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INDIAN INSTITUTE OF TECHNOLOGY ROORKEE

Department of Mechanical and Industrial Engineering


SYNOPSIS
of the Ph.D. thesis entitled

Understanding Interfacial Entrainment Processes at Adiabatic


Three-Phase Domain and Liquid-Liquid Boiling

Proposed to be submitted in
partial fulfillment of the requirements for the Degree of
DOCTOR OF PHILOSOPHY
of the
INDIAN INSTITUTE OF TECHNOLOGY ROORKEE
by

Rupak Kumar
(Enrollment No. 18920030)

Supervisor
Dr. Arup Kumar Das

DEPARTMENT OF MECHANICAL AND INDUSTRIAL ENGINEERING


INDIAN INSTITUTE OF TECHNOLOGY, ROORKEE
ROORKEE – 247667, INDIA
May 2023
Understanding Interfacial Entrainment Processes at Adiabatic
Three-Phase Domain and Liquid-Liquid Boiling
1. Introduction

Interfacial entrainment of gaseous phase from liquid-liquid contact plane is relevant in various
industrial applications such as oil and gas exploration, emulsification, liquid-liquid extraction,
chemical processing, and iron processing. Moreover, buoyancy driven runaway of bubbles is
also a great passive technique of mixing to enhance the heat and mass transfer across the liquid-
liquid interface. The dynamic evolution of phase boundaries during such entrainment and
subsequent merging, splitting, reorientation etc. have significant role in governing the process
parameters of various fluidics devices.

2. Literature review and lacuna

Entrainment at a liquid-liquid interface through different routes has been summarized below.
Subsequently the lacuna of the literature is highlighted and objectives of the thesis are framed.

2.1 Entrainment at an adiabatic liquid-liquid interface induced by a gaseous phase

Many researchers have studied bubble bypass through a liquid-liquid interface in a pool. Both
experimental and numerical efforts are noticed (Bonhomme et al., 2012; Dietrich et al., 2008;
Emery et al., 2018; Kemiha et al., 2007; Uemura et al., 2010). Taylor bubble bypass through
liquid-liquid interface in conduit was only studied by Kar (2017) through experimental efforts.
Hence, fluidic understanding of the interfacial dynamics is still due which can be targeted using
numerical study of the phenomenon.

2.2 Entrainment at a liquid-liquid interface induced by nucleation

Nucleation at liquid-liquid interface has been studied experimentally by many researchers


(Apfel, 1972; Dincer et al., 1977; Drake et al., 1975a, 1975b; Enger, T; Hartman, 1971; Gordon
et al., 1961; Henry et al., 1974; Novaković and Stefanović, 1964), but most of the studies have
focused on boil-off rate only and no effort has been made to understand associated interfacial
dynamics.

3. Lacuna in literature and objectives of the present study

Based on the identified gaps of literature survey, following objectives are taken for study.
• Objective 1: Perform a detailed numerical study depicting entrainment at liquid-liquid
interface due to bypass of a Taylor bubble in a conduit and associated fluidic issues. The
effect of thermophysical properties on entrainment dynamics is also studied.
• Objective 2: Understand the effect of impact height, size, and film temperature of the
droplet on the fluidics of the immiscible drop impact onto a hot oil film.
• Objective 3: Interfacial dynamics during boiling of a sheet/film of a cryogen (LN2) over
a liquid contact.
• Objective 4: Numerically analyze the boiling of a cryogen (LN2) on solid (multi-mode)
and liquid contact.

4. List of contributions

The present dissertation attempts to investigate entrainment induced by uprise of Taylor bubble
and nucleation at a liquid-liquid interface. Careful experimentation and well resolved
numerical simulations are tried in the process. The study focusses on behavior of different
phases at a liquid-liquid interface in an adiabatic and diabatic configuration. Key findings in
each of these studies are as follows:

4.1. Entrainment at liquid-liquid interface in a conduit by a Taylor bubble

18
PDMS PDMS PDMS Linear film drainage
16
PDMS PDMS Retained film drainage
14
Air Air
Air Transition
12
Air
10 Gravity Capillary
δ*

Air 8 driven driven


Air
6
drainage drainage
4
2
0
Water Water Water Water Water 0 0.25 0.5 0.75 1 1.25 1.5
(a) (b) (c) (d) (e) t*

(a) (b)
Fig. 4.1 (a) Different fluidic stages during Taylor bubble bypass through liquid-liquid
interface in a conduit. (b) Transition from gravity driven drainage to cavity driven drainage.

• In the first part of dissertation, a 2D simulation with absolutely finer meshes is performed
to identify different fluidic stages (approach, encapsulation, de-encapsulation,
entrainment, and detrainment) when a Taylor bubble crosses water-PDMS interface in a
conduit (Fig. 4.1 (a)).
• During encapsulation stages, water film drains linearly under dominant buoyancy force
until the film thickness reaches capillary length scale (𝛿𝑐𝑟𝑖𝑡 = √𝜎/𝜌𝑔) thereafter, the
entrapped film drain rate retards (Fig. 4.1 (b)).
• De-encapsulation stage initiates with the sudden rupture and subsequent readjustment of
radius of curvature of bubble nose which leads to formation of surface waves on the
interface of Taylor bubble. Film disintegrates into multiple micro droplets due to the
presence of surface tension gradient.
• Near the end of de-encapsulation stage, a high pressure zone is created below the Taylor
bubble. Due to the retraction of ruptured film, formation of water column below the
bubble is noticed. Closed wake behind the bubble in heavier fluid (PDMS) helps the
entrained column to grow further. After reaching a maximum height, the column starts
to retract and merge back to the water bulk in the de-entrainment stage.
• Simulations for different fluid combinations to study the effect of fluid combinations
showed splitting of the Taylor bubble with little entrainment and unified bypass with
entrainment.
• Entrained volume is found to decrease with an increase in size of the bubble and
decreasing viscosity ratio. Presence of trailing bubble decreased the entrained volume by
40 % .

4.2. Boiling of an impacting droplet on liquid contact

• In the second part of dissertation, boiling of a methanol droplet on a mustard oil substrate
has been experimentally investigated by varying temperature from boiling point to
critical point to understand rapid phase transition and corresponding interfacial
characteristics.
• Based on the Weber number of the droplet and nondimensionalized average temperature
of the substrate, five different regimes (droplet protrusion, droplet pinch-off, droplet
splatter, droplet rebound, and cavity crater explosion) have been identified and a regime
map has been proposed (Fig. 4.2 (a)).
• Cavity crater explosion regime has been observed for high weber number (𝑊𝑒 70 −
80). At high We, droplet showed higher inertial force to penetrate the thin film of oil and
establish direct contact with base plate leading to rapid phase transition. Similar
phenomenon is also observed at very high temperature (𝑇𝑎𝑣𝑔 /𝑇𝐶 > 1) and low viscosity
(𝜇𝑜𝑖𝑙 /𝜇𝑑𝑟𝑜𝑝 < 0 055) of the substrate.

200
1000
180
Droplet potrusion Droplet pinch-off Droplet rebound Microbubble nucleation
900 Bubble burusting
Cavity explosion Droplet splatter
160
Shooting jets
800
140 Liedenfrost
2 4 5 700 We = 13.79
120
We = 41.37
600
We

100 We = 68.95
Rebound limit

Re
80 500

60 400
1
40 300

20 3 200
0 100
0.6 0.65 0.7 0.75 0.8 0.85 0.9 0.95 1 1.05 1.1 1.15 1.2
Tavg / Tc 0
0 0.05 0.1 0.15 0.2 0.25 0.3 0.35 0.4
Ja

(a) (b)
Fig. 4.2 (a) Phenomenological regime map based on weber number and nondimensionalized
average film temperature. (b) Prediction of rebound limit of the droplet based on oil film
Reynolds number and Jacob number.

• Effect of droplet size and impact height on droplet dynamics at Leidenfrost point of the
droplet was also investigated and a critical Weber number has been identified below
which bubble bursting has been observed.
• Correlations have also been proposed to predict the oil film Reynolds number to
understand the interfacial dynamics and the boiling characteristics (Fig. 4.2 (b)).

4.3. Boiling of a sheet/film of liquid nitrogen (LN2) on water

• In this part of the dissertation, boiling of LN2 sheet for different water temperatures, and
salinity, and liquid contacts (water, kerosene, methanol and toluene) has been
experimentally investigated.
• LN2 sheet boiling over water surface produces ice for lower base fluid temperatures. No
such behavior is observed at higher temperatures. Presence of salinity in the base fluid
delays the evaporation rate.
1.2
Projected area, Ap (mm2) 5000.00
C 1

(Wo - W) / (Wo)
4000.00
0.8
B
3000.00
A 0.6
2000.00 Water Toluene
0.4
1000.00 −
0.2 Kerosene Methanol

0.00 0
10.00 15.00 20.00 25.00 30.00 35.00 40.00 45.00 0 10 20 30 40 50 60
Equivalent diameter, deq (mm) Time, t (s)

(a) (b)
Fig. 4.3 (a) Bubbling regimes (A, B or C) during boiling of LN2 sheet of different volume
over water surface. (b) Boil-off rate of LN2 film on different base fluids .

• Different amount of LN2 is poured over the water surface and the length of the sheet is
calculated using image analysis, which is then compared with the critical wavelength
required for film boiling and three different regimes are identified (Fig. 4.3 (a)) i.e. no
bubbling (A) (bubble levitates over the water surface), moderate bubbling (B) and
vigorous bubbling (C).
• For no bubbling regime, where LN2 levitates over the water surface, vapor flux generated
from the water/LN2 interface balances the weight of LN2 sheet.
• Vapor cloud generated during LN2 boiling over the water surface has been quantified
with the help of single point source-detector technique coupled with the array of the
thermocouples.
• In order to understand the effect of thermophysical properties of the base fluid on the
evaporation rate of LN2, boiling of LN2 film on four different base fluids ( methane,
water, toluene and kerosene) was investigated. It was found from the study that lower
density fluids has higher evaporation rate (Fig. 4.3(b)).

4.4. Multi-mode boiling of LN2 film over solid and liquid contacts

• In the last part of dissertation, boiling of LN2 film on solid contact and liquid contact
have been investigated through numerical simulation. In the case of boiling on a solid
surface, bubble frequency, bubble diameter and heat flux increases linearly with the
increase in wall superheat.
0.15 0.0251495
0.025149
t = 0.0325 s

Volume (mm3)
0.0251485

0.125 0.025148

Before 0.0251475
0.025147
vapor film

Volume (mm3 )
0.0251465
0.1 collapse 0.025146
0 0.01 0.02 0.03 0.04
Flow time (s)

0.075 After
vapor film
0.05 collapse

0.025 00
0
0 0.025 0.05 0.075 0.1 0.125 0.15
Flow time (s)

(a) (b)
Fig. 4.4 (a) Asymmetry in bubble growth and the departure of 2nd batch of vapor bubbles.
(b) Change of vapor generation rate before and after the vapor film collapse.

• At a very high wall superheat, departure of vapor bubbles is governed by inviscid Taylor-
Helmholtz instability during boiling of LN2 on solid surface in multi-mode. Moreover,
after the departure of first generation of vapor bubbles, localized vortices causes
asymmetry in bubble growth and departure of second generation of vapor bubbles (Fig.
4.4 (a)).
• Boiling of LN2 film over a liquid contact (water) has also been investigated in the
subsequent study. In case of boiling on a liquid contact, presence of a vapor film, absence
of sufficient heat flux and dominance of thermocapillary force over vapor thrust causes
film thickness to reduce over time and collapse after some time. Rate of thinning of vapor
film thickness is found to be slower as compared to the inviscid theory of liquid/gas
pinch-off. Collapse of vapor film leads to sharp jump in the evaporation rate (Fig. 4.4
(b)). l

5. Organization and objectives of the thesis

The thesis is organized as follows:

In the first chapter of the thesis, a comprehensive introduction of entrainment due to motion of
a third phase and nucleation at a liquid-liquid interface is provided. Related literature are cited
to explain the present status of knowledge and highlight the gaps. To bridge the gap, efforts
have been made to study some of these issues which are reported in subsequent chapters. In
chapter 2, results of numerical simulation studying entrainment at liquid-liquid interface is
discussed. Boiling of a droplet over liquid film and liquid-liquid film boiling are also tried
experimentally. Observations of these experiments are reported in chapter 3. Efforts towards
numerical simulation of boiling of cryogen at solid and liquid surface is presented in chapter
4. Finally, some important conclusions and scope of future works are listed in chapter 5.

6. List of publications from dissertation work

1. Kumar, R., & Das, A. K. (2023). Entrainment dynamics of a Taylor bubble crossing
stratified liquid–liquid interface. Chemical Engineering Science, 269, 118463.
https://doi.org/10.1016/J.CES.2023.118463.
2. Kumar, R., & Das, A. K. (2022). Numerical study of boiling of liquid nitrogen at solid
and liquid contact planes. International Journal of Heat and Mass Transfer, 183,
122075. https://doi.org/10.1016//j.ijheatmasstransfer.2021.122075.
3. Kumar, R., Lokesh, & Das, A. K. (2022). Fluidics of an immiscible drop impact onto
a hot oil film. Physics of Fluids, 34(1), 1–29. https://doi.org/10.1063/5.0077605.
4. Kumar, R., Rohilla, L., & Das, A. K. (2021). Understanding interfacial behaviour
during boiling of nitrogen from liquid-liquid contact plane. International Journal of
Heat and Mass Transfer, 165, 120661.
https://doi.org/10.1016/j.ijheatmasstransfer.2020.120661.
5. Kumar, R., Rohilla, L., & Das, A. K. (2020). Passage of a Taylor Bubble through a
Stratified Liquid-Liquid Interface. Industrial and Engineering Chemistry Research,
59(9), 3757–3771. https://doi.org/10.1021/acs.iecr.9b04235.

Reference:

• Apfel, R. E. (1972). Water Superheated to 279.5° C at Atmospheric Pressure. Nature


Physical Science 1972 238:82, 238(82), 63–64. https://doi.org/10.1038/physci238063a0
• Bonhomme, R., Magnaudet, J., Duval, F., & Piar, B. (2012). Inertial dynamics of air
bubbles crossing a horizontal fluid-fluid interface. Journal of Fluid Mechanics, 707,
405–443. https://doi.org/10.1017/jfm.2012.288
• Dietrich, N., Poncin, S., Pheulpin, S., & Li, H. Z. (2008). Passage of a bubble through a
liquid-liquid interface. AIChE Journal, 54(3), 594–600.
https://doi.org/10.1002/AIC.11399
• Dincer, A. K., Drake, E. M., & Reid, R. C. (1977). Boiling of liquid nitrogen and methane
on water. The effect of initial water temperature. International Journal of Heat and Mass
Transfer, 20(2), 176–177. https://doi.org/10.1016/0017-9310(77)90011-4
• Drake, E. M., Jeje, A. A., & Reid, R. C. (1975a). Transient boiling of liquefied cryogens
on a water surface. II. Light hydrocarbon mixtures. International Journal of Heat and
Mass Transfer, 18(12), 1369–1375. https://doi.org/10.1016/0017-9310(75)90250-1
• Drake, E. M., Jeje, A. A., & Reid, R. C. (1975b). Transient Boiling of Liquefied on a
Water Surface Cryogens i. Nitrogen, Methane and Ethane. Ht. J. Hear Moss Transfer,
18, 1361–1368.
• Emery, T. S., Raghupathi, P. A., & Kandlikar, S. G. (2018). Flow Regimes and Transition
Criteria during Passage of Bubbles through a Liquid-Liquid Interface. Langmuir, 34(23),
6766–6776. https://doi.org/10.1021/acs.langmuir.8b01217
• Enger, T; Hartman, D. E. (1971). LNG spillage on water. I. Exploratory research on
rapid phase transformation.
• Gordon, K. F., Singh, T., & Weissman, E. Y. (1961). Boiling heat transfer between
immiscible liquids. International Journal of Heat and Mass Transfer, 3(2), 90–93.
https://doi.org/10.1016/0017-9310(61)90071-0
• Henry, R. E., Quinn, D. J., & Spleha, E. A. (1974). An experimental study of the
minimum film boiling point for liquid-liquid systems. International Heat Transfer
Conference 5, 101–104. https://doi.org/10.1615/IHTC5.280
• Kar, A. (2017). Experimental Studies on Entrainment At Liquid-Liquid Interface Due To
the. July.
• Kemiha, M., Olmos, E., Fei, W., Poncin, S., & Li, H. Z. (2007). Passage of a gas bubble
through a liquid-liquid interface. Industrial and Engineering Chemistry Research,
46(19), 6099–6104. https://doi.org/10.1021/IE061549V
• Novaković, M., & Stefanović, M. (1964). Boiling from a mercury surface. International
Journal of Heat and Mass Transfer, 7(7), 801–807. https://doi.org/10.1016/0017-
9310(64)90008-0
• Uemura, T., Ueda, Y., & Iguchi, M. (2010). Ripples on a rising bubble through an
immiscible two-liquid interface generate numerous micro droplets. EPL, 92(3).
https://doi.org/10.1209/0295-5075/92/34004

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