Laboratory of Chemical Reactor Engineering (SCR)

Group Chemical Reactor Engineering

(Prof.dr.ir. Jaap C. Schouten)

Introduction

The Chemical Reactor Engineering cluster is consisting of three research groups: the Chemical

Reactor Engineering group (SCR-CRE) headed by Jaap Schouten, the Micro Flow Chemistry &

Process Technology group (SCR-SFP) headed by Volker Hessel, and the Interfaces with Mass

Transfer group (SCR-SIM) headed by Cees van der Geld. The groups aim to perform high-quality

scientific and technological research in the chemical reactor engineering sciences with specific

emphasis on the design, development and operation of microfluidic processing systems,

microstructured reactors, high gravity- high shear reactors and structured multiphase reactors.

The research focuses on understanding and controlling the interaction of physical transport

phenomena, catalytic activity, and reaction and separation processes for a wide range of applications

and processes. Using this knowledge, we develop novel reactor concepts and integrated process

options, combining reactions with separations or multiple reactions in a single device.

The group's mission is to be among the world's top academic research groups in its field and to be

leading in the development of novel technologies for new, highly efficient, inherently safe, and robust

(micro)structured multiphase processing systems, which show the best productivity by a dedicated

design of all relevant dimensions and optimum choice of dedicated operational procedures.

Research

The research in the Chemical Reactor Engineering group is concentrated on three main topic area’s:

“high-gravity high-shear multiphase reactors”, “microstructured reactors and devices” and “catalysis

engineering”.

The research area of "high-gravity high-shear multiphase reactors" focuses on the development of

catalytic and non-catalytic multiphase reactor systems that use rotation to create high gravity and high

shear conditions. These conditions lead to excellent interphase mass transfer, excellent intraphase

mixing, and excellent fluid-to-wall heat transfer. Applications are especially in (exothermic) fast

reactions that are interphase mass transfer limited, are mixing limited, or are heat transfer limited.

Additionally, in a high gravity field two phases with different density can be contacted

countercurrently, which opens up possibilities for separation processes. Thus, distillation (gas-liquid),

extraction (liquid-liquid), and crystallization (liquid-solid) become feasible. The two main reactor

concepts that research is focusing on are the ‘spinning disc reactor’ and the ‘rotating foam reactor’.

The high-gravity high-shear conditions enable the use of extremely compact equipment for chemical

process industry. The equipment is easily a factor hundred smaller than conventional equipment. The

much smaller equipment size allows for the safe use of high temperatures and high pressures,

enlarging the economic process window. An additional benefit of the small equipment size is that

more expensive construction material can be used. Furthermore, individual parts can be coated with

plastics (teflon), diamant, corrosion resistive metals (gold, platina, tantalum) etc., with only a minor

increase in material costs. Even clean room technology can be used to etch specific microstructures

in the contact surfaces to enhance the performance. In 2012 the spin-off company ‘SpinID’ was

launched from within the group to commercialize the spinning disc reactor technology being

developed within this research line.

The research area of "microstructured reactors and devices" focuses on the development of

microchemical systems that provide intricate geometries with characteristic length scales of 10-100

µm for optimum mixing, mass and heat transfer, (catalytic) reaction, and product separation. The

challenge is to explore the potential benefits of these miniaturized chemical systems in terms of e.g.

productivity, selectivity, energy efficiency, new reaction pathways, safety, and environmental benign

manufacturing. A particular innovative aspect is to take benefit of microfabrication technologies for

integrating sensors and actuators for process monitoring and control. Areas of application include fuel

processing and hydrogen production, high-throughput catalyst screening, and chemicals synthesis

("process on a chip"). Research is focusing on scale-up of microreactors to industrial scale,

multifunctional reactors (combining multiple reactions or reaction with separation), and the preparation

of catalysts in microreactors.

The research area of “Catalysis Engineering” is bringing together the fields of Reactor Engineering

with Catalysis, one of the other focus points in the department. A state of the art catalyst requires a

state of the art reactor to function optimally and vice versa. In case one has an understanding of both

the catalyst and the processes occurring in the chemical reactor, it will be possible to develop a more

efficient system. Especially in a reaction system in which not only the desired reaction occurs, but

also competing reactions, causing a loss in selectivity or a deactivation of the catalyst, having an

understanding of the entire system will be very beneficial. An optimal design of the catalyst-reactor

system will only be possible by optimizing all the relevant length scales, from the site of the catalyst,

to the mass transfer length in the catalyst, to the catalyst particle size and shape (determining the

external mass transfer), and the macromixing behavior in the reactor (determining the local

environment of the catalyst). Within this research area, we are converting the reactor concepts

(rotating reactors and microreactors) that we are developing in the other research lines into catalytic

reactors, perform kinetic and mass transfer measurements on these catalytic systems to improve the

understanding of both the catalyst and reactor to improve them further and be able to model their

behavior.

Projects:

Design of Novel Bifunctional Gold-Ti- and Fe-modified Zeolite functional materials for the Catalytic

Oxidation of Hydrocarbons (S. Kanungo)

Mass and heat transfer gas-liquid flow through open structured random packings (L. Pezzi Martins

Loane)

Open micro-structured random packing in GLS reactors for FT catalyst and reactor development

(T. de Martino)

Biomass conversion to valuable chemicals (InSciTe) (V. Krzelj & M. Papaioannou)

High Gravity High Shear for Intensified Chemicals Production (HIGHSINC)

If you have questions or need information concerning the research or specific graduation projects,

please contact the staff, post-docs or Ph.D. students directly.

Also Research stages and Major projects can be carried out within the projects mentioned

hereafter.

Scientific staff Prof.dr.ir. J.C. Schouten STW 1.35 tel. 3088 J.C.Schouten@tue.nl Prof.dr.ir. J.T.F. Keurentjes STW 1.41 tel. 2850 J.T.F.Keurentjes@tue.nl Dr.ir. J. van der Schaaf STW 1.42 tel. 4712 J.vanderSchaaf@tue.nl Dr.ir. M.F. Neira D’Angelo STW 1.27 tel. 8281 M.F.Neira.dAngelo@tue.nl Postdoc Dr. L.A. Truter, MSc. STW 1.25 tel. 8278 l.a.truter@tue.nl Ph.D. students S. Kanungo, MSc. STW 1.23 tel. 8655 s.kanungo@tue.nl V. Krzelj, PDEng. STW 1.24 tel. 5507 v.krzelj@tue.nl E. Kertalli, MSc. STW 1.24 tel. 3544 e.kertalli@tue.nl M.T. de Martino, MSc. STW 1.22 tel. 8728 m.t.d.martino@tue.nl L. Pezzi Martins Loane,MSc. STW 1.28 tel. 8614 l.pezzi.martins-loane@tue.nl R. Sijabat STW 1.24 tel. 3273 r.r.sijabat@tue.nl P. Müller STW 1.23 M. Magosso STW 1.22 G.E. Cortes Garcia STW 1.24

Figure 1: Reactor set-up for conducting the catalytic measurements

Graduation projects in the Group Chemical Reactor Engineering:

Catalytic Oxidation of Hydrocarbons: Propene epoxidation and Methane activation

S. Kanungo, M.F. Neira D’Angelo, J.C. Schouten

Introduction

This graduation project deals with the direct catalytic production of two very important bulk chemicals:

propene oxide (annual production 7 million tons) and methanol (annual production 40 million tons).

Currently, propene oxide (PO) is produced in an environmentally stressing manner, which needs to be

replaced by a greener route. Past research, including ours, has shown that this can be done using

gold-titania (Au-Ti) catalysts and the latest catalyst development shows that this technology is inching

towards the required industrial standards.

With dwindling oil reserves, methane, which is available abundantly in nature, has recently come

under intense scrutiny. But current technologies can only convert methane to useful chemicals by

indirect routes, which come at a huge energy penalty. In this light, the direct oxidation of methane to

methanol would be highly desirable. Both reactions will be performed in our in-house flow set-up

using a mixture of the hydrocarbon (Methane/Propene), H2 and O2 in the gas phase on Au based

catalysts. Au centres on the catalyst will facilitate in-situ H2O2 production at benign conditions, which

will then selectively oxidize the hydrocarbon to yield the desired product.

Project Description

In this project, we will be investigating the applications of novel gold catalysts, studying the reaction

kinetics and also focusing at new reactor configurations in which to apply these catalysts in an optimal

manner.

Graduation Project

The following topics are available for graduation project:

1. Kinetic study and reactor modelling of novel Au catalysts for

propene epoxidation; effect of surface treatment on activity

and stability of these catalysts.

2. Application of Au catalysts for direct conversion of methane:

performance testing on macro and micro-reactor, kinetic

study and kinetic model development. Study on such

catalytic system/reaction condition has not yet been

reported.

References

1. Chen, J., Halin, S.J.A, Pidko, E.A, Verhoeven, M.W.G.M, Perez Ferrandez, D.M, Hensen, E.M.M, Schouten, J.C, Nijhuis, T.A, ChemCatChem, 2013, 5, 467-478

2. Kanungo, S., Ferrandez, D.M, Neira d'Angelo, M.F., Schouten, J.C., Nijhuis, T.A., J. Catal., submitted (in review), 2016

More information can be obtained with dr. Fernanda Neira D’Angelo (m.f.neira.dangelo@tue.nl).

Open micro-structured random packing in GLS reactors for FT catalyst and reactor

development

M.T. De Martino, M.F. Neira d’Angelo, J. van der Schaaf, J.C. Schouten

Project Background

In Fischer-Tropsch synthesis (FTS), syngas is converted to hydrocarbons and water by using

catalysts containing cobalt as active species; long-chain hydrocarbons (C5+) are the most desired

products in the broad product spectrum. The main issue for the reaction is the diffusional restrictions

in the porous network of FT catalysts which can strongly affect the product selectivity. In fact small

pores are required to provide high internal surface area, allowing for high dispersion of the active

species, but they hamper the diffusion of reactants and result in gradient formation. Besides the

process is exothermal and the temperature increase can either deactivate the catalytic solid or

produce more methane than C5+, therefore together with the species diffusion also the temperature

profile needs to be investigated in order to optimize the selectivity of the process.

Project Description

In this work, open structured Co-based packed catalysts are synthesized and tested during the FTS

with the aim to evaluate the effect of the mass transfer limitations on the process selectivity. As

catalyst supports aluminum solid-foams and fused silica capillary (Figure 1) will be used and their

performance will be tested in two different reactor setups.

The following topics are available for master projects:

Characterization and testing of Cobalt based catalysts

for the Fischer-Tropsch process. Investigation on the

catalytic activity and optimization of the working

conditions.

Adding a thermodynamic analysis to a pre-existent

reactor model in which extra and intra particle diffusions

are described, in order to take in account the product

condensation onto the catalytic surface. (Good knowledge of Matlab is required)

Heat balance modeling and validation by experiments, study of the temperature effect on the

catalyst with different supports.

References

1. A. Y. Khodakov, W. Chu, P. Fongarland, Chem. Rev. 2007, 107 (5), 1692 – 1744. 2. M.A. Leon Matheus, R. Tschentscher, T.A. Nijhuis, J. van der Schaaf, J.C. Schouten, Ind. Eng. Chem. Res. 2011, 50, 3184 More information can be obtained with dr. Fernanda Neira D’Angelo (m.f.neira.dangelo@tue.nl) .

Figure 1- Aluminum Foam and Fused Silica Capillary, used as support for the syntheses.

Biomass conversion to valuable chemicals-InSciTe project

M. Papaioannou, V. Krzelj, J. van der Schaaf, J.C. Schouten

Project description

The present project takes place at the Laboratory of Chemical Reactor Engineering at TU/e and it

aims to investigate the conversion of biomass to valuable chemicals. The research includes two

aspects: the chemistry; kinetics studies take place in order to observe the chemicals’ production and

identify unknown compounds. The second aspect is the process selection to perform the pre-

mentioned reactions.

Project background

The bio-based economy grows rapidly during the 21st century. So far, oil and natural gas are mostly

included in industry and they are the most widely used raw materials globally for the majority of

chemicals produced. During the recent years, there has been a development for the production of

these chemicals using biomass as feedstock. So, biomass has become a very attractive raw material

in order to replace petroleum as raw material. It consists of three main chemical groups: cellulose,

hemicellulose and lignin. Cellulose includes glucose, a basic chemical compound to produce HMF.

Hemicellulose contains a big variety of sugar monomers such as xylose and arabinose. Xylose is the

intermediate for furfural production. Cellulose and hemicellulose are approximately the 75% of the

total biomass composition. Finally, lignin is the 25% of biomass composition and links cellulose and

hemi-cellulose.

Based on the nature of the reactions, Spinning Disc Reactor is a promising equipment for chemicals

from biomass. The residence time is significantly decreased by performing reactive extraction. Thus,

the selectivity towards the desired products is increased and the system’s performance is improved.

The InSciTe project includes sub-projects carried out by two PhD students and they are interrelated

with the industry.

Information: More  information  can  be  obtained with  dr.ir.  John  van  der  Schaaf  (j.vanderschaaf@tue.nl).

BIOMASS

BIOMATERIA PLATFORM

CHEMICAL

COMMODITY

CHEMICALS

SPECIALTY CHEMICAL

S

BIOPOLYME

CHEMICAL INDUSTRY

Figure: Biomass industrial potentials

Transport Phenomena and Chemical Reaction in Slender Bubble Columns with Open-

Structure Random Packings

L. Pezzi Martins Loane, J.C. Schouten, J. van der Schaaf

Introduction

Traditionally trickle flow reactors are randomly packed with particles with small pores. The catalyst

inside of the pellets is only accessible via diffusion through the pores which would drive the catalyst

design towards small particles. However, to prevent an unacceptable high pressure drop, the particles

applied in a commercial trickle flow reactor are usually ‘’too large”. A way to circumvent these issues

is to use open-structure random packing (OSRP) as the catalytic active structure. OSRP are

essentially small pieces of foam with a specific shape and size and they are especially attractive as

they can be easily dumped into a column, acting as a packed bed. Structured foam blocks have been

proven to enhance mass and heat transfer and decrease pressure drop due to the intrinsic open pore

nature of a foam. The high accessible surface area that this type of packing offers makes it easy for

fluids to access the catalyst.

Figure: Left, traditional packed bed. Right, foam packing.

Project

In this project the hydrodynamic behavior of this novel type of packing as well as the mass and heat

transfer characteristics will be investigated. Both concurrent and countercurrent flow will be

investigated.

A correlation for liquid volume fraction and liquid axial dispersion, which will be performed by means

of residence time distribution experiments, together with pressure drop and flooding points will be the

primary goal of this project. Further on mass transfer experiments (CO2 absorption) and heat transfer

experiments will be performed and analyzed.

This project will be carried out in 2 different columns and with different sizes and shapes of OSRP.

Information: More information can be obtained with dr.ir. John van der Schaaf (j.vanderschaaf@tue.nl).