Fuel 101 (2012) 8489

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Fuel
journal homepage: www.elsevier.com/locate/fuel

Small-scale co-utilisation of coal and biomass

Michal L. Kubacki , Andrew B. Ross, Jenny M. Jones, Alan Williams
Energy and Resources Research Institute, School of Process, Environmental and Mechanical Engineering, University of Leeds, Leeds LS2 9JT, UK

a r t i c l e

i n f o

Article history:
Received 1 September 2010
Accepted 23 June 2011
Available online 25 August 2011
Keywords:
Co-combustion
Co-pyrolysis
Emissions
VOC
PAH

a b s t r a c t
Co-utilisation of coal and biomass for energy production results in pollutant reduction. Most notable is
the impact on NOx, SOx, volatile organic compounds (VOC) and polyaromatic hydrocarbons (PAH). The
aim of this study is to improve our understanding of the synergy in toxic organic emission reduction from
co-ring or co-gasifying coal and biomass. Co-combustion was studied by TGA and by burning briquettes
supported on a needle in a methane air ame. A range of coals of varying rank, different biomass, as well
as model compounds were used. Results show that non-additive combustion behaviour is not easily
explained by studying devolatilisation because of the difculty in replicating the conditions of temperature prole and residence time experienced by the volatiles. Thus, conicting behaviour is exhibited
depending upon pyrolysis technique. However, the atmosphere during experiments appears to be more
important. Non-additive combustion for both powdered and pelletised fuels was seen by TGA and studies
in a methaneair burner. The coal ignites and burns at a lower temperature because of the interaction
with the biomass volatile combustion region. Thus it is proposed that the reduction in emissions from
co-combustion arises from enhanced reaction of the coal volatiles by mixing with biomass volatiles in
a hot oxidising atmosphere.
2011 Elsevier Ltd. All rights reserved.

1. Introduction
The co-utilisation of coal and biomass for energy production results in pollutant reduction. Most notable is the impact on the
emission of NOx, SOx and volatile organic compounds (VOC) and
polyaromatic hydrocarbons (PAH) [14]. These latter compounds
arise largely from their formation and release during incomplete
combustion/gasication. PAH are particularly toxic carcinogens
and are listed by the United States Environmental Protection
Agency (USEPA) and the European Community as priority pollutants. There is evidence that co-ring or co-gasifying coal and biomass results in a signicant decrease in the emission of these
compared to coal alone. This is illustrated by our work for a
30 kW xed-bed domestic boiler [5]. The reduction in NOx is
thought to be due to competitive char burnout, while the reduction
in SO2 can be explained by sulphur xation in the ash due to the
increase in potassium and calcium from the biomass.
The synergistic activity observed for toxic organic emissions is
not well understood and involves chemical interaction between
the volatiles from each fuel coupled with possible catalytic activity
from the inorganic constituents of the fuels. Laboratory scale data
on synergies in co-pyrolysis is conicting. Several authors have reported non-additive behaviour [611] and previously [12] we have
observed that the volatile products from coal and from biomass
can interact with one another to produce a very different product
Corresponding author.
E-mail address: m.l.kubacki@leeds.ac.uk (M.L. Kubacki).
0016-2361/$ - see front matter 2011 Elsevier Ltd. All rights reserved.
doi:10.1016/j.fuel.2011.06.034

prole compared to those of either fuel pyrolysed individually,

which indicates the presence of labile species. In contrast, often
only additive behaviour has been reported [11,1316].
Thus, the reason for reduced organic emissions during co-utilisation in small scale appliances remains elusive. The question of
whether, and under what circumstances, volatiles from one fuel
interact with another has not been fully addressed. Thus, the aim
of the present study is to improve our understanding of the nonadditive behaviour of coal/biomass devolatilisation. This work is
of particular relevance to xed bed and uidised bed processes
where the bed temperature is ca. 1000 C (or there is a temperature
prole through the bed). In these cases particle heating and pyrolysis occurs relatively slowly and interaction between the volatiles
is possible.
The following parameters were studied (i) the effect of coal rank
and biomass type, (ii) the effect of minerals from one fuel in the
blend inuencing the other, (iii) the effect of pelletising, (iv) the effect of heating rate. This paper gives a selection of results from a
large parametric laboratory-scale study of co-pyrolysis and cocombustion [17]. The results are chosen to highlight instances
where non-additive behaviour was observed in comparison with
cases where additive behaviour was observed.
2. Experimental
A range of coals of varying rank and different biomass (with
varying inorganic content) were used in this work and their properties are summarised in Table 1. The proximate analysis was

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M.L. Kubacki et al. / Fuel 101 (2012) 8489

Table 1
Analysis of the fuels studied for additive versus non-additive behaviour.
Material

CVa

Ultimate analysis, % daf

H2O

VM

FC

Ash

HHV MJ/kg

Ob

Coals
Turoszow
Wujek
Kaltim Prima
Hambach
Julian

2.3
1.5
2.9
17.0
3.2

42.7
32.5
39.6
48.7
34.2

24.9
45.8
50.7
27.7
56.6

30.0
20.2
6.8
6.6
6.00

28.98
28.97
30.32
24.02
33.65

69.35
74.05
73.40
57.68
81.85

6.53
4.60
5.51
6.48
5.35

28.73
16.26
16.05
35.39
12.96

0.69
1.14
1.60
0.77
1.34

Biomass
Pine sawdust
Oat straw

3.6
2.2

80.5
67.6

14.5
26.2

1.4
4.0

22.82
19.72

53.12
47.81

7.10
6.59

41.60
41.19

0.49
0.70

S
0.65
1.19
1.94
0.12
0.50
<0.2
<0.2

Calculated according to Chaniwala and Parikh, Fuel 81 (2002) 10511063.

Measured oxygen.

60
-0.2
Kp

40

Kp & Oat

20

-0.3

Oat

0
0

100

200 300

400

500

600 700

800

-0.4
900

66

(a)

70
60
50
40
30
20
10
0

Kp

Temperature ( C)

60
-0.2
Hdm
Hdm & Oat
Oat

20

100

200

-0.3

300

400

500

600

700

800

-0.4
900

Temperature ( C)
Fig. 1. Mass loss and DTG curve of (a) Kaltim Prima (Kp), oat straw (Oat) and their
blend (Kp and Oat) and (b) Hambach demineralised (Hdm), oat straw (Oat) and
their blend (Hdm and Oat) as a function of temperature (25 C/min).

66
61

70
60

Oat
Theoretical

54

-0.1

Volatile matter % (dry) .

Mass (%)

80

(b)

0.0

100

40

Kp & Oat
Experimental

DTG (%/s)

(b)

53

-0.1

Figs. 14 give example comparisons for coalbiomass blends

where either non-additive or additive behaviours were observed.
Fig. 1 displays the TGA and derivative plot (DTG) for two different
coals blended with oat straw, while Fig. 2 summarises the measured and theoretical volatile matter yields. Repeat experiments
were performed to assess the error in the measured yields and
these are indicated in the gure caption. The results for the

60

Mass (%)

80

3.1. Pyrolysis tests

57

0.0

100

3. Results

DTG (%/s)

(a)

0.30.6 g in a 13 mm dye using a SPECAC press (10 t/in.2 for

60 s). Pieces from the pellets were used for STA and ame studies.
A study was also undertaken of the role of inherent minerals in copyrolysis and co-combustion. In this case, fuels were also studied
in a demineralised form. Here, demineralisation refers to washing in 2 M HCl. While this is not expected to remove all minerals
from the fuels, the successful removal of some of the key catalytic
components has been established [19,20].

39

conducted via thermogravimetry, and the ultimate analysis using a

CE Instruments Flash EA 1112. The straws, grasses and energy
crops were provided by Rothamsted Research, and the coals were
from the BCURA coal bank and from Institute for Chemical Processing of Coal, Zabrze, Poland.
Thermal behaviour was studied by in a Stanton Redcroft Simultaneous Analyser STA-780 Series in nitrogen at 25 C/min to 900 C
for pyrolysis proles, and in oxygen for burning proles. To study
thermal behaviour at higher heating rates, commercial CDS pyroprobe units (both 1000 and 5000 models) were applied, interfaced
to GCMS (Shimadzu 2010) or FID detectors (Perkin Elmer 8700
GCFID).
The third high heating rate study involved supporting particles
of 23 mm diameter in a platinum mesh basket supported in a
methaneair ame. A retractable water-cooled sheath surrounded
the basket at the start of the experiment. The thermal conversion
was followed by high speed video (Photo-Sonics Phantom V7) once
the sheath was retracted. Further details of this experimental setup and methodology can be found in Jones et al. [18].
Fuels were studied individually as well as in 50:50 mixtures,
both as loose powders and as pellets. Pellets were prepared from

Volatile matter % (dry) .

a
b

Proximate analysis (TGA) a.r.

50
40
30
20
10
0

Hdm

Hdm & Oat

Experimental
Theoretical

Oat

Fig. 2. Experimental and theoretical volatile matter yields during TGA pryolysis of
oat blended with either (a) Kaltim Prima (absolute error in the blend yield is 1.6%)
or (b) demineralised Hambach (absolute error in the blend yield is 0.1%).

86

M.L. Kubacki et al. / Fuel 101 (2012) 8489

demineralised Kaltim Primaoat straw blend indicate slight nonadditive behaviour, whereby the blend has a higher volatile yield
than expected on an additive basis. Higher gas yields have been reported [68]. The demineralised Hambachoat straw blend displays only additive behaviour.
Further evidence for increased volatile yield for the Kaltim Primaoat straw blend is seen in the evolved gas/volatile analysis,
where higher yields were observed than expected on an additive
basis. Example traces are shown in Fig. 3. Note that intensities
are normalised per mg of sample, and the blend contains 0.5 coal
and 0.5 biomass. Thus, for species such as methanol and formic
acid, which only arise from the biomass, we would expect lower
gas/volatile yields for the blends, compared to the biomass alone.
The apparent rst order kinetics for the decomposition of the
biomass and coal were computed from Fig. 1 and the ndings are
displayed in Fig. 4. The biomass decomposition in the Kaltim Primaoat straw blend appears faster than when oat straw is studied
individually. In contrast, the biomass decomposition rate in the
Hambachoat straw blend occurs with a very similar kinetic rate
to that observed when it studied alone.
In summary, in mixtures with oat straw some non-additive
behaviour was observed in pyrolysis. This comprised of a very
slight increase in the volatile matter yield and indications were
that the gas and light volatiles yields were most affected. Thus,

even though the decomposition steps might be well separated,

slight non-additive behaviour was often observed in the kinetics
of biomass pyrolysis in blends with oat straw. For mixtures with
pine (not shown) purely additive behaviour was observed regardless of the coal and pre-treatment (e.g. demineralisation). Oat
straw is high in potassium, a known catalytic metal in pyrolysis
reactions, and one which can increase the gas yield [19,21], hence
the inuence of inherent mineral was also investigated. Oat straw
was ashed at 550 C and this ash was mixed with various coals
which were then studied in pyrolysis. Fig. 5 shows the pyrolysisGCFID analysis of products from pyrolysis of this mixture, and
some indication of increased production of light hydrocarbons is
evident.
3.2. Combustion tests
Our original assumption in this study was that non-additive
behaviour occurred in the vapour phase due to mixing and reaction
of the hot volatiles above the bed of a combustion unit. While some
evidence of non-additive behaviour was present for coal blended
with oat straw, changes were small. Therefore, it was proposed
that the presence of combustion impacts on the reaction of the volatiles. It is probable that the passing of pyrolysis products through
high temperature regimes or through the high temperature char

Methanol

1.0E-03

Methanol

1.0E-03

Hdm
Hdm & Oat

Kp
Kp & Oat
Oat

5.0E-04

7.5E-04

Intensity

Intensity

7.5E-04

Oat

5.0E-04
2.5E-04

2.5E-04

0.0E+00

0.0E+00
0

100 200 300 400

500 600 700 800 900

500 600 700 800 900

Temperature ( C)

Temperature ( C)
Formic acid

7.5E-04

100 200 300 400

Formic acid

7.5E-04

Hdm

5.0E-04

Oat

2.5E-04

Intensity

Intensity

Kp
Kp & Oat

Hdm & Oat

Oat

5.0E-04

2.5E-04

0.0E+00

0.0E+00
0

100

200 300 400

500 600 700

800 900

Temperature ( C)

CO

1.5E-03

Kp
Kp & Oat
Oat

5.0E-04

Hdm
Hdm & Oat
Oat

1.0E-03

Intensity

Intensity

CO

1.3E-03

1.0E-03

100 200 300 400 500 600 700 800 900

o

Temperature ( C)

7.5E-04
5.0E-04
2.5E-04
0.0E+00

0.0E+00
0

100 200 300 400

500 600 700 800 900

o

Temperature ( C)

100 200 300 400

500 600 700 800 900

o

Temperature ( C)

Fig. 3. Evolved gas analysis during the pyrolysis and co-pyrolysis of Kaltim Prima (Kp)oat straw blends (LHS column) and demineralised Hambach (Hdm)oat straw blends
(RHS column).

87

M.L. Kubacki et al. / Fuel 101 (2012) 8489

(a)

(a)

-4.0

558

-4.5

554

-5.0

ln k

Kaltim Prima

562

550
-5.5

546

-6.0

542

-6.5

538

-7.0
0.0013

5 10 15 20 25 30 35 40 45 50 55 60 65

Time (min)
0.0014

0.0015

0.0016

0.0017

0.0018

-1

1/ T (K )
Kp
Kp & Oat coal peak

(b)

Kp & Oat biomass peak

Oat

Kaltim Prima & Oat ash

565
560
555
550

-4.5

545

-5.0

540
0

-5.5

5 10 15 20 25 30 35 40 45 50 55 60 65

Time (min)

-6.0

Fig. 5. Pyrolyis-GC-FID of light hydrocarbons produced from (a) Kaltim Prima and
(b) a blend of Kaltim Prima and oat straw ash. Both gures are on the same scales
and similar total mass was used (i.e. the amount of coal used is lower in (b)).

-7.0
0.0013

0.0014

0.0015

0.0016

0.0017

0.0018

-1

1/ T (K )
Hdm
Hdm & Oat coal peak

Hdm & Oat biomass peak

Oat

Fig. 4. Apparent rst order reaction kinetics for the pyrolysis of (a) Kaltim Prima
oat straw blends and (b) demineralised Hambachoat straw blends. Both coal
pyrolysis and biomass pyrolysis kinetics are shown.

bed or through regions of varying gas composition impacts on the

interaction and reaction of the volatile species. Hence the processes of pyrolysis and combustion are linked and as such need
to be studied together. As a rst investigation of this, the fuel mixtures were studied by temperature programmed combustion
experiments in a simultaneous thermal analyser.
Fig. 6 gives example of the type of synergy observed. In the
majority of cases studied, combustion was non-additive. The initial
(mainly biomass) decomposition and volatile combustion is delayed (i.e. occurs at higher temperature), and the char combustion
peak begins earlier (i.e. at lower temperature) compared to the
individual fuels. The overall duration of char combustion is shortened very slightly, although for the Wujek-pine blend this was not
observed. Volatile combustion peaks overlap each other and the
ash yield of the blends shift towards the coal ash yields. This is
probably due to components in coal ash xing volatile components
from the biomass ash. Similar results are observed for pelletized
blends, and for both oat straw and pine.
In addition to TGA studies, small pieces of briquettes were
burned in a methaneair ame and the combustion was interrogated by high-speed video capture, as illustrated in Fig. 7. The
duration of the volatile combustion ame was measured as a function of particle mass and the results are shown in Fig. 8. A best t
trend line was added for each of fuels. These plots also contain a
supplementary additive (add) function, which simulates the
location of the trend line of the blend if the reaction was proceeding in an additive manner. This line is calculated from the curves
produced by the parent fuels. Analysis of Hambach, oat straw
and their blend (Fig. 8a) reveals quite unexpected results for the

blend. The observed combustion time shifts towards the combustion time of the coal. It appears, the volatile release and combustion are slower than expected. This may be the result of different
pellet density for the blend, compared to the individual fuel, which
affects either the heating up of the pellet and/or the diffusion of
volatiles from the pellet. When Hambach was blended with demineralised oat straw, the images showed distinctly different combustion behaviour (Fig. 8b). The pellet of Hmb and Odm
undergoes volatile combustion at the same rate as Hambach coal,
while the Hmb and Oat blend has accelerated volatile combustion
relative to the coal, although the latter is still slower than would be

Time (min)

(a)
0.0

DTG (%/s)

-6.5

10

15

20

25

30

-0.2
Kp
Kp & Oat
Oat

-0.4

-0.6

(b)

Time (min)
0.0

10

15

20

25

30

-0.2

DTG (%/s)

ln k

(b)

-4.0

-0.4
-0.6
-0.8

Hdm
Hdm & Odm
Odm

-1.0
Fig. 6. Temperature programmed combustion, derivative weight loss curves for (a)
Kaltim Primaoat straw blends and (b) demineralised Hambachoat straw blends.

88

M.L. Kubacki et al. / Fuel 101 (2012) 8489

(a)

14

Mass (mg)

Fig. 7. Combustion of Hambach and oat straw: (a) 0 s shroud is slid off, (b) 2.06 s fully developed ame of volatiles, (c) 5.44 s volatile ame extinguishes, (d) 44.84 s
char burnout, slow shrinking, (e) 112.95 s char burnout, shrinking continuous, (f) 173.09 s bubbling ash nearly completely evaporates.

10

Hmb pt
Hmb & Oat pt
Hmb & Oat pt add
Oat pt

12
8
6
4
2
0

(b)

14

Mass (mg)

Time (s)

10

Hmb pt
Hmb & Oat pt
Hmb & Odm pt
Oat pt

12
8
6
4
2
0

Time (s)
Fig. 8. Volatile matter combustion time of (a) compressed Hambach (Hmb), oat
straw (Oat) and their blend, where: pt pellet and add is the calculated value; (b)
comparison with Hambach (Hmb) and demineralised oat straw (Odm) blend.

expected on an additive basis. Clearly, the minerals in oat straw

catalyse the volatile combustion of the blend with Hambach.
4. Discussion
For a xed-bed furnace [22], mechanisms for pollutant formation have been proposed to include a number of routes including:
(a) escaping of pyrolytic devolatilisation products round the outside of the ame; (b) partial pyrolysis in which released volatiles
react further including polymerisation of oxygenates; and (c)
complete breakdown of the volatiles to smaller fragments such as

acetylene followed by C2/C4 addition to form larger PAH and soot.

Sjostrom et al. [23] speculate that synergy in tar formation during
co-gasication of coal and biomass in a pressurised uidised bed
reactor, might result from initiation of coal decomposition by biomass decomposition radicals, this proposal being similar to route
(b) above. They also cite possible termination of recombination
reactions by light gases and hydrogen, and the work presented here
indicated a slight increase in this fraction of the volatile matter during co-pyrolysis. The possibility of alkali metal catalysed gasication reactions are also noted [22], and some evidence in support
of this has been presented here. However, our results indicate that
interaction and reaction of volatiles in the pyrolysis stage is not expected to be a major mechanism for pollutant reduction. Both low
heating rate TGA, batch reactor [17] and high heating rate (pyroprobe, wire mesh reactor [17]) studies as well as long and short residence time investigations support this conclusion. However,
oxidative pyrolysis would be needed to clarify if route (b) was a signicant possibility and this is suggested for future work.
In the combustion studies presented, the behaviour of the
blends display properties that are shifted towards those for the
coal alone and volatiles burn longer than expected. This may
change the temperature prole in the bed as observed experimentally [22] and impact on emissions. Some speculation for the inuence of co-combustion on pollutant formation via route (c), above,
can be made. During the co-combustion of coal and biomass in briquetted form, two effects have been reported the effect of biomass addition to coal combustion and the effect of the
briquetting process [22]. Both these effects have been seen in this
work whereby earlier ignition of biomass assists the ignition of
coal, and briquetting can result in a large overlap of the volatile
and char combustion stages. Studies of temperatures in a domestic
xed bed boiler [22] found that biomass burns at a lower temperature, and adding biomass to coal reduces the temperatures both
above and within the bed. It was proposed that this was mainly
a result of the lower caloric value of the fuel. However, the thermal analysis studies indicated that briquetting also affects the
burning rate, the volatile content and the rate of release. These factors can inuence the heat prole in a xed bed. Therefore it is possible that this, combined with the large amounts of oxygenated

M.L. Kubacki et al. / Fuel 101 (2012) 8489

volatiles (from the biomass) decreases the production of volatile

organic compounds and PAH/soot via the C2/C4 addition route.
5. Conclusions
The synergy observed in the organic emissions during the combustion of coal and biomass in small appliances is not simply due
to interactions of hot volatiles from coal and biomass above the
combustion bed. Co-pyrolysis studies suggest biomass type can
lead to a small affect on the rate of the coal pyrolysis, and on the
total volatile matter released, but that there are no gross changes
in the nature of the volatiles. Combustion studies indicate that
strong synergy can be observed, and the coal ignites and burns at
lower temperature as a result of the earlier ignition and combustion of the biomass. The overall combustion time is still dominated
by the coal char burn-out. Thus, the processes of pyrolysis and
combustion are linked and as such need to be studied together.
Acknowledgements
The authors are grateful for nancial support from the EPSRC
(GR/S01221) and for the loan of the high speed digital video camera from the EPSRC equipment pool.
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