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ABSTRACT
K~impf, N. and Schwertmann, U., 1983. Goethite and hematite in a climosequence in
southern Brazil and their application in classification of kaolinitic soils. Geoderma, 29 :
27--39.
The goethite/hematite + goethite ratio of 11 profiles of Oxisols, Ultisols and
Inceptisols along a 600 km E--W transect in S. Brazil varied systematically with climatic
and soil factors. The ratio increased with decreasing mean annual air temperature, increasing excess moisture (rainfall minus evapotranspiration), increasing soil organic carbon and
decreasing pH. This is explained in light of the current concept of goethite and hematite
formation in soils: higher temperatures favor hematite, whereas higher excess moisture,
higher organic carbon and lower pH favor goethite. A basis is suggested for using goetbite
and hematite in the mineralogical classes at the family level of Soil Taxonomy.
INTRODUCTION
T h e w o r l d w i d e d i s t r i b u t i o n o f soils s h o w s t h e d o m i n a n c e o f red a n d y e l l o w
soils w i t h high c h r o m a colors u n d e r warm h u m i d climates, such as the
M e d i t e r r a n e a n area a n d m o s t t r o p i c a l a n d s u b t r o p i c a l regions. In c o n t r a s t ,
soils of t e m p e r a t e h u m i d areas h a v e d o m i n a n t l y y e l l o w i s h colors with h u e s
s e l d o m r e d d e r t h a n 5 Y R . T h e y e l l o w a n d red colors are d e t e r m i n e d by
goethite (Gt) and hematite (Hm), respectively (Schwertmann and Lentze,
1 9 6 6 ) a n d t h e soil d i s t r i b u t i o n m a y be l i n k e d to t h a t o f t h e c o r r e s p o n d i n g
iron oxides.
T h e z o n a l a n d i n t r a z o n a l o c c u r r e n c e o f g o e t h i t e a n d h e m a t i t e has b e e n
d o c u m e n t e d in m a n y places ( T a y l o r a n d Graley, 1 9 6 7 ; S c h w e r t m a n n , 1 9 6 9 ;
F b l s t e r et al., 1 9 7 1 ; L a m o r o u x , 1 9 7 2 ; F a u c k , 1 9 7 4 ; D a v e y e t al., 1 9 7 5 ;
R e s e n d e , 1976). I n soils o f NW T a s m a n i a , T a y l o r a n d G r a l e y ( 1 9 6 7 ) o b s e r v e d
a decrease in t h e G t / H m r a t i o w h i c h c o r r e l a t e d w i t h a decrease in a l t i t u d e
f r o m 575 m t o sea level, an increase in t e m p e r a t u r e f r o m 9 to 12C, a n d a de*On leave from: Depto. Solos, Fac. Agronomia-UFRGS, Porto Alegre, Brazil.
0016-7061/83/0000--0000/$0.300
28
crease in rainfall from 1650 to 1080 mm. The same tendency is described by
Schwertmann et al. (1982) in an east--west soil sequence in southern Germany
where the temperature increases from 7.5 to 10.5C and the rainfall decreases
from 1000 to 600 mm. Except in these two studies no quantitative relationships between climate (or pedoclimate) and Gt/Hm ratios are available.
This work attempts to relate the goethite--hematite distribution in a soil
climosequence from volcanic rocks in southern Brazil to the following envirom
mental factors: (1) excess moisture (rainfall minus potential evapotranspiration calculated from annual values); (2) air temperature; (3) soil organic carbon
(4) soil pH; and (5) Fe, Mn, and Cu contents of the soils.
SOILS
Along a 600 km east--west transect of the Planalto Sulriograndense in Rio
Grande do Sul, Brazil (Fig. 1), elevation drops from 1200 to 90 m, annual rair~fall decreases from 2450 to 1650 mm, and mean annual temperature increases
from 14.1 to 20C. Eleven soil profiles representing the major local soil units
(Brasil, 1973) were sampled along the transect (Fig. 2). The soils are briefly described in Table I in terms of their major pedogenic features. The mineralogy
is dominated by kaolinite, with goethite and hematite and minor amounts of
Al-chlorite, quartz, cristobalite, halloysite, anatase, magnetite and ilmenite.
The low F e o / F e d ratio of the soils {<0.05) indicates that the iron oxides
are largely crystalline. Advanced weathering of the Oxisols and Ultisols is indicated by high F e d / F e t ratios of 0.75 to 0.99, whereas the Inceptisols tend
to have somewhat lower ratios in the range 0.46--0.85.
METHODS
29
MEAN ANNUALRAINFALL(ram)
AND
LO[ATtONOFSOILPROFILES
1900
?00
~1600
1600
1500
1200
r'
1300~'~'~-'-~
~30(
ScQte
~200
Fig. 1. Mean annual rainfall (ram) and locations of soil profiles (.) in the state of Rio
Grande do Sul, southern Brazil.
(Norrish and Taylor, 1961; K~impf and Schwertmann, 1982a) prior to quantitative estimation by X-ray diffraction. Self-supporting powder mounts were
made in a Perspex holder by backfilling and then gently pressing the sample
against filter paper to minimize preferred orientation. The diffractograms
were obtained with a Philips PW 1050 diffractometer equipped with a graphite
m o n o c h r o m a t o r using CoKa radiation (25mA, 35 KV) and 1/2 20/min scan
speed (2 sec TC, 1 divergence slit, 0.2 mm receiving slit, 1 scattering slit,
--
--
Born Jesus
Vacaria
Durox
-Estaqao
Paaso F o n d o
Estaq~io
S a n t o Angelo
S~o Borja
1C
2Lg
3Bj
4Va
3D
4Lv
5E
6Pf
7E
8Sa
9Sb
Haplohumox
Haplohumult
Haplumbrept
Umbric Dystrochrept
TyDic P a l e h u m u l t
Typic Haplohumox
Typic Palehumult
Typic Haplorthox
Typic Paleudult
Typic Haplohumox
--
--
--
Pachic H a p l u m b r e p t
Classification*:
.
.
.
.
V e g e t a t i o n .3
.
.
h i g h l a n d prairie,
conifers
rhyolite-dacite
h i g h l a n d prairie,
conifers
rhyolite-daeite
h i g h l a n d prairie.
conifers
basalt
h i g h l a n d prairie,
conifers
basalt
h i g h l a n d prairie,
conifers
rhyolite-dacite
mixed forest
basalt
s u b t r o p i c a l forest
s a n d s t o n e / b a s a l t prairie
basalt
s u b t r o p i c a l forest
basalt
s u b t r o p i c a l forest
basalt
prairie
rhyolite-dacite
Parent rock
.
.
.
1750
1750
1700
1700
1700
1650
1750
1700
1900
2450
2450
800
800
850
850
950
1100
800
700
650
600
600
Mean annual
.
rainfall p o t e n t i a l
(mm)
evotransp.
(ram)
16.6
16.6
17.4
17.4
19.3
20.0
16.6
15.6
15.0
14.1
14.1
temp.
(C)
740
780
720
650
390
90
800
950
1100
810
740
Altitude
(m)
.1Brasil, 1973. *: Soil T a x o n o m y (Soil Survey Staff. 1975 ). * ~Prairies at a l t i t u d e s o f - 700 m, a n d a mesic-udic c l i m a t e in
s o u t h e r n Brazil.
Soil u n i t .1
.
.
Profile
No .
TABLE I
31
A[+4ude ira!
P-EVT Lmm)
,1200
Tempero.ture (o[}
I000
I 20
-800
[,8
~\~"L - - "
~ ~- ~ /
Isr3on
,%
/ o ~--
o/
@--
,~//urq
"600
//
_
~iI
[clrbon IA~-hor,z 1
-2C'0
Ex
~I~Ckm
~o!s
pQ~ent
rock
I,0
C km
E~ST
PI'eud J[l
J HQpLOr+hO~
BGso[t
Jmbmorthox
HopLohumox
PQteudmt PoLeuduU
Sondstone
Bosott
Bosott
HopLumbrepl
Hoptohumutt
RhyoLite
Doclfe
Fig. 2. Climate, parent rocks and soils along the E--W transect.
400 or 1000 cps). The samples were X-rayed three times after re-pressing the
sample into the holder each time. Goethite and hematite were quantified by
comparing the integrated peak areas of the g o e t h i t e ( l l 0 ) and hematite(102)
lines with those of goethite and hematite standards extracted from soils. The
accuracy of this method was checked by comparing the amount of Fe as calculated from the amount of Gt+Hm determined by XRD (FeXRD) with the
amount of Fe determined chemically in the DCB-extract (Fe d ). The relationship between FeXR D and Fed was FeXR D = 0.97. Fe d - 1 . 0 7 (n = 45, r = 0.96)
and was therefore sufficiently accurate (for details see K~mpf and
Schwertmann, 1982 b).
RESULTS
From the mechanisms of hematite and goethite formation as deduced from
synthesis experiments it may be expected that the following soil environmental factors could influence the Gt/Hm ratio in soils: soil temperature, soil
moisture (replaced by mean annual temperature and excess moisture due to
lack of soil data), organic matter content, pH, and total Fe and other elements
(Schwertmann and Taylor, 1977). The relationship of each to the Gt/Gt+Hm
ratio was tested.
32
Air temperature
In both Ultisols and Oxisols an S-shaped relationship between the Hm/Gt+
Hm ratio (the H m / G t + H m ratio rather than the G t / G t + H m ratio was used in
this case because the former shows more clearly the direct influence of
temperature on the formation of hematite) and the mean annual air temperature was obvious (Fig. 3). At ~< 15C goethite was the only Fe oxide mineral
found, between 15.5 and 17.5C the H m / G t + H m ratio increased rapidly, reach
ing a m a x i m u m of about 0.8 but never 1.0. In additional samples from central
Brazil goethite occurred in a Typic Haptorthox even under an isothermic
(21.5C) and ustic (1311 mm) climate and in a Typic Acrorthox under an isohyperthermic (22.9C) and ustic (1564 mm) climate. Also, so far we have
never found a soil high in hematite which did not contain at least some goethite. It appears therefore that conditions in soils rarely occur where only
hematite can form w i t h o u t the formation of at least some goethite.
1.0-
1 I
I .... t-
0,8-
06-
Y 06
0.4-
j /
, ,oce[t,soLs
0.20
14
~
2
15
16
17
18
19
20
Mean annual air temperature ([}
o:,,ot+,
utt+s+ts
6()0
860
10'00
1200
Ramfatt rn+nus [vapotransptrubon imm)
Fig. 3. R e l a t i o n s h i p b e t w e e n H m / G t + H m r a t i o o f A a n d B h o r i z o n s a n d m e a n a n n u a l air
temperature.
Fig. 4. R e l a t i o n s h i p b e t w e e n G t / G t + H m r a t i o o f A a n d B h o r i z o n s a n d excess m o i s t u r e
(rainfall m i n u s p o t e n t i a l e v a p o t r a n s p i r a t i o n ) .
Excess moisture
The excess of rainfall over evapotranspiration was taken as a measure of the
a m o u n t of moisture available for pedogenic processes. The G t / G t + H m ratios
increased exponentially from 0.20 to 0.95 as excess moisture increased from
550 to 1000 m m (Fig. 4). Above ca. 1000 mm goethite seems to be the only
Fe oxide formed. An additional Inceptisol from an area with 1850 mm of excess moisture (not included in Fig. 4) also contained only goethite.
Organic carbon
An S-shaped correlation seemed also to exist between the Gt/Gt+Hm ratio
33
and the organic C percentage in the A1 horizon (Fig. 5). Between 2 and 3%
organic C the Gt/Gt+Hm ratio increased steeply, whereas above 3% organic C
hematite is no longer formed to any great extent. The influence of organic
components on goethite and hematite formation can also be deduced from
the individual profiles. As the c o n t e n t of organic C decreases with increasing
depth, a tendency toward a lower Gt/Gt+Hm ratio is apparent in Inceptisols
(r = 0.94) but less evident in most of the Oxisols and Ultisols (Fig. 6).
0.8"
Off
E
=.
0.~"
L~
0,2-
Orgoni: C~rbon(%)
Fig. 5. Relationship between Gt/Gt + Hm ratio and organic carbon of A1
0,8
[l
E
232
horizons of soils.
v
v
0,6
Incephsots
y : 0,73 + 0,18[nx
r:
0,~
0,9~"'n
r : 0,60"
0,
: 9
W 0X15015
y :0,2@*O.061n
D=16
v U[hsO(S
i
0cgamc Earbon 1%)
Fig. 6. Relationship between Gt/Gt + Hm ratio and organic carbon of all soil horizons.
pH(HaO)
A recent in-vitro experiment in which ferrihydrite was stored at 24C
showed that goethite increased at the expense of hematite when the pH decreased from 8 to 4 (Schwertmann, 1981). Although there is considerable scat~
34
ter in the data, an analogous negative relationship exists between G t / G t + H m
and soil pH(H20) within the range of 4.2--5.8 if the soils are grouped climatically into those below and those above 16C mean annual temperature (Fig. 7).
This again shows that temperature is an important factor. The somewhat although n o t significantly higher r-value of 0.86 for the lower-temperature
group of soils as compared to the one for the higher-temperature group seems
to indicate that pH is a more important factor in the lower-temperature range,
whereas temperature is more important in the higher-temperature range in a,>
cordance with the results plotted in Fig. 3. Naturally, if the temperature is t oc~
low for the formation of hematite, pH would no longer have any influence.
1
..
v
~ ....
08-
y = 3.00-0,~5x
"~,.~,
:[
* A i r Temperature 16,6-200C
0.6- ~-_._ ..
y = 1)1-0,33x
~.-
:> "
r : -0,69"~*n=22
.'~...
04v
0.20
4,0
4,4
a8
5'.2
5.6
610
pH (H20)
Fig. 7. Relationship b e t w e e n G t / G t + H m ratio and p H ( H 2 0 ) of A and B horizons for two
different ranges of m e a n annual air t e m p e r a t u r e
35
i0,2 0,.4
0~6
018
A~
)din
0
B1
)din
5t/G
10
AI
Gt;Gt*Hm
A3
FedlF
~2~
BI
B2
B2~
20
/\
B3
22] 3B
.~0
8Sn
Fig. 8. Depth functions of Gt/Gt+Hm and Fed/Fe t for profiles 8Sa and 3D.
The results will be discussed in light of our concept of goethite and hematite formation (Schwertmann and Taylor, 1977). Iron from silicates and other
primary sources released into solution may lead to a direct crystallization of
goethite if the solubility product of goethite, but n o t the much higher one of
ferrihydrite, is exceeded. If the solubility product of ferrihydrite is exceeded,
however, ferrihydrite will be formed and may then transform either to hematite via a dehydration--recrystallization process or, alternatively, to goethite
via dissolution of ferrihydrite. The ferrihydrite then acts as an Fe source for
crystal growth of goethite like any other Fe source. Factors favoring hematite
over goethite formation are therefore those which favor ferrihydrite formation,
such as a high release rate of Fe and a low concentration of organic compounds to complex the Fe, thereby allowing a somewhat higher concentration
of inorganic FeIII ions. In addition, once ferrihydrite is formed, hematite is
favored over goethite with increasing temperature because dehydration is involved in the ferrihydrite -~ hematite transformation.
The actual causal relationship between the various environmental factors
and the hematite--goethite relationship c a n n o t be elucidated from our study,
36
however, because of the strong intercorrelations among the factors considered,
such as temperature and excess moisture (r = - 0 . 8 6 ) and even soil organic matter and pH (r = 0.86). Even so, the type of relations found may be suitable to
test the general c o n c e p t described above.
Both higher air temperature and lower excess moisture may induce a higher
soil temperature which, in turn, favors hematite over goethite because it favors
the dehydration of ferrihydrite to hematite and accelerates the turn-over of
organic matter. A limiting temperature above which hematite can form can
not be given because other factors play a role as well. Thus, although hematite,
occurred at ca. 8C mean annual temperature (Schwertmann et al., 1982) in Bt
horizons of Alfisols on calcareous Wi]rmian gravel in the northern foreland ~f
the Alps, hematite was n o t detected below 15C in the Brazilian soils. In a
study on NW Tasmanian soils (Taylor and Graley, 1967) hematite was detected at a mean annual temperature of 9C. Independent of temperature, low
excess moisture may also favor dehydration of ferrihydrite to hematite by
lowering the activity of water in the soil. This is supported by in-vitro experiments of Torrent et al. (1982) who noticed an increasing rate of hematite formation from ferrihydrite as the relative humidity of the system dropped
from 99% to ca. 70%.
The effect of excess moisture on the distribution of yellow (hematite free)
and red (hematite containing) soils can also be seen within the same climatic
region. An example of this kind is described by Williams and Coventry (1979)
in N. Queensland where, within a toposequence, Yellow and Grey Earths are
associated with a high perched water table due to the underlying rock at shallow depths, whereas Red Earths prevail in well-drained situations with water
tables and parent rocks at greater depths.
The positive correlation between the concentration of organic c o m p o u n d s
and the Gt/Gt+Hm ratio observed in this study indicates that organic compounds favor goethite formation. This can be explained by their Fe-complexing ability which prevents formation of ferrihydrite and thereby that of
hematite.
The influence of pH has been explained elsewhere (Schwertmann, 1981).
The formation of goethite from ferrihydrite appears to be positively related to
the concentration of [Fe(OH)2 ]+ monomers which has its maximum around
pH 4 and decreases with increasing pH, thereby favoring hematite over goethite. The findings of this study are consistent with the earlier ones.
Finally, the depth function of Gt/Gt+Hm has to be explained. The dominance of goethite in the A horizon, if rich in organic matter, can be explained
as above. With increasing depth the influence of organic matter weakens and
this favors the formation of hematite. In the lower B and particularly in the C
horizon the Gt/Gt+Hm ratio again increases if the proportion of unweathered
non-oxidic Fe (e.g., from silicates) also increases (lower Fed/Fet). It is assumed that at this earlier stage of weathering the rate of Fe release is somewhat lower, leading to less ferrihydrite and, in turn, to less hematite. In addition, the maximum daily temperature is lower and excess moisture is higher in
37
these parts of the profile. In extreme cases, such as deep saprolites, goethite
may be the only oxide formed.
For two reasons we believe that the higher a m o u n t of hematite in the B
than in the C horizon is due to hematite formation from the remaining Fe reserves as the rate of weathering increases rather than from dehydration of
goethite already present. First, at surface temperatures the goethite -~
hematite transformation is energetically unfavorable. Secondly, hematite
forms readily in vitro at ambient temperatures from ferrihydrite
(Schwertmann, 1964, 1981).
So far, the distribution of hematite and goethite has been interpreted with
regard to the present pedogenic conditions. Probably, however, most of the
soils are rather old and therefore polygenetic, although no direct evidence for
this comes from profile morphology. It is possible, for example, that the goethite in the A horizon may be the result of a more recent hematite -~ goethite
transformation caused by a moister and/or cooler, i.e. C-preserving, climate
(Schwertmann, 1971). The fact that significant correlations exist between
(pedo)climatic factors and the present distribution of goethite and hematite
seems to indicate that similar differences in these factors must have existed
during former stages of soil development.
38
ratio of 0.60. This limit would be different for other mineralogical classes such
as the illitic and montmorillonitic (should be smectitic) classes because of
lower tendencies in the respective softs for hematite to be formed.
If the quantification of hematite can be done by simple color measurements
(Munsell notation, remission spectroscopy) (Torrent et al., 1980; Schwertmann
et al., 1981; K~mpf, 1981) the use of these mineralogical classes may be faciL
itated. In the softs used for this study the borderline value of Gt/Gt+Hm = 0.60
coincides with a dry Munsell hue of 6.25YR and a moist hue of approximately
3.75YR.
ACKNOWLEDGEMENTS
The authors are grateful to Mr. D.G. Schulze from this institute for critically reading the manuscript. One of us (N. Kiirnpf) acknowledges the financial
support by MEC-CAPES, Brazil (Grant 4617/76).
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