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Self-separation ionic liquid catalyst for the highly effective conversion of H_(2)S by α,β-unsaturated carboxylate esters under mild conditions

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Green Energy & Environment 2024年第9期9卷 1440-1448页

作者： Wenjie Xiong Xiaomin Zhang Xingbang Hu Youting Wu Key Laboratory of Mesoscopic Chemistry of MOE School of Chemistry and Chemical EngineeringNanjing UniversityNanjing210023China The Institute of Green Chemistry and Engineering School of Chemistry and Chemical EngineeringNanjing UniversitySuzhouJiangsu215163China

The deep-processing utility of pure hydrogen sulfide (H_(2)S) is a significant direction in natural gas chemical ***,a brand-new strategy of H_(2)S conversion by a,β-unsaturated carboxylate esters into thiols or thioethers using task-specific carboxylate ionic liquids (ILs) as catalyst has been developed,firstly accomplishing the phase separation of product and catalyst without introducing the third *** can be considered as a cascade reaction in which the product selectivity can be controlled by adjusting the molar ratio of H_(2)S to a,β-unsaturated carboxylate ***,the effects of ILs with different anions and cations,intermittent feeding operations,as well as pressure-time kinetic behaviors on cascade reaction were ***,the proposed interaction mechanism of H_(2)S conversion using butyl acrylate catalyzed by[Emim][Ac]was revealed by DFT-based theoretical *** approach enables the self-phase separation promotion of catalyst and product and achieves 99%quantitative conversion under mild conditions in the absence of solvent,making the entire process ecologically ***-efficiency reaction activity can still be maintained after ten cycles of the ***,the good results,combined with its simplicity of operation and the high recyclability of the catalyst,make this green method environmentally friendly and *** is anticipated that this self-separation method mediated by task-specific ILs will provide a feasible strategy for H_(2)S utilization,which will guide its application on an industrial scale.

关键词： Ionic liquid Cascade reaction Self-separation H_(2)S conversion Catalysis

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OH regulator of highly dispersed Ru sites on host Pd nanocrystals for selective ethanol electro-oxidation

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Nano Research 2024年第5期17卷 3863-3871页

作者： Zhihe Xiao Yueguang Chen Renjie Wu Yuwei He Chunfeng Shi Leyu Wang State Key Laboratory of Chemical Resource Engineering College of ChemistryBeijing University of Chemical TechnologyBeijing 100029China Research Institute of Petroleum Processing SINOPECBeijing 100083China

The ethanol oxidation reaction(EOR)is crucial in direct alcohol fuel cells and chemical ***,the electro-oxidation of ethanol molecules to produce acetaldehyde and carbon monoxide can poison the active sites of nanocatalysts,resulting in reduced performance and posing challenges in achieving high activity and selectivity for ethanol *** this study,we employed a dynamic seed-mediated method to precisely modify highly dispersed Ru sites onto well-defined Pd *** oxyphilic Ru sites serve as"OH valves",regulating water dissociation,while the surrounding Pd atomic arrangements control electronic states for the oxidation dehydrogenation of carbonaceous ***,Ru0.040@Pd nanocubes(Ru:Pd=0.04 at.%),featuring(100)facets in Ru-Pd4 configurations,demonstrate an outstanding mass activity of 6.53 A·mgPd^(-1) in EOR under alkaline conditions,which is 6.05 times higher than that of the commercial Pd/C catalyst(1.08 A·mgPd-1).Through in-situ experiments and theoretical investigations,we elucidate that the hydrophilic Ru atoms significantly promote the dynamic evolution of H_(2)O dissociation into OHads species,while the electron redistribution from Ru to adjacent Pd concurrently adjusts the selective oxidation of C_(2) *** host-guest interaction accelerates the subsequent oxidation of carbonaceous intermediates(CH_(3)CO_(ads))to acetate,while preventing the formation of toxic*CHx and*CO species,which constitutes the rate-determining step.

关键词： OH regulator atomic sites ethanol electro-oxidation host-guest interaction

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Alumina supported platinum-ceria catalyst for reverse water gas shift reaction

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Journal of Rare Earths 2025年第2期43卷 284-294,I0002页

作者： Na Jiang Weiwei Wang Haoxin Liu Meiyao Wu Chunjiang Jia Key Laboratory for Colloid and Interface Chemistry Key Laboratory of Special Aggregated MaterialsSchool of Chemistry and Chemical EngineeringShandong UniversityJinan 250100China

The activation of CO_(2)molecules is a fundamental step for their effective *** highdensity oxygen vacancies on the surface of reducible oxides is pivotal for the activation of CO_(2).In this work,we prepared a series of 0.5PtxCe/Al_(2)O_(3)(x=1,5,10,or 20)catalysts with varying Ce loading and 0.5 wt%of Pt for the reverse water gas shift(RWGS)*** size of CeO_(2)particle increases with Ce ***,the 0.5Pt5Ce/Al_(2)O_(3) catalyst with an average CeO_(2)particle size of 5.5 nm exhibits a very high CO_(2)conversion rate(116.4×10^(-5)mol_(CO_(2))/(g_(cat)·s))and CO selectivity(96.1%)at 600℃.Our experimental findings reveal that the small-size CeO_(2)in 0.5Pt5Ce/Al_(2)O_(3) possesses a greater capacity to generate reactive oxygen vacancies,promoting the adsorption and activation of CO_(2).In addition,the oxygen vacancies are cyclically generated and consumed during the reaction,which contributes to the elevated catalytic performance of the *** work provides a general strategy to construct rich oxygen vacancies on CeO_(2)for designing high-performance catalysts in C_(1) chemistry.

关键词： CO_(2)activation Ceria Oxygen vacancies Size-effect Reverse water gas shift reaction Rare earths

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Discontinuous solid solutions of anthracene-phenanthrene:Thermodynamics and crystallization kinetics

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Particuology 2022年第1期20卷 68-76页

作者： Zaixiang Zhang Ling Zhou Qiuxiang Yin School of Chemical Engineering and Technology State Key Laboratory of Chemical EngineeringTianjin UniversityTianjin 300072People's Republic of China

We explored such issues as the formation mechanism,structure and propriety of the solid solutions of anthracene(ANT)-phenanthrene(PHE).Solution crystallization and solid-state grinding were employed to prepare solid solutions under different *** thermal behavior and PXRD scanning results revealed the formation of discontinuous solid solutions,whose melting points and crystal lattices varied linearly with mixed *** with Materials Studio,the formation possibility of solid solutions were investigated by evaluating the change of the *** crystal morphology of the solid solutions have a positive correlation with the change of the major ***,the solution crystallization process of solid solution were studied using the population balance model.

关键词： Discontinuous solid solutions Thermal proprieties Crystal structure Morphology Crystallization kinetics

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Preparation of hollow spherical covalent organic frameworks via Oswald ripening under ambient conditions for immobilizing enzymes with improved catalytic performance

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Nano Research 2023年第1期16卷 281-289页

作者： Hao Zhao Guanhua Liu Yunting Liu Liya Zhou Li Ma Ying He Xiaobing Zheng Jing Gao Yanjun Jiang School of Chemical Engineering and Technology Hebei University of TechnologyTianjin 300130China State Key Laboratory of Biocatalysis and Enzyme Engineering School of Life SciencesHubei UniversityWuhan 430062China

The hollow spherical covalent organic frameworks(COFs)have a wide application prospect thanks to their special ***,the controllable synthesis of uniform and stable hollow COFs is still a *** herein propose a self-templated method for the preparation of hollow COFs through the Ostwald ripening mechanism under ambient conditions,which avoids most disadvantages of the commonly used hard-templating and soft-templating methods.A detailed time-dependent study reveals that the COFs are transformed from initial spheres to hollow spheres because of the inside-out Ostwald ripening *** obtained hollow spherical COFs have high crystallinity,specific surface area(2,036 m^(2)·g^(−1)),stability,and single-batch *** to unique hollow structure,clear through holes,and hydrophobic pore environment of the hollow spherical COFs,the obtained immobilized lipase(BCL@H-COF-OMe)exhibits higher thermostability,polar organic solvent tolerance,and *** BCL@H-COF-OMe also shows higher catalytic performance than the lipase immobilized on non-hollow COF and free lipase in the kinetic resolution of secondary *** study provides a simple approach for the preparation of hollow spherical COFs,and will promote the valuable research of COFs in the field of biocatalysis.

关键词： hollow spherical structure covalent organic framework Oswald ripening mechanism lipase kinetic resolution

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Conversion of syngas into lower olefins over a hybrid catalyst system

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Frontiers of chemical Science and engineering 2024年第10期18卷 95-104页

作者： Qiao Zhao Hongyu Wang Haoting Liang Xiaoxue Han Chongyang Wei Shiwei Wang Yue Wang Shouying Huang Xinbin Ma Key Laboratory for Green Chemical Technology of Ministry of Education Haihe Laboratory of Sustainable Chemical TransformationsSchool of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China School of Materials Science and Engineering National Institute for Advanced MaterialsTKL of Metal and Molecule-Based Material ChemistryNankai UniversityTianjin 300350China State Key Laboratory of Chemical Safety SINOPEC Research Institute of Safety Engineering Co.Ltd.Qingdao 266104China Zhejiang Institute of Tianjin University Ningbo Key Laboratory of Green Petrochemical Carbon Emission Reduction Technology and EquipmentNingbo 315200China

Lower olefins,produced from syngas through Fischer-Tropsch synthesis,has been gaining worldwide attention as a non-petroleum ***,the process demonstrates limited selectivity for target ***,a hybrid catalyst system utilizing Fe-based catalyst and SAPO-34 was shown to enhance the selectivity toward lower olefins.A comprehensive study was conducted to examine the impact of various operating conditions on catalytic performance,such as space velocity,pressure,and temperature,as well as catalyst combinations,including loading pattern,and mass ratio of metal and *** findings indicated that the addition of SAPO-34 was beneficial for enhancing catalytic ***,compared with AlPO-34 zeolite,the strong-acid site on SAPO-34 was identified to crack the long-chain hydrocarbons,thus contributing to the lower olefin ***,an excess of strong-acid sites was found to detrimentally impact the selectivity of lower olefins,attributed to the increased aromatization and polymerization of lower *** detailed analysis of a hybrid catalyst in Fischer-Tropsch synthesis provides a practical strategy for improving lower olefins selectivity,and has broader implications for the application of hybrid catalyst in diverse catalytic systems.

关键词： Fischer-Tropsch synthesis lower olefins SAPO-34 hybrid catalyst Febased catalyst

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Conversion of lignin oil and hemicellulose derivative into high-density jet fuel

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Journal of Energy Chemistry 2023年第2期77卷 452-460,I0012页

作者： Sichao Yang Chengxiang Shi Zhensheng Shen Lun Pan Zhenfeng Huang Xiangwen Zhang Ji-Jun Zou Key Laboratory for Green Chemical Technology of Ministry of Education School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China Collaborative Innovative Center of Chemical Science and Engineering(Tianjin) Tianjin 300072China Haihe Laboratory of Sustainable Chemical Transformations Tianjin 300192China

Synthesizing high-density fuel from lignocellulose can not only achieve green and low-carbon development,but also expand the feedstock source of hydrocarbon ***,we reported a route of producing high-density fuel from lignin oil and hemicellulose derivative cyclopentanol through alkylation and hydrodeoxygenation,HY with SiO_(2)/Al_(2)O_(3) molar ratio of 5.3 was screened as the alkylation catalyst in the reaction of model phenolic compounds and mixtures,and the reaction conditions were optimized to achieve conversion of phenolic compounds higher than 87%and selectivity of bicyclic and tricyclic products higher than 99%.Then two phenolic pools simulating the composition of two typic lignin oils were studied to validate the alkylation and analyze the competition mechanism of phenolic compounds in mixture ***,real lignin oil from depolymerized of beech powder was tested,and notably80%of phenolic monomers in the oil were converted into fuel *** hydrodeoxygenation,the alkylated product was converted to fuel blend with a density of 0.91 g/mL at 20℃and a freezing point lower than-60℃,very promising as high density *** work provides a facile and energyefficient way of synthesizing high-performance jet fuel directly from lignocellulosic derivatives,which decreases processing energy consumption and improve the utilization rate of feedstock.

关键词： High-density fuel Biofuel Lignin oil Alkylation Hydrodeoxygenation

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A homogeneous and mechanically stable artificial diffusion layer using rigid-flexible hybrid polymer for high-performance lithium metal batteries

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Journal of Energy Chemistry 2023年第1期76卷 631-638,I0015页

作者： Zhenkang Lin Yuyan Ma Wei Wang Yu He Menghao Wang Jun Tang Cheng Fan Kening Sun Beijing Key Laboratory for Chemical Power Source and Green Catalysis School of Chemistry and Chemical EngineeringBeijing Institute of TechnologyBeijing 100081China

Artificial solid electrolyte interphase(SEI) is promising to inhibit uncontrollable lithium dendrites and enable long cycling stability for lithium metal batteries. However, the essential mechanical stability is limited since organic layers generally have low modulus whereas intrinsic brittleness for inorganic ones remains a great concern. Polymer-based SEIs with rigid and flexible chains in adequate mechanical properties are supposed to address this issue. Herein, a homogeneous and mechanically stable diffusion layer is achieved by blending rigid chains of polyphenylene sulfone(PPSU) with flexible chains of poly(vinylidene fluoride)(PVDF) in a hybrid membrane, enabling uniform diffusion and stabilizing the lithium metal anode. The Li||Cu cell with the protected electrode exhibits a long lifetime more than 450 cycles(0.5 m A cm^(-2), 1.0 m A h cm^(-2))(fourfold longer than the control group) with higher average Coulombic efficiency of 98.7%. Enhanced performances are also observed at Li||Li and full cell configurations. The improved performances are attributed to the controlled morphology and stable interphase, according to scanning electron microscopy(SEM) and electrochemical impedance. This research advances the idea of uniform lithium plating and provides a new insight on how to create a homogeneous and mechanically stable diffusion layer using rigid-flexible polymers.

关键词： Lithium metal battery Lithium dendrite Uniform diffusion Rigid-flexible artificial layer Electrochemical impedance

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Peak-like three-dimensional CoFe_(2)O_(4)/carbon nanotube decorated bamboo fabrics for simultaneous solar-thermal evaporation of water and photocatalytic degradation of bisphenol A

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Journal of Materials Science & technology 2024年第12期179卷 40-49页

作者： Rui-Jie Pan Jing Wu Jin Qu Tingting Zhang Fan-Zhen Jiao Mang Zhao Meng-Yan Han Xiaofeng Li Zhong-Zhen Yu State Key Laboratory of Organic-Inorganic Composites College of Materials Science and EngineeringBeijing University of Chemical TechnologyBeijing 100029China Beijing Key Laboratory of Advanced Functional Polymer Composites Beijing University of Chemical TechnologyBeijing 100029China

Catalytic CoFe_(2)O_(4) and solar-thermal carbon nanotube decorated bamboo fabrics(CCBF)are fabricated for integrating efficient solar steam generation from wastewater with catalytic degradation of its organic *** to the numerous porous channels and polar groups of bamboo fabric and the efficient solar-thermal energy conversion of black carbon nanotubes,the porous and hydrophilic CCBF exhibits fast upward transport of water,efficient solar light absorption,and high solar-thermal energy conversion *** decorated CoFe_(2)O_(4) not only enhances the solar-thermal energy conversion efficiency of CCBF but also activates potassium peroxymonosulfate to generate abundant highly active species for catalytic degradation of bisphenol A(BPA).Furthermore,folding the CCBF into a peak-like 3D evaporator can en-hance solar energy utilization,and gain environmental energy for promoting solar-thermal water evapo-ration and catalytic degradation *** 3D CCBF evaporator achieves a water evaporation rate of 2.72 kg m^(-2) h^(-1) under 1-sun ***,100%of the BPA in the seawater can be degraded within 10 *** exceptional high purification efficiency of 27.72 kg m^(-2) h^(-1) is achieved with the 3D evaporator during a long-term treatment of BPA-containing seawater under 1-sun *** work demonstrates efficient purification of seawater/wastewater with both metal ions and organic pollutants by simultaneous solar-thermal evaporation of water and catalytic degradation of organic pollutants.

关键词： Solar-thermal water evaporation Seawater desalination Catalytic degradation Carbon nanotubes CoFe_(2)O_(4)

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Understanding of the electrochemical behaviors of aqueous zinc-manganese batteries:Reaction processes and failure mechanisms

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Green Energy & Environment 2022年第5期7卷 858-899页

作者： Xinyu Luo Wenchao Peng Yang Li Fengbao Zhang Xiaobin Fan School of Chemical Engineering and Technology State Key Laboratory of Chemical EngineeringCollaborative Innovation Center of Chemical Science and EngineeringTianjin UniversityTianjin300072China Chemistry and Chemical Engineering Guangdong Laboratory Shantou515031China

As one of the most common cathode materials for aqueous zinc-ion batteries(AZIBs),manganese oxides have the advantages of abundant reserves,low cost,and low ***,the electrochemical mechanism at the cathode of aqueous zinc-manganese batteries(AZMBs) is complicated due to different electrode materials,electrolytes and working *** complicated mechanisms severely limit the research progress of AZMBs system and the design of cells with better ***,the mechanism of AZMBs currently recognized by most researchers according to the classification of the main ions involved in the faradaic reaction is introduced in the *** a series of reasons that affect the electrochemical behavior of the battery are ***,the failure mechanisms of AZMBs over prolonged cycling are discussed,and the current insufficient research areas of the system are explained,along with the direction of further research being prospected.

关键词： battery manganese electrochemical

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