FORMULAS FOR CALCULATI NG THE HEATING VALUE OF COAL AND COAL CHAR: DEVELOPMENT,

TESTS AND USES

D. M. Mason and K . Gandhi
I nsti tute of Gas Technology
3424 S. State St.
Chicago, I l l i noi s 60616
The heati ng (cal ori f i c) val ue of coal and char is of great i mportance i n the
conversi on of coal to other usef ul forms of f uel , as wel l as i n its di rect use.
The si gni f i cance of the correl ati on of heati ng val ue wi th composition i n ordi nary
f uel usage is shown by the development, as earl y as 1940, of some 9 di f f erent for-
mulas f or cal cul ati ng heati ng val ue from the ul ti mate anal ysi s and 11formul as f or
cal cul ati ng i t from the proximate anal ysi s (1).
formulas have been proposed wi thi n the last three years (2,3,4). The correl ati on
i s perhaps of even greater importance f or the rati onal i zati on and modeling of con-
versi on processes now bei ng developed.
Three addi ti onal ul ti mate anal ysi s
Our own work on thi s problem was carri ed out f or a proj ect on preparati on of
a "Coal Conversion Systems Techni cal Data Book,"
of Energy and i ts predecessors.
supported by the U.S. Department
A data base (i ncl udi ng experi mental heati ng val ues, ul ti mate anal yses and some
other parameters) was establ i shed, consi sti ng of 121 samples from the Coal Research
Secti on of Pennsylvania State Uni versi ty ( 5 ) , and 681 samples anal yzed by the Bureau
of Mines and reported i n vari ous state and Federal government publ i cati ons (6,7,8,9).
The Penn State samples, representi ng l arge deposi ts of coal, had been sel ected f or
tabul ati on i n the Data Book (10). The data base covers a wide range of coal f i el ds
of the United States.
Four formulas were sel ected f or test. They are as fol l ows:
Dulong (1)
Q = 145.44 C +620.28 H +40.5 S - 77.54 (0)
Boie (11)
Q =
Grummel and Davis (1,121
151.2 C +499.77 H +45.0 S - 47.7 (O)+ 27.0 N
9 = [ ~~~~~~ +424.621 [C/3 +H - (0)/8 +s/ 8]
Mott and Spooner (1,13)
Q = 144.54 C +610.2 H +40.5 S - 62.46 (0) ( 0 ) 5 15%
30 96(0)
Q = 144.54 C +610.2 H +40.5 S - [65.88 - --"---](O) (O)> 15%
(100-A)
235
3)
I n the above, Q i s the gross heati ng val ue i n Btu/l b on the dry basi s and C , H,
S, (O), N, and A are the respecti ve contents oi carbon, hydrogen, sul f ur, oxygen,
ni trogen, and ash i n wei ght percent, al so on the dry basi s.
For a f ai r test of the formul as on samples representi ng commercial coal we
el i mi nated samples wi th more than 30% ash, l eavi ng a total of 775 samples i n the
data bank. Resul ts of appl yi ng the several formulas separatel y to the vari ous ranks
of coal and al so t o the combined ( al l ranks) data are presented i n Tabl e 1. The
bi as (average al gebrai c di f f erence between observed and cal cul ated val ues) and the
standard devi ati on af ter correcti on f or the bi as are the most si gni f i cant cri teri a.
For most of the formul as there are l arge di f f erences i n bi as among di f f erent ranks
of coal , so we have cal cul ated standard devi ati ons f or each rank af ter correcti ng
f or the bi as shown f or that rank. The standard devi ati on i s al so gi ven wi th
appl i cati on of a bi as correcti on averaged over al l ranks. Note that the often-used
Dulong formula has a substanti al bi as f or al l ranks, but of opposi te si gn f or low-
rank coal s compared wi th bituminous and anthraci te coal s. Thus the overal l bi as
is low, but no advantage is gai ned by i ts appl i cati on. Al s o note that al though
resul ts from the Boie equati on have the hi ghest bi as of any, af ter appl i cati on of
an overal l bi as correcti on the resul ts are among the best.
I n addi ti on to cal cul ati on wi th the formulas per se, we al so cal cul ated heati ng
val ues by use of Given and Y arzab's modified Parr equati on f or mi neral matter content,
and thei r correcti ons to obtai n carbon, hydrogen, sul f ur and oxygen on a mineral-
matter-free basi s (14). Thi s cal cul ati on requi res val ues f or pyri ti c sul f ur that
were not avai l abl e f or some of the samples. Kesul ts obtai ned wi th the modified Mott-
Spooner equati ons on 646 sari pl es having pyri ti c sul f ur contents are al so shown i n
Table 1; resul ts from other formulas were improved, but the Mott-Spooner equati on
gave the best resul ts. Detai l s of thi s cal cul ati on and f ul l resul ts are reported
el sewhere (15).
The data bank was al so subj ected t o a l east squares regressi on anal ysi s. Carbon,
hydrogen, sul f ur, ash, and oxygen terms were si gni f i cant; ni trogen and cross and
square terms were not. To avoi d the implied necessi ty of determi ni ng ni trogen, we
adopted an oxygen-pl us-ni trogen term.
as the Data Book Equati on, was as fol l ows:
The resul ti ng equati on, which we ref er to here
Q = 146.58 C +568.78 H +29.4 S - 6.58 A - 51.53 (0 +N) 5 4
When 100- C-H-S-A i s substi tuted f or O+N, an equi val ent form is obtai ned:
Q = 198.11 C +620.31 H +80.93 S +44.95 A - 5153 5b )
Resul ts from thi s new formul a are al so shown i n Table 1. The bi as f or di f f erent ranks
of coal ranges onl y from -45 Btu/l b on l i gni te to 13 Btu/l b on subbituminous coal and
does not show a trend wi th rank. The standard devi ati on i s si gni f i cantl y l ess than
those of the other unmodified formul as, even af ter improving these by a bi as correc-
ti on. The new formula has about the same accuracy as the Mott-Spooner wi th modified
Parr correcti ons, but the l atter i s more complicated and requi res pyri ti c sul f ur de-
termi nati on.
The ef f ect of ash content on the accuracy and preci si on of the formula was in-
vesti gated, wi th the resul ts shown i n Table 2. For thi s test, the formula was al so
appl i ed to the 27 hi gh-ash samples that had been removed from the data bank.
236
Tabl e 1. TEST OF FORMULAS FOR CALCULATION OF HEATI NG VALUE
Standard Devi ati on
Average Before Af ter Af ter Over-
No. of Absol ute Bias Rank Bi as all Bias**
Samples Devi ati on Correcti on Correcti on Correcti on
Btu/l b
Dulong
Anthraci te
Bituminous
Subbituminous
L i gni te
A l l Ranks
Boie
__
Anthraci te
Bituminous
Subbituminous
L i gni te
A l l Ranks
Grummel and Davis
Anthraci te
Bituminous
Subbituminous
L i gni te
A l l Ranks
Mott and Spooner
Anthraci te
Bituminous
Subbituminous
L i gni te
A l l Ranks
40
406
130
14 9
775
40
406
180
149
775
40
406
180
14 9
775
40
406
180
149
775
Mott & Spooner,
Modified Parr Basi s
A l l Ranks 646
New Formula
Anthraci te 40
Bituminous 406
Subbituminous 180
L i gni te 149
A l l Ranks 775
137
1 8 1
174
218
184
400
253
217
301
262
107
164
130
127
146
84
160
113
124
138
106
7 3
9 0
103
96
93
-123
-138
127
174
-15
- 400
-248
-207
-298
-256
79
-128
46
39
-44
-56
- 134
- 31
-85
-96
42
- 14
1 0
13
-45
0
157
2 2 1
213
255
223
417
279
249
330
291
134
208
16 8
171
189
107
197
152
170
178
-
93
124
140
137
129
* Average observed val ue - average cal cul ated val ue
** Bias obtai ned over al l ranks
97
173
170
185
-
100
129
138
138
-
106
164
1 6 1
16 7
-
9 1
144
14 9
147
-
-
92
1 2 3
1 3 9
1 2 9
1 2 9
237
146
212
222
266
222
17 7
129
146
145
13 9
165
184
185
187
184
100
149
162
147
150
132
93
124
140
13 7
129
Table 2. EFFECT OF ASH CONTENT ON THE CALCULA'I'ION OF HEATI NG VALUE
Ash Content, Number of Avg. Absolute Standard
W t % Samples Di fference Bias* Devi ati on
--
0-10
10-20
20- 30
>30
394
320
61
27
82
104
1 1 2
155
6 113
-15 144
26 141
20 211
*
Average of observed minus average of cal cul ated val ues
The absence of si gni f i cant bi as, here and among di f f erent ranks of coal , i ndi -
cates that no improvement by change i n the formula appears possi bl e as l ong as i t
i s based on ul ti mate anal ysi s onl v. The i ncrease of the standard devi ati on wi th
ash content can be attri buted to the ef f ects of di f f eri ng rati os of mi neral matter
t o ash, and di f f eri ng contri buti ons of the mi neral matter to determined carbon and
hydrogen contents.
vari ance i s l i near wi th ash content i ndi cated that the vari ance i ncreases by 4 / 2
(Btu/l b)z per percent of ash, and that the standard devi ati on on ash-free samples
would be 106 Btu/l b.
A computer anal ysi s of the data i n which i t was assumed that the
I t i s of i nterest t o determi ne whether the remai ni ng vari ance can actual l y be
attri buted to the l aboratory determi nati ons. The l atter can be esti mated accordi ng
to -
Var (exp) = Var Q +198.11' Var C +62U.312 Var H
+80.932 Var s +44.95' Var A
6)
where Var Q, Var C, etc. , are vari ances of the respecti ve determi nati ons. Some
preci si on data have become avai l abl e from the HYGASO program at I GT, which can be
used f or a test.
Sources of vari ance of the experi mental determi nati ons need to be considered f or
the purpose at hand. The heati ng val ue and the anal yti cal determi nati ons (carbon,
hydrogen, sul f ur, and ash) are al l run on a sample of coal (or char) thdL has been
ground f i ner than 60-mesh si eve si ze. Thus, the vari ance from sampling of the coarse
sample submi tted to the l aboratory i s not of concern. I f the moi sture content does
not change duri ng al l of the sample wi thdrawal s f or the vari ous determi nati ons, no
vari ance i s contri buted by the moi sture determi nati on; however, i f several days
el apse between heati ng val ue and carbon-hydrogen determi nati ons, a contri buti on from
thi s source is l i kel y, ei ther from the change i n moi sture or from the vari ance of i ts
redetermi nati on. Vari ance can al so be contri buted by day-to-day vari ati ons i n equip-
ment and operator; thus redetermi nati on on the same day would not serve the purpose.
I nstead, our procedure consi sted of resubmi tti ng from ti me to t i me a number of ground
samples of coal (i n the same 4-02 bottl es as ori gi nal l y sampled from) f or redetermi -
nati on of moi sture, heati ng val ue, carbon, hydrogen, sul f ur, and ash. Each reported
val ue f or carbon, hydrogen, ash, and heati ng val ue i s the average of two determi-
nati ons run at the same ti me; f or sul f ur onl y one determi nati on is made. Completion
of the dupl i cate anal ysi s ranged from 9 to 46 days af ter completion of the routi ne
anal ysi s. Sl i ght average changes i n val ues from the ori gi nal anal ysi s to the dupl i -
cate, such as an average decrease i n heati ng val ue of 13 Btu/l b, occurred; the
standard devi ati ons were cal cul ated both wi th and wi thout correcti on f or thi s bi as.
The dupl i cate di f f erences from thi s program were examined f or outl i ers. Three
sul f ur, one ash and one heati ng val ue, al l wi th di f f erences between dupl i cates
greater than 3.8 J2 u, were di scarded.
di f f erence of 2.8 J2 a, and al so havi ng a di f f erence between observed and cal cul ated
val ues of 3.5 a was al so di scarded.
sented i n Table 3.
I n addi ti on, a heati ng val ue wi th a dupl i cate
The anal ysi s of the remaining data i S pre-
238
The vari ance contri buted to the di f f erence between observed and cal cul ated
heati ng val ues by the vari ance of the experi mental determi nati ons can now be cal cu-
l ated accordi ng to Equation 6.
(Table 3) yi el ds the val ue 64 Btu/l b as the expected 0. Thi s represents 77% of
the vari ance found f or a l arge set of routi ne HYGAS data on r aw bi tumi nous coal
di scussed l ater i n thi s paper. The remainder of the vari ance can be attri buted
t o the ef f ect of outl yi ng l aboratory determi nati ons, and the ef f ect of mi neral
matter .
The standard devi ati ons af ter bi as correcti ons
Tabl e 3. SUMMARY OF HYGAS REPEATMILITY DATA
1
Standard Deviation**
No. of 'Average Before Bi as After Bias
Dupl i cates Value Bias* Correcti on Correcti on
Btul l b
W t %
Heating Value 56 11680 13 29 27
Carbon 41 64.07 0.037 0. 25 0.24
Hydrogen 41 4.52 0.028 0.051 0,051
Sul tur 55 4.39 -0.011 0.084 0.086
Ash 40 16.77 0.037 0.14 0. 14
*
**
Ori gi nal minus dupl i cate
Of reported val ues, each the average of two determi nati ons run at
the same t i me, except si ngl e determi nati ons f or sul f ur.
TEST AND USES
Data f or testi ng of the new formula were sol i ci ted from outsi de l aboratori es.
Resul ts from two l aboratori es presented i n Tabl e 4 show good preci si on, but the
l arge bi as val ues suggest the presence of systemati c error or di f f erence from the
ori gi nal data.
Resul ts from a thi rd l aboratory i l l ustrate an i mportant use of the formula. The
experi mental data covered a peri od of several years and were furni shed i n the sequence
i n which they were obtai ned by the l aboratory.
over 35% ash or less than 3% oxygen, because the l atter are l i kel y to be chars. On
the remaining data, the standard devi ati ons obtai ned from consecuti ve sets of 50
samples are shown i n Fi gure 1. On the f i r st 650 samples the bi as was 32 Btu/l b and
the standard devi ati on was 136 Btu/l b, i n good agreement wi th resul ts on the ori gi nal
data bank. On subsequent samples the resul ts i ndi cate a substanti al deteri orati on i n
l aboratory preci si on. Thus, a control chart of thi s ki nd can serve as a monitor of
l aboratory performance. Also, the di f f erence between observed and cal cul ated heati ng
val ues on an i ndi vi dual sample can be used by the l aboratory supervi sor as a cri teri on
of acceptabi l i ty of the heati ng val ue and carbon-hydrogen determi nati ons.
di f f erence is less sensi ti ve t o the sul f ur and ash val ues.
We el i mi nated a few samples havi ng
The
239
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241
Another i mportant use of a heati ng val ue formula is i n computer modeling of coal
conversi on processes.
char obtai ned at IGT under the HYGAS pi l ot pl ant program were anal yzed f or thi s pur-
pose. I n the HYGAS process, non-agglomerating coal s are dri ed but are not otherwi se
pretreated.
destroy thei r aggl omerati ng properti es. The resul ti ng product i s ref erred to here as
"pretreated coal " rather than "char". Samples ref erred to as "chars" are from later
i ntermedi ate stages or are spent (resi due) char. Ash i n the spent char from the runs
on bituminous coal averaged 36X, but ranged up t o about 85%. To augment the data from
runs on subbituminous and l i gni te coal s, we have added some samples taken from streams
that contai n feed coal i n addi ti on to char, such as the dust col l ected by a cyclone i n
the reactor product gas stream. Resul ts are presented i n Table 5, together wi th those
obtai ned on the ori gi nal data bank.
Data on heati ng val ue and composition of samples of coal and
Bituminous coal s are pretreated at temperatures of 750F to 800'F to
'Themost i mportant cri teri on f or use of a heati ng val ue formula i n a computer
model of a coal conversi on process is the bi as or average di f f erence between observed
and cal cul ated val ues, because i t shows how cl osel y the formula represents the prop-
erti es of the coal . On the 294 samples of r aw (untreated) bituminous coal s, the
cal cul ated val ues are, on the average, 18 Btu/l b l ess than the observed val ues. Thi s
di f f ers by onl y 8 Btu/l b from the val ue found on t he 406 samples of bituminous coal
i n the ori gi nal data bank. There i s onl y about a 20 percent chance that the di f f er-
ence is si gni f i cant; i f s o , i t can be attri buted to a sl i ghtl y lower ash content
obtai ned at I GT , because at IGT the amount of sul f ur tri oxi de i n ash is routi nel y
determined and deducted from the reported ash. Ash as customari l y determined i s
l i kel y t o contai n small amounts of sul f ur tri oxi de.
The standard devi ati on shown f or these coal samples is substanti al l y less than
was found on the bi tumi nous coal s of the ori gi nal data bank. The di f f erence may be
a resul t of the l i mi ted range of source of the HYGAS samples: al l were from the
I l l i noi s No. 6 seam and 95% were from a si ngl e mine; the ash content averaged 10.7L.
(The samples from the repeatabi l i ty set of data had hi gher ash, averagi ng about 17%).
On pretreated bi tumi nous coal the cal cul ated val ues are, on the average, 157 Btul l b
lower than the observed val ues. The Data Book formula i s thus unsati sf actory f or use
i n a computer model appl i ed to thi s materi al ; f or such use a bi as correcti on can be
appl i ed or a formula can be obtai ned by regressi on anal ysi s of the pretreated coal
data. The di f f erence i n bi as between the parent and pretreated coal , 139 Btu/l b, can
be attri buted to a di f f erence i n structure (bondi ng); the formula has al ready taken
i nto account di f f erences i n el emental composition. Such di f f erences i n structure
i ncl ude ef f ects of i ncorporati on of oxygen i n a di f f erent form from that ordi nari l y
present. I n other processes the di f f erence i n bi as may be greater or l ess, depend-
i ng on processi ng condi ti ons such as temperature and presence or absence of oxygen;
i n the HYGAS process the di f f erence i s reduced t o about 40 Btu/l b at the stage where
the temperature reaches about 1200F.
on the average, onl y 28 Btu/l b less than the observed val ues; the di f f erence i s of
about the same order f or chars from subbituminous coal and l i gni te.
formula could be obtai ned f or the chars from the bituminous coal , but the Data Book
formul a should be adequate f or most practi cal purposes; the accuracy shoul d be judged
accordi ng to uni t weight of coal feed rather than uni t weight of char.
On the set of sampl es of char from bi tumi nous coal s the cal cul ated val ues are,
A more accurate
CONCL USI ONS
A new fi ve-term formul a f or cal cul ati ng the heati ng val ue of coal from i ts car-
bon, hydrogen, sul f ur and ash content was obtai ned by regressi on anal ysi s of data on
775 sampl es of U. S. coal s of al l ranks. The standard devi ati on of the cal cul ated
val ue from the observed val ue was 129 Btu/l b, compared t o apparent standard devi ati ons
rangi ng from 178 to 229 Btu/l b obtai ned from the Dulong, Boie, Grummel and Davis,
and Matt and Spooner formul as.
An anal ysi s of the vari ance of the di f f erence between
242
Table 5. TEST ON HYGAS ROUTI NE SAMPLES OF THE DATA BOOK FOKMULA
FOR CALCULATION OF HEATING VALUE
No. of
Standard Devi ati on
Before Bias After Bias
\ HYGAS Data Bank
Samples Ui asd Correcti on Correcti on
Btufl b
Bituminous Coala
Raw Coal 294 18 73 71
Pretreated Coal 572 157 174 76
Chars
Fi rst Stage Hydrogasi fi cati on 105 58 98 79
Second Stage Hydrogasi fi cati on 106 2 106 106
Spent Char 5 70 28 97 Y2
A l l Char 781 28 98 94
Subbituminous Coalb
Coal
Chars
Mixtures of Coal and Char
Lignite'
Chars
Mixtures of Coal and Char
49 -47 69
80 15 59
66 15 55
80 34 78
44 12 88
21
57
53
77
7 1
Ori gi nal Data Bank
Bituminous Coal 406 10 124 124
Subbituminous Coal 180 13 140 140
L i gni te 149 -45 137 137
A l l Samples, I ncl udi ng Anthraci te 775 0 129 129
a From I l l i noi s No. 6 seam. About 1/8 of the samples were from runs on hvBb
coal from Sal i ne County, and the remainder from runs on hvCb coal from Chri sti an
County.
From the Rosebud Seam, Rosebud County, Montana.
From the Savage Mine, Richland County, Montana.
Average observed val ue minus average cal cul ated val ue.
243
observed and cal cul ated val ues obtai ned wi t h the new formula on I GT coal data
i ndi cated that at l east 77% i s contri buted by the vari ance of the experi mental deter-
mi nati ons; the remainder can be attri buted to the ef f ect of mi neral matter and out-
l yi ng experi mental determi nati ons.
Appl i cati on of the formul a to coal oxi dati vel y pretreated at 750F to 800F to
destroy aggl omerati ng properti es yi el ds a bi as i ndi cati ng that its heat of formation
is hi gher than expected from el emental and ash composi ti on by about 140 Btu/l b; thi s
i s attri buted to di f f erences i n structure (bonding) of the pretreated coal i n comparison
to unpretreated coal . The formula gi ves sati sf actory resul ts on hi gher temperature
HYGAS chars, and, wi th appl i cati on of a bi as correcti on, on pretreated coal
Thus, the formula is advantageous f or use i n the compvtei- model l i ng of coal con-
versi on processes and f or moni tori ng test data on coal and char.
Acknowledgement
The work reported her e was conducted as part of a proj ect, sponsored by the
U. S. Department of Energy, on preparati on of a Coal Conversion Systems 'Technical
Data Book. Use of data obtai ned under the HYGAS program i s gratef ul l y acknowledged.
LITERATURE CI TED
1.
2.
3.
4 .
5.
6.
7.
8.
9.
10.
11.
12.
Sel vi g, W. A. and Gi bson, F. H. , "Cal ori f i c Value of Coal ," i n Lowry, H. H. , 1-d.,
Chemistry of Coal Uti l i zati on 1, 139. New York: J ohn Wiley, 1945.
Subramaniam, T. K . , "How to Cal cul ate Btu '?slues of Coal ," Coal Age, g, 153-58
(1977) December
Lloyd, W. G. and Franci s, H. E., Personal Communication, 1979.
Lloyd, W. G. and Davenport, D. A., "Applying Thermodynamics to Fossi l Fuel s,''
J . Chem. Ed. 57, 56-60 (1980) J anuary.
Spackman, W.
Report" ERDA No. FE-0930-2, NTIS, Spri ngf i el d, Va. 1976.
Swanson, V . E. et., "Col l ecti on, Chemical Anal ysi s, and Eval uati on of Coal
Samples i n 1975," U.S. Department of the I nteri or, Geol ogi cal Survey, Open-File
Report 76-468, 1976.
Gilmour, E. H. and Dahl , G. G. , J r., "Montana Coal Anal yses," Bur. Mines Geol.
Spec. Publ . 43. Butte, Mont. 1976.
Gl ass, G. B. , "Analyses and Measured Secti ons of 54 Wyoming Coal Samples (Col-
l ected i n 1974)," Geol ogi cal Survey of Wyoming Rep. I nvest. No. 2. Laramie,
Wyo. 1975.
Sondreal , E. A . , Kube, W. R. and El der, J. L., "Anal ysi s of the Northern Great
Pl ai ns Provi nce L i gni tes and Their Ash," U.S. Bur. Mines Rep. I nvest. No. 7158.
Washington, 1968.
I nsti tute of Gas l echnol ogy, "Coal Conversion Systems Techni cal Data Book,"
U.S. Department of Energy NO. HCP/T2286-01, supt. of Documents, Washington, D.C.
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