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Atmospheric Environment 184 (2018) 1–8

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Atmospheric Environment
journal homepage: www.elsevier.com/locate/atmosenv

Emission characteristics of NOx, CO, NH3 and VOCs from gas-fired industrial T
boilers based on field measurements in Beijing city, China
Tao Yuea,b, Xiang Gaoa, Jiajia Gaob,∗, Yali Tongb, Kun Wangb, Penglai Zuob, Xiaoxi Zhangb,
Li Tongb, Chenlong Wangb, Yifeng Xuec
a
State Key Laboratory of Clean Energy Utilization, Zhejiang University, Hangzhou 310058, China
b
Department of Air Pollution Control, Beijing Municipal Institute of Labour Protection, Beijing 100054, China
c
National Engineering Research Center of Urban Environmental Pollution Control, Beijing Municipal Research Institute of Environmental Protection, Beijing 100037, China

A R T I C LE I N FO A B S T R A C T

Keywords: In the past decade, due to the management policies and coal combustion controls in Beijing, the consumption of
Gas-fired industrial boilers natural gas has increased gradually. Nevertheless, the research on the emission characteristics of gaseous pol-
Gaseous pollutants lutants emitted from gas-fired industrial boilers, especially considering the influence of low nitrogen (low-NOx)
Emission inventory retrofit policy of gas boilers, is scarcely. In this study, based on literature and field investigations, onsite mea-
Operating load
surements of NOx, CO, NH3 and VOCs (Volatile Organic Compounds) emissions from gas-fired industrial boilers
Flue gas recirculation
as well as the key factors that affected the emission of gaseous pollutants were discussed. Category-specific
emission factors (EFs) of NOx, CO, NH3 and VOCs were obtained from the field measurements of 1107 “low-
NOx” retrofitted and unabated gas-fired industrial boilers. Our results showed that operating load and control
measures were the two key factors affecting the formation of gaseous pollutants. The EFs of NOx (EFNOx) and CO
(EFCO) of atmospheric combustion boilers (ACBs) were much higher than the EFs of chamber combustion boilers
(CCBs). The total emissions of NOx, CO, NH3 and VOCs from gas-fired industrial boilers in Beijing in the year of
2015 were estimated at 10489.6 t, 3272.8 t, 196.4 t and 235.4 t, respectively. Alkanes, BTEX, oxygenated VOCs
and non-reactive organic matter were the four main chemical components of VOCs. As for the spatial dis-
tributions, the emissions of NOx, CO, NH3 and VOCs from gas-fired industrial boilers in Beijing were pre-
dominantly concentrated in central six urban districts. In the future, more detailed investigation and field tests
for all kinds of gas-fired industrial boilers are still greatly needed to achieve more reliable estimations of at-
mospheric pollutants from gas-fired industrial boilers.

1. Introduction (Xue et al., 2017).


Compared to coal, the particulate matter (PM) and SO2 emissions
Nowadays, with the rapid development of economy and an increase from natural gas combustion are less. However, NOx is considered to be
in primary energy consumption, Beijing is facing severe environmental the most significant gaseous pollutant emitted from natural gas com-
air pollution (Xue et al., 2016; Gao et al., 2018). Government has bustion (Simmons and Seakins, 2012; Zhang et al., 2016). NO and NO2
committed to control air pollution and improve ambient air quality by are the main components produced from gas combustion. When NO and
adjusting energy structure in recent years. With the implementation of NO2 are discharged into the atmosphere, nitric acid fog and nitrate are
the Clean Air Action Plan of Beijing 2013–2017, the energy structure of generated through a series of physicochemical reactions. Under sun-
Beijing is continuously optimized. The application fields of natural gas light, nitrate combines with hydrocarbons and ozone to produce pho-
are increasingly expanding so as to the gas consumption increases ra- tochemical smog, which has a great impact on the atmospheric en-
pidly. In 2015, according to the gas development and planning from the vironment and human health (Wu et al., 2010; Li et al., 2015; Feng
Beijing Gas Group Co. Ltd, the consumption of natural gas increased et al., 2016). In 2016, the gas used in heating accounted for more than
from 6.1 billion m3 in 2008 to 14.6 billion m3, and more than 78% of 30% in Beijing, and the gas-fired industrial boiler has been an im-
natural gas was used for heating and power generation (BMCCM, portant stationary source of NOx emission in Beijing (Yan et al., 2017).
2017). In addition, the capacity and amount of gas-fired industrial Nevertheless, the understanding of the emission characteristics of gas-
boilers both accounted for more than 85% of the total industrial boilers fired industrial boiler is limited. Considering the emission


Corresponding author.
E-mail address: jiajia11757@126.com (J. Gao).

https://doi.org/10.1016/j.atmosenv.2018.04.022
Received 2 February 2018; Received in revised form 11 April 2018; Accepted 13 April 2018
Available online 17 April 2018
1352-2310/ © 2018 Elsevier Ltd. All rights reserved.
T. Yue et al. Atmospheric Environment 184 (2018) 1–8

characteristics of gas-fired boiler, some studies have mainly focused on 2.2. Activity data
the NOx emission based on the field measurements (England et al.,
2001; Pulles and Heslinga, 2004; Wang et al., 2016; Xue et al., 2017). The natural gas consumption was obtained from the China
Wang et al. (2016) presented the status of NOx emissions of district Statistical Yearbook (NBSPRC, 2016), Beijing Statistical Yearbook
central heating gas boilers in Beijing by measuring eighty-five gas (BMBS, 2016) and other related references (Xue et al., 2017; Yan et al.,
boilers. Xue et al. (2017) established a NOx emission inventory in 2017). A database containing detailed information of 12266 gas-fired
Beijing based on the field measurements of five gas-fired industrial industrial boilers with a gross capacity of 39705 t/h was established at
boilers. However, limited largely and systematically field measured the unit level. The detailed information included the geographic loca-
data have been obtained to study the category-specific emission factors tion, operating load, combustion mode, installed capacity, annual nat-
(EFs) of NOx, CO, NH3 and VOCs for different types of gas-fired in- ural gas consumption, control technologies and pollutants concentra-
dustrial boilers, which is essential for the estimation of accurate emis- tion in the flue gas for each unit. Therein, combustion mode covered
sions and spatial variation of gaseous pollutants from gas-fired in- atmospheric combustion (AC) and chamber combustion (CC), and CC
dustrial boiler. was subdivided into direct-combustion machine (CCM), horizontal in-
Furthermore, according to the revised Emission Standard of Air ternal-combustion (HIC) and others. Moreover, the majority capacity of
Pollutants for Boilers in Beijing (BMEPB, 2015), the NOx emission of the gas-fired industrial boilers is below 10 t/h, which account for more
the new built boilers must be lower than 30 mg/m3 since April 1, 2017. than 90% of the total amount. In terms of combustion mode, more than
Simultaneously, for the retrofitted boilers, the emission standard of 80% of gas-fired industrial boilers is CC mode. The gas-fired industrial
NOx has dropped from 150 mg/m3 to 80 mg/m3. In order to ensure the boilers in this database accounted for 77.5% of the total gas-fired in-
implementation of this revised standard and encourage the low ni- dustrial boilers in Beijing, which could be well represent the status of
trogen (low-NOx) retrofit of existing gas (oil) boilers, Beijing municipal gas-fired industrial boilers in Beijing.
government proposed a Regulation of the Beijing Municipal Reward The geographic locations of gas-fired industrial boilers are pre-
Replaces Subsidy for the Gas (oil) Boiler Low-NOx Retrofit in June 4, sented in Fig. 1. As can be seen that gas-fired industrial boilers are
2016 (BMEPB, 2016). Although there are no emissions standards of CO, mainly distributed in central six urban districts, namely Chaoyang,
NH3 and VOCs for boilers at present, NH3 and VOCs are the precursor of Dongcheng, Fengtai, Haidian, Shijingshan, and Xicheng district. It is
PM2.5 secondary transformation. Additionally, CO, NH3 and VOCs are related to the substitution of coal-fired boilers with gas-fired industrial
the essential gaseous pollutants that should be considered in the am- boilers in urban district. Gas-fired industrial boilers are mainly used for
bient air quality model. Thus, with the increase in the number and heating and living in Beijing central urban district due to the high po-
capacity of gas-fired industrial boilers, the emission of CO, NH3 and pulation density (Yan et al., 2017).
VOCs should be pay more attention.
However, seldom studies have been focused on the changes of the
2.3. Field measurements
emission characteristics after the implementation of revised emission
standard and relevant administration policies for the low-NOx retrofit
To investigate the actual EFs of gaseous pollutants (NOx, CO, NH3,
of gas-fired industrial boilers. In the present study, we focused on in-
VOCs) from gas-fired industrial boiler, 1107 boilers were tested and
vestigating the emission characteristics of NOx, CO, NH3 and VOCs
analyzed (Table 1). It included 862 unabated gas-fired industrial boilers
emitted before and after the implementation of low nitrogen reforming
and 245 gas-fired industrial boilers with low NOx combustion techni-
policy of gas-fired boilers. The key factor that affected the emission of
ques. Among these of 862 unabated gas-fired industrial boilers, there
gaseous pollutants were also discussed. Category-specific EFs of NOx,
were 281 AC boilers and 581 CC boilers. While CC boilers accounted for
CO, NH3 and VOCs were obtained based on field measurements for
the majority part of the 245 gas-fired industrial boilers. In the field
1107 low-NOx retrofitted and unabated gas-fired industrial boilers. The
measurements, operating load were controlled to above 75% to reflect
high spatial resolution of gaseous pollutant emission inventories
the real emission level of gaseous pollutants emitted from gas-fired
(3 km × 3 km) were established and analyzed based on detailed in-
industrial boilers (Yan et al., 2017).
formation from gas-fired industrial boilers, including boiler position,
To clarify the influence of operating load and control measures on
boiler type, operating load, combustion mode, installed capacity, etc.
gaseous pollutants emission (NOx, CO, SO2), the gaseous pollutants
Monte Carlo simulation was applied to calculate the uncertainty.

2. Data and methods

2.1. Study domain

Beijing, the capital city of China, is located in the Northern part of


the North China Plain (39°54′ N, 116°23′E) covered a total area of
16,410.54 km2 with 16 administrative districts. It is surrounded by the
Taihang and Yanshan Mountains to the west, north and northeast. As
the center of politics and culture of China, the population has already
exceeded 21.7 million in 2016 (BMBS, 2016). With the rapid economic
development, population expansion and urbanization, Beijing has ex-
perienced an ever-increasing energy consumption and the sharp in-
crease of emissions of massive pollutants to the environment. In order
to mitigate air pollution and improve air quality, Beijing municipal
government has adopted numerous measures to reduce atmospheric
pollutants emissions in recent years (He et al., 2014; Xue et al., 2016).
In 2016, Beijing municipal government encouraged natural gas-fired
industrial boilers to achieve low NOx combustion by equipping low
NOx burners (LNBs) or post-combustion abatement techniques.
Fig. 1. Geographical locations of gas-fired industrial boilers in Beijing.

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T. Yue et al. Atmospheric Environment 184 (2018) 1–8

Table 1 2.6. Uncertainty analysis


Summery of gas-fired industrial boilers in field measurements.
Category Combustion mode Numbers In order to know the uncertainties of the inventory, Monte Carlo
simulation analysis is conducted to quantify the uncertainties of NOx,
Without low NOx Atmospheric – 281 CO, NH3 and VOCs emissions from gas-fired industrial boilers. The
combustion combustion (AC)
probability distributions of input parameters for activity levels and EFs
techniques Chamber Direct-combustion 14
combustion (CC) machine (CCM)
were determined based on the author's judgments or previous related
Horizontal internal 213 references (Zhao et al., 2011; Xue et al., 2017; Yan et al., 2017), which
combustion (HIC) could be seen in supplementary section (Table S1).
Other modes 354
With low NOx combustion techniques 245
Total number of gas-fired industrial boilers on field measurements 1107 3. Result and discussion

3.1. Influence factors of gaseous pollutants emitted from gas-fired industrial


concentrations in the flue gas of a typical 1.4 MW gas-fired industrial boilers
boiler (WNS1.4–0.7/95/70-Q) equipped with a LNB and Flue Gas
Recirculation (FGR) were detected at different operating load (46%, Precious studies have reported that operating load and control
60%, 73%, 90%, 95%) and variable amount of FGR, respectively. measures were the priority factors to affect the emission of gaseous
The flue gas analyzer (Testo 350, TESTO, Germany) was used to pollutants by regulating the O2 content, combustion temperature and
analyze the O2 content, flue gas temperature, flue gas velocity, and the gas flow velocity during combustion process (Ma et al., 2016; Yan et al.,
concentration of NOx, SO2 and CO at the outlet of the gas-fired in- 2017). To clarify the role of above two factors during the main gaseous
dustrial boilers according to the corresponding standard methods pollutants emission, the pollutants outlet concentration, O2 content,
(MEPPRC, 2014; 2000; 2007). Portable Fourier infrared flue gas ana- flue gas velocity and chamber temperature were detected by one gas-
lyzer (DX4000, GASMET, Finland) was used to analyze the concentra- fired industrial boiler with the capacity of 1.4 MW. Flue Gas Re-
tion of NH3 according to the corresponding detection methods circulation (FGR) technology as one of the main NOx emission controls
(MEPPRC, 2007). In order to investigate VOCs, flue gas samples were used in industrial boiler was discussed in this article.
put in polyvinyl fluorite (PVF) bags by vacuum chamber (Laoying 2081,
LAOYING, China) then back to the laboratory. The VOCs was de-
termined following the gas chromatography-mass spectrometry (GC- 3.1.1. The whole process analysis of gas-fired industrial boilers
MS) method (MEPPRC, 2007). Atmospheric pressure was measured by The whole process of gas-fired industrial boiler covers the start to
an atmospheric pressure gauge (Testo 511, Testo, USA). For quality the stable operation process. Analyzing the whole process can help
assurance and control, the gas analyzers were calibrated with zero gas clarify the real emissions of gaseous pollutants. When the operating
and targeted standard gases (NO, NO2, CO, and O2) before the first test load is more than 90%, the chamber temperature is high, which facil-
of the day. The duration of each sampling was determined by relevant itates the formulation of thermal-NOx. The FGR system also works well
standards and specifications. under high operating load. Therefore, we set the whole process at op-
erating load of 95% with FGR and 90% without FGR, respectively, to
analyze the emission characteristics of NOx, CO and SO2, as shown in
2.4. Emission factors Figs. 2–5. As the chamber temperature is quite difficult to detect, in this
article we assumed that the variation trend of flue gas temperature is
The category-specific EFs of NOx, CO, NH3 and VOCs were calcu- similar to that of the chamber temperature.
lated according to field measurements based on the following formula: In terms of the gas-fired industrial boiler operated at 95% load with
FGR, the duration was about 140 s from the start to stable operation.
EFi, j = (Ci, j × Qi, j × 10−3)/(4 × Si, j ) (1) 0–100 s was the purge stage when fresh air was inlet. Within this stage,
the flue gas O2 content was relatively high and gaseous pollutants
Where the subscripts i, j represents the specific pollutant NOx, CO, NH3 emitted from gas-fired industrial boiler were not detected. As shown in
and VOCs and combustion mode, separately; EFi, j is the emission factor Figs. 2 and 3, 100–140 s was the start stage when gaseous pollutants
for pollutant i and combustion mode j, g/m3; C is the emission con- emission and flue gas characteristics varied quickly. Generally, the NOx
centration of pollutants in the flue gas, mg/m3; Q is the flue gas volume, emission from the combustion of gas-fired boilers is a group of nitrogen
m3/h; S is the feeding rate of natural gas, Nm3/h. monoxide (NO) and nitrogen dioxide (NO2). NO is the main component

2.5. Emission inventory

Typically, the gas-fired industrial boiler is treated as the stationary


source. Annual emissions of NOx, CO, NH3 and VOCs from gas-fired
industrial boilers in Beijing were calculated using the Emission factor
method. The method for the bottom-up emission inventory of NOx, CO,
NH3 and VOCs can be expressed using the following basic formula:

Ei = ∑ EFi,j × Aj × 10−6
j (2)

Where the subscripts i represents the specific pollutant, namely NOx,


CO, NH3 and VOCs; j represents the combustion mode; Ei is the emis-
sions of specific pollutant i, t; EFij is the emission factor of pollutant i
and combustion mode j calculated based on formula (1), g/m3; Aj is the Fig. 2. The variation of pollutants emission with run time at 95% operating
natural gas consumption, m3. load and FGR.

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T. Yue et al. Atmospheric Environment 184 (2018) 1–8

Fig. 4. The variation of O2 content, gas velocity and gas temperature with run
Fig. 3. The variation of O2 content, gas velocity and gas temperature with run
time at 95% operating load and without FGR.
time at 95% operating load and FGR.

accounting for more than 95% usually and is further oxidized to NO2 in
the atmosphere (Wei and Peng, 2016). The formation of NOx in gas-
fired boilers is complex and primarily due to the oxidation of nitrogen
in the air. Three main mechanisms are involved in, thermal mechanism
(Zeldovich mechanism), prompt mechanism (Fenimore mechanism)
and the N2O-intermediate mechanism (Miller and Bowman, 1989). The
NOx concentration firstly increased to 62.50 mg/m3 at 105 s in which
NO only accounted for a small proportion of NOx. It was mainly re-
sulted from the dominant generation of N2O-intermediates in the poor
fuel and low temperature combustion conditions. Simultaneously, the
NOx concentration further increased to 73.27 mg/m3 at 110 s, and then
dropped to 27.95 mg/m3 at 140 s with the prompt-NOx being pre-
dominant of NOx. During 105–125 s, the chamber temperature gradu-
ally increased and flue gas velocity decreased. The CO concentration
was ranged from 27.46 to 274.88 mg/m3, indicating the incomplete
combustion of natural gas. With the further increase of chamber tem-
perature and the flue gas amount of FGR, the CO concentration de- Fig. 5. The variation of pollutants emission with run time at 90% operating
creased to 5.59 mg/m3 and the flue gas velocity rose to 11.8 m/s at load and without FGR.
140 s.
The boiler reached stable combustion stage after 140 s when the flue
gas O2 content and velocity stabilized at about 4.89% and 13.1 m/s,
respectively. Meanwhile, the NOx concentration maintained at about
27.9 mg/m3 with the NO/NO2 volume ratio of 6, and the thermal-NOx
became the dominant component. The concentration of SO2 kept at a
relatively low level at < 2 mg/m3 and < 6 mg/m3 during the whole
operating process, respectively.
Furthermore, the gas-fired industrial boiler operated at 90% load
without FGR was investigated to do contrastive analysis, as presented in
Figs. 4 and 5. The results showed that the variation trend of gaseous
pollutants (NOx, CO, SO2) emission, the flue gas O2 content and velo-
city, and chamber temperature of the boiler operated at 90% load
without FGR were in line with that of the boiler operated at 95% load
with FGR. The duration was about 150 s from the start to stable op-
eration in terms of the gas-fired industrial boiler operated at 90% load
without FGR. The flue gas O2 content and velocity maintained at about
6.93% and 11.2 m/s after 150 s, respectively. While, the NOx con-
centration of the gas-fired industrial boiler without FGR was approxi- Fig. 6. Effect of operating load on pollutants emission without FGR.
mately 2.1 times of the gas-fired industrial boiler with FGR. The FGR
technology would be discussed later in this article.
were investigated with a capacity of 1.4 MW gas-fired industrial boiler
at 95%、90%、73%、60% and 46% operating load. The FGR was shut
3.1.2. Influence of operating load on the gaseous pollutants emission from up during the operation of the gas-fired industrial boiler. As shown in
gas-fired industrial boilers Fig. 6, the concentration of NOx and SO2 could meet the emission
Studies have investigated that operating load is quite significant to standard of gaseous pollutants for boilers in Beijing City (BMEPB,
the formation of NOx, SO2 and CO during combustion process (Ma 2015), and the CO concentration was maintained at a low level
et al., 2016). To clarify the influence of operating load, the gaseous (< 1 mg/m3) for the investigated operating load. The variation of flue
pollutants concentration, flue gas velocity and chamber temperature

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T. Yue et al. Atmospheric Environment 184 (2018) 1–8

in the original flue gas was further consumed through recirculation.


In conclusion, operating load and control measures are the two
important factors to affect the formulation of gaseous pollutants of gas-
fired industrial boilers. With the increasing of operating load, the
chamber temperature increased, which promoted the formulation of
thermal-NOx. Nevertheless, when the operating load was close to
100%, the formation of NOx was mainly manipulated by velocity of fuel
gas. The FGR technology can decrease the chamber temperature and O2
concentration in the combustion zone, and then inhibit the formation of
thermal-NOx.

3.2. Category-specific emission factors of NOx, CO, NH3 and VOCs based
on field measurements

The EFs of NOx and CO, obtained from the filed measurements of
1107 gas-fired industrial boilers, were presented in Fig.S2 and sum-
Fig. 7. Effect of operating load on O2 content, gas velocity and gas temperature marized in Table 2. As can be seen, all the EFNOx of gas-fired industrial
without FGR. boilers were fitting to normal distribution curve. For the gas-fired in-
dustrial boilers without low-NOx combustion techniques, EFNOx and
gas velocity and temperature were presented in Fig. 7. Flue gas velocity EFCO of ACBs were 3.08 and 0.54 g/m3, which were about 2.2 and 1.2
increased as the operating load increased, and there was a relatively times higher than the EFs of CCBs, respectively. It indicated that
sharp increase at 95% operating load. The flue gas temperature in- combustion mode was the significant factor affecting the formation of
creased in the whole process following the increase of operating load. gaseous pollutants. While, for CCBs, the EFNOx with CCMs, HICs and
Typically, the thermal-NOx is the dominant component of the NOx OMs were 1.41, 1.43 and 1.34 g/m3, respectively. The EFCO with CCMs,
emitted from the gas-fired industrial boiler, therefore, the chamber HICs and OMs were both 0.44 g/m3. It revealed that the boiler type was
temperature is the critical factor for the thermal-NOx formation during not the crucial factor affecting the EFNOx and EFCO. In addition, EFNOx
the natural gas combustion (Korpela et al., 2015; Yan et al., 2017). As and EFCO of gas-fired industrial boilers with low-NOx combustion
we assumed previously, the change of the flue gas temperature was techniques have also be given in our study. For retrofitted boilers with
consistent with that of the chamber temperature. The NOx concentra- NOx emissions of 80 mg/m3, the EFNOx and EFCO were 0.59 and 0.15 g/
tion increased from 55.3 to 61.8 mg/m3 when the operating load m3. For new or retrofitted boilers with NOx emissions of 30 mg/m3, the
changed from 46% to 73%, which could be attributed to the increase of EFNOx and EFCO were 0.25 and 0.11 g/m3. By comparison with gas-fired
thermal-NOx at higher chamber temperature. Nevertheless, NOx con- industrial boilers without low-NOx combustion techniques, the EFNOx
centration decreased to 59.1 mg/m3 at 90% operating load, which was and EFCO with low-NOx combustion techniques were lowest. It sug-
related to the decrease of chamber temperature. When the gas-fired gested that application of advanced pollution control technologies and
industrial boiler operated at 95% load, the flue gas velocity increased to strict emission standards can significantly reduce the pollutants emis-
12.9 m/s rapidly, which could be the reason of the slight decrease of sion.
NOx concentration even although the chamber temperature increased So far, there are few studies about NH3 and VOCs emissions from
as well. The relatively high flue gas velocity reflected that the gas flow gas-fired industrial boilers. In this study, the EFs of NH3 and VOCs were
retention time in the chamber was too short to form more thermal-NOx. also given by the field measurements of 20 gas-fired industrial boilers.
Due to limited testing data, only the average of EFNH3 and EFVOCs from
the retrofitted CCBs with low-NOx combustion techniques were given
3.1.3. Influence of Flue Gas Recirculation on the gaseous pollutants emitted in Table 2. The average EFs of NH3 and VOCs were 0.032 and 0.038 g/
from gas-fired industrial boilers m3, respectively.
Flue Gas Recirculation (FGR) technology is an important low NOx Moreover, as depicted in Table S1, multiple EFs of gas-fired in-
combustion technology, which is widely used in NOx emission control dustrial boilers from various locations were carried out during the past
of gas-fired industrial boilers. The FGR technology reduces NOx emis- few years. Because the ACBs were absent or phased out gradually, in
sion in the flue gas by returning a part of the flue gas into the com- our present study, the EFs of CCBs were selected and compared with
bustion zone. As the temperature and O2 content of the returning flue other research. EFNOx and EFCO in present study were lower than the
gas is relatively low, the FGR technology can decrease the chamber emission levels of AP-42 (EPA, 2018), Pulles and Heslinga (2004) and
temperature and O2 concentration in the combustion zone, and then Xue et al. (2017). Whereas in the present study, the EFNOx and EFCO
inhibit the formation of thermal-NOx. The flue gas amount of FGR was were almost on the same level in comparison to those observed in Yan
expressed by Flue Gas Recirculation Rate (FGRR), which was namely et al. (2017) research. In the study of Yan et al. (2017), EFs of gas-fired
the ratio of the amount of flue gas used for recirculation to the total industrial boilers with two combustion modes and three boiler types
amount of flue gas without recirculation. were displayed based on field test. However, low-NOx retrofitted policy
To study the effect of FGR, the relationship between gaseous pol- was not considered in Yan's study. Presently, Beijing has adopted to
lutants outlet concentration and FGRR was investigated with a capacity numerous environmental policies to control and improve air quality.
of 1.4 MW boiler at operating load of 95%, 90%, 73%. As shown in The adjustment of energy structure and the application of advanced
Fig. 8, when boiler operated at relatively low load (< 70% operating pollution control technology will affect the emission of pollutants.
load), combustion became unstable as the FGRR varied, so the oper- Thus, in order to obtain more accurate emission characteristics of gas-
ating load < 70% was not considered in this article. The results showed fired industrial boilers, a set of systematic and integrated EFs for var-
that the NOx concentration decreased when the FGRR increased for all ious pollutants compiled for numerous low-NOx retrofitted gas-fired
investigated operating load, whereas the SO2 and CO concentration was industrial boilers for Beijing is very essential.
not varied considerably and maintained at a relatively low level. In
addition, there was no obvious variation of the flue gas temperature 3.3. Chemical species of VOCs from gas-fired industrial boilers
and velocity as the FGRR increased. The O2 content of the flue gas
decreased with the increased of the FGRR, which indicated that oxygen During our sampling periods, the concentrations of VOCs were

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T. Yue et al. Atmospheric Environment 184 (2018) 1–8

Fig. 8. The relationship between concentration of gaseous pollutants and FGRR.

Table 2
Emission factors of NOx from gas-fired industrial boilers in Beijing.
Category Combustion mode EF (g/m3)

NOx CO NH3 VOCs

Without low NOx combustion technique Atmospheric combustion boilers (ACBs) 3.08 0.54 0.032 0.038
Chamber combustion boilers (CCBs) Direct-combustion machine (CCM) 1.41 0.44
Horizontal internal combustion (HIC) 1.43 0.44
Other modes (OM) 1.34 0.44
With low NOx combustion boilers (LNBs), with the goal of CNOx < 30 mg/m3 0.25 0.11
With low NOx combustion boilers (LNBs), with the goal of CNOx < 80 mg/m3 0.59 0.15

Table 3 3.4. Emission inventory of NOx, CO, NH3 and VOCs from gas-fired
Regional emissions of NOx, CO, NH3 and VOCs from gas-fired industrial boilers industrial boilers in 2015
in Beijing in 2015.
Districts NOX (t) CO (t) NH3 (t) VOC (t) According to the category-specific EFs of pollutants in this study and
the consumption of natural gas, the emissions of NOx, CO, NH3 and
Chaoyang 2503.7 775.8 46.5 55.8 VOCs from gas-fired industrial boilers from Beijing in the year of 2015
Dongcheng 641.0 194.2 11.6 13.9
were estimated. The total emissions were estimated at 10489.6 t of
Fengtai 910.1 288.0 17.3 20.7
Haidian 2624.0 811.8 48.7 58.3 NOx, 3272.8 t of CO, 196.4 t of NH3 and 235.4 t of VOCs, respectively.
Shijingshan 117.5 36.9 2.2 2.7 Additionally, the NOx emissions of gas-fired industrial boilers ac-
Xicheng 498.6 152.7 9.1 10.9 counted for 7.6% of total emissions from Beijing in 2015, which was
Changping 554.7 174.3 10.5 12.5 obtained from the Beijing Environmental Statement 2015 (BMEPB,
Daxing 1029.9 329.2 19.8 23.7
Fangshan 409.1 129.7 7.8 9.4
2015). In comparison, the emissions of NOx from gas-fired boilers in
Huairou 116.4 36.9 2.2 2.7 Beijing in the year 2014 were 1.1 times higher than in our research
Mentougou 6.7 2.1 0.1 0.2 (Yan et al., 2017). Due to the application of strict emission standards
Miyun 119.3 39.0 2.4 2.8 and reward policy of low nitrogen (low-NOx) retrofit of existing gas
Pinggu 50.4 16.1 1.0 1.2
(oil) boilers, some advanced pollution control technologies were used,
Shunyi 239.4 74.1 4.5 5.3
Tongzhou 658.7 208.6 12.5 15.0 which could significantly reduce the pollutants emission.
Yanqing 10.0 3.2 0.2 0.2 Furthermore, the spatial distributions of emissions from gas-fired
Total 10489.6 3272.8 196.4 235.4 industrial boilers were closely related to the levels of economic devel-
opment and industrial production, the supplies of energy, the demands
of winter concentrated heating, and populations in the sixteen districts
ranged from 1.48 to 2.18 mg/m3. The detected chemical species of of Beijing. Table 3 illustrated the spatial emissions of NOx, CO, NH3 and
VOCs included alkanes, BTEX (benzene, toluene, and xylene), oxyge- VOCs from gas-fired industrial boilers. The emission inventory was
nated VOCs (methanol, acetaldehyde and other higher aldehydes) and spatially allocated into 3 km × 3 km grid cells, as showed in Fig. 9. As
non-reactive organic matter. The total concentrations of these four can be seen, the emissions of NOx, CO, NH3 and VOCs from gas-fired
patterns of VOCs accounted for 72%, 6%, 4%, and 18%, respectively. industrial boilers in Beijing were predominantly concentrated in central
Alkanes was the major species in VOCs. As for BTEX, it was the typical six urban districts, which accounting for 68.9–69.5% of the total
anthropogenic emitted organics in the atmosphere, which not only emissions. It was due to the large number of gas-fired industrial boilers
endanger human health but also actively participate in photochemical and the dense population in central urban districts. Haidian rank as the
reactions, generating O3 and secondary organic aerosols. As illustrated first district with NOx, CO, NH3 and VOCs emissions, with the average
in Fig.S1, BTEX and Oxygenated VOCs accounted for 14% and 19% of largest proportion of 24.9% for the total emission. Chaoyang and
VOCs from EPA SMOKE Model, which were substantially higher than Fengtai districts are next after that. Correspondingly, due to the geo-
the data from our research. However, in our study, Non-reactive or- graphic conditions of rural areas that seriously hindered the installation
ganic matter has a high proportion of 18%, reflecting a higher level of natural gas pipelines, the consumption of natural gas and the emis-
than the EPA SMOKE Model data. sions of NOx, CO, NH3 and VOCs were lower than in rural areas than
that in central six urban districts of Beijing.

6
T. Yue et al. Atmospheric Environment 184 (2018) 1–8

Fig. 9. Spatial distribution characteristics of NOx, CO, NH3 and VOCs from gas-fired industrial boilers in Beijing.

Several factors influence the estimation of the emissions of pollu- 10489.6 t, 3272.8 t, 196.4 t and 235.4 t, respectively. The NOx emis-
tants, including activity levels and emission factors. To better under- sions of gas-fired industrial boilers accounted for 7.6% of total emis-
stand the uncertainties of our inventory, Monte Carlo simulation was sions from Beijing in the year of 2015. Alkanes, BTEX (benzene, to-
used to quantify the uncertainties of pollutants emissions from gas-fired luene, and xylene), oxygenated VOCs (methanol, acetaldehyde and
industrial boilers. Table S2 illustrated the uncertainties (95% con- other higher aldehydes) and non-reactive organic matter were the four
fidence interval around the arithmetic mean value) in Beijing atmo- main chemical components of VOCs. As for the spatial distributions, the
spheric emissions of NOx, CO, NH3 and VOCs from gas-fired industrial emissions of NOx, CO, NH3 and VOCs from gas-fired industrial boilers
boilers in 2015. As Table S2 shown, NH3 and VOCs were demonstrated in Beijing were predominantly concentrated in central six urban dis-
to have the highest uncertainties of (−26.3–47.8%) and tricts, which accounting for 68.9–69.5% of the total emissions. Haidian
(−54.1–54.5%), respectively. These high uncertainties mainly resulted rank as the first district with NOx, CO, NH3 and VOCs emissions.
from inadequate field tests data for Beijing gas-fired industrial boilers Due to inadequate field tests data, the inventory of NH3 and VOCs
combustion processes. In comparison, NOx and CO show relatively low from gas-fired industrial boilers have relatively higher uncertainties of
uncertainties, because these pollutants were the dominant pollutants (−26.3–47.8%) and (−54.1–54.5%), respectively. In the future, in
emitted from the combustion processes of gas-fired industrial boilers order to achieve more reliable estimations of atmospheric pollutants
and there were many field tests to measure the actual emission level of from gas-fired industrial boilers in China, especially for toxic VOCs,
these pollutants. Thus, more detailed investigation and field tests for all more detailed investigation and field tests for all kinds of gas-fired in-
kinds of gas-fired industrial boilers are still very necessary for a better dustrial boilers are still greatly needed.
understanding of the emissions of these atmospheric pollutants in the
future, especially for toxic VOCs.
Acknowledge
4. Conclusion
This work was supported by the National Key Research and
In this paper, based on abundant and systematic field measure- Development Program of China (2016YFC0208103), the National
ments, we have established a comprehensive emission inventory of Natural Science Foundation of China (21607008), the Youth Core Plan
NOx, CO, NH3 and VOCs from gas-fired industrial boilers in Beijing in (YC201808, YC201810), the Building of Innovation Team Plan
the year of 2015. Two influence factors, operating load and control (IG201804N), and the Green Shoots Plan (2017–02). We also thank the
measures, were discussed to clarify the effects on gaseous pollutants editors and the anonymous reviewers for their valuable comments and
emissions (NOx, CO, SO2). The total emissions of NOx, CO, NH3 and suggestions on our paper.
VOCs from gas-fired industrial boilers in Beijing were estimated at

7
T. Yue et al. Atmospheric Environment 184 (2018) 1–8

Appendix A. Supplementary data HJ 693–2014, Stationary Source Emission-Determination of Nitrogen Oxides-Fixed


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doi.org/10.1016/j.atmosenv.2018.04.022. HJ/T 57–2000, Determination of Sulphur Dioxide from Exhausted Gas of Stationary
Source Fixed-potential Electrolysis Method [S]. Standards Press of China, Beijing.
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