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Cobalt-nitrogen co-doped porous carbon sphere as highly efficient catalyst for liquid-phase cyclohexane oxidation with molecular oxygen and the active sites investigation

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Frontiers of chemical Science and engineering 2024年第3期18卷 101-112页

作者： Lei Chen Yuan Sun Jinshan Chi Wei Xiong Pingle Liu Fang Hao College of chemical engineering National&Local United Engineering Research Centre for Chemical Process Simulation and IntensificationXiangtan UniversityXiangtan411105China

The selective oxidation of cyclohexane to cyclohexanone and cyclohexanol(KA oil)is a challenging issue in the chemical industry.At present the industrial conversion of cyclohexane to cyclohexanone and cyclohexanol is normally controlled at less than 5%selectivity.Thus,the development of highly active and stable catalysts for the aerobic oxidation of cyclohexane is necessary to overcome this low-efficiency process.Therefore,we have developed a cobalt-nitrogen co-doped porous sphere catalyst,Co-NC-x(x is the Zn/Co molar ratio,where x=0,0.5,1,2,and 4)by pyrolyzing resorcinol-formaldehyde resin microspheres.It achieved 88.28%cyclohexanone and cyclohexanol selectivity and a cyclohexane conversion of 8.88%under Co-NC-2.The results showed that the introduction of zinc effectively alleviated the aggregation of Co nanoparticles and optimized the structural properties of the material.In addition,Co0 and pyridinic-N are proposed to be the possible active species,and their proportion efficiently increased in the presence of Zn^(2+)species.In this study,we developed a novel strategy to design highly active catalysts for cyclohexane oxidation.

关键词： KA oil production cyclohexane selective oxidation cobalt-nitrogen co-doped porous carbon spheres metal-organic framework

Synthesis of spherical nano-ZSM-5 zeolite with intergranular mesoporous for alkylation of ethylbenzene with ethanol to produce m-diethylbenzene

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Chinese Journal of chemical engineering 2024年第3期67卷 298-309页

作者： Siyue Wang Jinhong Li Qingxin Xu Shengjie Song Yu'ni Jiang Lidong Chen Xin Shi Weiguo Cheng Faculty of Chemistry and chemical engineering Liaoning Normal UniversityDalian 110629China Beijing Key Laboratory of Ionic Liquids Clean process Key Laboratory of Green Process and EngineeringInstitute of Process EngineeringChinese Academy of SciencesBeijing 100190China

Catalytic synthesis of m-diethylbenzene(m-DEB)through alkylation of ethylbenzene(EB)may be a promising alternative route in comparison with traditional rectification of mixed DEB,for which the top priority is to develop efficient and stable heterogeneous catalysts.Here,the spherical nano-ZSM-5 zeolite with abundant intergranular mesoporous is synthesized by the seed-mediated growth method for alkylation of EB with ethanol to produce m-DEB.The results show that the spherical nano-ZSM-5 zeolite exhibits better stability and higher alkylation activity at a lower temperature than those of commercial micropore ZSM-5.And then,the spherical nano-ZSM-5 is further modified by La_(2)O_(3) through acid treatment followed by immersion method.The acid treatment causes nano-ZSM-5 to exhibit the increased pore size but decreased the acid sites,and subsequent La_(2)O_(3) loading reintroduces the weak acid sites.As a result,the HNO_(3)-La_(2)O_(3)-modified catalyst exhibits a slight increase in EB conversion and DEB yield in comparison with unmodified one,and meanwhile,it still maintains high m-DEB selectivity.The catalyst after acid treatment achieves higher catalytic stability besides maintaining the high alkylation activity of EB with ethanol.The present study on the spherical nano-HZSM-5 zeolite and its modification catalyst with excellent alkylation ability provides new insights into the production of mDEB.

关键词： Zeolite Modification Alkylation reaction m-diethylbenzene Catalyst Fixed-bed

Three-stage pyrolysis–steam reforming–water gas shift processing of household,commercial and industrial waste plastics for hydrogen production

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Waste Disposal and Sustainable Energy 2024年第1期6卷 25-37页

作者： Rayed Alshareef Robert Sait-Stewart Mohamad A.Nahil Paul T.Williams School of chemical and process engineering University of LeedsLeedsLS29JTUK

Five common single plastics and nine different household,commercial and industrial waste plastics were processed using a three-stage(i)pyrolysis,(ii)catalytic steam reforming and(iii)water gas shift reaction system to produce hydrogen.Pyrolysis of plastics produces a range of different hydrocarbon species which are subsequently catalytically steam reformed to produce H_(2)and CO and then undergo water gas shift reaction to produce further H_(2).The process mimics the commercial process for hydrogen production from natural gas.processing of the single polyalkene plastics(high-density polyethylene(HDPE),low-density polyethylene(LDPE),and polypropylene(PP))produced similar H_(2)yields between 115 mmol and 120 mmol per gram plastic.Even though PS produced an aromatic product slate from the pyrolysis stage,further stages of reforming and water gas shift reaction produced a gas yield and composition similar to that of the polyalkene plastics(115 mmol H_(2)per gram plastic).PET gave significantly lower H_(2)yield(41 mmol per gram plastic)due to the formation of mainly CO,CO_(2)and organic acids from the pyrolysis stage which were not conducive to further reforming and water gas shift reaction.A mixture of the single plastics typical of that found in municipal solid waste produced a H_(2)yield of 102 mmol per gram plastic.Knowing the gas yields and composition from the single plastics enabled an estimation of the yields from a simulated waste plastic mixture and a‘real-world’waste plastic mixture to be determined.The different household,commercial and industrial waste plastic mixtures produced H_(2)yields between 70 mmol and 107 mmol per gram plastic.The H_(2)yield and gas composition from the single waste plastics gave an indication of the type of plastics in the mixed waste plastic samples.

关键词： Waste plastic Hydrogen Catalyst Pyrolysis reforming Water gas shift

Alternative technology for the recovery of butyl acetate with low concentration:high capacity adsorbent and high efficiency adsorption

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Green chemical engineering 2024年第2期5卷 236-244页

作者： Chi Ma Lihong Zhao Zhengxin Mao Hao Su Qingfen Liu CAS Key Laboratory of Green process and engineering Institute of Process EngineeringChinese Academy of SciencesBeijing100190China School of chemical engineering University of Chinese Academy of SciencesBeijing100049China

Industrial pharmaceutical wastewater usually contains butyl acetate(BA)with a concentration of 1 wt%-7 wt%,and the traditional method for BA recovery is distillation with high energy consumption.Adsorption method is developed to recover BA with low concentration for the high efficiency and low energy consumption.Medium polar polyacrylate resins with macroporous structure of 233.1 nm and average particle size of about 526.5μm are successfully synthesized by suspension polymerization and used for the BA adsorption and desorption.The maximum adsorption capacity reaches 171.1 mg g^(-1)with relative standard deviation(RSD)value of 0.2%,which is more than twice the results in the literature.The BA desorption rate is 97.0%at 100℃with RSD value of 0.4%,and the resins are beneficial to the reuse in the adsorption-desorption cycle.The adsorption thermodynamics and kinetics are investigated,and the BA adsorption is a spontaneous and endothermic process with the increase of disorder degree.This process is mainly contributed by physical absorption and agree well with Freundlich model and pseudo-first-order adsorption kinetic model.The adsorption method avoids boiling a large amount of wastewater and hopefully provides a novel alternative technology for the BA recovery.

关键词： Butyl acetate recovery Resin adsorption Desorption Thermodynamics Kinetics

Insight into the role of ethylene glycol on thermodynamics and nucleation kinetics of dimethyl terephthalate in mixed solvent system

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Particuology 2024年第2期85卷 1-12页

作者： Yujin Zhang Chunyan Shi Jing Tang Li Liu Dongxia Yan Qing Zhou Xingmei Lu Songyan Jia College of chemical engineering Shenyang University of Chemical TechnologyShenyang110142China Bejing Key Laboratoryoflonic Liquids Clean process CAS Key LaboratoryofGreen Process and EngineeringState Key Laboratoryof Multiphase Complex SystemsInstitute of Process EngineeringChinese Academy of SciencesBeijing100190China School of Chemistry and chemical engineering Qingdao UniversityQingdao266071China Henan Institute of Advanced Technology Zhengzhou UniversityZhengzhou450001China School of chemical engineering University of Chinese Academy of SciencesBeijing100049China

Dissolution and nucleation are two essential processes for industrial crystallization.This paper in-vestigates the effect of ethylene glycol addition on the crystallization behavior of dimethyl terephthalate(DMT)in solution.The DMT solubility in mixed solvent system(methanol-ethylene glycol)was deter-mined by isothermal satiation approach,and the solubility was associated using seven models.The model fitting results were consistent with the experimental values.Based on the results,the metastable zone width(MSZW)of DMT was detected by the polythermal approach;the modified Sangwal's theory was used to investigate the nucleation behavior,which can provide a new way of thought for better analysis of the crystallization behavior.The results demonstrated that MSZW was associated with various elements,such as cooling rate,saturation temperature and mass fraction of ethylene glycol.The addition of ethylene glycol slowed down the nucleation rate as shown by the broadening of MSZW.We derive the solid-liquid interface energy,the nucleation driving force,the critical nucleation size and the critical Gibbs free energy according to the classical nucleation theory.It is demonstrated that the nucleation driving force and the solid-liquid interface energy are dependent and jointly influence the MSZW.

关键词： Dissolution Nucleation Solubility Apparent thermodynamic parameters Metastable zone width Solid-liquid interface energy

Role of methoxy and C_(α)-based substituents in electrochemical oxidation mechanisms and bond cleavage selectivity of β-O-4 lignin model compounds

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Green Energy & Environment 2024年第1期9卷 114-125页

作者： Yang Zhou Qiang Zeng Hongyan He Kejia Wu Fuqiao Liu Xuehui Li School of Chemistry and chemical engineering The Guangdong Provincial Key Laboratory of Green Chemical Product TechnologyState Key Laboratory of Pulp and Paper EngineeringSouth China University of TechnologyGuangzhouGuangdong510640China CAS Key Laboratory of Green process and engineering Institute of Process EngineeringChinese Academy of SciencesBeijing100190China

In order to better understand the specific substituent effects on the electrochemical oxidation process of β-O-4 bond, a series of methoxyphenyl type β-O-4 dimer model compounds with different localized methoxyl groups, including 2-(2-methoxyphenoxy)-1-phenylethanone, 2-(2-methoxyphenoxy)-1-phenylethanol, 2-(2-methoxyphenoxy)-1-(4-methoxyphenyl)ethanone, 2-(2-methoxyphenoxy)-1-(4-methoxyphenyl)ethanol, 2-(2,6-dimethoxyphenoxy)-1-(4-methoxyphenyl)ethanone, 2-(2,6-dimethoxyphenoxy)-1-(4-methoxyphenyl)ethanol have been selected and their electrochemical properties have been studied experimentally by cyclic voltammetry, and FT-IR spectroelectrochemistry. Combining with electrolysis products distribution analysis and density functional theory calculations, oxidation mechanisms of all six model dimers have been explored. In particular, a total effect from substituents of both para-methoxy(on the aryl ring closing to Cα) and Cα-OH on the oxidation mechanisms has been clearly observed, showing a significant selectivity on the Cα-Cβbond cleavage induced by electrochemical oxidations.

关键词： Lignin model compounds β-O-4 dimers Electrochemical oxidation Oxidation mechanisms Substituent effect

Recent Advances in Catalytic Carbonylation Reactions in Alternative Reaction Media

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Chinese Journal of Chemistry 2024年第4期42卷 406-429页

作者： Csaba Árvai László T.Mika department of chemical and Environmental process engineering Faculty of Chemical Technology and BiotechnologyBudapest University of Technology and EconomicsMűegyetem rkp.3H-1111 BudapestHungary

Since the discovery of the hydroformylation(oxo-synthesis or Roelen reaction)and the Reppe-reaction,the transition metal-catalyzed carbonylation reactions,providing versatile,facile,and even atom-economic methods for the selective incorporation of C=O functionality to various skeletons,have gained tremendous importance in synthetic organic chemistry from laboratories to industrial applications.The carbonylation of carbon-carbon multiple bonds,aromatic halides,triflates,etc.,in the presence of various nucleophiles has led the way to produce aldehydes,carboxylic acids,esters,amides,etc.,in the fine chemical industry.However,these protocols usually proceed in conventional,fossil-based,and usually toxic reaction environments.Thus,several attempts have been directed to developing efficient carbonylation methods in alternative,less harmful,non-fossil-based and even in renewable reaction media.In this review,we overview the recent applications of alternative solvents such as water,biomass-based alcohols,γ-valerolactone(GVL),2-methyltetrahydrofuran(2-MeTHF),ionic liquids(ILs),deep eutectic solvents(DES),alkyl levulinates,limonene,α-pinene,and dimethyl carbonate as well as fluorous media to improve efficiency,safety and environmentally benign nature of carbonylation protocols.

关键词： Carbonylation Catalysis Solvents Green chemistry Carbon monoxide Transition metals Homogeneous catalysis Palladium

Event-triggered sliding mode control of linear repetitive processes and its application in metal rolling process

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Science China(Information Sciences) 2024年第3期67卷 167-181页

作者： Xinyu LV Yugang NIU James LAM Key Laboratory of Smart Manufacturing in Energy chemical process (East China University of Science and Technology) Ministry of Education department of Mechanical engineering The University of Hong Kong

This paper investigates the design problem of a sliding mode controller for linear repetitive processes(LRPs) with a finite pass length on each pass. Under limited communication resources, an eventtriggered mechanism is implemented from the sensors to the controller, whose triggered sequence is consistent with the evolution direction of LRPs. To periodically orchestrate communication between the controller and actuator, a round-robin scheduling mechanism is established based on the pass length. A sliding function involving the state and pass profile is constructed, and the sliding mode controller is designed using triggered states and pass profile signals. Feasible controller gains are attained to ensure the stability of the resultant closed-loop system. Finally, the proposed strategy is implemented for a multi-roll metal rolling process.

关键词： event-triggered mechanism linear repetitive processes metal rolling process round-robin scheduling sliding mode control

Effects of orientation on the fatigue crack growth behaviors of the ZK60 magnesium alloy in air and PBS

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Journal of Magnesium and Alloys 2024年第1期12卷 281-294页

作者： Jiaqi Hu Zheng Liu Zuoliang Ning Hong Gao School of chemical engineering and Technology Tianjin UniversityTianjin 300072China Tianjin Key Laboratory of chemical process Safety and Equipment Technology Tianjin 300072China

Strong anisotropic corrosion and mechanical properties caused by specimen orientations greatly limit the applications of wrought magnesium alloys.To investigate the influences of specimen orientation,the corrosion tests and(corrosion)fatigue crack growth tests were conducted.The rolled and transverse surfaces of the materials show distinct corrosion rate differences in the stable corrosion stage,but the truth is the opposite for the initial stage of corrosion.In air,specimen orientations have a significant influence on the plastic deformation mechanisms near the crack tip,which results in different fatigue fracture surfaces and cracking paths.Compared with R-T specimens,N-T specimens show a slower fatigue crack growth(FCG)rate in air,which can be attributed to crack closure effects and deformation twinning near the crack tip.The corrosion environment will not significantly change the main plastic deformation mechanisms for the same type of specimen.However,the FCG rate in phosphate buffer saline(PBS)is one order of magnitude higher than that in air,which is caused by the combined effects of hydrogen-induced cracking and anodic dissolution.Owing to the similar corrosion rates at crack tips,the specimens with different orientations display close FCG rates in PBS.

关键词： Magnesium alloy Orientation Corrosion Fatigue crack growth