International Journal of Coal Geology, 10 (1988) 99-108 99

Elsevier Science Publishers B.V., Amsterdam - Printed in The Netherlands

A Statistical Approach to the Study of the

Distribution of Trace E l e m e n t s and their Organic/
Inorganic Affinity in L o w e r G o n d w a n a Coals of
India

K.N. MUKHERJEE 1N.R. DUTTA1, D. CHANDRA2 H.S. PANDALAI2 and M.P. SINGH3
1Ex-Coal Wing, Geological Survey of India, Calcutta, India
2Department of Applied Geology, Indian School of Mines, Dhanbad-826004, India
3Department of Geology, Banaras Hindu University- Varanasi, India
(Received February 26, 1987; accepted October 26, 1987)

ABSTRACT

Mukherjee, K.N., Dutta, N.R., Chandra, D., Pandalai, H.S. and Singh, M.P., 1988. A statistical
approach to the study of the distribution of trace elements and their organic/inorganic affinity
in Lower Gondwana coals of India. Int. J. Coal. Geol., 10: 99-108.

Trace-element analyses of seventy six coal samples representing all the major Lower Gondwana
coal basins of India were carried out. Eighteen trace elements, viz., B, Ba, Co, Cr, Cu, Ga, Ge, La,
Mn, Mo, Nb, Ni, Pb, Sn, St, V, Y and Zr were determined quantitatively in coal ash. An attempt
was made to correlate the coals of different coalfields on the basis of multivariate analysis. In
addition, the organic/inorganic affinities between the trace elements were established by the coef-
ficients of correlation between the trace elements and ash present. A synthesis of the data reveals
that there is similarity in the concentration ranges of trace elements among the coal seams of
different coalfields, but the possibility of environmental differences exists due to the statistically
different multivariate means of the trace-element concentrations.
It is inferred that Ge, Cr, Y and La occur in these coals as organo-metallic complexes and
chelates. The elements Ni, Co, Ga, V and Cu show both organic and inorganic association, whereas
Mn and Ba are exclusively incorporated in the inorganic fractions.

INTRODUCTION

Following t h e lines o f t h e p i o n e e r i n g w o r k of R a m g e (1927), G o l d s c h m i d t

(1930,1933) a n d G o l d s c h m i d t a n d P e t e r s (1933), a n u m b e r of w o r k e r s have
s t u d i e d t h e d i s t r i b u t i o n o f t r a c e e l e m e n t s in coals f r o m n e a r l y all t h e m a j o r
coalfields o f t h e world. H o w e v e r , such studies o n I n d i a n coals have b e e n lim-
ited. T h e s e were first i n i t i a t e d b y M u k h e r j e e a n d D u t t a (1949) a n d studies on
t h e Ge c o n t e n t s o f v a r i o u s I n d i a n coals have b e e n m a d e b y I y e r a n d S u n d a r a m

0166-5162/88/$03.50 © 1988 Elsevier Science Publishers B.V.

100

(1955), Das (1958), Rao and Rao (1965) and Banerjee et al., (1972). Other
workers who have studied trace-element distributions in Indian coals include
Mukherjee and Ghosh (1976), Mullik and Ahmad (1979), Chandra et al.
( 1981 ), and Mukherjee et al. ( 1981,1982 ), Singh et al. ( 1983,1985 ) and Pareek
and Bardhan (1985). The aim of the present work was to study the distribution
of trace elements in coals belonging to the Barakar Formation of the Lower
Gondwana sequences of all major basins in Peninsular India.

SAMPLE COLLECTION AND ANALYTICAL PROCEDURE

For the present investigation coal samples were collected from all major
coalfields of Peninsular India, thus coalfields in Darjeeling, Arunachal Pra-
desh and Sikkim were not analysed.
A total of 76 coal samples was initially analysed. Table 1 gives details of the
samples collected from each coalfield. They were collected from both opencast
and underground workings and some subsurface borehole cores were also ob-
tained. Channel sampling was done in working mines and split core samples
were procured from the different boreholes.
The samples were reduced to 500 g, precautions being taken to avoid con-
tamination, and a representative part of this reduced quantity was used for the
study. First the samples were ashed at 450 °C under controlled conditions of
air flow. The ash obtained was then mixed with an equal quantity of spec pure
carbon and arced in a Jarrel Ash 3.4-m Ebert grating spectrograph. Direct-
current excitation at 14 amp using graphite-necked electrodes (National SPKL
4200) was performed. Synthetic standards in simulated coal ash were used for
standardisation. The total-energy method of quantitative spectrographic anal-
ysis as described by Bastron et al. (1960) was followed for quantification, with
an overall standard accuracy of 10 to 15%.

RESULTS

A maximum of 18 trace elements were analysed in the samples. Table 2 shows

the average content and the standard deviations with respect to each of them.
The mean values of the trace elements recorded in the coal ash are broadly
comparable to the values compiled by Bouska (1981) and Valkovic ( 1983 ) for
different coalfields. However, the values of B, Co, Cu, Ge, Ni and Pb are on the
low side, whereas the mean value for Sn is relatively high. The standard devia-
tions show a fairly high variations in the case of Ba, Ga, Ge, Mo, Pb, Sn, Sr
and Y.
For a comparative study of trace-element distribution the coals of the eight
major lower Gondwana basins have been grouped into three divisions on the
basis of their geographic proximity (Table 1 ). The first group consists of basins
I and II (25 samples), the second includes basins III-V (26 samples) and the
 101

TABLE 1

Details of the coal samples collected and analysed for trace-element contents

Basin Coalfields No. of

samples
Region I
I Damodar-Koel Valley Raniganj coalfield 9
Jharia coalfield 6
East Bokaro coalfield 2
West Bokaro coalfield 2
Ramgarth coalfield 1
South Karanpura coalfield 1
North Karanpura coalfield 1
II Gali-Rajmahal-Purnea- Hura coalfield 3
Malda through Panchwara coalfield
Brahmani coalfield

Region H
III Mahanadi valley
Talcher coalfield 1
Ib Valley coalfield 3
Korba coalfield 2
Hasdo-Arand coalfield 1
IV Transitional belt between Chirimiri coalfield 6
Mahanadi and Son valley
V Son valley Johilla coalfield 1
Sohagpur coalfield 3
Singrauli coalfield 5
Bisrampur coalfield 2
Jhillimilli coalfield 2

Region III
VI Satpura valley
Pench-Kanhan coalfield 6
VII Wardha-Pranhita valley Kamthi coalfield 3
Manuguru coalfield
Kothagudem coalfield
VIII Godavari valley Yellendu coalfield 16
Bellampalli coalfield

t h i r d g r o u p is r e p r e s e n t e d b y b a s i n s V I - V I I I (25 s a m p l e s ) . T h e r a n g e s o f vari-
a t i o n s { m i n i m u m a n d m a x i m u m values ) are s h o w n in T a b l e 3. A c o m p a r i s o n
of the t r a c e e l e m e n t c o n c e n t r a t i o n s (min. a n d max. values) of t h e s e t h r e e
regions reveals a c o n s p i c u o u s difference b e t w e e n regions I a n d II in r e s p e c t to
102

TABLE 2

Mean values and standard deviations of trace elements in coal ash from coal seams of the Barakar
Formation. The average ash content and its standard deviation is given at the bottom.

Element No. of Mean values Standard Coefficient of

samples (p.p.m.) deviation variation
(p.p.m.) (%)

B 70 18.30 8.62 47.10

Ba 71 385.76 233.37 60.50
Co 71 23.30 11.07 47.51
Cr 71 119.10 61.50 51.64
Cu 71 82.89 46.80 56.46
Ga 71 20.23 18.00 88.67
Ge 22 30.41 24.33 80.00
La 71 29.38 12.46 42.40
Mn 71 575.20 226.47 39.37
Mo 12 13.00 15.07 115.92
Nb 61 21.67 4.58 21.14
Ni 71 80.23 34.56 43.08
Pb 71 33.91 24.70 72.84
Sn 30 37.36 91.22 244.16
Sr 69 167.57 142.20 84.86
V 71 114.23 47.57 41.64
Y 71 48.45 34.31 70.81
Zr 71 278.70 136.92 49.13
Ash 71 29.34% 11.00 37.49

the concentrations of Ba, Ga, Ge, Mn, Sr and Y. To study whether it is statis-
tically valid to differentiate or establish any similarity among the coals of these
three geographic divisions, an attempt was made to examine whether the mul-
tivariate means of each of these divisions were significantly different. On ac-
count of the inequality of means, the test for equality of variances could not be
established.
However, an attempt was made to study the interrelationships among the
trace elements with special reference to their mode of fixation in coal and their
dependence on coal facies. The coefficients of correlation between trace ele-
ments and ash % in the 76 samples from the eight basins have been calculated
(Table 4). In addition, the geochemical affinity of trace elements was estab-
lished on the basis of cluster analysis of 9 selected trace elements and ash %
in 76 coal samples. These results are shown in Fig. 1.
The results indicate that of all the trace elements analysed, Ga shows the
closest relationship with ash content. According to Bouska and Honek (1962),
Ga is associated with the alumino-silicate minerals present in coal and its con-
centration, in general, was greater in coal seams than in the adjacent claystone
 103

TABLE 3

Range of variation of t r a c e - e l e m e n t c o n t e n t in coal a s h from t h e B a r a k a r F o r m a t i o n in each of

t h e three major geographic groupings of G o n d w a n a coalfields

Element Range of values (min. a n d m a x . ) in p p m

Region I Region II Region III

1. B 3 - 32 5- 31 10- 38
2. Ba 266-1622 99- 908 78-2413
3. Co < 1 0 - 70 10- 32 13- 56
4. Cr 6 0 - 286 60- 249 48- 222
5. Cu 27- 163 30- 321 53- 117
6. Ga < 1 0 - 160 11- 24 10- 28
7. Ge <5- 50 5 - 60 60- 96
8. La 18- 60 20- 51 19- 75
9. Mn 20-1189 150-1163 290-1240
10. Mo <5- 60 7- 13 (N.A.)
ll. Nb 17- 34 18- 29 15- 29
12. Ni 15- 250 35- 145 46- 130
13. Pb 10- 70 8- 89 17- 53
14. Sn < 1 0 - 40 14- 50 10- 13
15. Sr 50- 900 47- 153 64- 488
16. V 67- 183 84- 258 45- 146
17. Y 26- 300 28- 111 30- 90
18. Zr 100- 668 20- 863 174- 500

N.A. = N o t analysed.

TABLE4

Coefficients of correlation between values of ash and 12 trace elements analysed in coals from the Barakar
Formation presented in matrix form. Numbers in parenthesis against each variable indicate the number of
samples in which each of them were analysed.

Ash Ge Ni Co Cu Pb Zr Mn Cr Ba Ga V Y
(69) (22) (71) (69) (71) (71) (71) (71) (71) (71) (71) (71) (71)

Ash 1.00
Ge -0.12 1.00
Ni -0.16 0.58 1.00
Co - 0.09 0.62 0.69 1.00
Cu -0.10 0.37 0.50 0.16 1.00
Pb -0.09 0.25 0.27 0.04 0.41 1.00
Zr 0.09 -0.23 -0.08 -0.12 -0.04 -0.02 1.00
Mn -0.30 0.10 0.11 0.07 0.13 0.09 0.06 1.00
Cr 0.10 0.25 0.54 0.40 0.62 0.29 -0.13 -0.13 1.00
Ba 0.02 -0.01 0.20 0.22 0.19 0.17 0.21 -0.05 0.16 1.00
Ga 0.02 0.22 0.58 0.56 0.06 0.18 -0.01 -0.19 0.22 0.24 1.00
V 0.30 0.00 0.21 0.09 0.12 0.12 0.52 -0.24 0.33 0.18 0.16 1.00
Y -0.05 0.34 0.52 0.49 0.10 0.15 -0.19 -0.10 0.15 0.05 0.83 0.01 1.00
104

Ash Ga Zr Mn Cr V Ni Co C

0.74.¢

0.562

0-373
l- 0.749

0.562

0"373

0"23
0.185 0.165
. 1 0.1 0

0-003 0-003

Fig. 1. Dendograambased on linear correlationcoefficientscomputedby weightedpair-group.

of the Upper Doubrava Member of the Ostrava-Karvina Coalfield (Bouska,

1981 ). In addition, Zubovic (1966) suggested that Ga, V, Ni, Cr, Co, Y, Cu and
Sn are capable of forming metallo-organic complexes. Apart from these two
reports, a synthesis of the trace-element data available from the different coal-
fields of the world shows that Ga has a strong affinity with the inorganic con-
stituents (clays) of coal and a weak affinity for the organic constituents (Singh,
1986). Moreover, in the present analysis, though Ga shows the closest rela-
tionship with ash content, the coefficient of correlation between the two is only
+0.274. Also, Ga shows a fairly good correlation with Ni and Co. It appears
therefore that Ga has a fair association with alumino-silicates and partially
with organic matter as organo-metallic complex similar to that of Co and Ni.
This may be due to its strong chalcophile and weak lithophile character.
Due to the association of vanadium with organic material, Leutwein and
Rosier (1956) observed a relationship between V and Ga. However, V is also
known to be concentrated exclusively in the organic component of coals (Rey-
nolds, 1948; Uzunov, 1965,1967; Manskaya and Drozdova, 1968; Bouska, 1981 ).
In the coals studied here, V is related most closely with Cr, whereas its coeffi-
cient of correlation with Ga is only + 0.167. Chromium is known to be associ-
ated with organic matter (Bouska, 1981; Gluskoter et al., 1977) and Cr content
is positively correlated with V (Kudelasek, 1959). The coefficients of correla-
tion between Cr and V in the present study are not high. However, cluster
analysis reveals the mutually closest relationship between these elements.
Cluster analysis shows a close relationship between Mn and Zr. Otte (1953)
 105

and Swaine (1977) suggested that Mn exists exclusively in the inorganic con-
stituents of coal, probably together with carbonates, silicates or oxides. Fur-
ther, Otte (1953) observed that Zr is concentrated in vitrains. Bouska ( 1981 )
has also shown its affinity towards the organic fractions of coal. Deul and An-
nell (1956) and Rush et al. (1975) have indicated the association of Zr with
the inorganic fractions. In the present study, the positive relation of Zr with
Ge and Ni points to its occurrence in these coals as organo-metallic compounds.
Cobalt, Ni and Cu show fairly a close similarity in their distribution in the
samples studied. These elements appear to be incorporated in the sulfide-min-
eral phases, though Ni, Cr and to a lesser extent Cu, are perhaps capable of
forming organo-metallic complexes. This is inferred because of their fair po-
sitive correlation with elements such as Cr, and Y. The reasonably good posi-
tive correlation of Ni with Cr and Cu is significant and is perhaps due to the
ready availability of donor elements with which these elements could be bonded
in organo-metallic complexes.
In other Barakar coals, Cu shows a significant positive correlation with Ni
and Cr. Copper is known to accumulate in plants and can also be associated
with sulfides (Bouska, 1981 ). Fraser (1961) found an organo-metallic complex
chelated with Cu in Canadian peat. Zubovic (1966) also suggested that Cu is
capable of forming such complexes. The formation of an organic complex was
also reported by Ong and Swanson (1966). However, Zubovic (1966) sug-
gested that where anaerobic hydrogen sulfide activity is dominant, Cu can be
expected in sulfide form due to the relative stability of the sulfide in compari-
son to the chelates. Where sulfide ion activity is low, Cu can be incorporated
as organic chelates. In the present study, the correlation of Cu with Ni and Cr
in the Barakar Formation coals probably indicates that Cu and partly Ni and
Cr exist as organo-metallic chelates.
The mechanism of fixation of lead appears to be different from most of the
elements studied. In the coals of the Barakar Formation, it has a correlation
with most of the elements. Hinds (1912) was the first to report the presence
of galena in certain coals. Chow and Earl (1972), who discussed the origin of
lead in coal samples, suggest that it is perhaps incorporated into coal forming
material prior to coalification, probably by circulating groundwater.
In general, the germanium content is fairly low in the coal ash of the Barakar
coals. It shows a positive correlation with Co and Ni, and in the BII and BIV
seams of the Raniganj coalfield, Ge contents have a fairly positive correlation
with Pb, Zr and Mn. Germanium has been attributed the highest organic af-
finity amongst all elements by Zubovic ( 1966 ), Manskaya and Kodina (1975)
and several others. Germanium like V, Ga, Ni, Cr, Cu, Y, Co and Ca, forms
stable organic chelates. However, because of its later introduction into the
coal-forming milieu, Ge probably replaces other chelated metals (Zubovic,
1966).
106

In any case, the retention of Ge in coal is a function of the pH and sorbed

Ge contents can be reduced considerably by desorption (Bouska, 1981). The
low concentration of Ge in coal ash in the present investigation points to its
strong affinity and association with organic constituents.
Thus the elements that exhibit a fair degree of correlation in the samples
analysed in the present study and that because of their inter-relationships are
inferred to occur predominantly or partly as organo-metallic chelates are Ge,
Cr, Y, Ni, Co, Ga, Zr, Cu and perhaps La. Of these, Ge, Cr, Y and La seem to
be predominantly bound with organic matter, whereas Ni and Co are perhaps
incorporated partly in pyrite and Cu in a sulfide phase. The Zr content in the
Barakar coals appears to be due to the presence of zircon, and the Ga contents
is inferred to be partly contributed by alumino-silicate minerals. On account
of the diverse phases in which these elements occur, the coefficients of corre-
lation between them are not very high. In addition, the incorporation of some
of these elements in inorganic constituents of coal and the formation of or-
gano-metallic chelates are also influenced by the donor elements to which the
metals are bonded {Zubovic, 1966). Vanadium, however, shows a poor corre-
lation with most of these elements except Cr. Both the Cr and V contents are
perhaps influenced by the pH and Eh of the coal facies.

CONCLUSIONS

The conclusions that can be drawn from this study are as follows:
(1) The average trace-elements concentrations in coal ash of coal seams
belonging to the Permian Barakar Formation, from all major coalfields of In-
dia, are comparable with the broad range of contents of these elements in coal
ash from coal formation of other parts of the world.
(2) Though most of the coal seams of the Barakar Formation in different
coalfields in India have comparable ranges of trace-element contents, they
cannot be inferred to have formed under identical conditions on account of the
statistically significant differences in the multivariate means of trace-element
contents.
(3) The elements that are inferred to be predominantly associated with or-
ganic matter and perhaps to exist as organo-metallic compounds and chelates
are Ge, Cr, Y and La. The other elements which at least in part exist as organic
chelates are Ni, Co, Ga and Cu. Nickel and Co are perhaps also incorporated
in pyrite, Ga partly in alumino-silicate minerals, and Cu as a sulphide.
(4) Vanadium contents in the sample are poorly correlated with this group
of elements that are associated with organic matter and V appears to partly
associated with inorganic (alumino-silicate) components of coal in the larger
group of coals of Barakar Formation. The content of V and Cr as organo-me-
tallic chelates appears to be significantly affected by the pH and Eh of the coal-
forming environment.
 107

{5) M a n g a n e s e a n d B a a r e e x c l u s i v e l y i n c o r p o r a t e d i n t h e i n o r g a n i c p h a s e s .
H o w e v e r , t h e c o e f f i c i e n t o f c o r r e l a t i o n b e t w e e n t h e s e e l e m e n t s is n o t s i g n i f i c a n t .

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