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William P. Johnson
Professor
Geology & Geophysics
Civil & Environmental Engineering (adjunct)
University of Utah
Complexity of particle filtration in porous media requires many
kinetic parameters, mechanistic basis needed for robust prediction
THE
UNIVERSITY
Particle filtration in porous media involves limited diffusion, and so OF UTAH
is partly deterministic, allowing prediction of attachment rates
From:
Susa Stonedahl
St. Ambrose U.
http://susa.stonedahl.com/research.html
Washington County Fair,
New York, September 1999
Diameter (m)
10-10 10-9 10-8 10-7 10-6 10-5 10-4 10-3 10-2
1A 1 um 1 mm
molecules
colloids
suspended particles
0.5
0.4 Filtration
0.3 C C 2C
= v +D kfC
0.2 t x x 2
C kf
= exp( L)
0.1 Co v
0.0
0.0 0.5 1.0 1.5 2.0 2.5 3.0 3.5 4.0 4.5 5.0
Pore Volumes
DLVO theory: Unfavorable conditions (repulsion)
Born repulsion
Sep. dist. = 200 nm
Increased ioniclayer
strength
Repulsive
Electric double repulsion
+ + Repulsive
+ Barrier Secondary
Force
Sep. dist. minimum
+ +
+ = 50 nm 1 50 200
+
Attractive
+ Separation distance (nm)
Primary
minimum
Van der waals attraction
Sep. dist.
< 0.2 nm
Column experiments breakthrough-elution behavior
and distribution of retained colloids
Breakthrough-elution behavior
= + +
+
C=C0
Unfavorable
C
(at L)
Favorable
= +
Ln Csed
More
Unfavorable
sticky
Less sticky = big challenge for
design and protection
Favorable
1.1 m microspheres
1.0E+09
# of Retained Microspheres
1.0E+08
1.0E+07
0.00 0.10 0.20
Up-gradient Down-gradient Low Co
Same as Meters
Down-
gradient
Simulation
translationz = u zt t
Newtons
Place the 2nd
Numerical
Change + law
particle
approximationold = new
mmp p
z
t z
Favorable conditions, 10 m colloids
The key is the forward flow stagnation zone
Strategy:
Force/torque balance
Which particles intercept surface?
Variables:
Many starting locations upstream
Different colloid sizes
Different fluid velocities
Result:
Key = forward flow stagnation zone
Diffusion and settling help
Collector efficiency () =
stream lines # intercept / # introduced
Upscaling porous media as a series of collectors
C0
1
1 1 =
0
C1
2
2 1 = = 1
1 0
C2
3 1 2 3
3 1 = = = 1
2 0 0 0 1 2 1
C3
= From ADE
0
Cn-1
Nc 1 = = 1
1
Cn
Gives kf as a function of velocity
( and kf remain constant across distance)
Agreement between theory (blue) and experiment (black)
High
diffusion
High
settling
Repulsive
1 10 20
Attractive
1.00E-04
1.00E-05
separation
minimum
1.00E-07
Repulsive
1.00E-08 = Barrier
Primary
sticks/strikes = chemistry
minimum
= near surface transport
intercept/introduced = physics = bulk transport
1.00E-09
Force
0.00E+00 1.00E-04 2.00E-04 3.00E-04 4.00E-04
Attractive Repulsive 5.00E-04
r(m) (meters) Semi-empirical only!
Transport distance
No detachment either!
But the surface isnt all repulsive!
There are nanoscale zones of attraction
1 10 20
Separation dist (nm)
P
Z
dA
nA
D
h
e1
nS
dS
e0
Unfavorable: 33% coverage; 350 nm heterodomains; 10 m colloids
Quantifying Heterodomains impinging jet
Radial Higher ionic
stagnation strength =
point flow deeper
(impinging jet) secondary
energy
TIRF minimum
Total internal
reflection Low ionic
fluorescence strength =
shallow
Particles secondary
(2-m) energy
fluoresce minimum
when within
~150 nm of
surface
Johnson and Tong,
2006, ES&T 40(16),
5015-5021
1.2e-5
Different sizes
different diffusion 8.0e-6
behavior
Y (m)
4.0e-6
1.95 m
1.0e-6
Cross-sectional view
H (m)
surface at H = 0
1.0e-7
1.0e-8
-4.0e-6 0.0 4.0e-6 8.0e-6 1.2e-5
X (m)
1.5E-09 Net interaction depends on heterodomain size
versus zone of interaction (ZOI)
1.0E-09
F (N) 5.0E-10
-1x10-7 m
-1x10-8 m
-1x10-9 m
-1x10-6 m Mechanistic simulations in impinging jet geometry - movie
-1x10-7 m
-1x10-8 m
-1x10-9 m
Hetero-domains:
120 nm radius
% coverage
changes with:
a) Mineral
b) pH
Pazmino et
al, 2014,
Langmuir,
30(19),
54125421
Trauscht et
al, 2015,
Langmuir,
31 (34),
93669378
1.0E+00 a MSRlog= 0.98 1.0E+00
Silica b
Muscovite
1.0E-01 Albite 1.0E-01
Elimelech
Maxwell
1.0E-02 1.0E-02
MSRlog= 0.80
1.0E-03 1.0E-03
1.0E-03
1.0E+00 1.0E-02 1.0E-01 1.0E+00 1.0E-03
1.0E+00 1.0E-02 1.0E-01 1.0E+00
c Experimental d Experimental
Discrete Hetergneity
modified Ncol
1.0E-01 1.0E-01
1.0E-02 1.0E-02
1.0E-03 1.0E-03
1.0E-03 1.0E-02 1.0E-01 1.0E+00 1.0E-03 1.0E-02 1.0E-01 1.0E+00
Experimental Experimental
1.00
Muscovite
= 0.52(% )0.56 p
Coeficient of Ncol optimized eq.
Trauscht et
al, 2015,
0.10 Langmuir,
31 (34),
Silica 93669378
Albite
132
=
0 1
0.01
0.001 0.01 0.1 1
Surface Coverage (%)
Pazmino et
al, 2014,
Environ. Sci.
Technol.,
48(16),
92279235
Experiment IS at 0 seconds Simulation IS at 15 seconds
1.00E-03
1.00E-03 v = 2 m/day
v = 2 m/day
1.00E-04
1.00E-04
1.00E-05 1.00E-05
Fav Sim
1.00E-06 Fav 0.2 nm RMS Fav Sim
1.00E-06
Fav 38 nm RMS Fav 38 nm RMS
Unf 0.2 nm RMS Unfav 38 nm RMS
Unfav 38 nm RMS Fav 546 nm RMS
1.00E-07 1.00E-07
Unfav 546 nm RMS
1.00E-08 1.00E-08
1.00E-03
v = 8 m/day v = 8 m/day
1.00E-04
1.00E-05
1.00E-08
0.01 0.1 1 10 0.01 0.1 1 10
Colloid Diameter (m) Colloid Diameter (m)
Blocking emerges organically from limited parking spots?
= + +
C=C0
C
(at L)
C=0
Time
1.5E-09 Slight differences in colloids emerge as
large differences in stickiness?
1.0E-09
Less
sticky More
sticky
More
F (N) 5.0E-10
sticky
Ln Csed