Processes > Surface Complexation

Surface complexation model_Effect of dosage on uranium removal

(1/1)

Francis Adu:
Dear All,

I would be glad if anyone could share his/her thought on my model for me. I am modeling the removal of uranium by iron, silicon, and aluminum hydroxides. The main objective is to study the effect of varying the adsorbent dosage on the removal at a fixed pH of 8. In the model attached; I am only varying the dosage from 0.05-0.2g. However, when I change the mass, there is no appreciable change in the removal as I am recording also 100% removal at all the different dosages. I would be glad if anyone could check my codes or suggest any reason why significant differences are not recorded whenever there is a change in the dosage. I have attached the codes below for your reference;


PHASES 1

    fix_pH
    H+ = H+
    log_k     0


SURFACE_MASTER_SPECIES 1
       Surf_al  Surf_alOH
       Surf_si  Surf_siOH
       Surf_fe  Surf_feOH
     
SURFACE_SPECIES 1
Surf_alOH = Surf_alOH
log_k 0.0
-no_check
Surf_alOH + H+ = Surf_alOH2+
log_k  12.3

Surf_alOH = Surf_alO- + H+
log_k  -13.16

Surf_alOH + UO2+2 = Surf_alOUO2+ + H+
log_k   1.4

Surf_alOH + 2UO2+2 + CO3-2 + 3H2O = Surf_alO(UO2)2CO3(OH)3-2 + 4H+
 log_k     0.99

Surf_siOH = Surf_siOH
 log_k    0.0

Surf_siOH + H+ = Surf_siOH2+
 log_k    -0.95

Surf_siOH = Surf_siO- + H+
 log_k     -6.90

Surf_siOH + UO2+2 = Surf_siOUO2+ + H+
log_k      0.99

Surf_siOH + UO2OH+ = Surf_siOUO2OH + H+
 log_k     1.0

Surf_siOH + UO2(CO3)3-4 = Surf_siOHUO2(CO3)3-4
 log_k     8.0

Surf_siOH + UO2(OH)3- = Surf_siOHUO2(OH)3-
 log_k     6.90

 Surf_feOH = Surf_feOH
  log_k 0.0

Surf_feOH +H+ = Surf_feOH2+
  log_k 7.47

Surf_feOH = Surf_feO- + H+
  log_k -9.51

Surf_feOH + UO2+2 = Surf_feOUO2+ + H+
 log_k  5.20

Surf_feOH + UO2+2 + CO3-2 = Surf_feOHUO2CO3
  log_k 15.95


SURFACE 1
Surf_siOH  2.773e-04 500  0.05
Surf_alOH  9.243e-06
Surf_feOH  8.596e-04

SOLUTION 1
    temp      20
    pH        8
    pe        4
    redox     pe
    units     mmol/l
    density   1
    C(4)      1
    Cl        10
    Na        11
    U         250 ug/L
    -water    0.1 # kg
END

Thank you

dlparkhurst:
I'm not sure how you were adjusting the surface parameters. If you changed only the number of grams, then the number of sorption sites would not vary; only the surface area would change. The surface area would most affect the potential factor, which is related to the amount of work needed to bring a charged ion from solution to a surface site.

Regardless of the surface area, the number of sites is sufficient to remove almost all of the uranium. Surf_fe is the most important surface site for sorbing the uranium.

Another way to define the number of surface sites is by use of the -sites DENSITY option, which allows the number of sites to depend on the number of grams that is defined. The input is sites per nanometer squared. I have adjusted the SURFACE definition to use -site DENSITY to produce the same number of sites in your definition for 0.05 g. I repeated the calculation with fewer and fewer grams, which corresponded to fewer and fewer sites. The amount of U sorbed is plotted against the total number of Surf sites. It requires about 1e-4 fewer sites before uranium is not completely sorbed. You seemed to expect a variation as the number of sites increased from 0.05 g. You need to look at the log Ks of the sorption reactions if you want sorption to be less complete.



--- Code: ---PHASES 1

    fix_pH
    H+ = H+
    log_k     0


SURFACE_MASTER_SPECIES 1
       Surf_al  Surf_alOH
       Surf_si  Surf_siOH
       Surf_fe  Surf_feOH
     
SURFACE_SPECIES 1
Surf_alOH = Surf_alOH
log_k 0.0
-no_check
Surf_alOH + H+ = Surf_alOH2+
log_k  12.3

Surf_alOH = Surf_alO- + H+
log_k  -13.16

Surf_alOH + UO2+2 = Surf_alOUO2+ + H+
log_k   1.4

Surf_alOH + 2UO2+2 + CO3-2 + 3H2O = Surf_alO(UO2)2CO3(OH)3-2 + 4H+
log_k     0.99

Surf_siOH = Surf_siOH
log_k    0.0

Surf_siOH + H+ = Surf_siOH2+
log_k    -0.95

Surf_siOH = Surf_siO- + H+
log_k     -6.90

Surf_siOH + UO2+2 = Surf_siOUO2+ + H+
log_k      0.99

Surf_siOH + UO2OH+ = Surf_siOUO2OH + H+
log_k     1.0

Surf_siOH + UO2(CO3)3-4 = Surf_siOHUO2(CO3)3-4
log_k     8.0

Surf_siOH + UO2(OH)3- = Surf_siOHUO2(OH)3-
log_k     6.90

Surf_feOH = Surf_feOH
  log_k 0.0

Surf_feOH +H+ = Surf_feOH2+
  log_k 7.47

Surf_feOH = Surf_feO- + H+
log_k -9.51
 
Surf_feOH + UO2+2 = Surf_feOUO2+ + H+
log_k  5.20

Surf_feOH + UO2+2 + CO3-2 = Surf_feOHUO2CO3
log_k 15.95

SOLUTION 1
    temp      20
    pH        8
    pe        4
    redox     pe
    units     mmol/l
    density   1
    C(4)      1
    Cl        10
    Na        11
    U         250 ug/L
    -water    0.1 # kg
END
#SURFACE 1
#Surf_siOH  2.773e-04 500  0.05
#Surf_alOH  9.243e-06
#Surf_feOH  8.596e-04

     
END
USER_GRAPH 1
    -axis_titles            "Surf sites, moles" "U sorbed, moles" ""
    -axis_scale x_axis      auto auto auto auto log
    -axis_scale y_axis      auto auto auto auto log
    -initial_solutions      false
    -connect_simulations    true
    -plot_concentration_vs  x
  -start
10 GRAPH_X TOTMOL("Surf_al") + TOTMOL("Surf_fe") + TOTMOL("Surf_si")
20 GRAPH_Y SURF("U","Surf")
  -end
    -active                 true
USE solution 1
SURFACE 1
    -sites DENSITY
    Surf_siOH  6.6803 500  0.05
    Surf_alOH  0.22267
    Surf_feOH    20.708   
END
USE solution 1
SURFACE 1
    -sites DENSITY
    Surf_siOH  6.6803 500  0.0005
    Surf_alOH  0.22267
    Surf_feOH    20.708   
END
USE solution 1
SURFACE 1
    -sites DENSITY
    Surf_siOH  6.6803 500  0.000005
    Surf_alOH  0.22267
    Surf_feOH    20.708   
END
USE solution 1
SURFACE 1
    -sites DENSITY
    Surf_siOH  6.6803 500  0.0000005
    Surf_alOH  0.22267
    Surf_feOH    20.708   
END
USE solution 1
SURFACE 1
    -sites DENSITY
    Surf_siOH  6.6803 500  0.00000005
    Surf_alOH  0.22267
    Surf_feOH    20.708   
END
USE solution 1
SURFACE 1
    -sites DENSITY
    Surf_siOH  6.6803 500  0.000000005
    Surf_alOH  0.22267
    Surf_feOH    20.708   
END


--- End code ---

Francis Adu:
Dear Parkhurst,

Thank you very much for your time in answering my question. The explanation has explicitly clarified a lot of things for me.

Navigation

[0] Message Index

Go to full version