Paper no.

<3132281>

APCChE 2015 Congress incorporating Chemeca 2015

27 Sept 01 Oct 2015, Melbourne, Victoria

Atmospheric Emissions from the Co-Combustion of Biomass Tars and

Synthesis Gas during Biochar and Bioenergy Production
Lewis Dunnigan1*, Peter Ashman1, Xiangping Zhang2, Chi Wai Kwong1
1
2

The University of Adelaide, Adelaide, SA 5000, Australia

Institute of Process Engineering, Chinese Academy of Sciences, Beijing, China
Corresponding author. Email: lewis.dunnigan@adelaide.edu.au

Abstract: Small, distributed biomass energy and biochar production systems using pyrolysis is one of
the potential options to effectively process and utilize biomass resources on site of cultivation. Cocombustion of the biomass tar and synthesis gas products in a small pyrolysis system enhances
energy output and avoids the need for tar handling. An experimental study was performed using rice
husk as the feedstock to evaluate the co-combustion performance of biomass tar and synthesis gas in
a laboratory-scale pyrolysis-combustion facility. Atmospheric emissions, including PM and gaseous
pollutants, resulting from the co-combustion process were determined. The results were used to
estimate the emissions associated with biochar production. It was found that coarse particles (PM10)

resulting from the combustion of biomass tar in a low temperature combustion environment (850 C)
dominate the mass-size distribution of the particulate emissions. Even though a high ash content
feedstock (rice husk) was used in this study, the PM emission factor of this co-combustion method
was substantially lower than the conventional solid or liquid fuel combustion process due to the
separation of ash in the solid product. However, the high ash content of the feedstock would influence
the emissions associated with biochar production for carbon sequestration.
Keywords: biomass, biochar, distributed approach, co-combustion, renewable energy, emissions, PM,
flue gas.

1 Introduction

In the world today there are approximately 1.4 billion people who live without easy access to
electricity. The majority of these people live in isolated and rural communities [1]. It has been
suggested that wastes from agricultural processes can be used to produce sustainable energy, as the
carbon emitted during combustion of these feedstocks is taken up by the re-growing biomass in a wellmanaged growth and use cycle [2]. These waste products can also be converted into biochar, a solid
product of biomass pyrolysis. Biochar has the potential to offset CO2 emissions by sequestering
carbon. In addition, when it is added to soil it can improve soil fertility, increase agricultural
productivity, and reduce pressure on old-growth forests [3].
Slow pyrolysis of biomass has the potential to simultaneously produce biochar and renewable energy.
In large-scale centralised pyrolysis operations, a gas cleaning system is used to separate the liquid
products (tar/bio-oil) from gaseous products in order to generate a clean (tar-free) syngas for
combustion [4][5][6]. The heat required for the endothermic pyrolysis is then supplied by the
combustion of synthesis gas and the excessive heat can be used to provide heat for other energy
services. Even though the separated liquid can be further upgraded to produce liquid fuels for internal
combustion engines, the transportation of the low-density biomass feedstock to the centralised
pyrolysis facility and the upgrading process of the liquid pyrolysis product can offset the CO 2 neutral
benefits of biomass [5][7].
As a result, the distributed approach for the on-site conversion of biomass, and particularly for
agricultural wastes, has greater potential to minimise CO2 emissions than the centralised process as it
avoids carbon outputs from the transportation and upgrading processes. Here, instead of separating
out the tar for further upgrading, the synthesis gas and tar are co-combusted to maximize heat
generation. The advantages of doing this are the following: (1) There is no need to handle the acidic

1
486

and corrosive tar as it might be cost prohibitive and (2) The significant energy content of the tar can be
used to generate heat on-site rather than be separated out.
However, such an approach is not entirely clean as the tar is a mixture of complex organic
compounds and their combustion may result in higher particulate matter (PM) and gaseous emissions
when compared to the tar-free syngas combustion. The emissions resulting from this co-combustion
approach for biochar production and renewable energy generation are yet to be determined.
In this study rice husk was selected as the agricultural waste because of their wide availability.
Conservative estimates suggest that approximately 822 million tonnes of rice husk are produced
worldwide and about 97% of the total is produced by developing countries [8]. However, the high ash
content of rice husk makes it problematic to be utilized as a feedstock in combustion and gasification.
Currently rice husk is considered a waste that is either burnt on-site of cultivation or simply left to
naturally decompose in a landfill.
The aims of this study are to: (1) determine the influence of pyrolysis temperature on the distribution of
solid, tar, and gaseous pyrolysis products and the composition of the synthesis gas product and (2)
Determine the emission factors of PM and gaseous pollutants (CO 2 and CO) from the co-combustion
of the pyrolysis synthesis gas and tar products.

2 Experimental
2.1 Feedstock Preparation and Characterization

The agricultural waste used was rice husk, which was provided by CopRice (Leeton, New South
Wales, Australia). The rice husk was grinded and dried until the moisture content was as close to zero
as possible. This drying process would typically be done overnight for a minimum of 15 hours.
Proximate analysis of the rice husk and biochar was carried out using a thermogravimetric analyser
(TGA) (SETARAM, Labsys). Approximately 65 mg of sample was used to determine the weight
fractions of volatiles, ash, and fixed carbon according to ASTM E1131. Moisture content of the rice
husk was determined by the oven-drying method, ASTM D3173-11.

Ultimate analysis of the rice husk was carried out using a CHN determinator (LECO, TruSpec CHN).
The ultimate analysis for C, H, N, O was carried out following ASTM D5373. The oxygen content was
calculated by difference.

2.2 Pyrolysis and Combustion

Figure 1 shows the schematic diagram of the pyrolysis-combustion system in the experiments. Rice
husk, after the pre-processing stage, was loaded into a hopper and fed into the main screw at a
feeding rate of 1.5 g/min. The biomass was then transported along the entire length of the screw
reactor where it was heated. A carrier gas (N2) flowrate of 0.25 l/min was provided through the hopper
to remove any air from the system. The solid biochar product would be collected under gravity in a
char pot after the pyrolysis process. A flowrate of 0.1 l/min of N 2 was provided from the charpot to
avoid stagnation of the combustible pyrolysis gas inside the collection vessel.
The pyrolysis gas was then mixed with air in a burner situated inside a vertical 3 zone tube furnace

(Carbolite , GVC 12/1050). The combustion air was filtered with an in-line HEPA filtration unit

(Whatman , Hepa-Cap 150) before mixing.

The piping between the outlet of the pyrolysis heaters and the combustion region was maintained at

around 350 C to prevent condensation of the tar. The gaseous combustion products were contained
within a quartz tube inside the furnace.

A combination of 500 C pyrolysis and 850 C combustion temperature was chosen to represent the
conditions that would be expected in a typical small-scale pyrolysis-combustion facility located next to
a source of agricultural wastes. This temperature combination was chosen to maximise the yield of
biochar [8] and represent the wall temperature of a typical small-scale industrial boiler [9][10][11].

487

Figure 1: Schematic diagram of the pyrolysis-combustion and sampling systems (TC = temperature
control).

2.3 Pyrolysis Gas Sampling

In order to analyse the pyrolysis synthesis gas, a Teflon gas sampling bag was connected directly to
the top of the burner. Once the bag was filled completely it was connected to a micro-GC (Agilent
Technologies, 490 Micro GC) for gas analysis.
The heating value of the synthesis gas mixture was calculated using equation 1:

Where mi is the mass fraction of component i and LHVi is the lower heating value of component i
(MJ/kg).

2.4 Pyrolysis Tar Sampling

The yield of tar resulting from the pyrolysis of rice husk was obtained at 500, 600, 700, and 800 C.
Separation of the tar from the synthesis gas was achieved using a condensation train consisting of

eight 50 ml test tubes in series immersed in an ice/water mixture ( 0 C). Piping between the pyrolysis

heater and the first test tube was maintained at around 350 C to prevent condensation of the tar. The
connections between each of the test tubes were insulated. The total weight of the condensation train
was measured before and after each run. The weight of gas produced was calculated as the
difference between the amount of feed used and the combined weight of tar and biochar.

2.5 Flue Gas Sampling

The flue gas from the combustion of the pyrolysis gas was sampled from the outlet of the electric
furnace. Two separate samplings ports were positioned on the stainless steel piping between the air
dilution tunnel (ADT) and the top of the quartz pipe situated inside the furnace.

488

The CO2 analysis of the flue gas was carried out using a portable NDIR meter (CO2meter.com, CM

0017) with a resolution of 0.5 vol%. A portable CO/O 2 analyser (Bacharach, Fyrite INSIGHT Plus)
was used to analyse the CO level in the flue gas with a resolution of 5% and O2 level with a resolution
of 0.3%.

2.6 Dilution and PM Sampling

An 8-Stage Anderson cascade impactor (CI) was used to collect the PM and generate mass-size
distributions. The size range of the CI was 0.43 - 10 m. The CI was situated immediately downstream
of an ADT. The ADT was used to (1) supply a mixture of air and flue gas that had a volumetric rate of
28.3 l/min to the CI; (2) provide a dilution ratio of 8 so as to not overload the CI and (3) decrease the
temperature of the flue gas. As all of the flue gas was sampled, isokinetic sampling was not required
[12].
Quartz fiber filter papers were prepared for collection of the PM following an adapted methodology
outlined in the USEPA method 5 [13] and Method 501 [14]. The filter papers were dried and weighed
before and after the experiments and the average results from a set of three separate 30 min runs
were used.
In order to avoid resolution problems associated with the differing channel widths of the CI, a
normalised plot of the emission factors was produced using equation 2:

Where M is the mass collected in each stage of the CI, D p,u is the upper stage diameter and Dp,l is the
lower stage diameter.

3 Results and Discussion

3.1 Feedstock Characteristics

The ultimate and proximate analysis results of rice husk are shown in table 1:
a

Table 1: Proximate and ultimate analysis of the rice husk feedstock as received. by difference.
Proximate Analysis
Moisture
Volatiles
Fixed Carbon
Ash
Ultimate Analysis
C
H
N
a
O

8.1%
51.3%
17.4%
22.2%
38.1%
5.3%
0.2%
56.4%

The proximate analysis of the rice husk shows that they have a high amount of ash (22.2%), the
majority of which is silica (91.8%) [15]. The ash content of rice husk is significantly higher than other
types of biomass. Typical ash contents for other agricultural wastes vary between 0.3 8.4% [4][5].
The problems associated with fouling and slagging would therefore be an issue if rice husk is used in
other types of processes such as combustion.
The moisture content of the rice husk as received was 8.1%, which is at the low end for biomasses
typically used for biochar production (6 50%) [16][18][19]. The low moisture content, along with the
reasonably consistent aspect ratio of the grinded and sieved feedstock, meant that rice husk was
processed with relative ease, with no bridging or clumps forming.
The ultimate analysis indicated that rice husk have a relatively low C content (38.1%), when compared
to other biomass [16][17].

3.2 Biochar Characteristics

It was found that the C content of the biochar produced at 500 C was 43.5%, while the hydrogen
content was found to be 1.9%, nitrogen 0.9%, and oxygen 53.7%. Biochars produced from other forms

489

of biomass typically have a C content between 85 95% [19]. The low C content of the biochar
reflects the high ash content of the rice husk feedstock. As a result, the majority of the ash is removed
in the biochar product prior to combustion of the synthesis gas and tar mixture.

3.3 Pyrolysis Vapour Composition

100
90

Product Mass Distribution (%)

80
70
60
Gas

50

Liquid

40

Solid

30
20
10
0

500

600
700
Temperature (C)

800

Figure 2: Influence of temperature on distribution of solid, tar, and gas in pyrolysis products.

Figure 2 shows that between 500 C and 800 C the yield of tar decreases from 22.4 to 16.0%, while the
gas yield increases from 37.6 to 48.1%. This trend is consistent with other studies of biomass
pyrolysis [16][20]. Maximum yields of tar are obtained at lower temperatures as higher temperatures

(>600 C) promote secondary cracking which leads to a greater production rate and therefore yield of
gas [20].

490

30

Gas Composition (vol %)

25

20

CO
H2
CO2
CH4

15

10

500

600

700
Pyrolysis Temperature (C)

800

Figure 3: Composition of the rice husk synthesis gas (corrected to 50 vol% nitrogen) at 500, 600, 700,

and 800 C. The four main constituents of the synthesis gas (CO, H2, CO2, and CH4) are shown in
terms of their volume percentage.
Figure 3 shows that the main constituents of the synthesis gas at each temperature are CO, H2, CO2,
and CH4. It was found that CO and H2 in the synthesis gas increased significantly with the pyrolysis
temperature, while CO2 showed the opposite trend. This is due to the fact that the release of CO 2 is
mainly caused by the cracking and reforming of carboxyl groups which can be easily decomposed at

relatively low temperatures [3]. CH4 concentration was not found to vary significantly between 500 C

and 700 C, before increasing to around 6% at 800 C. It has been suggested that the secondary
reactions of volatiles at high temperatures generate mostly CO, H 2, and CH4 rather than CO2 [21][22].
Aside from the gas species presented in Figure 3, trace amounts of ethane and propane were also
detected at different temperatures. The LHV of the synthesis and carrier gas mixture increases from

around 3 MJ/kg at 500 C to 5 MJ/kg at 800 C due to the increase in H2 and CH4.

3.4 Combustion of Pyrolysis Vapour

Rice husk underwent pyrolysis at 500C and the vapour generated was combusted at 850C. This
pyrolysis temperature corresponds to a tar fraction in the pyrolysis vapour of 22.4%. The CO2 and CO
levels of the flue gas at 5% O2 were maintained at around 15 vol% and 400 ppmv respectively. This
resulted in gaseous emission factors of 626.8 mg/gsyngas/tar for CO2 and 1 mg/gsyngas/tar for CO.
Figure 4 and 5 shows the typical and normalised particle size distribution, respectively, during the
combustion of the pyrolysis vapour at 850C. It is clear that the coarse particulates ( 9 - 10 m) are
the predominant size of PM generated from the co-combustion of the tar and synthesis gas products
of rice husk pyrolysis. This result closely resembles the PM mass-size distributions found often in fueloil combustion [24][25].

491

0.45
0.4

Emission Factor (mg/gfeed)

0.35
0.3
0.25
0.2
0.15
0.1
0.05
0

0.43-0.65

0.65-1.1

1.1-2.1

2.1-3.3
3.3-4.7
Stage Size (m)

4.7-5.8

5.8-9

9-10

Figure 4: Emission factors of each size fraction of PM collected in the CI.

6

Normalised Emission Factor (mg/gfeed)

0.1

1
Stage Size (m)

10

Figure 5: Normalised plot of the emission factors of each size fraction of PM collected in the CI.

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Combustion temperature significantly affects the mass-size distribution of the particles generated.
Both unimodal distributions [26][27] and bimodal distributions [27][28] have been reported in solid fuel

combustion studies. In this study, a relatively low combustion temperature of 850 C was used to
replicate the small-scale biochar production system. This low temperature would not be sufficient to
vaporise the inorganic compounds in tar or fine char entrained with the pyrolysis vapour. Particle size
distributions dominated around 10 m are largely formed by coalescing inorganic material that is
produced as the carbonaceous char combusted [24]. However, further study is needed to investigate
the particle formation mechanism during combustion of the pyrolysis vapour.
Emission factors for PM10 and PM2.1 from the combustion of the pyrolysis vapour were estimated to be
1.87 and 0.46 mg/gfeed, respectively. This corresponds to 3.16 mg/gsyngas/tar for PM10 and 0.78

mg/gsyngas/tar for PM 2.1 as only approximately 60% of the mass of the feedstock at 500 C pyrolysis is
combusted. The PM10 and PM2.1 emission factors were compared with literature for biomass
combustion (table 2). It was found that the PM emission factors estimated in this study were in the
lower range of the literature values for solid biomass combustion even though a high ash feedstock
(rice husk) was used. This is because most of the ash was pre separated in the biochar and not
involved in the combustion process.
Table 2: Emission factors of PM generated from different feedstocks and combustion devices.
Ref.
[12]
[12]
[12]
[12]
[12]
[12]
[12]
[29]
[29]
[30]
[31]
This
Study

Feedstock
Coal
Coal
Wood Waste
Crop
Residue
Wood
Softwood
Wood
Kerosene
Oil
Coalbriquette
Various
Woods
Rice Husks

Combustion Device
Spreader Stoker
Overfeed Stoker
Fired Boiler
Cooking stove

PM10 Emission Factor

5.99 mg/gfeed
2.72 mg/gfeed
2.94 - 7.67 mg/gfeed
2.32 mg/gfeed

Residential Stove
Fireplace
Open Combustion
Lamp
Lamp
Coal-Stove

3 - 28 mg/gfeed
13 mg/gfeed
6.6 mg/gfeed
3.27 - 9.04 mg/gfeed
0.35 - 7.32 mg/gfeed
7.33 mg/gfeed

Cooking Stove

0.7 - 4.1 mg/gfeed

Co-Combustion of Tar and

Synthesis Gas from Pyrolysis

3.16 mg/gfeed

It is clear that further work is needed to explain in greater detail the predominant PM formation
mechanisms at play here. The influence of the operating conditions on both the profile of the masssize distribution, as well as the relative amount of PM generated, would be of great use in any future
replication of such a process in practice.

3.5 Emissions Associated with Biochar Production

The atmospheric emissions associated with the production of biochar were estimated in this study.
With rice husk used as the biomass feedstock, the carbon content of the char produced at 500C was
around 43.5%. If all the pyrolysis vapour was used to generate heat for the pyrolysis process and
biochar was used to sequester carbon, then around 2073 mg of CO2 and 3.4 mg CO will be released
for every gram of carbon sequestered. In addition, 10.5 mg of PM10 and 2.6 mg of PM2.1 would be
generated for every gram of carbon sequestered. This is considered to be high as the carbon content
of the rice husk biochar was low when compared to biochar produced from low ash feedstocks
[16][17].

4 Conclusion

This paper presents a preliminary study aimed at estimating the atmospheric emissions from the cocombustion of biomass tar and synthesis gas during biochar and bioenergy production. Fuel
characteristics along with gaseous and PM emissions were quantified. It was found that the PM and
gaseous emissions from the co-combustion process were substantially lower than the conventional
solid or liquid fuel combustion processes even though a high ash content feedstock was used.
However, the carbon emissions associated with the production of biochar for carbon sequestration is
high because of the high ash content of the rice husk.

493

Acknowledgements

This funding of this research is supported by the Government of South Australia through the Premiers
Research and Industry Fund- Catalyst Research Grants (CGR72).

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Presenting Author Biography

Lewis Dunnigan began his PhD at the University of Adelaide in early 2014 under the supervision of
Chi Wai (Philip) Kwong and Peter Ashman (both University of Adelaide) and Xiangping Zhang
(Institute of Process Engineering, Chinese Academy of Sciences). His PhD project is focused on
establishing the emissions from the co-generation of renewable energy and biochar from agricultural
wastes. He graduated with a Master of Engineering (Chemical Engineering) from the University of
Edinburgh in 2013.

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