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Environmental Pollution 216 (2016) 182e197

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Environmental Pollution
journal homepage: www.elsevier.com/locate/envpol

Review

Gas aring and resultant air pollution: A review focusing on black


carbon*
Olusegun G. Fawole a, c, X.-M. Cai a, A.R. MacKenzie a, b, *
a
School of Geography, Earth and Environmental Sciences, University of Birmingham, Edgbaston, Birmingham, B15 2TT, UK
b
Birmingham Institute of Forest Research, University of Birmingham, Edgbaston, Birmingham, B15 2TT, UK
c
Environmental Research Laboratory, Department of Physics, Obafemi Awolowo University, Ile-Ife, 220005, Nigeria

a r t i c l e i n f o a b s t r a c t

Article history: Gas aring is a prominent source of VOCs, CO, CO2, SO2, PAH, NOX and soot (black carbon), all of which
Received 23 February 2016 are important pollutants which interact, directly and indirectly, in the Earths climatic processes. Glob-
Received in revised form ally, over 130 billion cubic metres of gas are ared annually. We review the contribution of gas aring to
24 May 2016
air pollution on local, regional and global scales, with special emphasis on black carbon (BC, soot). The
Accepted 26 May 2016
temporal and spatial characteristics of gas aring distinguishes it from mobile combustion sources
(transport), while the open-ame nature of gas aring distinguishes it from industrial point-sources; the
high temperature, ame control, and spatial compactness distinguishes gas aring from both biomass
Keywords:
Gas aring
burning and domestic fuel-use. All of these distinguishing factors inuence the quantity and charac-
Oil and gas teristics of BC production from gas aring, so that it is important to consider this source separately in
Black carbon emissions inventories and environmental eld studies. Estimate of the yield of pollutants from gas aring
Incomplete combustion have, to date, paid little or no attention to the emission of BC with the assumption often being made that
Hydrocarbon aring produces a smokeless ame. In gas ares, soot yield is known to depend on a number of factors,
Emission factors and there is a need to develop emission estimates and modelling frameworks that take these factors into
consideration. Hence, emission inventories, especially of the soot yield from gas aring should give
adequate consideration to the variation of fuel gas composition, and to combustion characteristics, which
are strong determinants of the nature and quantity of pollutants emitted. The buoyant nature of gas
aring plume, often at temperatures in the range of 2000 K, coupled with the height of the stack enables
some of the pollutants to escape further into the free troposphere aiding their long-range transport,
which is often not well-captured by model studies.
2016 Elsevier Ltd. All rights reserved.

1. Introduction estimated to provide 52.8% of the worlds energy (13113 Mtoe);


with oil and natural gas accounting for 31.5% and 21.3% respectively
1.1. Motivation (IEA, 2013).
Human reliance on oil and gas as an energy source is not
Humans need energy to drive their technology and hence, make without its attendant impact on the environment. During produc-
life pleasurable and worth living. Different forms of energy are in tion, detrimental impacts on the environment (air, water and soil)
use and new ones are developed in order to meet the increasing include: oil spills and leakages; venting; sludge disposal; and ar-
needs of society (MacKay, 2008). This quest for dependable, ing (Almanza et al., 2012; Osuji and Adesiyan, 2005; Osuji and
affordable and environmentally benign energy sources has Onojake, 2004; Sonibare et al., 2010). The post-production impact
occurred throughout human history; for the last century or so, of oil and gas on the environment is also a major source of concern,
crude oil has been the focus of world energy. In 2011, crude oil was but is not the subject of this review.
Gas aring is often a routine daily activity in oil elds around the
world, particularly in oil-rich regions of the world where the
*
This paper has been recommended for acceptance by Dr. Hageman Kimberly infrastructure to capture, store and utilise the gas produced is not
Jill. available. Flaring is most often associated with Nigeria and the
* Corresponding author.
Russian Arctic, but it does still occur in more developed economies:
E-mail address: a.r.mackenzie@bham.ac.uk (A.R. MacKenzie).

http://dx.doi.org/10.1016/j.envpol.2016.05.075
0269-7491/ 2016 Elsevier Ltd. All rights reserved.
O.G. Fawole et al. / Environmental Pollution 216 (2016) 182e197 183

(Bond et al., 2013), while in Russia, it is estimated to have the


Variables used and their meanings largest contribution of 36.2% to anthropogenic BC emission (Huang
et al., 2015). From a 3-year model simulation, more than 40% of
ue exit velocity of the ue gas (m s1) annual mean BC near the surface in the Arctic is estimated to be
s the air-fuel ratio contribution from gas aring (Stohl et al., 2013).
re, r the fuel gas and ambient densities respectively Considering the small number of nations that still are gas, a
(kg m3) contribution of 4% to global BC represents a signicant skew in the
g acceleration due to gravity (m s2) global apportionment of BC emissions. On a regional scale, the
DTf mean peak ame temperature rise, K (taken as the contribution of this overlooked source of ambient aerosol loading
difference between the adiabatic ame temperature is likely to be signicant.
and the ambient temperature)
de burner diameter (m) 1.2. Review summary
no kinematic viscosity of the gas-air mixture (m2 s1)
L characteristic ame length (m) For this review, we have collated previous studies (1984e2015)
m_ o mass ux of the ue gas at the burner exit on gas aring and its contributions to ambient aerosol loadings.
This review is the rst to cover virtually every aspects of gas aring
(kgm2 s1)
fs stoichiometric mixture fraction (process, trends, chemistry, ame dynamics and environmental
impact). The review starts with a brief assessment of the level and
equivalence ratio
T ambient temperature distribution of oil and gas reserves around continents of the world.
Compositional variation of the natural gas ared and their ther-
modynamic properties are discussed because they are likely to have
signicant impact on pollutant emission rates and overall amount.
the North Dakota Bakken shale region, for instance (see, e.g., http:// Next, we provide a discussion of the temporal and geographical
www.eia.gov/todayinenergy/detail.cfm?id23752, last accessed on trends in gas aring, including brief comments about how weather
29 January 2016). Despite several calls by international bodies such conditions in regions where gas aring is common will impact
as the World Banks Global Gas Flaring Reduction (GGFR) initiative, near-eld dispersion and long-range transport. This is followed by a
the volume of gas ared globally appears to have plateaued at broad discussion of the gas aring process itself; highlighting how
around 130 billion cubic metres (bcm) since 2008, or may even engineering and technology decisions impact on the emission of air
have increased (see section 1.4, below). According to GGFR (2013), pollutants. Finally, several techniques used to estimate emissions
there was an increase of 2 bcm in the volume of gas ared in 2011 from gas aring are discussed. Throughout this review, special
compared to the previous year. The latest in this series of initiatives attention is paid to soot (i.e. carbonaceous aerosol predominantly
by the World Bank - Zero Routine Flaring by 2030 - was launched by composed of BC) emission from gas aring because of the now
the Secretary-General of the United Nations, Ban Ki-Moon and known contribution of BC to global warming and the apparent
World Banks President, Jim Yong Kim, in May 2015 (see http:// neglect of the contribution of gas aring to ambient air aerosol
www.worldbank.org/en/programs/zero-routine-aring-by-2030, loadings in inventories and global models.
last accessed on January 29, 2016).
Gas aring, a prominent source of black carbon (BC) and other 1.3. Global oil and gas reserves
pollutants, has been ignored or underestimated in emission in-
ventories and models, as a result of which models are struggling to World-proven natural gas and oil reserves at the end of 2012
predict measurements of BC in regions of intense gas aring. The stood at 187.3 and 1668.9 trillion cubic metres (tcm) respectively,
intensity of gas aring and specics of atmospheric transport can sufcient to meet 55.7 years of global production (BP, 2013). The
combine to enhance the role of gas aring emissions over very large distribution of these reserves among regions of the world is shown
areas (e.g., the Arctic) (Stohl et al., 2013). Presently, treatment of in Fig. 1(a) and (b). The natural gas collected during the exploration
emissions from gas aring is rather rudimentary in most global of crude oil from the Earths crust can be a very good source of fuel;
emission inventories. As at 2015, to the best of our knowledge, only transported in pipes for industrial or domestic use and also recycled
two global pollutants inventories explicitly accounted for emissions back into the processing operation (Davoudi et al., 2013; Elvidge
from gas aring (see section 4.5). et al., 2009).
Gas aring is classied as a miscellaneous BC-rich source, a In developing countries and oil-rich regions where the tech-
group which includes aviation and shipping which together nology, infrastructure, and market structure to put all of the natural
contribute about 9% to global BC emission (Bond et al., 2013). Gas gas to meaningful use are not available or inadequate, the excess
aring is a very different type of combustion compared to other BC natural gas then becomes a waste stream and is ared or vented.
sources in this category; gas aring is characterised by either fuel- Gas aring has been termed gross waste by the World Banks
regulated or oxidant-regulated open-re (see below) resulting in initiative against gas aring (Global gas aring reduction: GGFR),
ames that can be 8e10 m in length, with ame temperature as because aring represents direct injection of fossil carbon into the
high as 2000 K. Gas aring is a year-round activity in most of the atmosphere without capture and utilization of the heat produced
intensive aring regions of the world, and so differs from transport by combustion.
sources in being stationary and differs from other stationary sour-
ces (e.g. cooking and biomass burning) by being relatively constant 1.4. Temporal and geographical trends in gas aring
in time. The GAINS (Greenhouse gas Air pollution INteractions and
Synergies) model estimated that gas aring contributes about 4% of The all-time peak of volume of gas ared, 172 bcm, was in 2003
total anthropogenic BC emissions, majority of which are from the (Elvidge et al., 2009) although see estimates for 2012, below.
leading gas-aring nations; Russia, Nigeria, and countries in the Fig. 2(a) shows the quantity of natural gas produced by the top 10
Middle East (Bond et al., 2013; Stohl et al., 2013). Gas aring is oil producing nations of the world between 2000 and 2011, and for
estimated to contribute 260 Gg to global BC estimates annually comparison, Fig. 2(b) shows the estimated quantity of gas ared by
these major oil producing nations during the same period of time.
184 O.G. Fawole et al. / Environmental Pollution 216 (2016) 182e197

Fig. 1. (a) The distribution of world natural gas reserves (b): The distribution of world oil reserves (adapted from BP (2013).

The estimated volume of gas ared globally in 2012 is also shown in about 20% in the central tendencies of the estimates for both years
Fig. 2(b): the 2012 data is obtained from Elvidge et al. (2015). Data and is well outside the combined uncertainty bounds of both es-
for the plots in Fig. 2(a) and (b) are from IEA (2012) and GGFR timates. An increment of about 20% over four years, stands in stark
(2012), respectively. Between 2008 and 2011, there was no signif- contrast to the decrease anticipated as a result of the World Banks
icant decrease in the amount of natural gas ared. In fact, there was Global Gas Flaring Reduction (GGFR) initiative. A new dimension to
a slight increase between 2010 and 2011. According to (BP, 2015), the problem is the inclusion of three new countries e India, Egypt
the production excludes the quantity ared or recycled. Therefore, and Turkmenistan - in the list of top 20 gas aring countries.
total fossil fuel extracted and ultimately released to the environ- The geographical location of the sources of gas aring emissions
ment is the sum of the production and quantity ared. (as monitored from space, see Fig. 4), the atmospheric behaviour of
Fig. 3 gives the temporal variation of the fraction of total gas emitted pollutants, and the pollutant matrix from other sources
extracted that is ared between 2000 and 2011. Nigeria, Libya and into which emission are made, determine to a large extent the ef-
Kazakhstan still are a sizeable amount of their total production. As fect gas aring emissions will have on regional pollution loadings
at 2011, Nigeria and Libya ared about 30% of their total gas and on climate. BC emissions in the peri-Arctic and West African
extracted while Kazakhstan ares about 15%. The 30% (15.2 bcm) Monsoon (WAM) regions have the potential to interact with
ared by Nigeria is more than twice Libyas total gas extracted regional radiative energy budgets and atmospheric circulations,
(6.3 bcm) for the same period. Russia and Nigeria together account leading to impacts on their respective regional climates. Gas aring
for about 35% of the gas ared globally (Elvidge et al., 2009). emissions in the tropics, especially the WAM and South Asian
Although the fraction of gas ared is decreasing for most countries Monsoon (SAM), could have signicant regional impact as a result
and for the largest emitters, several countries show at or of the intense convective activities and cloud formation in these
increasing fractions of gas ared. The estimated quantity of natural regions.
gas ared in the US and Canada, as shown in Fig. 2(b), are just for Monsoon circulations are characterised by large-scale seasonal
the off-shore aring which is presumably responsible for the very reversals of wind regimes. Regions often referred to as monsoonal
low quantities recorded. After 2006, there is a factor of 22 and 10 include tropical and near-tropical regions which experience a
increase in aring from USA and Canada, respectively, resulting, summer rainfall maximum and most of these regions have a double
presumably, from increased exploitation of unconventional hy- rainfall maximum (Barry and Chorley, 2009). The annual climatic
drocarbon reservoirs (fracking). regime over West Africa has many similarities to that of South Asia.
Table 1 gives the estimates, from satellite data, of the quantity of Both are characterised by surface air-ow which is determined by
gas aring by the top 20 gas aring nations of the world in 2008 the position of the leading edge of a monsoon trough. Winds are
and a brief summary of the climatic conditions of the region based south-westerly to the south of the trough and north-easterly to the
on the Ko ppen climate classication (see, e.g., Holden (2005)). North. The lack of a large mountain range in the north of West
Fig. 4, reproduced, with permission, from Casadio et al. (2012), Africa strongly enhances the northward advance of the WAM
shows the global geographic distribution of gas aring sites ob- compared to its South Asian counterpart. The position of the
tained by remote sensing techniques. In Africa, the aring spots are leading edge of the WAM trough may oscillate greatly from day-to-
clustered around the North - Algeria, Libya and Egypt - as well as day through several degrees of latitude (Barry and Chorley, 2009).
around the Atlantic Ocean especially the Niger Delta area of Nigeria. In the WAM, deep convection occurs in organised systems known
In Europe, they are around Russia and Kazakhstan, and Iran, Iraq, as Mesoscale Convective Systems (MCS) (Mari et al., 2011; Mathon
Kuwait, and Saudi Arabia in the Middle East. Satellite remote and Laurent, 2001). Deep convection in the tropics associated with
sensing not only gives a general picture of the spatial distribution of the ITCZ is responsible for intense mixing, venting of the atmo-
ares, but also a gross estimation globally at national levels. spheric boundary layer, and long-range transport of aerosol (Law
Elvidge et al. (2015), using data collected by National Aero- et al., 2010; Reeves et al., 2010; Sultan and Janicot, 2003).
nautics and Space Administration/National Oceanic and Atmo-
spheric Administration Visible Infrared Imaging Radiometer Suite 2. Oil and gas production
(VIIRS), identied more than 7000 active are globally in 2012: the
bulk of which were found in the upstream sector of the oil and gas 2.1. Exploration and exploitation
industries. In 2012, the estimated volume of gas ared globally is
143 13.6 bcm (Elvidge et al., 2015). Compared to 119.3 2.11 bcm Oil exploration can be a very complex and capital intensive
estimated for 2008 (Elvidge et al., 2009), this is an increment of process as oil deposits are often located in reservoirs buried far into
O.G. Fawole et al. / Environmental Pollution 216 (2016) 182e197 185

Fig. 3. Trend of quantity ared compared to total production (data from Fig. 2).

fuel gas to refer to natural gas that is ared. The quantity of con-
taminants expelled at this stage of processing depends on the
technology employed, quantity of crude oil processed, are ge-
ometry and design, prevailing meteorological conditions and the
composition of the ared gas (E & P Forum, 1994; Ismail and
Umukoro, 2014; Johnson and Coderre, 2011; Obanijesu et al.,
2009; Ouf et al., 2008; Sonibare and Akeredolu, 2004; Talebi
et al., 2014).
Oil and gas are produced in many wells in different parts of the
world at rates varying from 50 m3 to 700 m3 per day. As a result of
the diverse nature of the geological features of the area where these
explorations take place, the composition of oil and gas varies from
one station to another.

2.2. Composition of natural gas

The composition of natural gas from 10 stations from around the


world is given in Table 2. Fuel gas is a combination of C1 to C7
hydrocarbons which are predominantly alkanes. A typical fuel gas
sample contains CH4, C2H6, C3H8, n-C4H10, i-C4H10, n-C5H12, i-C5H12,
Fig. 2. Trend of natural gas (a) production and (b) aring in major oil producing na-
C6H14, C7H16, H2S, CO2 and N2, where n and i stand for normal
tions between 2000 and 2011 (adapted from IEA (2012) and (GGFR, 2012) respec-
tively). The estimate for 2012 is from Elvidge et al. (2015). i.e., straight chained, iso or branched-chained alkanes, respec-
tively. The separation of gas and liquid is not perfect at the Flow
Stations and as such trace amounts of liquid can occur in the gas
the Earth. These locations can be in very remote and inhospitable stream, enhancing the abundance of higher molecular weight al-
parts of the Earth and can be either on- or off-shore. The multi- kanes in the fuel gas.
staged process of exploration, exploitation and processing of
crude oil in its raw form from the Earths crust can be broadly 2.3. Thermodynamic properties of varying fuel gas compositions
divided into upstream, midstream and downstream. Environ-
mental contaminants are expelled into the ambient environment - The higher heating value (HHV) is the total enthalpy of the
soil, air and water - at different stages of the process. Crude oil is complete combustion reaction for the gas mixture, plus the heat of
found in reservoirs which also contain gas. This gas is known as condensation of the water produced during combustion; lower
associated natural gas, and it is separated from the crude oil at a heating value (LHV) is the total enthalpy of the complete com-
Flow Station. Natural gas includes both non-associated gas origi- bustion when water remains present in its gaseous form only
nating from elds producing only gaseous hydrocarbons, and (Flagan and Seinfeld, 2012). The Volumetric heating value (VHV),
associated gas produced in association with crude oil (IEA, 2012). measured in kJ mol1, usually refer to the HHV unless otherwise
Natural gas comprises mainly hydrocarbons, predominantly short- stated. In gas aring, HHV, calculable using data from standard
chained alkanes. At the separation stage, some of the natural gas is thermodynamic tables, denes the total amount of energy available
captured for domestic and industrial use while the rest is disposed to provide buoyancy to the are. Buoyancy is an important
of, usually by aring in open ames. Below, we will use the term parameter in determining the dispersion of are emissions
186 O.G. Fawole et al. / Environmental Pollution 216 (2016) 182e197

Table 1
Year 2008 estimated gas ared by top 20 gas aring nations with an estimated error of 2.11 bcm.

Rank Country Gas Flared Regional climate Commentsa


(bcm)

1 Russia 40.5 (Dfa, Dfb, Dwa, Dwb), (Dfc,Dfd, Peri-Arctic emissions; pole-ward atmospheric ow around Tibetan anticyclone in northern hemisphere
Dwc, Dwd) and ET winter
2 Nigeria 15.1 Am and Aw Tropical monsoon and trade-wind littoral and tropical wet and dry climate resulting from West African
monsoon winds that changes direction with season; climatic condition is controlled by trade wind and
movement of the ITCZ
3 Iran 10.4 Bwh Tropical and subtropical desert climate characterised by large diurnal temperature range. Deep turbulent
boundary layer during the day; shallow stable boundary layer at night. Large-scale subsidence (descending
branch of the Hadley circulation) above the boundary layer.
4 Iraq 7.0 Bsh Mid-latitude steppe and desert climate characterised by semiarid annual rainfall distribution
5 Algeria 5.5 Bwh As for Iran
6 Kazakhstan 5.2 Bwk Mid-latitude arid wet and dry climate
7 Libya 3.8 Bwh As for Iran
8 Saudi 3.5 Bwh As for Iran
Arabia
9 Angola 3.1 Cwa Humid subtropical climate; equatorward and poleward circulation during winter and summer respectively
cause changes in the movement of air masses from the cold polar and warm tropics within this climate.
10 Qatar 3.0 Bwh As for Iran
11 Uzbekistan 2.7 Csa Mediterranean climate; it is controlled by the variation between subtropical high in summer and polar
westerlies in winter
12 Mexico 2.6 Af, Aw, Bsh, Bsk, Bwh, Cwa, Complex climatic condition; two tropical, two dry and three temperate climates
Cwb, Cfa, Cfb
13 Venezuela 2.6 Aw Tropical wet-dry climate
14 Indonesia 2.3 Aw, Am As for Nigeria (see comment above)
15 USA 2.3 Bsk, Bsh, Bwk, Csa, Csb, Af Mediterranean/dry summer subtropical climate characterised by moist winter and hot dry summer;
subtropical anticyclones are key factor that control this climate
16 China 2.3 Cfa, Cwa Humid subtropical climate; during winter the climate is inuenced by the Siberian cold and during summer
there is an inow warm of air from the west
17 Oman 1.9 Bwh As for Iran
18 Malaysia 1.9 Af Tropical rainforest characterised by constant high temperatures and evenly distributed high precipitation;
controlled by movement of the ITCZ and rising air along trade wind coast. Strongly affected by el Nino
Southern Oscillation
19 Canada 1.8 Dfb, Dfd, Dsc, Af As for Russia (see above)
20 Kuwait 1.8 Bwh As for Iran
TOTAL 119.3
a
See Holden (2005).
Source: Quantity of gas ared is obtained from Elvidge et al. (2009).

Fig. 4. Flaring hot spot sites (1991e2009) as monitored from space are indicated as red spots while grey spots represent position of active volcanoes during the same period Casadio
et al. (2012). (For interpretation of the references to colour in this gure legend, the reader is referred to the web version of this article.)

(Beychok, 1994; Leahey and Davies, 1984). The heat content of a fuel shows the extent of dependence of HHV on the molar mass, and
gas depends on its molar mass and by extension the density of the hence, density of the fuel gas. These properties of the fuel gas,
fuel. Fig. 5 presents the best t line relating HHV to the molar mass varies with the fuel composition. Note that the HHV values for the
of the fuel gases from the Flow Stations given in Table 2. This plot laboratory ares in Table 1 are lower than the HHV for the Flow
O.G. Fawole et al. / Environmental Pollution 216 (2016) 182e197 187

Table 2
Composition (in mole %) and Some Properties of Fuel Gas from Field Stations and Literature.

Composition Flow stations Lab-based

1 2 3 4 5 6 7 8 9 10 A B

CH4 74.3 79.85 56.9 55.5 82.23 78.41 68.14 68.42 72.32 69.58 85.24 74.54
C2H6 14.0 11.54 21.2 18.0 2.38 5.68 14.22 7.65 2.41 0.25 7.06 12.17
C3H8 5.8 2.25 6.0 9.8 4.24 0.23 10.27 11.27 6.24 12.54 3.11 5.37
nC4H10 2.0 2.58 3.7 4.5 0.94 0.70 3.23 4.39 8.12 2.35 1.44 2.49
iC4H10 e 0.14 e e 5.12 4.12 2.38 4.42 5.12 5.12 e e
nC5H12 0.9 3.24 1.6 1.6 2.25 9.12 0.75 0.94 3.14 5.20 e e
iC5H12 e e e e 2.14 0.25 1.01 1.55 2.48 2.54 e e
C6H14 e 0.14 e e 0.25 0.23 e 0.18 0.15 1.97 e e
N2 2.9 0.1 e 0.2 e 0.05 e 0.16 e 0.24 1.24 2.15
CO2 e 0.16 7.1 8.9 0.45 1.21 e 1.02 e 0.21 1.91 3.28
H2S 0.1 e 3.5 1.5 e e e e 0.02 e e e
a
C:H 0.2659 0.2715 0.2569 0.2602 0.2730 0.2751 0.2860 0.2852 0.2893 0.2924 0.2541 0.2570
a
Molar mass (g mol1) 21.4 21.4 25.8 26.9 22.9 24.7 24.3 25.8 27.0 28.6 19.2 21.5
a
Molar mass (g mol1) 20.5 21.3 22.7 22.9 22.7 24.1 24.3 25.3 27.0 28.4 18.0 19.4
without CO2 and N2
a
HHV (MJ m3) 44.8 46.4 47.8 48.7 49.1 52.0 52.2 54.2 57.2 60.3 39.8 42.5

2 and 5e10 are adapted from Sonibare and Akeredolu (2004), 1, 3 and 4 from Ismail and Umukoro (2014) and lab-based (A&B) from McEwen and Johnson (2012).
Compositions 1, 3 and 4 are from Saudi Arabia, Kuwait and Iraq respectively while 2 and 5e10 are from different ow stations in Nigeria.
C:H mass-weighted carbon to hydrogen ratio.
a
Evaluated in this work.

Station fuel gases. Coderre, 2011). Emergency aring is unplanned: it is carried out at
large facilities for safety purposes for a short duration of time.
3. Overview of the gas aring processes During emergency aring, a large volume of gas is disposed of
quickly and, hence, the ow rate of the fuel gas is very high. Process
Gas aring is carried out with the aim to convert its hydrocarbon aring is an intermittent disposal of unwanted gas that may last for
content, especially methane, to products that are less hazardous to a few hours or a couple of days at often low ow rate. It occurs
the immediate vicinity of the are site. Gas aring is classied as a during well-testing as well as start-up and shutdown of process
stationary combustion source for the purpose of air pollution units. Production aring may occur continuously for years as long as
regulation (USEPA, 2008). The combustion process involves the the oil is being explored and exploited. The ow rate can be very
rapid oxidation of the fuel gas with the release of heat, gaseous and high at particular times especially during the initial development of
particulate pollutants, whose nature and quantity depend on the a gas well (Johnson and Coderre, 2011). As a result of the length of
amount and composition of gas fuel burned, the combustion time involved, which can be years, and the ow rate of the gas
characteristics as well as the are geometry and design (Ouf et al., ared, production aring is the major process of concern for
2008; Torres et al., 2012a). regional and global pollution, including interaction with climate.
Gas aring may be categorized as emergency, process and pro-
duction aring depending on the basis of the aring (Johnson and
3.1. Gas aring emission and its environmental impact

Gas aring is the process of disposing of gas (referred to as fuel


gas in this review), by combustion in an open ame in the open
atmosphere, using a burner tip designed specically for that pur-
pose, in the course of routine oil and gas production operations
(McEwen and Johnson, 2012; OGP, 2000; Stone et al., 1992). Gas
aring is a source of greenhouse gases, precursor gases, VOCs,
polycyclic aromatic hydrocarbon (PAH) and particulate matter (PM)
in the form of soot (Ana et al., 2012; Johnson et al., 2013; McEwen
and Johnson, 2012; USEPA, 2011; USEPA, 2012). These pollutants
have been identied to have serious detrimental impact on ani-
mals, vegetation and human (Burney and Ramanathan, 2014; Dung
et al., 2008; Pope III et al., 2002; USEPA, 2010). The soot emitted
from the combustion of natural gas is predominantly black carbon
(BC) (Johnson et al., 2013; Smith and Chughtai, 1995).
BC is a strong climate forcer and plays a prominent role in the
nature of the Earths climate because of its ability to absorb solar
radiation, and hence, to result in a changed vertical gradient of
warming by incoming solar radiation (Ramana et al., 2010;
Ramanathan and Carmichael, 2008). It also affects cloud pro-
cesses as well as decreasing surface albedo on ice and snow causing
them to melt faster (IPCC, 2007). It can be short-lived in the at-
mosphere, as it is removed from the atmosphere by dry and wet
Fig. 5. Higher heating value (HHV) as a function of molar mass of fuel gas for the Flow deposition (although insoluble in water, it is wettable, particularly
Station data reported in Table 1. when aged by atmospheric oxidation). When mixed with other
188 O.G. Fawole et al. / Environmental Pollution 216 (2016) 182e197

aerosol components in the atmosphere, BC can affect the climate X


for longer as its residence time is increased in that state (Bond et al., Cx Hy m O2 /pCO2 qCO rC vO2 fH2 O da;b Ca Hb
2013; Flanner et al., 2007; Quinn et al., 2008; Ramana et al., 2010). a;b
Within current estimated uncertainties, BC is the second highest (1b)
contributor to global warming just after CO2 (IPCC, 2007), and also
For ideal complete combustion, the oxidation of the hydro-
the main light-absorbing component of atmospheric aerosols
carbon yields carbon dioxide and water only (equation (1a)), while
(Bond et al., 2013; Chung and Seinfeld, 2005; Jacobson, 2002;
the oxidation of the sulphur (as H2S) and nitrogen content of the
Ramanathan and Carmichael, 2008; Seinfeld, 2008).
fuel gas gives SO2 and NOX respectively. In gas aring, NOX is pro-
The radiative forcing capacity of a cloud of aerosol particles
duced by thermal cracking of the nitrogen content of the fuel gas
depends on the ratio of the BC to other components in the cloud
and entrained atmospheric nitrogen. The amount of carbon-
(Ramana et al., 2010). The ubiquitous nature of BC coupled with its
containing emission (CO2, CO, CaHb, and BC) given off depends on
several effects on the Earths climate makes the study of its sources
the molar mass of non-CO2 carbon per mole of the fuel gas (cf.
and emission rates important. If adequate measures are put in place
Table 2). Smoking of a gas are does not necessarily imply that the
to reduce BC emission, short-term reduction of radiative forcing can
combustion process is highly inefcient; because a small amount of
be achieved in the Arctic and other oil rich regions of the world
soot can absorb and scatter perceptible amounts of visible light, a
(Arctic Council, 2013; Feichter and Stier, 2012; Tripathi et al., 2005).
are with a combustion efciency of 99% could still smoke visibly
Studies have shown that the contributions from oil and gas
(Castineira and Edgar, 2006).
processing, especially gas ares, to air pollution have been severely
underestimated (Edwards et al., 2013; Johansson et al., 2014;
Schultz, 2014; Stohl et al., 2013). This is arguably due to the fact 3.2. Emissions measurements around real-world gas aring sites
that emission factors (EF) often used to estimate the emissions of
pollutants from the oil and gas sector, especially gas aring, are too Few data of pollutants measurement around gas aring sites are
general and independent of site specics such as fuel composition publicly available. Data from the ACCESS aircraft campaign exper-
and combustion characteristics. There is a pressing research need iment in the Arctic (Norway) and a couple of ground-based in-situ
for more measurements and development of EFs estimates that measurements in Nigeria and the US show signicant contributions
vary with the fuel gas composition and combustion characteristics. from gas aring to ambient air concentrations of these pollutants.
At the local scale, ground-level measurements within one kilo- In-situ ground measurements of air pollutants around typical oil
metre downwind of the aring sites have indicated an elevated and gas facilities where varying degrees of gas aring take place
concentration of particulate and gaseous pollutants (Edwards et al., have been undertaken in the US (Edwards et al., 2013, 2014;
2013; Obanijesu et al., 2009; Sonibare et al., 2010). Likewise, on a Johansson et al., 2014), Mexico (Villasenor et al., 2003), Norway
regional scale, ight campaign during ACCESS (Arctic Climate (Roiger et al., 2015) and, Nigeria (Ana et al., 2012; Nwaichi and
Change Economy and Society) around oil and gas installations in Uzazobona, 2011; Obanijesu et al., 2009; Sonibare et al., 2010).
Heidrun, Norway reported elevated concentrations of NO, SO2 and Continuous noise levels higher than the WHO limit of 70 dB were
CO in the lower troposphere (Roiger et al., 2015). also observed around some gas aring sites in Nigeria
NOX (NO NO2), SO2, CO2, CO and unburned hydrocarbon are (Abdulkareem and Odigure, 2006; Avwiri and Nte, 2004).
the major pollutant constituents of gas aring plumes (USEPA, A 4-month sampling of three air pollutants (SO2, CO and NO2)
1995). The low amount of the nitrogen and sulphur content of around six ow stations in the Niger Delta area of Nigeria was
the fuel gas notwithstanding, the NOX and SO2 emission from gas undertaken by Obanijesu et al. (2009) and Sonibare et al. (2010).
aring remain signicant because the ambient background level of The measurements were made at 60, 200 and 500 m downwind of
both pollutants are usually low. Hence, gas aring can substantially the aring sites. Although to a varying degree depending on the
enhance the local concentrations of these pollutants. Complete capacity of the station, gas aring is a prominent daily activity
combustion is often not achieved in most aring conditions (Leahey within the stations. Mean pollutants measurements around the six
et al., 2001). During incomplete combustion, methane (CH4) and ow stations are shown in Fig. 6(a), (b) and (c). The variation bar on
other unburned components of the fuel gas are given off and some the bar-plots shows the standard deviation of the measurements
fuel components are partially oxidized to CO and soot rather than over the four-month period. The nature and extent of dispersion of
completely oxidized to CO2 (RTI, 2011; Strosher, 2000; Villasenor pollutants from a stationary source depend on the local meteo-
et al., 2003). Equation 1a and b, respectively, give simplied rology and topography of the area. As shown in Fig. 6(a)e(c), the
equations for the ideal complete and partial oxidation of the fuel trend of the measurements from the aring sites are similar to
gas. In equation (1b), rC0 denotes soot production, vO2 excess observations from dispersion model studies where concentrations
oxygen in the case of fuel-lean combustion and CaHb are PAH and of pollutants decreases exponentially with distance from the source
other semi-volatile organics resulting from the pyrolysis of hy- (Hodgson et al., 2007). Site 4 is the only place where a signicant
drocarbons in the fuel gas. The value of m in equation (1b) de- deviation from this trend, especially for CO and NO2, was observed,
termines a fuel-lean (over-red; m > x y/4) or fuel-rich (under- suggesting the likelihood of contributions from other source(s).
red; m < x y/4) combustion process. The level of combustion A summary of the few available in-situ ground measurements
(oxidation) of the fuel gas is dependent on a number of factors: the downwind of gas aring sites in other regions of the world are
nature of the ame during combustion, the level of mixing of the given in Table 3.
gas and air in the reaction zone, the amount of oxidant (oxygen)
available, the VHV of the fuel gas and the prevailing condition of the 3.3. Types of ares
ambient wind (Stone et al., 1992). Flare design and geometry are
also key determinants of the level of combustion of the fuel gas. Based on the design and operating condition of the system,
ares can be categorized as air-assisted, steam-assisted, non-assisted
 and pressure-assisted. Flares are assisted primarily to enhance the
y y
Cx Hy x O2 /xCO2 H2 O (1a) turbulence and mixing of the fuel gas and air in the combustion
4 2 zone, so as to suppress smoking of the resulting ame (Castineira
and Edgar, 2006; Enviroware, 2012; Torres et al., 2012a). The
O.G. Fawole et al. / Environmental Pollution 216 (2016) 182e197 189

Fig. 6. a: Spatial variation of SO2 concentration downwind of six gas aring sites (adapted from Obanijesu et al. (2009)). b: Spatial variation of CO concentration downwind of six gas
aring sites (adapted from Sonibare et al. (2010)). c: Spatial variation of NO2 concentration downwind of six gas aring sites (adapted from Sonibare et al. (2010)).

Table 3
Pollutant measurements around several oil and gas facilities.

BC (ng kg1) O3 (ppbv) VOC (ppbv) PAH (ng m3) NO (ppbv) NO2 (ppbv) SO2 (ppbv) CO (ppbv) Ref

e >120 100e350 e >3.5 >7.5 e >80 Edwards et al. (2013)


>40 >25 e e >1.2 e >1.2 >90 (Roiger et al., 2015)
e e e 0.34e3.3  104 e e e e (Ana et al., 2012)

choice of assistance, therefore, affects ame chemistry, as discussed actual air-fuel mass ratio. 4 < 1 implies fuel-lean mixture, that is,
below. Air and pressure-assisted ares are not as efcient as steam- more oxygen than is needed for the combustion of the fuel is
assisted ares in terms of the carbon conversion efciency (CCE) available; 4 1, a stoichiometric mixture, where the exact amount
(Castineira and Edgar, 2006). Complete combustion of the fuel gas of oxygen needed is made available, and 4 > 1, a fuel-rich mixture,
requires sufcient air for combustion and adequate mixing of the less oxygen than is needed is available for the combustion of the
air and fuel gas. The efciency of a gas are at a given moment in fuel. Burners used in gas aring and the entire gas aring set-up are
time depends on the HHV of fuel gas (see Table 2), design of the designed to produce a ame operating at 4 ~1 taking into account
burner, mixing of air and fuel gas in the combustion zone, the economic aspects such as cost effectiveness of applying a pro-
composition of the fuel gas, wind speed and direction, and ambient cess like steam assistance.
temperature and pressure (Kostiuk et al., 2004; Stone et al., 1992;
Torres et al., 2012b). 3.3.1. Steam- assisted are
Equivalence ratio, 4, is a measure of the amount of oxygen Steam-assisted are involves the introduction of steam jet into
available for the combustion of the fuel gas (Flagan and Seinfeld, the combustion zone of the are to provide added momentum and
2012; McAllister et al., 2011). It is dened as: turbulence to the fuel gas and air, enhancing mixing and as such
  suppressing the tendency for smoke in the are (Castineira and
A Edgar, 2006; Mller-Dethlefs and Schlader, 1976; Stone et al.,
F
1992). It is the most efcient assist given to are to suppress
4  s (2)
A smoking during combustion because the steam affects ame
F chemistry as well as mixing. The steam acts to break up long-chain
a
    hydrocarbons to smaller chains that burn with less smoke
where A is the stoichiometric air-fuel mass ratio and A is the (Castineira and Edgar, 2006; Fortner et al., 2012; Mller-Dethlefs
F F
s a
190 O.G. Fawole et al. / Environmental Pollution 216 (2016) 182e197

and Schlader, 1976; Torres et al., 2012a). Steam undergoes thermal 3.3.4. Non-assisted are
dissociation in a are ame to give H and OH free radicals that react For non-assisted ares, no provision is given to provide mo-
with carbon to give CH2- and eCHO radical moieties. The steam- mentum and enhanced mixing for the fuel gas and air. The method
induced free radicals enhance the formation of C]O bonds rather is often used for gases with low VHV, that is, fuel gas having low C-
than CeC bonds, promoting completeness of combustion. The to-H ratio (in alkanes, C-to-H ratio increases from a minimum value
steam can also react with intermediate products like CO, oxidizing of 0.25 for methane; see Table 2). The C-to-H ratio determines the
it further to CO2 (Castineira and Edgar, 2006; Mller-Dethlefs and smoking tendency of hydrocarbons, with smokiness increasing
Schlader, 1976). with C-to-H (USEPA, 1995). Note that the experimental fuel gas
compositions listed in Table 2 are at or below the lowest C-to-H
CO (g) H2O (g) CO2 (g) H2 (g) (DH 41 kJ mol1) (3) ratio of the Flow Station gas compositions listed. Non-assisted
aring is used for gases that require smaller amounts of air to un-
For a steam assisted are, combustion efciency starts to dergo complete combustion (Enviroware, 2012; Stone et al., 1992).
decrease when the steam-to-fuel gas ratio goes beyond a threshold Table 4 summarises the features of the different types of ares
which depends on the heat content of the fuel gas and the location discussed in Section 3.3.
at which the steam is injected into the combustion zone in the are
(USEPA, 2014). In the US, a lower heating value (LHV) limit of 4. Estimating emissions from gas aring
11.18 MJ/m3 is imposed on fuel gas in order to be suitable for steam-
assisted ares (Castineira and Edgar, 2006). Fuel gas with high heat Emissions from a typical gas are can be solids, liquids or gases.
content promotes higher combustion efciency in steam-assisted As a result of the inaccessible nature of full-scale real-world gas
ares (McDaniel and Tichenor, 1983; Torres et al., 2012b). Over- ares, several techniques have been used to quantify the amount of
steaming results when too much steam is injected into the com- emissions from such ares. Such methods include measurement or
bustion zone; over-steaming is analogous to over-aeration in air- source monitoring often by lab-based, pilot-study-based or eld-
assisted ares. Over-steaming causes a decrease in the ame tem- based study (Johnson et al., 2011; McEwen and Johnson, 2012),
perature by serving as a heat sink. A decrease in combustion ef- application of emission factors obtained from measurements and
ciency of the are results, along with, increased noise caused by scaling calculations (Giwa et al., 2014; Huang et al., 2015; Sonibare
cavitation created within the ame (Castineira and Edgar, 2006; and Akeredolu, 2004; Talebi et al., 2014; USEPA, 1995) and, simu-
Stone et al., 1992). lations, often by computational uid dynamics (CFD) (Almanza
The formation of NOX in steam-assisted ares is reduced, et al., 2012).
compared to non-assisted ares, and further reduced at large In real-world ares, complete combustion cannot be achieved
values of equivalence ratio (4) due to a drop in the ame temper- always and everywhere. Incomplete combustion of the fuel gas can
ature (Miyauchi et al., 1981; Mller-Dethlefs and Schlader, 1976). be due to poor efciency of the are system, ame temperature
Steam-assisted ares are rather expensive to maintain, especially (ame dynamical characteristics), insufcient oxygen resulting in
for large gas facilities, as a large-scale steam generator is required. poor stoichiometric air/fuel gas mixing ratio, the condition of the
fuel gas in the combustion zone and prevailing ambient meteoro-
3.3.2. Air-assisted are logical condition (Stone et al., 1992). Carbon monoxide (CO) can
In air-assisted ares, forced air from a low-pressure blower is represent 24e80% (on carbon a molar basis) of emissions for an
used as an additional source of momentum and turbulence to the incomplete combustion process (Torres et al., 2012b).
fuel gas in the combustion zone and, hence, enhances the mixing of
the fuel gas and air in the zone (Castineira and Edgar, 2006; Stone 4.1. Determining the ame regime
et al., 1992; Torres et al., 2012a). Air-assisted aring involves the
installation of an air blower that provides the forced air at the It is important to dene clearly the conguration of the re
bottom of the stack. The major advantages of the air-assisted are (are) as this is essential for an adequate estimation of the yield and
are that it is less expensive to run, extends the life-span of the are transport of pollutant species from the combustion process. Flames
by cooling the tip of the are and is easier to maintain than other can be classied along a spectrum ranging from turbulent diffusion
congurations (Castineira and Edgar, 2006). For an air-assisted ames (of the kinds discussed above) to pool res (e.g. tar-pool re)
are, the combustion efciency of the are decreases linearly based on the nature and dynamics of the fuel in the ame as well as
above a threshold limit of the air assist to fuel-gas ratio, but the rate the design of the burning process (Delichatsios, 1987, 1993a). In this
of decrease is slow for a fuel gas with a higher VHV (Torres et al., review we are concerned with gas ares, which are classied as
2012b). Incomplete combustion can occur when air-fuel gas ratios turbulent jet-diffusion ames. They are so classied because of the
go beyond the optimum value, to the extent that the ame may be high pressure associated with the release of the fuel gas into the
put out as a result of over-aeration (Castineira and Edgar, 2006). ame.
Jet-diffusion ames in the environment can be categorized
3.3.3. Pressure-assisted are based on the momentum ux ratio, R, of the jet plume versus the
In pressure assisted ares, the fuel gas stream pressure is horizontal momentum ux of the ambient wind (Huang and Wang,
controlled by varying the volume ow of the fuel gas, and used to 1999). Flares with high R (R > 10) may be further categorized
enhance the mixing of the fuel gas and air in the combustion zone. depending on whether the ame characteristics are driven by the
A high-pressure burner is used to promote atomization of any buoyancy of the hot plume or momentum of the fuel gas (McEwen
liquid hydrocarbon and enhance the mixing of the fuel gas with air and Johnson, 2012). Both buoyancy and momentum are important
to bring about a complete or near-complete combustion. Pressure in determining the character of ares. A combination of several
assistance often requires signicant amount of space in a remote dimensionless parameters e Richardson number, Richardson ratio,
area because of the burners arrangement at ground level. Fuel gas re Froude number, gas Froude number, and Reynolds number -
exit velocity increases with pressure at the burner. Pressure- have been used in studies to congure the regime of the ame in a
assisted ares usually have burners arranged on the ground and jet-diffusion ame. The Froude numbers measure the ratio of the
as such must be located carefully within the oil and gas production inertia force on an element of the uid (in this case, gas or re) to
plant (Enviroware, 2012; Stone et al., 1992). the weight of (i.e. gravitational force acting on) the uid element.
O.G. Fawole et al. / Environmental Pollution 216 (2016) 182e197 191

Table 4
Summary of the properties of are types.

Steam-assisted Air-assisted Pressure-assisted Non-assisted

Method Steam is introduced into the Air is introduced from a blower to The vent pressure of the gas ow is used to No assistance is given to the
combustion zone to enhance enhance the mixing and turbulence of enhance mixing at the tip of the are combustion process
mixing. the fuel gas in the combustion zone burner
Efciency Most efcient in terms of Less efcient than the steam assisted Not as efcient as steam and air-assisted Only efcient for non-sooting
suppressing soot formation. are but relatively efcient that the but can equally suppress sooting. combustion especially in light
Some of the CO formed can be other two types hydrocarbons
oxidized to CO2
Benets Fuel with high heat value, and Prolongs the life span of the are tip. Enhance combustion efciency when the Can be used for occasional
hence, high sooting propensity Less expensive than steam-assisted and gas ux pressure is sufciently high emergency aring of near
can be disposed of with relatively easy to maintain, hence, it is the most enough without the additional cost of smokeless gas
less soot commonly used. steam and air generation
Relative size They are often large ares as they Not as large as the steam assisted. May be of same size as air-assisted are Often smaller in size compared to
include the steam generator and depending on the ow capacity of the the other types
are usually employed in large gas facility
facilities.
Shortcoming Over-steaming can result in Over- aeration can also result in less The uctuation of gas ow pressure has a Cannot be used for dense fuels with
reduced efciency of are. It is efciency. A limit of air assist to gas ratio bearing consequence on the efciency of high sooting propensity which are
also expensive to maintain on a must be maintained for effectiveness of the combustion. Requires large space in a typical gas in oil and gas processing
large-scale the are. remote area. facilities

The re Froude number, Frf , gas Froude number, Frg and Reynolds expressed in g m3 (pollutant produced per unit volume of raw
number, Re, have proved to be useful dimensionless parameter to material consumed), g kg1 (pollutant produced per unit mass of
dene the ame regime (Becker and Liang, 1982; Delichatsios, raw material consumed), g km1 (pollutant produced per unit
1993a, 1993b, 1987; Sivathanu and Faeth, 1990). distance travelled). Emission factors have been compiled by several
agencies, which include the US Environmental Protection Agency
3
=
ue f s 2 (USEPA), the European Environmental Agency (EEA), the United
Frg  1 4 = (4) Kingdom Department for Environment, Food and Rural Affairs
gde 2 rre
1 =
(Defra), and GAINS (Greenhouse gas Air Pollution Interactions and

Synergies), for several source categories based on technical sessions
of lab-based studies, pilot studies or actual eld measurements. Of
3
=
ue fs 2 these agencies, ECLIPSE and USEPA have EFs specically for emis-
Frf  1 2  1 4
= = (5) sions from gas ares: the GAINS emission factor for BC from gas
DTf re aring is 1.6 g m3: the equivalent USEPA value has four discrete
T gde r
values between 0 and 6.4 g m3 depending on the smokiness of the

ame (see below). Stohl et al. (2013) in their study used emission
ue de factor of 1.6 g m3 obtained from ECLIPSE (Evaluating the Climate
Res (6)
yo and Air Quality Impacts of Short-lived Pollutants) emissions data
set to simulation BC emissions in the Arctic.
1 It is difcult to carry out an accurate estimate of emission from
fs (7) gas ares directly from eld measurements. Conventional experi-
S1  
DT mental techniques are not suited due to the severe operating
In the denition of Frf in equation 5; Tf g is the effective conditions that occur in the aring process and the almost unin-
acceleration generated by individual hot eddies burning at the habitable nature of the gas aring area to both man and the eld
ame temperature (Delichatsios, 1987). Among the three dimen- equipment during the process of gas aring (Umukoro and Ismail,
sionless numbers dened by equations (4)e(6), the Reynolds 2015; McDaniel and Tichenor, 1983; McEwen and Johnson, 2012;
number is used to determine the status of ow, either turbulent or RTI, 2011; Talebi et al., 2014). As a result of the unsteady and opa-
laminar. The re Froude number, Frf, is used to identify the domi- que nature of gas are ames, remote sensing provides only a
nant mechanism between buoyant-generated turbulence and partial answer to the difculties of in-situ monitoring.
momentum-generated turbulence. In practice, Frf can be used to In Chapter 13 of USEPAs 5th edition of the compilation of air
parameterise soot yield from turbulent diffusion ames pollutant emission factors known as AP-42, published in January
(Delichatsios, 1993b; McEwen and Johnson, 2012). 1995, emission factors (EF) for pollutant emitted from industrial
aring of waste gas were given; these were recently updated in
4.2. Emission factors (EF) for gas aring emissions 2014 (though still in the draft stage) except those for soot. The EFs
published in 1995 were based on a study conducted by McDaniel
The Emission factor (EF) of a pollutant is the amount of the and Tichenor (1983) aimed at determining combustion efciency
pollutant released into the atmosphere per unit activity or per unit and hydrocarbon destruction efciency for ares operated under
raw material consumed. It can be obtained from experimental different condition. The recent updates of EFs in AP-42 give emis-
measurements carried out on several sources which represent a sion factors of 0.17 kg GJ1, 1.43 kg GJ1 and 0e6.4 g m3 are given
particular emission source type. For example, road transport for CO, NOx and soot, respectively.
emission factor can be compiled by measuring the amount of each The fuel used in the pilot study to estimate EFs for industrial
pollutant (CO2, CO, PM, NOx) given off by cars (petrol and diesel), are pollutants in the AP-42 compilation was predominantly pro-
heavy duty vehicles and motorbikes per litre of fuel burned for pylene and inert diluents. As such, the EFs, especially for soot, might
every km travelled (Gertler et al., 1998; USEPA, 1995; Zhang and not be an adequate representation of a typical are in the oil and
Morawska, 2002) under given driving conditions. It is often
192 O.G. Fawole et al. / Environmental Pollution 216 (2016) 182e197

gas industry with varying fuel gas composition (Table 2). For AP-42, Several attempts have been made to quantify and study the
the collection of soot at the experimental stage was not done by a characteristics of soot yield from gas ares using various ap-
conventionally accurate method. For instance, the particulate proaches in lab-based, pilot-based and eld-based studies as well
matter (soot) given off was not collected isokinetically in accor- as simulation techniques. Emission factors from some of these
dance with USEPAs method 5 for sampling particulate matter from studies are given in Table 5. Other emission factors not highlighted
stationary source (USEPA, 2000). An emission factor of 0.0 mg L1 in this table are based on the USEPAs AP-42 emission factors.
(microgram per litre of fuel gas at standard temperature and The studies by Johnson et al. (2011, 2013) gave emission rates
pressure) given for soot in non-smoking ares of industrial ares in (g s1) and not emission factors (g m3) because both were actually
AP-42 is of limited utility and presumably denotes an upper limit of eld studies that quantied the soot given off per unit time by
0.05 mg L1, because the soot yield from ares is never likely to be estimating the travel (speed) of the soot in space using a charge
precisely zero. Even seemingly modest emission of soot (BC) can be couple device camera (CCD) camera viewing a real eld are.
signicant, given what is now known of the effects of BC on climate, Emission of soot from the combustion of hydrocarbon varies
weather and human health from ndings in recent studies (Bond with the VHV of the gas and, as such, the emission factor for soot
et al., 2013; Ramanathan and Carmichael, 2008; Stocker et al., can be estimated from its VHV (McDaniel and Tichenor, 1983; RTI,
2013; Tripathi et al., 2005; Wang et al., 2014). 2011; Torres et al., 2012b). McEwen and Johnson (2012), using a
The mass/mole balancing technique for estimating the yield of lab-based experiment, studied the BC emission from the combus-
pollutants from the combustion of hydrocarbon is a widely used tion of hydrocarbon. The study varied the VHV of the fuel gas and
technique. Using this technique, Umukoro and Ismael (2015) and measured the soot yield for each combustion process. The VHV
Sonibare and Akeredolu (2004) estimated the yield for SO2, NOX, used here is the higher heating value (HHV), or gross heating value.
CO2 and CO from the combustion of fuel gas (hydrocarbon with The relationship between the two variables (soot yield and HHV)
inert diluents) at various levels of combustion. Both studies did not obtained from the study by McEwen and Johnson (2012) is given in
account for unburned carbon (soot) even for their severely equation (8):
incomplete combustion process reactions. Umukoro and Ismail
(2015) varied combustion efciency (CE) and air available for EFsoot 0:0578VHV  2:09 (8)
combustion, and with CE as low as 0.5 (50%) still did not account for When the composition of the fuel gas is known, its VHV can be
unburned carbon. calculated from standard thermochemical tables (cf. Table 2). It
should, however, be noted that because the VHV contains no in-
4.3. Soot emission from gas aring formation on ame dynamics, this relationship is only appropriate
for the ame dynamics conditions of the experiment. Although,
Soot, which is predominantly black carbon (BC), is a product of equation (8) is a readily available relationship to estimate soot
the incomplete combustion of biomass, solid fuel and fossil fuel emission from hydrocarbon combustion, its application is restricted
(Goldberg, 1985; Koch et al., 2009). Globally, fossil fuel combustion to a complete or near-complete combustion process. Inserting the
is estimated to contribute 3 Mt of BC to the atmosphere annually estimated VHV into the relation developed by McEwen and
(Bond et al., 2004). Annually, the contribution of gas aring to Johnson (2012) gives an estimate of the soot yield in g m3.
global BC concentration is estimated to be 260 Gg (Bond et al.,
2013), that is approximately 0.1% of the total contribution from
fossil-fuel use, of which Russia is estimated to contribute 81.0 Gg 4.4. Scaling soot emission from lab-based studies
(Huang et al., 2015).
The formation and quantication of soot from the combustion of Lab-based studies of emissions from ares are the most com-
hydrocarbon is a rather complex thermo-chemical process that is mon and readily available method to estimate emissions from full-
not well understood, despite decades of research (Castineira and scale ares. However, considering the size (diameter) of the are
Edgar, 2006; Haynes and Wagner, 1981; Johnson et al., 2011; stack, ow rate of fuel gas, exit velocity, and the resultant buoyancy
Maricq, 2009). Soot given off from the combustion of hydrocar- of full-scale are, there is a need to scale up the emissions yield
bon is predominantly elemental carbon and the amount given off from lab-based studies to be representative of a full scale are. In
depends on a number of factors, including the efciency of the earlier studies, several dimensionless parameter have been
combustion process and the re dynamical characteristics. considered for such scaling purpose; these include Richardson ra-
The diameter of soot particles emitted ranges between 10 and tio, RiL (Becker and Liang, 1982), re Froude number, Frf (McEwen
200 nm and most commonly lies between 10 and 50 nm. Fig. 7 and Johnson, 2012), and the rst Damko hler ratio, Da1 (Becker
shows a TEM micrograph of soot particle and agglomerates from and Liang, 1982). Richardson ratio, RiL , is dened as the ratio of
acetylene ames. The very ne particle of soot are from seemingly the buoyancy-generated turbulent kinetic energy (TKE) of the
non-sooting ames while at the other extreme are those from ame to the TKE of emitted gas jet at the exit:
heavily sooting ames (Flagan and Seinfeld, 2012; Glassman, 1996;
 
Haynes and Wagner, 1981). Combustion of hydrocarbon compo- gL3 r
RiL (9)
nents of the fuel gas has PAH and BC signatures which can be used
ue de 2 re
as tracers for emissions from the aring of fuel gas (Fortner et al.,
2012; Maricq, 2009). Richardson ratio is the basis to assess the turbulent regime of
Soot is formed when the carbon particles are cooled below their the ame: when RiL 1, buoyancy-induced mixing between
ignition temperature and there is a deciency of oxygen (Stone emitted gas jet and background air is much weaker than jet-
et al., 1992). Considering the variation of the composition of gas induced mixing, and consequently the ame is dominated by
ared from one station to the other, EFs available for estimating forced convection; when RiL [1, jet-induced mixing is much
emissions from gas ares are overly generalised. The fuel gas used weaker than buoyancy-induced mixing and the ame is dominated
in most of the studies to estimate the EFs is either propylene or by natural convection. Fire Froude number, Frf , is dened in
propane or a mixture of both with nitrogen added to alter the heat Equation (5) and can be interpreted as the ratio of the jets inertia to
content as well as the use of predominantly methane-based fuels the buoyancy force acting on it. Fire Froude number can be used to
which are known to be low-sooting. assess the dominating force to stretch the ame: when Frf [1,
O.G. Fawole et al. / Environmental Pollution 216 (2016) 182e197 193

Fig. 7. TEM micrograph of soot (a) microstructure (b) agglomerates (Tumolva et al., 2010).

Table 5
A Summary of Emission Factors/Emission rate for Soot from Industrial Flares.

Study (year) Emission factor (g m3 of fuel burned) Emission rate (g s1) Type of study Fuel

USEPA (1995) 0.0, 0.9, 4.2 6.4a e Pilot study 80% propylene 20% propane
Johnson et al. (2011) e 2.0 (0.66) Field study associated natural gas
Almanza et al. (2012) e 0.025e0.22 CFD simulation Associated natural gas
McEwen and Johnson (2012) 0.51 e Lab-scale are Hydrocarbon (alkanes)
Johnson et al. (2013) e 0.067 Field study e
GAINS 2011 1.6 e Modelling e
IMP (2006) b e 3.37 Simulation Associated natural gas
CAPP (2007) 2.563 e e Associated natural gas
a
0.0 is for non-smoking ame, 0.9 for light smoking ares, 4.2 for averagely smoking are and 6.4 for heavily smoking ares.
b
Cited in (Almanza et al., 2012).

the jets momentum is the dominating factor and when Frf 1, the The rst Damko hler ratio, Da1, however, is dened as the ratio of
ames buoyancy force is the dominating factor. Comparing Frf residence time of fuel in ame (tres ) to chemical time of burning
against RiL , we understand that both are used to assess the domi- process (tchem ):
nating factor between jet-related quantity and buoyancy-related  
quantity, but there are two differences: (1) the quantity is mo- residence time in flame; tres L 
Da1 tchem (11)
mentum ( velocity) for Frf , but TKE ( velocity  velocity) for RiL ; chemical time; tchem ue
(2) the ratios between jet-related quantity and buoyancy-related
quantity are reciprocal: RiL (buoyancy-related quantity)/(jet- It describes the extent of the oxidation process within the ame
related quantity) whereas Frf (jet-related quantity)/(buoyancy in relation to the oxidants feed rate. For a large Da1 (i.e.
-related quantity). Therefore, these two parameters are closely tres [tchem ), the velocity uctuating component does not have
related and mathematically their relationship should be RiL Frf2 . much inuence on the chemistry of the ame. The chemical reac-
Precise relationship between them can be derived from Equations tion is able to proceed to completion within the residence time in
(5) and (9): the combustion zone, resulting in intensive chemical reaction and
hot diffusion ame. For a small Da1 (i.e. tchem [tres ), turbulence
 3 2 
= 3 ! can signicantly affect the chemistry and structure of the ame.
r L T The rate of chemical reaction and hence, heat release may be
RiL $fs3 $Ff2 r (10)
re de DTf affected, causing combustion product to be mixed with reactants
 3 within a time interval shorter than the chemical reaction time
It is noted that L can be interpreted as the volume expan-
de
!1 (Liberman, 2010; William, 1985). From the perspective of processes,
T
Da1 involves an extra dimension (i.e. chemical processes) which is
sion ratio of the aring gas due to burning and DTf can be not reected by either RiL or Frf . In principle, we should consider
Da1 as one more scaling parameter.
approximated as the temperature rising ratio of the aring gas due
to burning. Based on the gas law, these two are proportional to each
other for an isobaric process (from the exit to the ame tip) which is
 3 !1 4.5. Soot modelling
a good assumption for gas aring, i.e. dL DTT , or equiva-
e f
Mathematical modelling is a technique that has been used by
 3 !
scientist and engineers over the years to understand the relation-
L T
lently, de DTf zconst. Therefore, Equation (10) conrms the ship between sets of input and output parameters in a process,
especially where the real world process is often remote or grossly
relationship of RiL Ff2 r. This suggests a strong dependence be- complicated to assess. The region of validity of such model outputs
tween adopting RiL and adopting Frf as the scaling parameter. is often limited as several assumptions and constants are applied in
194 O.G. Fawole et al. / Environmental Pollution 216 (2016) 182e197

the modelling to further simplify the process being studied. the left represent the growth and nucleation, respectively.
Soot formation and oxidation in pre-mixed and non-premixed Lautenberger et al. (2005) developed a CFD model to study the
(diffusion) hydrocarbon ames have been studied using several formation and oxidation of soot. Since their model was to generate
modelling techniques including computational uid dynamics sufciently accurate predictions of soot emission concentrations in
(CFD). The main problem with mathematical modelling of turbu- order to estimate CFD simulations of re radiation from turbulent
lent combustion of hydrocarbon is the problem of modelling tur- ames, considerations were given only to phenomena which were
bulent ow and chemical kinetics and the interaction between ow essential. Soot estimation in their model was based on a further
and chemical reaction (Magnussen and Hjertager, 1977). Kennedy simplied form of the two-equation model of Moss et al. (1989).
(1997) classied the models for soot formation as empirical cor- There are no fuel-specic constants in their estimations, but rather,
relations, semi-empirical correlation models and models with they used the laminar smoke point height to account for the
detailed chemistry and physics of soot formation. The ame tem- sooting propensity of different fuels. The smoke point of a ame is
perature, C:H ratio and number of carbon atoms in the fuel (hy- its length just before the onset of the release of visible smoke.
drocarbon) are important parameters considered to have strong Length of a ame is dependent on the extent of completeness of the
inuence on the sooting propensity of the hydrocarbon (Harris combustion and heat content of the fuel gas (Beychok, 1994).
et al., 1986). These parameters have been the basis of measure- The use of CFD simulation soot has made it possible to make
ments used in most empirical correlation models. predictions about the relationships between the various processes
In their study to modelling soot formation and combustion, involved in soot formation and oxidation in both pre-mixed and
Magnussen and Hjertager (1977) assumed that soot is formed from diffusion hydrocarbon ames as well as the sensitivity of the soot
a gaseous hydrocarbon in two stages (a) formation of radical nuclei, formation to some of the complex phenomena. However, the ve-
and (b) soot particle formation from these nuclei. Applying ex- racity of CFD simulation results in limited by the availability of eld
pressions for the rate of formation of radical nuclei and rate of soot measurements for model evaluation.
particle formation expressions developed by Tesner et al. (1971a)
(Tesner et al., 1971b); in their model, tested on both pre-mixed
and diffusion ame, they predicted soot concentrations that are 4.6. Gas aring emissions in global models and inventories
in close agreement with experimental data. They concluded that
soot formed and was contained in eddies and burned away during To the best of our knowledge, the only two emission datasets
turbulence dissipation. that explicitly includes gas aring emissions are EDGAR (Emissions
Moss et al. (1989), using a two-equation model for the evolution Database for Global Atmospheric Research) and ECLIPSE (Evalu-
of soot volume fraction and number density, simulated the for- ating the Climate and Air Quality ImPacts of Short-livEd Pollutants)
mation of soot. They included the inuences of nucleation, surface gridded emissions datasets.
growth and coagulation on the rate of soot formation. As given in In EDGAR v4.2, for gas venting and aring, emissions were
equation 12(a) and (b), their model contains simplied expressions calculated for 1994 onwards using the amount of gas ared esti-
to quantify particle nucleation, growth and coagulation; using mated from satellite observations of intensities of light from
three empirical constants that are dependent on the fuel to control various gas ares. The estimated quantities of gas ared and
the rate of these processes. A major nding from their study is that emission factors obtained from either inventory guidance docu-
soot volume fraction is proportional to the square of pressure. ments or condential information were used to generate gridded
annual emission datasets for different countries on a resolution of
 
8 n 9
0.1 x 0.1. In 2005, the inclusion of new primary data sources for
d
< No =  2
n gas aring in EDGAR v4.2 gives rise to a change of 75% of EDGAR
az  bz (12a) 4.1 value (130 Tg) in global CO2 emission (European Commission,
: dt ; N0
2009).
ECLIPSE is provided by the IIASA (International Institute for
 
dfv Applied Systems Analysis). Emission calculations for the historical
rs gzn dz (12b)
dt years (2005e2010) were developed in a series of regional and
global projects. For gas aring, emissions were calculated using
where rs is the assumed density for solid carbon (1.8  103 kg-3), No data available from NOAA, NASA and the World Bank collaborative
is Avogadros number and z is the mixture fraction. Rates of the work to estimate the volume of gas ared globally. The volume of
processes are expected to be a function of the mixture fraction. The gas ared was estimated using NASA MODIS active re detection
rates of the processes are dened explicitly in terms of the fuel products (Elvidge et al., 2007, 2011). Emission factors and other
density, r, temperature. T, and fuel mole fraction, Xc as described in parameterizations were obtained from peer-reviewed data on
equation (13): emission performance of various technologies. The calculation was

9
>
>
    >
=

aCa r2 T 1=2 Xc exp Ta=T ; bCb T 1=2 gCg rT 1=2 Xc exp Tg T ; dCd a (13)
>
>
>
;

coefcients Ca,b,g,d and activation temperatures, Ta and Tg are ob- performed with the IIASA GAINS model (Klimont et al., 2013). The
tained from experimental data. In equation (12a), the rst and ECLIPSE v4 global emission dataset is available on a 0.5 x 0.5 lon-
second term on the left are nucleation and coagulation processes, lat resolution.
respectively. And, in equation (12b), the rst and second term on Stohl et al. (2013), performing a 3-year black carbon (BC)
O.G. Fawole et al. / Environmental Pollution 216 (2016) 182e197 195

simulation in the Arctic, using a Lagrangian particle dispersion inventories.


model FLEXPART driven by the ECLIPSE dataset, estimated that Global models need to update the sources of BC to include gas
more than 40% of mean surface BC surface concentration in the aring, especially in regions prone to long-range transfer of gas
Arctic is attributable to gas aring. Although, more studies on the aring emission from leading gas aring nations including Russia,
sensitivity of global models to gas aring emission is needed to give Nigeria and the Middle East.
a clear and precise quantication of the contribution of gas aring
emission to global aerosol loadings, the change in global CO2 level Acknowledgment
in EDGAR4.2 underscores the importance of an explicit inclusion of
gas aring emissions in global models. Olusegun G. Fawole is highly grateful to the UK government for
funding his PhD studies through the UK Commonwealth Scholar-
5. Conclusions ships Commission (CSCUK) NGCA-2013-70. The authors appreciate
the anonymous reviewers for their helpful criticisms and
The World Bank has been at the fore-front of the campaign to comments.
reduce gas aring through the public-private partnership project
Global Gas Flaring Reduction (GGFR) (http://www.worldbank.
Glossary
org/en/programs/gasaringreduction). The Zero Routine Flaring
by 2030 initiative was launched in April 2015 by the World Bank,
1. Heating value e the heat evolved per unit of a gas when it un-
United Nations, governments and oil companies. As at April 17,
dergoes complete combustion at standard temperature and
2015, a total of nine countries have agreed to the Zero Routine
pressure. It can be measured in unit mass, unit mole or unit
Flaring by 2030 initiative. At the time of writing, some major
volume.
aring nations have yet to sign up to the initiative. Indeed, some
2. Higher (gross) heating value (HHV) e The heating value when
major aring countries still struggle to meet targets for gas aring
all of the water present in the combustion product in gas phase
set in the late 1980s. A steep increase in aring since 2006 has been
condenses to liquid.
reported for the USA and Canada, associated, presumably, with the
3. Lower (net) heating value (LHV) - The heating value when all of
exploitation of unconventional hydrocarbon reservoirs.
the water present in the combustion product remains in the gas
Considering the wide spectrum, quantity and effects of pollut-
phase.
ants emitted from gas aring, coupled with the estimated quantity
4. Volumetric heating value (VHV) e Total heat evolved per unit
of gas ared globally, it is surprising that so little effort has been put
volume of a gas.
into adequately understanding the yield of pollutants, especially
5. Equivalent ratio, 4 - This is the ratio of the stoichiometric air-fuel
BC, from the process in real world eld situations. The wide vari-
mass ratio to the actual air-fuel mass ratio
ation of fuel gas compositions from ow stations around the world
6. Mtoe e Million tonnes of oil equivalent
underpins the importance of developing strategies that take these
7. Laminar smoke point - The length of ame from a gas jet just
compositions into consideration when estimating emissions.
before the onset of the release of visible smoke.
The steep decrease in the fraction of total gas production ared
between 2000 and 2006 seems to have stabilised between 2007
and 2010, and the fraction has even increased in 2011. The overall
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