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Boehmite-supported CuO as a catalyst for catalytic transfer hydrogenation of 5-hydroxymethylfurfural

《化学科学与工程前沿（英文）》 2023年 第17卷 第4期   页码 415-424 doi: 10.1007/s11705-022-2225-4

摘要： 2,5-bis(hydroxymethyl)furan (BHMF) is an important monomer of polyester. Its oxygen-containing rigid ring structure and symmetrical diol functional group establish it as an alternative to petroleum-based monomer with unique advantages for the prodution of the degradable bio-based polyester materials. Herein, we prepared a boehmite-supported copper-oxide catalyst for the selective hydrogenation of 5-hydroxymethylfurfural into BHMF via catalytic transfer hydrogenation (CTH). Further, ethanol successfully replaced conventional high-pressure hydrogen as the hydrogen donor, with up to 96.9% BHMF selectivity achieved under suitable conditions. Through characterization and factor investigations, it was noted that CuO is crucial for high BHMF selectivity. Furthermore, kinetic studies revealed a higher by-product activation energy compared to that of BHMF, which explained the influence of reaction temperature on product distribution. To establish the catalyst structure-activity correlation, a possible mechanism was proposed. The copper-oxide catalyst deactivated following CTH because ethanol reduced the CuO, which consequently decreased the active sites. Finally, calcination of the catalyst in air recovered its activity. These results will have a positive impact on hydrogenation processes in the biomass industry.

关键词： biomass     5-hydroxymethylfurfural     2     5-bis(hydroxymethyl)furan     transfer hydrogenation     catalysis    

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Kinetics of halogen-exchange fluorination of 2,6-dichlorobenzaldehyde

LIANG Zhengyong, LI Bindong, FENG Chao

《化学科学与工程前沿（英文）》 2008年 第2卷 第1期   页码 59-62 doi: 10.1007/s11705-008-0008-1

摘要： Under the conditions of phase transfer catalysis and nitrobenzene as the solvent, the halogen-exchange fluorination of 2,6-dichlorobenzaldehyde using KF as fluorinating agent was studied. The kinetics was investigated and the reaction rate constants were obtained under the optimum conditions of (KF):(2,6-dichlorobenzaldehyde):(PhPBr):n(acetone-furan crown ether) = 4:1:0.1:0.05 and temperatures of 433 K, 443 K, 453 K and 463 K. The results illustrated the activation energy of the first and the second step is 4.57 × 10 J·mol and 3.53 × 10 J·mol, respectively. The pre-exponential factor is 4.50 × 10 h and 1.08 × 10 h, respectively. Thus a reliable kinetics data could be obtained for further research.

关键词： reaction     solvent     transfer catalysis     activation     nitrobenzene    

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Cobalt nitride enabled benzimidazoles production from furyl/aryl bio-alcohols and -nitroanilines without an external H-source

《化学科学与工程前沿（英文）》 2023年 第17卷 第1期   页码 68-81 doi: 10.1007/s11705-022-2174-y

摘要： Benzimidazole derivatives have wide-spectrum biological activities and pharmacological effects, but remain challenging to be produced from biomass feedstocks. Here, we report a green hydrogen transfer strategy for the efficient one-pot production of benzimidazoles from a wide range of bio-alcohols and o-nitroanilines enabled by cobalt nitride species on hierarchically porous and recyclable nitrogen-doped carbon catalysts (Co/CNx-T, T denotes the pyrolysis temperature) without using an external hydrogen source and base additive. Among the tested catalysts, Co/CNx-700 exhibited superior catalytic performance, furnishing 2-substituted benzimidazoles in 65%–92% yields. Detailed mechanistic studies manifest that the coordination between Co2+ and N with appropriate electronic state on the porous nitrogen-doped carbon having structural defects, as well as the remarkable synergetic effect of Co/N dual sites contribute to the pronounced activity of Co/CNx-700, while too high pyrolysis temperature may cause the breakage of the catalyst Co–N bond to lower down its activity. Also, it is revealed that the initial dehydrogenation of bio-alcohol and the subsequent cyclodehydrogenation are closely correlated with the hydrogenation of nitro groups. The catalytic hydrogen transfer-coupling protocol opens a new avenue for the synthesis of N-heterocyclic compounds from biomass.

关键词： biomass conversion     furanic compounds     benzimidazoles     hydrogen transfer     bifunctional catalysis    

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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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标题 作者 时间 类型 操作

Boehmite-supported CuO as a catalyst for catalytic transfer hydrogenation of 5-hydroxymethylfurfural

期刊论文

Kinetics of halogen-exchange fluorination of 2,6-dichlorobenzaldehyde

LIANG Zhengyong, LI Bindong, FENG Chao

期刊论文

Cobalt nitride enabled benzimidazoles production from furyl/aryl bio-alcohols and -nitroanilines without an external H-source

期刊论文

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