasma     CO2 conversion    

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Frontiers of Catalysis Chemistry and Technology

《化学科学与工程前沿（英文）》 2018年 第12卷 第1期   页码 1-2 doi: 10.1007/s11705-018-1704-0

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Scaling up of cluster beam deposition technology for catalysis application

《化学科学与工程前沿（英文）》 2021年 第15卷 第6期   页码 1360-1379 doi: 10.1007/s11705-021-2101-7

摘要： Many research works have demonstrated that the combination of atomically precise cluster deposition and theoretical calculations is able to address fundamental aspects of size-effects, cluster-support interactions, and reaction mechanisms of cluster materials. Although the wet chemistry method has been widely used to synthesize nanoparticles, the gas-phase synthesis and size-selected strategy was the only method to prepare supported metal clusters with precise numbers of atoms for a long time. However, the low throughput of the physical synthesis method has severely constrained its wider adoption for catalysis applications. In this review, we introduce the latest progress on three types of cluster source which have the most promising potential for scale-up, including sputtering gas aggregation source, pulsed microplasma cluster source, and matrix assembly cluster source. While the sputtering gas aggregation source is leading ahead with a production rate of ~20 mg·h–1, the pulsed microplasma source has the smallest physical dimensions which makes it possible to compact multiple such devices into a small volume for multiplied production rate. The matrix assembly source has the shortest development history, but already show an impressive deposition rate of ~10 mg·h–1. At the end of the review, the possible routes for further throughput scale-up are envisaged.

关键词： nanoparticle     cluster     cluster beam deposition     magnetron sputtering     heterogeneous catalysis    

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Preface to special issue on “Advanced Materials and Catalysis”

《化学科学与工程前沿（英文）》 2021年 第15卷 第6期   页码 1357-1359 doi: 10.1007/s11705-021-2119-x

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Shape selective catalysis in methylation of toluene: Development, challenges and perspectives

Jian Zhou, Zhicheng Liu, Yangdong Wang, Dejin Kong, Zaiku Xie

《化学科学与工程前沿（英文）》 2018年 第12卷 第1期   页码 103-112 doi: 10.1007/s11705-017-1671-x

摘要： Toluene methylation with methanol offers an alternative method to produce -xylene by gathering methyl group directly from C1 chemical sources. It supplies a “molecular engineering” process to realize directional conversion of toluene/methanol molecules by selective catalysis in complicated methylation system. In this review, we introduce the synthesis method of -xylene, the development history of methylation catalysts and reaction mechanism, and the effect of reaction condition in -selective technical process. If constructing -xylene as the single target product, the major challenge to develop -selective toluene methylation is to improve the -xylene selectivity without, or as little as possible, losing the fraction of methanol for methylation. To reach higher yield of -xylene and more methanol usage in methylation, zeolite catalyst design should consider improving mass transfer and afterwards covering external acid sites by surface modification to get short “micro-tunnels” with shape selectivity. A solid understanding of mass transfer will benefit realizing the aim of converting more methanol feedstock into -methyl group.

关键词： shape selective catalysis     methylation of toluene    

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Preface to special issue on “Engineering Nanostructured Materials for Advanced Energy and Environmental Catalysis

《化学科学与工程前沿（英文）》 2023年 第17卷 第11期   页码 1621-1622 doi: 10.1007/s11705-023-2365-1

摘要： Preface to special issue on “Engineering Nanostructured Materials for Advanced Energy and Environmental Catalysis”
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Catalysis of semihydrogenation of acetylene to ethylene: current trends, challenges, and outlook

《化学科学与工程前沿（英文）》 2022年 第16卷 第7期   页码 1031-1059 doi: 10.1007/s11705-021-2113-3

摘要： Ethylene is an important feedstock for various industrial processes, particularly in the polymer industry. Unfortunately, during naphtha cracking to produce ethylene, there are instances of acetylene presence in the product stream, which poisons the Ziegler–Natta polymerization catalysts. Thus, appropriate process modification, optimization, and in particular, catalyst design are essential to ensure the production of highly pure ethylene that is suitable as a feedstock in polymerization reactions. Accordingly, carefully selected process parameters and the application of various catalyst systems have been optimized for this purpose. This review provides a holistic view of the recent reports on the selective hydrogenation of acetylene. Previously published reviews were limited to Pd catalysts. However, effective new metal and non-metal catalysts have been explored for selective acetylene hydrogenation. Updates on this recent progress and more comprehensive computational studies that are now available for the reaction are described herein. In addition to the favored Pd catalysts, other catalyst systems including mono, bimetallic, trimetallic, and ionic catalysts are presented. The specific role(s) that each process parameter plays to achieve high acetylene conversion and ethylene selectivity is discussed. Attempts have been made to elucidate the possible catalyst deactivation mechanisms involved in the reaction. Extensive reports suggest that acetylene adsorption occurs through an active single-site mechanism rather than via dual active sites. An increase in the reaction temperature affords high acetylene conversion and ethylene selectivity to obtain reactant streams free of ethylene. Conflicting findings to this trend have reported the presence of ethylene in the feed stream. This review will serve as a useful resource of condensed information for researchers in the field of acetylene-selective hydrogenation.

关键词： selectivity     hydrogenation     acetylene     ethylene     palladium    

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Pd nano-catalyst supported on biowaste-derived porous nanofibrous carbon microspheres for efficient catalysis

《化学科学与工程前沿（英文）》 2023年 第17卷 第9期   页码 1289-1300 doi: 10.1007/s11705-023-2299-7

摘要： Environmental pollution caused by the presence of aromatic aldehydes and dyes in wastewater is a serious global concern. An effective strategy for the removal of these pollutants is their catalytic conversion, possibly to valuable compounds. Therefore, the design of efficient, stable and long-lifetime catalysts is a worthwhile research goal. Herein, we used nanofibrous carbon microspheres (NCM) derived from the carbohydrate chitin present in seafood waste, and characterized by interconnected nanofibrous networks and N/O-containing groups, as carriers for the manufacture of a highly dispersed, efficient and stable Pd nano-catalyst (mean diameter ca. 2.52 nm). Importantly, the carbonised chitin’s graphitized structure, defect presence and large surface area could promote the transport of electrons between NCM and Pd, thereby endowing NCM supported Pd catalyst with high catalytic activity. The NCM supported Pd catalyst was employed in the degradation of some representative dyes and the chemoselective hydrogenation of aromatic aldehydes; this species exhibited excellent catalytic activity and stability, as well as applicability to a broad range of aromatic aldehydes, suggesting its potential use in green industrial catalysis.

关键词： biowaste chitin     nanofibrous     palladium     nano-catalyst     catalysis    

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Hollow carbon spheres and their noble metal-free hybrids in catalysis

《化学科学与工程前沿（英文）》 2021年 第15卷 第6期   页码 1380-1407 doi: 10.1007/s11705-021-2097-z

摘要： Hollow carbon spheres have garnered great interest owing to their high surface area, large surface-to-volume ratio and reduced transmission lengths. Herein, we overview hollow carbon sphere-based materials and their noble metal-free hybrids in catalysis. Firstly, we summarize the key fabrication techniques for various kinds of hollow carbon spheres, with a particular emphasis on controlling pore structure and surface morphology, and then heterogeneous doping as well as their metal-free/containing hybrids are presented; next, possible applications for non-noble metal/hollow carbon sphere hybrids in the area of energy-related catalysis, including oxygen reduction reaction, hydrogen evolution reaction, oxygen evolution reaction, water splitting, rechargeable Zn-air batteries and pollutant degradation are discussed; finally, we introduce the various challenges and opportunities offered by hollow carbon spheres from the perspective of synthesis and catalysis.

关键词： hollow carbon spheres     functionalization     noble metal-free     catalysis    

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Effect of light scattering on the performance of a direct absorption solar collector

Kwang Hyun WON, Bong Jae LEE

《能源前沿（英文）》 2018年 第12卷 第1期   页码 169-177 doi: 10.1007/s11708-018-0527-5

摘要： Recently, a solar thermal collector often employs nanoparticle suspension to absorb the solar radiation directly by a working fluid as well as to enhance its thermal performance. The collector efficiency of a direct absorption solar collector (DASC) is very sensitive to optical properties of the working fluid, such as absorption and scattering coefficients. Most of the existing studies have neglected particle scattering by assuming that the size of nanoparticle suspension is much smaller than the wavelength of solar radiation (i.e., Rayleigh scattering is applicable). If the nanoparticle suspension is made of metal, however, the scattering cross-section of metallic nanoparticles could be comparable to their absorption cross-section depending on the particle size, especially when the localized surface plasmon (LSP) is excited. Therefore, for the DASC utilizing a plasmonic nanofluid supporting the LSP, light scattering from metallic particle suspension must be taken into account in the thermal analysis. The present study investigates the scattering effect on the thermal performance of the DASC employing plasmonic nanofluid as a working fluid. In the analysis, the Monte Carlo method is employed to numerically solve the radiative transfer equation considering the volume scattering inside the nanofluid. It is found that the light scattering can improve the collector performance if the scattering coefficient of nanofluid is carefully engineered depending on its value of the absorption coefficient.

关键词： direct absorption solar collector     plasmonic nanofluid     light scattering    

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标题 作者 时间 类型 操作

基于超构表面等离激元透镜的高速并行近场直写纳米光刻系统

胡跃强, 李苓, 王榕, 宋剑, 王鸿栋, 段辉高, 纪佳馨, 孟永钢

期刊论文

Recent advances in cycloaddition of CO with epoxides: halogen-free catalysis and mechanistic insights

期刊论文

Plasmonic Au nanoparticles supported on both sides of TiO2 hollow spheres for maximising photocatalytic

Jianwei Lu, Lan Lan, Xiaoteng Terence Liu, Na Wang, Xiaolei Fan

期刊论文

Magnetic-porous microspheres with synergistic catalytic activity of small-sized gold nanoparticles and titania matrix

Kadriye Özlem Hamaloğlu, Ebru Sağ, Çiğdem Kip, Erhan Şenlik, Berna Saraçoğlu Kaya, Ali Tuncel

期刊论文

Application of heterogeneous catalysis to biodiesel synthesis using microalgae oil

期刊论文

Plasma-catalysis: Is it just a question of scale?

J. Christopher Whitehead

期刊论文

Frontiers of Catalysis Chemistry and Technology

期刊论文

Scaling up of cluster beam deposition technology for catalysis application

期刊论文

Preface to special issue on “Advanced Materials and Catalysis”

期刊论文

Shape selective catalysis in methylation of toluene: Development, challenges and perspectives

Jian Zhou, Zhicheng Liu, Yangdong Wang, Dejin Kong, Zaiku Xie

期刊论文

Preface to special issue on “Engineering Nanostructured Materials for Advanced Energy and Environmental Catalysis

期刊论文

Catalysis of semihydrogenation of acetylene to ethylene: current trends, challenges, and outlook

期刊论文

Pd nano-catalyst supported on biowaste-derived porous nanofibrous carbon microspheres for efficient catalysis

期刊论文

Hollow carbon spheres and their noble metal-free hybrids in catalysis

期刊论文

Effect of light scattering on the performance of a direct absorption solar collector

Kwang Hyun WON, Bong Jae LEE

期刊论文