WP 1 : ULTRASOUNDTom Van Gerven

1st progress meetingAmersfoort, 08.07.2013

Objectives last 6 months

30.01.2013

• Overall objective: development of tailored equipment for ultrasound-assisted multiphase processes (reactive synthesis and cooling crystallisation, reactive L/L extraction, VLE)

• Objective 1st year: data generation for enabling local positioning of the ultrasound energy at the interfaces, and experimental determination of flow and temperature profiles

Progress & status quo

30.01.2013

• Task 1.1.1 Reactive extraction– Start up of Jinu John (KUL, April 1st, 2013)– Selection of solvents– Design of set-up

Progress & status quo

30.01.2013

• Task 1.1.2 Reactive synthesis and cooling crystallisation– Start up of Jeroen Jordens (KUL, January 1st), Bjorn Gielen

(KUL, April 1st) and Rohit Kacker (TUD, April 1st) – First version flow and batch reactor operational and

characterised– MSZW for paracetamol recorded at different frequencies,

degradation of paracetamol being studied, PSD and crystal morphology preliminary data

– Seeding crystals synthesized; primary nucleation time studied– US field characterisation in preparation

Progress & status quo

30.01.2013

• Task 1.1.3 VLE– Matthias Wierschem started PhD at TUDO in June– Dr. Gunjan Agrahari (PhD IIT Kanpur, India) starts

at KUL on July 15– Kolja Neuman starts PhD at TUDO in August

Main achievements

30.01.2013

• Extraction: selection of solvents

Sl No Chemical NameViscosity

(25°C)Surface Tension (25°C)

VolatilitySp.

GravitySpeed of

sound (at 25°C)

Specific Acoustic ImpedanceVapour pr.

(21°C) Boiling point

cP N/m mm Hg °C at 20°C m/s Mrayl1 Toluene 0.59 0.0279 23.2 110.5 0.86 1330 1.144

2 Methyl Isobutyl Ketone 0.61 0.024 16.5 116 0.801 1222 0.979

3 2-methyl tetrahydrofuran 0.47 0.0246 155 79 0.86 1202 1.034

4 Chloroform 0.57 0.0267 169 61 1.48 979 1.449

5 Dichloromethane 0.44 0.0272 376 40 1.33 1070 1.423

6 2-Butanol 3.7 0.0225 13.2 99.5 0.807 1240 1.001

7 Cyclohexane 0.98 0.0246 78.8 81 0.778 1454 1.131

8 Carbon tertrachloride 0.97 0.0264 99.6 76 1.58 926 1.463

9 Cyclohexanone 2.2 0.0345 3.1 156 0.948 1423 1.349

10 Acetophenone 1.74 0.039 0.35 82 1.024 1492 1.528

11 Chlorobenzene 0.8 0.0323 9.5 132 1.106 1273 1.408

12 Hexane 0.31 0.0178 128 69 0.659 1112 0.733

13 Diisopropyl ether 0.33 0.018 123 68 0.724 976 0.707

14 Tributyl phosphate 3.88 0.0278 27 180 0.979 1272 1.245

Variation ofViscosity

Surface Tension

Vapour Pressure

Main achievements

30.01.2013

Extraction: design of set-up

Main achievements

30.01.2013

• Crystallisation: set-ups

Saturated solution

Use of water bath for sonication

US generator and amplifier

Cooling bath

First-version flow reactor

Batch reactor

Main achievements

30.01.2013

• Crystallisation: MSZW

• Exchangeable bottom (transducer)• 8 W calorimetric power• Frequencies 40-1140 kHz

• 20 g/L paracetamol in water• Start at 40°C• Cooling rate: 0.7°C/min

Main achievements

30.01.2013

• Crystallisation: MSZW

0

2

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12

14

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0 100 200 300 400 500 600 700 800 900 1000 1100 1200

Aver

age

redu

ction

in M

SZW

(°C)

Frequency (kHz)

• Decrease in effect of ultrasound on MSZW with increasing frequencies• Fastest nucleation at lowest frequency

Main achievements

30.01.2013

• Crystallisation: PSD

Silent conditions SonicationMean diameter (µm) Span Mean diameter (µm) Span

Batch 447,63 0,9902 65,56 1,097

Milliflow 303,38 0,6888 25,96 1,365

50

1090

DDDSpan

Main achievements

30.01.2013

• Crystallisation: seeding crystals

With US:lots of crystals after 30 seconds

Without US: few crystals after 15 minutes

Main achievements

30.01.2013

• Characterization of the US field in present set-up

o Effect of US on control of nucleationo High intensity focused at a point/region

o Process Design: Use of water (waterbath) for impedance matching.

Main achievements

30.01.2013

• Second-version flow reactorsMeasurement acoustic properties

Lambda/2matching layer

Lambda/4reactor prototype

PFA tube PP tube

Problems & deviations

30.01.2013

• Delayed start up of VLE workThree researchers have started and should deliver results in due time

Plan for the next 6 months

30.01.2013

• Continue with data generation for crystallization (batch and continuous) at KUL and TUD

• Pilot experiments with OBFC: in cooperation with JP• Set-up ready for extraction and generation of data• Dedicated flow reactor by SM ready for nucleation• Characterization methods for US field ready (PIV/PIT,

T, chemiluminescence, etc.) and generation of data• Start up of VLE task; interaction foreseen between

KUL and TUDO in august/september

Deliverables & milestones

30.01.2013

Deliverables for Year 1• Set of experimental data available for comparison

between US and non-US and for input to modelling• Start with modelling for process design and control

Milestones• Month 12: set of experimental data available• Month 18: models for process design ready

Interactions with other WPs

30.01.2013

• Interaction with WP2 on:– Microwave evaporative crystallisation– Microwave VLE

• Spill-overs to WP4&5 • Interaction between WP1 members: – Meeting in Leuven, April 8th, 2013 (KUL, TUD, SM, JP)– Meeting in Dresden, May 22nd, 2013 (KUL, TUD, SM)– Meeting Amersfoort, July 8th, 2013 (KUL, TUD, SM, JP)– Material and mails going back & forth frequently

Additional slides

30.01.2013

MSZW

30.01.2013

0

5

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40-90 kHz transducer

silent

165kHz transducer

silent

Meinhardt transducer

silent

40.7 97.7 165 570 850 1140

Aver

age

MSZ

W (°

C)Frequency (kHz)

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0 200 400 600 800 1000 1200

MSZ

W (°

C)

Frequency (kHz)