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Composition and Association of Arsenian Goldfieldite from the Marian gold

deposit, Northern Luzon, Philippines

Article  in  Mineralogy and Petrology · January 1989

DOI: 10.1007/BF01164325

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Mineralogy and Petrology (1989) 40:145-154
Mineralogy
ano
Petrology
© by Springer-Verlag 1989

Composition and Association of Arsenian

Go|dfieldite from the Marian Gold Deposit,
Northern Luzon, Philippines
U. Knittel

Department of Geology, University of Melbourne, Parkville, Victoria, Australia

With 3 Figures

Received September 20, 1988;

accepted January 12, 1989

Summary
Arsenian goldfieldite from the Marian Gold Mine, Philippines, which is hosted
by the Cordon Syenite Complex, forms a solid solution series with Zn-rich ten-
nantite, in contrast to goldfieldite from Goldfield (Nevada), Kamchatka and
Uzbekistan, which are Zn-poor and form solid solution series with tetrahedrite.
Goldfieldite from Butte (Montana) and the Lower Caucasus is very similar to the
Marian goldfieldite. In all deposits except those at Butte and in the Lesser Caucasus,
goldfieldite is associated with native Au, altaite, and Au-Ag-tellurides. Both the
Marian gold deposit and the vein systems at Butte are associated with porphyry
copper mineralization.

Zusammenfassung
Zusammensetzung und Paragenese yon arsenhaMgem Goldfieldit aus der GoldlagerstiJtte
Marian, Nord-Luzon, Philippinen
As-reicher Goldfieldit der Marian Gold Lagerst~itte (Philippinen) bildet eine
Mischkristall-Reihe mit Zn-reichem Tennantit und steht damit in Gegensatz zu Gold-
fieldit von Goldfield (Nevada), Kamtschatka und Uzbekistan, welche Zn-arm sind und
Mischkristalle mit Tetrahedrit bilden. Goldfieldit von Butte (Montana) und aus dem
Kleinen Kaukasus hat eine ~ihnliche Zusammensetzung wie der der Marian Vererzung.
Goldfieldit ist in allen Vorkommen, ausgenommen Butte und dem Kleinen Kaukasus,
mit gediegen Au, Altait und Au-Ag-Telluriden vergesellschaftet. Sowohl die Marian
Vererzung als auch die vererzten G~inge von Butte sind an "porphyry copper"-
Vererzungen gebunden.
146 U. Knittel

Introduction

The occurrence of Te-bearing tetrahedrite was first reported by Sharwood (1907),

who investigated ores from the M o h a w k Mine, Goldfield, Nevada. An analysis by
Palmer, published in Ransome et al. (1909), was subsequently interpreted to indicate
that the material analyzed was a mixture of several minerals or a member of the
tetrahedrite-tennatite group (Thompson, 1946 and references therein). Thompson
(1946) confirmed that the material is a m e m b e r of the tetrahedrite group, because
he was able to obtain a X-ray powder diffractogram which could be indexed as
tetrahedrite, but suggested the name "goldfieldite", proposed by Ransome et al.
(1909), be dropped. Later, some argument arose as to whether Te replaces S or (Sb,
As) (Kalbskopf, 1974 and references therein)• Kalbskopf(1974) resolved the discus-
sion by showing that intensities of reflections in X-ray powder diffractograms
obtained from synthetic goldfieldite agreed well with calculated intensities if it was
assumed that Te replaces As and Sb. Furthermore, he found that replacement of

~_0_0m ~X,

Japan) / i~ , ,J/ / ~ / ,
_/ ~ , ~// t ! / i

/ ~ /
.,~..J .i
/ volcanics /"//
c. [ { ~ S I
/ /
i I
/ :
1

/ ~ . . ~ " iL~)] '~ / / / / phonolite

i % / I r

w
f \' i ~ _/
b-'\\,7/
t't l/
,j
\ ._
',_.-" /
,-~ " .
/ % /~,, N
i ~ . ~-~.. ~, .', ;-., , -,
(7--- -/ ~~ ' , Z ~ ,-// , ~i ;-L,, , ,l
V ~ , "t2// , ,. I
~ ,, I#•. ~ - I
/ I ,= I [
//"'~- M ar ia, Gold Mine ~ -~Ii /. S / / ~ / ~~~ ._ // .'/ DS
- , A ,i

t ~k^-..._ .,o J ~ .'~IIM-'" i I

x, ~ . ~ _ ~\ ~ .~ ~ '-"..~fll~ll , ~ mo,,o,it, , ,,
.C~ ~ °o/I
"~:~///~ll.., ' , M / ~"-t
,
.
-.
\
% l
/ • ~,.. aporphyryCu (. . ~ /
-- ~ 1 4% ~ -- t \ ,, )mineralizationS. e I \ /
v"t d J <,> / -. I ", "-; '~'
"-,a k ~ \ % i

~- ~ "~'-'-,,~ ~ Ladolam ~ \ ts ~ -~ -,, A " ..,

Fig. 1. Map of the southwestern margin of the Pacific ocean showing localities mentioned
in the text. Inset is a simplified map of the part of the Cordon Syenite Complex that hosts
the Marian Gold deposit (A alluvium, L lusitanite (= marie alkali syenite, Streckeisen, 1976),
M monzonite, pS = porphyritic syenite and alkali syenite, pslcS = pseudoleucite-bearing
syenite, S syenite; based on Alapan, 1982 and Knittel, 1982)
 Composition and Association of Arsenian Goldfieldite 147

Sb 3+ and As 3+ by Te 4÷ is coupled with a decrease in Cu TM and thus derived the

formula Cu6[4]Cu6_xTM (TeS3)4S, with x close to 2 for goldfieldite. In contrast,
Novgorodova et al. (1978, cited by Sakharova et al., 1984) suggested that the sub-
stitution of Te 4+ for S b 3+ is compensated by the reduction of Cu 2÷ to Cu +
(see below).
Only a few microprobe analyses of goldfieldite have been published. Levy (1967)
reported one analysis of goldfieldite from Goldfield; Springer (1969) gave two
analyses for tellurian tennantite and goldfieldite from Butte, Montana, and Frenzel
et al. (1975) provided an analysis ofgoldfieldite from Sardinia. More recently, Tsepin
et al. (1977), Spiridonov et al. (1984), Loginov et al. (1983), and Sakharova et al. (1984)
reported nearly two dozen analyses for tellurian tetrahedrite-tennatite and gold-
fieldite from eastern Uzbekistan, the Lesser Caucasus and Kamchatka. From these
data it appears that, with the exception of goldfieldite from Butte (Springer, 1969)
and the Lesser Caucasus (Loginov et al. (1983), goldfieldite forms a solid-solution
series with tetrahedrite. Spiridonov et al. (1984) distinguished tellurian tetrahedrite-
tennatite (Te < Sb or As, atomic proportion) from goldfieldite (Te > Sb or As) and
this subdivision will be followed here.
This paper reports the occurrence of goldfieldite and tellurian tennantite from
the Marian Gold Mine (northern Luzon, Philippines; Fig. 1), which, in contrast to
occurrences in Uzbekistan and Kamchatka and similar to the goldfieldite of Butte,
forms a solid solution series with tennantite. Variable Te contents in goldfieldite
from the Marian mine allow evaluation of the extent of chemical variation in this
solid solution series.

The Marian Gold Deposit

Gold mineralization associated with the Cordon Syenite Complex (northern Luzon,
Philippines) is remarkable among the 57 noteworthy gold deposits found in the arc
systems at the western margin of the Pacific Plate between Japan and Fiji, for the
following reasons (Sillitoe, 1988):
- - T h e magmatic complex hosting the mineralization has been dated at 25 Ma
(Knittel, 1983) and thus the mineralization appears to be the oldest significant
gold mineralization in the Western Pacific.
- - I t is one of three deposits associated with alkaline rocks; the other two being the
large epithermal deposits of Lihir (Ladolam) (Davies and Ballantyne, 1987; Plimer
et al., 1988) and Fiji (Emperor Mine) (Ahmad et al., 1987 and references therein)
Furthermore, a mineralogical study of the potassic igneous rocks hosting the
mineralization has shown that they are derived from precursors with affinities to
lamproites. This discovery is striking, because _Rockand Groves (1988) have recently
suggested that gold in many epithermal deposits may have been derived from
lamprophyres, a diverse group of rocks which, arguably, includes lamproites (Rock,
1987).
The Cordon Syenite Complex consists of several textural varieties of syenite,
monzonite, and lusitanite (= mafic alkali syenite; Streekeisen, 1976), which have
intruded co-magmatic pyroclastic flow deposits. Chemically these rocks are char-
acterized by K 2 0 > Na 2O, low (Na + K)/A1 (atomic ratio) and relatively high SiO 2
contents (for details see Knittel, 1987).
148 U. Knittel

Au-rich porphyry copper mineralization is associated with the monzonites,

which are the most highly evolved phases of the intrusion (Baquiran, 1975, Sillitoe,
1979, Knittel, 1982). Sillitoe (1979) and Knittel, (1982) found that the porphyry
copper mineralization resembles some porphyry deposits of the Canadian Cordillera,
which are likewise hosted by alkaline rocks (Barr et al., 1976).
Numerous quartz-K-feldspar veins cut through the intrusion. They contain
abundant sulfides and small amounts of electrum and tellurides where they
cut through the lusitanite stocks (Alapan, 1982, Knittel, 1982). The abundance of
tellurides appears to be a typical feature of precious metal deposits associated with
alkaline rocks (Mutschler et al., 1985). The lusitanite is intensely altered in about
1 m wide zones adjacent to the veins with all mafic minerals (40-55 vol. ~o clino-
pyroxene, biotite and magnetite) being replaced by pyrite. The intensity of the
wallrock alteration and the lack of similar alteration and mineralization in syenite
and monzonite suggest that the reaction of the hydrothermal fluids with the wall-
rocks (loss of S to the wallrock) was the main cause for the deposition of the ore
minerals (Knittel, 1982). This mechanism for Au deposition has also been suggested
by Neall and Philipps (1987) for an Au deposit in Kambalda, Western Australia, on
the basis of the alteration assemblage in the host rocks and thermodynamic con-
siderations. Though this concept is certainly applicable only to a minority of
epithermal Au deposits, it explains the old observation that auriferous veins are
often richest where they cross-cut mafic host rocks (e.g. Schneiderh6hn, 1941). The
relationship between the porphyry style mineralization and the veins is not clear,
but a common origin is suggested by the observation that both are contemporane-
ous within the analytical precision of about 1 m.y. (Knittel, 1983). Nash and
Cunningham (1973) and Rice et al. (1985) have suggested that similar epithermal
Au--sulfide--telluride veins in the Central City and Boulder County Districts,
Colorado, are related to underlying porphyry-Mo systems. Sillitoe (1988) likewise
argued for a direct or indirect magmatic origin of precious metals in the majority
of the gold deposits in the Western Pacific. The veins have been mined for about 7
years (1978-1984).

Goldfieldite
Goldfieldite i n t h e Marian ores is commonly intergrown with tennantite, either as
thin (5-20/~m), often multiple lamellae in the latter or as individual grains (up to
about 1 mm wide). Both minerals have very similar reflectivities, but goldfieldite has
a pinkish-grey colour, which distinguishes it from tennatite. This difference in colour
is distinct only in oil but very faint in air.
Representative microprobe analyses of goldfieldite and tellurian .tennatites are
given in Table 1. From these data it is evident that, similar to Butte (Springer, 1969),
a Te-rich (arsenian goldfieldite) and a Te-poor (tellurian tennantite) mineral occur.
About one half of the analyses contain 0.01-0.05~o Ag, while the other half does not
contain detectable Ag. The majority of analyses lacked Au. Bi was not detected in
all analyses. Goldfieldite from Kamchatka (Sakharova et al., 1984), on the other
hand, is rich in Au (0.2-0.9~), Ag (0.0-2.3~), and Bi (0.5-7.0~), while goldfieldite
from Uzbekistan (Tsepin et al., 1977) contains 0.7-1.5~o Ag, but neither Au nor Bi.
Figure 2 illustrates the chemical variation of goldfieldite from the Marian Gold
Deposit relative to its Te content. It is obvious that Cu is positively correlated with
 Composition and Association of Arsenian Goldfieldite 149

Table 1. Representative microprobe analyses of arsenian goldfieldite, tellurian tennantite,

tennantite and tetrahedrite from the Marian Gold Mine

t 2 3 4 5 6

Cu 46.18 45.95 45.00 43.95 41.63 38.30

Zn 0,11 0.80 1.90 2.98 6.80 9.15
Fe 0,01 0.24 0.10 0.20 0.77 0.84
Ag 0.00 0.00 0.01 0.02 0.04 n,d.
Au 0.00 0.02 0.00 0.01 0,00 n,d.
Sb 1.14 1.66 2.81 3.74 0.04 18.50
As 7.72 9.17 9.97 10.84 19.38 7.62
Te 17.68 15.10 12.06 9.75 0,11 n.d.
S 26.92 26.91 27.13 27.25 29.14 24.69
Z 99.76 99.85 98.98 98.74 97.91 99.10
structural formulae on the basis of $3.25
Cu 2.81 2.80 2.72 2.64 2.34 2.54
Zn 0.01 0.05 0.11 0.17 0.37 0.59
Fe 0.00 0.02 0.01 0.01 0.05 0.06
Z 2.82 2.87 2.84 2.82 2.76 3.19
Sb 0.04 0.05 0.09 0.12 0.00 0.64
As 0.40 0.47 0.51 0.55 0.93 0.43
Te 0.54 0.46 0.36 0.29 0.00 n.d.
E 0.98 0.98 0.96 0.96 0.93 1.07

n.d. -- not determined; Bi was undetected in an analyses.

1: arsenian goldfieldite; 2, 3, 4: tellurian tennantite; 5: tennantite; 6: tetrahedrite.

Te, while the Zn contents drop to values close to zero for Te-rich varieties. As and
Sb likewise decrease with increasing Te. Fe appears to have a very weak negative
correlation with Te. The constant sums of (Te + As + S b ) = 0.96-0.98 (cations
normalized to $3.25) indicate that, in natural goldfieldite, Te replaces As and Sn (cf.
Kalbskopf, 1974). Furthermore, sums of (Cu + Zn + Fe) of 2,78-2,87 confirm the
deficiencies in (Cu + Zn + Fe) suggested by Kalbskopf (1974), as a consequence of
the replacement of Sb 3÷ and As 3+ by Te 4+. Similar deficiencies are not observed in
the Russian and Butte analyses, where (Cu + Zn + Fe) scatter between 2.89 and
3.11 (Tsepin et al., 1977; Loginov et al. (1983); Sakharova et al., 1984; Spiridonov et
al., 1984; Springer, 1969)..Novgorodova et al. (1978; cited by Sakharova et al., 1984)
interpreted this feature as indication that the substitution of Te 4+ for Sb 3+ is
compensated by the reduction of Cu 2÷ to Cu ÷.
Comparison of the data for goldfieldite from the Marian deposit with published
data for goldfieldite from other deposits shows that the former is characterized by
high As/Sb ratios (Fig. 3) indicating that the goldfieldite from Cordon forms a solid
solution series with tennantite rather than tetrahedrite. In this respect it resembles
goldfieldite from Butte (Springer (1969) and tellurian tennatite from the Lesser
Caucasus (Loginov et al., 1983) and differs from goldfieldite from Goldfield (Levy,
1967), K a m c h a t k a (Sakharova et al., 1984), and Uzbekistan (Tsepin et al., 1977;
150 U. Knittel
"--7
I
AA
2,9-- A
oV
V
2.7- --
V
V o~
o o
V
Cu %
ii

2.5-
2.3
I-- I

04.-
0.3-
Zn
0.2-
oo
0"1 t V ~ V °v~ AA
0.0 --

I, 1 -
V

0.3-
Fe
0.2-
X7
0,1- ~7
8o AA
0.0- • ooO~ o ~
oI I - I I
0.6-
0.5~ v W
~7 x7
O.#-
Sb
0.3- %
0.2- Fig. 2. Chemical variation of goldfieldite
0.1-
and tellurian tetrahedrites/tennantites
°~ °° o relative to their Te-content (cations on
0.0- the basis of 83.25 ). Symbols: open circles:
I
1.0- Marian Gold Mine (this paper), closed
circles: Butte (Springer, 1969), square:
0.8- Goldfield (Levy, 1967), triangles: eastern
As
0.6- Uzbekistan (upward pointing: Tsepin et
oO.~ o
o al., 1977; downward pointing: Spiridonov
0.4- X7
V
et al., 1984), stars: Kamchatka (Sakha-
W ~7
O.2- ~zx" rova et al., 1984), diamonds: Lesser
Caucasus (Loginov et al., 1983). Where
I I 1 I
0.0 0.2 0.4. 0.6 0.8 data points coincide, only one symbol
Te was plotted

Spiridonov et al., 1984). Altogether the available data (Fig. 3) suggest unlimited
isomorphic exchange of Sb, As, and Te.

Other Minerals

Similar to other epithermal gold-mineralizations in the Philippines (Sillitoe, 1988),

the Marian gold deposit is relatively rich in sulfides and sulfosalts (pyrite, sphalerite,
 Composition and Association of Arsenian Goldfieldite 151
Te

lye. I
/6" i

/ G~ 11

/ I II

t O/ 0 ~"~"
~l-O ~"

~ V
11 i

/ !
!
i

•
, I
L
V

// iI

As .v Sb

Fig. 3. Variation in As-Sb-Te of goldfieldite and tel]urian tetrahedrites/tennantites from the

Marian Gold Mine, Goldfield, Butte, eastern Uzbekistan, and Kamchatka (symbols and
sources as in Fig. 2)

galena, chalcopyrite, tetrahedrite, and tennatite, in order of decreasing abundance).

Native gold is a common inclusion in galena, frequently associated or intergrown
with altaite. Gold also occurs on fractures in pyrite, sphalerite and tennanite. Its
average grain size is about 9 microns, largest grains attaining diameters of 30
microns. The silver content of the gold is 7-9 wt.-%.
Altaite is the most common telluride in the Marian ores. Almost invariably it
occurs as inclusions in galena. In addition hessite, calaverite, and a Au-Ag telluride
intermediate between petzite and hessite occur rarely.

Discussion

The paragenesis of goldfieldite in the Marian deposit is essentially the same as in

the Kamchatka deposit, where it is associated with the sulphides chalcopyrite,
pyrite, and galena, the tellurides calaverite, petzite, sylvanite, rucklidgeite and altaite
and native gold and tellurium (Sakharova et al., 1984). These minerais occur in
quartz and quartz-adularia-carbonate veins within a large volcanotectonic structure
(Sakharova et al., 1984). The Uzbekistan goldfieldite was found in a deposit con-
sidered as relatively rich in sulphides in view of the shallow depth of its formation
(Tsepin et al., 1977). It is intimately intergrown with tetrahedrite, stannoluzonite,
stibioluzonite, stannite, chalcopyrite, pyrite, Au-Ag-tellurides, and native gold
(Tsepin et al., 1977). At Goldfeld, goldfieldite occurs together with pyrite, marcasite,
sphalerite, wurzite, tennantite, famatinite, bismuthinite, petzite, hessite, sylvanite,
and native gold (Tolman and Ambrose, 1934). Microphotographs (Tolman and
152 U. Knittel

Ambrose, 1934, Figs. 6, 8, 10, 13, 18) show that it is usually intergrown with famatinite
and bismuthinite (which were deposited prior to goldfieldite) and native gold and
Au-Ag-tellurides (deposited after goldfieldite).
At Butte native gold and a goldfieldite resembling that from the Marian Deposit
occur, but no other Te-bearing minerals have been found (Meyer et al., 1968);
colusite from Butte, which has been considered to contain Te (Meyer et al., 1968,
Tab. 1), does not contain Te according to microprobe analyses of Springer (1969).
Interestingly, both the Marian deposit and the vein system at Butte are associated
with porphyry copper mineralization (Baquiran, 1975; Sillitoe, 1979; Knittel,
1982; Meyer et al., 1968). The tellurian tennatite from the Lesser Caucasus,
which closely resembles that from the Marian mineralization, occurs in an
enargite-rich massive sulfide deposit (Loginov et al., 1983). The goldfieldite
from Sardinia, which is also associated with a Cu-deposit (a subvolcanic
epithermal copper-arsenic deposit, Frenzel et al., 1975), however, is Sb rich.
For the occurrences from Kamchatka and Uzbekistan it is not known whether
they are associated with copper mineralization but from the description it might
be inferred that at least the Kamchatka deposit resembles the Emporer Mine
in Fiji or the Goldfield deposits in its structural setting in the caldera of a young
volcano.
The deposits at Goldfield are associated with intermediate to silicic members of
a relatively potassic calc-alkaline suite (Ashley and Silberman, 1976). The deposits
in Kamchatka and Sardinia are likewise hosted by intermediate to silicic calc-
alkaline volcanics (Sakharova et al., 1984; Frenzel et al., 1975). The Butte mineraliza-
tion is related to the quartz monzonite of the Boulder Batholith (Meyer et al., 1968).
Goldfieldite has previously not been reported from any of the precious metal
deposits associated with alkaline rocks, though ores associated with alkaline rocks
tend to be Te-rich (Mutschler et al., 1985).
In summary, it appears that goldfieldite occurs principally in polymetallic,
mineralogically complex ores. It is commonly associated with sulphides, Au-Ag-
tellurides and native gold. Sakharova et al. (1984) suggested that goldfieldite
"may be regarded as typomorphic of gold-telluride deposits localized in volcanic
regions". The available data may be interpreted to indicate that arsenian gold-
fieldite (or tellurian tennatite) is more common in polymetallic Cu-mineralizations
(the occurrence in Sardinia would be an exception), while Sb-rich goldfieldite
and tellurian tetrahedrite seem to be prevalent in base metal poor previous metal
deposits.

Acknowledgements

I wish to thank W. W. Brown for the permission to collect ore samples from the
Marian Gold Mine, G. Friedrich for the use the electron microprobe at the Institut
fiir Mineralogie und Lagerstfittenlehre der RWTH Aachen, A. Wiechowski and
G. Thiele for help with the microprobe analyses, N. Archbold and G. Feck, who
helped to obtain relevant literature and A. Cundari, B. Birch, and two anonymous
reviewers (in particular the one who undertook it to recalculate the mineral formulae
and found the error in Table 1) for comments on an earlier draft, which helped to
improve the manuscript.
 Composition and Association of Arsenian Goldfieldite 153

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Author's address: Dr. U. Knittel, Department of Geology, University of Melbourne,

Parkville, Victoria 3052, Australia.

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