Experimental studies on multiphase flow in an air lift

contactor

By
Ankit Ojha
ENGG01202201055

Bhabha Atomic Research Centre, Mumbai

A thesis submitted to the

Board of Studies in Engineering Sciences

In partial fulfillment of requirements

for the Degree of
MASTER OF TECHNOLOGY
Of
HOMI BHABHA NATIONAL INSTITUTE

December, 2023

I
II
 ACKNOWLEDGEMENT

I would like to express my deepest sense of gratitude towards my project guide Dr. Nirvik
Sen and technology advisor Shri Debmalya Mukherjee who supervised my work and
provided me with valuable suggestions during the project. Their support and guidance were
invaluable towards unhindered progress of this project.

I would also like to convey my regards to Dr K.K Singh, Head, PMDS, who provided me the
opportunity and the resources to carry out this project in a systematic manner.

I would also like to extend my sincere obligation towards the entire staff of Chemical
Engineering Division who have helped me in this endeavor.

Ankit Ojha

III
 Table of content

ACKNOWLEDGEMENT.........................................................................................................II

LIST OF FIGURES....................................................................................................................3

PRESENT STATUS OF WORK...............................................................................................5

ABSTRACT...............................................................................................................................7

CHAPTER 1 Introduction......................................................................................................9

1.1 Liquid - Liquid extraction...............................................................................................9

1.2 Equipment’s used for liquid-liquid extraction..............................................................10

1.2.1 Air lift contactors:..............................................................................................10

1.2.2 Mixer settler:......................................................................................................10

1.2.3 Centrifugal Extractor:.........................................................................................11

1.2.4 Packed column:..................................................................................................12

1.2.5 Sieve column:.....................................................................................................12

1.2.6 Pulse column:.....................................................................................................12

1.3 Motivation of work.......................................................................................................13

1.4 Outline of thesis............................................................................................................13

CHAPTER 2 literature review..............................................................................................15

2.1. Literature survey on two phase flow in airlift contactor...........................................15

CHAPTER 3 Experimental studies on gas-liquid two-phase flow....................................19

3.1 Experimental setup and procedure.................................................................................19

3.1.1. Material used..........................................................................................................19

3.1.2. Experimental setup.................................................................................................19

3.1.3. Analysis of the image stack....................................................................................22

3.2 Comparison of different indices of mixing time............................................................25

3.3 Results and Discussion...................................................................................................29

3.3.1. Effect of air flow rate on mixing time........................................................................29

1
 3.3.2. Effect of submergence on mixing time..................................................................32

3.3.3. Effect of air flow rate on gas-liquid hydrodynamics.............................................36

3.3.4. Effect of air flow rate on ejection length of bubble swarm....................................37

3.3.5. Effect of air flow rate on bubble size distribution..................................................38

3.3.6. Effect of submergence on bubble size distribution................................................41

CHAPTER 4 Experimental studies on gas-liquid-liquid three phase flow.......................43

4.1 Experiments...............................................................................................................43

4.1.1 Material used......................................................................................................43

4.1.2 Experimental setup and procedure.....................................................................43

4.2 Results and Discussion..............................................................................................46

4.2.1 Effect of airflow rate and O/A ratio on dispersion band thickness in mixer......46

4.2.3 Effect of air flow rate and O/A ratio on drop size distribution..........................49

4.2.4 Effect of O/A ratio on mixing time in aqueous phase........................................53

CHAPTER 5 Measurement of mixing time with ultrasonic probe...................................55

5.1 Experimental setup....................................................................................................55

5.2 Ultrasonic (UT) Sensor and associated electronics...................................................56

5.3 Signal processing and mixing time analysis..............................................................57

5.4 Result and discussion................................................................................................62

CHAPTER 6 Conclusion.......................................................................................................63

6.1 Gas-liquid two phase flow.........................................................................................63

6.2 Gas-liquid-liquid three phase flow............................................................................64

2
 LIST OF FIGURES

Figure 1: Air lift contactor ( rajeshwari et al. 2019).................................................................9

Figure 2: Mixer Settler (law. et al. 2008)................................................................................10
Figure 3: Centrifugal Extractor (law. et al. 2008)...................................................................11
Figure 4: Experimental setup..................................................................................................21
Figure 5: Schematic of air lift mixing element.......................................................................22
Figure 6: Photograph of experimental setup taken after tracer injection (from Left to right)
(Q=35 LPM, submergence =17.4 cm).....................................................................................23
Figure 7: Snapshot showing location where intensity is measured........................................24
Figure 8: Temporal variation of intensity at top of glass beaker for 35 LPM air flow rate and
17.4 cm submergence a) without Kalman filtering at top and b) with Kalman filtering at top
c) without Kalman filtering at bottom d) without Kalman filtering at bottom........................25
Figure 9: Comparison of estimated values of t95 for raw (left) and smoothed (right) data.....27
Figure 10: Comparison of estimated values of t95 for raw (left) and smoothed (right) data...29
Figure 11: Variance based mixing time for raw (left) and smoothed (right) data..................30
Figure 12: Variation of mixing time with air flow rate. (b) Experimental setup of mixing
element c) Snapshot of mixer at different flow rate.................................................................33
Figure 13: Snapshots of the tracer mixing dynamics at different air flow rates.....................35
Figure 14: Effect of submergence on mixing time.................................................................35
Figure 15: Snapshots of the tracer mixing dynamics at different submergence level............36
Figure 16: a) Effect of location of tracer injection on mixing time and b) visual
representation (top view) of location of tracer injection (0 degree, 90 degree, 180 degree and
360 degree respectively from left to right)...............................................................................38
Figure 17: a) Snapshot of ejection length variation with air flow rate b) Graphical
representation of variation of ejection length with air flow rate..............................................40
Figure 18: Effect of air flow rate on a) bubble size distribution.............................................41
Figure 19: Variation of Sauter mean bubble diameter with airflow rate................................42
Figure 20: Bubble size distribution at different submergence level.......................................44
Figure 21: Sauter mean bubble diameter at different submergence level...............................44
Figure 22: Schematic of experimental setup...........................................................................46
Figure 23: Experimental setup of CALMSU..........................................................................47
Figure 24: Mixing element of CALMSU................................................................................47

3
Figure 25: Effect of O/A ratio and air flow rate on Dispersion band thickness in mixer.......48
Figure 26: Dispersion band thickness in mixer at constant O/A ratio of 1 and air flow rate of
20, 30, 40 and 50 LPM respectively (left to right)...................................................................48
Figure 27: Settling chamber schematic...................................................................................50
Figure 28 Dispersion band thickness in settler at constant air flow rate of 40 LPM and O/A
ratio of 1,2 and 3 ( Left to right)..............................................................................................50
Figure 29: Effect of O/A ratio and air flow rate on Dispersion band thickness in mixer.......51
Figure 30: Effect of O/A ratio and air flow rate on Sauter mean drop size............................52
Figure 31: Drop size distribution at 40 LPM and O/A ratio =1 and 2....................................52
Figure 32: Drop size distribution at 50 and 30 LPM at O/A ratio =1.....................................53
Figure 33: Error bar plot for mixing time change (y axis to 0 to 250 sec). Put plot of
dispersion band thickness for O/A=2.......................................................................................54
Figure 34: Mixing time at different O/A ratio and at constant air flow rate of 20 LPM........55
Figure 35: Mixing dynamics in 3 phase flow at time 5 sec, 50 sec, 100 sec and 150 sec ( left
to right)for O/A ratio of 1 at 20 LPM......................................................................................55
Figure 36: Mixing time at different O/A ratio and at constant air flow rate of 20.................56
Figure 37: Experimental setup for mixing time measurement with UT probe.......................58
Figure 38: Filter magnitude response.....................................................................................58
Figure 39: Normalised amplitude echo obtained in each acquisition for 0.25 milli-second for
an air flow rate of 40 LPM and submergence of 17.4 cm........................................................59
Figure 40: Normalized UT curve for 50 LPM and 17.4 cm submergence.............................61
Figure 41: Typical C-scan image............................................................................................62
Figure 43: Zoomed view of normalised two dimensional image 17.4 cm submergence and 30
LPM air flow rate.....................................................................................................................63
Figure 42: Echo of UT at submergence of 17.4 cm and air flow rate of 30, 40 LPM............63
Figure 44: Echo of UT at 40 LPM and submergence of 11.4 cm and 15.4 cm......................63
Figure 45: Signal at time t1, t2 and t3......................................................................................64
Figure 46: Correlation value at different time........................................................................65
Figure 47: Correlation(y axis) vs time(x axis)........................................................................65
Figure 48: comparison of mixing time obtained from UT experiments and colorimetry for
different air flow rate...............................................................................................................66
Figure 49: comparison of mixing time for colorimtery and UT for different submergence
level..........................................................................................................................................67

4
5
 ABSTRACT
Air-lift-based solvent extraction (SX) contactors are promising in both the front and back-end

of the nuclear fuel cycle. Such contactors rely on air-induced lifting and eventual dispersion

of one liquid phase (generally organic) into another (generally aqueous). Mass transfer of

solute occurs because of the interfacial area generated due to dispersion, and yet there is no

moving component in the contactor that may require maintenance after prolonged use. This

makes these contactors attractive in applications requiring handling of highly radioactive

materials (e.g., reprocessing, radiochemical separations/purification, etc.). Hydrodynamic

studies and mixing calculations under gas-liquid two-phase flow in a novel air-lift contactor

are reported in the first part of this report. A photographic technique involving a coloured

tracer is used. Distribution of the tracer is tracked using a high-speed imaging system for the

determination of mixing time. Systematic experiments are carried out to determine the effect

of air flow rate, submergence of the mixer, and location of tracer addition on mixing time.

Experiments were also performed to determine the effect of air flow rate and submergence on

bubble size distribution and the estimation of Saunter mean bubble diameter. The next part of

this report deals with experimental studies in gas-liquid-liquid three-phase flow. Experiments

were performed for three-phase gas-liquid-liquid flow with mixing driven by air using a

mixing element. The dispersion band thickness and drop size distribution are found to be

dependent on the air flow rate and organic-to-aqueous ratio (O/A). The mixing time in the

aqueous phase of gas-liquid-liquid flow is determined using colour tracer and digital image

analysis and is reported in the same section. The last part of this report deals with

experimental studies performed using the Nobel ultrasonic (UT) technique for mixing time

calculation. The mixing obtained from the UT technique is then compared with mixing time

obtained using colormetry. The experiments and analysis conducted in this work constitute

6
fundamental research aimed at characterizing two- and three-phase flows in a novel air-lift

mixer-settler. Further research is required to fully characterize the system.

7
 CHAPTER 1
Introduction

1.1 Liquid - Liquid extraction

Liquid-liquid extraction, also known as solvent extraction or partitioning, is a fundamental

separation technique used in various industries and research fields. It involves the transfer of

a solute from one liquid phase to another based on its differential solubility.

Liquid-liquid extraction is employed for a range of purposes, including the isolation and

concentration of valuable compounds, removal of impurities, separation of different

components from a mixture, and recovery of desired substances from complex

matrices(Muller et al. 2000). It is commonly used in the pharmaceutical industry for drug

discovery and production (Mansour et al.2017), in the petroleum industry for refining and oil

extraction, in environmental analysis for water and soil remediation, and in nuclear fuel cycle

processes for reprocessing and separation of radioactive materials (Drain et al. 2003). One of

the key applications of liquid-liquid extraction in the nuclear industry is in the reprocessing of

spent nuclear fuel. During reprocessing, liquid-liquid extraction is used to separate and

recover valuable isotopes from the spent fuel, allowing for their reuse in nuclear reactors or

for the production of new fuel. This process helps in the management of nuclear waste and

the reduction of the environmental impact associated with the disposal of spent fuel (Todd et

al. 2000).

The equipment used in liquid-liquid extraction depends on the scale and complexity of the

process. At a laboratory scale, separator funnels or glass extraction columns are often

employed. These allow for the controlled mixing of immiscible liquid phases, followed by

phase separation through gravity or centrifugation. In industrial settings, more advanced

equipment such as extraction towers, mixer-settlers, and centrifugal extractors, airlift

8
contactors are utilized to handle larger volumes and achieve higher separation efficiencies

(law et al. 2008).

Extraction towers consist of a series of packed beds or sieve plates, facilitating continuous

counter-current contact between the two liquid phases. Mixer-settlers employ mechanical

agitation to enhance mass transfer and settle the separated phases for further processing.

Centrifugal extractors utilize centrifugal force to enhance the separation process (quick mass

transfer and highly efficient phase separation), allowing for higher throughput and improved

efficiency (law et al. 2008).

1.2 Equipment’s used for liquid-liquid extraction

1.2.1 Air-lift contactors:

Air-lift contactors are innovative and efficient systems used in various

industries for a wide range of applications. These contactors rely on the

principle of air-induced lifting and dispersion of one liquid phase into

another, allowing for efficient mass transfer without the need for moving

parts (Lade et al. 2015). The unique design and operation of air-lift

contactors make them attractive for applications requiring the handling of

Figure 1: Air lift
contactor ( rajeshwari
highly radioactive materials, such as reprocessing, radiochemical separations,
et al. 2019)
and purification processes in the nuclear industry (rajeshwari et al. 2019).

1.2.2 Mixer Settler:

A mixer-settler is an equipment used for liquid-liquid extraction, involving the separation and

purification of components from liquid mixtures. It consists of interconnected vessels for

mixing and settling immiscible liquid phases. In the mixer, the phases are agitated to promote

mass transfer and solute transfer based on solubility differences. The mixture then flows to

the settler, where gravity aids in phase separation, with the heavier phase settling at the

9
bottom and the lighter phase forming a distinct layer on top. The separated phases are

collected separately for further processing Mixer-settlers are widely used in industries such as

chemicals, pharmaceuticals, and mining, as well as in the nuclear fuel cycle for the extraction

and purification of radioactive isotopes from spent fuel. They are valued for their efficiency,

scalability, and ease of operation (Hossain et al. 1983)..

Figure 2: Mixer Settler (law. et al. 2008)

1.2.3 Centrifugal Extractor:

A centrifugal extractor is a type of liquid-liquid extraction equipment that utilizes centrifugal

force to achieve efficient separation and extraction of components from liquid mixtures. It

consists of a rotating drum or rotor, inside a stator (Jealous et al. 1951). The two liquids are

fed to the annular gap where very fine droplets are formed leading to very fast mass transfer.

The mixed phase is then led to the hollow region inside the rotor where centrifugal forces

separates out the mixed phase into clear liquids (law et al.2008). Centrifugal extractors are

commonly used in industries such as pharmaceuticals, petrochemicals, and food processing,

where high throughput and rapid separations are required.

10
 Figure 3: Centrifugal Extractor (law. et al. 2008)

1.2.4 Packed column:

A packed column is a type of liquid-liquid contactor that utilizes a column filled with packing

material to enhance the contact and mixing between immiscible liquid phases. The packing

material, often in the form of structured packing or random packing, provides a large surface

area for mass transfer between the phases. As the liquid phases flow through the packed

column, intimate contact occurs, allowing for the transfer of solutes and desired components.

Packed columns are widely used in industrial processes for liquid-liquid extraction,

distillation, and absorption. They offer advantages such as high separation efficiency,

scalability, and versatility in handling a wide range of liquid mixtures (Seibert et al. 1988).

1.2.5 Sieve column:

A sieve column is another type of liquid-liquid contactor used for efficient contact and

mixing of immiscible liquid phases. It consists of a column containing a series of horizontal

or inclined perforated plates, known as sieves or decks, with holes or slots. The liquid phases

flow through the column, and as they encounter the sieves, they are distributed across the

column, promoting contact and mixing. The sieve column enhances mass transfer and allows

11
for the extraction and separation of desired components. Sieve columns are commonly

employed in industries such as chemical processing, pharmaceuticals, and environmental

engineering, where efficient liquid-liquid extraction is required. They offer benefits such as

high separation efficiency, flexibility in design, and ease of operation and maintenance.

1.2.6 Pulse column:

A pulse column in the nuclear field is a vertical column used for solvent extraction processes,

particularly in nuclear fuel reprocessing. It employs pulsating liquid flows to enhance the

separation of radioactive isotopes from a liquid stream. The periodic liquid pulsation

improves mixing and mass transfer between the phases, aiding in the selective extraction of

specific isotopes. Pulse columns offer efficient and flexible operation, contributing to the

purification and recovery of nuclear materials in a nuclear fuel cycle.( law et al. 2008)

1.3 Mixing time in contactors

Mixing time is a crucial parameter in various scientific and engineering fields where efficient

mixing is essential for achieving desired outcomes. It refers to the duration required for a

mixture to achieve homogeneity or uniformity within a vessel (Lamberto et.al., 2001).

Mixing time plays a vital role in determining the quality, consistency, and overall

performance of numerous processes involving fluids, chemicals, and materials (Olaofe et al.

2013).In the field of chemical engineering, mixing time greatly impacts chemical reactions.

Efficient mixing ensures proper dispersion of reactants, leading to faster reaction rates,

increased yield, and improved product quality (Holford J. M et al., 1999). It is especially

critical in industrial processes such as polymerization, fermentation, and pharmaceutical

manufacturing, where precise control over mixing time is necessary to achieve desired

chemical transformations (Towler et al., 2021).Biochemical engineering heavily relies on

mixing time to ensure optimal conditions for biological reactions. In bioreactors and

fermentation processes, mixing time affects the distribution of nutrients, gases, and

12
microorganisms, directly influencing cell growth, product formation, and metabolic

efficiency (Portner et al., 2005). Controlling mixing time allows for uniform conditions

throughout the reactor, promoting consistent yields and reducing potential drawbacks like

substrate limitation and cell inhomogeneity (Liu et al., 2018).Environmental engineering also

benefits from a thorough understanding of mixing time. In applications such as water and

wastewater treatment, mixing time determines the efficiency of processes like flocculation,

sedimentation, and disinfection (Chadwick et al., 2021). Adequate mixing ensures proper

contact between treatment agents and contaminants, maximizing removal efficiency and

enhancing water quality (Qasim et al., 2017). Furthermore, mixing time is significant in other

scientific disciplines, including material science, food processing, and even astrophysics. In

material science, it affects the dispersion of additives, particles, and fillers within composites,

influencing the final material properties (Chong et al. 2007). In the food industry, mixing

time impacts product texture, flavor, and stability (Rielly et al., 1997). Even in astrophysics,

understanding mixing timescales is essential for modeling stellar processes, such as nuclear

reactions and convective transport (Straka et al. 2007).Overall, the importance of mixing time

lies in its ability to optimize processes, improve product quality, and enhance efficiency

across a wide range of scientific and engineering disciplines . By precisely controlling mixing

time, researchers and engineers can achieve better outcomes in fields such as chemical

engineering, biochemical engineering, environmental engineering, material science, food

science, and astrophysics (Wu et al., 2022). Understanding mixing time helps engineers and

scientists in optimizing chemical processes, ensuring uniform distribution of ingredients, and

improving product quality in various industries. In liquid liquid extraction equipment mixing

time is used as a crucial parameters for scale up particularly in nuclear industry. The scale up

equipment mixing time is measured first before contaminating it with radioactive products for

13
mass transfer measurements. If the mixing time obtained is satisfactory then mass transfer

measurement are carried out otherwise it is rejected there itself.

1.4 Motivation of work

The rationale behind undertaking experimental studies on gas-liquid and gas-liquid-liquid

flows within air-lift contactors stems from the need to deepen our comprehension and

elevate the performance of this system. In the nuclear industry, three types of liquid-liquid

extraction (LLE) equipment are primarily utilized, namely, mixer-settler, pulse column, and

centrifugal extractor. Each possesses its own set of advantages and disadvantages. The

mixer-settler is favored in scenarios with low headspace but a large footprint; however, it

necessitates regular maintenance due to moving parts and motors. The pulse column is

particularly employed in areas with a low footprint but higher headspace, and it lacks

moving parts. On the other hand, the centrifugal extractor finds use where there is low

headspace and a small footprint, but it also requires maintenance due to moving parts.

Air-lift contactors present unparalleled advantages in the nuclear industry, requiring low

footprint, low headspace, and no moving parts. This is highly desirable in the nuclear sector,

especially in applications involving the handling of highly radioactive materials. Due to its

compact size, it can be retrofitted into existing plants, reducing both shielding and capital

costs. Despite its current use in the backend of the nuclear cycle, there is a lack of

fundamental understanding of its physics. This report aims to investigate the hydrodynamic

aspects of two-phase flow and three-phase flow within an air-lift contactor.

Hydrodynamic studies provide insights into the optimal operating range of equipment and

the impact of various operating parameters on system performance. Experimental studies in

gas-liquid and gas-liquid-liquid flows within air-lift contactors will yield valuable insights

into the dynamics and mixing characteristics inherent in these systems. Given the

14
complexity of the overall three-phase system, we initially conducted systematic studies on

gas-liquid flows. Experiments were systematically carried out to determine the effects of

various parameters, such as air flow rate, submergence level, and injection angles, on mixing

time and other hydrodynamic parameters like bubble jet length and bubble diameter. In the

context of three-phase flow, experiments were conducted to observe the effects of the O/A

ratio (volume of organic to aqueous phase) and air flow rate on dispersion band thickness

and drop size. Furthermore, mixing time in the aqueous phase was calculated, providing

crucial information for optimizing the design and operation of air-lift contactors. This

optimization aims to enhance efficiency, improve separation, and reduce operating costs.

1.5 Outline of thesis

The present thesis comprises six chapters, each addressing specific aspects of the research.

Chapter 1: serves as an introduction, providing an overview of liquid-liquid extraction and

air lift contactors. It sets the foundation for the subsequent chapters by highlighting the

various type of contactors used for liquid-liquid extraction in chemical processes and unit

operations.

Chapter 2: focuses on the literature survey conducted on air lift mixing equipment to

identify gap areas where further research is needed and comprehensive review of previous

studies published in context to air lift contactors.

Chapter 3: delves into experimental studies on gas-liquid two-phase flow, specifically

examining the effects of air flow rate, submergence, and tracer injection location on mixing

time. Additionally, the impact of air flow rate, submergence on jet length and bubble

diameter is also investigated in detail.

Chapter 4: deals with experiments studies on three phase gas-liquid-liquid flow. The three

15
phase flow being very complex hence systematic experiments are performed where only one

parameter is varied at once. Effect of O/A ratio and air flow rate on dispersion band

thickness, bubble size distribution and mixing time in aqueous phase is reported in this

chapter.

Chapter 5: presents feasibility study of mixing time by employing cutting edge advance

noninvasive techniques such as ultrasonic signal processing. The results obtained from these

studies are compared with mixing time data acquired through colorimetry. This comparative

study sheds light on the effectiveness of different measurement methods contributing to

valuable insights to the research.

Chapter 6: typically comprises the conclusion section, summarizing the findings and

outcomes of the performed experiments in two phase and three phase flow using different

technique, providing insights into the research objectives.

16
 CHAPTER 2
literature review

2.1.Literature survey on two phase flow in airlift contactor

Air-lift based solvent extraction (SX) contactors represents an important class of equipment

in hydrometallurgical and/or chemical industries. Such contactors rely on air induced lifting

and eventual dispersion of one liquid phase (generally organic) into another (generally

aqueous). Mass transfer of solute occurs because of interfacial area generated due to

dispersion and yet there is no moving component in the contactor which may require

maintenance after prolonged use. Absence of maintenance prone moving parts makes these

contactors robust and reliable. Another important factor is that unlike classical stirred tanks

contactors air-lift contactors do not lead to formation of very fine droplets. Formation of fine

droplets often aggravates operating problems like third phase/crud formation during operation

of solvent extraction cascades. This is particularly significant for hydrometallurgical

industries working with ores containing good quantities of silica. Absence of moving parts

also makes air-lift contactors extremely attractive in applications requiring handling of

radioactive materials (e.g. reprocessing, radiochemical separations/purification etc.). This

aspect has made air-lift SX contactors a vital equipment in back-end as well as front-end of

nuclear fuel cycle. The design of these contactors typically involve two separate inlet ports

for pumping of aqueous and organic phases (Lade et al., 2015). The pumping action is due to

the density difference created by air injection. Typically there is a dedicated air connection

for pumping of each phase. This design renders these contactors unique in their design and

make them differ from classical internal/external air-lift reactors that are prevalent in

industrial settings like air-lift bio reactors. One of the primary application of a classical air-

lift bio reactor is to mix the contents of the reactors using injected air. Determination of

17
mixing and/or circulation time is a classical technique to determine/quantify the effectiveness

of an air-lift type of reactor/contactor.

Several studies on determination of mixing/circulation time in external/internal air-lift

bioreactors have been reported. Sarkela and co-workers reported mixing and circulation time

to quantify the mixing performance of different geometries of air-lift reactor with helical flow

promoter (Sarkela et al., 2019). Mixing time in an external air-lift reactor was determined and

correlated to the liquid flow velocity (Gavrilescu and Tudose, 1997). The authors also studied

the effect of different geometrical parameters on mixing time. Gas hold up, mixing time and

liquid circulation velocity were reported in a concentric tube air-lift bio reactor as a function

of gas velocity (Merchuk et al., 1998). The authors reported presence of three different flow

regimes dependent on gas flow rate. Comparison of mixing time and liquid circulation

velocity in a square cross section air-lift reactor vis-à-vis a classical round/cylindrical air-lift

reactor was reported (Lu et al., 2000). Mixing characteristics in an internal air-lift reactor

with a low aspect ratio was reported (Zhang et al., 2014). Mixing time along with oxygen

mass transfer coefficient has been reported in a novel internal air-lift reactor where in the

internal draft tube was made of wire mesh (Fu et al., 2013). Recently mixing characteristic in

an external-loop air-lift fluidized bed reactor was also reported (Prończuk and Bizon, 2019).

Quality of mixing in an external air-lift packed bed reactor was also reported using the non-

invasive technique of electrical resistance tomography (Hamood-ur-Rehman et al., 2012).

Though there are studies on gas-liquid flows in air-lift based equipment/devices (e.g. bio

reactors) all of these feature air injection at the bottom of the riser. The riser can be placed

internally or externally, It may be of different shapes or made of even wire mesh. In

comparison there are only a handful of studies reporting a device based on air-lift principle to

lift and disperse one liquid into another. There are only a couple of studies on use of an air-

lift based mixer-settler (Lade et al., 2015; Rajeshwari et al., 2019). Lade et al., 2015 reported

18
a 10 stage combined air-lift based mixer settler unit (CALMSU) to extract dissolved TBP in

0.3 M HNO3 into dodecane. They reported volumetric mass transfer coefficient and specific

power consumption for mass transfer studies. However, the effects of operating parameters

on key hydrodynamic variables (like drop size, dispersion band thickness etc.) were not

studied. Similarly, Rajeshwari et al., 2019 reported a single stage cylindrical air-lift based

mixing device to extract U(VI) from 4 M HNO3 solution using 1.1 M TBP in dodecane

(batch studies). However, investigation of hydrodynamic variables was not done.

Quantification of the mixing characteristics of the mixing element of such CALMSU has not

been reported in literature. The present work intends to address this specific gap area.

Determination of mixing time represents the time it requires for an injected tracer to spread

uniformly across the entire volume of the equipment. Mixing time can be determined using

an invasive technique like placing a pH/conductivity probe at a specific point inside the

contactor or it can be done using a suitable non-invasive technique. Due to it’s simplicity and

ease of implementation an invasive point measurement technique is often employed. But

presence of a probe disturbs the flow filed and may affect the results depending on volume of

the equipment used. Amongst non-invasive techniques photographic/colorimetric technique

is the most widely used one. Initially colorimetry technique were used for mixing time

calculation based on human perception of color. Quantification of colorimetry using digital

image analysis is done to avoid human visual error. Colorimetry in combination with digital

image processing has been reported in various studies for measuring mixing time in stirred

vessels (Vega-Alvarado, 2011; cabaret et al., 2007; Kocaba et al.,2012; Reichmann et al.,

2018). Colorimetry with digital image analysis is commonly used for visualizing the flow

field and identifying conditions like presence of dead zones and/or segregated flow

(Norwood, and Metzner, 1960).

19
In this work, the technique of colorimetry along with digital image analysis is used to

measure mixing time in the novel air-lift contactor discussed above (mixing element of

CALMSU). A high speed imaging system and ultrasonic signal processing techniques are

used for capturing stack of images used in analysis of gas-liquid two phase flow and gas-

liquid liquid three phase flow. Water,30% TBP in dodecane and 0.01 M nitric acid are used

as the working fluid. The parameter such as dispersion band thickness, mixing time, bubble

and drop size distribution is estimated by analysis of the data generated through colorimetry

and UT. In mixing time calculation video (stack of images) is analysed to determine three

different types of mixing indices namely t 95 , t 99 and variance based. Different techniques are

used to smoothen out the raw intensity-time data are also compared. Measurement are taken

at different axial locations namely at top, middle and bottom of vessel to ensure throughout

mixing. A systematic study is carried out to determine the effect of air flow rate,

submergence of the mixer, location of tracer addition on mixing time. In final stage of two

phase flow experiments were done to measure hydrodynamic parameters such as bubble

diameter distribution, mean bubble size and bubble cloud ejection length in gas-liquid two

phase flow. At last effect of air flow rate and O/A ratio on dispersion band thickness, mixing

time in aqueous phase and drop size distribution in gas-liquid-liquid flow is reported in this

work. The dispersion band thickness and bubble size distribution are important parameters

used in mass transfer studies.

2.2.Gap Area

Based on the literature survey mentioned above, the following gap areas are identified:

Gas-Liquid Flow:

The use of non-invasive techniques to estimate mixing/circulation time and/or axial mixing,
as well as impact of air flow rate and submergence on bubble diamter in air-lift based
contactors is not reported.

Gas-Liquid-Liquid Flow:

20
Detailed information on the effect of operating/geometrical parameters on hydrodynamic
variables such as drop size, dispersion band thickness, etc., in air-lift based contactors is not
available. The use of non-invasive techniques to determine the kinetics of mass transfer as
well as mixing characteristics in gas-liquid-liquid flow in air-lift based contactors is not
reported.

21
 CHAPTER 3

Experimental studies on gas-liquid two-phase flow

In this chapter we present the experimental studies that have been carried out on gas-liquid

two-phase flow in an air lift mixing element. Experiments have been carried in a batch

manner where the mixer was placed inside a glass vessel and different hydrodynamic

variables were quantified. Effect of air flow rate, submergence, and tracer injection location

on mixing time have been studied. Additionally, the impact of air flow rate on jet length and

bubble diameter is also investigated in detail. All the results and corresponding discussions

are reported below

3.1 Experimental setup and procedure

3.1.1. Material used
Methylene blue powder used for preparation of tracer in the experiments (AR grade) was

procured from Sigma Aldrich. The tracer used was a 150 ppm solution of methylene blue in

DM water (Type 2, MilliQ). DM water (type 2, MilliQ) was used as the working fluid. Air

obtained from an oil-free laboratory compressor was used.

3.1.2. Experimental setup

22
Figure 4: Experimental setup

23
The experimental setup comprised of a 5L glass beaker, the mixing element, pneumatic

connection along with a calibrated rotameter and an oil-free laboratory compressor. The

schematics of the process is shown in Fig. 4. while the geometrical details of the mixing

element is shown in Fig. 5. Briefly the mixer comprises of two suction ports (A and B)

Incoming air to the air reservoir (R) is injected into the liquid through two air nozzles (0.81

mm inner diameter). The exit ports of these nozzles (port a, port b) open near the bottom of

two dedicated chambers (Ac, Bc). As air starts bubbling in these chambers effective density in

these chambers is reduced which creates a pressure difference and water gushes inside

through suction port A and B. The resultant air-water mixture moves upwards and exit

through the 3.2 mm exit holes (H) drilled at the front side. Thus there are two inlets through

which water will gush in shown as suction A and suction B in Fig. 5. This will enhance

uniformity of mixing across the entire volume because the ports are located at different

elevations. In a typical experiment

Figure 5: Schematic of air lift mixing element

24
we fill DM water up to pre-determined level and then slowly increase the air flow rate up to

pre-determined values as measured in the rotameter. Once steady state operation is

established 5 mL of tracer is added at a pre-determined location using a syringe. Care is taken

to ensure that the tracer volume is added as quickly as possible. In all cases the injection was

complete within less than 0.6 sec or 75 frames (verified with available video recording 125

fps). As mentioned earlier the tracer is 150 ppm of methylene blue in water. At this

concentration density of the tracer is the same as that of DM water yet its movement can be

tracked due to its intense blue colour. A high speed camera is used to acquire the image stack

of the mixing process and a LED based diffused illumination system is used to provide good

contrast. An image acquisition rate 125 frames/s is used for capturing the dynamics of tracer

mixing in the beaker. Fig. 6. shows a typical example of the tracer mixing in the breaker in

presence of the mixing element. Apart from mixing time measurements, experiments are also

carried out to determine hydrodynamics parameters such as bubble size distribution and

bubble ejection length. For these experiments once the steady state is attained, high-speed

images of the region near the holes (H) are acquired at a rate of 1000 frames/s.

Figure 6: Photograph of experimental setup taken after tracer injection (from Left to right) (Q=35
LPM, submergence =17.4 cm)

25
 Top(13.5 cm)

Centre( 10.26 cm)

(
Bottom( 5.13 cm)

Figure 7: Snapshot showing location where intensity is measured

3.1.3. Analysis of the image stack

For data analysis, an open source image processing software (ImageJ) was used to quantify

pixel intensity at three different locations - top, centre, and bottom - of the glass beaker ( Fig.

7) and highest of the three mixing time is taken as final mixing time to ensure throughout

mixing. As the bubbles move upward their shadow create random fluctuation in the intensity

value which is not attributed to the mixing of the tracer. This problem is more pronounced at

the top region of the vessel. A Kalman filtering process, as implemented in ImageJ, is used to

get rid of such frequency fluctuations and smoothen the intensity curve. The kalman filter is a

recursive prediction/correction algorithm which is based on the Kalman Filter to remove high

gain noise from stacks. It is very useful for noisy time-lapse movies. The effect of Kalman

filter can be seen in Fig. 8a and Fig. 8b which showthe intensity-time data at top location. If

there is no fluctuation (due to absence of bubble at the bottom location) in the intensity data

then Kalman filter will have no effect on data as shown in Fig. 8c and Fig. 8d. However, at

the top location where there is a significant presence of bubbles Kalman filtering makes a

significant improvement (Fig. 8a and Fig. 8b). As mixing progressed, the intensity (after

Kalman filtering) continuously decreases till a new steady state value is achieved, as depicted

in Fig. 8b and Error: Reference source not found8d. Even after applying Kalman filtering

some noise remain in the intensity-time data.

26
 (a) (b)

(d)
(c)

Figure 8: Temporal variation of intensity at top of glass beaker for 35 LPM air flow rate and
17.4 cm submergence a) without Kalman filtering at top and b) with Kalman filtering at top
c) without Kalman filtering at bottom d) without Kalman filtering at bottom.

At this stage we have tried to do a second round of smoothening using a moving average

technique and analysis is done to compare mixing indices determined from both the raw data

(only a first round of Kalman filtering) and the smoothened data (a second round of moving

average based smoothening on top of Kalman filtering). We have used three different

techniques to determine the mixing time. Determination of mixing time is based on

estimation of the time frame when a new steady state is attained. Thus it is critical to have a

27
consistent way of determining the time of onset of this this new steady state. We have

compared three different algorithm for this. In the first case we have estimated the widely

used mixing index t95. In this case a steady state intensity (Ifinal) is first manually selected

based on the average intensity values of last 1000 frame where a plateau is observed. The

video is taken long enough to ensure complete mixing of the tracer. Hence I 95 is determined
¿
as per Eqn. (1). Thereafter the revised intensity values at time t ( I 95 ,t ) is determined as per

condition given in Eqn (1a). Basically what Eqn. 1a does is it replaces value of intensity with

I 95 if I t differ by less than 5% of I 95 (95% of mixing intensity). If not, then value of

intensity remains the same. The intensity value obtained after applying this condition is
¿
termed as revised intensity value ( I 95 ,t ). Finally the onset of the new steady state is

determined as the first instant of time when there is no change of the revised intensity value (
¿ ¿
I 95 ,t ). Care is taken to ensure that there is no change in value of ( I 95 ,t ) for at least 20

consecutive frames. This ensures that the algorithm works even when there is undershoot or

overshoot of intensity values about the new steady state. Then t 95 is the difference between

the above mentioned time instant and the instant of trace injection (t 0). t0 is considered to be

the time when the tracer is first observed in the video. For the second case we have

considered another widely used mixing index t 99. In this case the methodology is exactly the

same as that for estimation of t95 except for the equations for estimation of I 99. In this case I99
¿
is estimated from Eqn. (2). Revised intensity values ( I 99 ,t ) are obtained as per Eqn. (2a).

Once again onset of new steady state is determined as the first instant of time when there is
¿
no change of the revised intensity value ( I 99 ,t ) for at least 20 consecutive frames. The indices

t 95and t 99 are essentially the time required for the tracer to mix to an extent of 95% and 99%,

respectively. Time can be calculated from frame number by equation 2(b).

I 95= |100
95
×I |
final (1)

28
if
| | I 95−I t
I 95
¿ ¿
× 100<5 , then I 95 ,t =I 95 , else I 95 ,t =I t (1a)

I 99= |100
99
×I | final (2)

if
| | I 99−I t
I 99
¿ ¿
× 100<0.01 , then I 99 ,t =I 99 , else I 99 ,t =I t (2a)

Frame number
M time(sec )=
Fps

(2b)

The third algorithm is the estimation of mixing time by determining the variance of intensity

versus time. This variance (determined as per Eqn. (3)) is plotted as a function of time.

∑ ( xi −μ )
2
2
σ =
N (3)

As the tracer mixes across the volume of the beaker the intensity changes with time. The

Time frame for I*95,t reaching a steady state Time frame for I*95,t reaching a steady

value (A) = 2323 state value (A) = 2460

Time frame of appearance of colour in the Time frame of appearance of colour in the

image (B)=373 frame image (B)=373 frame

95 % Mixing time (t95) = (A-B)/125 (where 95 % Mixing time (t95) = (A-B)/125

125 is the frame per second of the acquired (where 125 is the frame per second of the

29
 videos) = 15.6 sec acquired videos) = 16.6 sec

Figure 9: Comparison of estimated values of t95 for raw (left) and smoothed (right) data

Variance calculated from Eqn. 3 will be non-zero during initial mixing. However, as the rate

of mixing reduces with time it tends to converge to a value close to zero. The onset of the

new steady state is determined as the time instant when the variance reaches a value very

close to zero (0.02). Care is taken to ensure that the values of variance remains below 0.02 for

at least 20 frames so as to ensure that the algorithm works even there is an overshoot or

undershoot of intensity value. Then t var (variance based mixing time) is the difference

between the above mentioned time instant and the instant of trace injection (t 0).

3.2 Comparison of different indices of mixing time

In this section we compare the three mixing indices described above. For each mixing index

we have used two sets of intensity-time data which have undergone a single level of Kalman

filtering (labelled as raw data) and that which have undergone moving averaged based

smoothening in addition to Kalman filtering (labelled as smoothened data). Fig. 9 below

shows the estimation of t95 from raw and smoothed data as per the procedure mentioned

earlier. The plot is shown for the zero degree tracer injection point in the beaker for an air

flow rate of 35 LPM and a submergence of 17.4 cm.

It can be seen from Fig. 9 that for both data set a plateau can be identified in the plot of I*

with frame number. This is because of application of Eqn. (1) and (1a) to the original

intensity-time data. Onset of this plateau is used to visually determine t n for each case while t 0

(time of first appearance of colour in the video) is the same for both cases. 95 % mixing

index is essentially the difference between t n and t0. As can be seen from Fig. 9 values of t95

30
are similar for both data series but visual detection of the onset of plateau region is easier and

more conservative for smoothened data set.

Fig. 10 shows the estimation of t99 from raw and smoothed data. This procedure differs from

that for t95 only in terms of determination of I* data set as mentioned in equation 2 and 2a.

Once again the plot is shown for the zero degree tracer injection location in the beaker for an

air flow rate of 35 LPM and a submergence of 17.4 cm.

Time frame for I*99,t reaching a steady state Time frame for I*99,t reaching a steady state

value (A) = 3482 value (A) = 3516

Time frame of appearance of colour in the Time frame of appearance of colour in the

image (B)= 373 frame image (B)= 373 frame

99 % Mixing time (t99) = (A-B)/125 (where 99 % Mixing time (t99) = (A-B)/125 (where

125 is the frame per second of the acquired 125 is the frame per second of the acquired

videos) = 24.8 sec videos) = 25.1 sec

Figure 10: Comparison of estimated values of t95 for raw (left) and smoothed (right) data

It can be observed from Fig. 10 that for both data set variation of I* with frame number is

similar. However, in this case definition of I* (Eq 2a) is different from that for t 95. Hence the

plateau so evident in Fig. 9 at around 2300-2500 frames appears much later. This is clearly

because in this case we are considering even minor variations of intensity as the tracer

homogenises to a greater extent. For this case onset of this plateau is seen at around 3482 th

31
and 3516th frames. Corresponding values of mixing time (t 99) are determined to be 24.8 and

25.1 sec for raw and smoothened data series. In this case also using the smoothened data

leads to easier identification and more conservative value of the onset of the plateau. Finally

Fig. 11 shows the estimation of variance based mixing index from raw and smoothed data.

Once again the plot is shown for the zero degree tracer location in the beaker for an air flow

rate of 35 LPM and a submergence of 17.4 cm.

Time frame for variance reaching a value of Time frame for variance value reaching a

0.02 (A) cannot be determined in this case. value of 0.02 (A) = 1116

Hence estimation of mixing time (variance) Time frame of appearance of colour in the

cannot be done for this data set. image (B)= 373 frame

99 % Mixing time (t99) = (A-B)/125 (where

125 is the frame per second of the acquired

videos) = 5.94 sec

Figure 11: Variance based mixing time for raw (left) and smoothed (right) data

In this case it can be seen that both for raw and smoothened data the initial dip in intensity

due to mixing of dark blue coloured tracer with bulk water is captured quite well by high

values of variance. These elevated values indicate a substantial deviation in intensity values

over time. Once the overall decrease in intensity reaches a point where variance is minimal,

the values stabilize near zero. We select the instant of time when value of variance falls

32
below 0.02. The difference between this time (tn) and the instant the tracer is injected (t0) is

the mixing time (variance based). It can be seen that mixing time determined is 5.94 s and is

much less than t95 and t99. Another important point is that we could not carry out the analysis

of mixing time using this technique with the raw data set because variance value was highly

fluctuating in nature. This also indicates smoothened data are easy to analyse and visualise.

Table 1 compares the mixing indices determined using the three algorithms. It can be seen

that mixing time determined using the variance method is the lowest, followed by time for

95% mixing. Mixing time for 99% mixing is the highest. This essentially means that the

variance based technique is able to capture the major fluctuation in pixel intensity as the

tracer mixes. Thereafter, variance reaches near zero value. The finer level of fluctuations in

intensity can be determined successively using 95% mixing (Eqn. 1-1a) and 99% mixing

(Eqn. 2-2a) algorithm. The fact that t99 is the highest is also anticipated because this

represents the time at which near complete mixing of the tracer has been achieved.

Table 1: Mixing time obtained from three different algorithms

Method t99 t95 Variance

Raw Data 24.8 15.6 Cannot be

determined

Moving Average 25.1 16.6 5.94

For the rest of the work we have selected t 99 with moving average smoothening as the

representative mixing index. This is because this gives the time for near complete mixing of

the tracer and is easy to analyse. Also the design of the mixing element will be more

conservative.

33
3.3 Results and Discussion

3.3.1. Effect of air flow rate on mixing time

As the mixing element is air driven it is natural to expect that air flow rate will have a

significant effect on the mixing characteristics of the device. In this section we have reported

the effect of air flow rate on t 99. The experimental setup comprises of 3.5 L of DM water in a

5 L glass beaker. Submergence is 17.4 cm (corresponding volume being 3.5 L). The air flow

rate is systematically varied from 35 LPM to 60 LPM to investigate its impact on mixing

time. The tracer is released in front of the port B of the mixing element at zero degree. Fig.

12(a) shows the effect of Q (air flow rate) on t 99. As can be seen with an increase in Q,

mixing time is reducing till a critical value at 50 LPM. Further increase in Q beyond 50 LPM

is seen to increase mixing time. Initially an increase in Q will increase the relative presence

of gas in chamber Ac and Bc leading to an increase in pressure differential at ports ‘a’ and ‘b’.

This will increase the circulation rate, which in turn will reduce mixing time. Different

regions of the experimental setup are clearly marked in Fig. 12(b) for ready reference.

However, beyond a critical air flow rate of 50 LPM air starts going out through port ‘a’. At

this stage the kinetic energy of the incoming air equals or just exceeds the static (pressure)

head at point ‘a’. Due to this some air starts leaking/bubbling out through port ‘a’. Same is

true for port ‘b’. However this done not mean that gas hold up in chambers A c and Bc will

become stagnant after gas flow rate of 50 LPM as evidenced later (section 3.3). The rate of

increase in gas hold up inside A c and Bc only reduces. This reduces the rate of decrease in

static head inside Ac and Bc at location of port a and b with gas flow rate. However, the

significant factor here is the presence of bubbles outside the mixing element. Due to the large

density difference between water and air presence of even a small fraction of gas outside the

mixing element significantly reduces static head in the region of the beaker around port a. On

an overall basis the net pressure differential across the region inside A c/Bc and outside the

34
mixing element (at the location of ports a and b) decreases, which in turn decreases

circulation rate eventually increasing mixing time. The results shown in Fig. 12 (a) has been

repeated (experiments corresponding to air flow rate of 45, 50 and 55 LPM) three time so as

to ensure that the results are reliable. Coefficient of variance of the repeatability trials is

8.04%. Fig. 12 (c) shows the snapshots of the mixer in operation at different flow rates. It can

clearly be seen that beyond a flow rate of 50 some air bubbles are coming out of port a (lower

suction port encircled with red colour shown in Fig. 12c). Similar phenomena also happens

for port b but that is not visible in the images Fig. 12(c). At this stage it may be mentioned

that for the set of conditions mentioned here the mixer does not work at an air flow rate of 10

LPM. There is hardly any circulation at that flow rate.

(a) (b)

Q=30 LPM Q=40 LPM Q=45 LPM

35
 Q=50 LPM Q=55 LPM Q=60 LPM

Figure 12: (a) Variation of mixing time with air flow rate. (b) Experimental setup of mixing element
(c) Snapshot of mixer at different flow rate

Fig. 13 shows the evolution of the tracer as it mixes at three different air flow rates. The

snapshot are compared at 2 sec, 4 sec,10 sec and 20 sec fixed intervals of time. It can clearly

be seen from Fig. 13 that mixing time (t99) at an air flow rate of 50 LPM air flow is the

minimum. Fig. 7 also marks the three axial locations where mixing time has been determined.

t99 values reported earlier in Fig. 12 is the maximum among those determined for all three

locations.

Snapshot of tracer at airflow rate of 30 LPM at 0 sec, 2 sec, 4 sec, 10 sec, 20 sec after
tracer injection

Snapshot of tracer at airflow rate of 40 LPM at 0 sec, 2 sec, 4 sec, 10 sec, 20 sec after

36
 tracer injection

Snapshot of tracer at airflow rate of 50 LPM at 0 sec, 2 sec, 4 sec, 10 sec, 20 sec after
tracer injection

Snapshot of tracer at airflow rate of 60 LPM at 0 sec, 2 sec, 4 sec, 10 sec, 20 sec after
tracer injection
Figure 13: Snapshots of the tracer mixing dynamics at different air flow rates.

3.3.2. Effect of submergence on mixing time

This section focuses on investigating the effect of submergence on the mixing time (t 99) (Fig.

14). The air flow rate is maintained at a constant value of 40 LPM, while the submergence

level (or liquid head) is varied between 9.4 cm to 17.4 cm from the bottom. The

corresponding volume of DM water used is 9.4 cm and 17.4 cm respectively. The tracer is

released in front of the port B of the mixing element. Fig. 14 clearly shows variation of

mixing time with submergence.

37
 Figure 14: Effect of submergence on mixing time.

Fig. 15 shows the evolution of the tracer as it mixes at three different values of submergence.

The snapshot are compared at 0 sec, 2 sec, 4sec, 10 sec and 20 sec fixed intervals of time. It

can clearly be seen from Fig.15 that mixing time (t99) at the submergence value of 11.4 cm

(corresponding volume of 200o ml) is highest.

Snapshots of the tracer mixing dynamics at 0 sec, 2 sec,4 sec,10 sec and 20 sec after tracer
injection at submergence value of 9.4 cm(1500 ml)

38
 Snapshots of the tracer mixing dynamics at 0 sec, 2 sec,4 sec,10 sec and 20 sec after tracer
injection at submergence value of 11.4 cm (2000 ml)

Snapshots of the tracer mixing dynamics at 0 sec, 2 sec,4 sec,10 sec and 20 sec after tracer
injection at submergence value of 13.4 cm (2500 ml)

Snapshots of the tracer mixing dynamics at 0 sec, 2 sec,4 sec,10 sec and 20 sec after tracer
injection at submergence value of 15.4 cm (3000 ml)
Figure 15: Snapshots of the tracer mixing dynamics at different submergence level.

3.3.3. Effect of tracer injection location on mixing time.

Till now the tracer has been released in front of the port B of the mixing element. In this

section we discuss the influence of location of tracer addition on mixing time. The

submergence and air flow rate are maintained at constant values of 40 LPM and 17.4 cm

respectively. Fig. 16 (a) shows the effect of location of tracer addition on mixing time. Fig.

16 (b) shows pictorially the four different points where tracer is injected. Mixing time is seen

to be lower when the tracer is added at points mentioned as 0 and 180 degree which are just

39
next to suction ports a and b respectively. Mixing time is higher when tracer addition is at

locations mentioned 90 and 270 degrees because they are just next to discharge or exit holes.

This is because when the tracer is added just in front of suction ports it gets sucked in quickly

through the suction ports where as when it is injected at perpendicular position w.r.t suction.

It is pushed away from mixing element because of discharge velocity of air-water mixture

Figure 16: a) Effect of location of tracer injection on mixing time and b) visual representation (top
view) of
3.3.4. Effect of air flow rate on ejection length of bubble swarm

A set of experiments are carried out to investigate how the ejection length of the bubble

swarm is affected by gas flow rate. Submergence is kept fixed at 17.4 cm. As the gas-liquid

mixture in the chamber Ac and Bc comes out of 5 number (on each side) of 3 mm holes, it is

40
ejected out through the holes due to prevalence of a relatively higher velocity at the location

of the holes. As the gas flow is increased this local velocity at the hole will increase which is

expected to increase the ejection length of the bubble swarm. Fig. 17 (a) shows the typical

snapshot of the bubble swarm coming out of the holes at different air flow rates. The ejection

length is defined as the maximum linear distance from the surface of the mixing element

where air bubbles can be detected. As gas-liquid flow is inherently a transient phenomenon

this distance varies across different frames in the acquired video. The ejection length reported

in the subsequent figure (Fig. 17 (b)) is the average of at least 50 ejection length from

different frames for each gas flow rate. A clear increase in in ejection length with gas flow

rate is seen in Fig. 17 (b) due to increase in local velocity at the holes as mentioned above.

Snapshot of ejection length at 35 LPM , 50 LPM, 55 LPM and 60 LPM (from left to right)

(a)

41
 (b)

Figure 17: a) Snapshot of ejection length variation with air flow rate b) Graphical representation of
variation of ejection length with air flow rate

One interesting observation is that the ejection length keeps on increasing even after the air

flow rate of 50 LPM. Beyond this some bubbles are seen to come out of port ‘a’ and ‘b’. In

fact this is argued to be the reason why mixing time increases after 50 LPM. However,

ejection length remains almost constant after 50 LPM. This is because of the fact that the air

starts leaking beyond 50 LPM.

3.3.5. Effect of air flow rate on bubble size distribution

Another interesting aspect of gas-liquid flow in this novel mixing element is the

characterisation of the bubble diameter and bubble size distribution. The stack of images

acquired near the exit holes are analysed to determine the size distribution of the bubbles in

Fig. 18. Fig. 19 shows the variation of Sauter mean bubble diameter with respect to air flow

rate. The Sauter mean diameter is obtained from figure 18 by eqn. 3a. Where n i represent

number of bubbles of diameter di.

3
ni d i
Sauter mean diameter ∑
ni d i
2 (3a)

42
Figure 18: Effect of air flow rate on (a) bubble size distribution

43
 Figure 19: Variation of Sauter mean bubble diameter with airflow rate.

An interesting observation is that Sauter mean bubble diameter is seen to increase with an

increase in air flow rate up to 50 LPM. Thereafter there is rather sharp and consistent fall in

bubble diameter. This is also clearly revealed in the bubble sized distribution plots shown in

Fig. 18. As air flow rate increases relative presence of gas in chambers Ac and Bc also

increases. This increases the collision frequency of the bubble leading to enhanced rate of

bubble coalescence. This leads to formation of bigger bubbles at higher flow rates. Increase

of air flow has another effect. It increases the local flow velocity (and hence turbulent energy

dissipation rates) at the exit holes which will have a tendency the break the outgoing bubbles

into smaller bubbles. This effect will tend to reduce bubble size with an increase in air flow

rate. As air flow rate is increased up to 50 LPM the phenomenon of increased coalescence

rate in the chambers Ac and Bc dominates and hence net bubble size increase. After crossing

the threshold flow rate of 50 LPM it is the other way round. Here the rate of increase in gas

hold up in chambers Ac and Ab is less than before because some bubbles comes out of the

ports a and b. Hence rate of coalescence will be limited. But at higher local velocities at the

44
holes the influence of enhanced bubble breakage rate at the holes dominates. Thus on an

overall basis Sauter mean bubble size reduces.

3.3.6. Effect of submergence on bubble size distribution

Experiments are also conducted to determine the effect of submergence of the mixer on

bubble size distribution and Sauter mean bubble diameter. Experiments are carried out at 40

LPM and submergence of 13 cm, 13.4 cm, 15.4 cm and 19.4 cm. These values of

submergence ensures that the mixing element is completely dipped inside water (i.e. all exit

holes (H) are inside water). The stack of images captured using the camera focussed near the

exit holes (H) is analysed and bubble size distribution is obtained. The results are shown in

Fig. 20. The corresponding values of Sauter mean bubble diameter is also shown in Fig 21.

As the submergence is increased from 13 cm to 19.4 cm in a stepwise manner, the static

pressure at port “A” increases leading to higher local suction velocity. The increase in local

suction velocity will lead to higher turbulent energy dissipation rates at the exit holes which

in turn will increase the breakage rate of the bubbles leading to formation of smaller bubbles

(seen in Fig. 21).

45
 Figure 20: Bubble size distribution at different submergence level

Figure 21: Sauter mean bubble diameter at different submergence level

46
 CHAPTER 4
Experimental studies on gas-liquid-liquid three phase flow

Experiments have been carried out on gas-liquid-liquid three-phase flow in an air lift mixing

element integrated with a gravity settler in a batch manner where the mixer was placed at

center of mixing chamber and different hydrodynamics variable are quantified. Effect of air

flow rate, O/A ratio on dispersion band thickness and bubble size distribution is studied.

Additionally, the mixing time is calculated for aqueous phase, the effect of O/A ratio on

mixing time is discussed in detail. All the results and corresponding discussions are reported

below

4.1 Experiments
4.1.1 Material used
Tri-butyl phosphate (Ar grade, Sigma Aldrich) and anhydrous dodecane (Ar grade, sigma

Aldrich) was procured and a solution of 30% TBP in Dodecane was made. The solution was

then equilibrated with 0.01 Molar HNO3 for 24 hr. The equilibrated solution was then used as

organic phase and 0.01 molar HNO3 prepared in DM water ( Type-2,Milliq) was used as

aqueous phase. Methylene blue powder used as tracer in the experiments (AR grade) was

procured from Sigma Aldrich. The tracer used was a 150 ppm solution of methylene blue in

DM water (Type 2, MilliQ). Air from oil free compressor was used for lifting and mixing of

fluid using mixing element.

4.1.2 Experimental setup and procedure

The experimental setup comprised of a mixer-settler chamber, the mixing element, pneumatic

connection along with a calibrated rotameter and an oil-free laboratory compressor. The

schematics of the process is shown in Fig. 22. While the photograph of original setup is

shown in Fig. 23 Briefly the setup comprises of a mixing chamber of volume 0.5 litre and

settling chamber of volume 2 litre connected with each other through a vertical opening of

47
12.5 cm and 0.8 cm wide . A mixing element specification as given in sec. 3.1.2 and Fig. 24

is mounted at the centre of mixing chamber from the top. A LED based diffused illumination

system of Gs Vitec (model LT-v9-15, 240 watt) is used to provide good contrast and a high

speed imaging system (PHOTO -FASTCAM) was then used for recording video at 125 fps to

capture three phase dynamics as shown in Fig. 22. The stack of images were then used for

analysed for dispersion band thickness, Bubble size distribution and mixing dynamics in

aqueous phase.

48
Figure 22: Schematic of experimental setup

Figure 23: Experimental setup of CALMSU

49
 Figure 24: Mixing element of CALMSU

In a typical experiments the mixer-settler is filled with aqueous and organic solution up to

predetermined level depending on O/A ratio. The mixing element is then placed from top at

the centre of mixing chamber and air flow rate is adjusted from control valve ahead of

rotameter and mixing is done till stable dispersion band is achieved( steady state ). As air

starts bubbling in these chamber Ac and Bc effective density in these chambers is reduced

which creates a pressure difference between chambers and fluid outside mixing element and

hence organic phase gushes inside through suction port B while aqueous phase gushes

through port A. The resultant mixture moves upwards and exist through the 3.2 mm exit

holes (H) drilled at the sides.

After steady state is achieved a high speed camera (PHOTON- FASTCAM) is then used for

capturing stack of images for measurement of hydrodynamics. Stacks of images are then

analysed using ImageJ software for measurement of dispersion band thickness and bubble

size distriubution. Apart from hydrodynamics studies experiments are also carried out for

measurement of mixing time in aqueous phase. 5 ml of blue colour tracer soluble only in

50
aqueous phase is injected quickly ( in less than 1 sec for all case verified with video

recording) in aqueous phase. A high speed camera is used for capturing mixing dynamics in

mixing chamber. The stack of images were then processed with image J for mixing time

calculation. The typical example of mixing dynamics in aqueous phase is shown in Fig. 36.

4.2 Results and Discussion

4.2.1 Effect of airflow rate and O/A ratio on dispersion band thickness in mixer

Figure 25: Effect of O/A ratio and air flow rate on Dispersion band thickness in mixer

As mixing proceeds a dispersion band is formed at interface of organic and aqueous phase in

mixing and settling chamber. Since the mixing is air driven the dispersion band thicknesses is

naturally expected to be dependent on air flow rate while it was also found to be dependent

on organic to aqueous ratio. An increase in air flow rate have very interesting effect on

51
dispersion band thickness. The dispersion band increases or decreased depends on critical air

flow rate if air flow rate is greater than critical air flow rate the dispersion band thickness

decreases while if it is less than that the dispersion band thickness increases. Critical air flow

rate as defined in two phase flow in chapter 3 is the air flow rate sufficient to balance the

hydrodynamic pressure available at bottom section. At low O/A ratio the hydrodynamic

pressure available at bottom section near port A is high thus critical air flow rate observed at

O/A=1 is 40 LPM in Fig.25. As O/A ratio is increased from 1 to 3 while keeping total

volume of fluid same the hydrodynamics pressure available at bottom section is decreased

because of increase in organic phase volume (organic phase is lighter than aqueous phase).

The critical air flow rate thus observed at O/A ration of 2 and 3 is lower than 40 LPM and

hence the dispersion band thickness decrease with increase in air flow rate. Fig 26 shows the

variation of dispersion band thickness with air flow rate for O/A ratio of 1. At air flow rate of

40 LPM the whole view glass is filled with disperse phase with further increase in air flow

rate the dispersion band thickness settles to a new smaller value. This is because of the fact

that some amount of air starts leaking out from suction (A) hence not utilised for mixing.

The O/A ratio demonstrates a inverse relationship with dispersion band thickness as. As O/A

ratio is increased the pressure available at bottom of mixing chamber decreases leading to

lower suction velocity. The lower suction velocity have lower shear rate, lower deformation

and less drop breakage and hence larger drop size and thinner dispersion band . This effect is

verified from bubble size distribution plot of Fig. 30. As O/A ratio is increased the drop size

increases for a particular air flow rate.

4.2.2 Effect of airflow rate and O/A ratio on dispersion band thickness in settler

52
The mixing and settling chambers are connected by a long vertical opening however in

settling chamber there is no air bubbles and no driving force like air for mixing. The trends

Outlet of mixing Inlet of mixing

chamber chamber

Figure 27: Settling chamber schematic

Figure 28 Dispersion band thickness in settler at constant air flow rate of 40 LPM and O/A ratio of 1,2
and 3 ( Left to right)

observed in settling chamber somewhat resembles to what observed in mixing chamber but

the effect of decrease in dispersion band after critical air flow rate is not observed in settler

chamber. Fig. 28 shows that the dispersion band thickness observed in settler. A wedge type

dispersion band is formed this is because of the fact that as fluid flows from inlet of settler to

its outlet (as marked in Fig. 27) the drop coalesces with aqueous phase. The dispersion band

thickness shown in Fig. 29 is at the average of dispersion band thickness at inlet middle and

outlet of the settling chamber. This is a conservative approach followed to average out error

as dispersion band thickness at inlet is high due to mixer present adjacent to it.

53
 Figure 29: Effect of O/A ratio and air flow rate on Dispersion band thickness in mixer

4.2.3 Effect of air flow rate and O/A ratio on drop size distribution
This section discuss the variation of drop size w.r.t airflow rate and O/A ratio. At a particular

O/A ratio the drop size first decreases then increases this phenomena is because of increase in

shear rate that reaches to a critical value then decreases as air starts leaking from suction port

as discussed in chapter 3. While an increase in O/A ratio decreases the suction velocity of

both phase and hence the shear rate between organic and aqueous phase decreases leading to

lower deformation and lower breakage of drops and hence higher drop size is observed in

Fig. 30. The drop size distribution at different air flow rate and O/A ratio is given in Fig. 31

to Fig. 32. The x axis curve is drop diameter in cm while y axis curve is normalised fraction

of population. 25 number of bubbles are taken for each distribution.

54
Figure 30: Effect of O/A ratio and air flow rate on Sauter mean drop size

Figure 31: Drop size distribution at 40 LPM and O/A ratio =1 and 2

55
 Figure 32: Drop size distribution at 50 and 30 LPM at O/A ratio =1

4.2.4 Effect of air flow rate mixing time in aqueous phase.

The mixing time in aqueous phase is dependent on characteristics time for drop to
coalesce with interface. At O/A ratio of 2 the dispersion band thickness is almost same at
different air flow rate. Hence the time taken by ink to diffuse via dispersion band to get
into continuous aqueous phase will be almost same. This is reflected in Fig. 33 at
different air flow rate the mixing time is almost same. The experiments done for mixing
time calculation was repeated twice at three different flow rate for O/A ratio of 2. The
coefficient of variance of data was 8.35%. The error plot for mixing time at different air
flow rate is given in Fig.33.

56
 Figure 33: Error bar plot for mixing time change (y axis to 0 to 250 sec). Put plot of dispersion
band thickness for O/A=2

4.2.5 Effect of O/A ratio on mixing time in aqueous phase

57
 Figure 35: Mixing dynamics in 3 phase flow at time 5 sec, 50 sec, 100 sec and 150 sec ( left to right)for
O/A ratio of 1 at 20 LPM

Figure 34: Mixing time at different O/A ratio and at constant air flow rate of 20 LPM

Mixing time analysis include injecting of 5 ml of tracer (methylene blue) which is soluble

only in aqueous phase. Care is taken to ensure that the tracer volume is added as quickly as

possible. In all cases the injection was complete with in less than 1 sec or 125 frames

(verified with available video recording 125 fps). At this concentration density of the tracer is

the same as that of DM water yet it’s movement can be tracked due to it’s intense blue

colour. The mixing time in aqueous phase is governed by time taken by ink to diffuse through

58
dispersion band thickness after it is discharged from top exit holes. The mixing dynamics in

aqueous phase is shown in Fig. 34.

The mixing time is measured at centre (marked with solid red line) in aqueous phase and

highest of the three mixing time is taken as final mixing time to ensure throughout mixing.

The mixing time is calculated based on algorithm given in chapter 3 for t 99 in 2 phase flow. It

is observed that mixing time is highest for O/A ratio of 1. Since diffusion through dispersion

band thickness is slowest step (because characteristic time for drop to interface coalescence is

more than that for mixing) the mixing time is highest where dispersion band thickness is

highest i.e at O/A =1 at all air flow rate as shown in Fig. 35 and Fig. 36. Since dispersion

band thickness is highest at O/A ratio of 1 the corresponding mixing time is highest.

Figure 35: Mixing time at different O/A ratio and at constant air flow rate of 20

59
 CHAPTER 5
Measurement of mixing time with ultrasonic probe

5.1 Experimental setup

Ultra sonic probe is anon invasive technique for measurement of parameters. In chapter 2 and

3 we have already seen measurement of hydrodynamics parameters using a noninvasive

technique i.e. calorimetry. However the calorimetric methods requires visual access to the

system while UT measurement don’t need it. Therefore it become very important since most

of the industrial system don’t have visual access. In this chapter we do the experimental

studies to find feasibility of mixing time calculation in an air lift contactor using an ultrasonic

probe for two phase flow. The experiments are conducted in a flat-bottomed 5 litre glass

beaker. Demineralized water is used as the bulk liquid and an air lift mixing element is kept

at the centre of glass beaker. Air from an oil free compressor is used for lifting and mixing of

fluid in beaker. Fig 31 shows the experimental setup. Liquid is filled upto 17.4 cm in beaker

and air flow rate is adjusted with a calibrated rotameter located at the upstream of mixing

element. The air flow rate and submergence is varied during experiments to determine its

effects on mixing time. In first case, the submergence is kept constant at 17.4 cm and air flow

rate is varied between 30 to 50 LPM, and in subsequent experiments airflow rate is kept

constant at 40 LPM and submergence is varied between 11.4 cm to 15.4 cm. The UT sensor

(details in next section) is placed in contact with the exterior of glass beaker (using a suitable

acoustic couplant) and is held in place throughout the experiment. The schematic of

experimental setup is shown in Fig. 37. A concentrated solution of ammonium nitrate (250

g/L) is used as the tracer. An important requirement for a suitable tracer solution is that sound

velocity in it should be widely different from that of bulk liquid (DM water in this case). Any

concentrated salt solution would typically meet this criterion. Ammonium nitrate is chosen

because of its ready availability and high saturation solubility in water. Thus the tracer is

60
essentially a liquid that is completely miscible with the original fluid in all proportions. The

tracer is added at the edge of the vessel diagonally opposite to the location of the UT sensor

for all experiments. However, it is not limited to any specific angular separation between the

tracer addition and sensor and will work equally well for other angular location. UT data

acquisition was started after 5 minutes of operation. This time is sufficient to get steady state

based on our previous experiments experience. After a period of 5 s from start of data

acquisition, the tracer (5 mL) is injected quickly. The ultrasound data acquisition is continued

for a minute. The acquired data is filtered to reduce noise. Fig. 38

Figure 36: Experimental setup for mixing time measurement with UT probe

Figure 37: Filter magnitude response

Shows image of filter used. The filtered data are then converted into C-Scan images which

are used for mixing time calculation and other analysis.

61
 5.2 Ultrasonic (UT) Sensor and associated electronics

A 2.25 MHz contact type transducer (in pulse-echo mode) is used. The choice of frequency

was based on fact that it was used earlier for other mixing time experiments. The sensor

transducer (enclosed in SS-316 casing) is energized with negative spike voltage of 120 V

with pulse duration of 200 ns. The same sensor is thereafter used as receiver for the reflected

echo, which is amplified using a low noise amplifier (LNA) and digitized at 80 million

samples per second (MSPS) at 12-bit resolution. This process is repeated 50 times every

second (pulse repetition frequency, PRF), thus achieving a scanning rate of 20 ms. All data

are recorded in the PC in near-real time and used for subsequent analysis.

5.3 Signal processing and mixing time analysis

First echo obtained from mixing
element (Echo of interest)
Second echo
obtained from
vessel wall

Figure 38: Normalised amplitude echo obtained in each acquisition for 0.25 milli-second for an air

flow rate of 40 LPM and submergence of 17.4 cm

62
Fig. 39 shows the UT signal received by sensor in 1 scan. In each scan there are two observed

echo, first is obtained from mixing element while second echo is obtained from vessel wall.

The enlarge view of echo of interest i.e from time 70 to 112.5 micro sec is shown in Fig. 40.

The fig 40 consist of 3 plots, namely Plot 1, Plot 2 and Plot 3. The plot 1 is echo before

mixing by air is started. The red dotted line in Plot 1 shows the onset or starting of first echo

multiple echoes of smaller magnitude are observed before the onset of echo of interest

because of air bubbles as shown in plot 2 of fig 40. These echoes are observed because size

of air bubbles diameters are comparable with UT wavelength (~0.5 mm). The Plot 3 is the

echo plot after the mixing has been completed. As the mixing progresses, the echo onset is

gets delayed, which can be observed in plot 1 and plot 3. In Plot 1, the onset is observed

before 95 micro sec while in Plot 3 it is observed after 95 micro sec (highlighted with red dot

line in Fig. 42). This is because of the fact that as ammonium nitrate is mixing into solution,

the speed of sound is changing in medium, which will change the time of flight.

63
 Plot 1

Plot 2

Plot 3

Figure 39: Normalized UT curve for 50 LPM and 17.4 cm submergence

64
Fig. 42 shows a typical C-Scan curve the region marked with dotted black double arrow

represent situation in front of sensor before mixing. It can be observed from visualisation that

as mixing proceeds, the onset time changes which is shown by red colour bracket. At the end

of mixing, the onset time settle to a new steady state value marked with dotted blue double

arrow. The mixing time is calculated from difference of scan numbers during mixing divided

by number of scan per sec as given in eq. 5

Similarly C-Scan at other experimental condition are given in fig 43 and Fig. 44.

Figure 43: Echo of UT at 40 LPM and submergence of 11.4 cm and 15.4 cm

5.4 Correlation algorithm for mixing time calculation

Mixing time onset can be calculated from correlation technique. Here a reference signal is
selected and other signals are moved with time “t” by superimposing on reference signal by
The two dimensional image (C-Scan) created from 3000 scan taken in 1 minute with a rate of
eqn. 5a
50 scan per sec is shown in Fig. 41. The two dimensional image created is then used for
echo(T): ∑ sig [n] . ref [n+T]
calculation of mixing time based on change in onset value observed visually. The zoomed
(5a)
view
WhenoftheFig. 41 is
signal shown
at time “t”inisFig. 42 for measurement
superimposed completelyof
themixing time.
value of The y axis
correlation represent
coefficient is
highest. The signal
scan number with 50at scan
different instance
per second of time
while is shown
x axis showsin fig.45
data .The signal
acquired in eachcorrelation with
scan at rate of
reference is shown in fig. 46. The value of onset obtained is shown in fig. 47.
80 million data per second.

65
4000

3000

2000

1000

0
6000 6500 7000 7500 8000 8500 9000

4000

3000

2000

1000

0
6000 6500 7000 7500 8000 8500 9000

4000

3000

2000

1000

0
6000 6500 7000 7500 8000 8500 9000

Figure 44: Signal at time t1, t2 and t3

66
 Figure 45: Correlation value at different time

echo by correlation
5

-5

-10

-15

-20

-25

-30

-35

-40

-45

0 500 1000 1500 2000 2500 3000

Figure 46: Correlation(y axis) vs time(x axis)

67
 5.5 Result and discussion

The mixing time obtained from C-scan of UT signal are then compared with mixing time

obtained from colorimetric experiments done for same submergence and air flow rate. Fig 48

shows comparison studies of mixing time obtained from both method at different air flow rate

keeping submergence constant at 17.4 cm. Fig 49 shows the comparison studies of mixing

time obtained from both method at different submergence keeping air flow rate constant at 40

LPM. The mixing time value obtained from UT experiments are comparable with mixing

time values obtained from colorimetry. The mixing values obtained from UT signals

represent time required to attained uniformity in front of sensor while value of mixing time

obtained from colorimtry is time required to attain uniformity at top, bottom and centre.

Figure 47: comparison of mixing time obtained from UT experiments and colorimetry
for different air flow rate

Figure 48: comparison of mixing time for colorimtery and UT for different submergence level

68
 CHAPTER 6
Conclusion

6.1 Gas-liquid two phase flow

A novel air lift based mixing element with two suction ports at different levels is

characterised in terms of it’s mixing efficiency and gas-liquid hydrodynamics. Experiments

are carried out in a 5 L glass vessel and mixing dynamics of a tracer (methylene blue

solution) is tracked using a high speed imagining system. DM Water is used as the working

fluid. Mixing time is estimated by analysis of the video using an open source image

processing software (Image-J). The acquired stack of images are filtered to get rid of the

interference of shadows of bubbles rising up. Three different algorithms/indices to

determine mixing time, namely t95 and t99 and variance based mixing time are compared. The

analysis is carried out on two types of intensity-time data set raw data and smoothen data

(moving average based). A comparison reveals that variance based mixing index only

captures the major/gross fluctuations in intensity due to mixing of the tracer where as t 95 and

t99 indices capture even finer levels of fluctuations. As t 99 provides a rather conservative

estimate of mixing performance of the mixing element this is adopted in the entire study. A

systematic study is carried out to determine the effect of air flow rate, submergence of the

mixer and location of tracer addition on mixing time. An increase in air flow rate has an

interesting trend on mixing time. Mixing time reduces with an increase in air flow rate till 50

LPM beyond which it starts to increase. Beyond 50 LPM some fraction of the injected gas

leaks through inlet ports which reduces the pressure differential leading to a drop in

circulation rate and hence an increase in mixing time. An increase in submergence is also

seen to first increase mixing time and then beyond a certain point decrease mixing time. This

is due to an interplay between an increases in volume of liquid (across which tracer must

mix) and increase in pressure differential and consequential circulation rate with increase in

69
submergence. It is also seen that when the tracer is added just next to the suction port the

mixing time is less. This is because in such a case tracer particles are immediately pulled into

the mixing element. Apart from mixing time measurements effect of the air flow rate on

bubble diameter distribution, Sauter mean bubble size and bubble cloud ejection distance are

also measured. An increase in gas flow rate increase the ejection length of the bubble swarm

due to an increase in local velocity at the exit holes in the mixing element. Also an increase in

air flow rate has a non-monotonic trend of bubble size distribution. The Sauter mean bubble

size first increase with an increase in air flow rate due to increase in rate of coalescence in

chambers Ac and Bc, reach a maxima (at the same location at which mixing time trend with

flow rate reverses) and then decreases due to rate of bubble breakage at higher local

velocities at the exit holes in the mixing element. In addition to this effect of submergence on

bubble diameter is measured. Smaller diameter bubble are observed with increase in

submergence. The increase in submergence results in higher local suction velocity. Which

increase the bubble breakage rate.

6.2 Gas-liquid-liquid three phase flow

Fundamental studies on gas liquid-liquid three phase flows was done for characterisation of a

novel air lift mixer settler in batch mode.30% TBP in dodecane was used as organic phase

and 0.01 M nitric acid was used as aqueous phase. A high speed imagining system was used

for capturing video. The captured stack of images were than analysed with image-J software

to see effect of air flow rate and organic to aqueous ratio(O/A) on dispersion band thickness,

bubble size distribution and mixing time in aqueous phase. The study reveals that air flow

rate significantly influence the dispersion band thickness. When the air flow rate exceeded a

critical value, the dispersion band thickness decreases, while it increases when the flow rate

fell below this critical value. The critical air flow rate is influenced by the O/A ratio. As the

O/A ratio increased the critical value decreases as static pressure available at bottom

70
decreases. The O/A ratio has inverse relationship with dispersion band thickness. As O/A

ratio is increased the dispersion band thickness decreases for a typical air flow rate. This is

because of reduced suction velocities, lower shear rates, and fewer drop breakages. Air flow

rate also influenced bubble size distribution. At a constant O/A ratio, an increase in air flow

rate initially reduced bubble size, but it eventually increased. This behaviour was attributed to

changes in shear rate, particularly when it reached a critical value.

Finally, in the aqueous phase, mixing time was measured using a tracer. The mixing time was

longest at an O/A ratio of 1 because of the slow diffusion through the dispersion band

thickness, which is the slowest step in the mixing process.

6.3 Ultrasonic technique

In the series of mixing time measurement with UT technique experiments were conducted in

a 5-liter flat-bottomed glass beaker, with demineralized water serving as the bulk liquid. At

the heart of the setup, an air lift mixing element was placed to facilitate mixing. The driving

force for the mixing process came from air supplied by an oil-free compressor. The primary

objective was to investigate the influence of both air flow rate and submergence on the

mixing time of the system.The experiments were divided into two sets. In the first set, the

submergence level was maintained at a constant 17.4 cm, while the air flow rate was

systematically varied within a range of 30 to 50 LPM. In the second set, the air flow rate was

held steady at 40 LPM, while the submergence levels were altered, ranging from 11.4 cm to

15.4 cm.

To measure the mixing time, ultrasonic (UT) sensors were employed. The tracer used in the

experiments was a concentrated solution of ammonium nitrate, chosen for its significant

difference in sound velocity compared to the bulk liquid, which was demineralized water.

The tracer solution was introduced into the vessel opposite to the location of the UT sensor.

71
The UT sensor, operating at a frequency of 2.25 MHz in pulse-echo mode, played a dual role,

first emitting a negative spike voltage of 120 V with a pulse duration of 200 ns, and then

receiving and amplifying the reflected echo using a low noise amplifier (LNA). These echoes

were digitized at a rate of 80 million samples per second (MSPS) with a 12-bit resolution,

and this process was repeated 50 times every second. The entire data was recorded in near-

real time for subsequent analysis. Mixing time analysis was facilitated by the creation of C-

Scan images from a series of 3000 scans taken within a minute. The scans were captured at a

rate of 50 scans per second. The mixing time was then calculated based on the change in the

onset value, reflecting the time required for the system to achieve uniformity in front of the

sensor.

Overall, this study concentrated on examining how air flow rate and submergence influenced

mixing time using UT sensors and a specialized tracer solution. The results from UT

experiments were compared to those obtained from colorimetry, demonstrating the reliability

of the UT method for measuring mixing time.

Future scope of work

1. Modelling of key parameters such as mixing time is reported in this work:- In

this work experimental studies and calculation of key parameters is reported. These

modelling of these key parameters for two phase and three phase flow is not reported

in this work.

2. Experimental studies to determine effect of geometry and physical properties on

hydrodynamics variables in two phase flow: - This work only covers the effect of

operating parameters on hydrodynamics variables such as bubble size distribution, jet

length, submergence etc. However experiments can be performed to find out effect of

geometry and physical properties.

72
3. Experimental studies for quantification of mass transfer in gas-liquid-liquid

flow:-Experiments can be performed on three phase flow system for calculation of

mass transfer coefficient and other important parameters.

4. Development of algorithm for mixing time calculation using UT signals:- The

signal obtained from UT sensors have multiple echoes before echoes of onset and it

required advance signal processing to automate this work. In this work each signal is

processed individually by visualisation for finding mixing time.

5. Procurement of ultra-low frequency ultrasonic sensors:- Since the frequency of

sensor used right now is 2.25 Mhz . The wavelength of the wave generated by this

sensor is comparable with bubble diameter. Hence sensor of lower frequency around

0.5 Mhz is required.

Notation

t99 Time corresponding to 95% sec

of mixing

t95 Time corresponding to 99% sec

of mixing

I95 95% of final intensity

I99 99% of final intensity

Ifinal Final intensity

It Intensity at time t

fps Frame per second

¿
I 95 ,t Revised intensity value at

time t after applying

equation 1a.

73
 ¿
I 99 ,t Revised intensity value at

time t after applying

equation 2a.

t0 Ink injection time sec

tn Steady state time sec

tvar Variance based mixing time sec

Greek
2
σ Variance

References

Cabaret, F., Bonnot, S., Fradette, L. and Tanguy, P.A., 2007. Mixing time analysis using
colorimetric methods and image processing. Industrial & engineering chemistry research,
46(14), pp.5032-5042.

Chadwick, A., Morfett, J., & Borthwick, M. (2021). Hydraulics in civil and
environmental engineering. Crc Press

Drain, F., Vinoche, R. and Duhamet, J., 2003. 40 years of experience with liquid-liquid
extraction equipment in the nuclear industry. SGN, Montigny-le-Bretonneux, 78182
Saint-Quentin-en-Yvelines Cedex (FR); COGEMA, 2 rue Paul Dautier, BP 4, 78141
Vilizy Cedex (FR); CEA VALRHO, BP 171, 30207 Bagnols-sur-Ceze Cedex (FR).

Gavrilescu, M. and Tudose, R.Z., 1997. Mixing studies in external-loop airlift reactors.
Chemical Engineering Journal, 66(2), pp.97-104.

74
Gharehbagh, F.S. and Mousavian, S.M.A., 2009. Hydrodynamic characterization of
mixer-settlers. Journal of the Taiwan Institute of Chemical Engineers, 40(3), pp.302-312.

Hamood-ur-Rehman, M., Dahman, Y. and Ein-Mozaffari, F., 2012. Investigation of

mixing characteristics in a packed-bed external loop airlift bioreactor using tomography
images. Chemical engineering journal, 213, pp.50-61.

Hossain, K.T., Sarkar, S., Mumford, C.J. and Phillips, C.R., 1983. Hydrodynamics of
mixer-settlers. Industrial & Engineering Chemistry Process Design and Development,
22(4), pp.553-563.

Holford, J. M., & Linden, P. F. (1999). Turbulent mixing in a stratified fluid. Dynamics
of atmospheres and oceans, 30(2-4), 173-198.

Kocaba, V., Gallucci, E. and Scrivener, K.L., 2012. Methods for determination of degree
of reaction of slag in blended cement pastes. Cement and Concrete Research, 42(3),
pp.511-525.

Lade, V.G., Wankhede, P.C. and Rathod, V.K., 2015. Removal of tributyl phosphate from
aqueous stream in a pilot scale combined air-lift mixer-settler unit: Process intensification
studies. Chemical Engineering and Processing: Process Intensification, 95, pp.72-79.

Lamberto, D. J., Alvarez, M. M., & Muzzio, F. J. (2001). Computational analysis of

regular and chaotic mixing in a stirred tank reactor. Chemical Engineering Science,
56(16), 4887-4899.

Law, J.D. and Todd, T.A., 2008. Liquid-liquid extraction equipment (No. INL/CON-08-
15151). Idaho National Lab.(INL), Idaho Falls, ID (United States).

Liu, W., Jia, H., Wang, J., Zhang, H., Xin, C., & Zhang, Y. (2018). Microbial fuel cell
and membrane bioreactor coupling system: recent trends. Environmental Science and
Pollution Research, 25, 23631-23644.

75
Lu, X., Ding, J., Wang, Y. and Shi, J., 2000. Comparison of the hydrodynamics and mass
transfer characteristics of a modified square airlift reactor with common airlift reactors.
Chemical Engineering Science, 55(12), pp.2257-2263

Müller, E., Berger, R., Blass, E., Sluyts, D. and Pfennig, A., 2000. Liquid–liquid
extraction. Ullmann's Encyclopedia of Industrial Chemistry.

Merchuk, J.C., Contreras, A., Garcia, F. and Molina, E., 1998. Studies of mixing in a
concentric tube airlift bioreactor with different spargers. Chemical Engineering Science,
53(4), pp.709-719.

Norwood, K.W. and Metzner, A.B., 1960. Flow patterns and mixing rates in agitated
vessels. AIChE Journal, 6(3), pp.432-437.

Olaofe, O. O., Buist, K. A., Deen, N. G., van der Hoef, M. A., & Kuipers, J. A. M.
(2013). Particle Mixing and Segregation in Gas-Solid Fluidized Beds Containing Binary
Mixtures.

Prończuk, M. and Bizon, K., 2019. Investigation of the liquid mixing characteristic of an
external-loop hybrid fluidized-bed airlift reactor. Chemical Engineering Science, 210,
p.115231.

Qasim, S. R. (2017). Wastewater treatment plants: planning, design, and operation.

Routledge.

Rajeswari, S., Karunakaran, R., Kalaiarasu, T., Robert Selvan, B. and Venkatesan, K.A.,

2019. Performance evaluation of a cylindrical air-lift mixer-settler device and

optimization of process parameters for the extraction of uranium (VI) from nitric acid

medium. Journal of Radioanalytical and Nuclear Chemistry, 322, pp.415-422.

76
Rielly, C. D. (1997). Mixing in food processing. Chemical engineering for the food

industry, 383-433

Reichmann, F., Jirmann, Y. and Kockmann, N., 2018, June. Mixing Time Scale
Measurement With Fast Exothermic Reactions Using Microchannel Reaction
Calorimetry. In International Conference on Nanochannels, Microchannels, and
Minichannels (Vol. 51197, p. V001T12A001). American Society of Mechanical
Engineers

Särkelä, R., Eerikäinen, T., Pitkänen, J.P. and Bankar, S., 2019. Mixing efficiency studies
in an airlift bioreactor with helical flow promoters for improved reactor performance.
Chemical Engineering and Processing-Process Intensification, 137, pp.80-86.

Straka, C. W., Lebreton, Y., Monteiro, M. J. P. F. G., & Zahn, J. P. (2007). Modeling
stellar interiors with rotational mixing. European Astronomical Society Publications
Series, 26, 49-64.

Towler, G., & Sinnott, R. (2021). Chemical engineering design: principles, practice and
economics of plant and process design. Butterworth-Heinemann.

Vega‐Alvarado, L., Taboada, B., Hidalgo‐Millán, A. and Ascanio, G., 2011. An image
analysis method for the measurement of mixing times in stirred vessels. Chemical
engineering & technology, 34(6), pp.859-866.

ZHANG, W., Yumei, Y.O.N.G., ZHANG, G., Chao, Y.A.N.G. and Zaisha, M.A.O.,
2014. Mixing characteristics and bubble behavior in an airlift internal loop reactor with
low aspect ratio. Chinese Journal of Chemical Engineering, 22(6), pp.611-621.

77