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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 *** present the industrial conversion of cyclohexane to cyclohexanone and cyclohexanol is normally controlled at less than 5%***,the development of highly active and stable catalysts for the aerobic oxidation of cyclohexane is necessary to overcome this low-efficiency ***,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 *** achieved 88.28%cyclohexanone and cyclohexanol selectivity and a cyclohexane conversion of 8.88%under *** results showed that the introduction of zinc effectively alleviated the aggregation of Co nanoparticles and optimized the structural properties of the *** addition,Co0 and pyridinic-N are proposed to be the possible active species,and their proportion efficiently increased in the presence of Zn^(2+)*** 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

Plasma-exfoliated g-C_(3)N_(4) with oxygen doping: tailoring photocatalytic properties

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Frontiers of chemical Science and engineering 2024年第2期18卷 27-39页

作者： Yuxin Li Junxin Guo Rui Han Zhao Wang National engineering research centre of Industry Crystallization Technology School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China

Heteroatom doping and defect engineering have been proposed as effective ways to modulate the energy band structure and improve the photocatalytic activity of g-C_(3)N_(4). In this work, ultrathin defective g-C_(3)N_(4) was successfully prepared using cold plasma. Plasma exfoliation reduces the thickness of g-C_(3)N_(4) from 10 nm to 3 nm, while simultaneously introducing a large number of nitrogen defects and oxygen atoms into g-C_(3)N_(4). The amount of doped O was regulated by varying the time and power of the plasma treatment. Due to N vacancies, O atoms formed strong bonds with C atoms, resulting in O doping in g-C_(3)N_(4). The mechanism of plasma treatment involves oxygen etching and gas expansion. Photocatalytic experiments demonstrated that appropriate amount of O doping improved the photocatalytic degradation of rhodamine B compared with pure g-C_(3)N_(4). The introduction of O optimized the energy band structure and photoelectric properties of g-C_(3)N_(4). Active species trapping experiments revealed ·O_(2)^(–) as the main active species during the degradation.

关键词： graphitic carbon nitride cold plasma oxygen doping nitrogen defect visible-light photocatalysis

CFD-PBM coupled modeling of the liquid-liquid dispersion characteristics and structure optimization for Kenics static mixer

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Chinese Journal of chemical engineering 2024年第6期70卷 173-188页

作者： Junhai Deng Shilin Lan Juchang Wu Shenghua Du Weidong Liu Luchang Han Yefeng Zhou National&Local United engineering research centre for chemical Process Simulation and Intensification Chemical Process Simulation and Optimization Engineering Research Center of Ministry of EducationXiangtan UniversityXiangtan 411105China Hunan Haili chemical Industry Company Limited Changsha 410000China

Kenics static mixers(KSM)are extensively used in industrial mixing-reaction processes by virtue of high mixing efficiency,low power homogenization and easy continuous *** liquid droplet size and its distribution and thus revealing the dispersion characteristics are of great significance for structural optimization and process intensification in the *** this work,a computational fluid dynamics-population balance model(CFD-PBM)coupled method is employed to systematically investigate the effects of operating conditions and structural parameters of KSM on droplet size and its distribution,to further reveal the liquid-liquid dispersion *** indicate that higher Reynolds numbers or higher dispersed phase volume fractions increase energy dissipation,reducing Sauter mean diameter(SMD)of dispersed phase droplets and with a shift in droplet size distribution(DSD)towards smaller *** aspect ratios,greater blade twist and assembly angles amplify shear rate,leading to smaller droplet size and a narrower DSD in the smaller *** degree of impact exerted by the aspect ratio is notably ***,mixing elements with different spin enhance shear and stretching *** to the same spin,SMD becomes 3.7-5.8 times smaller in the smaller size range with a significantly narrower *** into account the pressure drop and efficiency in a comprehensive manner,optimized structural parameters for the mixing element encompass an aspect ratio of 1-1.5,a blade twist angle of 180°,an assembly angle of 90°,and interlaced assembly of adjacent elements with different *** work provides vital theoretical underpinning and future reference for enhancing KSM performance.

关键词： CFD Population balance Liquid-liquid dispersion Kenics static mixer

High adsorption selectivity of activated carbon and carbon molecular sieve boosting CO_(2)/N_(2) and CH_(4)/N_(2) separation

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Chinese Journal of chemical engineering 2024年第3期67卷 282-297页

作者： Siang Chen Wenling Wu Zhaoyang Niu Deqi Kong Wenbin Li Zhongli Tang Donghui Zhang The research Center of chemical engineering School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China

Flue gas and coal bed methane are two important sources of greenhouse *** swing adsorption process has a wide range of application in the field of gas separation,and the selection of adsorbent is *** this regard,in order to assess the better adsorbent for separating CO_(2) from flue gas and CH_(4) from coal bed methane,adsorption isotherms of CO_(2),CH_(4) and N_(2) on activated carbon and carbon molecular sieve are measured at 303.15,318.15 and 333.15 K,and up to 250 *** experimental data fit better with Langmuir 2 compared to Langmuir 3 and Langmuir-Freundlich models,and Clausius-Clapeyron equation was used to calculate the isosteric *** the order of the adsorbed amount and the adsorption heat on the two adsorbents are CO_(2)>CH_(4)>N_(2).The adsorption kinetics are calculated by the pseudo-first kinetic model,and the order of adsorption rates on activated carbon is N_(2)-CH_(4)>CO_(2),while on carbon molecular sieve,it is CO_(2)-N_(2)>CH_(4).It is shown that relative molecular mass and adsorption heat are the primary effect on kinetics for activated carbon,while kinetic diameter is the main resistance factor for carbon molecular ***,the adsorption selectivity of CH_(4)/N_(2) and CO_(2)/N_(2) were estimated with the ideal adsorption solution theory,and carbon molecular sieve performed best at 318.15 K for both CO_(2) and CH_(4) *** study suggested that activated carbon is a better choice for separating flue gas and carbon molecular sieve can be a strong candidate for separating coal bed methane.

关键词： Activated carbon Carbon molecular sieve Adsorbent evaluation Adsorption equilibrium and kinetics Heat of adsorption Selectivity

Optimization of biofuel supply chain integrated with petroleum refineries under carbon trade policy

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Frontiers of chemical Science and engineering 2024年第3期18卷 113-122页

作者： Wenhui Zhang Yiqing Luo Xigang Yuan chemical engineering research Center School of Chemical Engineering and TechnologyTianjin UniversityTianjin300350China State Key Laboratory of chemical engineering Tianjin UniversityTianjin300350China

The use of fossil fuels results in significant carbon dioxide *** have been increasingly adopted as sustainable alternatives to fossil fuel to address this environmental *** petroleum refineries into biofuel supply chains is an effective approach to mitigating greenhouse gas emissions and improving environmental *** this study,an integrated supply chain optimization framework was established,considering the carbon trade *** addition,a mixed-integer nonlinear programming model was developed to optimize the selection of biomass suppliers,construction of pretreatment plants and biorefineries,integration of petroleum refineries,and selection of transportation routes with the objective of minimizing the total annual *** example is presented to illustrate the applicability of the *** optimization results show that integrating petroleum refineries into biofuel supply chains effectively mitigates carbon *** trade policies can have a direct impact on the total annual cost and carbon emissions of the supply chain.

关键词： renewable energy biofuel supply chain carbon trade policy

research progress on simulation of multiscale mass transfer processes in gas-solid system by computational mass transfer

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Particuology 2024年第7期90卷 478-492页

作者： Xu Li Yaohui Wang Leifu Li Runye Zhang Hailun Ren Wenbin Li Zhongli Tang Donghui Zhang The research Center of chemical engineering School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China The Department of chemical engineering Tianjin Renai CollegeTianjin 301636China Collaborative Innovation Center of chemical Science and engineering(Tianjin) School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China

Particle-fluid system is one of the most popular systems in chemical *** to complex interface structure and high-velocity turbulence,the momentum and mass transfer exhibit nonlinear characteristics,which pose a great challenge for further study and *** solve this problem,computational mass transfer(CMT)emerged and has been proved to be effective in deeply exploring the mass transfer behavior of particle-fluid ***,this paper reviews recent gas-solid numerical studies of turbulence issues from empirical to theoretical,then discusses interphase mass transfer rate models and the interfacial interaction ***,the present study particularly reviews researches on mass transfer process of fixed and fluidized regime by CMT,providing reliable analysis of turbulent anisotropy diffusivity as well as multiscale structure and presenting theoretical instruction for the industrial optimization of mass transfer processes in chemical engineering.

关键词： Fixed bed Fluidized bed Computational mass transfer Turbulent mass diffusion Multiscale Anisotropy

Removal of rubidium from brine by an integrated film of sulfonated polysulfone/graphene/potassium copper ferricyanide

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Chinese Journal of chemical engineering 2024年第5期69卷 112-121页

作者： Huanxi Xu Peihua Lin Pei-Jun Liu Hai-Gang Liu Hui-Bin Guo Chao-Xiang Wu Ming Fang Xu Zhang Guan-Ping Jin Anhui Province engineering research Center of Flexible and Intelligent Materials School of Chemistry and Chemical EngineeringHefei University of TechnologyHefei 230009China chemical Design and research Institute Co. LTD of Qinghai ProvinceQinghai Engineering and Technology Research Center of Fine ChemicalXining 810008China

A novel integrated film of sulfonated polysulfone/graphene/potassium copper ferricyanide(KCuFC/SPSG)was used for selectively extracting rubidium ion(Rb^(+))from *** form KCuFC/SPSG,the precursor film of sulfonated polysulfone/graphene(SPSG)was synthesized by phase conversion process,which was alternately immersed in 0.1 mol·L^(-1)CuSO_(4)/K_(4)[Fe(CN)_(6)]by in-situ adsorption coupled co-precipitation *** data such as nuclear magnetic resonance spectrometer,Fourier transform infrared spectroscope,X-ray photoelectron spectroscope,X-ray diffraction,scanning electron microscope,and energy dispersive spectroscopy all verified that abundant KCuFC were uniformly located on the *** resulting KCuFC/SPSG was used in film separation *** the solution was fed into the system,the Rb^(+)could be selectively adsorption by KCuFC/*** the saturation adsorption,0.5 mol·L^(-1)NH_(4)Cl/HCl was fed into the film cell,Rb^(+)could be quickly desorbed by ion-exchange between Rb^(+)and NH_(4)^(+)in the lattice of *** purpose of separating and recovering Rb^(+)from the brine can be achieved after the repeated *** effects of pH,adsorption time,and interferential ions on the adsorption capacity of Rb^(+)were investigated by batch *** adsorption behavior fits the pseudo-second order kinetic process,while KCuFC has a higher adsorption capacity(Langmuir maximum sorption 165.4 mg·g^(-1)).In addition,KCuFC/SPSG shows excellent selectivity for Rb^(+)even in complex brine ***/SPSG could maintain 93.5%extraction efficiency after five adsorption/desorption cycles.

关键词： Rubidium extraction Potassium copper ferricyanide Sulfonated polysulfone Graphene oxide Adsorption

Reducing the vacancies associated with ferroelectric polarization to promote photocatalytic overall water splitting

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Science China Chemistry 2024年第10期67卷 3258-3264页

作者： Haozhi Qi Yuyang Kang Jian-An Liu Lichang Yin Wenyu Zhang Shangyi Ma Jianhang Qiu Lingli Li Weijin Hu Lianzhou Wang Gang Liu Institute of Metal research Chinese Academy of Sciences School of Materials Science and engineering University of Science and Technology of China Nanomaterials centre School of Chemical Engineering and Australian Institute for Bioengineering and NanotechnologyThe University of Queensland

Ferroelectric materials hold great promise in photocatalytic water splitting because their built-in electric field induced by the depolarization field can fulfill the separation of photogenerated ***,a number of intrinsic charged vacancy defects are simultaneously generated to screen the depolarized field for stabilizing the crystal structure,always resulting in severe recombination of photogenerated carriers and thus poor overall water splitting ***,we proposed a strategy to promote the separation and transport of photogenerated carriers of ferroelectric photocatalysts by adjusting the ferroelectric polarization and altering the coordination environment of elements to reduce the defect ***,we prepared a series of Ta-doped PbTiO3with low Pb(VPb) and O（VO） vacancy concentrations by reducing the polarization intensity and strengthening the Pb–O *** Ta-doped PbTiO3shows efficient charge separation and greatly enhanced photocatalytic overall water splitting activity with the assistance of *** work highlights the importance of regulating ferroelectric polarization and vacancy defect concentration by the doping strategy in charge separation for photocatalytic water splitting.

关键词： PbTiO3 ferroelectric polarization vacancy defect element doping photocatalytic overall water splitting

Corrosion behaviors and kinetics of nanoscale zero-valent iron in water:A review

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Journal of Environmental Sciences 2024年第1期135卷 391-406页

作者： Chenliu Tang Xingyu Wang Yufei Zhang Nuo Liu Xiang Hu research Group of Water Pollution Control and Water Reclamation College of Chemical EngineeringBeijing University of Chemical TechnologyBeijing 100029China Shanghai Collaborative Innovation centre for WEEE Recycling School of Resources and Environmental EngineeringShanghai Polytechnic UniversityShanghai 201209China

Knowledge on corrosion behaviors and kinetics of nanoscale zero-valent iron(nZVI)in aquatic environment is particularly significant for understanding the reactivity,longevity and stability of nZVI,as well as providing theoretical guidance for developing a cost-effective nZVI-based technology and designing large-scale ***,this review gives a holistic overview on the corrosion behaviors and kinetics of nZVI in ***,Eh-pH diagram is introduced to predict the thermodynamics trend of iron *** morphological,structural,and compositional evolution of(modified-)nZVI under different environmental conditions,assisted with microscopic and spectroscopic evidence,is then ***,common analytical methods and characterization technologies are categorized to establish time-resolved corrosion kinetics of nZVI in ***,stable models for calculating the corrosion rate constant of nZVI as well as electrochemical methods for monitoring the redox reaction are discussed,emphasizing their capabilities in studying the dynamic iron corrosion ***,in the future,more efforts are encouraged to study the corrosion behaviors of nZVI in long-term practical application and further build nanoparticles with precisely tailored *** expect that our work can deepen the understanding of the nZVI chemistry in aquatic environment.

关键词： Nanoscale zero-valent iron(nZVI) Corrosion behaviors Corrosion kinetics nZVI evolution

Organic polymorphic crystals with multi-stimuli response:excellent mechanical elasticity,novel two-stage heterotropic photochromism and self-reversible acidichromism

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Science China Materials 2024年第9期67卷 2796-2806页

作者： Yutong Yao Ting Wang Hui Yu Zhicheng Jiang Wenbo Wu Hongtu Zhao Hongchang Wu Na Wang Xin Huang Hongxun Hao National engineering research Center of Industrial Crystallization Technology School of Chemical Engineering and TechnologyTianjin UniversityTianjin300072China Collaborative Innovation Center of chemical Science and engineering(Tianjin) Tianjin300072China State Key Laboratory of chemical engineering School of Chemical Engineering and TechnologyTianjin UniversityTianjin300072China

Smart multi-stimuli responsive organic materials have become increasingly favored due to their advantages of high stability and easy *** this study,a cyanostilbene derivative((αZ)-2-chloro-α-[(4-methoxyphenyl)methylene]-5-pyridinehyde,TAR)was successfully synthesized,and its polymorphs(TAR-1 and TAR-2)exhibited multiple responsive behaviors under different stimulus ***-1 is supposed to have excellent mechanical properties,while TAR-2 shows fascinating heterotropic photochromism(green-cyan-yellow)under different intensities of ultraviolet(UV)irradiation,which has never been reported in previous *** investigation revealed that this was attributed to different degrees of[2+2]cycloaddition induced by UV *** addition,both polymorphs could be protonated during Trifluoroacetic acid fuming and deprotonate automatically after fuming,accompanied by the significant variation in ***,two scenarios were designed based on their unique stimuli-responsive properties,which proved their promising potential in fields of information security and anti-counterfeiting encryption.

关键词： elastic bending heterotropic photochromism self-reversible acidichromism