Combustion and Flame 217 (2020) 314–320

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Combustion and Flame

journal homepage: www.elsevier.com/locate/combustflame

The temperature dependence of the laminar burning velocity and

superadiabatic flame temperature phenomenon for NH3 /air flames
Xinlu Han a, Zhihua Wang a,∗, Yong He a, Yingzu Liu a, Yanqun Zhu a, Alexander A. Konnov b
a
State Key Laboratory of Clean Energy Utilization, Zhejiang University, Hangzhou 310027, PR China
b
Division of Combustion Physics, Lund University, Lund S-22100, Sweden

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

Article history: Combustion of ammonia (NH3 ) as a carbon-free alternative fuel has been recently widely studied, with
Received 10 March 2020 vast majority of the burning velocity data obtained at room temperature. In the present study, the lami-
Revised 16 April 2020
nar burning velocity SL of NH3 /air mixtures has been measured at unburnt gas temperature Tu from 298 K
Accepted 17 April 2020
to 448 K, covering equivalence ratios from 0.85 to 1.25 and at 1 atm using the heat flux method. Kinetic
Available online 7 May 2020
simulations were made with five literature mechanisms developed for NH3 combustion, i.e., Nakamura et
Keywords: al., Otomo et al., San Diego, Okafor et al., and Mei et al. mechanisms, and the influence of radiation heat
Laminar burning velocity losses was considered. Using the obtained burning velocity data at different temperatures, the temper-
Elevated temperature ature dependence coefficients α in SS0L = ( TTu0 )α were derived, and compared with different models’ pre-
L u
Temperature dependence
dictions. Further analyses of the temperature dependence of SL were carried out through examination of
Ammonia flame
the overall activation energy, temperature and species profiles as well as the reaction paths, and a unique
flame structure at the rich side of adiabatic NH3 /air flames was found, which resembles ‘over-rich’ phe-
nomena in hydrocarbon flames. At equivalence ratio larger than 1.1 ± 0.05, the NH3 /air flames become
so rich that (1) the NH2 radical overwhelms the H and OH radicals in maximum mole fraction; (2) after
the flame front, H2 O converts back to H2 with NO formed at the same time, causing the superadiabatic
flame temperature phenomena, i.e. adiabatic flame temperature being lower than the maximum achieved
in the flame. Moreover, local minimum NO concentration is found right after the over-rich NH3 /air flame
front, which may be helpful in reducing NO emissions from NH3 flames in practical applications.
© 2020 The Combustion Institute. Published by Elsevier Inc. All rights reserved.

1. Introduction
Ammonia (NH3 ) has recently gained more and more attention
by the combustion community as a promising alternative fuel.
Comparing with traditional fossil fuels, NH3 releases no carbon
dioxide (CO2 ) when burning, which is advantageous facing the
threat of global warming. Also, due to its matured usage in, e.g.,
fertilizer industry, the fuel NH3 can be incorporated into modern
life with less investment on its production and transportation.
As an important global combustion characteristic, laminar burn-
ing velocity (SL ) of NH3 has been investigated in several experi-
mental studies. For the measurements fuelled with pure NH3 , most
experiments were concentrated on NH3 /air combustion at room
temperature and pressure, e.g., Takizawa et al. [1], Ronney [2],
Pfahl et al. [3], Jabbour and Clodic [4], and Han et al. [5]. The
NH3 /air burning velocities at pressures up to 5 atm have been
measured by Hayakawa et al. [6] and Ichikawa et al. [7], and for
∗
Corresponding author.
E-mail address: wangzh@zju.edu.cn (Z. Wang).
the same pressure range Mei et al. [8] provided several oxy-fuel
NH3 burning velocity data. There are also NH3 /O2 flame results re-
ported by Liu et al. [9] where the effect of pressure from 0.5 to
1.6 atm was investigated. However, it is noted that these literature
data for NH3 /air flames are all at room temperature, and the data
obtained at elevated temperatures are only found in the early work
of Cohen [10] from 323 to 423 K employing a flat flame burner,
and in the recent work of Lhuillier et al. [11] from 298 to 473 K
using spherical flame method.
Besides, temperature dependence of NH3 burning velocity in
the form of Eq. (1) [12,13],
 α
SL Tu
= (1)
SL0 Tu0
and the corresponding α coefficient are also seldom investigated
in literature. The α coefficient is important because with SL0 at a
reference temperature Tu0 (e.g., 298 K) known, specified α value is
helpful for deriving SL at various Tu ,which is also powerful indica-
tor of the SL data consistency [14,15]. For NH3 /air flames, the only
experimentally derived α values from Cohen [10] and Lhuillier et

https://doi.org/10.1016/j.combustflame.2020.04.013
0010-2180/© 2020 The Combustion Institute. Published by Elsevier Inc. All rights reserved.
 X. Han, Z. Wang and Y. He et al. / Combustion and Flame 217 (2020) 314–320 315

al. [11] are in conflict. Cohen [10] reported the α coefficient to be

approximately equal to unity, while that derived by Lhuillier et al.
[11] is around 2 at stoichiometry. A fitted α correlation equation
from numerical simulations can be found in the work by Gold-
mann and Dinkelacker [16] using kinetic mechanism from Mathieu
and Petersen [17]. Considering the uncertainty in experiments and
kinetic modelling, the limited works are insufficient for accurate α
evaluation of NH3 /air flames.
In light of the background outlined above, the aims of this
investigation are: (1) to measure the laminar burning velocity of
NH3 /air flames at different unburnt temperatures; (2) to validate
kinetic mechanisms using the experimental SL ; (3) to evaluate the
temperature coefficient α and analyse the flame structure changes
at different equivalence ratios from experimental and numerical
data.

2. Experimental details

The experiment setup used herein is similar to that in our re-

cent work on NH3 flames [5]. Atmospheric adiabatic burning veloc-
ities of NH3 /air flames were measured by the heat flux method at
unburnt temperatures 298–448 K with 25 K step. For each unburnt
temperature, the measured equivalence ratios φ were changed
from 0.85 to 1.25 with 0.05 increment. Influence of the buoyancy
instability and NH3 adsorption on metal surfaces of the burner was
considered negligible for the measurement results [5]. The mea-
sured burning velocities at 298 K (Tu0 ) were used as the reference
SL0 when deriving Eq. (2).
 
ln SL /SL0
αTu →Tu0 =   (2)
ln Tu /Tu 0

The uncertainty of the measured SL , SL , was evaluated from

the thermocouple readout scatterings of the burner temperature as
well as from the uncertainties arising from Mass Flow Controllers.
The uncertainty of the α coefficient derived from experimental SL
was evaluated through the uncertainty propagation as
 
1 S L SL0
αTu0 →Tu =   + (3)
ln Tu /Tu0 SL SL0

More details about the experimental uncertainty can be found

in our previous publications [5,18,19].

3. Numerical details

Flame simulations in this work were carried out using ANSYS
CHEMKIN 17.0 [20], Premixed Flame Speed module, and calcula-
tions of the equilibrium state were achieved through the Equi-
librium module. The literature kinetic mechanisms used here are
Nakamura et al. [21], Otomo et al. [22], San Diego [23], Okafor et
al. [24], and Mei et al. [8], all targeting at the oxidation of NH3 as
main fuel component. Soret effect and multicomponent transport
were considered in all simulation cases.
Nakamura et al. [25] reported that considering radiation heat
loss strongly influences the simulated burning velocity results of
NH3 /air flames, which mimics more the situation of real exper-
imental flames with inevitable flame radiation. Therefore, in the
present study, simulations with radiative heat loss were made to
compare with the experimental SL and the derived α coefficients.
Calculations of the radiative losses were achieved by adding the
absorption coefficients of NH3 , NO, N2 O, and H2 O species [25] into
the thermodynamic input file of different mechanisms and then
enabling the ‘Include Gas Radiation’ option in CHEMKIN. Separate
simulations without radiative heat loss were also made in order to
analyse the adiabatic flame structure of NH3 /air flames.
Fig. 1. Laminar burning velocity of NH3 /air flames at 1 atm, (a) present experimen-
tal results at different Tu ; (b) 298 K data comparing with literature experimental
and simulation results considering radiative heat loss; (c) 448 K data comparing
with simulation results considering radiative heat loss.
4. Results and discussion
4.1. Burning velocity and its temperature dependence
Figure 1 shows the present measurements of the laminar burn-
ing velocity at different Tu . At 298 K, the present experimental re-
sults agree well with the literature data from Han et al. [5], Tak-
izawa et al. [1], Ronney [2], Pfahl et al. [3], Jabbour and Clodic [4],
Hayakawa et al. [6], Ichikawa et al. [7], Mei et al. [8], and Lhuillier
et al. [11]. Error bars show the experimental uncertainty, which is
around 10% for majority of the experimental data. This uncertainty
range is not as fine as that for hydrocarbon flames using the same
heat flux method, which is mostly attributed to the low measure-
ment sensitivity [18] of NH3 flames resulting in the increased un-
316 X. Han, Z. Wang and Y. He et al. / Combustion and Flame 217 (2020) 314–320
ln (SL /SL0 )
Fig. 2. α = ln (Tu /Tu0 )
derived from Tu0 = 298 K and Tu = 448 K for NH3 /air flames.
certainty caused by thermocouple readout scattering. The compar-
ison of the present experimental data at 423 K with the literature
data from Cohen [10] and Lhuillier et al. [11] can be found in the
Supplementary material.
Figure 1 also includes simulation results considering radiative
heat losses. For each mechanism, same tendency is found at 298 K
and 448 K, while due to the exponential increase of SL at ele-
vated Tu (see Eq. (1)), larger absolute discrepancies among different
mechanisms are found at 448 K. Simulations using Nakamura et
al. mechanism [21] are always higher than the present experimen-
tal data, regardless of equivalence ratio φ . Mechanisms from San
Diego [23] and Mei et al. [8] under-estimate by around 20% the
fuel-lean and over-estimate over 40% the fuel-rich side SL results
of the present experiments. Overall, Otomo et al. [22] and Okafor
et al. [24] mechanisms have the best prediction performance, of
which the relative difference compared with the present experi-
mental data is within ± 10%.
Figure 2 shows the temperature coefficient α derived from the
present experimental SL data and from the simulated SL with ra-
diative heat loss. Also shown are the experimentally derived val-
ues from Lhuillier et al. [11] and correlation reported by Gold-
mann and Dinkelacker [16]. For the experimental data, minimum
α 298 K → 448 K = 1.86 is found at φ = 1.1 with also lowest un-
certainty of αT 0 →Tu = 0.54. The simulation results by San Diego
u
[23] and Mei et al. [8] mechanisms have best agreement with
the experimental data, in contrast with their inferior performance
on predicting SL compared to Otomo et al. [22] and Okafor et al.
[24] mechanisms in Fig. 1. The present α values agree well with
that from Lhuillier et al. [11] at φ = 1.0 and 1.2, while the φ = 0.8
point was not measured in the present experiments. As has been
mentioned in Introduction, the α value of Cohen [10] is equal to
unity, which is significantly lower than the present and Lhuillier
et al. [11] data, thus not shown in the figure. The α derived from
Goldmann and Dinkelacker [16] correlation exceeds by 10% that
derived from the present experiment and simulations at around
φ = 1.1, which can be attributed to uncertainties of the selected
mechanism [17] and of the correlation fitting processes. Effect of
radiative heat loss consideration on the simulated α is shown in
the Supplementary material to be notable at especially the off-
stoichiometry sides, indicating the need to consider it in validating
not only burning velocity of ammonia, but also temperature coef-
ficients α . Since α is a powerful indicator of the SL data consis-
tency [14,15], the agreement of the present experimentally derived
Fig. 3. Ea
and x fitted using adiabatic simulation results.
2R
α with other datasets show clearly that the present SL results are
consistent at different Tu .
4.2. Adiabatic flame structure analyses
In the following, analyses were carried out using adiabatic sim-
ulation results, thus focusing on the flame structure changes aris-
ing from chemistry. Considering the oxidation process using a one-
step global reaction, the overall activation energy Ea and reaction
order n should be different when there are different flame struc-
tures, which then can be identified. Ea and a synthetic parameter
related to reaction order, x, can be derived from the α coefficient
through Eq. (4) [18],
Ea
αTu0 →Tu = ·X +x (4)
2R
where X is related to the adiabatic flame temperature. Analyses
of Ea using this equation have helped identify the flame struc-
ture change between the moderate-rich and over-rich regions of
methane, ethane, and propane+air flames in our previous publi-
cations [18,19], where details of the derivation procedure can be
found.
Figure 3 shows the relationship of 2ERa and x vs. φ . The selected
four mechanisms reproduce well either the experimental SL or α
in Figs. 1 and 2. In Fig. 3, rich-side turning points at φ = 1.15 are
found from the simulation results using Otomo et al. [22], Okafor
et al. [24], and Mei et al. [8] mechanisms, where the overall activa-
tion energy Ea and x reaching valley and peak values, respectively.
Results by San Diego mechanism [23] show similar tendency, while
the turning point being leaner at φ = 1.1. The presence of the turn-
ing points in Ea and x profiles indicates that there may be flame
structure change in the fuel-rich side of NH3 /air flames.
Figure 4 shows adiabatic flame simulation results at 298 K of
the spatial profiles of temperature, net heat release rate, and mole
fractions of H2 O, H2 , OH, H, N2 , NO at φ = 1.1 and φ = 1.15.
The net heat release rate was adopted directly from the ANSYS
CHEMKIN output. Results by Otomo et al. [22], Okafor et al. [24],
and Mei et al. [8] mechanisms were chosen because they have
turning points at the same equivalence ratio in Fig. 3. In Fig. 4, they
show the same tendencies in the spatial profiles investigated. Con-
 X. Han, Z. Wang and Y. He et al. / Combustion and Flame 217 (2020) 314–320 317

Fig. 4. Spatial profiles of temperature and net heat release rate (a) and (b), and mole fractions of H2 O and H2 (c) and (d); OH and H (e) and (f); N2 and NO (g) and (h) at
298 K. Panels in the left and right columns represent φ = 1.1 and φ = 1.15 flames, respectively. Position of the maximum net heat release rate set at distance = 1 cm.
318 X. Han, Z. Wang and Y. He et al. / Combustion and Flame 217 (2020) 314–320

Fig. 5. Reaction pathways in NH3 /air flames calculated using Okafor et al. mecha- Fig. 6. Rate of production of OH at the distance = 3.0 cm in NH3 /air flames calcu-
nism at 298 K. Left: φ = 1.1; right: φ = 1.15. lated using Okafor et al. mechanism at 298 K.

trary to φ = 1.1 flame, simulation results at φ = 1.15 show supera-

diabatic flame temperature (SAFT), i.e., the maximum flame tem-
perature exceeding the equilibrium (adiabatic) one, which is in line
with the negative net heat release rate after the flame front staying
for a much longer distance at φ = 1.15 than at φ = 1.1. It is also
noticed that after the flame front, the [H2 O] and [H2 ] for φ = 1.15
flame gradually decreases and increases, respectively, while this
tendency can’t be found in φ = 1.1 flame. Based on the above com-
parison, the H2 O is apparently converting to H2 in φ = 1.15 NH3
flame tail (the region downstream the large temperature gradient
flame front), which was also found for the methane, ethane, and
propane+air flames in their over-rich regions [19]. For the [OH]
and [H] profiles in Fig. 4(e) and (f), decreases of their concentra-
tions right after the flame front are found at both equivalence ra-
tios, however after this decrease, [OH] and [H] take a much longer
distance to reach the equilibrium states for the φ = 1.15 flame than Fig. 7. Maximum mole fractions of dominant intermediate species in NH3 /air
for φ = 1.1 flame. Difference can hardly be found in the [N2 ] pro- flames, simulated at 298 K using Okafor et al. mechanism.
files, while in the same panels (g, h), the [NO] continually goes
down at φ = 1.1, and shows non-monotonic behaviour at φ = 1.15.
The differences discussed above confirm essential changes in the consumed partly by R2 and R3 at φ = 1.15, and the increase of [H]
flame structure around the turning points seen in Fig. 3. in Fig. 4 can be attributed to the production of H through these
Figure 5 shows the reaction pathways in φ = 1.1 and φ = 1.15 two reactions together with that through R5. R4 also consumes
NH3 /air flames. Data in this figure were taken from the 298 K H2 O, together with the H2 O consumption through R1, responsible
simulation results using Okafor et al. [24] mechanism, at a dis- for the decrease of [H2 O] in Fig. 4. At the same time, NO is pro-
tance = 3 cm (2 cm downstream the position of the maximum duced by R2; and from the analyses of HNO ROP (not shown here),
net heat release rate). Obvious difference can be found in Fig. 5 for the HNO formed by R3 is quickly consumed by R5 to form NO, ex-
the direction of arrows connecting H2 and H2 O species, validating plaining the increase of [NO] in Fig. 4.
the assumption discussed above that there is H2 O–H2 conversion
in φ = 1.15 NH3 +air flame tail. For φ = 1.1 and φ = 1.15 reac- OH + H2 = H + H2 O (R1)
tion pathways, direction differences are also noted for the arrows
attaching to OH. N + OH = NO + H (R2)
Figure 6 shows the rate of production (ROP) of OH, which fol-
lows the finding of the pathways arrow direction changes in Fig. 5. NH + OH = HNO + H (R3)
The mechanism and distance chosen in Fig. 6 are the same as
those in Fig. 5. Though the total OH ROP is nearly the same for H + OH + M = H2O +M (R4)
φ = 1.1 and φ = 1.15 flames, the absolute ROP contribution of
several reactions is found dramatically larger for φ = 1.15 than H + NO + M = HNO + M (R5)
for φ = 1.1 flames, therefore the ROP at φ = 1.1 has been mul-
tiplied by 10 in Fig. 6 to facilitate comparison. There are 3 re- In contrast to the φ = 1.15 case discussed above, at φ = 1.1,
actions, R1-R3, showing opposite sign of ROP at different equiva- directions of R1-R3 and R5 are all different and the absolute ROP
lence ratios. At φ = 1.15, R1 has the largest positive OH ROP, and of R1-R3 is indeed small, resulting in that (1) [H2 O], [H2 ], [OH], [H]
the increase of [H2 ] in Fig. 4 at the distance = 3.0 cm can be ex- staying unchanged with the net heat release rate approaching zero
plained since R1 produces OH and H2 at the same time. The SAFT and no SAFT found; (2) [NO] decreases at the distance = 3.0 cm.
and negative net heat release rate can also be understood since the Figure 7 shows the maximum mole fractions of dominant in-
H2 O–H2 conversion through R1 is endothermic. The OH formed is termediate species in NH3 /air flames, in order to inspect the flame
 X. Han, Z. Wang and Y. He et al. / Combustion and Flame 217 (2020) 314–320
Fig. 8. Differences of the local maximum flame temperature and corresponding
equilibrium flame temperature for NH3 /air flames at 298 K.
structure change and identify important radicals at different φ . At
the rich side of flame compositions, with φ increasing, the max-
imum concentrations of all radicals go down except NH2 , whose
maximum concentration increases gradually and overwhelms that
of OH, H, and NO at φ > 1.15. From the integrated ROP analyses
by Okafor et al. [24] and in our previous study [5], typical fuel-
rich species N2 H2 , N2 H3 , N2 H4 , and H2 NN are generated mostly by
NH2 , and thus the relative abundance of NH2 compared to other
species points out that the flame is ‘very rich’. Based on this char-
acteristic, the names ‘moderate-rich’ and ‘over-rich’ can be given
to the regions before and after the aforementioned flame structure
turning point, respectively.
Analyses presented from Figs. 3–7 have been repeated using
different mechanisms as well as at different unburnt temperatures,
similar results were found with the turning equivalence ratios to
over-rich flames. They are slightly different using different mech-
anisms, nevertheless all indicating that the shown over-rich flame
characteristics are common features and not a peculiarity arising
from a certain mechanism.
Figure 8 shows differences between the local maximum flame
temperature (or maximum temperature at the end point of the
computational domain if there is no SAFT behavior) and corre-
sponding equilibrium flame temperature for NH3 /air flames at
298 K, which can be used to identify the beginning of the over-
rich regions predicted by different mechanisms through the inter-
ception points of T = Tmax − Teq and T = 0 lines. Different T
values are seen for different mechanisms in Fig. 8, especially at
the fuel-rich side; and the predicted over-rich turning points vary
within φ = 1.1 ± 0.05. It is also noted that at the leaner side, the
local maximum temperature, which is around the flame front, is
lower than the equilibrium temperature by about 10 K, indicating
that there are exothermic reactions slowly releasing heat at the far
away tails of NH3 /air flames.
Compared with the over-rich flames of hydrocarbons [19], the
over-rich NH3 /air flames share the same characteristics of the SAFT
and H2 O–H2 conversion after the flame front, while several dif-
ferences can also be found. Firstly, there are no obvious over-rich
turning points shown in the NH3 /air temperature coefficient α pro-
files in Fig. 2. Secondly, in the absence of C element in NH3 , the
radical that overwhelms the importance of H and OH radicals in
the flame front is NH2 in NH3 /air flames rather than CH3 in hy-
drocarbon flames. Also, the O element (in the form of OH radi-
cal) released by the H2 O–H2 conversion in the over-rich NH3 /air
flames forms NO rather than CO, resulting in the local increase of
NO concentration after the flame front. As has been discussed by
Kobayashi et al. [26], the adiabatic NH3 flames have lower flame
319
temperature thus lower equilibrium NO concentrations than the
adiabatic CH4 flames, while NO is abundant in the NH3 flame front
(see Figs. 4(g) and (h) and 7), and its concentration can only de-
crease in very long adiabatic post flame zone, which is hard to
achieve in real applications, making NOx emission a main concern
in the NH3 combustion. The present recognition of the over-rich
NH3 flame structure is therefore important because there is al-
ways a local minimum of [NO] within 1 cm after the over-rich
flame front (see Fig. 4(h)), i.e., a low [NO] level can be reached
with much shorter adiabatic zone needed, which may be helpful
for reducing the NOx emission in practical applications.
5. Conclusions
New measurements of the NH3 /air burning velocities at differ-
ent unburnt temperatures and 1 atm have been performed using
the heat flux method. Five recently published ammonia combus-
tion mechanisms were compared with the experimental data. The
temperature coefficients α of NH3 /air flames were derived from
the burning velocity results, and obvious differences were found
in the simulation results with and without radiation heat loss.
By analyses of the overall activation energy, temperature and
species profiles as well as the reaction pathways, characteristics of
the over-rich NH3 /air flames were revealed. At equivalence ratio
larger than 1.1 ± 0.05, the NH3 +air adiabatic flame becomes so
rich that (1) the NH2 radical overwhelms the H and OH radicals
in maximum mole fraction; (2) after the flame front, H2 O con-
verts back to H2 with NO formed at the same time, causing the
superadiabatic flame structure. In the over-rich NH3 /air flames, a
point with local minimum NO concentration is found right after
the flame front, which may be helpful in reducing the NO emis-
sions from NH3 flames in real applications.
Declaration of Competing Interest
The authors declare that they have no known competing finan-
cial interests or personal relationships that could have appeared to
influence the work reported in this paper.
Acknowledgments
This work was supported by the National Natural Science Foun-
dation of China (51876192, 51621005) and National Scholarship for
Building High Level Universities (China Scholarship Council).
Supplementary material
Supplementary material associated with this article can be
found, in the online version, at doi:10.1016/j.combustflame.2020.
04.013.
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