Influence of Particle Size and Single‐Tube Diameter on Thermal Behavior of Fischer‐Tropsch Reactors. Part II. Eggshell Catalysts and Optimal Reactor Performance

The optimal combination of particle and tube size for simulation of a single tube of a wall‐cooled multitubular Fischer‐Tropsch (FT) reactor with cobalt as catalyst was determined. The maximum size of the tubes, realized without temperature runaway, enhances with increasing particle size until an optimal value is reached, thereby improving the production rate of liquid fuels per tube. Reasons for this are that heat transfer to the cooled tube wall for a given tube size is considerably enhanced by increasing the particle size and that the influence of pore diffusion on the effective rate of FT synthesis gets stronger with rising particle size, which reduces the temperature sensitivity of the reactor and decreases the danger of a temperature runaway. The simulations indicate that the use of FT eggshell catalysts is not an option for fixed‐bed reactors. The temperature sensitivity of the reactor is strongly enhanced, which decreases the maximum tube size and with that the productivity per tube. All these effects are valid in general for wall‐cooled fixed‐bed reactors. Respective criteria are presented.     

Dynamic modeling and simulations of the behavior of a fixed‐bed reactor‐exchanger used for CO2 methanation

A multidimensional heterogeneous and dynamic model of a fixed‐bed heat exchanger reactor used for CO₂ methanation has been developed in this work that is based on mass, energy and momentum balances in the gas phase and mass and energy balances for the catalyst phase. The dynamic behavior of this reactor is simulated for transient variations in inlet gas temperature, cooling temperature, gas inlet flow rate, and outlet pressure. Simulation results showed that wrong‐way behaviors can occur for any abrupt temperature changes. Conversely, temperature ramp changes enable to attenuate and even fade the wrong‐way behavior. Traveling hot spots appear only when the change of an operating condition shifts the reactor from an ignited steady state to a non‐ignited one. Inlet gas flow rate variations reveal overshoots and undershoots of the reactor maximum temperature. © 2017 American Institute of Chemical Engineers AIChE J, 64: 468–480, 2018     

Microwave‐Assisted Continuous‐Flow Reactor Based on a Ridged Waveguide

Microwave‐assisted continuous‐flow reactors (MCFRs) are a valuable alternative to conventional reactors for accelerating chemical reactions. However, despite several interesting applications, only little quantitative research has been conducted on the temperature uniformity of the heating load. With water as a common inorganic solvent, a novel MCFR type based on a special ridged waveguide for heating water is studied by optimizing some parameters of micropipes in order to achieve better temperature uniformity. Compared to the original reactor, the standard deviation of the electric field decreased significantly when using the optimized reactor under the same heating conditions while the average electric field density increased. The optimized results were verified by experiments.     

Microstructured Fischer‐Tropsch Reactor Scale‐up and Opportunities for Decentralized Application

Current projects focusing on the energy transition in traffic will rely on a high‐level technology mix for their commissioning. One of those technologies is the Fischer‐Tropsch synthesis (FTS) that converts synthesis gas into hydrocarbons of different chain lengths. A microstructured packed‐bed reactor for low‐temperature FTS is tested towards its versatility for biomass‐based syngas with a high inert gas dilution. Investigations include overall productivity, conversion, and product selectivity. A 60‐times larger pilot‐scale reactor is further tested. Evaporation cooling is introduced which allows to increase the available energy extraction from the system. From that scale on, an autothermal operation at elevated conversion levels is applicable.     

Analysis of solar‐driven gasification of biochar trickling through an interconnected porous structure

The efficient transfer of high‐temperature solar heat to the reaction site is crucial for the yield and selectivity of the solar‐driven gasification of biomass. The performance of a gas‐solid trickle‐bed reactor constructed from a high thermal conductivity porous ceramic packing has been investigated. Beech char particles were used as the model feedstock. A two‐dimensional finite‐volume model coupling chemical reaction with conduction, convection, and radiation of heat within the packing was developed and tested against measured temperatures and gasification rates. The sensitivity of the gasification rate and reactor temperatures to variations of the packing's pore diameter, porosity, thermal conductivity, and particle loading was numerically studied. A numerical comparison with a moving bed projected a more uniform temperature distribution and higher gasification rates due to the increased heat transfer via combined radiation and conduction through the trickle bed. © 2014 American Institute of Chemical Engineers AIChE J, 61: 867–879, 2015     

Parametric analysis of Fischer‐tropsch synthesis in a catalytic microchannel reactor

Fischer‐Tropsch synthesis (FTS) involves highly exothermic conversion of syngas to a wide range of hydrocarbons, but demands isothermal conditions due to the strong dependence of product distribution on temperature. Running FTS in microchannel reactors is promising, as the sub‐millimeter dimensions can lead to significant intensification that inherently favors robust temperature control. This study involves computer‐based FTS simulations in a heat‐exchange integrated microchannel network composed of horizontal groups of square‐shaped cooling and wall‐coated, catalytic reaction channels. Effects of material type and thickness of the wall separating the channels, side length of the cooling channel, coolant flow rate, and channel wall texture on reaction temperature are investigated. Use of thicker walls with high thermal conductivities and micro‐baffles on the catalytic reaction channel wall favor near‐isothermal conditions. Response of reaction temperature against coolant flow rate is significant. Using cooling channels with smaller side lengths, however, is shown to be insufficient for temperature control. © 2011 American Institute of Chemical Engineers AIChE J, 2012     

Modeling of the sheet‐molding process for poly(methyl methacrylate)

The sheet‐molding process for the production of poly(methyl methacrylate) (PMMA) involves an isothermal batch reactor followed by polymerization in a mold (the latter is referred to as a “sheet reactor”). The temperature at the outer walls of the mold varies with time. In addition, due to finite rates of heat transfer in the viscous reaction mass, spatial temperature gradients are present inside the mold. Further, the volume of the reaction mass also decreases with polymerization. These several physicochemical phenomena are incorporated into the model developed for this process. It was found that the monomer conversion attains high values of near‐unity in most of the inner region in the mold. This is because of the high temperatures there, since the heat generated due to the exothermicity of the polymerization cannot be removed fast enough. However, the temperature of the mold walls has to be increased in the later stages of polymerization so that the material near the outer edges can also attain high conversions of about 98%. This would give PMMA sheets having excellent mechanical strength. The effects of important operating (decision) variables were studied and it was observed that the heat‐transfer resistance in the mold influences the spatial distribution of the temperature, which, in turn, influences the various properties (e.g., monomer conversion, number‐average molecular weight, and polydispersity index) of the product significantly. © 2001 John Wiley & Sons, Inc. J Appl Polym Sci 81: 1951–1971, 2001     

CO2 methanation: Optimal start‐up control of a fixed‐bed reactor for power‐to‐gas applications

Utilizing volatile renewable energy sources (e.g., solar, wind) for chemical production systems requires a deeper understanding of their dynamic operation modes. Taking the example of a methanation reactor in the context of power‐to‐gas applications, a dynamic optimization approach is used to identify control trajectories for a time optimal reactor start‐up avoiding distinct hot spot formation. For the optimization, we develop a dynamic, two‐dimensional model of a fixed‐bed tube reactor for carbon dioxide methanation which is based on the reaction scheme of the underlying exothermic Sabatier reaction mechanism. While controlling dynamic hot spot formation inside the catalyst bed, we prove the applicability of our methodology and investigate the feasibility of dynamic carbon dioxide methanation. © 2016 American Institute of Chemical Engineers AIChE J, 63: 23–31, 2017     

Micro‐structured Bi1.5Y0.3Sm0.2O3−δ catalysts for oxidative coupling of methane

Bi_1.5Y_0.3Sm_0.2O_3?δ (BYS), a ceramic material showing great activity and selectivity to oxidative coupling of methane (OCM), has been fabricated into catalyst rings (i.e., capillary tubes) with a plurality of self‐organized radial microchannels. The unique microchannels inside such BYS catalyst rings allow easier access of reactants, as well as increased the surface area, which potentially contributes to higher reaction efficiencies due to improved mass transfer. The micro‐structured BYS catalyst rings were investigated systematically via two types of reactors; (1) randomly packed fixed bed reactor and (2) monolithic‐like structured reactor. These two reactor designs have different flow patterns of reactants, that is, non‐ideal and ideal flows, which can significantly affect the final OCM performance. A remarkable improvement in C₂₊ yield (Y_C2+ > 20%) was obtained in the monolith‐like structured reactor, in contrast to randomly packed powder and micro‐structured rings (Y_C2+ < 15%), which proves the advantages of using a micro‐structured catalyst with an ideal flow in the feed for OCM. © 2015 American Institute of Chemical Engineers AIChE J, 61: 3451–3458, 2015     

Linear model predictive control for transport‐reaction processes

The article deals with systematic development of linear model predictive control algorithms for linear transport‐reaction models emerging from chemical engineering practice. The finite‐horizon constrained optimal control problems are addressed for the systems varying from the convection dominated models described by hyperbolic partial differential equations (PDEs) to the diffusion models described by parabolic PDEs. The novelty of the design procedure lies in the fact that spatial discretization and/or any other type of spatial approximation of the process model plant is not considered and the system is completely captured with the proposed Cayley‐Tustin transformation, which maps a plant model from a continuous to a discrete state space setting. The issues of optimality and constrained stabilization are addressed within the controller design setting leading to the finite constrained quadratic regulator problem, which is easily realized and is no more computationally intensive than the existing algorithms. The methodology is demonstrated for examples of hyperbolic/parabolic PDEs. © 2017 American Institute of Chemical Engineers AIChE J, 63: 2644–2659, 2017     

Multistage rotor‐stator spinning disc reactor

The scale up of a rotor‐stator spinning disc reactor by stacking single stage rotor‐stator units in series is demonstrated. The gas‐liquid mass transfer per stage is equal to the mass transfer in a single stage spinning disc reactor. The pressure drop per stage increases with increasing rotational disc speed and liquid flow rate. The pressure drop is more than a factor 2 higher for gas‐liquid flow than for liquid flow only, and is up to 0.64 bar at 459 rad s^?1. The high mass and heat transfer coefficients in the (multistage) rotor‐stator spinning disc reactor make it especially suitable for reactions with dangerous reactants, highly exothermic reactions and reactions where selectivity issues can be solved by high mass transfer rates. Additionally, the multistage rotor‐stator spinning disc reactor mimics plug flow behavior, which is beneficial for most processes. © 2011 American Institute of Chemical Engineers AIChE J, 2012     

Progress in membrane gas–liquid reactors

Gas–liquid reactions are crucially important in chemical synthesis and industries. In recent years, membrane gas–liquid reactors have attracted great attentions due to their high selectivity, productivity and efficiency, and easy process control and scale‐up. Membrane gas–liquid reactors can be divided into three categories: dispersive membrane reactor, non‐dispersive membrane reactor and pore flowthrough reactor. The progress in membrane gas–liquid reactors, including features, applications, advantages and limits, is briefly reviewed. © 2012 Society of Chemical Industry     

Influence of ash agglomerating fluidized bed reactor scale‐up on coal gasification characteristics

To study the influence of fluidized‐bed reactor scale‐up on coal gasification characteristics, a model of the ash agglomerating fluidized‐bed reactor has been developed using an equivalent reactor network method. With the reactor network model, the scale‐up effects of a gasifier were studied in terms of the characteristics of the chemical reactions in the jet zone, the annulus dense‐phase zone and the freeboard zone. Results showed that the changes occurred in the inequality proportion of the volume of the jet zone during the reactor scale‐up. Taking into consideration the utilization of a portion of the backflow gas, the expansion of the jet zone volume and the coal particle residence time, the temperature of the jet zone was increased from 1592 to 1662 K. Also, both the annulus dense‐phase zone temperature and the freeboard zone temperature decreased, causing subsequent decrease in the carbon conversion efficiency. © 2014 American Institute of Chemical Engineers AIChE J, 60: 1821–1829, 2014     

Energy Savings through Microwave Selective Heating of Pd/AC Catalyst Particulates in a Fixed‐Bed Reactor

Microwave radiation is a novel energy source to drive chemical reactions. In conventional reactors, however, the heat created either escapes through uninsulated reactor walls, or the microwave radiation is attenuated by insulated walls. Here, microwave selective heating of Pd catalyst particles supported on activated carbon particulates was examined in a fixed‐bed reactor using a novel vacuum‐filled Dewar‐like double‐walled continuous‐flow reactor. This reactor was developed toward energy savings in performing such organic reactions as the transformation of the hydride methyl cyclohexane to toluene.     

Evaluation of Multipoint Dosing Strategy in a Miniaturized Tubular Reactor: Nitration of Salicylic Acid

A 2D non‐isothermal reaction engineering model for a tubular reactor was developed for a complex reaction network of salicylic acid nitration. The influence of different operating and design parameters was studied to minimize the amount of secondary nitration products and limit the maximum temperature inside the reactor. Critical temperature effects were observed for larger reaction tubes, whereas close to isothermal conditions were perceived in smaller tubes. With single‐point dosing of both reactants, complete conversion can be achieved but formation of secondary nitration products cannot be avoided. For a given number of dosing points, a suitable combination of the operating parameters allowed to achieve complete conversion and better yield of the desired product.     

Maldistribution susceptibility of monolith reactors: Case study of glucose hydrogenation performance

In this work an ultrafast electron beam X‐ray modality was applied for the first time to characterize the gas–liquid Taylor flow inside each channel of an opaque honeycomb monolith structure ( ) for and . Significant spatial and temporal deviations in the phase holdup as well as in the gas bubble and liquid slug lengths were found. To evaluate the impact of Taylor flow maldistribution on the reactor performance, the data of more than unit cells were used to simulate the reactor productivity in the hydrogenation of glucose. The results verify that a monolith reactor solely designed by using superficial velocities and empirical correlations for gas bubble and liquid slug lengths fails significantly in achieving high product selectivity and the desired conversion. The developed methods are a solid base to design and select proper distributors ensuring the favorable flow configurations for specific chemical processes. © 2016 American Institute of Chemical Engineers AIChE J, 62: 4346–4364, 2016     

Turbulent mixing in the confined swirling flow of a multi‐inlet vortex reactor

Turbulent mixing in the confined swirling flow of a multi‐inlet vortex reactor (MIVR) was investigated using planar laser induced fluorescence (PLIF). The investigated Reynolds numbers based on the bulk inlet velocity ranged from 3290 to 8225, and the Schmidt number of the passive scalar was 1250. Measurements were taken in the MIVR at three different heights (¼, ½, and ¾ planes). The mixing characteristics and performance of the MIVR were investigated using instantaneous PLIF fields and pointwise statistics such as mixture fraction mean, variance, and one‐point concentration probability density function. It was found that the scalar is stretched along velocity streamlines, forming a spiral mixing pattern in the free‐vortex region. In the forced‐vortex region, mixing intensifies as the turbulent fluctuations increase significantly there. The mixing mechanisms in the MIVR were revealed by identifying specific segregation zones. At Re = 8225 the mixing in the free‐vortex region was dominated by both large‐scale structures and turbulent diffusion, while in the forced‐vortex region mixing is dominated by turbulent diffusion. © 2016 American Institute of Chemical Engineers AIChE J, 63: 2409–2419, 2017