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A novel strategy for loading metal cocatalysts onto hollow nano-TiO_(2)inner surface with highly enhanced H_(2)production activity

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Green Energy & Environment 2023年第2期8卷 509-518页

作者： Nan Chen Yu Zhou Songtao Cao Ruixin Wang weizhou jiao School of Chemical Engineering and Technology North University of ChinaTaiyuanShanxi030051China

The loading strategy of cocatalysts affects its activity exerting and atom utilization.Here,a novel strategy for loading precious metal(Pt)cocatalysts by means of ultrathin N-doped carbon layer is reported.The strategy is based on a pyrolysis process of predesigned N-containing polymers and Pt complexes on hard-template surface,during which Pt can be reduced by carbon from pyrolysis at high temperatures.Finally,the hollow TiO_(2)composite with stable and dispersed Pt on its inner surface was prepared.It shows an ultrahigh photocatalytic H_(2)production activity as high as 25.7 mmol h^(-1)g^(-1)with methanol as sacrificial regent,and displays an apparent quantum yield as 13.2%.The improved photocatalytic activity and stability can be attributed to the highly dispersed and ultrafine Pt nanoparticles,enhanced interaction between Pt-species and carbon support,fast photo-excited electron transport from the high graphitization degree of NC layers,ample oxygen vacancies/defects,as well as the manipulated local charge distribution of Pt/NC-layer configuration.Additionally,the universality of the proposed strategy was demonstrated by replacing metal sources(such as,Ru and Pd).This work presented a promising strategy for the design and development of novel photocatalysts,which shows a broad application prospect.

关键词： Ultrathin carbon layer Ultrafine Pt nanoparticles Loading Hollow photocatalyst Photocatalytic hydrogen production

Removal of nitric oxide from simulated flue gas using aqueous persulfate with activation of ferrous ethylenediaminetetraacetate in the rotating packed bed

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Frontiers of Chemical Science and Engineering 2023年第4期17卷 460-469页

作者： Da Guo Guisheng Qi Dong Chen Jiabao Niu Youzhi Liu weizhou jiao Shanxi Province Key Laboratory of Higee-Oriented Chemical Engineering North University of ChinaTaiyuan 030051China School of Chemistry and Chemical Engineering North University of ChinaTaiyuan 030051China

Nitric oxide being a major gas pollutant has attracted much attention and various technologies have been developed to reduce NO emission to preserve the environment.Advanced persulfate oxidation technology is a workable and effective choice for wet flue gas denitrification due to its high efficiency and green advantages.However,NO absorption rate is limited and affected by mass transfer limitation of NO and aqueous persulfate in traditional reactors.In this study,a rotating packed bed(RPB)was employed as a gas-liquid absorption device to elevate the NO removal efficiency(η_(NO))by aqueous persulfate((NH_(4))_(2)S_(2)O_(8))activated by ferrous ethylenediaminetetraacetate(Fe^(^(2+))-EDTA).The experimental results regarding the NO absorption were obtained by investigating the effect of various operating parameters on the removal efficiency of NO in RPB.Increasing the concentration of(NH_(4))_(2)S_(2)O_(8) and liquid-gas ratio could promoted the oxidation and absorption of NO while theη_(NO) decreased with the increase of the gas flow and NO concentration.In addition,improving the high gravity factor increased theη_(NO) and the total volumetric mass transfer coefficient(K_(G)α )which raise theη_(NO) up to more than 75%under the investigated system.These observations proved that the RPB can enhance the gas-liquid mass transfer process in NO absorption.The correlation formula between K_(G)α and the influencing factors was determined by regression calculation,which is used to guide the industrial scale-up application of the system in NO removal.The presence of O_(2) also had a negative effect on the NO removal process and through electron spin resonance spectrometer detection and product analysis,it was revealed that Fe^(2+)-EDTA activated(NH_(4))2S_(2)O_(8) to produce•SO_(4)^(-),•OH and•O_(2)^(-),played a leading role in the oxidation of NO,to produce NO_(3)^(-)as the final product.The obtained results demonstrated a good applicable potential of RPB/PS/Fe^(2+)-EDTA in the removal of NO from flue gases.

关键词： rotating packed bed Fe2+-EDTA sulfate radical hydroxyl radical NO removal efficiency

An optimization method for enhancement of gas–liquid mass transfer in a bubble column reactor based on the entropy generation extremum principle

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Chinese Journal of Chemical Engineering 2023年第1期53卷 83-88页

作者： Chao Zhang Youzhi Liu weizhou jiao Hongyan Shen Xigang Yuan Shengkun Jia Shanxi Province Key Laboratory of Higee-Oriented Chemical Engineering North University of ChinaTaiyuan 030051China State Key Laboratory for Chemical Engineering School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China

In this study,an optimization method is proposed to enhance the gas–liquid mass transfer in bubble column reactor based on the entropy generation extremum principle.The mass transfer–induced entropy generation can be maximized with the increase of mass transfer rate,based on which the velocity field can be optimized.The oxygen gas–liquid mass transfer is the major rate–limiting step of the toluene emissions biodegradation process in bubble column reactor,so the entropy generation due to oxygen mass transfer is used as the objective function,and the conservation equations of the gas–liquid flow and species concentration are taken as constraints.This optimization problem is solved by the calculus of variations,the optimal liquid flow pattern is obtained and the relationship of the maximum mass transfer enhancement on viscous dissipation is revealed,which can be used to improve the design of internal structure of the bubble column reactor.

关键词： Entropy generation Bubble column reactor Optimization Biodegradation Flow field

Kinetics of the direct reaction between ozone and phenol by high-gravity intensified heterogeneous catalytic ozonation

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Chinese Journal of Chemical Engineering 2023年第1期53卷 317-323页

作者： Kechang Gao Shengjuan Shao Zhixing Li Jiaxin Jing weizhou jiao Youzhi Liu Shanxi Province Key Laboratory of Higee-Oriented Chemical Engineering North University of ChinaTaiyuan 030051China

In this study,high-gravity intensified heterogeneous catalytic ozonation is utilized for treatment of phenol-containing wastewater,and the kinetics of the direct reaction between ozone and phenol in the presence of excess tertiary butanol(TBA)is investigated.It is revealed that the direct reaction between ozone and phenol in the rotating packed bed(RPB)follows the pseudo-first-order kinetics with a reaction rate constant higher than that in the conventional bubbling reactor(BR).Under different conditions of temperature,initial pH,high-gravity factor,and gaseous ozone concentration,the apparent reaction rate constant varies in the range of 0.0160–0.115 min-1.An empirical power-exponential model is established to characterize the effects of these parameters on the direct reaction between ozone and phenol by high-gravity intensified heterogeneous catalytic ozonation.

关键词： High-gravity technique Heterogeneous catalysis Ozone Phenol Kinetics of the direct reaction

High-gravity intensified iron-carbon micro-electrolysis for degradation of dinitrotoluene

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Frontiers of Chemical Science and Engineering 2022年第11期16卷 1595-1605页

作者： Jiaxin Jing weizhou jiao Zhixing Li Kechang Gao Jingwen Zhang Gaomiao Ren Youzhi Liu Shanxi Province Key Laboratory of Higee-Oriented Chemical Engineering North University of ChinaTaiyuan 030051China

The application of iron–carbon(Fe–C)micro-electrolysis to wastewater treatment is limited by the passivation potential of the Fe–C packing.In order to address this problem,high-gravity intensified Fe–C micro-electrolysis was proposed in this study for degradation of dinitrotoluene wastewater in a rotating packed bed(RPB)using commercial Fe–C particles as the packing.The effects of reaction time,high-gravity factor,liquid flow rate and initial solution pH were investigated.The degradation intermediates were determined by gas chromatography-mass spectrometry,and the possible degradation pathways of nitro compounds by Fe–C micro-electrolysis in RPB were also proposed.It is found that under optimal conditions,the removal rate of nitro compounds reaches 68.4%at 100 min.The removal rate is maintained at approximately 68%after 4 cycles in RPB,but it is decreased substantially from 57.9%to 36.8%in a stirred tank reactor.This is because RPB can increase the specific surface area and the renewal of the liquid–solid interface,and as a result the degradation efficiency of Fe–C micro-electrolysis is improved and the active sites on the Fe–C surface can be regenerated for continuous use.In conclusion,high-gravity intensified Fe–C micro-electrolysis can weaken the passivation of Fe–C particles and extend their service life.

关键词： high-gravity technology rotating packed bed Fe–C micro-electrolysis dinitrotoluene wastewater active sites

Degradation of nitrobenzene-containing wastewater by sequential nanoscale zero valent iron-persulfate process

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Green Energy & Environment 2021年第6期6卷 910-919页

作者： Jingjuan Qiao weizhou jiao Youzhi Liu Shanxi Province Key Laboratory of Higee-Oriented Chemical Engineering North University of ChinaTaiyuanShanxi030051China

As nitrobenzene(NB)is structurally stable and difficult to degrade due to the presence of an electron withdrawing group(nitro group).The sequential nanoscale zero valent iron-persulfate(NZVI-Na_(2)S_(2)O_(8))process was proposed in this study for the degradation NB-containing wastewater.The results showed that the NB degradation efficiency and the total organic carbon removal efficiency in the sequential NZVINa_(2)S_(2)O_(8)process were 100%and 49.25%,respectively,at a NB concentration of 200 mg L^(-1),a NZVI concentration of 0.75 g L^(-1),a Na_(2)S_(2)O_(8)concentration of 26.8 mmol L^(-1),an initial pH of 5,and a reaction time of 30 min,which were higher than those(88.53%and 35.24%,respectively)obtained in the NZVI/Na_(2)S_(2)O_(8)process.Sulfate radicals(SO_(4)·-)and hydroxyl radicals(·OH)generated in the reaction were identified directly by electron paramagnetic resonance spectroscopy and indirectly by radical capture experiments,and it was shown that both SO_(4)^(·-)and·OH played a major role in the sequential NZVI-Na_(2)S_(2)O_(8)process.The possible pathways involved in the reduction of NB to aniline(AN)and the further oxidative degradation of AN were determined by gas chromatography-mass spectrometry.

关键词： Nanoscale zero valent iron Impinging stream-rotating packed bed Sequential NZVI-Na2S2O8process Nitrobenzene Degradation pathways

功能性填料在超重力旋转填料床中的应用和研究进展

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化工学报 2024年第4期75卷 1414-1428页

作者：程婷焦纬洲刘有智中北大学超重力化工过程山西省重点实验室山西太原030051 太原工业学院环境与安全工程系山西太原030008

填料作为旋转填料床的核心部件,是物料微观混合和传质反应过程发生的重要场所。填料的结构、材质组成、填装方式决定了填料的功能性,进而直接影响到旋转填料床的传质性能、使用寿命和应用范围,故而增强填料的功能性显得尤为重要。功能... 详细信息

填料作为旋转填料床的核心部件,是物料微观混合和传质反应过程发生的重要场所。填料的结构、材质组成、填装方式决定了填料的功能性,进而直接影响到旋转填料床的传质性能、使用寿命和应用范围,故而增强填料的功能性显得尤为重要。功能性填料通过改变常用填料的表面性质、调节形态、设计结构等手段,使填料具有如吸附、催化、疏水等的功能特性,在提高旋转填料床的性能和运行效果方面表现出优异的成效。综述了在旋转填料床中功能性填料的主要分类与特点,总结分析了近年来功能性散装填料和规整填料在旋转填料床中的应用情况,从增强传质特性和改善液体流动行为方面分析了填料功能特性的体现,并对功能性填料的发展方向和工业化前景做出了展望。

关键词：超重力旋转填料床功能性填料传质催化

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Oxidation of benzyl alcohols to ketones and aldehydes by O3 process enhanced using high-gravity technology

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Chinese Journal of Chemical Engineering 2020年第3期28卷 808-814页

作者： Wenqiang Gao Lei Du weizhou jiao Youzhi Liu Shanxi Province Key Laboratory of Higee-Oriented Chemical Engineering North University of ChinaTaiyuan 030051China Department of Chemistry and Chemical Engineering Luliang UniversityLuliang033000China

In this study,a practical process for ozonization of benzyl alcohols to ketones and aldehydes in a rotating packed bed(RPB-O3)reactor has been developed.Using 1-phenylethanol as a model reactant,the performance of RPB-O3 process in different solvents has been compared with the commonly used stirred tank reactor(STR-O3).Ethyl acetate was the optimum solvent for the conversion of 1-phenylenthanol to acetophenone in RPB-O3 process,with 78%yield after 30 min.In a parallel STR-O3 experiment,the yield of acetophenone was50%.Other experimental variables,i.e.O3 concentration,reaction time,high-gravity factor and liquid flow rate were also optimized.The highest yield of acetophenone was obtained using O3 concentration of 80 mg·L-1,reaction time of 30 min,high gravity factor of 40 and liquid flow rate of 120 L·h-1.Under the optimized reaction conditions,a series of structurally diverse primary and secondary alcohols was oxidized with(19%–92%)yield.The ozonization mechanism was studied by Electron Paramagnetic Resonance(EPR)spectroscopy,monitoring the radical species formed upon self-decomposition of O3.The characteristic quadruple peak with the 1:2:2:1 intensity ratio that corresponds to hydroxyl radicals(·OH)was observed in the electron paramagnetic resonance(EPR)spectrum,indicating an indirect oxidation mechanism of alcohols via·OH radical.

关键词： Ozone Benzyl alcohols Aldehydes and ketones High-gravity technology

Numerical simulation and experimental study of the characteristics of packing feature size on liquid flow in a rotating packed bed

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Chinese Journal of Chemical Engineering 2021年第6期34卷 22-31页

作者： Xifan Duan Zhiguo Yuan Youzhi Liu Hangtian Li weizhou jiao Shanxi Province Key Laboratory of Higee-Oriented Chemical Engineering North University of ChinaTaiyuan 030051China

Rotating packed bed has high efficiency of gas-liquid mass transfer.So it is significant to investigate fluid motion in rotating packed bed.Numerical simulations of the effects of packing feature size on liquid flow characteristics in a rotating packed bed are reported in this paper.The particle image velocimetry is compared with the numerical simulations to validate the turbulent model.Results show that the liquid exists in the packing zone in the form of droplet and liquid line,and the cavity is droplet.When the radial thickness of the packing is less than 0.101 m,liquid line and droplets appear in the cavity.When rotational speed and radial thickness of the packing increase,the average diameter of the droplets becomes smaller,and the droplet size distribution becomes uniform.As the initial velocity of the liquid increases,the average droplet diameter increases and the uniformity of particle size distribution become worse.The droplet velocity increases with the radial thickness of the packing increasing,and gradually decreases when it reaches the cavity region.The effect of packing thickness is most substantial through linear fitting.The predicted and simulated values are within±15%.The cumulative volume distribution curves of the experimental and simulated droplets are consistent with the R-R distribution.

关键词： Chemical process strengthening equipment Rotating packed bed Computational fluid dynamics Particle image velocimetry Sieve packing