MINING GEOLOGY, 27, 379•`399, 1977

Mineralogical Studies on the Occurrence of Nickeliferous

Laterite Deposists in the Southwestern Pacific Area*

Yoshio OGURA

Abstract: Systematic field and laboratory studies of profile of several nickeliferous laterite deposits in the
Southwestern Pacific area, show their genetic relationship with the underlying ultramafic rocks. The transformation
of the fresh parent rock to the final product was traced mineralogically, petrographically and geochemically.
Deposits can be divided into two layers. The upper part is composed of oxidized red laterite ore and the lower one
contains so-called garnieritic ore, actually saprolite or decomposed serpentinite.
A clear difference exists between the chemical compositions and mineralogy in the upper and lower layers.
Goethite is the principal mineral in the upper layer and serpentine is most common in the lower one. In some cases,
a thin secondary silica layer is intercalated near the boundary. Conversion of serpentinite to laterite is reflected by
an increase in Fe2O3 and a decrease in SiO2 and MgO. Minor elements show no difference between serpentinite
and laterite. Iron in laterite occurs mainly as hydrated oxide. Nickel is concentrated with goethite in laterite and
partly with hydrous nickel-iron-magnesium silicates in the decomposed serpentinite layers.
Electron-Probe microanalyses of laterite have shown that the concentration of Ni and Fe in laterite is
relatively uniform. On the other hand, the replacement of Mg by Ni and Fe is clearly evident in the decomposed
serpentinite layer.
Mobilities of Ni and Fe by leaching in both the laterite and the garnieritic ores were examined by the citric
acid method. The amount of soluble nickel and iron in laterite is higher than that of decomposed serpentinite.
X-ray diffraction studies on numerous garnierite samples in the district indicate that they contain either
abundant 10A (talc-like) minerals or a mixtures of 10A and 7A (serpentine group) minerals. Samples con-
taining only 7A minerals are scare.

3. The chemical association of specific

Introduction
elements with stable or unstable minerals
Although weathering of mafic and ultra- during weathering.
mafic rocks has long been proposed as the 4. Flat or nearly flat wide plateau with
mechanisms for the origin of laterite and surfaces elevated sufficiently above sea level
garnieritic ores by soil. scientists and geolo- to insure adequate drainage.
5. A geologically long stable period
gists, data concerning the details of geology
and chemistry are rather scarce. during which the above conditions hold, to
The following conditions are generally allow extensive and collective leaching of the
thought to be essential for the development parent rock.
of nickeliferous laterite. The islands of the Southwestern Pacific,
1. The existence of an ultramafic rock in the Carribean Sea and Central America,
such as peridotite, serpentinite, etc. satisfy these conditions.
2. A semi-humid or humid tropical or It is known that the weathering products
monsoon climate with regularly alternating of soils in the tropics are mainly composed of
dry and wet seasons. ferric oxide and are often thickest and most
conspicuous where the underlying rock is
*Received August 8, 1977; in revised form Septem-
an iron-magnesium rich mafic or ultramafic
ber 16,1977. rock.
**Resources Research Institute , Kawaguchi, Saitama,
The mechanism of formation of the
Japan.
Key words: Pulot, Lateritization, Garnieritization, De- weathered products is very complicated as
composed serpentinite (saprolite), Citric acid method. it is affected by such factors as the chemical

379
 380 Y. OGURA MINING GEOLOGY:

nature of the original rocks, pH, Eh of

circulating water, topography, climate and
the degree of the laterization process at the
time of formation and the effect of reweather-
ing after formation. In view of these factors,
considerable fluctuation is observed, depend-
ing on the depth and place of sampling, in
constituent minerals and chemical com-
ponents.
In this paper, a typical parent rock-
decomposed serpentinite (saprolite)-laterite
sequence in Pulot, Philippines, is described
in detail and the implications of garnieritiza-
tion and laterization are discussed. The
transformation of the parent rock to garni-
critic ore and/or laterite from Toronto and
Acoje, Philippines, Pomallaa and Gebe ,
Indonesia, and Baie Ngo, Poya , Bourail
and Kouaoua, New Caledonia are also
considered.
General Aspect of Ore Deposits
Numerous ultramafic masses are distri-
buted over the Southwestern Pacific region
Fig.1 A model columnar profile of mineralogical
extending along the Philippines-Indonesia-
variations of nickeliferous laterite deposit by dep-
Solomon Islands-New Caledonia chain .
th, Pulot.
Major lateritic nickel deposits are associated
with these ultramafics. in the particle size among the three sub-
The details of petrology of the ultramafics, zones.
their origin and distribution are not de- The uppermost sub-zone of the decom-
scribed here as they require further study . posed serpentinite zone, below the laterite,
A model profile is shown in Fig.1 , of the is composed of clayey soil formed by the
formation of a nickeliferous laterite deposit decomposition of green serpentinite and
from the surface to bed rock (depth about contains small fragments of hard decom-
20m, Pulot, Philippines). In this profile, the posed serpentinite. The feature becomes
upper laterite zone and the lower decom- more and more common with depth . A
posed serpentinite zone are differentiated, thin layer of secondary silica up to 3 cm
with the boundary between them at a depth wide which occurs near the boundary be-
of about 8m. tween the laterite and the decomposed
A difference in the constituent minerals serpentinite zones is characteristic for this
can be observed between the two layers . The sub-zone. This silica layer is covered by a
laterite zone can be further classified into 3 brown coloured clayey substance. The main
sub-zones. The upper sub-zone occurs near constituent mineral is quart•¬ although it
the blackish brown surface soil containing shows a colloform structure similar to that
concretions of iron ore of about 1 mm in observed in many of the precipitated min-
diameter. The second sub-zone is composed erals. This is assumed to be a zone formed by
of a porous, yellowish brown clayey soil, the concentration of re-precipitated silica
and the basal sub-zone consists of a brownish derived from the original rock during the

yellow, fine, soft soil. There is no regularity lateritization process. A similar

, completely
 27(6), 1977 Occurrence of Nickeliferous
silicified thin layer, composed of secondary
silica and iron oxide*1 can be occasionally
observed at the boundary of the laterite and
decomposed serpentinite zones in other
regions. This suggests an explanation for the
dissolution and precipitation of components
during the weathering process. (OGURAand
HAMADA,1973).
The upper part of the decomposed ser-
pentinite zone is composed of clay formed by
the decomposition of serpentinite fragments.
It is characterized by a high content of Ni
indicated by the frequent presence of gar-
nierite on the surface of the serpentinite
fragments. The layer between this zone and
the bed rock is composed chiefly of hard,
light brownish-green decomposed serpentin-
ite fragments. There is no significant differ-
ence in the mineral content between this
layer and the bed rock.
On the other hand, some workers (e.g.,
ESGUERRA, 1961; SATSUMA,1972) have
proposed a transition zone between the
above described sequence of laterite and
decomposed serpentinite. According to this
scheme, Zone I extends from the surface
to a depth of about lm and is the layer in
which excessive oxidation takes place. Zone
II is a laterite zone composed chiefly of
ferric hydroxide and extends from the
bottom of Zone I to the next transitional
zone, Zone III, in which the laterite zone
changes to decomposed serpentinite and is
composed chiefly of clay minerals. If this
transitional zone is fixed, it can be assumed
that the above mentioned thin layer of
secondary silica corresponds to this zone.
Zone IV is the layer from Zone III to the
bed rock and is composed chiefly of clayey
minerals with blocks of serpentinite. Usually,
there are very few cases of identification of
such minerals as talc, montmorillonite,
chlorite, etc., and it is not necessary to
differentiate the transitional zone between
the laterite and decomposed serpentinite
zone. As Zone I is present near the surface,
dehydration and oxidation are naturally
*1 Probably correlates with "birbirite" of DE WAAL
(1973)
Laterite Deposits 381
very marked. Although it differs slightly
from Zone II when observed with the naked
eye, a difference is not particularly apparent
in the original constituent minerals. Zones
I to III can therefore be included in the zone
of the laterite layer.
In general, lateritic nickel beds can be
classified into two types according to their
origin: residual deposits are those in which
the source rock was weathered in situ and
sedimentary deposits in which the residual
substances were transported and deposited
or precipitated eleswhere. The deposits
described here are assumed to be residual
deposits. The following facts support this
view.
1) A change is observed in the metal and
non-metal content with depth. 2) The
appearance of ores in the upper and lower
parts of the deposit differs and coarsening
of particle size with depth is not observed.
3) Trace components are common to the
layers of laterite, decomposed serpentinite
and bed rock, and 4) A layer of secondary
silica enrichment is concentrated between the
laterite zone and the decomposed serpen-
tinite layer.
Chemical Composition
Major Elements
Table I shows that there is a large decrease
in MgO and SiO2 and increase in Fe2O3
from the bed rock-decomposed serpentinite
layer to the laterite layer. With regard to
other components, alkalis are almost constant
and there is an increase in A12O3, NiO,
Cr2O3 and Ti02. This pattern is in good
agreement with the leaching of Si02 and
MgO from the source rock by the lateritiza-
tion leaving residual Ni, Fe and Cr.
Some regularity can be observed with
depth as the Ni content (0.6-1.1 %) increases.
Si decreases and Mg shows a gradual increase
with depth of the laterite layer from the
surface. Also, there is, naturally, a sudden
increase in Si near the area where the thin
layer of secondary silica is present. Ni
content (1 %-2.3 %) varies with depth in
the decomposed serpentinite zone (Fig. 2
 382 Y. OGURA MINING GEOLOGY:

and Table 2). MgO-Fe2O3+NiO (Fig.3), it is clear

From the triangular projection of SiO2-
Table1. Chemical analyses of the serpentinized
harzburgite, decomposed serpentinite and laterite
a nd pH of its aqueous solution extracted (Pulot) .
that SiO2 decreases in a relatively stepwise
manner with progressive weathering. Plots
of bed rock, decomposed serpentinite and
laterite lie on a , line extending to the
Fe2O3+NiO (goethite) apex rather than
that to the SiO2-MgO 50/50 line (serpen-
tine).
As seen from Table 1, the ratios Mg/Fe+

Table2. Chemical analyses of some components

and citric acid soluble part of NiO and Fe2O3of
laterite, decomposed serpentinite and bed rock by
depth, and pH of its aqueous solution extracted
(Pulot).

1 and 2: Serpentinized harzburgite , (1) with a

few relic orthopyroxene, (2) with pseudomorphs
of serpentine derived from pyroxene. 3 and 4:
Completely serpentinized harzburgite (bed
rock). 5 and 6: Decomposed serpentinite, (5)
saprolite zone, depth 12m, (6) depth 10m . 7
and 8: Laterite, (7) laterite zone, depth 4m,
(8) depth 2m. Depth's figures are same as those
in Fig.2.

PERCENT SCALE

Fig.2 Chemical variations of some major and trace elements , and pH with depth through serpentinite-late-
rite sequence, Pulot.
27(6), 1977 Occurrence of Nickeliferous Laterite Deposits 383

Ni and Mg/Si show a sharp decline, while the

Fig.3 Triangular diagram (SiO2-MgO-Fe2O3+
NiO) representing the variation of composition
of bed rock-serpentinite-laterite sequence by
depth, Pulot and Toronto.
Table3. Chemical analyses and characteristics
ritic nickel ores studied from several localities
Felsic/Mafic ratio shows a slight decrease
during the bed rock-decomposed serpen-
tinite-laterite sequence. Fe/Si increases re-
markably in the lateritized part.
Analyses of major components in the
source rock-decomposed serpentinite (gar-
nieritic ore*2) samples from several localities
in the district are shown in Table 3. Com-
parison with analyses of ultramafic rocks
from different geologic environments with
different degrees of serpentinization and/or
weathering are not very significant. If the
serpentinization and/or weathering of ultra-
mafic rock is accompanied by only very
small changes in the ratio of M values*3, a
comparison of this ratio can be made for
*2 Average of 20
,000t
*3 M=(Mg+Ni)•~100/Mg+Ni+Fe2++Fe3++Mn
of the source rocks and garnie-
of Southwestern Pacific area.

1-3: Serpentinized harzburgite, (1-2) Acoje, (3) Toronto; 4: Harzburgite, New

Caledonia (after RODGERS, 1975);5-12: Garnieritic nickel ore, (5) Baie Ngo*, (6)
Poya*, (7) Bourail*, (8) Kouaoua*, (9) Pomalaa*, (10-12) Toronto.
*Average of 20,000 t.
S: Serpentine, P: Pyroxene, O: Olivine, C: Chlorite, T: Talc, Q: Quartz, G:
Goethite, Tr: Tremolite. Other figures are same as those in Table1.
 384 Y. OGURA MINING GEOLOGY:

various ultramafic intrusives. As seen in nickel ore is demonstrated in Fig.4. The

Table3, the M values of source rocks, components of each of the garnieritic ores
ranging from 87.0 to 89.3, in the district are are distributed in a narrow region having
similar to those of other ultramafics an inclination of approximately 45•‹ to the

(RUCKMICK and NOBLE,1959; GREEN,1964; horizontal axis of the figure. It suggests

TAKEDAand ONUKI,1973). roughly equal quantitative movement of the
Although there is small difference in the components. The Felsic/Mafic*4 ratio and
M values of the analysed source rocks, there Mg/Si ratio are also plotted against the M
is some gap between that of the source rock values of the associated source rocks and gar-
and that of the garnieritic ore. It is probably nieritic ores. Points show a scattered distri-
due to the formation of phyllosilicates bution within the range of the garnieritic
resulting from the break up of the nesosil- ores. There is a rough tendency for the
icates (olivine) and inosilicates (pyroxene) Felsic/Mafic ratio to become higher and the
during the garnieritization process. It can Mg/Si ratio to decrease with a decrease of
be shown that the M values of the garnieritic M values. The behavior of Felsic/Mafic
ores from the several localities in the dis- and Mg/Si ratios are less regular than that
trict fall within the range of about 80 to 60. of the Mg/Fe+Ni ratios during the forma-
Correlation between M values and Mg/Fe+ tion of the source rock-garnieritic ore
Ni ratios of the source rock and garnieritic sequence.

Minor Elements

The variation of some trace elements in the

samples from several localities of bed rock-

decomposed serpentinite-laterite sequence

and the acid treatment residue (explained

later) of these samples have been examined

spectrochemically as shown in Table4. A

few specimens of garnierite were also

analysed. It is generally said that the

behavior of trace elements such as Co, Cr,

V, Mn, Ni, Ti and Fe are not remarkably

different from each other. Consequently,

it can be assumed that there is a mutually

close relation between the source rock and

the final product. On the other hand, Cu

and Mo have increased in the source rock-

serpentinite-laterite sequence. The elements

which were not detected in the serpentinite

layer but detected in the laterite layer are

Fig.4 Variation diagram of the source rock and Ba, Sb and Pb. Also Ga was not detected

garnieritic ores in several localities of the South- in any of the layers. It is assumed that Be
western Pacific region. which is present in the source rock behaves
1•` 3: Serpentinized harzburgite, shown in
sympathetically with Al and is present in
Table 3-(1)-(3).
garnierite specimens in the serpentinite
4: Harzburgite, shown in Table 3-(4).
zone. Cr, Mn, Cu and In were detected,
5•`12: Garnieritic ore, shown in Table 3.
although the quantities were small, in the
A, B: Serpentinized harzburgite, shown in Table

1-(1),(2). above mentioned secondary silica layer.

C, D: Bed rock, shown in Table1-(3),(4). *4Felsic (Felsic elements) -(Si+K+Na)+Ca

○:Serpentinized harzburgite, ◎: Bed rock, 〓: Mafic (Mafic elements)-(Mg+Fe+Ti+Mn)+
Garnieriticore. Al
21(6),1977 Occurrence of Nickeliferous Laterite Deposits 385

Table4. Average of spectrographic determination of trace elements in laterite, de-

composed serpentinite, bed rock, secondary silica and garnierite, and citric acid treated
residue of laterite and decomposed serpentinite from several locations of Southwestern
Pacific area.

Laterite; 1 and 2: Pulot, 3: Toronto, 4: Acoje, 5: Pomalaa, Decomposed serpentinite;

6 and 7: Pulot, 8: Toronto, 9: Pomalaa, Bed rock; 10 and 11: Pulot, 12: Toronto,
13: Pomalaa, Secondary Silica; 14: Pulot, Garnierite; 15: Toronto (10 A type), 16:
Acoje (7 A type), 17: Pulot (mixed type of 10 A and 7 A), Residue (after treatment
of citric acid method); 18: Acoje (laterite), 19: Pulot (decomposed serpentinite).
Note: Numbers in parentheses indicate number of analyses.

When laterite compositions of various lo-

calities are compared, the content of Cu and

Co of the Pulot region is smaller than that

of the Acoje region.

Constituent Minerals

Results of X-ray diffraction of constituent

minerals of the laterite layer and decom-

posed serpentinite layer are shown in Fig.5.

(110), (130), (111), (141) and (240) peaks of

ƒ¿-FeO¥OH (goethite) and the peaks of

chromite are present in samples from the

sub-divisional I (upper), II (middle) and

III (lower) zones of the laterite layer. The

peaks of goethite in Zone II are higher in

intensity and sharper in comparison with

those in Zone I. In Zone III the peak

intensity is weak, indicating the more

clayey state and lower crystallinity of the

Fig.5 X-ray diffraction patterns of laterite and

decomposed serpentinite (Upper) and citric acid
reated residue (Lower), Pulot.
L(I): upper part of laterite zone, L(II): middle
part of laterite zone, L(III) : lower part of laterite
zone, D. S.: upper part of decomposed serpen-
tinite,D.S'. :lower part of decomposed serpentinite.
 386
mineral. Besides these minerals, some li-
monite, hematite, magnetite and mag-
hemite etc. are also present.
It is well known that the composition of
the constituent minerals of the laterite
layer is complicated. In many cases they are
accumulations of fine particles. The presence
of iron oxide with the fine particles of
goethite masks the other minerals so that
their characteristics are not clearly defined.
Consequently, X-ray diffraction of the
residue after removing of iron oxide was
carried out in this study.
Samples of the serpentinite layer have a
strong 7 A peak which is characteristic of
serpentine. No goethite peaks were observed
(Fig. 5). For this layer the existence of
garnierite had been predicted, but X-ray
diffraction analysis indicated no character-
istic peaks of this minerals.
In the basal rock there is no X-ray diffrac-
tion peaks corresponding to pyroxene. The
existence of clinochrysotile has been con-
firmed by electron diffraction (OGURAand
HAMADA,1973).
Also, X-ray diffraction of the residue of
the citric acid treatment of laterite and
serpentinite are shown in Fig.5. In this
figure, not only is insoluble Ni absent in the
X-ray diffraction of the samples of the
citric acid treated residue of the laterite
zone but also the goethite peaks are lost or
very low so that it can be assumed that both
Ni and Fe have been dissolved.
Table5. Chemical analyses of several components and citric acid soluble
part of NiO and Fe2O3 of laterite by size distribution (Acoje).
Y. OGURA MINING GEOLOGY:
Nickel Minerals
There have been several views regarding
the form of Ni in the oxidation zone of
laterite layer (e.g., SANTOS-YNIGOand
ESGUERRA,1959; KRAUSKOPF 1967). One of
these is that Ni is simply absorbed on iron
oxide in the ionic form (e.g., KINOSHITA,
et al. 1963) but proof of this is weak at
present and the possibility of the element
being present as a Ni mineral is stressed.
Ni in the oxidation zone can be considered
to be fixed in heavy minerals, in soluble
and insoluble (by the citric acid method*5)
Ni-bearing minerals. It is assumed that
some substitution of Ni contained in lim
onite, chiefly as soluble Ni, takes place
with goethite. Also, it is believedthat inso-
luble Ni takes the form of a hydrous magne-
sium-silicate.
Citric acid soluble part of Ni and Fe of
laterite and serpentinite is given in Table2.
The ratio of insoluble Ni and soluble Ni
of the oxidation zone in the laterite layer
varies according to the areas of production.
Soluble Ni exceeds 90% on average in the
Acoje region, and Fe in the same sample is
normally about 95%. Soluble ratios of Ni
and Fe of samples from the Pulot laterite
varies from 45% to 85% and 55% to 85%,
respectively (Table2). Therefore, the soluble
ratio of both components seems to be parallel
*5 Sodium Dithionite-Citrate-Versene method as "iron
oxide removal from soils and clays" proposed by
AGUILERA and JACKSON, 1953.
27(6),1977 Occurrence of Nickeliferous Laterite Deposits 387

Temperature (•Ž)

Fig.7 DTA and TG curves of decomposed ser-

pentinite (No.1) and citric acid treated residue
(No.2), Acoje.

though it cannot be said that the behavior

of these three elements by weathering is

necessarily the same, the possibility of some

Ni being present in the hydroxide form can

be inferred.

It is necessary to consider now the relation

Particle size (Mesh) between the solubility of nickel hydroxide

and the pH of coexisting solution both at the

Fig.6 Variation, according to the particle size,
time of its formation and during the sub-
of chemical composition of laterite from Acoje.
I: Minimum contents of Fe, Ni and Al2O3 in 100 sequent weathering process. If it is assumed
-150 mesh and Mn and Co in-325 mesh are that Ni can be present as a hydroxide
expressed as 100, respectively. (e.g. in the form of Ni(OH)2) in the laterite
and this supports the possibility of Ni zone, pH values for precipitation of Ni(OH)2

substituting for iron hydroxide. is 6.6. The observed pH value of aqueous

The soluble Ni/Fe ratio of samples varies solution extracted from laterite layer varies

from 0.91 to 1 in the Acoje region according from 5.6 to 6.1 as seen in Table1 and 2.

to particle size, (Table5), and proves that Consequently, it is hard to decide if nickel

Fe and Ni are closely related in particle size hydroxide is present in the laterite zone.

also. Further, the following facts became In the serpentinite layer, no difference is

clear from Fig.6 in which particle size and observed in the position and intensity of

analyses of water sieved samples of the X-ray peaks between the original mineral

laterite layer in the Acoje region ore were and citric acid treated residue (Fig.5).

compared. The Fe, Ni and Al2O3 group Further, no difference was observed between

which is lowest near 100-200 mesh and the both in the DTA results (Fig.7). Heat-

MgO, Mn and Co group which is highest absorption peaks below 100•Ž and 620•Ž,

near it were observed. This contrast may and the heat-generation peak at 820•Ž

reflect the mineral constitution of each are almost equal (same as seen in serpentine

fractions. Almost all of the Fe of the former group minerals). It is therefore supposed
that garnieritic nickel ore is mainly of silicate
group was present in the hydroxide form as
type, insoluble in acid. Although the rate of
goethite, which was approximately 80% of
the composition ore of the laterite layer. dissolution in citric acid solution of both Ni

By analogy with bauxite, Al is present as and Fe samples from the serpentinite is

hydroxide. Ni is distributed similarly with lower than that of samples from the laterite

Fe and Al among the particle size fractions layer (Fig.8), it is noted that the presence

and suggests the possibility that Ni is of slightly dissolved Ni and Fe may indicate
the presence of hydroxide in this layer also.
present in the form of hydroxide, and al-
388 Y. OGURA MINING GEOLOGY:

Roasting Temperature (•Ž)

Fig.9 Relation of roasting temperature with

solubility of artificial reagent of nickel and ferric
hydroxide and Acoje laterite and decomposed
serpentinite by citric acid method.

The solubilities of Ni and Fe become poor

near the thin layer of secondary silica at

Solubility(%)
the boundary between the laterite and
Fig.8 Variation of the citric acid soluble part of serpentinite layers.
NiO and Fe2O3 during laterite-serpentinite-bed A study of solubilities of artifical reagents
rock sequence by depth, Pulot. Here, chrome rep-
of Ni and Fe hydroxide and their heat-
resents the results of soluble part using HCI.
treated sample in citric acid was carried out
If the laterite and serpentinite layers are and it was found that they are dissolved
divided with respect to depth into the follow- completely when the samples are treated
ing 4 zones of I) 0-1m, II) 1.5-8m, III) above 300•Ž (Fig.9). There is a sharp
9-11m, and IV) 11.5-20m, from the surface decrease in the solubility when the samples
to bed rock, the calculated rates of dissolu- are treated above 600•Ž. The solubilities of
tion of Ni for the various zones become artifical reagent, laterite and serpentinite
103.3, 158.9, 152.1 and 120.6 and those of layers and their heat-treated samples are

Fe 104.2, 131.5, 130.8 and 11.56 (the ratio shown in the same figure. The artificial
of dissolution of Ni and Fe at 0m level is sample and its heat-treated sample are
taken as 100). Zone I is weathered for a soluble when they are in the hydroxide form
long time after formation of the laterite but they become rapidly insoluble by their
layer and it can therefore be considered that transition to oxide on heating. Dissolution
the mobilities of both Ni and Fe soluble behaviours of the laterite and serpentinite

parts for acid treatment in the sample have layers are different. Their solubility is not

become relatively poor. Zone II with the as straight forward as that of the reagent.
characteristics of the laterite layer show The complexity of their formation process
an increase of the solubilities of Ni and Fe can be inferred from the fact that the con-
with depth up to the boundary of serpen- stituent minerals of the laterite layer are
tinite layer. Zone III represents the serpen- not necessarily hydroxides alone, nor those
tinite zone (garnieritic nickel ore) with of the serpentinite layer are silicates.
highly soluble Ni and Fe. In Zone IV, there
Electron-Probe X-ray Microanalyses
is no distinct trend in the solubilities of Ni
and Fe but it can be assumed that they A number of EPMA studies have been
decrease gradually with increase in depth. made for determining the distribution of
21(6), 1977 Occurrence of Nickeliferous Laterite Deposits 389

Plate I

Backscattered electron
FeKa X-ray
image (composition)•~1000 image

NiKa A-ray AlKa A-ray

image image

CrKa A-ray
SiKa X-ray
image image

Plate I. Electron beam-scanning photographs of back-scattered electrons and selected characteristic Ka

radiations of laterite, Pulot. Accelerating potential 25 KV.
390 Y. OGURA MINING GEOLOGY:

Plate II

Backsc cattered eiectron MgKa X-ray

image (composition)•~600 image

NiKa X-ray FeKa X-ray

image image

SiKa X-rav AlKa A-ray

image image

Plate II. Electron beam-scanning photographs of back-scattered electrons and selected characteristic Ka
radiations of decomposed serpentinite. Pulot. Accelerating potential 25 KV.
27(6), 1977 Occurrence of Nickeliferous Laterite Deposits 391

DISTANCE TRAVERSED ACROSS THE LATERITE, MICRONS

Fig.10 Electron probe travers across laterite (line A-B of Plate I, B.E.C.),
Pulot.

nickel and other elements within laterite,

decomposed serpentinite and garnierite
specimens.
Plate I illustrates the element distribution
in samples from the laterite layer. Fe is
almost uniformly distributed with high
concentration as the principal chemical
component in the matrix, as is Ni although in
lower concentration. Ni is located in the
distribution area of Fe (goethite), suggesting
a close relation between the concentration
of the two elements. The concentration of
Al, Si and Mg etc. is roughly uniform in
distribution. Scanning-analysis of the main
elements of the laterite matrix, also show
a rather uniform distribution of Fe and Ni, DISTANCE ALONG TRAVERSE IN MICRONS

Al, etc. (Fig.10). Fig.11 Electron probe travers across serpentine

In most of the serpentinite sample Ni is
also distributed with nearly uniform con-
centration, as well as Mg, Si, Al and Fe
etc. It is supposed that these elements in the
samples have attained a stationary state of
weathering in their respective formational
environment.
Some decomposed serpentinites show a
marked irregular element distribution. Gran-
ular or banded structures are occasionally
pseudomorph after olivine in decomposed serpen-
tinite (line B-C; serpentine pseudomorph: A-B,
C-D; decomposed serpentinite of Plate II, B.E.
C.), Pulot.
found where the distribution of Mg is low
and that of Ni and Fe high (Plate II). In
these parts some of the Mg ions would have
been replaced by Ni and Fe ions, probably
through the alteration of primary minerals
such as olivine. The presence of Mg, Ni
 392
and Fe in pseudomorphs of serpentine after
olivine is clear from Fig.11.
In phyllosilicates ion-interchange occurs
mainly in the octahedral sites, with the
tetrahedral sites remaining the same. If a
similar form of ion interchange occurs in
serpentine in the serpentinite layer, this
interchange is most likely to occur in the
octahedral lamina.
Ni easily substitutes for Mg in the ser-
pentine octahedra without any structural
distortion which explains why Ni is high and
Mg low. In addition Mg is also replaced
by Fe. Consequently, the nickel component
is partly present in hydrous nickel-iron-
magnesium silicates in the decomposed
serpentinite layers.
Garnieritization
In the Southwestern Pacific region, the
original rocks of the nickeliferous laterite
deposits are reported to be dunite, harz-
burgite, lherzolite and wehrlite, etc. These
ultramafic rocks, classified as"Alpine Type,"
are partially or completely serpentinized.
The average Ni content of the unaltered
original peridotite in various localities varies
from 0.2%-0.5%. Lateritic layers derived
from these peridotites have Ni concentra-
tions of some 1% and the serpentinite layer
has concentrations ranging from 2.5%-3%.
This suggests a rather complicated weather-
ing process of alteration (laterization and/
or garnieritization), besides the serpentini-
zation.
The addition of water during the process of
ore-formation must be considered as well
as serpentinization. The specific gravity
of rocks diminishes, and their volume
increases, unless a considerable amount of
SiO2 and MgO are removed from the orig-
inal rock. However, there is no direct
evidence of the removal of Si and Mg both
in the original rock or in its surroundings,
except some possibility of their existence as
secondary silica or magnesium hydroxide
(brucite) in certain places, e.g. the thin
secondary silica layer at the boundary
between the laterite and serpentinite layers
Y. OGURA MINING GEOLOGY :
as described above. For certain rocks,
e.g. harzburgite, the formation of brucite
is theoretically impossible(DE WAAL,1973).
It is difficult to imagine Si and Mg moving
a long distance by diffusionin a solid phase
during elutriation of Si and Mg during
weathering. It is more reasonable to assume
that the movement of such substances took
place by solution. Mg is dissolved if the
solution is acidic but Si is more stable in
an acidic solution and dissolvesmore easily
in an alkaline solution. Under acidic con-
ditions, it is inferred that a complicated
weathering process takes place, with Ni
dissolved in solution and Fe, Co and Cr
remaining, separation of Ni and Fe, and
concentration of Ni with an increase in
pH by rain water (underground water).
Ni dissolves more readily relative to Ca,
Fe2+, and Co in a dilute carbonate solution
during the early stage of weathering of a
source rock containing alkali metals. The
amount of Ni dissolved in surface water
during the early stage of weathering is
larger than that remaining in the residual
hydroxides and oxides. However, it is
presumed that soluble Ni moves downward
by repeated elutriation with water con-
taining a large amount of carbon dioxide
gas (rain water). An acidic solution con-
taining Ni is probably neutralized in the
basal part of the laterite and serpentinite
layers in which the alkalinity is somewhat
greater. Thus, at least a portion of Ni would
be adsorbed on the surface of Mg and Si
colloids which are abundant in the lower
layer. This process has probably caused the
formation of the garnieritic ore layer.
In order to clarify the fact that the laterite
and serpentinite layers were formed by dis-
solution and precipitation of chemical com-
ponents from the sourcerock during weather-
ing, measurements of pH values of aqueous
solution extracted from samples obtained
from different depths in both layers for
each of the investigated areas were perfor-
med. One gram of uniform mesh sample
from each depth was mixed with 10cc of
distilled water for 90sec. in a mortar, and
27(6),1977 Occurrence of Nickeliferous Laterite Deposits 393

the pH of the ground material was measured.

It was found that there is a tendency for
the pH value to move to the alkali side
almost linearly with increasing depth. In
Fig.2, the pH is distinctly alkaline in the
serpentinite layer and base of the section,
but with the development of laterite it
becomes weakly acid, attaining a minimum
of 5.1 in the surface zone. The average
values are 5.2-6.0, 7.2-9.0, and 8.6-8.8 in
laterite, serpentinite and bed rock, respec-
tively. Also, the pH of the garnieritic nickel
ores fall within the range from 8.8 to 8.5
(Table3). It is interesting to note that
these values are approximately the same as
the abrasion pH values of some minerals. It
can be concluded from the pH and solubility
curve (chemical equilibrium) of hydroxide
(Fig.12, LOUGHNAN,1969), that different Depth
minerals are formed in the laterite and
Fig.13 Chemical components in relation to depth
serpentinite layers, and precipitation and of garnieritic ores from some localities of the Sou-
concentration of the various components thwestern Pacific region. Here, depth is expressed
were repeated with changing pH. by adjusting the top of the nickel ore (layer) as
The interrelation of depth and chemical 0 m.

components (Mg, Ni, Fe) of garnieritic

nickel ore samples from some localities are
shown in Fig.13. With depth (the depth is
adjusted so that the top of the Ni ore layer is
0m), Ni and Fe contents increase, with
almost equal tendency for Mg to decrease.
This increase and decrease make a very
pH
Fig.12 Solubility in relation to pH for some com-
ponents released by chemical weathering. (after
LOUGHNAN,1969)
Here, solubility curve of Ni (OH)2 is plotted in
the figure, calculates from the LATIMER'S(1952)
data.
marked contrast, and seem to represent
nearly equal interchange by these elements.
The variation of Mg is not as marked as that
of Ni and Fe.
Ni in aqueous solution occurs as Ni2+,
similar to Fe2+, Zn2+ and Mn2+. Provided
that Fe could exist in the serpentinite layer,
in the form of divalent hydroxide, it would
be precipitated on the alkaline side of
pH. But in layers where the pH is between
the lower value and the precipitation value:
as given above, it is presumed that Fe2+
may be more mobile than in the form of a
divalent hydroxide, so that Fe2+ and Ni
may behave in the same manner (simul-
taneous precipitation may also be possible).
Therefore, it is supposed that Fe also took
part as well as Ni, in the substitution of Mg
during the process of Ni-ore formation in the
serpentinite layer.
Residual Serpentinite Boulders
In Gebe island, Indonesia, weathered
residual boulders are classified into the three
394 Y. OGURA MINING GEOLOGY:

types by SATSUMA (1972) ; Type I is yellow, nickel and often contain 2%-3%, sometimes
fine grained, homogeneous and a little up to 3%-4% Ni. The average content of
powdery. It is considered to have been iron is 5%-6%.
derived from an olivine rich rock with Several samples of the Type3 boulders
little pyroxene. Primary minerals are mostly were studied by EPMA. Both by line-
decomposed and altered to serpentine. scanning and point-analysis no nickel could
Bastite is rarely observed. Type2 resembles be detected in the bastite, but in the B and
to Type 1 except that the boulders have a
pale green tinge. Type3 is pseudoporphyritic
with porphyroblasts of bastite after pyroxene.
The Type3 boulder is composed of three
parts; A, B and C, that is, A) Bastite, derived
from pyroxene, remaining as porphyroblasts
in the rock, B) Surrounding parts of the
bastites, which are grey or dark grey showing
cleavages under the microscope, and are
considered to be serpentine probably de-
rived from orthopyroxene, C) Brown parts
which occupy the rest of the boulders and
are serpentine pseudomorphs after olivine
Fig.14 Photomicrograph of the residual serpenti-
with a mech structure (Fig.14). The mode
nite boulder "type3", Gebe.
is as follows; A) bastite, 10-15%, B) ser- A: Bastite (A-part), B: Serpentine pseudomorph
pentine after pyroxene, 25-30%, and C) ser- after pyroxene (B-part), C: Serpentine pseudo-

pentine pseudomorphs after olivine, 55- morph after olivine (C-part). Plane polarized

60%. The Type3 boulders are also rich in light (•~70)

DISTANCE TRAVERSED ACROSS THE RESIDUAL DECOMPOSED SERPENTINITE BOULDER. MICRONS

Fig.15 Electron probe travers across residual serpentinite boulder "type 3", Gebe.
(I) : Serpentine pseudomorph after olivine (C-part).
(II): Serpentine pseudomorph after pyroxene (B-part).
27(6),1977 Occurrence of Nickeliferous Laterite Deposits 395

Table6. Electron probe analyses of B and C Mg and Ni replace each other for a wide
parts of residual serpentinite boulder "type range, and if the entire replacement is
3", Gebe.
possible Ni contents of these minerals are
calculated as 0%-46.18% in Ni-serpentine

and 0%-36.39% in Ni-talc on the basis of

the following chemical formulae;

3(Mg, Ni)O.2SiO2¥2H2O
•\( Ni-serpentine)

3(Mg, Ni)O.4SiO2• H2O

(Ni-talc)
The green tint of these minerals seems to
*Chemical analyses . be roughly proportional with their Ni

contents, i.e. a greenish tint indicates high

C parts notable concentrations of nickel are Ni content.
present. These results are given in Table 6. pH-solubility graphs for each chemical
There is a sympathetic variation of Ni and component of the minerals show that SiO2
Fe in the B part (Fig.15). In the C part,
precipitates easily, as the solution becomes
as in the B part, there is a concentration of more acid and Mg(OH)2 is easily precipi-
Ni and although Fe concentration is marked, tated when the solution becomes alkaline
it is smaller than in the B part. Namely,
(above pH value of 6.6 up to 10, see Fig.15).
nickel content is richer in the B part than Since the ratio of SiO2/MgO in the Ni-talc
in the C part except one case and iron mineral and Ni-serpentine mineral is 4:3
content shows also the same tendency and 2:3 respectively, the Ni-talc mineral
without exception. would have been formed in more acidic
In general, it has been considered that conditions than the Ni-serpentine minerals.
the C part is a nickel-source in the rock and From a number of X-ray diffraction data
that the B part is poor in nickel. However, obtained for the specimens in the district,
it may be assumed that the B part altered three types have been distinguished :1) talc-
more than C part so far as in nickel and like mineral with a strong peak of 10A
iron content.
(green), 2) Serpentine-group mineral with a
The Mg content of the fresh ultramafic strong peak of the 7.4A basal reflection
rock from this area varies in the range of
(yellowish green), and 3) mixture of these
40%-50% whereas Mg from 34%-36% in forms with both the 7A and 10A peaks
the B and C parts. The Mg content therefore
(bluish green). Among the samples*6 ex-
remains much more constant than those amined, the type-l or type-3 minerals are
of nickel and iron during the process of abundant, and those of type-2 which show
garnieritization. the single 7A peak are very scarce except in
The behavior of Ni, Fe and Mg in the some samples from New Caledonia. It is
residual serpentinite boulders shows a therefore suggested that the 10A type of
similar tendency to those of some garnieritic
garnierite is more easily to be formed by the
ores in the decomposed serpentinite layer replacement of Mg by Ni during the
described above. weathering process (garnieritization) than

Garnierite that of the 7A type. From the notable

difference in the intensity of the character-

X-ray diffraction patterns of garnieritic istic 7A, 10A and other peaks of garnierite
ore indicate that most samples resemble observed in samples from different localities
serpentine-group minerals or a talc-like and in individual samples from the same
mineral, or mixture. In the serpentine- *6Of 34 specimens from Philippines and Indonesia,
group and talc-like minerals, two principal 10A-type is 19, mixed type of 10A and 7A is 13
nickel carriers in the ores, it is likely that and 7A-type is 2.
 396 Y. OGURA MINING GEOLOGY:

Table7. Chemical analyses and structural for-

mulae of various garnierites

1: 10A-type garnierite, Toronto. 2: 7A-type

garnierite, Acoje. 3: Mixture of 10A-type and 7

A-type garnierite, Pulot.

(a) H2O+=weight loss from 110-1000•Ž.

(b) Oct.=(R2++3/2R3+).

Analyses and structual formulae of each

of the three types selected from pure gar-

nierite specimens from the Philippines are

given in Table 7. There is no remarkable

chemical difference between each of the

three types, but some deviation from the

compositions of serpentine group minerals

and of talc (corresponding to the serpentine

Fig.16 X-ray diffraction patterns of garniertes, formula of Mg3Si2O5(OH)4 and talc formula
heated at various temperatures.
of Mg3Si4O10(OH)2) as regards both the
No.1: 10A-type garnierite, Toronto . No.2: 7A-
octahedral/tetrahedral cation ratios can
type garnierite, Acoje. No.3: Mixture of 10A-
be recognized as suggested by BRINDLEY and
type and 7A-type garnierite, Pulot.
HANG (1973).
locality, the genetic processes of the mineral For each of the three types classified by
are probably very complex. means of X-ray diffraction the DTA curve
From X-ray diffraction patterns of heated is shown in Fig.17. As seen in the figure,
specimens in the district (Fig.16), the the curves of the three samples differ a
following results are apparent. In type-l little from each other. Type-1 shows no
samples, the 10A peak shows minor change marked peak of heat-absorption and heat-
up to 800•Ž, except for some sharpening,
generation after the peak of adsorped water
and it vanishes beyond 900•Ž. In samples of below 100•Ž, excepting a peak of heat-
type-2, a gradual weakening of the intensity absorption near 800•Ž; type-2 shows the
of the 7.5A peak is seen with heating up to second large peak of heat-absorption near
600•Ž, and it vanishes at 700•Ž. In samples 580•Ž, after the peak of adsorbed water,
of type-3, the 10A peak disappears at 900•Ž and again at 830•Ž a heat-generation peak
and the 7.4A peak vanishes at 700•Ž, is seen, presumably due to a transformation
suggesting the presence of two kinds of to other material. Type-3 shows no marked
minerals. peak of heat-absorption and heat-generation,
 27(6), 1977 Occurrence of Nickeliferous Laterite Deposits 397

are largely controlled by the degree of the

lateritization and/or garnieritization of the
original rock. Topography and climate are
also important. The weathering products
have been subjected to complicated proc
-esses, but, over-all, the materials in laterite
and the decomposed serpentinite (garnieritic
ore) layer have a restricted range of ore-
grade and constituent minerals.
Concerning the bed rock-decomposed
serpentinite (garnieritic ore)-laterite se-
quence, the following points are important:
)1 The upper layer is laterite and the lower
layer consists of decomposed serpentinite
(garnieritic nickel ore). The principal min-
erals are goethite in the upper layer and
serpentine in the lower one. 2) A completely
silicified thin layer composed of secondary
silica can be observed occasionally at
the boundary between the two layers. 3)
There is a large decrease in MgO and SiO2
and increase in Fe2O3 from the source rock
through the decomposed serpentinite into
the laterite. The distribution behavior of
the minor elements indicates a mutually
close relation in the conversion process
of serpentinite to laterite. 4) M values of
the source rock and garnieritic nickel ore
Temperature (•Ž)
range from 89-87 and from 80-60, respec-
Fig.17 DTA and TG curves of garnierites. tively, and the Felsic/Mafic and Mg/Si
No.1 : 10 A-type garnierite, Toronto. No. 2 :7 A- ratios are more or less regular in comparison
type garnierite, Acoje. No. 3: Mixture of 10 A- with the Mg/Fe+Ni ratio during the
type and 7A-type garnierite, Pulot. formation of the so-called garnierite ore.
excepting a rather small peak of heat- 5) Nickel is concentrated with goethite in
generation at 780•Ž. In almost all samples the laterite and partly consists of hydrous
of the same kind from other districts a heat- nickel-iron-magnesium silicate in the de-
absorption peak at 100•Ž-200•Ž, the second composed serpentinite layer. 6) In the
small heat-absorption peak of 600•Ž-700•Ž, decomposed serpentinite layer, Mg is re-
and a heat-generation peak at 800•Ž-900•Ž placed by Ni and Fe in pseudomorphs of
are present (KATO, 1961. etc.). While the serpentine after olivine. 7) Most of the
above, type-2 shows a somewhat similar Ni and Fe in the laterite can be dissolved by
tendency, types-l and-3 markedly differ citric acid treatment, but in a sample
from type-2. from the serpentinite layer, almost no
difference is observed by X-ray diffraction
Conclusions
and DTA etc. between the original mineral
The nickeliferous laterite deposits in the and the citric acid treated residue. 8) The
Southwestern Pacific area are formed by pH value of aqueous solution extracted
weathering in situ of ultramafic rocks. from sample is distinctly alkaline in the
Major differences of the weathering products serpentinite layer (7.2-9.0) and bed rock
 398 Y. OGURA
(8.6-8.8), but with the development of
laterite it becomes mildly acid (5.2-6.0).
9) A distinct distribution state of Ni, Fe
and Mg is observed in serpentinite residual
boulders. 10) From X-ray diffraction anal-
lysis, the garnierite samples in the district
contain abundant talc-like minerals and
mixed type of talc-like minerals and serpen-
tine group minerals. Single 7A peak (ser-
pentine group) minerals are scarce.
Acknowledgements: The writer wishes
to extend his acknowledgements to Mr. Y.
HAMADA of the ResourcesResearch Institute
for his kind discussion and encouragement
throughout this work. The writer is indepted
to Dr. A. SATSUMA of the Sumitomo Metal
Co., Ltd. for valuable suggestion. Further,
the writer is grateful to Messrs.N. NAOEand
S. HAMADA of the Pacific Metals Co., Ltd.
for their continuing guidance and interest.
Finally, the writer is also grateful to Dr.
R. I. GAITof the Royal Ontario Museum,
Canada for his critical reading of the
manuscript.
References
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 21(6),1977 Occurrence of Nickeliferous Laterite Deposits 399

西 南 太平 洋 地 域 の含 ニ ッケル ・ラテ ラ イ ト鉱 床 の

鉱物学的研究 お よび産状

小 倉 義 雄

要 旨

西 南 太 平 洋 地 域(お も に フ ィ リピ ン ・イ ン ドネ シ ア お し た仮 晶 の 蛇 紋 石 中で,Niお よ びFeイオ ンに ょ っ てMg

よび ニ ュー カ レ ドニ ア)の い くつか の含 ニ ッケ ル ・ラテ イ オ ン が置 き換 え られ て い る もの が み と め られ る.

ライ ト鉱 床 につ い て,そ の産 状,基 盤 岩 との 関連,構 成 化 学 成 分 的 に,上 述 の 生 成 過 程 中 で のFe2O3の 増 加,

鉱 物 の性 状,化 学 成 分,生 成過 程 な どに つ い て の べ た. SiO2,MgOの 減 少 とい う主 成 分 の 移 動 は,一 般 的に

超 塩 基 性岩 に 由来 す る これ ら風化 残 留 鉱 床 は,お もに いわれ て い る ラテ ライ ト化 作 用 の傾 向 と同 じで は あ るが,

原 岩 の鉱 物 構 成 や ラテ ライ ト化/ガ ー ニエ ラ イ ト化 作 用 局部 的 に 二 次 的 のSiの 濃 集 部(薄 層)が あ っ た りNi成

の変 質 程 度 に規 制 され,さ らに 地形 ・気 候 な ど の要 因 も 分 の と くに 高 い 帯 が あ っ た り して,生 成 作 用 の 過 程 で の
加 わ っ て複 雑 な 過 程 を経 て生 成 され る ので あ ろ うが,最 複 雑 性 を示 してい る.し か し原 岩 お よ び ガ ー ニエ ライ ト

終 産 物 で あ る ラテ ライ ト・ガ ー ニエ ラ イ ト鉱 石 は あ る 限 鉱 石 のM値 は そ れ ぞ れ89∼87,80∼60の 範 囲に入 るよ う

られ た範 囲 の 品 位,構 成鉱 物 か ら な っ て い る. で あ る.

基 盤 岩 → 変 質 蛇 紋 岩 層(ガ ー ニ エ ライ ト鉱石)→ ラテ 当地 域 の ガ ー ニ エ ライ ト(ニ ュー カ レ ドニ ア の一 部 を

ラ イ ト層 の生 成 過 程 で,ラ テ ライ ト層 中 の ニ ッケ ル の 形 除 く)はX線 的 に10Å 型(滑 石)の 鉱 物 と10Å と7Å

態 は お も に水 酸 化 物 の形 で針 鉄 鉱 に と もな わ れ,変 質 蛇 (蛇紋 石)の 混 合型 の もの が 多 く,単 独7Å ピ ー ク(蛇

紋 岩 層 で は一 部 含 水 ニ ッケ ル 鉄 マ グネ シ ウ ム珪 酸 塩 の 形 紋 石 類)の 鉱物 は 少 な い

で存 在 す る と思 わ れ,同 層 中 に 初 生 の か ん らん 石 を交 代