Processes > Reactive transport modelling

Water cleaning by air stripping

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MichaelZ20:
Thank you, David!

MichaelZ20:
Hi David!
I tried to reproduce the experimental data of ammonia removal (https://doi.org/10.1016/j.cej.2024.153715) by using the proposed approach.
For achieving the final experimental percent of ammonia removal the simulation gives about 3 L of the passing air, whereas in the experiment -120 L.
Could you please look through the attached input file? Do I omit something? Thank you in advance.

--- Code: ---DATABASE c:\phreeqc\database\minteq.v4.dat
TITLE
SOLUTION_MASTER_SPECIES
Oxg         Oxg       0         Oxg             32     
N           NO3-      0         14.0067         14.0067
N(-3)       NH4+      0         14.0067
N(0)        N2        0         14.0067
Phenol      Phenol    0         Phenol         94.11

SOLUTION_SPECIES
Oxg = Oxg
log_k  0
Phenol = Phenol
Log_k  0
NH4+ = NH3 + H+
        log_k -9.252
        delta_h 12.48 kcal
        -analytic 0.6322 -0.001225 -2835.76
        -gamma 2.5 0
2 NO3- + 12 H+ + 10 e- = N2 + 6 H2O
        log_k 207.08
        delta_h -312.13 kcal
NO3- + 10 H+ + 8 e- = NH4+ + 3 H2O
        log_k 119.077
        delta_h -187.055 kcal

PHASES
Oxg(g)
        O2 + 4 H+ + 4 e- = 2 H2O
        log_k 83.0894
        delta_h -571.66 kJ
N2(g)
        N2 = N2
        log_k -3.26
        delta_h -1.358 kcal
NH3(g)
        NH3 = NH3
        log_k 1.77
        delta_h -8.17 kcal
Phenol(g)
Phenol = Phenol
-log_k -3.45
-delta_h 96.4 KJ
Fix_pH
H+ = H+
log_k  0

GAS_PHASE 0
-fixed_volume
-pressure        1                   
-volume          0.2     # L in headspace
-temperature    25
N2(g)            0.78    # a portion of N2 in atmospheric air
Oxg(g)           0.242   # a portion of O2 in atmospheric air
CO2(g)           0.00044 # a portion of CO2 in atmospheric air 
NH3(g)           1e-6    # a portion of NH3 in atmospheric air
Phenol(g) 1e-6    # a portion of Phenol in atmospheric air
END           

SOLUTION 0 Initial water
units mg/l
Density 1 calculate
pH     7.7 
temp   25
N(-3)    5470  #  Total ammonia nitrogen: 4500 mg/l
Acetate  4620   
Phenol   1640
Cl 10 charge
water 1   
END

MIX 1
0  0.1    # 100 mL
SAVE SOLUTION 0

SELECTED_OUTPUT; -reset false; -file NH3_gas.txt

USER_PUNCH 
-start               
10 for i = 0 to 120 step 1     
20   punch "USE SOLUTION 0" + eol$
25   punch "EQUILIBRIUM_PHASES" + eol$
27   punch "  Fix_pH  -9.3  NaOH  10" + eol$
30   punch "USE GAS_PHASE 0" + eol$
40   punch "REACTION_TEMPERATURE 85" + eol$
45   punch "SAVE SOLUTION 0" + eol$
50   punch "END" + eol$
60 next i
-end
END

PRINT; -reset false; -selected_out false

USER_GRAPH 1
-axis_titles  "The total volume of air passed, L"  "Ammonium mass removal, %"
  -start
10 GRAPH_X GAS_VM * (GAS("NH3(g)") + GAS("N2(g)") + GAS("Oxg(g)") + GAS("CO2(g)") + GAS("H2O(g)") + GAS("Phenol(g)")) * (SIM_NO - 3)
20 GRAPH_Y ((0.3917 - TOT("N(-3)")) / 0.3917) * 100
  -end
INCLUDE$ NH3_gas.txt
END

--- End code ---

dlparkhurst:
Mainly, I think you need to consider disequilibrium in the nitrogen system. I would use Amm.dat with the extra gases added, although you really don't need the other gases; if pH is fixed, the main reaction is simply between ammonia and the head space.

Here is a revision of your script. It takes about 120 L of introduced air to remove virtually all of the ammonia, assuming it reacts independently of all other aqueous species and gases. I redefined the gases to avoid Peng-Robinson calculations, which is reasonable at low pressures.


--- Code: ---#DATABASE c:\phreeqc\database\minteq.v4.dat
TITLE
SOLUTION_MASTER_SPECIES
    Phenol        Phenol           0     Phenol          94.11
    Acetate       Acetate-         1     59.045          59.045

SOLUTION_SPECIES
Phenol = Phenol
    log_k     0
Acetate- = Acetate-
    log_k     0
Acetate- + H+ = H(Acetate)
    log_k     4.757
    delta_h   0.41 kJ
    -gamma    0 0

PHASES
Amm(g)
    Amm = Amm
    log_k     1.7966
    -analytical_expression -18.758 0.0003367 2511.3 4.8619 39.192 0
Oxg(g)
    Oxg = Oxg
    -analytical_expression -7.5001 0.0078981 0 0 200270 0
N2(g)
    N2 = N2
    log_k     -3.1864
    -analytical_expression -58.453 0.001818 3199 17.909 -27460 0
CO2(g)
    CO2 = CO2
    log_k     -1.468
    delta_h   -4.776 kcal
    -analytical_expression 10.5624 -0.023547 -3972.8 0 587460 1.9194e-05
H2O(g)
    H2O = H2O
    log_k     1.506
    delta_h   -44.03 kJ
    -analytical_expression -16.5066 -0.0020013 2710.7 3.7646 0 2.24e-06
Phenol(g)
    Phenol = Phenol
    log_k     -3.45
    delta_h   96.4 kJ
Fix_pH
    H+ = H+
    log_k     0

GAS_PHASE 0
    -fixed_volume
    -pressure 1
    -volume 0.2
    -temperature 25
    Amm(g)    1e-06
    CO2(g)    0.00044
    N2(g)     0.78
    Oxg(g)    0.242
    Phenol(g) 1e-06
END           

SOLUTION 0 Initial water
    temp      25
    pH        7.7
    pe        4
    redox     pe
    units     mg/l
    density   1
    Acetate   4620
    Amm       5470 as N
    Cl        10 charge
    Phenol    1640
    -water    1 # kg
END

MIX 1
0  0.1    # 100 mL
SAVE SOLUTION 0

SELECTED_OUTPUT; -reset false; -file NH3_gas.txt

USER_PUNCH 1
    -headings
    -start
 10 FOR i = 0 TO 5*120 STEP 1
 20 PUNCH "USE SOLUTION 0"+EOL$
 30 PUNCH "EQUILIBRIUM_PHASES"+EOL$
 40 PUNCH "  Fix_pH  -9.3  NaOH  10"+EOL$
 50 PUNCH "USE GAS_PHASE 0"+EOL$
 60 PUNCH "REACTION_TEMPERATURE 1"+EOL$
 70 PUNCH "85"+EOL$
 80 PUNCH "SAVE SOLUTION 0"+EOL$
 90 PUNCH "END"+EOL$
100 NEXT i
    -end
END
SELECTED_OUTPUT 1
-active false
END

USER_GRAPH 1
    -headings               vol %_removal Amm
    -axis_titles            "The total volume of air introduced, L" "Ammonium mass removal, %" "Amm, mol/kgw"
    -initial_solutions      false
    -connect_simulations    true
    -plot_concentration_vs  x
  -start
10 stp = GET(0)+1
20 PUT(stp, 0)
30 GRAPH_X stp * 0.2
40 GRAPH_Y((0.3917-TOT("Amm"))/0.3917)*100
50 GRAPH_SY TOT("Amm")
  -end
    -active                 true
INCLUDE$ NH3_gas.txt
END

--- End code ---

MichaelZ20:
Thank you, David!

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