Construction and Building Materials 147 (2017) 543–549

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Construction and Building Materials

journal homepage: www.elsevier.com/locate/conbuildmat

Investigation on the microstructure and mechanism of geopolymer

with different proportion of quartz and K-feldspar
Linan Tian, Wuwei Feng ⇑, Hongwen Ma ⇑, Shaogang Zhang, Hao Shi
Beijing Key Laboratory of Materials Utilization of Nonmetallic Minerals and Solid Wastes, National Laboratory of Mineral Materials, China University of Geosciences, Beijing
100083, China
School of Materials Science and Technology, China University of Geosciences, Beijing 100083, China

h i g h l i g h t s g r a p h i c a l a b s t r a c t

Effect of the aggregate contents of

quartz and K-feldspar on the
compressive and bending strength is
studied.

Determine the optimum modulus of
alkaline activator at different
proportions of quartz and K-feldspar.

Microstructure and microanalysis of
the region between the aggregate and
matrix are studied.

a r t i c l e i n f o a b s t r a c t

Article history: Geopolymer appears to be an alternative to ordinary Portland cement as a new sustainable material. The
Received 22 October 2016 effect of the aggregate contents of quartz and K-feldspar on the microstructure and mechanical proper-
Received in revised form 30 March 2017 ties of Geopolymer samples was investigated in the present study. It was found that the aggregate
Accepted 12 April 2017
contents influence the compressive strength and bending strength of geopolymeric bricks. Also, The
K-feldspar/quartz mass ratio (F/Q) has a linear relation with the modulus of alkaline activator at the peak
value of bending strength. This is due to the fact that the quartz reacts with the sodium hydroxide and
Keywords:
forms [H2SiO4]2 which is the main component of sodium silicate, and that the K-feldspar has the ability
Geopolymeric brick
Alkaline activator
to provide additional alkaline. The results of electron-microprobe analysis indicated that the matrix
Aggregate phase is composed of more amount of [ASiAOAAlAOASiA]n polymerization monomer with increasing
Strength alkaline activator modulus ratio when K+ is not involved in the reaction. However, the polymerization
Microstructure monomer of [ASiAOAAlA]n was only favored despite of variation of alkaline activator modulus when
the K+ exists.
Ó 2017 Elsevier Ltd. All rights reserved.

1. Introduction

Ordinary Portland cement (OPC) is widely used in construction

materials in the world, which, however, has high emissions of car-
⇑ Corresponding authors at: Beijing Key Laboratory of Materials Utilization of
bon dioxide (CO2) ranging from 0.66 to 0.82 kg per kilogram of OPC
Nonmetallic Minerals and Solid Wastes, National Laboratory of Mineral Materials,
China University of Geosciences, Beijing 100083, China.
manufactured [1–4]. The main causes of CO2 emissions can be
E-mail addresses: wfeng@cugb.edu.cn (W. Feng), mahw@cugb.edu.cn (H. Ma). attributed to: (i) the calcination of the key ingredients, limestone;

http://dx.doi.org/10.1016/j.conbuildmat.2017.04.102
0950-0618/Ó 2017 Elsevier Ltd. All rights reserved.
544 L. Tian et al. / Construction and Building Materials 147 (2017) 543–549

and (ii) the high energy consumption by heating raw materials in a

rotating kiln at above 1400 °C [2]. Besides, significant expansion
and cracking in concrete structures caused by alkali aggregate
reaction (AAR) is one of the main durability problems when OPC
is used in concrete [5].
Disposal of piles of tailings has been a worldwide problem. In
recent years, with the further continuing exploitation of mineral
resources, especially for the mining of low-grade mineral
resources, the amount of tailings rose sharply, which became a
big threat on the ecological environment. Using feldspar and
quartz rich tailings as aggregate to produce building materials
can reduce the production cost of building materials and mean-
while also consume piles of tailings, which realize the comprehen-
sive utilization of resources. The contents of feldspar and quartz in
tailings vary in a large range, and the effect of different contents of
aggregate of feldspar and quartz on the properties of building
material is still unknown.
As a new sustainable material, geopolymer can provide an alter- Fig. 2. X-ray diffraction pattern of the metakaolin.
native to OPC, which is formed by alkali-activated aluminosilicate
materials like metakaolin, coal fly ash, and metallurgical slag after
quartz and K-feldspar sands were 15.066 m2/g and 19.585 m2/g, respectively. The
curing at ambient temperature or temperature between 60 and
aggregate used in this study are comprised of quartz and K-feldspar sands, with
120 °C [6]. Due to the avoidance of calcining limestone and burning the mass fraction content of quartz ranging from 20% to 100%. Metakaolin, an alu-
fossil fuels, using geopolymer instead of cements reduce the CO2 minosilicate raw material, was obtained by the calcination of kaolinite at 750 °C for
emissions greatly [1,2]. Although the effects of several parameters, 4 hours in a muffle. There is no distinct diffraction peak in the X-ray diffraction pat-
such as aluminosilicate raw material [8–12], curing condition [13– tern of metakaolin except the hump between 20 and 37 degree (Fig. 2), which indi-
cates an amorphous state of metakaolin. In order to demonstrate an apparent effect
16], ratio of reactant[17–19], reaction kinetics and mechanisms of aggregate on mechanical properties, the solid mixture was obtained by the mix-
[20–24], and the composition of polymer-geopolymer [25–28], ing of aggregates and metakaolin with a mass ratio of 3 according to our previous
on the properties of geopolymer have been studied over the last experience. The chemical compositions of metakaolin, quartz and K-feldspar deter-
several years, there’s almost no researches reported about the role mined by X-ray Fluorescence (XRF) are listed in Table 1.
Alkaline activators used in geopolymers were consisted of sodium hydroxide
of aggregate species and contents in geopolymer. It’s still not clear
(95% of purity, Beijing Chemical Reagent Ltd. China) and water glass (Modu-
how aggregate behave in the concentrate alkaline paste and influ- lus = 2.46, w(Na2O) = 15.17 and w(SiO2) = 36.22 by mass, Baume degree 50°, Beijing
ence the macroscopical properties of the geopolymer. In this study Chemical Reagent Ltd. China). Distilled water was used to dissolve the sodium
the effect of aggregate content of quartz and K-feldspar on the hydroxide solid to avoid the unknown contaminants in the mixing water [29].
mechanical and microstructural properties of the alkali-activated The mixed sodium hydroxide solution was prepared 24 h before addition to solid
aluminosilicates. Alkaline activators were added to solid mixture with a L/S (liquid
paste is investigated. In addition, this study is of great significance to solid mass ratio) of 0.36. Previous study showed that the modulus ratio of alka-
for the utilization of feldspar quartz rich tailings as the aggregate of line activators solution between 1.2 and 1.4 lead to high bending and compressive
geopolymer. strength of geopolymer [7]. Therefore, the modulus of alkaline activator solution in
this study was set to 1.13–1.42.
2. Experimental
2.2. Preparation
2.1. Materials
Metakaolin and aggregate were mixed in a cement mixer for 3 min, followed by
The aggregate used in geopolymer was usually natural rocks like granite and the addition of mixed alkaline activators. The ratio of metakaolin (g)/solid powder
quartzite which mainly consist of silicate and/or aluminosilicate minerals with (g) and alkaline activator (g)/solid powder (g) were 0.25 and 0.36, respectively. The
stable chemical properties, corrosion resistance and high hardness [29]. In order resulting paste was transferred to a stainless steel mould, and then was pressed
to make certain the aggregate has enough large superficial area to react with the under an isostatic pressure of 10 MPa for 5 min. After being removed from the
matrix completely, quartz sand and K-feldspar sand were selected and ground mould, the sample was dried at 80 °C in an oven for setting for 24 h, and then main-
finely to a particle size less than 100 lm (Fig. 1). The surface area of the fines of tained in atmosphere for 27 days.

2.3. Methods

The compression test was performed on the cylinder samples with diameter of
40 mm and height of 100 mm, and the bending strength was determined on cuboid
samples with size of 40 mm  40 mm  160 mm. The failure load of bending test
was determined by the load-distortion curve obtained from three-point bending
test using an electronic universal testing machine. The standars for measuring
the compressive strength and bending strength is based on the Chinese standar
GB28635-2012/ Concrete paving bricks. The microstructure of sample was studied
by the scanning electron microscope (SEM, Hitachi, S2300), and polarizing micro-
scope analysis (POM, caikon, XP400), respectively. Chemical composition was mea-
sured by electron probe microanalysis (EPMA, JXR-8230) with beam spot size of
5 lm at 50 nA and 20 kV.

3. Results

3.1. Compressive strength

Compressive strength of the as-prepared geopolymeric bricks is

shown in Fig. 3. Note that samples using alkaline activators solu-
Fig. 1. Particle size distribution of the K-feldspar and quartz sands. tion with a modulus ratio of 1.18 and aggregate with K-feldspar/
 L. Tian et al. / Construction and Building Materials 147 (2017) 543–549 545

Table 1
The chemical compositions of metakaolin, quartz and K-feldspar (wB%).

Sample SiO2 TiO2 Al2O3 Fe2O3 MnO MgO CaO Na2O K2O P2O5 LOI Total
MKL-2 49.75 1.58 43.23 1.35 0.02 0.03 0.24 0.10 0.05 0.05 2.99 99.39
QC-1 96.33 0.03 0.40 1.13 0.01 0.21 0.12 – 0.08 0.05 0.05 99.66
KF-12 66.52 – 18.20 0.38 0.01 – 0.48 2.48 10.52 0.03 0.62 99.29

Fig. 3. Compressive strength vs alkaline activator modulus ratio curves under Fig. 4. Bending strength vs alkaline activator modulus ratio curves under different
different K-feldspar/quartz ratio for geopolymeric bricks. K-feldspar/quartz ratio in geopolymeric bricks.

quartz ratio (F/Q) of 0.2 were named GM 1.18-F/Q 0.2. Similarly,

samples with F/Q of 0.4 and activator modulus ratio of 1.18 as well strength compared with OPC. The bending strength also increased
as F/Q of 0.2 and activator modulus ratio of 1.37 were named GM first and then decreased with the increase of activator modulus
1.18-F/Q 0.4 and GM 1.37-F/Q 0.2, respectively. ratio, but with maximum corresponding to different alkaline acti-
The compressive strength of the geopolymeric bricks with dif- vator modulus. The bending strength was roughly the same when
ferent F/Q was very similar when activator modulus varies from the activator modulus is 1.37 and 1.42. The geopolymeric bricks
1.13 to 1.42 (Fig. 3), which increased first and then decreased with with aggregate being composed only of quartz (F/Q = 0) possess
an increase of activator modulus ratio, and reached the maximum highest bending strength when alkaline activator modulus ratio
value at the activator modulus of 1.33. Previous studies about the was below 1.37. It was also found that the bending strength
geopolymeric paste showed that SiO2/Na2O molar ratio is a signif- decreases with the increase of F/Q. With the increase of F/Q, the
icant parameter which affects the compressive strength [30]. The alkaline activator modulus corresponding to the maximum of
increase of compressive strength is mainly due to the appropriate bending strength shifted from 1.24 to 1.37.
SiO2/Na2O molar ratio and an increase of polymerization degree.
The increase of NaOH concentration provides better dissolution
3.3. SEM analysis
of silicate and aluminate species and lead to the increase of
inter-molecular bond strength. The reduction in strength is proba-
Fig. 5 show SEM micrographs of the sample GM 1.33 - F/Q 0.2.
bly due to the excess of unreacted NaOH.
As it can be seen in the figure, the aggregate are of different size,
The shapes of the compressive strength vs alkaline activator
which are wrapped in alumino-silicate gels, sometimes with the
modulus curve with different F/Q were almost the same when
unreacted metakaolin. Some extent of corrosion can often be
the SiO2/Na2O molar ratio ranged from 1.24 to 1.42, which did
observed on the surface of aggregate, as shown in Fig. 5
not hold for the activator modulus ratio below 1.24 most probably
(a) and (b). Also, the porous cracks left by the evaporation of water
because the excess sodium hydroxide absorbed carbon dioxide
in the matrix can also be seen. The fracture surfaces of geopoly-
(CO2) from the air and transformed into sodium carbonate. This
meric brick are shown in Fig. 5(c) and (d). It can be seen that the
part of free carbonate appeared at the surface of geopolymeric
aggregate are tightly bound to the matrix, and the morphology of
bricks by the capillarity of transpiration, which is known as ‘‘efflo-
the region between the aggregate and matrix is obviously different
rescence”. The compressive strength decreased with the increase of
from that of matrix. The fresh fracture surface indicates that the
F/Q when the SiO2/Na2O molar ratio was 1.13 and 1.18. The
chemical bonds generated by geopolymerisation between aggre-
strength behavior observed here can be explained by the role of
gate and matrix are strong and increase the mechanical properties
the aggregate in geopolymer, which was usually ignored in OPC
of the sample, which is different from OPC.
[31]. In geopolymer the dissolution of aggregate in the presence
of alkalis hydroxide will enhance bond intensity at the interface
3.4. POM and EPMA analysis
of paste and aggregate.

The polarizing microscope (POM) images of geopolymeric

3.2. Bending strength bricks GM 1.33-F/Q 0.2 and GM 1.24-F/Q 0.2 were shown in
Fig. 6, in which different mineral phases could be identified by
Bending strength of geopolymeric bricks is shown in Fig. 4. It comprehensive analysis. It can be seen that the boundary between
can be seen that geopolymeric bricks possess very high bending quartz and matrix was not clearly, and some quartz particle has
546 L. Tian et al. / Construction and Building Materials 147 (2017) 543–549

Fig. 5. SEM micrograph of geopolymeric brick GM 1.33 - F/Q 0.2. (Note: a and b showed the corrosion surface of aggregate; c and d showed the fresh fracture surface of
aggregate.)

(a) GM 1.33-F/Q 0.2 (b) GM 1.24- F/Q 0.2

Fig. 6. Photographs of GM 1.33-F/Q 0.2 and GM 1.24-F/Q 0.2 bricks observed in perpendicular polarized microscope. (Note: Qtz represents quartz; Kfs represents K-feldspar;
the elemental composition of the sites marked by A, B, C, D, E and F were analyzed by electron probe microanalysis.)
 L. Tian et al. / Construction and Building Materials 147 (2017) 543–549 547

Table 2
Composition of aggregate and matrix (wB%) determined by electron probe microanalysis.

Site SiO2 TiO2 Al2O3 FeO MnO MgO CaO Na2O K2O Total
A 46.80 0.10 20.38 0.35 – 0.05 0.51 18.69 – 86.88
B 86.51 – 4.48 – – – – 3.67 – 96.44
C 41.19 0.14 26.14 0.48 0.10 0.66 0.43 11.38 7.11 87.62
D 39.11 0.55 21.29 0.34 – 0.12 0.72 24.47 – 86.59
E 90.85 – 0.85 – – – – 0.80 – 92.51
F 40.89 0.21 26.69 0.13 – 0.31 0.22 11.98 6.87 87.29

Fig. 8. Relation between F/Q ratio and modulus of alkaline activator at the peak
Fig. 7. Relations between bending strength and compressive strength according to
value of bending strength.
modulus of alkaline activator in geopolymeric bricks made with different aggregate
content.

already corroded into small pieces. The extent of edge corrosion of
quartz was greater than that of K-feldspar, which suggests that the
quartz formed more chemical bonds with the matrix than K-
feldspar in alkaline solution. This may be the explanation why
the geopolymeric bricks with lower F/Q achieve better mechanics
performance.
In order to analyze the surface reaction between matrix and
aggregate, the sites marked by A, B, C, D, E and F, as shown in
these two linear curves. Therefore, the samples with higher F/Q
ratio demonstrate more stable ratio of bending-compressive
strength.
Besides, the F/Q ratio has a linear relationship with the modulus
of alkaline activator which corresponds to the maximum of bend-
ing strength, as shown in Fig. 8. Take the aggregate of quartz for
example, quartz can be dissolved in the alkaline solution to form
[SiO2(OH)2]2, the chemical reaction is given as
SiO2 þ 2OH ! ½SiO2 ðOHÞ2 
2

Fig. 6, were measured by electron probe microanalysis (EPMA)

and the results are listed in Table 2. Site A and D represent the The modulus of sodium silicate is described as
matrix which is far from aggregate, site B and E represent the area M ¼ nðSiO2 Þ=nðNa2 OÞ
which is between the matrix and quartz, and site C and F represent
the area which is between the matrix and K-feldspar. It can be seen So the modulus of alkaline activator can be described as
from Table 2 that site A and D are composed of sodium aluminosil- nwg ðSiO2 Þ
icate; site B and E consist mainly of quartz pieces, together with M¼
nwg ðNa2 OÞ þ 2nðNaOHÞ
few sodium aluminosilicate; and site C and F consist of sodium-
potassium aluminosilicate. These observations are strong evi- Considering the [SiO2(OH)2]2 formed by quartz, so
dences which confirms that the potassium in K-feldspar can be dis- 2
nwg ðSiO2 Þ þ nð½SiO2 ðOHÞ2 
solved in alkaline solution and enter into the aluminosilicate M0 ¼
matrix. nwg ðNa2 OÞ þ 2nðNaOHÞ
When the alkaline solution reacted completely with metakao-
lin, the geopolymeric bricks achieve the best bending strength, so
4. Discussion
modulus of alkaline solution (M) is a fixed value, and then
2
Relations between bending strength and compressive strength nð½ðSiO2 ÞððOHÞ2 
M0 ¼ M þ
of geopolymeric bricks are shown in Fig. 7. The slope of two linear nwg ðNa2 OÞ þ 2nðNaOHÞ
fitting curves is approximately equal to the ratio of bending-
compressive strength. According to literatures, the ratio of As is known, the formed [SiO2(OH)2]2 has a quantitative rela-
bending-compressive strength of Geopolymeric bricks are mainly tion (A) with the quartz aggregate,
2
between these two linear curves, namely, between 0.122 and nð½SiO2 ðOHÞ2  Þ ¼ AnðQuartzÞ, and nwg(Na2O) + 2n(NaOH) is a
0.169. Besides, some of the points lying outside these two linear fixed value. Setting the value B ¼ nwg ðNa2 OÞþ2nðNaOHÞ
A
, so
curves are mainly from samples with the F/Q ratio of 0, 0.2 or
0.4. It is clear that samples with low F/Q ratio mainly lie outside M0 ¼ M þ BnðQuartzÞ
548 L. Tian et al. / Construction and Building Materials 147 (2017) 543–549
Table 3
Component molar ratio of matrix.
Sites n(Si)/n(Al) n(K + Na)/n(Al)
A 1.94 1.50
B 19.98 2.01
C 1.33 1.01
D 1.56 1.89
E 95.76 1.74
F 1.29 1.02
Therefore, the F/Q ratio has a linear relationship with modulus
of alkaline activator in theory. And the reaction of K-feldspar with
alkaline solution is similar to quartz. The structure of K-feldspar
can be destroyed by the concentrated alkaline solution and the
K+ spread into the aluminosilicate gels to balance the charge of
[Al(OH)4]. Therefore, the K-feldspar have the ability to provide
additional alkaline, and thus can decrease the consumption of
sodium hydroxide in geopolymerization.
The three dimensional aluminosilicate framework could be
classified into four monomers types according to the different n
(Si)/n(Al) ratios in matrix [6]: (1) poly (sialate) (n(Si)/n(Al) = 1,
PS); (2) poly (sialate-siloxo) (n(Si)/n(Al) = 2, PSS); (3) poly
(sialate-disiloxo) (n(Si)/n(Al) = 3, PSDS); and (4) poly (sialate-
multisiloxo) (n(Si)/n(Al) > 3, PSMS). The component molar ratio
of matrix was shown in Table 3. The n(Si)/n(Al) ratio for site A with
activator modulus of 1.33 is approximately 2, which means the
polymerization monomer was mainly PSS type
([ASiAOAAlAOASiA]n). The site D with activator modulus of
1.24 has a n(Si)/n(Al) of 1.56, which suggest that it consists of both
[ASiAOAAlAOASiA]n and [ASiAOAAlA]n polymerization mono-
mers. Therefore, the [ASiAOAAlAOASiA]n polymerization mono-
mer was easier formed under higher alkaline activator modulus
ratio. The n(Si)/n(Al) value for sites B and E are very larger probably
due to probing mainly on quartz. The n(Si)/n(Al) for sites C and F
have the similar values, 1.33 and 1.29, which is greatly smaller
than the n(Si)/n(Al) of 3 for K-feldspar. It means sites C and F
belong to K-containing matrix phase, rather than locating on the
surface of K-feldspar. In addition, the similar n(Si)/n(Al) value
which approximates to 1 for sites C and F indicated that both sites
are mainly composed of PS type ([ASiAOAAlA]n) polymerization
monomer. Therefore, different from observation in the area of
matrix, variation of activator modulus does not exert substantial
effect on the polymerization monomer type for the K-containing
area between matrix and K-feldspar.
In geopolymer, alkali metal ions are mainly distributed in inter-
stitial sites of the three-dimensional framework of aluminum sili-
cate to balance the negative charge of alumina tetrahedron. Due to
the incompleteness of polymerization reaction, part of alkali metal
ions usually still exists in the skeleton of aluminum silicate. There-
fore, n(K + Na)/n(Al) is usually between 1 and 1.6 in a normal
geopolymer materials [7]. Sites A and D represent matrix phase
which does not contain K ion. The A site with activator modulus
of 1.33 has the n(Na)/n(Al) of 1.50. As for site A, the alkali metal
ions are not excess, which exists in forms of interstitial ion and
SiAOANa, AlAOANa bonds. Therefore, GM 1.33-F/Q 0.2 sample
demonstrated good mechanical property. With decreasing activa-
tor modulus to 1.24 (Site D), the n(Na)/n(Al) increases to 1.94, indi-
cating existence of excess alkali metal ions which will precipitate
from the sample surface in a free form. This explained the lower
mechanical property of GM 1.24-F/Q 0.2 sample. Sites B and E does
not contain K ion, in which the existence of excess Na+ is due to the
formation of poly-sodium silicate, the product of reaction between
quartz and sodium hydroxide solution. Sites C and F are near K-
feldspar and therefore contain K+. The n(K + Na)/n(Al) is 1.01 and
1.02 for both sites, respectively, which is lower than the counter-
part of matrix. This is due to the fact that K+ is more capable of
entering into the matrix to balance the negative charge of polysia-
late than Na+, and thus increases the rate of ionization and
dissolution.
The matrix of geopolymer is mainly composed of amorphous
aluminosilicate gel, which has a short-range order three-
dimensional network, such as nano-zeolite [32]. The matrix will
partially evolves into a small mounts of zeolites when curing time
was prolonged [33]. These zeolites may be crystal-structurally sim-
ilar with analcite and hydroxysodalite according to the result of
EPMA. Base on our experimental results and thermodynamic cal-
culation, the main chemical reactions that may occurr in this
research are given as below.
SiO2 þ 2OH ! ½H2 SiO4 
2
ð1Þ

Al2 Si2 O7 þ 6OH þ 3H2 O ! 2½AlðOHÞ4  þ 2½H2 SiO4 
2
ð2Þ

KAlSi3 O8 þ 6OH þ 2H2 O ! Kþ þ ½AlðOHÞ4  þ 3½H2 SiO4 
2
ð3Þ

Naþ þ ½AlðOHÞ4  þ 2½H2 SiO4 
2
! NaAlSi2 O6  H2 O þ 4OH þ 2H2 O ð4Þ

ð8  zÞNaþ þ zKþ þ 6½AlðOHÞ4  þ 6½H2 SiO4 
2
! ðNa8z Kz ÞAl6 Si6 O24 ðOHÞ2  12H2 O þ 10OH ð5Þ
5. Conclusion
This work presents studies on effect of different F/Q ratio and
activator modulus ratio on the microstructure and mechanical
properties of geopolymeric bricks. Main conclusions are summa-
rized as follows:
1. The aggregate contents of quartz and/or K-feldspar do not influ-
ence the compressive strength of geopolymeric bricks notably.
the geopolymeric bricks made with lower F/Q ratio achieve bet-
ter bending strength. It means that the quartz might forms
more chemical bonds with the matrix than K-feldspar in alka-
line solution.
2. The relation between F/Q ratio and modulus of alkaline activa-
tor at the peak value of bending strength is linear. Because the
potassium in K-feldspar can be dissolved in alkaline solution
and enter into the aluminosilicate matrix, and thus can
decrease the consumption of sodium hydroxide needed for
geopolymerization. Besides, the quartz reacts with the sodium
hydroxide and forms [H2SiO4]2 which is the main component
of sodium silicate.
3. The matrix phase formed more [ASiAOAAlAOASiA]n polymer-
ization monomer with higher alkaline activator modulus ratio
when K+ is not involved in the reaction. However, only the poly-
merization monomer of [ASiAOAAlA]n was favored against
change of alkaline activator modulus when the K+ exists.
Acknowledgement
This work was financially supported by the funds from the
China Geological Survey Project (Grant no. 12120113087700).
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