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# September 2006 - original design by David Parkhurst
# 19 February 2010 - additions by David Kinniburgh
# 13 December 2010 - reformulate in terms of uncharged surface master species
# this avoids the undesirable addition/removal of charge when adding/removing a surface
# thanks to Tony Appelo for pointing this out.
# This database is a temporary database until such time that a critically-assessed database is compiled.
# It is based solely on the published work of Hiemstra, van Riemsdijk and co-workers.
# So far, it only contains data for goethite and to a lesser extent ferrihydrite
# Goethite
# HR1999: Hiemstra T, van Riemsdijk, WH. J Colloid Interface Sci 210, 182-193 (1999)
# HR2000: Hiemstra T, van Riemsdijk, WH. J Colloid Interface Sci 225, 94-104 (2000)
# HRR2004: Hiemstra T, Rahnemaie R, van Riemsdijk, WH. J Colloid Interface Sci 278, 282-290 (2004)
# WKHMR2005: Weng LP, van Riemsdijk WH, Koopal LK, Geochim Cosmochim Acta 69, 325-339 (2005)
# WRKH2006: Weng LP, van Riemsdijk WH, Koopal LK, Hiemstra T. J Colloid Interface Sci 302, 442-457 (2006)
# RHR2006a: Rahnemaie R, Hiemstra T, van Riemsdijk, WH. J Colloid Interface Sci 293, 312-321 (2006)
# RHR2006b: Rahnemaie R, Hiemstra T, van Riemsdijk, WH. J Colloid Interface Sci 297, 379-388 (2006)
# HR2006: Hiemstra T, van Riemsdijk WH. J Colloid Interface Sci 301, 1-18 (2006)
# SHR2006: Stachowicz M, Hiemstra T, van Riemsdijk, WH. J Colloid Interface Sci 302, 62-75 (2006)
# RHR2007a: Rahnemaie R, Hiemstra T, van Riemsdijk, WH. J Colloid Interface Sci 315, 415-425 (2007)
# RHR2007b: Rahnemaie R, Hiemstra T, van Riemsdijk, WH. Langmuir 23, 3680-3689 (2007)
# HBR2007: Hiemstra T, Barnett MO, van Riemsdijk, WH. J Colloid Interface Sci 310, 8-17 (2007)
# HRR2007: Hiemstra T, Rietra RPJJ, van Riemsdijk, WH. Croatica Chemica Acta 80, 313-324 (2007)
# SHR2007: Stachowicz M, Hiemstra T, van Riemsdijk, WH. Envtl Sci Technol 41, 5620-5625 (2007)
# WRH2007: Weng LP, van Riemsdijk WH, Hiemstra T. J Colloid Interface Sci 314, 107-118 (2007)
# SHR2008: Stachowicz M, Hiemstra T, van Riemsdijk, WH. J Colloid Interface Sci 320, 400-414 (2008)
# WRH2008a: Weng LP, van Riemsdijk WH, Hiemstra T. Geochim Cosmochim Acta 72, 5857-5870 (2008)
# WRH2008b: Weng LP, van Riemsdijk WH, Hiemstra T. Envtl Sci Technol 42, 8747-8752 (2008)
# NB There is no guarantee that the following data are internally consistent, or are consistent with the
# aqueous database that you use.
# Refer to the original papers for the associated aqueous model.
# this formulation in terms of uncharged surface master species makes convergence slightly more difficult than
# the charged formulation...
# and so we relax the convergence criterion - reduce it if necessary
KNOBS
-c 1e-8 # this can help convergence with this master species but make sure SELECTED_OUTPUT<CR> -high_precision false
SOLUTION_MASTER_SPECIES
[N5] [N5]O3- 0 14 14
Perchlorate Perchlorate- 0 35 35
SOLUTION_SPECIES
[N5]O3- = [N5]O3-
log_k 0
Perchlorate- = Perchlorate-
log_k 0
# Goethite
SURFACE_MASTER_SPECIES
## Goe_uni Goe_uniOH-0.5
## Goe_tri Goe_triO-0.5
Goe_uni Goe_uniOH1.5 # PHREEQC needs a neutral species for coupling
Goe_tri Goe_triOH0.5 # surface sites and for changing goethite concentrations
SURFACE_SPECIES
#
# Fe3-O sites
#
## Goe_triO-0.5 = Goe_triO-0.5
## -cd_music 0 0 0 0 0
## log_k 0
Goe_triOH0.5 = Goe_triOH0.5
-cd_music 0 0 0 0 0
log_k 0
Goe_triOH0.5 = Goe_triO-0.5 + 0.5H+
-cd_music -0.5 0 0 0 0
log_k 10 # make Goe_triOH0.5 a negligible species - small but not too small!
Goe_triO-0.5 + H+ = Goe_triOH+0.5
-cd_music 1 0 0 0 0
log_k 9.20 # SHR2008
Goe_triO-0.5 + Li+ = Goe_triOLi+0.5
-cd_music 0 1 0 0 0
log_k 0.10 # HR2006, SHR2008
Goe_triO-0.5 + Na+ = Goe_triONa+0.5
-cd_music 0 1 0 0 0
log_k -0.60 # HR2006, SHR2008
Goe_triO-0.5 + K+ = Goe_triOK+0.5
-cd_music 0 1 0 0 0
log_k -1.61 # HR2006
Goe_triO-0.5 + H+ + NO3- = Goe_triOHNO3-0.5
-cd_music 1 -1 0 0 0
log_k 8.52 # HR2006a = 9.20 + (-0.68), SHR2008
Goe_triO-0.5 + H+ + [N5]O3- = Goe_triOH[N5]O3-0.5
-cd_music 1 -1 0 0 0
log_k 8.52 # HR2006a = 9.20 + (-0.68), SHR2008
Goe_triO-0.5 + H+ + Cl- = Goe_triOHCl-0.5
-cd_music 1 -1 0 0 0
log_k 8.75 # HR2006a = 9.20 + (-0.45)
#
# Fe-O sites
#
## Goe_uniOH-0.5 = Goe_uniOH-0.5
## -cd_music 0 0 0 0 0
## log_k 0
Goe_uniOH1.5 = Goe_uniOH1.5
-cd_music 0 0 0 0 0
log_k 0
Goe_uniOH1.5 = Goe_uniOH-0.5 + 0.5H+
-cd_music -0.5 0 0 0 0
log_k 10 # make Goe_uniOH1.5 a negligible species - small but not too small!
Goe_uniOH-0.5 + H+ = Goe_uniOH2+0.5
-cd_music 1 0 0 0 0
log_k 9.20 # SHR2008
Goe_uniOH-0.5 + Li+ = Goe_uniOHLi+0.5
-cd_music 0 1 0 0 0
log_k 0.10 # HR2006, SHR2008
Goe_uniOH-0.5 + Na+ = Goe_uniOHNa+0.5
-cd_music 0 1 0 0 0
log_k -0.60 # HR2006, SHR2008
Goe_uniOH-0.5 + K+ = Goe_uniOHK+0.5
-cd_music 0 1 0 0 0
log_k -1.61 # HR2006
Goe_uniOH-0.5 + H+ + NO3- = Goe_uniOH2NO3-0.5
-cd_music 1 -1 0 0 0
log_k 8.52 # HR2006a = 9.20 + (-0.68), SHR2008
Goe_uniOH-0.5 + H+ + [N5]O3- = Goe_uniOH2[N5]O3-0.5
-cd_music 1 -1 0 0 0
log_k 8.52 # HR2006a = 9.20 + (-0.68), SHR2008
Goe_uniOH-0.5 + H+ + Cl- = Goe_uniOH2Cl-0.5
-cd_music 1 -1 0 0 0
log_k 8.75 # HR2006a = 9.20 + (-0.45)
#
# Cations
#
# Iron
# Ferrous
# 2Goe_uniOH-0.5 + Fe+2 = (Goe_uniOH)2Fe+1
# log_k 8.47
# -cd_music 0.73 1.27 0 0 0
# Ferrous with surface oxidation to ferric
# 2Goe_uniOH-0.5 + Fe+2 + 2H2O = (Goe_uniOH)2Fe(OH)2-1 + 2H+
# log_k -9.31
# -cd_music 0.17 -0.17 0 0 0
# Ferrous-arsenite surface complex
# Goe_uniOH-0.5 + Fe+2 + H3AsO3 = Goe_uniOAs(OH)3Fe+0.5 + H+
# log_k 3.35
# -cd_music 0.08 0.92 0 0 0
# Calcium
Goe_uniOH-0.5 + Ca+2 = Goe_uniOHCa+1.5
log_k 2.85 # SHR2008 2.93 WRH2008a
-cd_music 0.0 2.0 0 0 0
Goe_triO-0.5 + Ca+2 = Goe_triOCa+1.5
log_k 2.85 # SHR2008 2.93 WRH2008a
-cd_music 0.0 2.0 0 0 0
Goe_uniOH-0.5 + Ca+2 = Goe_uniOHCa+1.5
log_k 3.69 # SHR2008 3.66 WRH2008a
-cd_music 0.32 1.68 0 0 0
Goe_uniOH-0.5 + Ca+2 + H2O = Goe_uniOHCaOH+0.5 + H+
log_k -9.17 # SHR2008 -9.21 WRH2008a
-cd_music 0.32 0.68 0 0 0
# Magnesium
2Goe_uniOH-0.5 + Mg+2 = (Goe_uniOH)2Mg+1
log_k 4.89 # SHR2008
-cd_music 0.71 1.29 0 0 0
2Goe_uniOH-0.5 + Mg+2 + H2O = (Goe_uniOH)2MgOH + H+
log_k -6.44 # SHR2008
-cd_music 0.71 0.29 0 0 0
# Copper
2Goe_uniOH-0.5 + Cu+2 = (Goe_uniOH)2Cu+1
log_k 9.18 # WRH2008
-cd_music 0.84 1.16 0 0 0
2Goe_uniOH-0.5 + Cu+2 + H2O = (Goe_uniOH)2CuOH + H+
log_k 3.60 # WRH2008a
-cd_music 0.84 0.16 0 0 0
2Goe_uniOH-0.5 + 2Cu+2 + 2H2O = (Goe_uniOH)2Cu2(OH)2+1 + 2H+
log_k 3.65 # WRH2008a
-cd_music 0.84 1.16 0 0 0
2Goe_uniOH-0.5 + 2Cu+2 + 3H2O = (Goe_uniOH)2Cu2(OH)3 + 3H+
log_k -3.10 # WRH2008a
-cd_music 0.84 0.16 0 0 0
#
# Anions
#
#
# Arsenate
#
Goe_uniOH-0.5 + 2H+ + AsO4-3 = Goe_uniOAsO2OH-1.5 + H2O
log_k 26.60 # SHR2008
-cd_music 0.30 -1.30 0 0 0
2Goe_uniOH-0.5 + 2H+ + AsO4-3 = (Goe_uniO)2AsO2-2 + 2H2O
log_k 29.77 # SHR2008
-cd_music 0.47 -1.47 0 0 0
2Goe_uniOH-0.5 + 3H+ + AsO4-3 = (Goe_uniO)2AsOOH- + 2H2O
log_k 33.00 # SHR2008
-cd_music 0.58 -0.58 0 0 0
#
# Arsenite
#
Goe_uniOH-0.5 + H3AsO3 = Goe_uniOAs(OH)2-0.5 + H2O
log_k 4.91 # SHR2008
-cd_music 0.16 -0.16 0 0 0
2Goe_uniOH-0.5 + H3AsO3 = (Goe_uniO)2AsOH-1 + 2H2O
log_k 7.26 # SHR2008
-cd_music 0.34 -0.34 0 0 0
#
# Phosphate
#
Goe_uniOH-0.5 + 2H+ + PO4-3 = Goe_uniOPO2OH-1.5 + H2O
log_k 27.65 # SHR2008
-cd_music 0.28 -1.28 0 0 0
2Goe_uniOH-0.5 + 2H+ + PO4-3 = (Goe_uniO)2PO2-2 + 2H2O
log_k 29.77 # SHR2008
-cd_music 0.46 -1.46 0 0 0
# 2Goe_uniOH-0.5 + 2H+ + PO4-3 + H+ = (Goe_uniO)2POOH- + 2H2O
# log_k 35.4 # SHR2008
# -cd_music 0.58 -0.58 0 0 0
#
# Carbonate
#
2Goe_uniOH-0.5 + 2H+ + CO3-2 = (Goe_uniO)2CO- + 2H2O
log_k 22.33 # SHR2008
-cd_music 0.68 -0.68 0 0 0
#
# Sulphate
#
Goe_uniOH-0.5 + H+ + SO4-2 = Goe_uniOSO3-1.5 + H2O
log_k 9.37 # HR2006
-cd_music 0.5 -1.5 0 0 0
Goe_uniOH-0.5 + H+ + SO4-2 = Goe_uniOSO3-1.5 + H2O
log_k 11.06 # HR2006
-cd_music 1 -1.84 -0.16 0 0
#
# Silica
#
2Goe_uniOH-0.5 + H4SiO4 = (Goe_uniO)2Si(OH)2-1 + 2H2O
log_k 5.85 # HBR2007
-cd_music 0.29 -0.29 0 0 0
2Goe_uniOH-0.5 + 4H4SiO4 = (Goe_uniO)2SiOHOSi3O2(OH)7-1 + 5H2O
log_k 13.98 # HBR2007
-cd_music 0.29 -0.29 0 0 0
2Goe_uniOH-0.5 + 4H4SiO4 = (Goe_uniO)2SiOHOSi3O3(OH)6-2 + 5H2O + H+
log_k 7.47 # HBR2007
-cd_music 0.29 -1.29 0 0 0
###################################################################################################
#
# Ferrihydrite (Fhy)
#
# HvR2009: Hiemstra & van Riemsdijk (2009) Geochim. Cosmochim. Acta 73, 4423-4436.
# HvRRU2009: Hiemstra et al. (2009) Geochim. Cosmochim. Acta 73, 4437-4451.
# The U sorption is sensitive to the aqueous U database used. See HvRRU2009, Table A1.
# The aqueous model used by Hiemstra et al. here is consistent with the NEA database:
# http://migrationdb.jaea.go.jp/tdb_e/d_page_e/d_0500_e.html
SURFACE_MASTER_SPECIES
## Fhy_unie Fhy_unieOH-0.5
## Fhy_unic Fhy_unicOH-0.5
## Fhy_tri Fhy_triO-0.5
Fhy_unie Fhy_unieOH1.5
Fhy_unic Fhy_unicOH1.5
Fhy_tri Fhy_triOH0.5
SURFACE_SPECIES
#
# Fe3-O sites
#
## Fhy_triO-0.5 = Fhy_triO-0.5
## -cd_music 0 0 0 0 0
## log_k 0
Fhy_triOH0.5 = Fhy_triOH0.5
-cd_music 0 0 0 0 0
log_k 0
Fhy_triOH0.5 = Fhy_triO-0.5 + 0.5H+
-cd_music -0.5 0 0 0 0
log_k 10 # make neglible
Fhy_triO-0.5 + H+ = Fhy_triOH+0.5
-cd_music 1 0 0 0 0
log_k 8.06 #HvR2009
Fhy_triO-0.5 + Na+ = Fhy_triONa+0.5
-cd_music 0 1 0 0 0
log_k -0.60 #HvR2009
Fhy_triO-0.5 + H+ + NO3- = Fhy_triOHNO3-0.5
-cd_music 1 -1 0 0 0
log_k 7.38 #HvR2009
Fhy_triO-0.5 + H+ + [N5]O3- = Fhy_triOH[N5]O3-0.5
-cd_music 1 -1 0 0 0
log_k 7.38 #HvR2009
Fhy_triO-0.5 + H+ + Cl- = Fhy_triOHCl-0.5
-cd_music 1 -1 0 0 0
log_k 7.61 #HvR2009
Fhy_triO-0.5 + H+ + Perchlorate- = Fhy_triOHPerchlorate-0.5
-cd_music 1 -1 0 0 0
log_k 6.36 #HvR2009
#
# Fe-Oa sites (edge sharing)
#
## Fhy_unieOH-0.5 = Fhy_unieOH-0.5
## -cd_music 0 0 0 0 0
## log_k 0
Fhy_unieOH1.5 = Fhy_unieOH1.5
-cd_music 0 0 0 0 0
log_k 0
Fhy_unieOH1.5 = Fhy_unieOH-0.5 + 0.5H+
-cd_music -0.5 0 0 0 0
log_k 10 # make neglible
Fhy_unieOH-0.5 + H+ = Fhy_unieOH2+0.5
-cd_music 1 0 0 0 0
log_k 8.06 #HvR2009
Fhy_unieOH-0.5 + Na+ = Fhy_unieOHNa+0.5
-cd_music 0 1 0 0 0
log_k -0.60 #HvR2009
Fhy_unieOH-0.5 + H+ + NO3- = Fhy_unieOH2NO3-0.5
-cd_music 1 -1 0 0 0
log_k 7.38 #HvR2009
Fhy_unieOH-0.5 + H+ + [N5]O3- = Fhy_unieOH2[N5]O3-0.5
-cd_music 1 -1 0 0 0
log_k 7.38 #HvR2009
Fhy_unieOH-0.5 + H+ + Cl- = Fhy_unieOH2Cl-0.5
-cd_music 1 -1 0 0 0
log_k 7.61 #HvR2009
Fhy_unieOH-0.5 + H+ + Perchlorate- = Fhy_unieOH2Perchlorate-0.5
-cd_music 1 -1 0 0 0
log_k 6.36 #HvR2009
#
# Fe-Ob sites (double corner sharing)
#
## Fhy_unicOH-0.5 = Fhy_unicOH-0.5
## -cd_music 0 0 0 0 0
## log_k 0
Fhy_unicOH1.5 = Fhy_unicOH1.5
-cd_music 0 0 0 0 0
log_k 0
Fhy_unicOH1.5 = Fhy_unicOH-0.5 + 0.5H+
-cd_music -0.5 0 0 0 0
log_k 10 # make neglible
Fhy_unicOH-0.5 + H+ = Fhy_unicOH2+0.5
-cd_music 1 0 0 0 0
log_k 8.06 #HvR2009
Fhy_unicOH-0.5 + Na+ = Fhy_unicOHNa+0.5
-cd_music 0 1 0 0 0
log_k -0.60 #HvR2009
Fhy_unicOH-0.5 + H+ + NO3- = Fhy_unicOH2NO3-0.5
-cd_music 1 -1 0 0 0
log_k 7.38 #HvR2009
Fhy_unicOH-0.5 + H+ + [N5]O3- = Fhy_unicOH2[N5]O3-0.5
-cd_music 1 -1 0 0 0
log_k 7.38 #HvR2009
Fhy_unicOH-0.5 + H+ + Cl- = Fhy_unicOH2Cl-0.5
-cd_music 1 -1 0 0 0
log_k 7.61 #HvR2009
Fhy_unicOH-0.5 + H+ + Perchlorate- = Fhy_unicOH2Perchlorate-0.5
-cd_music 1 -1 0 0 0
log_k 6.36 #HvR2009
# Carbonate
2Fhy_unicOH-0.5 + 2H+ + CO3-2 = Fhy_unic2O2CO- + 2H2O
-cd_music 0.62 -0.62 0 0 0
log_k 21.50 #HvRRU2009
# Uranium and carbonate
2Fhy_unieOH-0.5 + UO2+2 = Fhy_unie2(OH)2UO2+
-cd_music 0.9 1.1 0 0 0
log_k 9.0 #HvRRU2009
2Fhy_unieOH-0.5 + UO2+2 + H2O = Fhy_unie2(OH)2UO2OH + H+
-cd_music 0.9 0.1 0 0 0
log_k 3.30 #HvRRU2009
2Fhy_unieOH-0.5 + UO2+2 + 2H2O = Fhy_unie2(OH)2UO2(OH)2- + 2H+
-cd_music 0.9 -0.9 0 0 0
log_k -5.3 #HvRRU2009
2Fhy_unieOH-0.5 + UO2+2 + CO3-2 + H2O = Fhy_unie2(OH)2UO2CO3(OH)-2 + H+
-cd_music 0.9 -1.9 0 0 0
log_k 10.49 #HvRRU2009
Fhy_unicOH-0.5 + UO2+2 + 3CO3-2 + H+ = Fhy_unic(OCO2)UO2(CO3)2-3.5 + H2O
-cd_music 0.33 -3.33 0 0 0
log_k 36.63 #HvRRU2009
Fhy_unieOH-0.5 + UO2+2 + 3CO3-2 + H+ = Fhy_unie(OCO2)UO2(CO3)2-3.5 + H2O
-cd_music 0.33 -3.33 0 0 0
log_k 36.63 #HvRRU2009
2Fhy_unieOH-0.5 + 3UO2+2 + 6H2O = Fhy_unie2(OH)2(UO2)3(OH)6- + 6H+
-cd_music 0.9 -0.9 0 0 0
log_k -15.8 #HvRRU2009
2Fhy_unieOH-0.5 + 3UO2+2 + CO3-2 + 3H2O = Fhy_unie2(OH)2(UO2)3(OH)3CO3 + 3H+
-cd_music 0.9 0.1 0 0 0
log_k 14.6 #HvRRU2009
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