Print version. Lecture #42 Precipitation and Dissolution: Iron & Predominance Diagrams (Stumm & Morgan, Chapt.7) Benjamin; Chapter
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1 Updated: 3 November 03 Print version Lecture #4 Precipitation and Dissolution: Iron & Predominance Diagrams (Stumm & Morgan, Chapt.7) Benjamin; Chapter David Reckhow CEE 680 #4
2 opics Ferrous Carbonate vs C Mixed carbonate/hydroxide diagrams Log C vs ph Predominance diagrams David Reckhow CEE 680 #4
3 Ferrous Carbonate/Hydroxide Hydroxide Equilibria Log K Fe(OH) (s) = Fe OH 4.5 Fe(OH) (s) = FeOH OH 9.4 Fe(OH) (s) OH = Fe(OH) 3 5. Carbonate Equilibria FeCO 3 (s) = Fe CO FeCO 3 (s) OH = FeOH CO FeCO 3 (s) 3OH = Fe(OH) 3 CO 3.3 David Reckhow CEE 680 #4 3
4 0 Fe Fe(OH) 3 4 H Fe(OH) Fe(OH) Feotal 5 6 OH Log C Fe(OH) David Reckhow CEE 680 #4 ph 4
5 0 Fe otal FeCO 3 mid C 3 4 H Fe(OH) FeCO Log C 7 Fe 8 OH 9 0 Fe(OH) 3 3 C = David Reckhow CEE 680 #4 ph 5
6 0 Fe otal FeCO 3 low C 3 4 H Fe(OH) FeCO 3 5 Log C 6 7 Fe 8 9 OH Fe(OH) C = David Reckhow CEE 680 #4 ph 6
7 0 FeCO 3 3 H Fe otal high C 4 FeCO Fe(OH) Log C OH C = 0 Fe(OH) 3 Fe David Reckhow CEE 680 #4 ph 7
8 0 Fe otal Mid C 3 Combined I H Fe(OH) Log C OH Fe 0 Fe(OH) 3 3 C = David Reckhow CEE 680 #4 ph 8
9 0 Fe otal Mid C 3 H FeCO 3 Fe(OH) Combined 4 II 5 Fe(OH) 6 Log C OH Fe 0 Fe(OH) 3 3 C = David Reckhow CEE 680 #4 ph 9
10 0 Fe otal Low C 3 Combined I H Fe(OH) Log C OH Fe(OH) 3 Fe 3 C = David Reckhow CEE 680 #4 ph 0
11 0 FeCO 3 Fe otal Low C 3 H Fe(OH) Combined II 4 5 Fe(OH) 6 Log C OH Fe 0 Fe(OH) 3 3 C = David Reckhow CEE 680 #4 ph
12 0 Fe otal High C H 3 Combined I 4 5 Fe(OH) 6 Log C OH 0 Fe(OH) 3 Fe 3 C = David Reckhow CEE 680 #4 ph
13 0 Fe otal High C 3 H FeCO 3 Fe(OH) Combined 4 II 5 Fe(OH) 6 Log C OH 0 Fe(OH) 3 Fe 3 C = David Reckhow CEE 680 #4 ph 3
14 Predominance Diagrams: Basics Soluble species David Reckhow CEE 680 #4 4
15 Fe, Cl, OH system I David Reckhow CEE 680 #4 5
16 Fe, Cl, OH system II David Reckhow CEE 680 #4 6
17 Fe, Cl, OH system III Final predominance diagram Benjamin Figure 8.0, pg 39 David Reckhow CEE 680 #4 7
18 Solubility & Domains A. solubility at C =0 3 M B. activity ratio diagram at C =0 3 M C. Predominance diagram for Fe = 0 4 M Stumm & Morgan, 996, Figure 7.4, pg. 39 David Reckhow CEE 680 #4 8
19 Fig 8.7 in Benjamin David Reckhow CEE 680 #4 9
20 Predominance Diagrams with Solid Phases Consider Ferrous Carbonate & Ferrous Hydroxide Fe =0 5 Closed System On a Log C vs ph axis Open system On a Log p CO vs ph axis David Reckhow CEE 680 #4 0
21 Ferrous Carbonate Equ. Fe(OH) (s) = Fe OH Fe(OH) (s) = Fe(OH) OH Fe(OH) (s) OH = Fe(OH) FeCO 3 (s) = Fe CO 3 FeCO 3 (s) OH = Fe(OH) CO 3 FeCO 3 (s) 3OH = Fe(OH) 3 CO David Reckhow CEE 680 #4
22 0 H OH Log C David Reckhow CEE 680 #4 ph
23 0 H OH Log Log p C CO David Reckhow CEE 680 #4 ph 3
24 Predominance Diagrams: Guidance I Multiple levels Benjamin, pg.39 CEE 680 web site Increasing Complexity No solids solid solids > solids Only OH complexes Mg(OH) Aluminosilicates Ligand complexes too Fe /OH / Fe(OH), Cl high Cl phdependent ligand speciation Complexing and phdependent ligand Fe(OH) / FeCO 3 David Reckhow CEE 680 #4 4
25 Predominance Diagrams: Guidance II hree types of lines ype A: concerns soluble species only defines where the two principal soluble species are at equal concentration in the noprecipitate zone One predominates on the left side of the line, and the other on the right side ype B: concerns one precipitate only defines the precipitate zone, the boundary between precipitation and no precipitation Where solubility criterion (Me ) can no longer be met hese depend on total soluble metal concentration ype C: concerns two precipitates defines boundary between two different solid phases (precipitates) David Reckhow CEE 680 #4 5
26 Fe(OH) & FeCO 3 example I ype A lines: concern soluble species Fe to Fe(OH) use first equilibria set species equal to each other 0 [ Fe 4.5 = [ Fe = [ OH [ OH [ OH ph = 0 = 0 = 0 = [ OH [ OH = K = 0 w 8.9 / [ FeOH = [ FeOH = Equation #A [ OH [ OH David Reckhow CEE 680 #4 6
27 Fe(OH) & FeCO 3 example II ype A lines: concern soluble species Fe(OH) to Fe(OH) 3 use nd & 3 rd equilibria set species equal to each other [ FeOH = [ FeOH = [ OH [ OH [ OH ph = 0 = 0 = =.85 [ OH [ OH = = 0 K w 3.7 / 0 5. [ Fe( OH ) [ Fe( OH ) = 3 = [ OH [ OH Equation #A David Reckhow CEE 680 #4 7
28 0 A lines 3 Also showing Ligand pks Labelled L, L Log C H HCO 3 CO CO 3 3 Fe FeOH Fe(OH) 3 3 #L #A #L #A David Reckhow CEE 680 #4 8 ph
29 Fe(OH) & FeCO 3 example III ype B lines: concern one precipitate Fe(OH) (s) First look at Fe and the precipitate But Fe(OH) ph=8.9.85, so this assumption is invalid! 0 = 0 [ Fe log[ Fe = 0 David Reckhow CEE 680 # ph = [ Fe 4.5 = 6.75 [ OH K w = [ Fe And assuming, [Fe Fe =0 5, hen: ph = 6.75 = K w [ Fe
30 Fe(OH) & FeCO 3 example IV ype B lines: concern one precipitate Fe(OH) (s) Next look at FeOH and the precipitate Again Fe(OH) ph=8.9.85, so now this assumption is valid. Equation #B ph = [ FeOH = 0 [ OH [ FeOH = [ FeOH = 0 David Reckhow CEE 680 # K = 4.6 log[ FeOH w And assuming, [FeOH Fe =0 5, hen: ph = 4.6 ph = K w [ FeOH
31 Fe(OH) & FeCO 3 example V ype B lines: concern one precipitate Fe(OH) (s) Next look at Fe(OH) 3 and the precipitate Fe(OH) 3 ph>.85, so this assumption is valid. Equation #B 0 5. ph [ Fe( OH ) 3 [ ( ) [ = = Fe OH H 3 [ OH K w = 0 K [ Fe( OH ) = 0 [ Fe( OH ) = 9. log[ Fe( OH ) And assuming, [Fe(OH) 3 Fe =0 5, hen: ph = ph = 4. David Reckhow CEE 680 #4 3 w 3 3 3
32 0 B Lines for Fe(OH) Log C Fe FeOH Fe(OH) (s) #B #B Fe(OH) Fe = 0 5 M David Reckhow CEE 680 #4 3 ph #L #A #L #A
33 Fe(OH) & FeCO 3 example VI ype B lines for Fe(CO) 3(s) Incorporates both a metal (Fe) and a ligand (CO 3 ) that undergo phdependent speciation hus there are certain combinations of species that must be considered (the 5 below) and some that never coexist and therefore don t need to be considered ph for L < >0.3 ph for M < >.85 Dominant species Fe H CO 3 Fe HCO 3 FeOH HCO 3 FeOH CO 3 Fe(OH) 3 CO 3 ph range < >.85 Equ # B3a B3b B4b B4c B5c Soluble Species Predominance able David Reckhow CEE 680 #4 33
34 Fe(OH) & FeCO 3 example VII ype B lines Fe(CO 3 ) (s) First look at Fe and the precipitate at low ph 0 α 0.7 C logc = [ Fe [ CO3 = [ Fe α = K K K K = [ Fe = 0 = 0.7 K K K [ Fe = 0.7 = 5.9 log[ Fe K K pk K pk C K ph C log[ Fe C H CO 3 (Assumption #) ph Fe ph<8.9, so the assumptions are only valid in that ph range: <6.3 Equation #B3a Assumption #, [Fe Fe =0 5, hen: logc logc = 5.9 log Fe ph = 5.9 ( 5) ph = 0.9 ph David Reckhow CEE 680 #4 34
35 Fe(OH) & FeCO 3 example VIII ype B lines Fe(CO 3 ) (s) First look at Fe and the precipitate at mid ph = [ Fe [ CO3 = [ Fe α α = 0.7 C logc K K K [ = = [ Fe = 0 H K K 0.7 K [ Fe = 0.7 = 0.4 log[ Fe pk K C log[ Fe ph C HCO 3 (Assumption #) ph Fe ph<8.9, so the assumptions are only valid in the ph range; Equation #B3b Assumption #, [Fe Fe =0 5, hen: logc logc = 0.4 log Fe ph = 0.4 ( 5) ph = 4.6 ph David Reckhow CEE 680 #4 35
36 Fe(OH) & FeCO 3 example IX So far we ve looked at the low and mid range ph for Fe and the carbonate precipitate (lines B3a and B3b, boxed in table below) No need to look at the highest ph range (no B3c), because we know that Fe and CO 3 don t coexist as dominant species ph for L < >0.3 ph for M < >.85 Dominant species Fe H CO 3 Fe HCO 3 FeOH HCO 3 FeOH CO 3 Fe(OH) 3 CO 3 ph range < >.85 Equ # B3a B3b B4b B4c B5c David Reckhow CEE 680 #4 36
37 Fe(OH) & FeCO 3 example X ype B lines Fe(CO 3 ) (s) Next look at FeOH and the precipitate at mid ph FeOH ph=8.9.85, so the assumptions are only valid in the ph range; Equation #B4b.6 0 = [ FeOH [ CO3 /[ OH = [ FeOH α C /[ OH 5 0 Assumption #, [FeOH Fe =0 5, hen: logc logc = 9.3 log Fe = 9.3 ( 5) = 4.3 David Reckhow CEE 680 #4 37 α logc 5.6 C = K K K = 0 = 0 [ = H K K = [ FeOH K = 9.3 log[ FeOH [ FeOH [ FeOH = 5.6 pk w pk HCO 3 (Assumption #) K K log[ FeOH C [ OH K w [ OH
38 Fe(OH) & FeCO 3 example XI ype B lines Fe(CO 3 ) (s) Next look at FeOH and the precipitate at high ph FeOH ph=8.9.85, so the assumptions are only valid in the ph range; Equation #B4c.6 0 = [ FeOH [ CO3 /[ OH = [ FeOH α C /[ OH 5 0 logc Assumption #, [FeOH Fe =0 5, hen: logc logc = 9.6 log Fe ph = 9.6 ( 5) ph = 4.6 ph David Reckhow CEE 680 #4 38 C α 5.6 [ = K K = [ FeOH = 0 = = 5.6 H K pk C [ FeOH [ FeOH [ OH K log[ FeOH = 9.6 log[ FeOH w CO 3 (Assumption #) [ OH w ph ph
39 Fe(OH) & FeCO 3 example XII At this point we ve looked at the relevant ph ranges for Fe or Fe(OH) and the carbonate precipitate (lines B3a,B3b,B4b and B4c, boxed in table below) No need to look at the lowest ph range for FeOH, and we only need to look at the highest ph range for Fe(OH) 3 (no B3c, B5a, B5b) ph for L < >0.3 ph for M < >.85 Dominant species Fe H CO 3 Fe HCO 3 FeOH HCO 3 FeOH CO 3 Fe(OH) 3 CO 3 ph range < >.85 Equ # B3a B3b B4b B4c B5c David Reckhow CEE 680 #4 39
40 0.3 [ ( ) [ /[ 3 = Fe OH 3 CO3 OH = Fe OH 3 α C OH [ ( ) /[ 3 Fe(OH) & FeCO 3 example XIII ype B lines Fe(CO 3 ) (s) Finally look at Fe(OH) 3 and the precipitate at high ph Fe(OH) 3 ph>.85, so the assumptions are only valid in the ph range; >.85 Equation #B5c 0.3 C logc Assumption #, [Fe(OH) 3 Fe =0 5, hen: logc logc = 43.4 LogFe 3pH = 43.3 ( 5) 3pH = pH David Reckhow CEE 680 #4 40 α [ = K K = [ Fe( OH ) = 0 = H K =.3 3pK = 43.3 log[ Fe( OH ) C [ Fe( OH ) [ Fe( OH ) w CO 3 (Assumption #) [ OH 3 3 [ OH K 3 w log[ Fe( OH ) pH 3pH
41 0 #B3a #B5c B Lines for FeCO #B3b FeCO 3 (s) #B4c 5 #B4b Log C Fe FeOH Fe(OH) (s) #B #B Fe(OH) Fe = 0 5 M David Reckhow CEE 680 #4 4 ph #L #A #L #A
42 Fe(OH) & FeCO 3 example XIV ype C lines: concern interface between two different precipitates FeOH (s) and Fe(CO 3 ) (s) First look at Fe and the precipitate Fe(OH) (s) K so = [ Fe [ OH [ Fe [ CO = 0 = FeCO 3(s) K so = [ Fe = 0 [ OH 0.7 [ Fe [ CO 3 = K w Use for the C lines [ CO α C 3 logc = 0 = = logα 4. ph 3.5 David Reckhow CEE 680 #4 4
43 logc = logα 4. ph Fe(OH) & FeCO 3 example XV ype C lines FeOH (s) and Fe(CO 3 ) (s) Both phases exist Assumption # First look at low ph H CO 3 ph<6.3, so assumption # is only valid in that ph range: <6.3. his may be further restricted by assumption #, which can be evaluated when plotting. α = logc logc K K K K = K K K = log( KK = pk pk = 7.6 / 4. H CO 3 (Assumption #) ) 4. ph Equation #Ca David Reckhow CEE 680 #4 43
44 Fe(OH) & FeCO 3 example XVI ype C lines FeOH (s) and Fe(CO 3 ) (s) Both phases exist Assumption # Next look at mid ph HCO 3 ph= , so assumption # is only valid in that ph range: his may be further restricted by assumption #, which can be evaluated when plotting. α = logc logc K K K = logc = logα 4. ph K K HCO 3 (Assumption #) = log( K / ) 4. ph = pk 4. ph = 3.9 ph Equation #Cb David Reckhow CEE 680 #4 44
45 Fe(OH) & FeCO 3 example XVII ype C lines FeOH (s) and Fe(CO 3 ) (s) Both phases exist Assumption # Lastly look at high ph CO 3 ph>0.3, so assumption # is only valid in that ph range: >0.3. his may be further restricted by assumption #, which can be evaluated when plotting. α logc logc = K K logc = logα 4. ph K = log() 4. ph = 4. ph CO 3 (Assumption #) Equation #Cc David Reckhow CEE 680 #4 45
46 0 #B3a FeCO 3 (s) #B5c C lines 3 4 #B3b #Cb #Cc #B4c 5 #B4b Log C #Ca Fe FeOH Fe(OH) (s) #B #B Fe(OH) Fe = 0 5 M David Reckhow CEE 680 #4 46 ph #L #A #L #A
47 0 Crop C line #B3a FeCO 3 (s) #Cc #B5c Log C 3 4 Crop away portions that are in 5 noprecipitate zone Fe 9 0 #B3b #Cb #B4c #B4b FeOH Fe(OH) (s) #B #B Fe(OH) Fe = 0 5 M David Reckhow CEE 680 #4 ph 47 #L #A #L #A
48 0 #B3a Crop one B line 3 FeCO 3(s) lines 4 Part of B4b and all of B4c & B5c 5 are in the Fe(OH) (s) zone and 6 must be removed Log C 7 8 Fe 9 0 FeCO 3 (s) #Cc #B3b #Cb #B4b FeOH Fe(OH) (s) #B #B Fe(OH) Fe = 0 5 M David Reckhow CEE 680 #4 48 ph #L #A #L #A
49 0 Crop other B line #B3a FeCO 3 (s) #Cc Log C 3 Fe(OH) (s) lines 4 Part of B is in the FeCO 5 3(s) zone and must be removed Fe 9 0 #B3b #B4b #Cb FeOH Fe(OH) (s) #B #B Fe(OH) Fe = 0 5 M David Reckhow CEE 680 #4 49 ph #L #A #L #A
50 0 Crop A lines 3 4 Remove portion of A in 5 FeCO 3(s) zone Log C Fe 9 0 #B3a FeCO 3 (s) #Cc #B3b #B4b #Cb FeOH Fe(OH) (s) #B #B 3 4 Fe = 0 5 M David Reckhow CEE 680 #4 ph 50 #L #A #L #A
51 0 Domains #B3a FeCO 3 (s) #Cc #B3b #B4b #Cb Log C Fe FeOH Fe(OH) (s) #B #B Fe(OH) Fe = 0 5 M David Reckhow CEE 680 #4 ph 5 #A
52 0 FeCO 3 (s) Final Form Log C Fe FeOH Fe(OH) (s) Fe(OH) Fe = 0 5 M David Reckhow CEE 680 #4 5 ph
53 Ferrous Sulfide Stumm & Morgan, 996, Figure 7.7, pg. 40 David Reckhow CEE 680 #4 53
54 David Reckhow CEE 680 #4 54
55 Stumm & Morgan, 996, Figure 7.8, pg. 403 David Reckhow CEE 680 #4 55
56 o next lecture David Reckhow CEE 680 #4 56
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