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Synthesis of boron modified CoMo/Al

Hui Shang, Chong Guo, Pengfei Ye, Wenhui Zhang

《化学科学与工程前沿（英文）》 2021年 第15卷 第5期   页码 1088-1098 doi: 10.1007/s11705-020-1969-y

摘要： Catalytic hydrodesulfurization (HDS) technique is widely used for clean gasoline production. However, traditional HDS catalyst (CoMo/ -Al O ) exhibits high hydrogenation performance of olefins (HYDO), resulting in the loss of gasoline octane number. To achieve high HDS/HYDO ratio, the key issue is to reduce the interaction between active metals and the support, therefore, in this research, the modified CoMo/ -Al O catalysts with various boron amounts were investigated under traditional or microwave heating. The effects of preparing methods as well as boron amounts on the active phase, acidic properties and HDS catalytic activities were examined. Results show that the modification, especially under microwave treatment, can significantly weaken the interaction between the active component and the support by enlarging the surface area and pore diameter, and reducing the acidity of the support. As a result, the stacking numbers of MoS slabs were obviously improved by the modification and microwave treatment, contributing to higher edge/rim ratio, and resulting in higher HDS performance and selectivity to olefin.

关键词： CoMo catalyst     boron modification     surface acidity     microwave heating     selective hydrodesulfurization    

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Catalyst particle shapes and pore structure engineering for hydrodesulfurization and hydrodenitrogenation

《化学科学与工程前沿（英文）》 2022年 第16卷 第6期   页码 897-908 doi: 10.1007/s11705-021-2127-x

摘要： Catalyst particle shapes and pore structure engineering are crucial for alleviating internal diffusion limitations in the hydrodesulfurization (HDS)/hydrodenitrogenation (HDN) of gas oil. The effects of catalyst particle shapes (sphere, cylinder, trilobe, and tetralobe) and pore structures (pore diameter and porosity) on HDS/HDN performance at the particle scale are investigated via mathematical modeling. The relationship between particle shape and effectiveness factor is first established, and the specific surface areas of different catalyst particles show a positive correlation with the average HDS/HDN reaction rates. The catalyst particle shapes primarily alter the average HDS/HDN reaction rate to adjust the HDS/HDN effectiveness factor. An optimal average HDS/HDN reaction rate exists as the catalyst pore diameter and porosity increase, and this optimum value indicates a tradeoff between diffusion and reaction. In contrast to catalyst particle shapes, the catalyst pore diameter and the porosity of catalyst particles primarily alter the surface HDS/HDN reaction rate to adjust the HDS/HDN effectiveness factor. This study provides insights into the engineering of catalyst particle shapes and pore structures for improving HDS/HDN catalyst particle efficiency.

关键词： hydrodesulfurization     hydrodenitrogenation     particle shape     pore structure    

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Kinetic study of hydrodesulfurization of coker gas oil in a slurry reactor

Haiding XIANG, Tiefeng WANG

《化学科学与工程前沿（英文）》 2013年 第7卷 第2期   页码 139-144 doi: 10.1007/s11705-013-1323-8

摘要： Coker gas oil (CGO) is a poor-quality feedstock for fluidized bed catalytic cracking (FCC) or hydrocracking. The pretreatment of CGO, especially hydrotreating, can significantly improve the product quality and protect the catalyst. In this work, we studied the hydrodesulfurization (HDS) of CGO in a slurry reactor. All the experiments were carried out in an autoclave using a NiMo/Al O catalyst at reaction temperature 340°C–400°C, pressure 6–10 MPa, and stirring speed 800 r·min , with hydrogen-to-oil ratio in the range of 500–1500. The effects of the operating parameters on the desulfurization ratio were investigated and discussed. A macro reaction kinetic model was established for the HDS of CGO in the slurry reactor.

关键词： coker gas oil     hydrodesulfurization     slurry reactor     reaction kinetic model    

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Experimental and theoretical study of microwave enhanced catalytic hydrodesulfurization of thiophene

Hui Shang, Pengfei Ye, Yude Yue, Tianye Wang, Wenhui Zhang, Sainab Omar, Jiawei Wang

《化学科学与工程前沿（英文）》 2019年 第13卷 第4期   页码 744-758 doi: 10.1007/s11705-019-1839-7

摘要： Hydrodesulfurization (HDS) of thiophene, as a gasoline model oil, over an industrial Ni-Mo/Al O catalyst was investigated in a continuous system under microwave irradiation. The HDS efficiency was much higher (5%‒14%) under microwave irradiation than conventional heating. It was proved that the reaction was enhanced by both microwave thermal and non-thermal effects. Microwave selective heating caused hot spots inside the catalyst, thus improved the reaction rate. From the analysis of the non-thermal effect, the molecular collisions were significantly increased under microwave irradiation. However, instead of being reduced, the apparent activation energy increased. This may be due to the microwave treatment hindering the adsorption though upright S-bind (η ) and enhancing the parallel adsorption (η ), both adsorptions were considered to favor to the direct desulfurization route and the hydrogenation route respectively. Therefore, the HDS process was considered to proceed along the hydrogenation route under microwave irradiation.

关键词： thiophene     microwave irradiation     hydrodesulfurization     non-thermal microwave effect    

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Recent advances in selective acetylene hydrogenation using palladium containing catalysts

Alan J. McCue, James A. Anderson

《化学科学与工程前沿（英文）》 2015年 第9卷 第2期   页码 142-153 doi: 10.1007/s11705-015-1516-4

摘要： Recent advances with Pd containing catalysts for the selective hydrogenation of acetylene are described. The overview classifies enhancement of catalytic properties for monometallic and bimetallic Pd catalysts. Activity/selectivity of Pd catalysts can be modified by controlling particle shape/morphology or immobilisation on a support which interacts strongly with Pd particles. In both cases enhanced ethylene selectivity is generally associated with modifying ethylene adsorption strength and/or changes to hydride formation. Inorganic and organic selectivity modifiers (i.e., species adsorbed onto Pd particle surface) have also been shown to enhance ethylene selectivity. Inorganic modifiers such as TiO change Pd ensemble size and modify ethylene adsorption strength whereas organic modifiers such as diphenylsulfide are thought to create a surface template effect which favours acetylene adsorption with respect to ethylene. A number of metals and synthetic approaches have been explored to prepare Pd bimetallic catalysts. Examples where enhanced selectivity is observed are generally associated with decreased Pd ensemble size and/or hindering of the ease with which an unselective hydride phase is formed for Pd. A final class of bimetallic catalysts are discussed where Pd is not thought to be the primary reaction site but merely acts as a site where hydrogen dissociation and spillover occurs onto a second metal (Cu or Au) where the reaction takes place more selectively.

关键词： acetylene     ethylene     selective hydrogenation     palladium     bimetallic    

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Preparation of polysulfone-based block copolymer ultrafiltration membranes by selective swelling and

《化学科学与工程前沿（英文）》 2022年 第16卷 第5期   页码 745-754 doi: 10.1007/s11705-021-2038-x

摘要： Selective swelling of block copolymers of polysulfone-b-poly(ethylene glycol) is an emerging strategy to prepare new types of polysulfone ultrafiltration membranes. Herein, we prepared nanoporous polysulfone-b-poly(ethylene glycol) ultrafiltration membranes by selective swelling and further promoted their porosity and ultrafiltration performances by using CaCO3 nanoparticles as the sacrificial nanofillers. Different contents of CaCO3 nanoparticles were doped into the solution of polysulfone-b-poly(ethylene glycol), and thus obtained suspensions were used to prepare both self-supported and bi-layered composite structures. Selective swelling was performed on the obtained block copolymer structures in the solvent pair of ethanol/acetone, producing nanoporous membranes with poly(ethylene glycol) lined along pore walls. The CaCO3 nanoparticles dispersed in polysulfone-b-poly(ethylene glycol) were subsequently etched away by hydrochloric acid and the spaces initially occupied by CaCO3 provided extra pores to the block copolymer layers. The porosity of the membranes was increased with increasing CaCO3 content up to 41%, but further increase in the CaCO3 content led to partial collapse of the membrane. The sacrificial CaCO3 particles provided extra pores and enhanced the connectivity between adjacent pores. Consequently, the membranes prepared under optimized conditions exhibited up to 80% increase in water permeance with slight decrease in rejection compared to neat membranes without the use of sacrificial CaCO3 particles.

关键词： block copolymers     selective swelling     ultrafiltration     CaCO3 nanoparticles     sacrificial nanofillers    

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Highly efficient and selective removal of vanadium from tungstate solutions by microbubble floating-extraction

《化学科学与工程前沿（英文）》 2023年 第17卷 第5期   页码 581-593 doi: 10.1007/s11705-022-2235-2

摘要： Selective separation of dissolved tungsten and vanadium is of great significance for the utilization of the secondary resources of these elements. In this work, selective removal of vanadium from tungstate solutions via microbubble floating-extraction was systematically investigated. The results indicated that vanadium can be more easily mineralized over tungsten from tungstate solutions using methyl trioctyl ammonium chloride as mineralization reagent under weak alkaline conditions. Owing to the higher bubble and interface mass transfer rates, high-efficiency enrichment and deep separation of vanadium could be achieved easily. Additionally, the deep recovery of tungsten and vanadium from the floated organic phase could be easily realized using a mixed solution of sodium hydroxide and sodium chloride as stripping agents. The separation mechanism mainly included the formation of hydrophobic complexes, their attachment on the surface of rising bubbles, and their mass transfer at the oil–water interface. Under the optimal conditions, the removal efficiency of vanadium reached 98.5% with tungsten loss below 8% after two-stage microbubble floating-extraction. Therefore, the microbubble floating-extraction could be an efficient approach for separating selectively vanadium from tungstate solutions, exhibiting outstanding advantages of high separation efficiency and low consumption of organic solvents.

关键词： tungsten     vanadium     selective separation     reagent mineralization     microbubble floating-extraction    

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Mechanistic insights into the selective photocatalytic degradation of dyes over TiO/ZSM-11

《环境科学与工程前沿（英文）》 2023年 第17卷 第8期 doi: 10.1007/s11783-023-1701-5

摘要：

● TiO2/ZSM-11 was prepared by a facile solid state dispersion method.

关键词： Selective dye degradation     Photocatalysis     TiO2     ZSM-11     Chemisorption    

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Porous ultrathin-shell microcapsules designed by microfluidics for selective permeation and stimuli-triggered

《化学科学与工程前沿（英文）》   页码 1643-1650 doi: 10.1007/s11705-022-2201-z

摘要： Microcapsules are versatile delivery vehicles and widely used in various areas. Generally, microcapsules with solid shells lack selective permeation and only exhibit a simple release mode. Here, we use ultrathin-shell water-in-oil-in-water double emulsions as templates and design porous ultrathin-shell microcapsules for selective permeation and multiple stimuli-triggered release. After preparation of double emulsions by microfluidic devices, negatively charged shellac nanoparticles dispersed in the inner water core electrostatically complex with positively charged telechelic α,ω-diamino functionalized polydimethylsiloxane polymers dissolved in the middle oil shell at the water/oil interface, thus forming a porous shell of shellac nanoparticles cross-linked by telechelic polymers. Subsequently, the double emulsions become porous microcapsules upon evaporation of the middle oil phase. The porous ultrathin-shell microcapsules exhibit excellent properties, including tunable size, selective permeation and stimuli-triggered release. Small molecules or particles can diffuse across the shell, while large molecules or particles are encapsulated in the core, and release of the encapsulated cargos can be triggered by osmotic shock or a pH change. Due to their unique performance, porous ultrathin-shell microcapsules present promising platforms for various applications, such as drug delivery.

关键词： microcapsule     emulsion     microfluidics     selective permeation     stimuli-triggered release    

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Highly selective and green recovery of lithium ions from lithium iron phosphate powders with ozone

《化学科学与工程前沿（英文）》 2023年 第17卷 第6期   页码 749-758 doi: 10.1007/s11705-022-2261-0

摘要： Since lithium iron phosphate cathode material does not contain high-value metals other than lithium, it is therefore necessary to strike a balance between recovery efficiency and economic benefits in the recycling of waste lithium iron phosphate cathode materials. Here, we describe a selective recovery process that can achieve economically efficient recovery and an acceptable lithium leaching yield. Adjusting the acid concentration and amount of oxidant enables selective recovery of lithium ions. Iron is retained in the leaching residue as iron phosphate, which is easy to recycle. The effects of factors such as acid concentration, acid dosage, amount of oxidant, and reaction temperature on the leaching of lithium and iron are comprehensively explored, and the mechanism of selective leaching is clarified. This process greatly reduces the cost of processing equipment and chemicals. This increases the potential industrial use of this process and enables the green and efficient recycling of waste lithium iron phosphate cathode materials in the future.

关键词： lithium iron phosphate powder     stoichiometric number     selective leaching     lithium recovery    

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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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Design and operational considerations for selective catalytic reduction technologies at coal-fired boilers

Jeremy J. SCHREIFELS, Shuxiao WANG, Jiming HAO

《能源前沿（英文）》 2012年 第6卷 第1期   页码 98-105 doi: 10.1007/s11708-012-0171-4

摘要： By the end of 2010, China had approximately 650 GW of coal-fired electric generating capacity producing almost 75% of the country’s total electricity generation. As a result of the heavy reliance on coal for electricity generation, emissions of air pollutants, such as nitrogen oxides (NO ), are increasing. To address these growing emissions, the Ministry of Environmental Protection (MEP) has introduced new NO emission control policies to encourage the installation of selective catalytic reduction (SCR) technologies on a large number of coal-fired electric power plants. There is, however, limited experience with SCR in China. It is therefore useful to explore the lessons from the use of SCR technologies in other countries. This paper provides an overview of SCR technology performance at coal-fired electric power plants demonstrating emission removal rates between 65% and 92%. It also reviews the design and operational challenges that, if not addressed, can reduce the reliability, performance, and cost-effectiveness of SCR technologies. These challenges include heterogeneous flue gas conditions, catalyst degradation, ammonia slip, sulfur trioxide (SO ) formation, and fouling and corrosion of plant equipment. As China and the rest of the world work to reduce greenhouse gas emissions, carbon dioxide (CO ) emissions from parasitic load and urea-to-ammonia conversion may also become more important. If these challenges are properly addressed, SCR can reliably and effectively remove up to 90% of NO emissions at coal-fired power plants.

关键词： nitrogen oxides (NOx)     coal     selective catalytic reduction (SCR)     air pollution control    

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Low-temperature selective catalytic reduction of NO with NH based on MnO-CeO/ACFN

SHEN Boxiong, LIU Ting, SHI Zhanliang, SHI Jianwei, YANG Tingting, ZHAO Ning

《化学科学与工程前沿（英文）》 2008年 第2卷 第3期   页码 325-329 doi: 10.1007/s11705-008-0053-9

摘要： MnO-CeO/ACFN were prepared by the impregnation method and used as catalyst for selective catalytic reduction of NO with NH at 80°C–150°C. The catalyst was characterized by N-BET, scanning electron microscopy (SEM) and Fourier transform infrared spectroscopy (FT-IR). The fraction of the mesopore and the oxygen functional groups on the surface of activated carbon fiber (ACF) increased after the treatment with nitric acid, which was favorable to improve the catalytic activities of MnO-CeO/ACFN. The experimental results show that the conversion of NO is nearly 100% in the range 100°C–150°C under the optimal preparation conditions of MnO-CeO/ACFN. In addition, the effects of a series of performance parameters, including initial NH concentration, NO concentration and O concentration, on the conversion of NO were studied.

关键词： preparation     conversion     favorable     selective catalytic     MnO-CeO/ACFN    

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Multi-stage ammonia production for sorption selective catalytic reduction of NO

Chen ZHANG, Guoliang AN, Liwei WANG, Shaofei WU

《能源前沿（英文）》 2022年 第16卷 第5期   页码 840-851 doi: 10.1007/s11708-021-0797-1

摘要： Sorption selective catalytic reduction of nitrogen oxides (NOx) (sorption-SCR) has ever been proposed for replacing commercial urea selective catalytic reduction of NOx (urea-SCR), while only the single-stage sorption cycle is hitherto adopted for sorption-SCR. Herein, various multi-stage ammonia production cycles is built to solve the problem of relative high starting temperature with ammonia transfer (AT) unit and help detect the remaining ammonia in ammonia storage and delivery system (ASDS) with ammonia warning (AW) unit. Except for the single-stage ammonia production cycle with MnCl2, other sorption-SCR strategies all present overwhelming advantages over urea-SCR considering the much higher NOx conversion driven by the heat source lower than 100°C and better matching characteristics with low-temperature catalysts. Furthermore, the required mass of sorbent for each type of sorption-SCR is less than half of the mass of AdBlue for urea-SCR. Therefore, the multifunctional multi-stage sorption-SCR can realize compact and renewable ammonia storage and delivery with low thermal energy consumption and high NOx conversion, which brings a bright potential for efficient commercial de-NOx technology.

关键词： selective catalytic reduction (SCR)     nitrogen oxides (NOx)     ammonia     composite sorbent     chemisorption    

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Insight into the promotion mechanism of activated carbon on the monolithic honeycomb red mud catalyst for selective

《环境科学与工程前沿（英文）》 2021年 第15卷 第5期 doi: 10.1007/s11783-020-1337-7

摘要：

• Activated carbon was proposed to be an efficient accelerant for molded red mud catalyst.

关键词： NOx     Selective catalytic reduction     Iron-based catalyst     Red mud     Monolithic catalyst     Activated carbon    

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标题 作者 时间 类型 操作

Synthesis of boron modified CoMo/Al

Hui Shang, Chong Guo, Pengfei Ye, Wenhui Zhang

期刊论文

Catalyst particle shapes and pore structure engineering for hydrodesulfurization and hydrodenitrogenation

期刊论文

Kinetic study of hydrodesulfurization of coker gas oil in a slurry reactor

Haiding XIANG, Tiefeng WANG

期刊论文

Experimental and theoretical study of microwave enhanced catalytic hydrodesulfurization of thiophene

Hui Shang, Pengfei Ye, Yude Yue, Tianye Wang, Wenhui Zhang, Sainab Omar, Jiawei Wang

期刊论文

Recent advances in selective acetylene hydrogenation using palladium containing catalysts

Alan J. McCue, James A. Anderson

期刊论文

Preparation of polysulfone-based block copolymer ultrafiltration membranes by selective swelling and

期刊论文

Highly efficient and selective removal of vanadium from tungstate solutions by microbubble floating-extraction

期刊论文

Mechanistic insights into the selective photocatalytic degradation of dyes over TiO/ZSM-11

期刊论文

Porous ultrathin-shell microcapsules designed by microfluidics for selective permeation and stimuli-triggered

期刊论文

Highly selective and green recovery of lithium ions from lithium iron phosphate powders with ozone

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

Design and operational considerations for selective catalytic reduction technologies at coal-fired boilers

Jeremy J. SCHREIFELS, Shuxiao WANG, Jiming HAO

期刊论文

Low-temperature selective catalytic reduction of NO with NH based on MnO-CeO/ACFN

SHEN Boxiong, LIU Ting, SHI Zhanliang, SHI Jianwei, YANG Tingting, ZHAO Ning

期刊论文

Multi-stage ammonia production for sorption selective catalytic reduction of NO

Chen ZHANG, Guoliang AN, Liwei WANG, Shaofei WU

期刊论文

Insight into the promotion mechanism of activated carbon on the monolithic honeycomb red mud catalyst for selective

期刊论文