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3D multiphase flow simulation of Marangoni convection on reactive absorption of CO_(2) by monoethanolamine in microchannel

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Chinese Journal of chemical engineering 2022年第3期35卷 370-377页

作者： Shuai Chen Jiahong Lan Yu Zhang Jia Guo Zhikai Cao Yong Sha Department of Chemical and Biochemical Engineering College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China

A multiphase flow 3D numerical simulation method employing the coupled volume of fluid(VOF)and level set model is established to study the reactive absorption of CO_(2)by the monoethanolamine(MEA)aqueous solution in a falling film microchannel.Based on the flow-reaction-mass transfer model of the MEA-CO_(2)system in the falling film microchannel,the enhancement effect of the Marangoni convection in this reactive absorption process is analyzed.The enhancement factor of the Marangoni convection obtained in this work is in good agreement with experimental results in the literature.With consideration of the absorption ratio as well as the enhancement effect of the Marangoni convection,the influence of different MEA concentrations on absorption of CO_(2)is investigated.Furthermore,the appropriate MEA concentration for absorption enhanced by the Marangoni convection is acquired.

关键词： Numerical simulation Microchannel Falling film Marangoni convection MEA-CO_(2)

Supported catalytic packing prepared from ceramic packing for reactive distillation of ethyl acetate

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Chinese Journal of chemical engineering 2022年第10期50卷 205-214页

作者： Zhiwei Wang Jiannan Shi Xiaonan Liu Zhikai Cao Yong Sha Department of Chemical and Biochemical Engineering College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China

In this work,a strategy of"etching-modification filling-graft copolymerization"was proposed to load the acidic ionic polyionic liquid on the smooth ceramic surface.In this way,commercial ceramic Raschig rings were successfully transformed into the supported catalytic packing for the reactive distillation,and were further evaluated with esterification reaction of ethyl acetate by means of the fully mixed reactor,the ultrasonic destruction,the cyclic catalysis reaction and the lab-scale distillation column experiment.This catalyst coating has good adhesion with the substrate.It can withstand 24 h of ultrasound damage and shows good stability in three cycle catalytic experiments.This kind of coated catalyst has better catalytic activity than the commercial Amberlyst 15 dry.In the lab-scale reaction distillation,the supported catalyst Raschig ring can achieve a higher conversion in comparison with the tea bag catalytic packing of Amberlyst 15 dry under some conditions.

关键词： Supported catalyticpacking Ethyl acetate Reactive distillation Bonding strength

Hierarchical monolithic carbon with high transfer performance for hydrogen evolution reaction

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Journal of Energy Chemistry 2022年第10期31卷 41-48,I0002页

作者： Yazhang Lin Weijie Zhu Yunhua Li Department of Chemical and Biochemical Engineering College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005FujianChina

Electrocatalysis is an efficient green process for energy conversion.However,for gas-related electrocatalytic reaction,sluggish gas transport has inhibited significantly the promotion of electrocatalytic performances.Herein,hierarchical monolithic material 3 DPC-650 and 3 DPC-650@Ni/Ni(OH)_(2) were prepared by3 D printing polyethyleneimine cross-linking oxygenated carbon nanotube and following nickel electrodeposition.3 DPC-650 and 3 DPC-650@Ni/Ni(OH)_(2) have regular pore structure in consistence with3 D printing design and uniform dispersed elements.Amide bonds and carbon defects are presented on the surface of 3 DPC-650 and 3 DPC-650@Ni/Ni(OH)_(2) as well as uniformly distributed β-Ni(OH)_(2) on3 DPC-650@Ni/Ni(OH)_(2).3 DPC-650 and 3 DPC-650@Ni/Ni(OH)_(2) present lower overpotentials of 322 and160 mV for hydrogen evolution reaction in 1.0 M KOH at 50 mA cm^(-2),respectively.The ordered channel,high turnover frequency and electrochemically active surface area,hydrophilic and aerophobic properties result in the higher performance of 3 DPC-650 and 3 DPC-650@Ni/Ni(OH)_(2) than traditional supports(carbon paper,carbon cloth,and nickel foam) and electrocatalysts.This work provides an efficient pathway for design and preparation of the monolithic electrocatalyst and electrode used for electrochemical reactions where gas is involved.

关键词： 3D printing Hierarchical structure Monolith Mass transfer Charge transfer Hydrogen evolution reaction

Effects of ancillary ligands in acceptorless benzyl alcohol dehydrogenation mediated by phosphine-free cobalt complexes

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Frontiers of chemical Science and engineering 2023年第3期17卷 314-325页

作者： Yan Xu Lu Wang Junwei Wu Guanzhong Zhai Daohua Sun Department of Chemical and Biochemical Engineering College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China Department of Chemical and Biochemical Engineering National Engineering Laboratory for Green Chemical Productions of Alcohols−Ethers−EstersCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China Luoyang Ship Material Institute Luoyang 471039China

Acceptorless alcohol dehydrogenation stands out as one of the most promising strategies in hydrogen storage technologies.Among various catalytic systems for this reaction,cost-effective molecular catalysts using phosphine-free ligands have gained considerable attention.However,the central challenge for using non-precious metals is to overcome the propensity of reacting by oneelectron pathway.Herein,we synthesized a phosphine-freeη^(5)-C_(5)Me_(5)-Co complex by using the metal-ligand cooperative strategy and compared its activity with analogous catalysts toward acceptorless alcohol dehydrogenation.The catalyst showed excellent performance with a turnover number of 130.4 and a selectivity close to 100%.The improved performance among the class ofη^(5)-C_(5)Me_(5)-Co complexes could be attributed to the more accessible Co center and its cooperation with the redox-active ligand.To further study the systematic structure-activity relationship,we investigated the electronic structures ofη^(5)-C_(5)Me_(5)-Co complexes by a set of characterizations.The results showed that the redox-active ligand has a significant influence on theη^(5)-C_(5)Me_(5)-Co moiety.In the meantime,the proximal O−/OH group is beneficial for shuttling protons.For the catalytic cycle,two dehydrogenation scenarios were interrogated through density functional theory,and the result suggested that the outer-sphere pathway was preferred.The formation of a dihydrogen complex was the rate-determining step with aΔG value of 16.9 kcal∙mol‒1.The electron population demonstrated that theη^(5)-C_(5)Me_(5)ligand played a key role in stabilizing transition states during dehydrogenation steps.This work identified the roles of vital ligand components to boost catalytic performance and offered rationales for designing metal-ligand cooperative nonprecious metal complexes.

关键词： acceptorless alcohol dehydrogenation η^(5)-C_(5)Me_(5)-Co metal-ligand cooperation theoretical calculation

Measurement and correlation of solid–liquid phase equilibria for binary and ternary systems consisting of N-vinylpyrrolidone, 2-pyrrolidone and water

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Chinese Journal of chemical engineering 2018年第4期26卷 806-811页

作者： Ao Su Sifang Li Department of Chemical and Biochemical Engineering College of Chemistry and Chemical Engineering Xiamen University

The solid–liquid equilibria(SLE)for binary and ternary systems consisting of N-Vinylpyrrolidone(NVP),2-Pyrrolidone(2-P)and water are measured.The phase diagrams of NVP(1)+2-P(2),NVP(1)+water(2),NVP(1)+2-P(2)+1 wt%water(3)and NVP(1)+2-P(2)+2 wt%water(3)are identified as simple eutectic type with the eutectic points at 263.75 K(x_(1E)=0.5427),251.65 K(x_(1E)=0.3722),260.25 K(x_(1E)=0.5031)and256.55 K(x_(1E)=0.4684),respectively.The phase diagram of 2-P(1)+water(2)has two eutectic points(x_(1E)=0.1236,T_E=259.15 K and x_(1E)=0.7831,T_E=286.15 K)and one congruent melting point(x_(1C)=0.4997,T_C=303.55 K)because of the generation of a congruently melting addition compound:2-P·H_2O.The ideal solubility and the UNIFAC models were applied to predict the SLE,while the Wilson and NRTL models were employed in correlating the experimental data.The best correlation of the SLE data has been obtained by the Wilson model for the binary system of NVP+2-P.The UNIFAC model gives more satisfactory predictions than the ideal solubility model.

关键词：二进制液体组成系统关联测量水 NVP

Modified correlation for minimum fluidization velocity of low-density particles in inverse liquid-solid fluidized beds

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Particuology 2022年第12期71卷 56-62页

作者： Michael Nelson Saleh Srabet Tian Nan Dominic Pjontek Jesse Zhu Collaborative Innovation Center of chemical Science and engineering School of Chemical Engineering and TechnologyTianjin UniversityChina Particle Technology Research Centre Department of Chemical and Biochemical EngineeringWestern UniversityCanada

The minimum fluidization velocity(U_(mf))is a key parameter for the scale-up of inverse liquid-solid flu-idized beds.Theoretical predictions using common correlations were compared against experimental minimum fluidization velocity measurements of low density(28-638 kg/m^(3)),0.80-1.13 mm Styrofoam particles in a fluidized bed with a height of 4.5 m and 0.2 m diameter.The average absolute relative deviation for the predicted minimum fluidization velocity for particles below 300 kg/m^(3) was above 40%using the studied common correlations.A modified Wen and Yu correlation was thus proposed based on novel and past measurements with low-density and small-diameter particles,expanding the range for predicting U_(mf).The new correlation predicted U_(mf) with deviations below 15%for ST028,ST122 and ST300.This modified correlation also improved U_(mf) predictions for comparable particles from a previous study,demonstrating its validity for a larger range of low-density particles.

关键词： Liquid-solid fluidization Inverse fluidization Minimum fluidization velocity Low-density particles

Acute and chronic toxicity of nickel to nitrifiers at different temperatures

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Journal of Environmental Sciences 2019年第8期31卷 169-178页

作者： Xiaoguang Liu Mohammad M.I.Chowdhury Masuduz Zaman Mingu Kim George Nakhla department of Civil and Environmental engineering University of Western Ontario Department of Chemical and Biochemical Engineering University of Western Ontario

This study investigated the acute nickel toxicity on nitrification of low ammonia synthetic wastewater at 10, 23, and 35°C. The nickel inhibition half-velocity constants(K_(I,Ni)) for ammonia oxidizing bacteria(AOB) and nitrite oxidizing bacteria(NOB) based on Ni/MLSS ratio at 10, 23, and 35°C were 5.4 and 5.6 mg Ni/g MLSS, 4.6 and 3.5 mg Ni/g MLSS, and 9.1 and 2.7 mg Ni/g MLSS, respectively. In addition, chronic toxicity of nickel to nitrification of low ammonia synthetic wastewater was investigated at 10°C in two sequencing batch reactors(SBRs). Long-term SBRs operation and short-term batch tests were comparable with respect to the extent of inhibition and corresponding Ni/MLSS ratio. The μ_(max), b, and K_o of AOB were 0.16 day^(-1), 0.098 day^(-1) and 2.08 mg O_2/L after long-term acclimatization to nickel of 1 mg/L at 10°C, high dissolved oxygen(DO)(7 mg/L) and long solids retention time(SRT) of 63–70 days. Acute nickel toxicity of nitrifying bacteria was completely reversible.

关键词： Nickel inhibition Temperature Nitrifying culture Activated sludge Toxicity

Component analysis and risk assessment of biogas slurry from biogas plants

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Chinese Journal of chemical engineering 2022年第4期35卷 182-191页

作者： Lanting Ke Xiaobin Liu Bingqing Du Yuanpeng Wang Yanmei Zheng Qingbiao Li Department of Chemical and Biochemical Engineering College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China College of Food and Biology engineering Jimei UniversityXiamen 361021China

Massive amounts of biogas slurry are produced due to the development of biogas plants.The pollution features and the risk of biogas slurry were fully evaluated in this work.Thirty-one biogas slurry samples were collected from sixteen different cities and five different raw materials biogas plants(e.***.cattle manure,swine manure,straw-manure mixture,kitchen waste and chicken manure).The chemical oxygen demand(COD),ammonia nitrogen(NH_(4)^(+)-N),anions(e.g.Cl^(-1),SO_(4)^(2-),NO_(3)^(-)and PO_(4)^(3-)),antibiotics(e.***.sulphonamides,quinolones,β2-receptor agonists,macrolides,tetracyclines and crystal violet)and heavy metals(e.g.Cu,Cd,As,Cr,Hg,Zn and Pb)contents from these biogas slurry samples were systematically investigated.On this basis,risk assessment of biogas slurry was also performed.The concentrations of COD,NH_(4)^(+)-N and PO_(4)^(3-) in biogas slurry samples with chicken manure as raw material were significantly higher than those of other raw materials.Therefore,the biogas slurry from chicken manure raw material demonstrated the most serious eutrophication threat.The antibiotic contents in biogas slurry samples from swine manure were the highest among five raw materials,mostly sulphonamides,quinolones and tetracyclines.Biogas slurry revealed particularly serious arsenic contamination and moderate potential ecological risk.The quadratic polynomial stepwise regression model can quantitatively describe the correlation among NH_(4)^(+)-N,PO_(4)^(3+) and heavy metals concentration of biogas slurry.This work demonstrated a universal potential threat from biogas slurry that can provide supporting data and theoretical basis for harmless treatment and reuse of biogas slurry.

关键词： Biogas slurry Antibiotics Heavy metals Risk assessment

Novel eco-efficient reactive distillation process for dimethyl carbonate production by indirect alcoholysis of urea

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Frontiers of chemical Science and engineering 2022年第2期16卷 316-331页

作者： Iulian Patrașcu Costin S.Bîldea Anton A.Kiss Department of Chemical and Biochemical Engineering University“Politehnica”of Bucharest011061 BucharestRomania department of chemical engineering and Analytical Science The University of ManchesterManchester M139PLUK

Dimethyl carbonate is an eco-friendly essential chemical that can be sustainably produced from CO_(2),which is available from carbon capture activities or can even be captured from the air.The rapid increase in dimethyl carbonate demand is driven by the fast growth of polycarbonates,solvent,pharmaceutical,and lithium-ion battery industries.Dimethyl carbonate can be produced from CO_(2)through various chemical pathways,but the most convenient route reported is the indirect alcoholysis of urea.Previous research used techniques such as heat integration and reactive distillation to reduce the energy use and costs,but the use of an excess of methanol in the trans-esterification step led to an energy intensive extractive distillation required to break the dimethyl carbonate-methanol azeotrope.This work shows that the production of dimethyl carbonate by indirect alcoholysis of urea can be improved by using an excess of propylene carbonate(instead of an excess of methanol),a neat feat that we showed it requires only 2.64 kW·h·kg^(-1) dimethyl carbonate in a reaction-separation-recycle process,and a reactive distillation column that effectively replaces two conventional distillation columns and the reactor for dimethyl carbonate synthesis.Therefore,less equipment is required,the methanol-dimethyl carbonate azeotrope does not need to be recycled,and the overall savings are higher.Moreover,we propose the use of a reactive distillation column in a heat integrated process to obtain high purity dimethyl carbonate(>99.8 wt-%).The energy requirement is reduced by heat integration to just 1.25 kW·h·kg^(-1) dimethyl carbonate,which is about 52%lower than the reaction-separation-recycle process.To benefit from the energy savings,the dynamics and control of the process are provided for10%changes in the nominal rate of 32 ktpy dimethyl carbonate,and for uncertainties in reaction kinetics.

关键词： dimethyl carbonate reactive distillation process design plantwide control