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Gas permeability of biochar-amended clay: potential alternative landfill final

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Environ Sci Pollut Res
DOI 10.1007/s11356-015-4871-2

BIOLOGICAL WASTE AS RESOURCE, WITH A FOCUS ON FOOD WASTE

Gas permeability of biochar-amended clay: potential alternative

landfill final cover material
James Tsz Fung Wong 1 & Zhongkui Chen 1 & Charles Wang Wai Ng 1 &
Ming Hung Wong 1,2,3

Received: 16 February 2015 / Accepted: 9 June 2015

# Springer-Verlag Berlin Heidelberg 2015

Abstract Compacted biochar-amended clay (BAC) has been
proposed as an alternative landfill final cover material in this
study. Biochar has long been proposed to promote crop
growth, mitigate odor emission, and promote methane oxida-
tion in field soils. However, previous studies showed that soil-
gas permeability was increased upon biochar application,
which will promote landfill gas emission. The objective of
the present study is to investigate the possibility of using
compacted BAC as an alternative material in landfill final
cover by evaluating its gas permeability. BAC samples were
prepared by mixing 425-μm-sieved peanut shell biochar with
kaolin clay in different ratios (0, 5, 10, and 15 %, w/w) and
compacting at different degrees of compactions (DOC) (80,
85, and 90 %) with an optimum water content of 35 %. The
gas permeability of the BACs was measured by flexible wall
gas permeameter and the microstructure of the BACs was
analyzed by SEM with energy-dispersive x-ray spectroscopy
(EDX). The results show that the effects of biochar content on
Responsible editor: Zhihong Xu
* Charles Wang Wai Ng
cecwwng@ust.hk
* Ming Hung Wong
minghwong@ied.edu.hk
1
Department of Civil and Environmental Engineering, The Hong
Kong University of Science and Technology, Room 3556, Clear
Water Bay, Kowloon, Hong Kong SAR, China
2
Consortium on Health, Environment, Education and Research
(CHEER), The Hong Kong Institute of Education, Tai Po, Hong
Kong SAR, China
3
Department of Science and Environmental Studies, The Hong Kong
Institute of Education, Office B3-2/F-33, Tai Po, Hong Kong SAR,
China
BAC gas permeability is highly dependent on the DOC. At
high DOC (90 %), the gas permeability of BAC decreases
with increasing biochar content due to the combined effect
of the clay aggregation and the inhibition of biochar in the
gas flow. However, at low DOC (80 %), biochar incorporation
has no effects on gas permeability because it no longer acts as
a filling material to the retard gas flow. The results from the
present study imply that compacted BAC can be used as an
alternative final cover material with decreased gas permeabil-
ity when compared with clay.
Keywords Landfill final cover . Biochar . Biochar-amended
clay . Compacted soil cover . Gas permeability
Introduction
Biochar is a carbon-rich substance produced by heating bio-
mass, such as leaves and wood chips, at high temperature in an
oxygen-deficient condition (Lehmann and Joseph 2009). It
has been used in soil amendment to improve soil fertility
and as a pollutant sorbent for soil and water remediation
(Lehmann and Joseph 2009; Ahmad et al. 2014; Mohan
et al. 2014). In this study, compacted biochar-amended clay
(BAC) is proposed as an alternative landfill final cover mate-
rial. Compacted clay is widely used in landfill final covers in
arid and semi-arid regions, as recommended by the US
Environmental Protection Agency (US EPA 1989). The pri-
mary goal of a landfill final cover is to minimize the landfill
gas generated from waste degradation and reduce rain water
infiltration that leads to leachate production. Apart from com-
monly used clay, alternative final cover materials, such as
using municipal solid waste compost and sewage sludge, have
been proposed in many studies (Elshorbagy and Mohamed
2000; Kettunen et al. 2006; Scheutz et al. 2009).

Compost and sludge are derived from waste and are cost-
effective material to replace compacted clay. For instance, it
was estimated that US$20,000 to US$50,000 per acre could
be saved by replacing compacted clay layers by paper sludge
in the final cover in landfills (Moo-Young and Zimmie 1996).
However, compost and sludge are quite degradable, causing
changes in the amended soil properties. The design life of a
landfill is at least 100 years (Koerner 2012), implying that
incorporating compost or sludge in landfill final covers may
not be safe and sustainable. In comparison, biochar is also
derived from waste, but is more stable and highly resistant
to mineralization in soil (Lehmann 2007; Lehmann and
Joseph 2009). For example, biochar was found to have
remained unchanged for thousands of years in the soil in
Amazonia, which is a highly humid tropical area (Sombroek
et al. 2003). The highly stable properties of biochar make it
more suitable for use as an alternative final cover material,
when compared with other easily degradable matter, such as
compost.
Using biochar as an alternative final cover material offers
more than just cost saving and sustainability. Recently, several
studies have revealed the possibility of applying biochar in
landfill final covers to promote methane oxidation and thereby
reduce methane emission from landfills (Yu et al. 2013; Reddy
et al. 2014). In addition, biochar is also known as a super
sorbent that can absorb odorous compounds in landfill gases,
such as hydrogen sulfide (Shang et al. 2012, 2013; Xu et al.
2014).
The key properties that govern gas permeability of biochar
and biochar-amended soil are particle size distribution and
porous structure, which affect the water distribution in soil,
and therefore the gas permeability. A desired biochar used as
an amendment in landfill final cover soil would be with small
pore volume and pore diameter. Large pores would increase
gas permeability and promote landfill gas migration and emis-
sion from the landfill final cover. However, large surface area
is favored because more contaminants could be adsorbed.
There are various feedstocks suitable to be the biomass for
biochar production. In between, waste biomass such as pea-
nut shell and wheat straw are more suitable because of their
massive supply at low price. According to a previous study
(Zhao et al. 2013), among 12 biochar derived from waste
biomasses at 500 °C, including manure, sludge, waste
paper, etc., peanut shell biochar is with relatively small
pore volume (0.04 cm3 g−1) and average pore diameter
(3.72 nm) while with relatively large surface area
(43.5 m2 g−1). Therefore, peanut shell biochar was se-
lected to be investigated of its feasibility as an alterna-
tive material of landfill final cover.
However, previous researchers (Sun et al. 2013) revealed
that biochar application may increase the gas permeability of
agriculture soil (sandy loam) because of its inherently high
porosity. In fact, agricultural soil (varying from sand to clay)
Environ Sci Pollut Res
is rarely being highly compacted when compared with the
highly compacted (>90 % degree of compaction, DOC) soil
in landfill final cover. A lower DOC (i.e., bulk density) is
desired in agriculture to promote crop growth while higher
DOC is favored in landfill final cover to reduce landfill gas
migration. High compaction rate is a requirement of an
engineered landfill final cover in order to prevent water infil-
tration into the waste layer and landfill gas emission to the
atmosphere. It implies that investigation on the gas permeabil-
ity of compacted biochar-amended soil is needed prior to its
application. The difference in gas and water permeability re-
sults highly depends on the compaction level of the test soils,
which can result in different pore structure characteris-
tics (Bronick and Lal 2005). It is well accepted that soil
compaction has significant effects on the gas permeabil-
ity by soil structure modification (Moldrup et al. 2001;
Hamamoto et al. 2009; Deepagoda et al. 2011). In ad-
dition, biochar can promote soil aggregation (Asai et al.
2009; Liu et al. 2012), but compacted BAC aggregation
effects under different DOC were not considered likely,
again owing to the application of biochar only in agri-
cultural aspect. Therefore, it is necessary to understand
the gas flow characteristics of compacted biochar-
amended soil under different compaction conditions in
order to serve in practical applications.
The objective of the present study is to investigate the pos-
sibility of using compacted biochar-amended clay as an alter-
native soil layer in landfill final covers by measuring the gas
permeability. Peanut shell biochar and kaolin clay were used
to produce biochar-amended clay. The gas permeability of the
biochar-amended clay was measured by a flexible wall gas
permeameter and compared with pure kaolin clay. The micro-
structure of BACs was analyzed by a scanning electronic mi-
croscope (SEM) with energy-dispersive x-ray spectroscopy
(EDX).
Materials and methods
Preparation of biochar
Peanut shell biochar was produced by slow pyrolysis process.
The biomass was heated at 5–10 °C/min and retained at about
500 °C for 30–40 min. In general, 30 % of the biomass was
converted into biochar. Nitrogen gas was pumped into the
chamber to maintain an inert environment during the cooling
period. Water cooling system was installed to shorten the
cooling period. The biochar produced was sieved through 5-
mm sieve. In the present study, biochar was additionally
sieved through 425 μm in order to obtain a more homogenized
biochar-amended clay sample and prevent any possible pref-
erential flow during the gas permeability tests that may inter-
fere the results.
Environ Sci Pollut Res
Characterization of biochar and clay
The moisture content of biochar and clay were determined by
oven-dry method. Approximately 3 g of biochar (5 mm and
425-μm sieved) and kaolin clay were weighted into oven-
dried crucibles and heated at 105 °C in oven and dried to
constant weight. The heated crucibles were cooled at room
temperature in a desiccator for 30 min. Moisture content of
the sample is equal to the weight loss of the sample. Organic
matter and ash content were determined using similar method.
Approximately 0.25 g of biochar and clay were weighted into
oven-dried crucibles and heated at 105 °C in an oven to con-
stant weight to remove the water and then at 600 °C in a
muffle furnace for 16 h. The heated crucibles were cooled at
room temperature in a desiccator for 30 min. The total organic
matter is equal to the weight loss of the oven-dried samples
while the ash content is the residue in crucibles. For pH and
electrical conductivity (EC) measurement, 5 g of biochar and
clay were suspended in 250-ml deionized water. The mixtures
were shaken at 200 rpm for 1 h and stand for 30 min. The pH
was measured by the pH meter and the EC was measured by
the EC meter. The particle size distribution of the peanut shell
biochar and kaolin clay was analyzed in accordance with
ASTM standard D422 (ASTM 2007). Soil physiochemical
properties were analyzed in triplicate (n=3), except the parti-
cle size distribution. The significance of properties between
biochar (5 mm and 425-μm sieved) and clay were analyzed by
one-way analysis of variance (ANOVA) followed by the
Duncan’s multiple range test at 5 % probability level. The
statistical analyses were conducted using SPSS (version 17.0).
Gas permeability measurements
The gas permeability of the soil samples were measured by a
flexible wall air permeameter (Fig. 1). Biochar was air dried
and sieved through a 425-μm-pore size sieve and mixed with
clay at three different percentages (5, 10, 15 %, w/w) to pro-
duce BAC, which was then mixed with water to give an op-
timum 35 % gravimetric water content. After 2-day water
content homogenization, the BAC was compacted at different
degrees of compaction (80, 85, and 90 %) to become a
compacted soil column. The compacted columns were cov-
ered with an elastic membrane (flexible wall) and located in
the gas permeameter. The confining pressure of the
permeameter was then set at 20 kPa and air flow, with varying
base pressures, was applied. The air outflow rate was recorded
by a gas flow meter after the gas flow became stable, and the
gas permeability was calculated according to the generalized
Darcy’s law for compressive media (Bouazza and Vangpaisal
2003):
2QμLP1
K¼
tronic microscopy to investigate the interaction between the
A P22 −P12
where K is the gas permeability (m2), Q is the gas outflow rate
(m3/s), μ is the gas dynamic viscosity (Pa×s), L is the thick-
ness of the soil sample (m), P1 is the atmospheric pressure
(Pa), P2 is the applied gas pressure (Pa), and A is the cross-
section area of the sample (m2).
BAC Microstructure analysis
The microstructure and pore size characteristics of the biochar
and BAC were analyzed by scanning electronic microscope
(SEM) and energy-dispersive x-ray analysis (EDX), respec-
tively. A cubic BAC specimen of about 0.5 cm3 was removed
from each compacted BAC soil column, in triplicate, and fro-
zen by immersion in liquid nitrogen (−195 °C) for 5 min
(Gallé 2001). The frozen specimens were freeze dried, coated
with a thin layer of gold and then analyzed using a scanning
electron microscope (JEOL JSM 6390).
Results and discussion
The soil physiochemical properties of kaolin clay, peanut shell
biochar, and 425-μm sieved biochar that are related to gas
permeability were summarized in Table 1. The pH of clay is
acidic (5.20±0.03) while biochar is alkaline (9.98±0.01). The
sieved biochar is less alkaline (9.71±0.04, p<0.05) when
compared with the un-sieved one. This indicated that sieving
would alter the physiochemical properties of biochar. Similar
results were shown in organic matter, electrical conductivity,
and ash content. Sieving of biochar significantly reduced
(p<0.05) its organic matter from 30.15±3.07 to 51.91±0.09,
while significantly increased (p<0.05) its EC from 6.41±0.36
to 1.80±0.09 and ash content from 69.85±3.07 to 48.09±
0.09. The particle size of biochar used in this study (425-μm
sieved) had relatively larger particle sizes than clay, which
implies that clay would fill up pores between the biochar par-
ticles in the biochar-amended soil. The results of the tests
show that the gas permeability decreases with increasing bio-
char content, especially at relatively high degrees of compac-
tion (Fig. 2). The gas permeability increases with the degree of
compaction at a certain biochar content. With increase of the
biochar content, the rate of reduction of the gas permeability
increases. For instance, the gas permeability of 15 % BAC
was decreased by two orders of magnitude (3E-11 to 2E-
13 m2) by increasing the degree of compaction from 80 to
90 %. However, at low biochar content (i.e., 5 %), the gas
permeability of BAC was almost constant for all degrees of
compaction. This implies that gas permeability is mainly
governed by inter-pores of clay aggregates at low biochar
content.
The microstructure of BAC was analyzed by scanning elec-
biochar and clay particles (Fig. 3), while their chemical

Fig. 1 Overview of the flexible
wall air permeameter
composition was analyzed by EDX (Fig. 4). Peanut shell bio-
char is mainly composed of carbon (54.3 %), while clay is
mainly composed of aluminum (11.14 %) and silicon
(9.04 %). Biochar, clay aggregates, and their inter-pores are
clearly seen for BAC at 15 %, biochar content at 80 %
(Fig. 3a), and (Fig. 3b) DOC at 90 %. At low DOC, clay
aggregates were in loose contact with each other, with wide
gaps in between. It clearly demonstrated the aggregation effect
of the compacted clay. In this condition, the inter-pore voids
among the clay aggregates were partly filled by biochar, larger
in size as compared with the clay particles (Fig. 2). Thereby,
although biochar particles were located into the gas flow path-
ways, their contribution as a filling material is insignificant
since the inter-pores among the clay aggregates are large
enough for gas flow, when compared with the size of the
biochar particles. At low DOC and with increasing biochar
content, the gas permeability of BACs was also constant. It
provides confirmation that biochar addition into clay has no
significant effect on gas permeability. The higher gas perme-
ability primarily resulted from the soil aggregation effects at
low DOC. However, at higher DOC (Fig. 3b), the high
Table 1 Physiochemical properties of biochar and clay
Material Moisture pH Organic
content (%) matter (%)
Kaolin clay 0.87±0.06a 5.20±0.03a 31.26±1.18a
Peanut shell biochar 4.92±0.34b 9.98±0.01b 30.15±3.07a
(5-mm sieved)
Peanut shell biochar 4.73±0.19b 9.71±0.04c 51.91±0.09b
(425-μm sieved)
Values are presented in mean±SD (n=3). Values followed by the same letter on the same column indicate no significant difference (at the 0.05
probability level) according to the Duncan’s multiple range test
Environ Sci Pollut Res
compaction energy made more aggregates group together to
form bigger aggregates, resulting in a much smaller volume of
inter-pores among the clay aggregates than that presented at
low degrees of compaction (Moldrup et al. 2001). Meanwhile,
biochar particles were still located in the inter-pores of the clay
aggregates. Although the size of aggregates were similar to
those at low DOC, their contribution in acting as a filling
material to the gas flow is increased due to the reduction of
the inter-pore volume among the clay aggregates. Therefore,
the decrease of gas permeability at high DOC is caused by the
effects of clay aggregation and retardation of the biochar par-
ticles in the gas flow. The observed effects of the biochar
content and DOC on gas permeability clearly illustrate that
the soil-biochar interactions had a significant impact on the
gas transport behavior in compacted biochar-amended clay.
The results of this study were not consistent with those
presented by previous researchers (Kolb et al. 2007; Sun
et al. 2013). As mentioned by Kolb et al. (2007), the gas
permeability of biochar-amended soil was higher than that in
non-amended soil because of the higher air-filled porosity of
biochar (Fig. 3a) allowing more gas flow (Sun et al. 2013).
EC (ds m−1) Ash content (%) Particle size distribution (%)
>0.02 mm 0.002–0.02 mm <0.002 mm
6.49±0.02a 68.74±1.18a 0 0 100
6.41±0.36a 69.85±3.07a 63.92 28.30 7.78
1.80±0.09b 48.09±0.09b 0 72.10 27.90
Environ Sci Pollut Res

1e-7

1e-8 80% DOC

85% DOC
90% DOC
1e-9
G a s P e r m e a b ility ( m 2 )

1e-10

1e-11

1e-12

1e-13

1e-14

1e-15
0 2 4 6 8 10 12 14 16

Biochar Content (%, w/w)

Fig. 2 Gas permeability of the biochar-amended clay (BAC) with
different biochar content and degrees of compaction (DOC) at 35 %
gravimetric water content

Fig. 4 a SEM image (×1000) of a biochar-amended clay (BAC) sample.

b SEM–EDX spectra atomic percentage analysis of the biochar (blue) and
b clay (green) shown in panel a

However, previous studies mainly focused on the application of

biochar to agricultural soil, such as sandy loam and silty clay. In
addition, agricultural soil usually has a low degree of compaction
to benefit root growth and soil aeration (McHenry 2011). In the
present study, the soil was highly compacted, in consideration of
that focused in the landfill final cover. With such high compac-
tion, for example 90 %, the compacted biochar-amended soil
would inhibit water infiltration into the underlying waste layer
and landfill gas migration into the atmosphere (Raco et al. 2010).

Conclusion

Fig. 3 SEM image (×200) of the 15 % biochar-amended clay (BAC) Gas permeability of biochar-amended clay was investigated in
sample with 80 % (a) and 90 % (b) degree of compaction (DOC) order to evaluate its feasibility for use as an alternative

material in landfill final covers. The microstructure of the
BAC was observed by SEM in order to explore the interaction
between the biochar and clay particles with the effects of the
biochar content and DOC. The results show that the effects of
the biochar content on the BAC gas permeability vary with
DOC. At high DOC (i.e., 90 %), the gas permeability of the
BAC decreases with increasing biochar content due to the
combined effect of clay aggregation and biochar inhibition
in the gas flow. However, at low DOC (i.e., 80 %), the effects
of biochar incorporation on gas permeability is negligible be-
cause it no longer acts as a filling material to retard gas flow
(Sun et al. 2013). Results from the present study did not show
similar trends with those studies using biochar in agricultural
soils. The result revealed that the gas permeability of BAC
was reduced by increasing the biochar content and degree of
compaction. This suggested that apart from being a soil
amendment in agriculture, biochar-amended clay can be a
potential landfill final cover material in terms of the gas emis-
sion issue. Sieving of biochar would be essential to increase
the homogeneity of the landfill final cover upon mixing and
compaction process. However, sieving would significantly af-
fect the physiochemical properties of the biochar, such as par-
ticle size distribution and therefore the gas permeability.
Effects of biochar particle size distribution of biochar-
amended soil on gas permeability needs to be elucidated.
Acknowledgments This study was funded by the research grant
2012CB719805 of 2012CB719800 provided by the Ministry of Science
and Technology of the People’s Republic of China through the National
Basic Research Program (973 project) and Collaborative Research Fund
(CRF) provided by the Research Grants Council of the Hong Kong SAR
(HKUST6/CRF/12R). The authors would like to thank Mr. Yeung Yin
Hon and Ms. Charlotte Ma for their technical assistance.
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