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Formation of a hydrothermal kaolinite deposit from rhyolitic tuff in Jiangxi,

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Article in Journal of Earth Science · June 2014

DOI: 10.1007/s12583-014-0439-1

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Journal of Earth Science, Vol. 25, No. 3, p. 495–505, June 2014 ISSN 1674-487X
Printed in China
DOI: 10.1007/s12583-014-0439-1

Formation of a Hydrothermal Kaolinite Deposit from

Rhyolitic Tuff in Jiangxi, China
Ye Yuan*1, 2, Guanghai Shi1, Mengchu Yang1, Yinuo Wu1, Zhaochong Zhang1, Anjie Huang3, Jiajing Zhang2
1. State Key Laboratory of Geological Processes and Mineral Resources, China University of Geosciences, Beijing 100083, China
2. Geological Survey of Jiangxi Province, Nanchang 330030, China
3. Northeast Geological department of Jiangxi Geological Exploration Bureau, Shangrao 334000, China

ABSTRACT: The Longmen kaolinite deposit is one of the largest hydrothermal clay deposits of Ganxi
volcanic basin (northern Wuyi Mountain area, China). The pristine host rocks are rhyolitic
crystal-vitric tuff and minor lapilli tuff from the Late Jurassic Ehuling Formation. The ore consists of
kaolin-group minerals (kaolinite, dickite), pyrophyllite with minor quartz, sericite, pyrite, etc.. From
the host rocks to the transition zones (altered rocks) then to the vein ores, contents of SiO2 and TFe2O3
decrease, whereas Al2O3 and LOI increase, consistent with the contents increase of kaolin minerals and
pyrophyllite in the samples. The total REE abundances of the ores are much lower than that of the host
and altered rocks, Rb, Nb, Nd, Zr, Ti and Y are significantly depleted. Apparent zoning features of bulk
geochemistry and mineral component reflect that the kaolinite deposit occurred at the expense of the
host rock by ascending hydrothermal fluids with distinct removal of SiO2, TFe2O3, Na2O, K2O.
According to the mineral assemblage, the formation temperature of this deposit falls within the range
of 270–350 ℃. With regard to the industrial applications, the kaolinized ores are suitable for use in
ceramics and gemologic materials crafted for seal stones. Moreover, in mineralogical terms, this deposit
is also proved to be an excellent example for studying channeled hydrothermal alterations of rhyolitic
tuff.
KEY WORDS: China, geochemistry, hydrothermal alteration, Jiangxi, kaolinite, pyrophyllite.

1 INTRODUCTION produced one through many aspects such as geological features,

Volcanic rocks, especially those glass-rich types, are not mineralogical assemblages, chemical composition, zonal
stable under ambient conditions, and will transform into silicification and occurrence of Fe-oxide/hydroxide- and
secondary phases that are more thermodynamically stable. S-bearing phases, micromorphology of the clay and coexisting
Under conditions of short-lived alteration at low pressures non-clay minerals, and stable-isotope and fluid-inclusion
and/or low temperatures, common secondary minerals are characteristics (e.g., Erkoyun and Kadir, 2011; Simeone et al.,
glass-like or as poorly crystallized phases (Kawano and Tomita, 2005; Gilg et al., 2003, 1999; Boulvais et al., 2000; Sheppard
1997; Crovisier et al., 1992; Magonthier et al., 1992). At higher and Gilg, 1996; Marumo et al., 1980). However, hydrothermal
temperatures and for longer periods, phases with greater alterations of rhyolitic tuff do not always lead to formation of
crystallinity such as smectite and zeolite occur. For instance, kaolinite; pyrophyllite and smectite are more common due to
basaltic glass favors the formation of saponite; alkali-bearing the differences in fresh parent rock composition and
tuff prefers the formation of zeolite, while hydrothermal physicochemical conditions of mineralization (Simeone et al.,
solution of granitic composition favored smectite formation 2005).
(Banfield and Barker, 1998). Halloysite and kaolinite dominate Recently a new kaolinite deposit has been found in
in a condition of humid soil formed from volcanic ash and Longmen, Jiangxi province. The deposit occurs in the Upper
pumice (Wada, 1987). Thus, the varieties of secondary phases Jurassic volcanic rocks. Field observations reveal an obvious
depend on chemical composition, texture of the rocks and zonal structure, which is preliminarily regarded as a
physicochemical conditions of the surroundings (Garcίa- hydrothermal alteration deposit. About this deposit, however,
Romero et al., 2005; De La Fuente et al., 2000). there is less information about mineralogical and chemical
Hydrothermal kaolinite are distinguished from weathering- features, structure of alteration zoning, petrogenesis, quality
evaluation and, eventually, potential utilization. In this paper, the
*Corresponding author: yuenyeah@163.com bulk chemical and mineralogical features, zonal characteristics
© China University of Geosciences and Springer-Verlag Berlin are described, while formation of the deposit and some possible
Heidelberg 2014 utilizations of the deposit are discussed.

Manuscript received June 17, 2013. 2 GEOLOGICAL SETTING AND SAMPLING

Manuscript accepted September 12, 2013. The Longmen deposit is situated at ~66 km SE of

Yuan, Y., Shi, G. H., Yang, M. C., et al., 2014. Formation of a Hydrothermal Kaolinite Deposit from Rhyolitic Tuff in Jiangxi, China.
Journal of Earth Science, 25(3): 495–505, doi:10.1007/s12583-014-0439-1
496 Ye Yuan, Guanghai Shi, Mengchu Yang, Yinuo Wu, Zhaochong Zhang, Anjie Huang and Jiajing Zhang

Shangrao City, Jiangxi Province, China (118°05'32"E, at the Institute of Geology and Geophysics, Chinese Academy
28°06'35"N, GPS sampling position), at the north of the Wuyi of Sciences (IGGCAS). Analyses were performed under an
uplift area, on the western margin of Ganxi volcanic basin (Fig. operating voltage of 15 kV, a beam current of 10 nA and a spot
1). The strata in the area mainly consist of the Linshan size less than 10 μm. EPMA standards include the following
Formation (Lower Jurassic) and the Ehuling Formation (Upper minerals: andradite for Si and Ca, rutile for Ti, corundum for Al,
Jurassic). The latter hosts this hydrothermal kaolinite deposit, hematite for Fe, eskolaite for Cr, rhodonite for Mn, bunsenite
along with some Mo, Cu, Pb, Zn mining deposits as well for Ni, periclase for Mg, albite for Na, K-feldspar for K, and
(Zhang et al., 2009a, b). The strata in Longmen mining area are barite for Ba (Shi et al., 2010) and the results are listed in Table
part of the Middle-Upper Ehuling Formation. The middle part 1. The ore samples was additionally analyzed using a Rigaku
consists of the rhyolitic crystal-vitric tuff and altered rocks, and D/MAX-RC X-ray diffraction (XRD) at China University of
the upper part contains tuffaceous mudstone and crystal-vitric Geosciences (CUGB), with Cu-K radiation of wavelength
tuff breccias. N-E faults and N-W faults occur in the mining λ=1.540 6 Å and a graphite monochromator operated at 30 kV
area, along which small late-stage dykes, such as felsites, sillite, and 110 mA.
and quartz dykes, appear. The ore bodies, mostly as vein or Twelve samples selected were analyzed for bulk-rock
vein-like structures, occur in the altered rocks which is closely chemical compositions. Major elements were determined by
related to the fault (Fig. 2a), and shows obvious zoning in terms X-ray fluorescence spectroscopy (XRF) using a Phillips
of color and texture (Fig. 2b). Samples were collected from a PW2400 system at the IGGCAS. Fused glass discs were used
section of the Middle Ehuling Formation including and the analytical precision is better than 5%, as estimated from
crystal-vitric tuffs (LM01–LM06), altered rocks in the repeat analyses of GSR-3 (basalt, Chinese standard reference
transition zones (LM07–LM14) and the ores (LM15–LM23). materials; see Shi et al., 2008a). Trace elements were analyzed
using a VG-PQII inductively coupled plasma-mass spectrometry
3 METHODS (ICP-MS) at the IGGCAS. Precision for most trace elements is
A petrographic and mineralogical study of representative better than 5%, as determined by analyses of the GSR-3
samples from the different alteration zones was carried out. An standard (see Shi et al., 2008b; Tang et al., 2006). Major, trace
Olympus BX51 polarization microscope with a bulit-in and REE compositions are given in Table 2.
Olympus DP72 video camera and Image-Pro Plus image
processing software were used. Back-scattered electron (BSE) 4 PETROGRAPHY
images and chemical compositions of minerals in the samples The pristine host rock is rhyolitic welded tuff with incanus,
were obtained using a CAMECA-SX-51 electronic microprobe pale green and gray purplish red in color, and is composed of

Figure 1. Simplified geological map of the Longmen area.

Formation of a Hydrothermal Kaolinite Deposit from Rhyolitic Tuff in Jiangxi, China 497

Figure 2. Field images of Longmen kaolinite-pyrophyllite deposit. (a) Vein or vein-like ore body in the host tuff (length of the
picture ~30 m); (b) obvious color and texture zoning; (c) ore of high quality (sample LM19).

crystal fragments and matrix. The crystal fragments are tabular 5 MINERALOGIC COMPONENTS OF ORES
feldspar and granular quartz with 0.1 to 2.0 mm in length; on The XRD and EMPA results are given in Fig. 4 and Table
the other hand, the matrix comprises tiny grains (D<0.05 mm 1. Measurements byXRD reveal that kaolin minerals (kaolinite,
mostly) of feldspar, quartz, lithic dusts and glass (Fig. 3a). The dickite), pyrophyllite and minor quartz, sericite and hematite
transition zone contains altered rock in light grey to light occur in the ores. Kaolinite and pyrophyllite were characterized
greenish, with mineral components of kaolinite, quartz, by the (001) basal reflections at 7.20 and 9.26 Å, respectively,
pyrophyllite and sericite. Feldspar pseudomorph filled with and they are the prevalent clay minerals in other five analyzed
quartz+kaolinite (Fig. 3b), which reflects that alteration samples except one sample LM19 which nearly consists of
occurred within the surrounding tuff. Width of the zone varies dickite. When kaolinite and dickite are associated, it is not easy
greatly (from several mm to several cm) and boundary of the to differentiate them. Although some reflections overlap others,
host is distinct (Fig. 3c). The ores consist of micro- to kaolin polytypes can be differentiated by XRD patterns in the
crypto-crystalline kaolinite and pyrophyllite (<50 μm in length) range 18°–40° 2θ, the reflections at 3.95, 3.79, 3.43, 3.26, 2.94,
(Fig. 3d) with light grey, light yellow, light green in color, and 2.80, 2.32 and 2.21 Å are diagnostic of dickite (Bailey, 1980).
are characterized by massive structures with lepidoblastic The XRD result of sample LM15 indicates the presence of both
textures (Fig. 2c). Other minor minerals like sericite, diaspore kaolinite and dickite polytypes. According to measurement of
and pyrite also occur. Later-stage diaspore has a length of less crystallinity index by Hinckley (1963), the Hinckley index of
than 0.5 mm cutting through pyrophyllite aggregate. the kaolinites vary from 0.33 to 0.94, falling to a moderately
ordered domain with a few stacking fault. The EMPA results
reveal that the chemical compositions of kaolin minerals lie in
498 Ye Yuan, Guanghai Shi, Mengchu Yang, Yinuo Wu, Zhaochong Zhang, Anjie Huang and Jiajing Zhang

the range of its stoichiometric compositions, in which the wt.%–2.66 wt.% TFe2O3, 0.06 wt.%–0.22 wt.% CaO, 0.08
content of Si varies from 1.99 to 2.04 and octahedral Al shows wt.%–0.15 wt.% Na2O and 0.05 wt.%–0.32 wt.% K2O, 10.13
a range from 1.92 to 2.00. Two kinds of pyrophyllite polytype wt.%–14.53 wt.% LOI.
are identified according to the XRD patterns: two-layered The tuffs have seagull-shaped chondrite-normalized REE
monoclinic (2M) and one-layered triclinic (1Tc), and they pattern (Fig. 6) with obvious negative Eu anomaly
coexist in most of the ores (Brindley and Wardle, 1970). (δEu=0.27–0.31). Their total REE abundances of 233 ppm–
Sericite and quartz are identified both by EPMA and XRD, 336 ppm are higher than the adjacent tuffs of the same Erhuling
whereas diaspore is identified by EPMA (only Al detected) and Formation in Xujiadun, which show geochemical features of
crystal shape. Pyrite is confirmed from its chemical Type-A granite (Zhang et al., 2009a). However, their
composition and crystal shape, only Fe and S are detected by LREE/HREE ratios of 5.58–8.85, [La/Yb]N ratios of
energy-dispersive spectroscopy attached to the EMPA. 14.64–32.60, and [Gd/Lu]N ratios of 1.53–2.47 are higher than
those from Xujiadun, except for the similar [La/Sm]N ratios of
6 GEOCHEMICAL CHARACTERISTICS 3.17–8.72. Their contents of trace elements, such as Rb, Ba, Th,
The host tuffs have 68.02 wt.%–75.66 wt.% SiO2, 13.20 Zr, are slightly high (Fig. 7).
wt.% to 15.94 wt.% Al2O3, and 1.03 wt.% to 2.89 wt.% The altered rocks in the transition zone show almost the
Na2O+K2O (Table 2). All loss on ignition (LOI) values of the same pattern as the tuffs. Negative Eu anomaly (δEu=0.17–0.28)
four samples are high (3.94 wt.%–10.76 wt.%), possibly due to is measured. Total REE abundances are 231 ppm–1 003 ppm;
the later alteration. On a plot of total alkali content versus silica LREE/HREE ratios at 3.05–14.17, [La/Yb]N ratios at 11.6–102,
(LeBas et al., 1986), samples LM04, LM05 are rhyolite; LM03 [Gd/Lu]N ratios at 1.48–11.07, and [La/Sm]N ratios at
stands along the boundary between rhyolite and dacite; LM02 5.18–9.35.
with highest LOI falls into dacite area (Fig. 5). The kaolin belt have total REE abundances of 60
The transitional altered rocks have 63.82 wt.%–70.25 wt.% ppm–266 ppm, their LREE/HREE ratios are at 19.77–39.89,
SiO2, 1.11 wt.%–2.74 wt.% TFe2O3, 0.07 wt.%–0.13 wt.% CaO, [La/Yb]N rations at 281–554, [Gd/Lu]N ratios at 7.32–21.5,
0.10 wt.%–0.21 wt.% Na2O and 0.60 wt.%–4.53 wt.% K2O, [La/Sm]N ratios at 8.05–24.03. The contents of trace elements
19.36 wt.%–24.96 wt.% Al2O3, 4.10 wt.%–8.13 wt.% LOI. The like Rb, K, Nb, La, Ce, Zr, Ti, Y are the lowest among all
ores have lowest SiO2 ranging of 45.72 wt.%–54.11 wt.%, samples.
highest Al2O3 ranging of 32.16 wt.%–39.64 wt.%, 0.08

Figure 3. Photomicrographs and backscattered electron (BSE) images of the studied samples. (a) Tabular feldspar and
granular quartz (LM04); (b) kaolinite in a feldspar pseudomorph (LM10); (c) transition boundary between the host rock and
the ore (LM09); (d) fine-grained texture of the ore (LM17). Qtz. Quartz; Kfs. K-feldspar; Py. pyrite; Kln. kaolinite; Ser.
sericite; Prl. pyrophyllite; Tuf. tuff; abbreviations according to Bucher and Grapes (2011).
Formation of a Hydrothermal Kaolinite Deposit from Rhyolitic Tuff in Jiangxi, China 499

Table 1 Chemical composition (wt.%) of kaolin minerals, pyrophyllite and sericite of the ore from the
Longmen kaolinite-pyrophyllite deposit

Kaolin minerals Pyrophyllite Sericite Diaspore

Sample LM15 LM16 LM17 LM19 LM20 LM21 LM22 LM15 LM16 LM17 LM15 LM17 LM17
SiO2 47.21 46.02 46.98 45.58 46.37 46.41 45.33 64.61 66.22 65.51 48.12 51.17 0.43
Al2O3 38.01 37.17 37.18 38.76 38.56 38.42 38.44 28.51 27.07 27.65 34.04 32.56 78.97
TiO2 0.02 0.00 0.00 0.02 0.00 0.00 0.05 0.04 0.01 0.00 0.04 0.01 0.05
Cr2O3 0.03 0.04 0.06 0.04 0.04 0.00 0.07 0.03 0.02 0.00 0.00 0.04 0.04
FeO 0.16 0.03 0.00 0.04 0.02 0.02 0.04 0.26 0.15 0.06 0.03 0.78 0.03
MgO 0.00 0.00 0.00 0.02 0.00 0.00 0.00 0.00 0.02 0.00 0.00 0.04 0.01
MnO 0.00 0.02 0.00 0.00 0.00 0.00 0.00 0.00 0.01 0.00 0.00 0.00 0.02
CaO 0.09 0.04 0.06 0.02 0.02 0.00 0.06 0.08 0.03 0.04 0.00 0.03 0.00
Na2O 0.06 0.00 0.05 0.14 0.04 0.03 0.01 0.14 0.11 0.17 0.09 0.14 0.03
K2O 0.08 0.00 0.01 0.16 0.04 0.02 0.14 1.50 0.25 0.06 8.67 7.57 0.14
Total 85.66 83.32 84.34 84.80 85.09 84.90 84.14 95.17 93.89 93.49 90.99 92.34 79.72
Si 2.04 2.04 2.06 1.99 2.02 2.02 2.00 3.92 4.03 4.00 3.27 3.40
IV
Al 0.00 0.00 0.00 0.01 0.00 0.00 0.00 0.08 0.00 0.00 0.73 0.60
VI
Al 1.94 1.94 1.92 2.00 1.98 1.97 1.99 1.96 1.94 1.99 1.99 1.94
Ti 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00
Cr 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00
Fe2+ 0.01 0.00 0.00 0.00 0.00 0.00 0.00 0.01 0.01 0.00 0.00 0.04
Mg 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00
Mn 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00 0.00
Ca 0.00 0.00 0.00 0.00 0.00 0.00 0.01 0.01 0.00 0.00 0.00 0.00
Na 0.01 0.00 0.00 0.02 0.01 0.01 0.00 0.02 0.01 0.02 0.01 0.02
K 0.00 0.00 0.00 0.02 0.00 0.00 0.02 0.12 0.02 0.00 0.75 0.64
∑cat 4.00 3.98 3.98 4.04 4.01 4.00 4.02 6.12 6.01 6.01 6.75 6.64

The kaolin minerals formulae were calculated on the basis of seven oxygens, the pyrophyllite formulae were calculated on the basis
of eleven oxygens and the muscovite were normalized on the basis of fixed anions. Total Fe assumed as ferrous.

7 DISCUSSION homogeneous removal of the REE. As for the trace elements,

Chemical compositions from the tuffs and the ores are significantly depleted of Rb, Nb, Nd, Zr, Ti and Y,
transitional altered rocks to the kaolin veins show systematic reflecting their corresponding removal during kaolin
changes of hydrothermal alterations of rhyolitic tuff. From the formation from the tuff, which may have further geochemical
hosting tuffs to the ores, average contents of SiO2 and TFe2O3 implications.
decrease (SiO2 at 74.10 wt.%→66.99 wt.%→48.83 wt.%, Mineral components of the Longmen kaolin deposit also
TFe2O3 at 2.42 wt.%→1.73 wt.%→0.81 wt.%), whereas the suggest that the ore and related rocks could be used as a good
average contents of Al2O3 and LOI increase (Al2O3 at 14.70 example for studying alterations of rhyolitic tuff. The major
wt.%→22.34 wt.%→37.41 wt.%, LOI at 6.01 wt.%→5.36 mineral components of the ores are kaolinite group with more
wt.%→12.92 wt.%) (Fig. 8). Such changes in composition or less pyrophyllite. From the pristine host rocks to the
reflect a significant removal of SiO2 and Fe2O3, impregnation transitional altered rocks and then the ore core, the contents of
of fluids (equivalence of LOI), and concentration of Al2O3. SiO2 decrease while the contents of Al2O3 increase, consistent
Accordingly, average LREE/HREE ratios (7.36–11.45–29.88) with contents increase of kaolinite (dickite). An apparent
and average (La/Yb)N ratios (25.26–61.98–363.22) increase removal of K, Na and Ca, together with Fe and Mg, suggest an
from the hosting tuff towards the ore, suggesting a gradual open system for hydrothermal solution-involved metasomatism
increase of REE fractionation degree during alteration. Total for kaolinite (dickite) occurrence at the expense of the tuff. The
REE abundances of the tuffs and the altered transition rocks hydrothermal solution is inferred to be an acidic one as
(average=287.36 ppm and 438.42 ppm, respectively) relative suggested by Kadir et al. (2011). Occurrence of altered
to those of the ores (average=143.08 ppm) also show minerals can be deduced through the following reactions
significant removal of REE possibly gone with the removal of commonly acknowledged by other previous researchers (e.g.,
SiO2. Similar chondrite-normalized REE patterns (Fig. 6) Bottrill, 1998; Hemley and Jones, 1964). Normally, sericite is
may suggest an inherited connection between the ores, the an intermediate phase from feldspar to kaolinite and
altered rocks and the fresh parent rocks, and a nearly pyrophyllite, as revealed by reactions (1), (2), (3) and (4).

3K[AlSi3O8]+2H+→KAl2 [AlSi3O10](OH) 2+6SiO2+2K+ (1)

K-feldspar Sericite
500 Ye Yuan, Guanghai Shi, Mengchu Yang, Yinuo Wu, Zhaochong Zhang, Anjie Huang and Jiajing Zhang

Table 2 Major element (wt.%), trace and REE elements (ppm) contents of the samples from the Longmen deposit

Rock Crystal-vitric tuffs Transitional altered rocks Ores

Sample LM02 LM03 LM04 LM05 LM07 LM09 LM10 LM11 LM15 LM16 LM19 LM20
SiO2 68.02 72.33 75.66 74.40 63.82 69.55 70.25 64.35 54.11 48.22 45.72 47.27
TiO2 0.36 0.32 0.30 0.34 0.24 0.21 0.28 0.49 0.12 0.03 0.02 0.03
Al2O3 15.34 14.31 13.20 15.94 24.96 19.36 20.24 24.78 32.16 38.69 39.64 39.14
TFe2O3 2.92 0.88 3.91 1.95 1.60 2.74 1.11 1.48 2.66 0.08 0.15 0.35
MnO 0.02 0.00 0.02 0.01 0.01 0.01 0.01 0.01 0.01 0.00 0.00 0.00
MgO 0.18 0.27 0.18 0.06 0.01 0.09 0.02 0.06 0.13 0.00 0.00 0.00
CaO 0.17 0.15 0.34 0.10 0.07 0.11 0.13 0.08 0.22 0.05 0.06 0.09
Na2O 0.26 0.12 0.13 0.16 0.10 0.17 0.15 0.21 0.15 0.08 0.07 0.08
K2O 2.48 0.91 0.94 2.73 0.60 3.29 2.26 4.53 0.32 0.07 0.05 0.07
P2O5 0.07 0.09 0.09 0.12 0.11 0.07 0.34 0.08 0.13 0.20 0.20 0.14
LOI 10.76 4.42 4.94 3.94 8.13 4.22 5.00 4.10 10.13 13.29 14.53 13.71
Total 100.59 99.79 99.71 99.74 99.65 99.82 99.79 100.16 100.15 100.71 100.44 100.88
Alk 2.74 1.03 1.07 2.89 0.70 3.46 2.41 4.74 0.47 0.15 0.12 0.15
Sc 5.48 3.67 4.78 4.09 2.23 4.37 1.96 4.03 2.18 1.33 1.01 3.37
V 22.56 22.51 22.85 23.11 38.49 30.21 30.00 42.34 37.95 31.37 59.26 81.77
Cr 51.42 21.12 36.02 8.06 20.47 12.79 15.00 8.28 15.97 8.83 10.98 10.48
Co 2.55 2.08 2.96 1.70 1.55 2.54 1.36 1.33 2.46 0.83 0.99 0.96
Ni 11.89 22.41 19.55 1.33 4.11 1.79 5.91 2.63 6.25 2.57 3.55 5.67
Rb 39.58 32.48 26.77 102.34 20.97 134.98 83.37 202.00 5.44 0.70 0.39 1.10
Ga 22.09 18.28 14.82 19.53 24.70 25.28 25.29 56.92 44.95 25.62 40.81 33.46
Ba 347.03 89.32 98.15 382.22 20.91 59.29 97.49 30.48 39.45 37.28 40.42 190.86
Th 29.37 27.32 23.71 31.62 38.07 23.26 43.19 27.56 38.58 10.11 10.94 7.50
U 4.08 4.17 4.16 5.69 2.83 2.93 4.56 7.62 1.31 0.70 0.54 0.38
Ta 1.67 1.69 1.40 1.79 1.33 1.09 1.28 2.75 0.51 0.15 0.09 0.09
Pb 121.13 40.81 91.75 32.69 67.09 65.93 85.28 55.67 140.32 74.67 76.50 50.33
Nb 21.54 22.02 18.77 21.71 16.88 13.23 18.54 33.92 8.22 2.65 1.82 1.69
Sr 206.00 185.46 301.16 159.21 195.12 226.87 581.12 214.27 357.81 434.78 372.53 385.30
Y 14.41. 11.26 24.02 11.66 6.83 5.31 11.90 37.40 2.12 0.34 0.44 0.71
Zr 257.50 258.96 231.13 259.42 201.88 160.38 206.70 403.12 97.97 17.54 23.03 12.66
Hf 7.91 7.81 6.94 7.96 6.31 4.66 6.47 13.07 3.02 0.57 0.63 0.36
Zr/Hf 32.55 33.16 33.30 32.59 31.99 34.42 31.95 30.84 32.44 30.77 34.97 35.17
La 71.27 54.77 55.60 73.84 62.60 63.22 196.39 54.29 112.01 23.84 17.53 20.58
Ce 122.49 114.04 139.60 145.25 119.50 109.69 506.09 99.73 194.57 31.76 45.80 44.65
Pr 11.92 9.23 17.75 13.89 11.58 9.52 54.18 9.55 11.43 0.77 1.99 2.72
Nd 39.20 27.98 67.69 41.37 38.06 33.39 185.24 34.40 28.51 1.96 6.74 9.40
Sm 5.96 4.67 11.04 5.33 6.28 4.25 22.20 6.60 3.49 0.62 0.83 1.61
Eu 0.44 0.44 0.94 0.48 0.41 0.32 1.83 0.34 0.27 0.08 0.05 0.16
Gd 3.57 4.20 7.05 4.54 3.90 3.05 16.12 5.47 2.78 0.67 0.36 1.14
Tb 0.45 0.50 0.88 0.51 0.35 0.27 1.25 1.21 0.20 0.06 0.04 0.10
Dy 2.58 2.40 4.63 2.48 1.46 1.10 3.88 7.72 0.55 0.13 0.11 0.22
Ho 0.55 0.48 0.93 0.50 0.27 0.20 0.59 1.53 0.09 0.02 0.02 0.03
Er 1.75 1.35 2.62 1.45 0.75 0.60 1.55 3.84 0.23 0.04 0.05 0.07
Tm 0.28 0.20 0.40 0.23 0.11 0.10 0.21 0.53 0.04 0.01 0.01 0.01
Yb 1.83 1.34 2.56 1.53 0.65 0.62 1.29 3.16 0.23 0.03 0.04 0.05
Lu 0.29 0.21 0.40 0.24 0.10 0.09 0.18 0.46 0.04 0.00 0.01 0.01
∑REE 276.98 233.06 336.11 303.31 252.83 231.72 1002.90 266.23 356.54 60.32 74.00 81.45
LREE/HREE 7.92 7.10 5.58 8.85 12.53 14.17 16.03 3.05 34.38 25.49 39.89 19.77
Eu/Eu* 0.27 0.30 0.31 0.29 0.24 0.26 0.28 0.17 0.26 0.35 0.23 0.34
[La/Yb]N 26.21 27.20 14.64 32.60 64.54 69.31 102.48 11.58 328.33 554.12 281.33 289.09
[La/Sm]N 7.53 7.37 3.17 8.72 6.28 9.35 5.56 5.18 20.19 24.03 13.33 8.05
[Gd/Lu]N 1.53 2.47 2.22 2.32 5.10 4.03 11.07 1.48 9.60 21.50 7.32 18.42
Formation of a Hydrothermal Kaolinite Deposit from Rhyolitic Tuff in Jiangxi, China 501

Intensity (×10 3 cps) 4 K LM15 K K LM16

15
3
K

P
2 P P1 10
P1
P D Q KP
1 K K K 5
K
D H KP K P P
P KKK
K KK P 1 K K K
P 1K P 2 KK K KKKK
0 10 20 30 40 50 60
0
15 P LM17 D D LM19
P 10
Intensity (×10 3 cps)

8
10
6
K P
K
4
5
P2 2 DD D
M P 2P Q K PK K DD D D
M 2
K KK PP K
P K K K K P D D D D D D D
0 0
P
10 20 30 40 50 60

LM21
10
K 20 30 40 50 60
LM22
P
6
7.5 K
Intensity (×10 3 cps)

5
4 P
5.0 P P
3
M P1 M
P1 M 2 M P K
2.5 P K K
K M P 1 PK P P P P 1 M P1 K P2 P2 K K K K
P P2 2 P P P PP P M P K P PK K K P
M
0 0
10 20 30 40 50 60 10 20 30 40 50 60
2θ (degree) 2θ (degree)

Figure 4. X-ray diffraction patterns of the ores of LM15, LM16, LM17, LM19, LM21 and LM22 (P1. two-layered monoclinic
pyrophyllite; P2. one-layered triclinic pyrophyllite; K. kaolinite; D. dickite, Q. quartz; H. hematite; M. muscovite).

1 000 Tuffs
Transitional altered rocks
Sample/chondrite

16 100 Ores

LM02
14 LM03-LM05 10

1
12
Trachyte

0.1
La Ce Pr Nd Sm Eu Gd Tb Dy Ho Er Tm Yb Lu
10
Na2O+K2O (wt.%)

Figure 6. Chondrite-normalized REE diagrams for rocks

8 and ores from the deposit. Chondrite normalization values
are from Sun and McDonough (1989).
Rhyolite
6 1 000
Sample/primitive mantle

100
4 Dacite

10
2
1
0 Tuffs
65 70 75 80 85 0.1 Transitional altered rocks
Ores
SiO 2(wt.%)
Rb Ba Th K Nb La Ce Sr Nd P Zr Ga Sm Ti Y Yb
Figure 5. Total alkali content versus silica plot (after LeBas
et al., 1986) of the tuff. Figure 7. Primitive mantle-normalized trace element
diagrams for rocks and ores from the Longmen deposit.
Normalization values from Sun and McDonough (1989).
502 Ye Yuan, Guanghai Shi, Mengchu Yang, Yinuo Wu, Zhaochong Zhang, Anjie Huang and Jiajing Zhang

3(Na, Ca) [AlSi3O8]+K++2H+→KAl2[AlSi3O10](OH)2+6SiO2+3(Na+, Ca2+) (2)

Plagioclase Sericite

2KAl2[AlSi3O10](OH)2+2H++3H2O→3Al2Si2O5(OH)4+2K+ (3)
Sericite Kaolinite

4KAl2[AlSi3O10](OH)2+4H+→ 3Al2Si4O10(OH)2+6AlO(OH)+4K+ (4)

Sericite Pyrophyllite Diaspore

The above reactions involve a significant removal of SiO2, from feldspar via reaction (5), also with significant removal of
which is in consistent with our geochemical observations in SiO2. With SiO2, kaolinite could be transformed into
EMPA data. Alternatively, kaolinite could be formed directly pyrophyllite through reaction (6) with increasing temperature.

2NaAlSi3O8+H2O+2H+→Al2Si2O5(OH)4+4SiO2+2Na+ (5)
Plagioclase Kaolinite

Al2Si2O5(OH)4+2SiO2↔Al2Si4O10(OH)2+H2O (6)
Kaolinite Pyrophyllite

90 50
80 40
w(Al 2O 3) (%)
w(SiO 2) (%)

70 30

60 20

50 10
40 0
0.30 5
0.25 4
w(Na 2O) (%)

w(K 2O) (%)

0.20
3
0.15
2
0.10
1
0.05
0.00 0
0.30 0.40
0.25
0.30
w(MgO) (%)

w(CaO) (%)

0.20
0.15 0.20
0.10
0.10
0.05
0.00 0.00
0.50 20
0.40
15
w(TiO 2) (%)

w(LOI) (%)

0.30
10
0.20

0.10 5

0.00 0
0 2 0 3 0 4 0 5 0 7 0 9 1 0 11 1 5 1 6 1 9 2 0 0 2 0 3 0 4 0 5 0 7 0 9 1 0 11 1 5 1 6 1 9 2 0
LM LM LM LM LM LM LM LM LM LM LM LM LM LM LM LM LM LM LM LM LM LM LM LM

Figure 8. Plot showing variations of chemical compositions from the pristine host rocks to the ores (pristine host rocks
LM02–LM05, transitional altered rocks LM07 and LM09–LM11, ores LM15, LM16, LM19 and LM20).
Formation of a Hydrothermal Kaolinite Deposit from Rhyolitic Tuff in Jiangxi, China 503

Presence of sericite aggregate attached to the pristine rock are rare in China, the quality of this ore studied is high, which
(Fig. 3c) in this investigation suggests that feldspars in the is suitable for carving. Other four famous kaolinite deposits in
pristine rock, both K-feldspar and plagioclase, could be altered China include Shoushan (Fujian Province), Changhua
to form sericite at the presence of acidic solution following the (Zhejiang Province), Balin (Inner Mongolia) and Qingtian
reactions (1) and (2). K+ removed through reaction (1) could be (Zhejiang Province) (Gao and Di, 2010; Zhu, 2010; Chen et al.,
reactants for reaction (2). Further removal of K+ of sericite 2009; Wu and Cui, 1999). Each of the four deposits has a long
would lead to formation of kaolinite through reaction (3), and mining history of more than one hundred years, among which
would also produce pyrophillite through reaction (4) at higher the Shoushan stone has been mined since Song Dynasty, for
temperature than kaolinite at the same pressure (e.g., Hemley et more than 1 500 years. In this point, hydrothermal kaolin
al., 1980). A common occurrence of kaolinite in association deposit is of potential gemological significance.
with pyrophyllite in present investigation suggests occurrence
temperatures had been slightly higher than pure kaolinite 8 CONCLUSIONS
deposit for sometime (e.g., Kadir et al., 2011). Similarly, The Longmen kaolinite deposit is one of the largest
production of SiO2 formed by reactions (1), (2) and (5), hydrothermal clay deposits of Ganxi volcanic basin (northern
possibly corresponds to clay-poor Si-rich shell on the top of the Wuyi Mountain area, China). Host rocks of the deposit are
deposits by means of free SiO2 precipitation during or after the rhyolitic crystal-vitric tuff and minor lapilli tuff from the Late
ore forming (Chen et al., 1988). Jurassic Ehuling Formation. Apparent zoning features of bulk
The formation of kaolinite group mineral is often geochemistry and mineral component suggest an open system
observed in the acid alteration; however, the stable phase varies for hydrothermal solution-involved metasomatism for kaolinite
mainly with the varying ambient temperature. At low (dickite) occurrence at the expense of the tuff, and the
temperatures (typically <80 ℃) halloysite may be the preferred formation temperature of this deposit falls within the range of
stable phase. For example, the formation of the Northland 270–350 ℃ according to the mineral assemblage (kaolinite-
halloysite deposits in New Zealand is the result of the dickite-pyrophyllite-diaspore). The high quality ores of this
low-temperature but rapid alteration of glassy rhyolites; the deposit can be used not only for ceramic materials, but also be
volcanic glass has altered to halloysite rather than kaolinite used as carving materials.
(Harvey and Murray, 1993; Murray et al., 1977). Supporting
evidence is that six major halloysite deposits occur through ACKNOWLEDGMENTS
hydrothermal alteration of andesitic rocks in Turkey (Ece et al., The authors are greatly indebted to X J Li and L Chen for
2008; Ece and Schroeder, 2007). At temperatures greater than their kind support during the field work, Q Mao, Y G Ma, X
100 ℃, kaolinite is the preferred stable phase and, at higher Gao, H Li and X D Jin for their helps during the EPMA, XRD,
temperatures, dickite may replace kaolinite or associate with XRF and ICP-MS analysis. This research was supported by the
kaolinite. However, at even higher temperatures, pyrophyllite Innovative Research Team in University (No. B07011), the
will form instead of kaolinite group mineral (Inoue, 1995). Postdoctoral Research Fund of Jiangxi Province, China (No.
Consider that kaolinite, dickite and pyrophyllite occur in this 2013KY48) and the Fundamental Research Funds for the
deposit, their occurrence temperatures are more likely to fit on Central Universities of China (No. 2001YXL048).
the characteristics of an ascending fluid, which in turn agree
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