ASPECTS OF LIQUID AND VAPOR FLOW IN RETORTED OTT. SHAT.F.

                                     by                       '

                   Glenn 0. Brown and David B.  McWhorter      :
                   Agricultural and Chemical Engineering
                         Colorado State University
                        Fort Collins, Colorado 80523          '
             Presented at the 1986 Eastern Oil Shale Symposium,
                            Lexington,  Kentucky
                            November 19-21,  1986
                                   Notice
        The development of the information in this  document has been funded
wholly or in part by the United States Environmental  Protection Agency under
Cooperative Agreement CR812225 to Colorado State University.  It  has been
subject  to the Agency's peer  and administrative  review,  arid  it  has been
approved for publication.                                     j

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                           ASPECTS OF LIQUID AND VAPOR FLOW IN RETORTED  OIL SHALE

                                                     by

                                    Glenn 0. Brown and David B.  McWhorter
                                    Agricultural and Chemical Engineering
                                          Colorado State University
                                        Fort Collins,  Colorado 80523
                                                  Abstract                             '

                      Reclamation  and impact analysis  of retorted oil  shale piles will!
                      require  prediction  of water and solute  transport  rates over  the
                      entire  water  content range down to  and  including  the relatively
                      dry   region.     Experimental  measurements   of   water  transport
                      coefficients   in  relatively  dry oil shales have brought  forward
                      long-standing  questions  concerning   the mechanics  of combined
                      liquid/vapor  flow.   In an attempt to  ensure  proper  interpretation1
                      of experimental data,  a new analytical solution has been obtained
                      for  combined  liquid  and vapor  flow with solute transport.   The
                      solution  shows  that  the  relative   magnitudes  of  the separate
                      transport coefficients produce . many  of the  flow,  features  seen in
                      experimental   data,  and significant liquid transport  can occur in
                      regions  without  apparent solute transport.  This  development is
                      new and represents a significant  addition to understanding solute
                      transport.    As  such  its  methods and results can be applied to
                      other  problems in multiple phase transport  and to  materials such
                      as  high  volume  mining wastes and some  hazardous  waste disposal
                      sites.   The paper shows that an earlier conclusion  reached by  the
                      authors,   that  a  critical  water content exists in  retorted  oil!
                      shale below which solute transport ceases, is unjustified.
                   Introduction

     Research  into  the  movement  of  water  and
dissolved  constituents  in retorted oil shale has
been  motivated by the adverse impacts that can be
anticipated  if  leachate  is  generated  and left
uncontrolled  in the large disposal piles planned.
Accurate  prediction  of water and solute movement
through  disposal  piles will require measurements
of both water and solute transport over the entire
range  of solution contents, down to and including
the  relatively  dry region.  Dry region transport
phenomena are  of concern for two reasons.  First,
retorting produces a shale that is oven dried, and
it  is  expected that only enough water to control
dust  and  aid  compaction  will  be  added before
placement, and much of that may rapidly be lost to
evaporation.   Thus,  the  pile  initial condition
before infiltration of precipitation will probably
be  relatively  dry,  and leaching may be strongly
influenced by transport processes near the initial
condition.   Second,  an  earlier  study by Colder
Associates1 has proposed that piles be designed to
eliminate  pile leachate by evaporating all excess
infiltration.   Such  evaporation  would of course
require   the   portion   of  the  pile  near  the
evaporating interface to remain quite dry.
     In  a  previous  study ;by the authors2'3 the
hydraulic  and solute transport characteristics of
Lurgi   retorted  oil  shale;  were  measured  from'
saturation  (0.49  cm3/cm3) ; down  to  almost zero.
solution content.  These measurements were carried
out  by use of a dual source; gamma ray system4'5'8
which can simultaneously measure water content and
solute   concentrations   during  column  sorption
experiments.   The experiments showed, as expected
from  earlier studies7'8'8'1*"11, that water vapor
diffusion  becomes  the  dominant  water transport
mechanism in the retorted material at low solution
contents.    Empirical  examination  of  the  data
indicated   that   the  liquid  water  and  solute
transport   ceased  at  0.066  cm3/cm3  volumetric
solution  content and that all water transport was
by vapor diffusion.         :

     As  soon  as  these  results  were  obtained,
questions  arose  as  to  the accuracy of the data
Interpretation.    More   specifically,   it   was
questioned  if the solute transport observed was a
function  more  of  the  test  conditions,   and if
liquid  transport  actually  ceased  at  a  finite
solution  content.   Examination of the literature
showed  that  a  considerable  number of questions
remained   about   the  interactions  of  combined

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liquid/vapor  flow12'13'1*  and unexplained solute
transport  phenomena  which  occur  near low water
contentsl*.

      '.[n an attempt to ensure proper interpretation
of  the  experiment data  a theoretical model of two-
phase  water  and solute transport in a pore was
developed.   The  model  allows analytical numerical
solutions  to   the  unsteady sorption of solution.
The  model solutions   are able to produce many of
the  flow  features seen in the experimental data.
From the  results  it   can  be concluded that the
relative   magnitude  of  the  separate  liquid and
vapor  transport  coefficients  produce the solute
profiles   seen,   and    that  significant  liquid
transport  can  occur in a region without apparent
solute  transport.

              Phenomena of Interest

      In this   paper  two experimentally observed
phenomena  will be examined.  These phenomena have
been either unexplained or explained by thresholds
of    transport    processes  which  have  not  been
rigorously proven to exist.

Critical Water  Content

      Several    experimenters   have   observed  or
speculated on  the existence of a "critical" water
content below  which   liquid conduction of solute
ceases.    From  sorption or solute diffusion in dry
media,  Grismer  et al.6,  McWhorter and Brown2'3,
Rose1",  and  Porter  et al.ls speculated that the
.liquid  phase   becomes   discontinuous at low water
contents.    From  sorption   at   high  solution
concents,  Krupp  et  al.16,  Laryea et al.17, and
Robin  et  al.18   postulated  the  existence  of an
immobile   layer  of  water near the solid surface,
while  Van   Schaik    and  Kemper19,  Smiles  and
Gardiner20,  and  Bond   et  al.21  concluded  that
significant     anion     exclusion   effects   were
occurring.

      Most  of   the above  conclusions were based on
unsteady   infiltration  of   solution.   Typical
results  of  such  an   experiment  are  taken from
McWhorter  and Brown2 and are shown in Fig.  1.   In
this  experiment  Nal solution was injected into a
completely  dry column.   Water and l" were tracked
by  dual  source  gamma   ray.    After  significant
inflow   the  water  was  observed  to  develop  a
gradually  varying  profile,   but  the  solute was
restricted    to   water   contents   above   0.06
(cm3/cm3).

Solute  Concentration Humps

      Smiles et  al.1* observed, as shown in Fig. 2.
that,   on  infiltrating  soil  with  a low initial
solution  content,  there  was not perfect piston-
like  displacement of the resident fluid, as would
be  expected.   A  small  increase  or hump in the
resident  solute concentration was formed ahead of
the   wetting  front where the solute concentration
was   increased above the  initial.  This hump could
not   be  explained,  as   no  single  convectlve or
dispersive  process  can  explain  an  increase in
solute  concentration   in  a  region of increasing
solution  content.   The  same hump can be seen in
the   data   but  was   not  noted  by  Smiles  and
Phillip22.

      Likewise   McWhorter  and  Brown2'3  observed
large    Increases    in   the   invading   solute
concentration  behind  the  wetting  front:.   They
attributed the hump to evaporation.

     The  theoretical  model;, which is detailed in
the Appendix, will be applied to determine if these'
two  phenome a  can  be explained by the two-phase
transport  processes  without the aid of transport,
thresholds such as a critical water content.      :

                Method of Analysis

     The  phenomena  of interest will be explained
by  appeal to a theoretical solution of liquid and
vapor flow with solute transport in a porous media
of  known  hydraulic  properties.   To  obtain the
theoretical  solution  new  equations of water and!
solute   transport   have   been  developed.   The
derivation   of   these   transport  equations  is,
secondary   to   the   purpqse   of '  this  paper.
Therefore,  only the assumptions and final resultsL
will  be  presented here, while a brief derivation
is presented in the Appendix.

Model Assumptions
                            i
     The  developed  model assumes one-dimensional
horizontal  adsorption  of  !liquid  solute  into a
nearly  dry column of porous media as typical with
most  laboratory  experiments  of  interest  here.'
Solution  is transported by gradients of hydraulic
pressure,   but  it  is  assumed  that  the  water
characteristic  can  be  used to transform Darcy's
conductivity  to  a  diffusivity  where the liquid
flow is driven by gradients .of water content.  The
vapor  transport  is assumed to be driven by vapor
diffusion  but  again it is ^assumed that the vapor
adsorption  isotherm  can be used to transform the
driving  gradient  to  the  [liquid  water content.
These   well   established  ! transformations   are
routinely  used  by  investigators  in this field.
The  liquid  and vapor phases are assumed to be in
instantaneous   local   equilibrium;   i.e.,  where.
kinetic  effects  of  evaporation and condensation
are negligible.              '                      ;

     Solutes  are  present  in  both  the  initial
solution   and   the  invading  solution,   but  at
different  concentrations.   ; Solute is transported
only  in  the  liquid  phase.   The  solute is not
adsorbed  by  the  solid  phase and moves with the
mean  velocity  of  the  liquid  phase.   This last
assumption  implies  miscible  displacement; i.e.
the  initial  and  invading - solutes  are mixed by
only small-scale dispersive processes.
 column   has  a  uniform,   low  initial
content.   At  thd  start and during the
     The
solution
remainder  of  the  adsorption the column inlet is
maintained  at  a  constant ^solution content.  The
invading   solution   enters  the  column  with  a
constant   concentration.   , This  is  a  slightly
different  boundary  condition  than  used in some
experiments . 2 ' s

Diffustvtties               ,                      '

     Using   the   concept  of  liquid  and  vapor
diffusivities  it  can  be  istated  that the  total
water flux expressed as liquid volume is

                                          or  (la)
         - ' V<>

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 o
U
                                                   X (cm)
               Figure  1.   Solution Content  (9) and Relative Invading Solute Concentration

                          (C/CQ) Versus Column Position (x),  After Various Times.  These

                          Results Are  from  an Unsteady, Constant-Flux Experiment Performed
                          by McWhorter and  Brown2                                    ,

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i
                                                           i—i—i—i—i—i
                                                 i—i—i—i—i—i—i—i—i
                     0.2      0.4      0.6      0.8       1       1.2      1.4      1.6      1.8
                                            x/f
            Figure 2.  Solution Content (0) and Relative Resident Solute Concentration
                       (c/cn) Versus Relative Column Position (x/t1/2).  These Results

                       Are From an Unsteady Constant Concentration Experiment Performed
                       by Smiles et al.1*  (Curves Are Best Fit to Reported Data)

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 where
8.
               - total   equivalent   liquid
                 volumetric flux,

       DVW   -  vapor diffusivity,

       C^     -  concentration  of    water   in
                 solution,

       dp^/dff  -  slope  of   vapor   adsorption
                 isotherm,

       D^(0)   -  liquid diffusivity,

       t>       —  solution content,
       Dt(*)   -  total water diffusivity, and

       x       -  horizontal position.

 As  noted both  D,   and  D   are functions  of
With Eq. (la)  it is clear tKat the total water
                                                           Note that the vapor diffusivity is  greatest at the
                                                           lower   solution   contents,1   while    the  liquid
                                                           diffusivity    dominates   'as    solution   content
                                                           increases.   Nowhere  in   the  range of  interest is
                                                           either  transport  coefficient  zero.   The  total
                                                           diffusivity has the characteristic double maximum
                                                           of   most  porous  media.    these   functions  were
                                                           obtained  from   a  theoretical  model for a set of
                                                           plate  capillaries,   but  for this analysis any set
                                                           of  values   could  be used as  long  as they had the
                                                           same  general shape.  A different set of transport
                                                           coefficients   would  only  change  the  numerical
                                                           results,  not the general  conclusions.

                                                                From  the   Appendix,  the  general equation for
                                                           the  water flow  is           !
                                                                 A M
                                                                 2 dA
                                                          where
                                                                    A - x/t
               dA  '•"t  dA
                  1/2
                                               (2)
                       and
flow is the sum of the two components , bulk liquid
flow  and  vapor diffusion.  The fraction of water
transport in either phase at a particular position
is  simply  the  ratio of the phase diffusivity to
the total.

Assumed Diffusivities

     Values  of  the individual diffusivities must
be  assumed  to achieve a flow solution.  Figure 3
presents  the  assumed  values .  In the figure the
horizontal   axis   is   the  solution  volumetric
content,  6,  over  the  range of interest 0.02 to
0.10,  while the vertical axis is the diffusivity.

       0.0005
           t -  time  from start of sorption.

Equation  (2) is subject to   |

           ff(A-O) -  ff   ; a constant, and

           0(A«>) -  g   • a constant.
                                                                                                     (3)

                                                                                                     (4)
The  use  of  the transformed Boltzman coordinate,
A=x/t1/2    is   possible   due  to  the  boundary
conditions  used,  and  "normalizes" the solution.
That  is,  it allows the solution content profiles
from  different  times  to  be  collapsed onto one
another.   For  ease  of  reference,   A   can  "
             0.02
               Figure 3.   Assumed Values of Liquid (D^), Vapor (D ), and Total (D )

                          Diffusivities.  Note That Vapor Has a Maximum at Low Solution
                          Contents;  The Liquid, at High Solution Contents; and the Total,
                          a Minimum at an Intermediate Content

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thought  of  as a horizontal scale which stretches
uniformaly (like a rubber band) with time.

     The  evaporation  and  condensation along the
column can be determined by the relation:
              d MS}   A   d£_
             1  dfl      2 J dA  '                (:>)

where     e    -  the phase transfer, and

          A(0) -  transport function.

     The  transport  function  is calculated during
the  solution  procedure  and  is a function of the
diffusivities  and boundary conditions.  The phase
transfer variable  e  is positive for condensation
and negative for evaporation.

     The solute concentration  along  the column can
be   determined   by  solution of   the  following
differential equation:
                                                                    C      — inlet concentration of invading
                                                                             solute,  and
                                                                                      !

                                                                    C      -• initial   ;   concentration    of
                                                                             resident solute.

                                                               The  left-hand  side  of  Eq.   (6) represents
                                                          phase  transfer  and convective effects, while the
                                                          right-hand side represents  dispersion.
                                                                        Results and Discussion
CCA).
        [A(«> - f ]
subj ect  to :

          C(X-O)  - C

          C(A— )  - C
                        and
where
          C(A)   — solute concentration,
          D (0)  - coefficient
                   dispersion,
                                    of
,   (6)




   (7)

   (8)



solute
                                                          Flow Solution
     Figure 4 presents the solution of Eq.  (2)  for ,
solution  content  profiles i for  the  initial  and
boundary  conditions  given i -by  Eqs . (7 ) and ( 8 ) .
In  Fig.  4  the vertical ax:is is solution content!
and  the  horizontal axis the normalized distance,
x/t1/2.  As could be expected the solution content
falls  from  the  boundary  'condition at the inlet ,
(x/t1/2  -  0) , to the initial solution content at
about   x/t1/2   -   0.07.  'As  in  all  sorption
experiments where vapor transport plays a role, a,
"vapor nose" elongates the p'rofile.  This nose is,
due  to  the  secondary diffusivity naTimum at the
low  solution  contents  as Ishown in Fig. 3.  This
theoretical profile is similar and consistent with
experimentally observed profiles.

     Next, solving Eq. (5) for the evaporation and'
condensation  of  water  vapor  along  the  column
provides  the  data  plotted!  in Fig. 5.  ]in Fig. 5
the   vertical   axis   is  !the  normalized  phase
                                   0.02
                                                         0.04

                                             x/f'/2  (cm/s'/2)
                                                                                0.06
                                                                                                      0.08
                     Figure 4.   Calculated Solution Content ($) Versus Relative Position
                                (x/t1/2)

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        0.5

        0.4 -

        0.3 -

        0.2 -

        0.1 -
       -0.1 -
       -0.2 -
       -0.3 -
       -0.4 -
       -0.5
                                              T
                                                         T
                                  0.02
               0.04

A=  x/t'/2(cm/s'/2)
—I—
 0.06
                                                                                                    O.OB
                   Figure 5.   Calculated Evaporation and Condensation (e) Versus Relative
                              Position (x/t1'2)                                       |
 transfer,    e,  with   condensation  positive  and
 evaporation  negative.   Again the horizontal axis
 is   Che  normalized  distance   x/t1/2.  The point
 labeled A^, where e is zero at about 0.03 cm/s1'2,
 separates   the   regions   of   evaporation   and
 condensation.     In   consideration   of   solute
 transport  it  can  be stated that the evaporation
 behind   \^   will  tend  to  increase  the solute
 concentration, while the condensation ahead of the
 point  will  tend to reduce solute concentrations.
 The  maximum  evaporation  rate  occurs  at  about
 0.021 cm/s1'2,   while  the  maximum  condensation
 occurs at about 0.044 cm/s1'2.

     Finally, Eq. (6) must be solved to obtain the
 solute   concentration   along  the  column.    For
 illustrative  reasons  Eq. (6)  is solved assuming
 that the dispersive term on the right-hand side is
 zero.   This  allows the clear presentation of the
 convective  and  evaporation  effects  without the
blurring  caused by dispersion.   Figure 6 presents
 these results.  In Fig.  6 the vertical axis is the
normalized  solute  contents  C/C   and C/C .   The
 invad.ing solution has only advanced to a position.
labeled  A ,   of  about  0.018 cm/s1/2.    From the
 inlet  the  invading  solution concentration,  C/C
rises  from its injection value,  1, to a maximum o?
about  1.5  at A .   This increase in concentration
 is due to both evaporation and convective effects.

     Possibly   of   greater   interest   is    the
concentration  of the resident fluid,  C/C .  While
condensation  at  the  far end ahead of An dilutes
the  resident  solution,   as  could  be  expected,
convective  and  evaporative  effects   between  A
                 and   Ag   have the net effect of first increasing
                 the  concentration above 1 and then reducing it to
                 about  0.8.   If  dispersion  were  added,   these
                 concentration  profiles  would  be  blurred by the
                 smoothing  effect of the dispersion,  but the trend
                 would still be present.      I

                 Explanation of Phenomena of  Interest

                      We can  now explain the  two  phenomena of
                 interest.  First re-examine  Fig. 6.  Looking  only
                 at the invading solute concentration profile
                 (McUhorter and Brown2'3) it could be argued that a
                 "critical" water content occurred at position A
                 which (from the solution content profile,  Fig. H)
                 would be estimated to have a value of about 0.06.
                 Thus  it would be concluded that liquid diffusivity
                 dropped  to zero at  that point.   But this,  of
                 course, would be wrong.   From  Fig.  3 it can be
                 seen  that the liquid diffusivity is  about four
                 times the vapor value  at  that solution content.
                 The solute is limited to the  region  behind  A
                 simply because  that position  is as far ai
                 convection will  transport it  during a given
                 infiltration time.   Also note that  A   is not  an
                 explicit   function  of  the evaporation    The
                 evaporation front.  A   is well ahead of  A   and
                 AS  Is  also slishtly behind the position o!'
                 maximum evaporation.          '

                      Now  examine  the  resident  solution content
                 profile.   The  increase  in' solute  concentration
                 ahead  of   Ag   is  similar   to  the  unexplained
                 observation  of  Smiles et al.l<.  Thus their data
                 can be explained as the effects  of combined liquid
                 and vapor flow which they did not consider.

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  •a
  o
                                                                                                      0.08
                  Figure  6.
Calculated Solute Concentration (C/C  and C/C  )  Versus  Relative
                                    o       n           |
                             Position  (x/t'/2)
      Finally  note   that   in this  case  the minimum
 resident   solution   content   occurs  not  where
 condensation  is  a maximum but instead where  the
-phases  transfer  is zero.   This  point demonstrates
 clearly   that   the  solute  concentration  is  a
 function  of  both   convection and phase transfer,
 and  that  at  some positions convection alone  can
 produce concentration  changes.

 Conclusions
                                  The  development  of  the information in this
                             document  has been funded wholly or in part by the
                             United   States  Environmental  Protection  Agency
                             under  Cooperative  Agreement CR812225 to Colorado
                             State  University.   It  has  been  subject to.the
                             Agency's  peer  and  administrative review, and it
                             has been approved for publication.
     This   analysis  has shown that, in relatively
dry  retorted  oil shale, proper interpretation of
experimental  solute    transport    data   requires
careful  theoretical   considerations.   The  vapor
transport  of  water,  while  small when compared to
liquid   flow,    nevertheless  induces  convective
transport  processes in the  liquid phase which can
increase   or  dilute the concentration of  solutes.
Without  a  clear understanding of  the effects of
evaporation and condensation on solute convection
it is  easy to  misinterpret experimental data.

     Additional   analyses  of liquid  and vapor  flow
with  solute transport have  been performed.  These
 included    the     constant    concentration    with
 dispersion,  the  constant  flux boundary  with and
 without   dispersion,    and   a case with  actual
 measured oil shale liquid and vapor  diffusivities.
 Results  of  these analyses  will be  published  at  a
 later date.
                                                 References

                              1.  Colder  Associates,  1983.  Movement of Water.
                                  through  a  Processed Oil Shale Pile.   Report
                                  to AMOCO/Rio Blanco Dili Shale Co.,  March.
                                  HcWhorter,  D.B.,  and  Brown,  G.O. ,  1985.
                                  Adsorption and Flow  of ] Water  in Nearly Dry
                                  Lurgi Retorted Oil Shali.   Unpublished  report :
                                  prepared  for Standard!Oil Company,  AMOCO
                                  Research  Center, Colorado State University,
                                  February.               :
                                  McUhorter,   D.B.,   and  Brown,   G.O.,   1985.
                                  Liquid  and  Vapor Transport Coefficients  for
                                  Retorted  Oil Shale.  Proceedings of the 18th
                                  Oil  Shale  Symposium.   Colorado  School   of
                                  Mines Press, Colden, Colorado.

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 4.   Grlsmer,  M.E.,  1984.   Water and Salt Movement
     In Relatively Dry Soils.   Ph.D.  Dissertation,
     Department   of   Agricultural  and  Chemical
     Engineering,   Colorado State University,  Fort
     Collins,  Colorado.

 5.   Grismer,   M.E.,   McWhorter,  D.B.,  and Klute,
     A.,  1986.   Determination of Diffusivity and
     Hydraulic  Conductivity in Soils at Low Water
     Contents   from  Nondestructive Transient Flow
     Observations.  Soil Science, 141:10-19.

 6.   Grismer,   M.E.,   McWhorter,  D.B.,  and Klute,
     A., 1986.  Monitoring Water and Salt Movement
     in  Soils  at  Low  Solution  Contents.  Soil
     Science,  141:163-171.

 7.   Jackson,   R.D.,  1964a.  Water Vapor Diffusion
     in   Relatively  Dry  Soil:   I.  Theoretical
     Considerations   and   Sorption  Experiments.
     Soil Sci. Soc.  Am. Proc.  28:172-176.

 8.   Jackson,   R.D.,  1964b.  Water Vapor Diffusion
     in   Relatively  Dry  Soil:   II.   Desorption
     Experiments.     Soil   Sci.  Soc.   Am.  Proc.
     28:464-466.
 9.
     Jackson,  R.D.,
     in  Relatively
     Experiments.
     28:467-470.
1964c.  Water Vapor Diffusion
Dry  Soil:  III. Steady-State
Soil   Sci.  Soc.   Am.   Proc.
10.   Rose,  D.A.,  1963a.  Water Movement in Porous
     Materials:   I.  Isothermal  Vapor  Transfer.
     Brit. J. App. Phys. 14:256-262.

11.   Rose,  D.A.,  1963b.  Water Movement in Porous
     Materials:    II.   The   Separation  of  the
     Components  of Water Movement.  Brit.  J. App.
     Phys. 14:491-496.

12.   Cass,  A.,  Cambell,  G.S.,  and Jones,  T.L.,
     1984.   Enhancement  of  Thermal  Water Vapor
     Diffusion  in  soil.   Soil  Sci. Soc. Am. J.
     48:25-32.

13.   Jurry,  W.A.,  and Lety, J. Jr., 1979.  Water
     Vapor  Movement  in  Soil:  Reconciliation of
     Theory and Experiment.  Soil Sci. Soc. Am. J.
     43:823-827.

14.   Smiles,  D.E.,  Phillip,  J.R.,  Knight,  J.H.,
     and   Elrick,   D.E.,   1978.    Hydrodynamic
     Disperion During Adsorption of Water by Soil.
     Soil Sci. Soc. Am. J. 44:229-234.

15.   Porter,  L.K.,  Kemper, W. D., Jackson,  R.D.,
     and  Stewart, B.A., 1960.  Chloride Diffusion
     in  Soils  as Influenced by Moisture Content.
     Soil Sci. Soc. Am. Proc. 24:460-463.

16.   Krupp. H.K.,  Biggar, J.W., and Nielsen,  D.R.,
     1972.   Relative Flow Rates of Salt and Water
     in  Soil.    Soil  Sci. Soc. Am.  Proc  36-412-
     417.

17.   Laryea, K.B., Elick, D.E., and Robin,  M.J.L.,
     1982.    Hydrodynamic   Dispersion  Involving
     Cationic   Adsorption   During   Unsaturated,
     Transient Water Flow in Soil.  Soil Sci. Soc.
     Am. J. 46:667-671.
18.  Robin, M.J.L., Laryea, K.£.,  and Elick,  D.E.,
     1983.     Hydrodynamic   ; Dispersion   During
     Adsorption  of  Water  by  Soil.   J.  Hydrol
     65:333-348.

19.  Van  Schaik,  J.C.,  and  Kemper, W.D.,  1966.
     Chloride  Diffusion  in  Clay-Water  Systems.
     Soil Sci.  Soc. Am. Proc. !30:22-25.

20.  Smiles,   D.E.,   and  Gardiner,   B.N.,  1982.
     Hydrodynamic   Dispersion   During  Unsteady,
     Unsaturated  Water  Flow  in Clay Soil.   Soil
     Sci. Soc.  Am. J. 46:9-14.

21.  Bond, W.J., Gardiner, B.N., and Smiles,  D.E.,   ,
     1982.     Constant-Flux  '' Adsorption   of   a
     Tritiated Calcium Chloride Solution by a Clay
     Soil  with  Anion  Exclusion.  Soil Sci. Soc.
     Am. J. 46:1133-1137.     I

22.  Smiles,   D.E.,    and  Phillip,   J.R.,.  1978.
     Solute  Transport  During Adsorption of Water
     by   Soil:   Laboratory   Studies  and  Their
     Practical  Implications.   Soil Sci. Soc.  Am.
     J. 42:537-544.           ;

23.  McWhorter, D.B., 1971.  Infiltration Affected
     by  Flow  of Air.  Hydrology Papers, Colorado
     State University, Fort Co'llins,  Colorado.

24.  Phillip,   J.R.,   1973.    On   Solving  the
     Unsaturated   Flow  Equation:   I. The  Flux-
     Concentration  Relation. I  Soil Sci. 116:328-
     335.

25.  Phillip,  J.R.,   and  Knight, J.H., 1974.   On
     Solving  the  Unsaturated Flow Equation:  III
     New  Quasi-Analytical  Technique.   Soil Sci.
     117:1-13.
                      Appendix
                              i
 Theoretical Development      (
                              i
      This  appendix  presents a development of the
 equations of water,  vapor, arid solute transport in
 porous  media.   This development has been kept as
 brief  as  possible  and is limited  to the case of
 constant  concentration  adsqrption  of  solution.
 Solutions   for   desorptlon   and   constant  flux
 sorption  have  been  obtained by similar methods,
 but  are  beyond  the  scope  of  this  paper.   A
 complete   development  of  this  theory  will  be
 published at a later date.   ,

      This  development  is  new  and represents a
 significant   addition   to  'understanding  solute
 transport.  As such its methods and  results can be
 applied   to  other  problems  in  multiple  phase
 transport.

      For  one-dimensional  sorption  of water vapor
 the mass flux of vapor, F  , is given by:
                                          F  -  -D
                                                 v dff
                     as.
                     3x
                                                                                  (A-l)
                                     where
                                          DV - vapor diffusivity,

                                          p  — vapor density,     •

                                          8  - volumetric water content, and

                                          x  — horizontal distance.

-------
     The  vapor  diffusivity  is a function of the
free  space  molecular  diffusion coefficient, the
tortuosity,   the   porosity,   and  the  solution
content.   The ratio  dp/d.8  is used to transform
the  driving  gradient  for  diffusion  from vapor
concentration  to  water content.  Its use assumes
that   a   unique  isothermal  equilibrium  exists
between  the  vapor and liquid phases.  Continuity
of vapor phase on a control volume of porous media
yields:
    •fe
 -D           E
3x  v dfl  3x
(A-2)
wheres
     4> — porosity,

     E — mass transfer to the liquid phase,  and

     t - time.

The  source term, E, in general is assumed to be a
function of  x  and  t.

     For  one-dimensional  horizontal   sorption of
liquid  solution,  the  mass  flux of water, F.  is
given by the relation:
                         ft a
     F2 - «t C* - -Cu D* fx"   '                (A'3)

where

     q. — liquid  volumetric flux,

     C  — water concentration in solution, and

     D^ - liquid  diffusivity.

The liquid diffusivity is related to the hydraulic
conductivity  and is a strong function  of solution
content.   Continuity of liquid phase on a control
volume of porous  media yields:
               -  -C       + E
                                              (A-4)
      Adding  Eqs.  (A-2)  and (A-4)  yields the total
 water continuity:
 Note in Eq.  (A-5)  the source terms have cancelled.
 Using  typical  vapor  adsorption isotherms,  it is
 simple  to show that 3/3t(^-0)p  « 3/3t(C 6) ,  and
 thus,  the first term can be dropped.  Likewise  for
 dilute  solutions,   it  can  be  shown  that  C  =
 constant  —  1.   With these assumptions Eq.  (A-5)
 becomes :
      3JL_3_ (v +
      3t   3x v C  &B
                              3x
                            (A-6)
 Now a combined diffusivity,  D ,  is defined as:
V V
t ~ C dB !L '
w
Equations (A-6) and
equation of water flow:
3 d '3 fr. o 9 ,
8t - 3x (Dt 3x> ' °r
^ - - 3- q
3t. 3x qt '
(A-7)
(A-7) yield a simple
(A-8a)
(A-8b)
                                        where   qc   is  the  total' water volunetric flux
                                        expressed as solution.  For constant concentration
                                        sorption, the initial and boundary conditions are:
                                             ff(«,t) - 6   , and

                                             9(0,t) - So   .

                                        Flow Solution Method
                                                          (A-9)

                                                         (A-10)

                                                         (A-ll)
                  McWhorter23   and   Phillip24   showed   that
             Eq. (A-8b)   could   be  solved  by  a  method  of
             fractional  flow where the flux at any  *(x,t)  is
             defined  as  a  fraction, F(0,t), of the influx at
             x-0, or:                    i
                                                                qt(x,t)
                                                               qo(t)|,
                                                         (A-12).
                                                           where  q (t)   is the inlet volumetric flux.

                                                                Phillip  and Knight25 proved that, for constant
                                                           concentration boundary condition (Eq. A-ll),  F was
                                                           not  a  function of time.  Thus, an exact solution
                                                           for'  the  flow  can  be  found  through  a   semi-
                                                           analytical calculation of F(0).  For this boundary
                                                           condition the inlet flux is'given by:

                                                                     qo(t) - S/t1/2,  ;                 (A-13)'

                                                           where    S    is   the  soil  sorptivity  constant
                                                           calculated from the fractional analysis.

                                                                With  use  of Eqs. (A-12) and (A-13), Eq. (A-
                                                           8b) is simplified further to:
                                                                3t
                                                 _   s_   a_
                                                      1/2 3x
                                                                                                       (A-14)
                                                                For  the  boundary  conditions of Eqs.  (A-9),
                                                           (A-10),   and  (A-ll)  the  Boltzman transformation
                                                           will ease the solution of Eq.  (A-14).   A transform
                                                           coordinate is defined as:  :
                                                                A - x/t
                                                                       1/2
                                                                                     (A-15)
                                        Making   this  substitution  into  Eqs.  (A-9),  (A-10),
                                         (A-ll),   and  (A-14) yields  a  differential equation
                                        of  flow:
                  -fdT-s5I^>  •
             which is equivalent to:
                    A AS.   d_    d£
                  " 2 dA ~ dA  t dA '
             Eq. (A-16) is subject to:

                  $ (•*>) — 9  , and
                                                                                                      (A-16a)
                                                                                   (A-16b)|
                                                         (A-17)

                                                         (A-18)
                                             With  Eq.   (A-16)  and'  the   fractional  flow
                                        analysis of F(0),  the flow profile at any time and
                                        position  can  be  determined  for given diffusivity
                                        functions  D  and  D;  or  D  .

                                             Of   importance   to  this  appendix  is  the.
                                        determination of the seepage  velocity, v(0.), of a
                                        particular solution content]  6,.   Using Eq^  (A-14)
                                        and  the definition of substantial derivatives, it
                                        can be shown that:          '
                                                                                   f
                                                                                     (A-19)
                                                       10

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Liquid Phase Analysis

     With  the  total  flow  analysis, the water
transport in either phase, the evaporation and the
condensation can be determined.  First, since  all
fluxes  (liquid,  vapor,  and  total) are driven by
dS/Bx, they can be related by the ratio of
diffusivities:
     With Eqs.  (A-12) and  (A-13):
          TN
                  ,-V2   „
where
                                            (A-20)
                                           (A-21a)
                                           (A-21b)

          A(0)  is  a  transport function equal to
           Returning to the liquid continuity, Eq.
                                                               Applying  the  chain  rule  to Eq.  (A-29)  and'
                                                          regrouping produce:          i         H       '
                                                                2
                                                                                              s  dA'
                                                          Now  it  can  be  noted that the first  term can be
                                                          replaced  with phase transfer term  e(0)   as given'
                                                          by Eq.  (A-24):
                                                               eC + (A
                                 si - si (»Ds
                                                                                                      (A-33)
                                                          This  is  the  basic  equation of solute  transport
                                                          when  water  is  transported!  in  vapor and  liquid
                                                          phases,  subject to the boundary conditions of Eqs
                                                          (A-30)  and (A-31).           :
                                            (A-4)

Again,   assuming   C^-  1,  making  the  Boltzman
transform, and substituting Eq. (A-21b) yields:

                                            (A-22)
       A d0   dA
       2 dA + dA - E (X'C) «=
Here   E'  is   E/C^.  Now note that the left-hand
side  is  only a function of  A.  It can be stated
from inspection that:
     E'(x,t) -
                                            (A-23)
Substituting  Eq.  (A-23)  into  (A-22)  yields  a
relationship for the evaporation/condensation:
     e^ ~ - 2 dA

Solute Transport
                     dA
                                            (A-24)
     With  the  known  flow  conditions  it is now
possible   to   predict   the   solute  transport.
Assuming  solute  is transported by convection and
Fickian  dispersion  in the liquid phase a control
volume  analysis  yields  the  equation  of solute
motion:
     at      3x
subject to:

     C(x,0) - C

     C(o,t) - C
               o
     C(co,t) - C
                           (en
                           (SD
                                            (A-25)



                                            (A-26)

                                            (A-27)

                                            (A-28)
whens  C  is the solute concentration, and  D   is
the  coefficient of solute dispersion.  Againf the
Boltzman transform is applied and  q.  is replaced
by Eq. (A-21b) to yield:
     ^A dflfi   d_      _ d_       dC
     2  dA  + dA (CA)   dA <•*  s dA
subject to:

     C(o) - C
             o

     C(») - C
                  and
(A-29)



(A-30)

(A-31)
                                                      11

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