Professional Documents
Culture Documents
org/cgi/content/full/4/8/eaat3276/DC1
Birgitt Boschitsch Stogin, Luke Gockowski, Hannah Feldstein, Houston Claure, Jing Wang, Tak-Sing Wong*
(available at advances.sciencemag.org/cgi/content/full/4/8/eaat3276/DC1)
Movie S7. Self-cleaning of liquid membranes. Our experimental setup involves a tilted
liquid membrane where contaminates (here, small sand particles) are passively removed
from the separation region by gravity, allowing the large particle to be collected. The
small particles are collected in the accumulation region and removed from the membrane
when the weight of the aggregate exceeds the capillary force exerted by the liquid
membrane (“aggregate removal”). Particles used here were sand (small particles) and
glass (large particles).
Fig. S1. A schematic diagram showing a bead passing through a liquid membrane.
Several variables used throughout our discussion are shown.
As the bead passes through the membrane, the membrane stretches, increasing the surface
energy. As this occurs, the bead-film contact line may slide along the bead surface, thus
changing the boundary conditions of the membrane over time. We anticipate that this
contact line motion is a function of the dynamics and geometry of the system, as well as
the advancing contact angle of the membrane on the bead surface. In an effort to make a
rough estimate of the maximum membrane stretching and thus the maximum change in
surface area of the membrane, we simplify our system by assuming that the membrane-
bead contact line remains fixed to the equator of the bead. Since the bead is traveling at
relatively low speeds and existing work (13) has shown that beads impacting films at low
Weber number (𝑊𝑒) generate catenoid surfaces (i.e., minimal surfaces), we assume that
in all of our experiments the membrane is approximately a minimal surface at each
moment in time as it stretches. Since a minimal surface has a mean curvature 𝜅 of zero
everywhere on the surface, the pressure difference Δ𝑝 across the membrane interfaces
should be approximately zero (based on the Young-Laplace equation, Δ𝑝 = 2𝛾𝜅) so we
ignore energy losses due to drag arising from film movement. The minimal surface
formed by two concentric circular boundaries is a catenoid, a surface that can be
represented as the surface of rotation (about the y-axis) of the following equation
𝑦 (S1)
𝑥 = 𝑎 cosh (𝑎)
where 𝑎 is a constant.
Since we assume (1) that the film remains attached to the bead at the equator and (2) the
membrane is a catenoid (with boundaries at the ring and at the bead equator), we
approximate the maximum film stretch area to be the area of the catenoid formed when
the liquid membrane is tangent to the equator of the bead at the bead-film contact line.
Any further stretching would mathematically allow membrane-bead intersection, which is
non-physical. The boundary conditions associated with these assumptions are
𝑥(𝑦max ) = 𝑅𝑓
𝑥(𝑦 = 0) = 𝑅𝑏
𝑑𝑥
| = 0
𝑑𝑦 𝑦=0
where 𝑅𝑓 is the film radius, 𝑅𝑏 is the bead radius, and 𝑦max is the vertical distance
between the film and the bead center associated with the maximum membrane stretch
area.
Solving equation S1 using the above boundary conditions, the catenary associated with
our maximal stretching conditions is
𝑦
𝑥 = 𝑅𝑏 cosh (𝑅 ) (S2)
𝑏
𝑅
𝑦max = 𝑅𝑏 cosh−1 (𝑅𝑓 ) (S3)
𝑏
The surface of revolution about the y-axis of this shape (i.e., a catenoid) has an area
𝐴cat (which accounts for the two sides of the film) given by
𝑅
where 𝜙 = 2 cosh−1 (𝑅𝑓 )
𝑏
We consider the maximum change in surface energy to be the difference between the
surface energy of a film with area 𝐴cat and that of the flat annular film (inner radius 𝑅𝑏 ,
outer radius 𝑅𝑓 ) at bead impact. The maximum surface energy change is thus given by
𝐸𝑠 = 𝜋𝛾𝑅𝑏2 [sinh 𝜙 + 𝜙] − 2𝜋𝛾(𝑅𝑓2 – 𝑅𝑏2 ) (S5)
As the liquid membrane contact line slides along the surface of the bead, energy may be
lost due to friction. This energy can be captured by the pinning energy. The pinning force
is given by Furmidge (27)
𝐹𝑃 = 2𝛾𝜋𝑅(𝛼)(cos𝜃𝑅 − cos𝜃𝐴 )
where 𝑅(𝛼) = 𝑅𝑏 sin𝛼 and 2𝜋𝑅(𝛼) is the perimeter of the film-bead contact line when
the contact line is at an angle 𝛼 from vertical (fig. S1). Since work is force multiplied by
distance, we can calculate the energy dissipated as the film moves from different values
of 𝛼 as follows
𝛼2
𝐸𝑃 = ∫ 2𝛾𝜋𝑅𝑏2 sin𝛼 ⋅ (cos 𝜃𝑅 − cos 𝜃𝐴 )𝑑𝛼
𝛼1
While the initial liquid membrane motion may be more of a wrapping than sliding
motion, we assume a sliding motion from 𝛼1 = 0 to 𝛼2 = 𝜋 (possibly leading to an
overestimate of 𝐸𝑃 ), leading to
4 (S7)
𝐸𝑢𝑏 = 𝜌𝑏 𝑔𝐻 ( 𝜋𝑅𝑏3 )
3
where 𝜌𝑏 is the bead density, 𝑔 is the magnitude of the acceleration due to gravity, and
𝐻 is the height above the membrane from which the bead was dropped, assuming all
potential energy is converted to kinetic energy. According to Equations S5, S6, and S7
and our experimental conditions, 𝐸𝑃 /𝐸𝑢𝑏 << 1 but 𝐸𝑠 is comparable to 𝐸𝑢𝑏 (fig. S2).
We thus conclude that, for our experiments, 𝐸𝑃 is negligible and define 𝐸 ∗ as
𝐸 (S8)
𝐸∗ = 𝐸 𝑠
𝑢𝑏
Fig. S2. Comparison of the relative magnitude of different energy terms. The relative
magnitude of different energy terms (𝐸𝑆 and 𝐸𝑃 ) compared to the kinetic energy (𝐸𝑢𝑏 ) at
bead impact with the liquid membrane for (A) glass, (B) polytetrafluoroethylene (PTFE),
and (C) polystyrene (PS) beads.
Fig. S3. Theoretical dependence of E* on relevant parameters. Here we plot ln𝐸 ∗
analytically, assuming we are dropping a glass bead (𝜌𝑏 = 2500 kg/m3) into the
membrane from height 𝐻. The plots on the right panels show a zoomed-in region of the
plots on the left panels for 0.01< 𝑅𝑏 /𝑅𝑓 < 0.1. (A, B) Influence of 𝑅𝑓 on 𝐸 ∗ : ln𝐸 ∗ as a
function of 𝑅𝑏 /𝑅𝑓 at a fixed drop height 𝐻 and surface tension 𝛾. The inset in (A) shows
a dimensional x-axis for clarity. Here we see that increasing 𝑅𝑓 should lead to an increase
in 𝑅𝑏,cr (the maximum value of 𝑅𝑏 where bead retention will occur) when all other
parameters are held constant. (C, D) Influence of 𝛾 on 𝐸 ∗ : ln𝐸 ∗ as a function of 𝑅𝑏 /𝑅𝑓 at
fixed 𝑅𝑓 and 𝐻 for different 𝛾. Here we see that increasing 𝛾 leads to an increase in 𝑅𝑏,cr
when all other parameters are held constant. (E, F) Influence of 𝐻 on 𝐸 ∗ : ln𝐸 ∗ as a
function of 𝑅𝑏 /𝑅𝑓 with a fixed 𝑅𝑓 and 𝛾 for different 𝐻. Here we see that an increase in
𝐻 leads to a decrease in 𝑅𝑏,cr when all other parameters are held constant. These
relationships only hold if the weight of the bead does not exceed the capillary force
acting on the bead.
Ring Radius (cm) [SDS] (M) Film Mass (mg) Thickness (μm)
Table S4. Advancing angles of liquid membrane solution droplets on a flat surface.
All advancing angle measurements for polytetrafluoroethylene (PTFE) and polystyrene
(PS) were taken using a drop volume addition and subtraction method. The advancing
angles of water and 10.6 mM SDS solution on glass were measured to be < 10∘ .
θA(o)