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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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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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Multifunctional heteroatom zeolites: construction and applications

《化学科学与工程前沿（英文）》 2021年 第15卷 第6期   页码 1462-1486 doi: 10.1007/s11705-021-2099-x

摘要： Multifunctional heteroatom zeolites have drawn broad attentions due to the possible synergistic effects in the catalytic reactions. Remarkable achievements have been made on the synthesis, characterization and catalytic applications of multifunctional heteroatom zeolite, while a review on this important topic is still missing. Herein, current research status of multifunctional heteroatom zeolites is briefly summarized, aiming to boost further researches. First, the synthesis strategies toward heteroatom zeolites are introduced, including the direct synthesis and postsynthesis routes; then, the spectroscopic techniques to identify the existing states of heteroatom sites and the corresponding physiochemical properties are shown and compared; finally, the catalytic applications of multifunctional heteroatom zeolites in various chemical reactions, especially in one-step tandem reactions, are discussed.

关键词： zeolite     multifunctional active sites     heteroatom     characterization     catalysis    

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Research Trends in Fischer--Tropsch Catalysis for Coal to Liquids Technology

Emiel J. M. Hensen,Peng Wang,Wayne Xu

《工程管理前沿（英文）》 2016年 第3卷 第4期   页码 321-330 doi: 10.15302/J-FEM-2016051

摘要： Fischer–Tropsch Synthesis (FTS) constitutes catalytic technology that converts synthesis gas to synthetic liquid fuels and chemicals. While synthesis gas can be obtained from any carbonaceous feedstock, current industrial FTS operations are almost exclusively based on natural gas. Due to the energy structure of China where cheap coal is abundant, coal to liquids (CTL) technology involving coal gasification, FTS and syncrude upgrading is increasingly being considered as a viable option to convert coal to clean transportation fuels. In this brief paper, we review some pertinent issues about Fe- and Co-based FTS catalysts. Fe is better suited to convert synthesis gas derived from coal gasification into fuels. The authors limit themselves to noting some important trends in the research on Fe-based catalysts. They focus on the preparation of phase-pure carbides and innovative cheap synthesis methods for obtaining active and stable catalysts. These approaches should be augmented by (1) computational investigations that are increasingly able to predict not only mechanism, reaction rates and selectivity but also optimum catalyst composition, as well as (2) characterization of the catalytic materials under conditions close to the operation in real reactors.

关键词： Fischer–Tropsch     FTS     CTL     Fe catalyst     iron carbide     computational modeling    

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Biomimetic Macrophage–Fe3O4@PLGA Particle-Triggered Intelligent Catalysis for Killing Multidrug-Resistant

Jieni Fu,Xiangmei Liu,Zhaoyang Li,Yufeng Zheng,Yu Zhang,Hui Jiang,Yanqin Liang,Shengli Zhu,Zhenduo Cui,Shuilin Wu,

《工程（英文）》 doi: 10.1016/j.eng.2023.05.022

摘要： Infections with multidrug-resistant (MRD) Gram-negative bacteria, such as MRD Escherichia coli (E. coli), remain a challenge due to the lack of safe antibiotics and high fatality rates under anti-infection therapies. This work presents a form of biomimetic intelligent catalysis inspired by the selective biocatalytic property of macrophages, consisting of an intelligent controlling center (a living macrophage, MΦ) and a Fenton reaction catalyst (Fe3O4@poly(lactic-co-glycolic acid) (PLGA) nanoparticles) for killing MDR E. coli without harming normal cells. The MΦ–Fe3O4@PLGA particles (i.e., the intelligent catalysis particles) exhibit selective biocatalysis activity toward MDR E. coli by producing H2O2 and lipid droplets (LDs). This process activates the lipid metabolism and glycan biosynthesis and metabolism pathways based on the result of RNA sequencing data analysis. The H2O2 further reacts with Fe3O4@PLGA to form highly toxic hydroxyl radicals (•OH), while the LDs contain antimicrobial peptides and can target MDR E. coli. The highly toxic •OH and antimicrobial peptides are shown to combat with MDR E. coli, such that the antibacterial efficiency of the MΦ–Fe3O4@PLGA particles against MDR E. coli is 99.29% ± 0.31% in vitro. More importantly, after several passages, the intelligent catalysis function of the MΦ–Fe3O4@PLGA particles is well maintained. Hence, the concept of biomimetic intelligent catalysts displays potential for treating diseases other than infections.

关键词： Multidrug-resistant Escherichia coli     Macrophage–Fe3O4@PLGA particles     Biomimetic intelligent catalysis    

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Synthesis of a new iron (III) porphyrin acrylate-styrene copolymer and its catalysis for hydroxylation

YU Hancheng, LI Xixian, HUANG Jinwang, JI Liangnian, CHEN Xianli

《化学科学与工程前沿（英文）》 2007年 第1卷 第1期   页码 65-67 doi: 10.1007/s11705-007-0013-9

摘要： A new iron (III) porphyrin acrylate-styrene copolymer, P[(PorFe)A-S], was synthesized by the reaction of iron (III) porphyrin acrylate with styrene and characterized by UV-Vis, Infrared spectra (IR), inductively coupled plasma-atomic emission spectrometry (ICP) and molecular weight determination. Its catalytic activity in the hydroxylation of cyclohexane for model cytochrome P450 in the P[(PorFe)A-S]-O ascrobate-thiosalicylic acid system has been studied. It was found that the P[(PorFe)A-S] has a higher catalytic activity than non-supported iron (III) porphyrin and its high catalytic activity remained in reuse. The catalytic activity of P[(PorFe)A-S] was discussed in the view of the microenvironment of iron (III) porphyrin. It is proposed that the atalytic activity of the P[(PorFe)A-S] may be further enhanced by construction of a homophase catalytic system containing the iron (III) porphyrin acrylate-styrene copolymer.

关键词： plasma-atomic emission     UV-Vis     weight determination     acrylate-styrene copolymer     styrene    

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标题 作者 时间 类型 操作

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

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

Multifunctional heteroatom zeolites: construction and applications

期刊论文

Research Trends in Fischer--Tropsch Catalysis for Coal to Liquids Technology

Emiel J. M. Hensen,Peng Wang,Wayne Xu

期刊论文

Biomimetic Macrophage–Fe3O4@PLGA Particle-Triggered Intelligent Catalysis for Killing Multidrug-Resistant

Jieni Fu,Xiangmei Liu,Zhaoyang Li,Yufeng Zheng,Yu Zhang,Hui Jiang,Yanqin Liang,Shengli Zhu,Zhenduo Cui,Shuilin Wu,

期刊论文

Synthesis of a new iron (III) porphyrin acrylate-styrene copolymer and its catalysis for hydroxylation

YU Hancheng, LI Xixian, HUANG Jinwang, JI Liangnian, CHEN Xianli

期刊论文