Preparation of Pd/c-Al_(2)O_(3)/nickel foam monolithic catalyst and its performance for selective hydrogenation in a rotating packed bed reactor

Selective hydrogenation plays an important role in chemical industries,yet its selectivity is usually limited by the mass transfer.In this work,the enhanced hydrogenation selectivity was achieved in a rotating packed bed(RPB)reactor with excellent mass transfer efficiency.Aiming to be used under the centrifugal filed,a monolithic catalyst Pd/c-Al_(2)O_(3)/nickel foam suiting for the shape and size of the rotor of RPB reactor was prepared by the electrophoretic deposition method.The mechanical strength of the catalyst can meet the requirement of high centrifugal force in the RPB.The hydrogenation selectivity in the RPB reactor using the 3-methyl-1-pentyn-3-ol hydrogenation system was 3–8 times higher than that in a stirred tank reactor under similar conditions.This work proves the feasibility of intensifying the selectivity of hydrogenation process in the RPB reactor.

Time-resolved characteristics of a nanosecond pulsed multi-hollow needle plate packed bed dielectric barrier discharge

In this paper,self-designed multi-hollow needle electrodes are used as a high-voltage electrode in a packed bed dielectric barrier discharge reactor to facilitate fast gas flow through the active discharge area and achieve large-volume stable discharge.The dynamic characteristics of the plasma,the generated active species,and the energy transfer mechanisms in both positive discharge(PD)and negative discharge(ND)are investigated by using fast-exposure intensified charge coupled device(ICCD)images and time-resolved optical emission spectra.The experimental results show that the discharge intensity,number of discharge channels,and discharge volume are obviously enhanced when the multi-needle electrode is replaced by a multihollow needle electrode.During a single voltage pulse period,PD mainly develops in a streamer mode,which results in a stronger discharge current,luminous intensity,and E/N compared with the diffuse mode observed in ND.In PD,as the gap between dielectric beads changes from 0 to250μm,the discharge between the dielectric bead gap changes from a partial discharge to a standing filamentary micro-discharge,which allows the plasma to leave the local area and is conducive to the propagation of surface streamers.In ND,the discharge only appears as a diffusionlike mode between the gap of dielectric beads,regardless of whether there is a discharge gap.Moreover,the generation of excited states N_(2)^(+)(B^(2)∑_(u)^(+))and N2(C^(3)Π_(u))is mainly observed in PD,which is attributed to the higher E/N in PD than that in ND.However,the generation of the OH(A^(2)∑^(+))radical in ND is higher than in PD.It is not directly dominated by E/N,but mainly by the resonant energy transfer process between metastable N_(2)(A^(3)∑_(u)^(+))and OH(X^(2)Π).Furthermore,both PD and ND demonstrate obvious energy relaxation processes of electron-to-vibration and vibration-to-vibration,and no vibration-to-rotation energy relaxation process is observed.

Meta-analysis of CO_(2) conversion,energy efficiency,and other performance data of plasma-catalysis reactors with the open access PIONEER database

This paper brings the comparison of performances of CO_(2)conversion by plasma and plasma-assisted catalysis based on the data collected from literature in this field,organised in an open access online database.This tool is open to all users to carry out their own analyses,but also to contributors who wish to add their data to the database in order to improve the relevance of the comparisons made,and ultimately to improve the efficiency of CO_(2)conversion by plasma-catalysis.The creation of this database and database user interface is motivated by the fact that plasma-catalysis is a fast-growing field for all CO_(2)conversion processes,be it methanation,dry reforming of methane,methanolisation,or others.As a result of this rapid increase,there is a need for a set of standard procedures to rigorously compare performances of different systems.However,this is currently not possible because the fundamental mechanisms of plasma-catalysis are still too poorly understood to define these standard procedures.Fortunately however,the accumulated data within the CO_(2)plasma-catalysis community has become large enough to warrant so-called“big data”studies more familiar in the fields of medicine and the social sciences.To enable comparisons between multiple data sets and make future research more effective,this work proposes the first database on CO_(2)conversion performances by plasma-catalysis open to the whole community.This database has been initiated in the framework of a H_(2)0_(2)0 European project and is called the“PIONEER Data Base”.The database gathers a large amount of CO_(2)conversion performance data such as conversion rate,energy efficiency,and selectivity for numerous plasma sources coupled with or without a catalyst.Each data set is associated with metadata describing the gas mixture,the plasma source,the nature of the catalyst,and the form of coupling with the plasma.Beyond the database itself,a data extraction tool with direct visualisation features or advanced filtering functionalities has been developed and is available online to the public.The simple and fast visualisation of the state of the art puts new results into context,identifies literal gaps in data,and consequently points towards promising research routes.More advanced data extraction illustrates the impact that the database can have in the understanding of plasma-catalyst coupling.Lessons learned from the review of a large amount of literature during the setup of the database lead to best practice advice to increase comparability between future CO_(2)plasma-catalytic studies.Finally,the community is strongly encouraged to contribute to the database not only to increase the visibility of their data but also the relevance of the comparisons allowed by this tool.

Comparing two IBM implementations for the simulation of uniform packed beds

Nowadays,the design of fixed packed bed reactors still relies on empirical correlations,which,especially for small tube to particle diameter ratios,are mostly too inaccurate because of the presence of wall effects.Therefore,the simulation of fixed packed bed reactors plays an important role to predict and control the flow and process parameters in such,nowadays and in the future.Because of its straightforward applicability to non-uniform packings with particles of arbitrary shapes,the immersed boundary method(IBM)has advantages over other numerical methods and is used more and more frequently.This paper compares two approaches of IBMs for the simulation of fixed bed reactors with spherical shaped particles.The classic,smooth approach is compared to the straightforward to implement blocked-off method for velocity fields above the fixed bed for particle Reynolds numbers of 300 and 500.Results from experimental inline PIV-measurements of the reactor to be simulated serve as a basis for comparison.Very good agreement with the experiment is found for both simulation methodologies with higher resolutions,considering the more stable flow at a particle Reynolds number of 300.Differences in the different IBM approaches occurred for the more unsteady flow at a particle Reynolds number of 500.Compared to the blocked-off method,the smooth IBM reflects the formation of additional jets and recirculation zones better right above the bed,though increasing the fluid mesh resolution improves the accuracy of the blocked-off method.Overall,a more diffusive behaviour is found for the blocked-off simulations due to the stairstep representation,which is avoided by using interpolation stencils as in the smooth IBM.With higher mesh refinement in the blocked-off IBM this effect can be reduced,but this also increases the computational effort.

Experimental and numerical investigation to elucidate the fluid flow through packed beds with structured particle packings

The present paper presents an experimental and numerical investigation of the dispersion of the gaseous jet flow and co-flow for the simple unit cell(SUC)and body-centred cubic(BCC)configuration of particles in packed beds.The experimental setup is built in such a way that suitable and simplified boundary conditions are imposed for the corresponding numerical framework,so the simulations can be done under very similar conditions as the experiments.Accordingly,a porous plate is used for the co-flow to achieve the uniform velocity and the fully developed flow is ensured for the jet flow.The SUC and BCC particle beds consist of 3D-printed spheres,and the non-isotropy near the walls is mostly eliminated by placing half-spheres at the channel walls.The flow velocities are analysed directly at the exit of the particle bed for both beds over 36 pores for the SUC configuration and 60 pores for the BCC configuration,for particle Reynolds numbers of 200,300,and 400.Stereo particle image velocimetry is experimentally arranged in such a way that the velocities over the entire region at the exit of the packed bed are obtained instantaneously.The numerical method consists of a state-of-the-art immersed boundary method with adaptive mesh refinement.The paper presents the pore jet structure and velocity field exiting from each pore for the SUC and BCC packed particle beds.The numerical and experimental studies show a good agreement for the SUC configuration for all flow velocities.For the BCC configuration,some differences can be observed in the pore jet flow structure between the simulations and the experiments,but the general flow velocity distribution shows a good overall agreement.The axial velocity is generally higher for the pores located near the centre of the packed bed than for the pores near the wall.In addition,the axial velocities are observed to increase near the peripheral pores of the packed bed.This behaviour is predominant for the BCC configuration as compared to the SUC configuration.The velocities near the peripheral pores can become even higher than those at the central pores for the BCC configuration.It is shown that both the experiments as well as the simulations can be used to study the complex fluid structures inside a packed bed reactor.

A Comparative Study on Heat Transfer Performance of Typical Petrochemical Reactors

The performance of heat transfer is a key issue for reactor design in petrochemical industry. Since the heat transfer in reactors is a complicated process and depends on multiple parameters, the evaluation of the heat transfer performance is usually challenging, and few previous studies gave an overall view of heat exchange performance of different types of reactors. In this review, heat transfer coefficients of two types of petrochemical reactors, including the packed bed and the fluidized bed, were systematically analyzed and compared based on a number of reported correlations. The relationship between heat transfer coefficients and fluid flow velocity in different reactors has been well established, which clearly demonstrates the varying range of their heat transfer coefficients. Heat transfer coefficients of gas-phase packed bed can exceed 200 W/m^2·K, rather than the suggested values(17—89 W/m^2·K) mentioned in the literature. The fluidized bed shows better performance for both two-phase and three-phase beds as compared to the packed bed. Systems with liquid phase also show better heat transfer performance than other phases because of the larger heat capacity of liquid. Thus the industrial three-phase fluidized beds have the best heat transfer performance with an overall heat transfer coefficient of greater than 1 000 W/m^2·K. The heat transfer results provided by this review can afford not only new insights into the heat transfer in typical reactors, but also the basis and guidelines for reactor design and selection.

Green and scalable electrochemical routes for cost‐effective mass production of MXenes for supercapacitor electrodes

One of the most unique properties of two-dimensional carbides and nitrides of transition metals(MXenes)is their excellent water dispersibility and yet possessing superior electrical conductivity but their industrial-scale application is limited by their costly chemical synthesis methods.In this work,the niche feature of MXenes was capitalized in the packed-bed electrochemical reactor to produce MXenes at an unprecedented reaction rate and yield with minimal chemical waste.A simple NH4F solution was employed as the green electrolyte,which could be used repeatedly without any loss in its efficacy.Surprisingly,both fluoride and ammonium were found to play critical roles in the electrochemical etching,functionalization,and expansion of the layered parent materials(MAXs)through which the liberation of ammonia gas was observed.The electrochemically produced MXenes with excellent conductivity,applied as supercapacitor electrodes,could deliver an ultrahigh volumetric capacity(1408 F cm^(−3))and a volumetric energy density(75.8 Wh L^(−1)).This revolutionary green,energy-efficient,and scalable electrochemical route will not only pave the way for industrial-scale production of MXenes but also open up a myriad of versatile electrochemical modifications for improved functional MXenes.

Growth of Hierarchically Structured High-Surface Area Alumina on FeCralloy~ Rods

The formation of metastable alumina phases due to the oxidation of commercial FeCralloy（R） rods （0.5 mm thickness） at various temperatures and time periods has been examined. This structured layer acts as an anchor to bind additional coatings of alumina via wash-coat techniques, thereby improving the layer thickness and increasing adhesion of the catalytic surface. Optimisation of the layer thickness and catalytic properties were conducted, using a range of analytical systems [scanning electron microscope （SEM）, energy dispersive X-ray （EDX） and X-ray diffraction （XRD）]. The modified FeCralloy（R） rods were tested in a fixed bed reactor rig to assess the impact on yield for the dehydrogenation of methylcyclohexane.

CFD modeling using heterogeneous reaction kinetics for catalytic dehydrogenation syngas reactions in a fixed-bed reactor

A comprehensive 2D computational fluid dynamics （CFD） model was developed to simulate the flow behavior and catalytic dehydrogenation reaction of syngas in a heterogenous fixed-bed reactor （FBR）. The model combined the porous medium CFD model with a reaction kinetics model. To acquire an accu- rate reaction kinetics model, a comprehensive reaction mechanism was studied for the heterogeneous catalytic dehydrogenation reaction ofsyngas over a supported metal catalyst. Based on the reaction mech- anism and a statistical test, a reliable kinetics model was proposed. The CFD model combined with the above kinetics model was validated with one set of experimental data. The CFD model was also used to predict key reaction variable distributions such as the temperature and the component concentrations in the reactor.