i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 7 ( 2 0 2 2 ) 3 6 0 4 6 e3 6 0 5 7

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Experimental and numerical study of the laminar

burning velocity of NH3/H2/air premixed flames at
elevated pressure and temperature

Bao-zhi Jin a,b, Yong-Feng Deng c, Guo-xiu Li a,b,*, Hong-meng Li a,b,**

a
School of Mechanical, Electronic and Control Engineering, Beijing Jiaotong University, Beijing, 100044, China
b
Beijing Key Laboratory of New Energy Vehicle Powertrain Technology (Beijing Jiaotong University), Beijing, 100044,
China
c
Xi'an Aerospace Propulsion Insititute, Xi'an, 710000, China

highlights

Laminar burning velocity of NH3/H2/air flames were studied using spherical flames.

Experimental data were measured under different XH2, 4, P and T conditions.

The experimental results are compared with simulation and published results.

Maximum mole fraction, normalized sensitivity and reaction pathway were studied.

article info abstract

Article history: Ammonia (NH3) is a carbon-free fuel that shows great research prospects due to its ideal
Received 21 May 2022 production and storage systems. The experimental data of the laminar burning velocity of
Received in revised form NH3/H2/air flame at different hydrogen ratios (XH2 ¼ 0.1e0.5), equivalent ratios (4 ¼ 0.8
19 August 2022 e1.3), initial pressures (P ¼ 0.1e0.7 MPa), and initial temperatures (T ¼ 298e493 K) were
Accepted 21 August 2022 measured. The laminar burning velocity of the NH3/H2/air flame increased upon increasing
Available online 16 September 2022 the hydrogen ratios and temperature, but it decreased upon increasing the pressure. The
equivalent ratio of the maximum laminar burning velocity was only affected by the pro-
Keywords: portion of reactants. The equivalence ratio value of the maximum laminar burning velocity
Ammonia was between 1.1 and 1.2 when XH2 ¼ 0.3. The chemical reaction kinetics of NH3/H2/air
Hydrogen flame under four different initial conditions was analyzed. The less NO maximum mole
Laminar burning velocity fraction was produced during rich combustion (4 > 1). The results provide a new reference
Elevated pressure for ammonia as an alternative fuel for internal combustion engines.
Elevated temperature © 2022 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.

* Corresponding author. School of Mechanical, Electronic and Control Engineering, Beijing Jiaotong University, Beijing 100044, PR China.
** Corresponding author. School of Mechanical, Electronic and Control Engineering, Beijing Jiaotong University, Beijing 100044, PR China.
E-mail addresses: Li_guoxiu@163.com (G.-x. Li), hongmengli@bjtu.edu.cn (H.-m. Li).
https://doi.org/10.1016/j.ijhydene.2022.08.198
0360-3199/© 2022 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.
 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 7 ( 2 0 2 2 ) 3 6 0 4 6 e3 6 0 5 7
Introduction
The use of fossil fuels has aggravated the global greenhouse
effect. To reduce the carbon dioxide emissions caused by
human activities, one of the most important research topics is
to find alternative fuels with low (even zero) carbon dioxide
emissions and high combustion efficiency [1]. In addition to
the use of renewable energies, ammonia (NH3) as a carbon-
free fuel has attracted more and more attention. Ammonia
has the advantages of a high energy density, mature prepa-
ration method, low cost, and easy availability. Its production,
transportation, and storage systems are full-fledged [2]. It can
be liquefied for storage and transportation at 0.8 MPa and
293 K, and it is much cheaper to produce than liquefied
hydrogen. Ammonia can be widely used in internal combus-
tion engines [3,4], fuel cells [5,6], and gas turbines [7e9].
Compared with the combustion of fuels such as CH4 [10] and
petroleum, ammonia has no carbon emissions, making it
more environmentally friendly [11,12].
The laminar burning velocity is an important parameter for
analyzing reaction fuel combustion characteristics and veri-
fying the chemical reaction mechanism during combustion
[13,14]. However, the laminar burning velocity of ammonia is
lower than that of natural gas [14], oil, and other traditional
fuels, which limits its development as a new fuel. In addition,
the incomplete combustion of ammonia produces harmful
gases such as nitrogen oxides (NOx). Many scholars have
studied ammonia combustion products and nitrogen oxide
emissions [15e17]. In recent years, three main solutions have
emerged to enhance the low laminar burning velocity of
ammonia during combustion: the premixed fuel, oxidizer
enhancement and turbulence enhancement [19]. The pre-
mixed fuel strategies involve mixing ammonia with other
more active fuels. It requires the active fuels to have similar
advantages and combustion characteristics to ammonia
[20e24]. The oxidizer enhancement strategies typically pro-
vide an oxygen-rich environment for the fuel [43e45]. Shres-
tha et al. [45] measured the laminar burning velocity of NH3/
oxygen by using helium as an inert gas. The turbulence
enhancement strategy is to provide turbulent environment for
fuel to increase the laminar burning velocity [44,53]. The
premixed fuel strategies focused in this paper.
Many scholars have investigated the mixing of NH3 with
active gases including CH4 [24,25], syngas [32e34], H2
[23,34,40,51,52], an oxygenated fuel [38,55e57], and cracking
ammonia [18]. The laminar burning velocity of NH3/CH4/air
mixture fuel has been studied in many literatures [24,25]. The
results have shown that the Markstein length increased upon
increasing the equivalence ratio and the proportion of NH3 in
the flame [25]. The unstretched laminar burning velocity of
NH3/CH4/air was measured at a high turbulence in a fan-stirred
constant-volume vessel [26]. The Karlovitz value increased
upon decreasing the Markstein length at the flame propagation
limit. Christian Brackmann et al. [27] measured the concen-
tration changes of amino groups (-NH) and nitric oxide (NO)
during NH3/CH4 flame combustion using laser-induced fluo-
rescence. Their experimental data were in good agreement
with the simulated data obtained using the predictive model
developed by Mendiara [28]. The addition of CH4 had
36047
significantly enhanced the ignition of NH3 in a rapid
compression machine [29]. Increasing the initial temperature
also increased the combustion limit of NH3/CH4 flame, but
non-premixed combustion will have higher COx and NOx
emissions, which will cause great environmental harm [30,31].
Ammonia can be used as a good substitute for oil in combus-
tion devices such as internal combustion engines [39]. There-
fore, many literatures have carried out experimental studies
on the combustion of NH3/syngas/air mixtures [32e34]. Many
mechanism models have been applied to NH3/syngas flame
combustion, and the simulation results of these mechanisms
for mixed fuels are differences between them [ [35e37]]. The
laminar burning velocity of NH3/air flame can be improved by
adding clean energy hydrogen [40], which has a greater impact
than other active gases [33]. NH3/H2/air combustion has sig-
nificant advantages for carbon-free combustion. The laminar
burning velocities of NH3/H2/air flame have been measured by
a variety of experimental methods using spherical flames [41]
and the heat flux method [34]. Increasing the hydrogen fraction
in fuel mixtures has significant effects on the laminar com-
bustion velocity, critical radius, reactivity, and flame stability.
The result is that the higher thermal conductivity and thermal
diffusivity of hydrogen increase the chemical reaction rate of
the hydrogen-blended mixtures [54]. He et al. [42] studied the
effect of hydrogen ratio on the ignition delay time of NH3/H2
flame in a rapid compression machine.
In addition to the above three types of fuel, the oxygenated
fuel and cracking ammonia strategies have also received
extensive attention. Zhihua Wang et al. [38] added ammonia
to the oxygenated fuels CH3OH and C2H5OH for premixed
combustion. The premixed fuel includes cracking ammonia
into nitrogen and hydrogen to increase the overall activity of
the premixed fuel. It does not require the addition of other
components to the NH3/air flame. The laminar burning ve-
locity of the cracking of the ammonia flame increases upon
enhancing the cracking of fuel mixtures [18]. Moreover, com-
bustion characteristics of dimethoxymethane [55], dimethyl
ether [56] and diethyl ether [57] mixtures with ammonia has
also been studied.
The purpose of this paper is to extend the previous work
[23,34,40,51,52] on adding H2 to NH3/air flame and to enrich
the experimental database of NH3/H2/air flame. Experimental
studies were carried out in this paper, and the laminar
burning velocities of NH3/H2/air flame were measured at
different hydrogen ratios (XH2 ¼ 0.1e0.5), equivalent ratios
(4 ¼ 0.8e1.3), initial pressures (P ¼ 0.1e0.7 MPa), and initial
temperatures (T ¼ 298e493 K). The chemical reaction kinetics
of NH3/H2/air flame was analyzed by three mechanisms
[25,47,48], and the effects of different initial conditions on the
maximum mole fractions, sensitivity analysis and reaction
path were studied.
Experimental setup and processing
Experimental set-up
Fig. 1 shows the schematic diagram of the high-pressure and
high-temperature experimental equipment. The experiment
was carried out in a stainless-steel constant-volume
36048 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 7 ( 2 0 2 2 ) 3 6 0 4 6 e3 6 0 5 7
Fig. 1 e Schematic diagram of the experimental measurement device.
combustion bomb with an inner diameter of 160 mm and an
effective length of 180 mm. A flexible heating sleeve made of
nickel-chromium wire was used to provide a maximum
temperature of 500 K. A K-type armored thermocouple was
used to measure the environmental temperature in real-time.
The initial pressure was provided by NH3 (99.999% purity), H2
(99.999% purity), and synthetic air (21%O2/79%N2 by volume).
During the experiments, a Leno single-stage rotary vane vac-
uum pump was used to evacuate the gas that had burned in a
combustion chamber to 0.001 MPa by using a heat-resistant
pressure gauge. Synthetic air was also used to clean residual
gas in the combustion chamber 3e4 times to avoid affecting
subsequent experiments.
A high-speed photography system was used to record the
premixed flame combustion process. Flame propagation
image were recorded with a FASTCAM SA-X2 high-speed
camera, with a resolution of 1024 * 1000 and a sampling fre-
quency of 13,500 fps. In this paper, the premixed fuel was
ignited by a pair of ignition electrodes in the constant-volume
combustion bomb. To avoid the impact of ignition energy and
chamber confinement on the experimental results, the effec-
tive radius of the flame is limited to 10e30 mm and the flame
has no obvious cell structure. Thresholding, which is a sub-
function of MATLAB software, was used to process flame
combustion schlieren photos. The laminar burning velocity of
the premixed combustion flame was obtained through the
above methods. Fig. 2 shows the flame image of NH3/H2/air
flame as a function of XH2 at 4 ¼ 1.0，P ¼ 0.5 MPa，T ¼ 298 K.
The center of NH3/H2/air flame will move up under the influ-
ence of buoyancy instability, especially at low hydrogen ratio.
The flame images with R > 20 mm were not obtained due to
buoyancy instability at XH2 ¼ 0.1 4 ¼ 1.0, P ¼ 0.5 MPa, and
T ¼ 298 K. It is interesting that the flame crack phenomenon
becomes obvious with the increase of XH2. The method of
multiple experiments were used to reduce the experimental
results uncertainties caused by systematic and linear fitting
uncertainties. The results of each group were averaged at least
3 times. The experimental uncertainties range are in the range
of 0.02e3.32 cm/s and are plotted as the error bars in the
following experimental results. All experimental data
excluded flame images with cellular structures in this paper.
Experimental conditions
The laminar burning velocity of NH3/H2/air flame was studied
at different hydrogen ratios (XH2), equivalent ratios (4), initial
pressures (P), and initial temperatures (T). The overall chem-
ical reaction equation for the complete combustion of NH3/H2/
air is:

3  XH2 3  XH2
1  XH2 NH3 þ XH2 H2 þ ðO2 þ 3:76N2 Þ ¼ H2 O
4 2
13:28  5:76XH2
þ N2 (1)
2
where XH2 is the mole fraction of hydrogen in the premixed
fuel. Synthetic air is made up of 21% oxygen and 79% nitrogen.
The equivalent ratio in this study was defined as:
 
nair
nNH3 þnH2
4¼  sh (2)
nair
nNH3 þnH2
where Xsh is the theoretical air-fuel ratio. The experimental
conditions of this study are shown in Table 1.
Experimental system verification
To verify the accuracy of the experimental system and ensure
the reliability of the experimental data, this work compared
multiple sets of experimental data with the results of many
scholars [23,25,34,40,47,48,51,52]. Fig. 3 shows the experi-
mental data of the laminar burning velocity of NH3/H2/air
flame as a function of XH2 compared with the experiment data
of Charles et al. [23], Han et al. [34], Ichikawa et al. [40], Lee et al.
[51], Li et al. [52] and the simulation results of Okafor et al. [25],
the GRI-mech [47] and Otomo et al. [48] at 4 ¼ 1.0, P ¼ 0.1 MPa
and T ¼ 298 K. The experimental data in this paper are in good
agreement with the experimental results of other authors and
simulation results of three mechanisms. The results verify the
reliability of this experimental measurement device.
Kinetic modeling approach
PREMIX model, which is a module of ChemkinPro [46] used to
measure the kinetics of chemical reactions, was used to
 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 7 ( 2 0 2 2 ) 3 6 0 4 6 e3 6 0 5 7 36049

Fig. 2 e Flame image of NH3/H2/air flame as a function of XH2 at 4 ¼ 1.0, P ¼ 0.5 MPa, and T ¼ 298 K.

Table 1 e Experimental conditions.

P/MPa T/K XH2 4
0.1, 0.3, 0.5, 0.7 298, 343, 393, 443 0.1e0.5 0.8e1.3

simulate the laminar burning velocities of NH3/H2/air flame

[49,50]. Three chemical mechanisms were used: the mecha-
nism of Okafor et al. [25], the GRI-mech 3.0 mechanism [47],
and the mechanism of Otomo et al. [48]. Here they were named
as the Okafor-Mech [25], the GRI-Mech [47], and the Otomo-
Mech [48] in this paper. The Okafor-Mech consists of 59 com-
ponents and 357 elementary reactions which has established
detailed chemical mechanism. The GRI-Mech is the most basic
N and H combustion mechanism. The Otomo-Mech is estab-
lished for NH3 combustion and can predict laminar burning
velocity and ignition delay time at high pressure. By comparing Fig. 3 e Laminar burning velocities of NH3/H2/air flame as a
the difference between the experimental data and numerical function of XH2 in the experimental work and in the work
simulation in Fig. 3. The Okafor-Mech, which has more accu- of Charles et al. [23], Han et al. [34], Ichikawa et al. [40], Lee
rately predicted the laminar burning velocity, was used to et al. [51], Li et al. [52] and the predicted results using three
analyze the chemical kinetics of NH3/H2/air flame. mechanisms at 4 ¼ 1.0, P ¼ 0.1 MPa and T ¼ 298 K.
36050 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 7 ( 2 0 2 2 ) 3 6 0 4 6 e3 6 0 5 7
Results and discussion
In this work, the experimental results of the laminar burning
velocity of NH3/H2/air flame for different initial hydrogen
mixing ratios (XH2), equivalent ratios (4), pressures (P), and
temperatures (T) are given. The gas allocation was calculated
according to the complete combustion equation (1), and the
premixed combustion experiment was carried out in a
constant-volume combustion bomb.
Effects of hydrogen enrichment
Fig. 3 shows the laminar burning velocities of NH3/H2/air
flames as a function of XH2, measured in this work and in the
works of Charles et al. [23], Han et al. [34], Ichikawa et al. [40],
Lee et al. [51], Li et al. [52], and the predicted laminar burning
velocities using three mechanisms [25,47,48]. Due to the low
activity of NH3 at P ¼ 0.1 MPa, T ¼ 298 K, it was difficult to
ignite. In this work, the laminar burning velocities of NH3/H2
at XH2 ¼ 0.1 were not obtained. Fig. 3 shows that the laminar
burning velocities increased nonlinearly upon increasing the
hydrogen fraction in premixed fuel. The experimental results
are in good agreement with these paper.The results showed
that upon increasing the proportion of hydrogen in the NH3/
H2/air mixture, the overall activity of reactants was improved.
Fig. 3 also compares three highly recognized prediction
mechanisms, which predicted relatively smaller laminar
burning velocities, especially upon increasing XH2, at 4 ¼ 1.0,
P ¼ 0.1 MPa, T ¼ 298 K. However, the Okafor-Mech and the
Otomo-Mech provided more accurate predictions than the
GRI-Mech.
Fig. 4 shows the laminar burning velocities of NH3/H2/air
flames, as a function of XH2 at P ¼ 0.1, 0.3, 0.5, and 0.7 MPa.
Experimental error bands have been taken into account. The
experimental data were controlled within the range of XH2<0.5
to study the influence of increasing XH2 on the laminar
burning velocities of NH3/H2/air flame. The laminar burning
velocities of NH3/H2/air flame increased upon increasing XH2
for all high-pressure conditions. No experimental data were
measured for XH2 ¼ 0.1 or 0.5 when P ¼ 0.7 Mpa because NH3/
H2/air flames were not easy to burn under such a high
Fig. 4 e Laminar burning velocities of NH3/H2/air flame as a
function of XH2 mixtures in the experimental work at
4 ¼ 1.0, T ¼ 298 K.
Fig. 5 e Laminar burning velocities of NH3/H2/air flame as a
function of XH2 mixtures in the experimental work at
4 ¼ 1.0 and P ¼ 0.1 MPa.
pressure, which will be explained in more detail in section 4.3.
When XH2 ¼ 0.1, P ¼ 0.1 Mpa, the laminar burning velocities of
NH3/H2/air flame were not obtained, but when XH2 ¼ 0.1,
P ¼ 0.3, 0.5 MPa, a spherical flame was obtained in the
constant-volume combustion bomb. This indicates that an
increase in the pressure at the same volume was accompa-
nied by an increase in the total amount of hydrogen, which
dominated the overall activity of the premixed fuel and
enhanced the propagation of the spherical flame. However,
when the pressure was too high (P ¼ 0.7 MPa), the activity of
the fuel mixture was inhibited upon increasing the pressure.
Fig. 5 shows the laminar burning velocities of NH3/H2/air
flame as a function of XH2 at T ¼ 298, 343, 393, 443, and 493 K.
The enhancement in the laminar burning velocities of NH3/
H2/air flame upon increasing XH2 was observed at all high-
temperature conditions, which is consistent with the
conclusion of Charles Lhuillier et al. [23]. The laminar burning
velocity of the premixed flame was impacted more signifi-
cantly by pressure and temperature at a high hydrogen ratio
(XH2 ¼ 0.5). Increasing the temperature at low XH2 had a
smaller effect on the laminar burning velocities of NH3/H2/air
flame than that at high XH2, which is consistent with the in-
crease in the hydrogen activity at a high temperature.
Effect of the equivalence ratio
To study the effect of 4 on the laminar velocities of NH3/H2/air
flame, XH2 ¼ 0.3 was adopted to obtain the laminar burning
velocities of NH3/H2/air flame at high pressures and temper-
atures. Fig. 6 shows the laminar burning velocities of NH3/H2/
air flames, as a function of 4(0.8e1.3) at T ¼ 298 K, and
P ¼ 0.1 MPa, 0.3 MPa, and 0.5 MPa. For 4 ¼ 1.3, the spherical
flame was extinguished during combustion at P ¼ 0.1 MPa,
T ¼ 298 K because the initial ignition energy propagated to the
preheating zone and was gradually consumed, but it could not
ignite the fuel mixture. The laminar burning velocity of NH3/
H2/air flame increased linearly upon increasing the 4 in the
lean flame, which was not applicable to rich flame. This is
consistent with the conclusion drawn by Han et al. [34], Ichi-
kawa et al. [40], and Lee et al. [49]. It was found that the
maximum laminar burning velocity of NH3/air flame appeared
around 4 ¼ 1.05, but the 4 of the maximum laminar burning
 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 7 ( 2 0 2 2 ) 3 6 0 4 6 e3 6 0 5 7
Fig. 6 e Laminar burning velocities of NH3/H2/air flame as a
function of 4 measured in the experimental work at
XH2 ¼ 0.3, T ¼ 298 K, and P ¼ 0.1 MPa, 0.3 MPa, and 0.5 MPa.
velocity of NH3/H2/air flame was about 1.15 from Fig. 6. The 4
of the maximum laminar burning velocity increased upon
increasing XH2 because the maximum laminar burning ve-
locity of H2/air flame appeared at 4 ¼ 1.8. The present work
found that when XH2 ¼ 0.3, the 4 value of the maximum
laminar burning velocity was 1.1, but the laminar burning
velocity at 4 ¼ 1.2 was not much lower than the numerical
value at 4 ¼ 1.1. The laminar burning velocity showed an
obvious downward trend when 4 > 1.2. Therefore, it can be
concluded that when XH2 ¼ 0.3 for the NH3/H2/air premixed
flame, the maximum laminar burning velocity appeared at
4 ¼ 1.15. To obtain a more accurate position requires a more
accurate premixed gas in the constant-volume combustion
bomb, which is hard to achieve under the existing conditions.
Fig. 7 shows the laminar burning velocities of NH3/H2/air
flames as a function of 4(0.8e1.3) at P ¼ 0.1 MPa and T ¼ 298 K,
343 K, 393 K, and 443 K. It can be seen that in all high-
temperature and high-pressure environments, the 4 value
of the maximum laminar burning velocity of NH3/H2/air
flame followed the same trend, which is consistent with
some of the conclusions of Charles Lhuillier et al. [23].
Increasing the temperature enhanced the energy of the flame
in the preheating zone so that the spherical flame could
Fig. 7 e Laminar burning velocities of NH3/H2/air flame as
a function of 4 measured in the experimental work at
XH2 ¼ 0.3, P ¼ 0.1 MPa and T ¼ 298 K, 343 K, 393 K, and
443 K.
36051
spread after being ignited. Then, the experimental laminar
burning velocities at high temperatures and 4 ¼ 1.3 were
obtained. At the same time, the 4 value of the maximum
laminar burning velocity at high temperature was also the
same thing as before, and no scholar has been able to deter-
mine the 4 value of the maximum laminar combustion ve-
locity at a high temperature.
Effect of pressure
The experimental laminar burning velocities of NH3/H2/air
flame at room temperature and high pressure were measured.
However, to evaluate the influence of increasing the pressure
on the laminar burning velocity in more detail, it is necessary
to measure the experimental data of NH3/H2/air flame at a
high pressure and high temperature. In this paper, the
laminar burning velocities of NH3/H2/air flame at different
pressures were measured by using the method of controlling
variables at the determined initial temperature at (a) T ¼ 343 K,
(b) T ¼ 393 K, and (c) T ¼ 443 K. Fig. 8 shows the laminar
burning velocities of NH3/H2/air flame as a fraction of 4 at
initial pressure (P ¼ 0.1 MPa, 0.3 MPa, 0.5 MPa). As can be seen,
the laminar burning velocities of NH3/H2/air flame were
inhibited by increasing the pressure at all initial temperatures,
but the inhibition degree was different in lean combustion
and rich combustion. The suppression degree during lean
combustion was lower than that under rich combustion.
Compared with Fig. 4 at a fixed 4, the laminar burning veloc-
ities of NH3/H2/air flame decreased upon increasing the
pressure, even though the hydrogen component of the pre-
mixed fuel increased continuously. Under a high partial
pressure, the ignition energy was consumed quickly, and the
energy in the reaction zone could not be transmitted to the
preheating zone, resulting in flame extinction. Interestingly,
this phenomenon occurred at both the endpoints of XH2 ¼ 0.1
and XH2 ¼ 0.5, at P ¼ 0.7 MPa. Scholars have tried many ex-
periments but have failed to make the flames spread. It can be
seen from Fig. 8 that pressure did not affect the 4 of the
maximum laminar burning velocity, which is consistent with
the conclusion of Bowen Mei et al. [18].
Effect of temperature
Fig. 9 shows the laminar burning velocities of NH3/H2/air
flame as a function of 4 at different high temperatures
(T ¼ 298 K, 343 K, 393 K, and 443 K), which shows the flame
propagation law under high pressures (P ¼ 0.3 MPa, 0.5 MPa). It
can be seen that the laminar burning velocities of NH3/H2/air
flame increased upon increasing the temperature, and all
pressures followed this trend. Some of the experimental data
are so close that the error band is almost invisible in the figure.
At a certain XH2, increasing the laminar burning velocity was
stable for every 50 K increase of temperature. However, when
the temperature was raised from 393 K to 443 K, the effect on
the laminar burning velocities of reactants was more signifi-
cant. However, it can be seen from Fig. 5 that the influence of a
higher temperature on the laminar burning velocities of NH3/
H2/air flame at a high XH2 was greater than that at a low XH2.
For XH2 ¼ 0.1, the reactivity was improved by increasing the
temperature, and the NH3/H2/air premixed flame spread
36052 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 7 ( 2 0 2 2 ) 3 6 0 4 6 e3 6 0 5 7
Fig. 8 e Laminar burning velocities of NH3/H2/air flame as a
function of 4 measured in the experimental work at
XH2 ¼ 0.3, P ¼ 0.1 MPa, 0.3 MPa, 0.5 MPa, and different high
temperatures: (a) T ¼ 343 K, (b) T ¼ 393 K, and (c) T ¼ 443 K.
smoothly at high temperatures. Similarly, the 4 value of the
maximum laminar burning velocity was between 4 ¼ 1.1 and
4 ¼ 1.2. Therefore, it can be concluded that no matter how the
external initial conditions changed when XH2 was determined,
the 4 values of the maximum laminar burning velocities were
unaffected, and was only related to the proportion of fuel
components. From lean combustion to the 4 value, the
laminar burning velocity increased upon increasing 4. After
Fig. 9 e Laminar burning velocities of NH3/H2/air flame as a
function of 4 measured in the experimental work at
XH2 ¼ 0.3, T ¼ 298 K, 343 K, 393 K, and 443 K and for
different high-pressure conditions: (a) P ¼ 0.3 MPa and (b)
P ¼ 0.5 MPa.
reaching this 4, the laminar combustion velocity decreased
upon further increasing 4, which was true for all initial
operating conditions. The influence of 4 on the flame during
enriched combustion was more significant than that during
lean combustion because the content of reactants in enriched
combustion was higher, and the inert N2 content in the
mixture was reduced, which increased the overall activity of
premixed fuel. This phenomenon was particularly obvious at
a high pressure.
Kinetic analyses
The dynamic simulations of NH3/H2/air laminar combustion
were carried out, and the maximum mole fraction, the
normalized sensitivity, and the main chemical reaction paths
for four different initial working conditions were obtained.
Fig. 10 shows the maximum mole fraction of the main
combustion products as a function of 4 for NH3/H2/air flame
by the Okafor-Mech. It can be seen that the maximum mole
fractions of the major products changed at different initial
conditions, but the overall law remained unchanged. The
initial mole fraction of O decreased from lean conditions to
rich conditions, the mole fraction of OH reached its maximum
 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 7 ( 2 0 2 2 ) 3 6 0 4 6 e3 6 0 5 7
Fig. 10 e The maximum mole fractions of the major products as a function of 4 at XH2 ¼ 0.3, P ¼ 0.1 MPa, 0.5 MPa, and
T ¼ 298 K, 443 K for NH3/H2/air flame by the Okafor-Mech.
at the theoretical complete combustion, and the mole fraction
of OH decreased rapidly when 4 > 1. It can be seen from Fig. 10
that the variation in the maximum mole fraction of H was
quite consistent with that of the laminar burning velocity of
NH3/H2/air flame. In addition, the maximum mole fraction of
H radicals in the combustion products decreased upon
increasing the initial P and increased upon increasing the
initial T. This observation is consistent with variations in the
laminar burning velocity at different initial P and initial T,
which indicates that H radicals played a dominant role in the
laminar burning velocities of NH3/H2/air flame. Because of the
increase in the fuel ratio under rich conditions, the content of
NH3 and decomposition products (NH2 and NH) increased
linearly, and the maximum molar fraction of N2O decreased
linearly. Interestingly, the maximum mole fraction of NH2 and
N2O had a linear relationship with 4, which was true under all
initial conditions. It can be seen that the variation in the
maximum mole fraction of NO and OH were highly similar.
This indicates that less NO was produced during rich com-
bustion, which is of great significance for environmental
protection and the feasibility of NH3 as a non-polluting fuel.
Fig. 11 shows the sensitivity analysis of the laminar
burning velocities for NH3/H2/air flame at XH2 ¼ 0.3,
P ¼ 0.1 MPa, 0.5 MPa, and T ¼ 298 K, 443 K. It can be seen that
for all initial conditions, the positive sensitivity coefficient of
the reaction H þ O2 / O þ OH was much higher than for other
36053
elementary reactions. This reaction dominated the overall
reaction, which is consistent with the conclusions drawn in
Fig. 10. The elementary reaction NH2 þ H / NH þ H2 has a
higher negative sensitivity coefficient in the rich flame.
However, the elementary reactions H þ O2þH2O/HO2þH2O
and NH2þNO/NNH þ OH played less-important roles as 4
increased. Furthermore, increasing P made the reactions
O þ H2/H þ OH, NH2þO/HNO þ H, and NNH þ O2/N2þHO2
become less important. On the contrary, the elementary re-
actions H þ HO2/O2þH2, 2OH(þM)/H2O2(þM), OH þ HO2-
/O2þH2O, OH þ H2O2/HO2þH2O, and NH þ O2/HNO þ O
became more important. The effect of the OH radical con-
sumption rate on the laminar burning velocities of NH3/H2/air
became more significant upon increasing P. Increasing T made
the elementary reaction N2H2 þ H / NNH þ H2 less important.
Therefore, it can be concluded that the sensitivity of the
elementary reactions was more dependent on P.
Fig. 12 shows the main reaction pathway of N-containing
species for NH3/H2/air flame by the Okafor-Mech. The main N-
containing chemical reaction path was to obtain the chemical
reaction rate of species production (ROP) of each species and
take the TOP15 elementary reactions by CHEMKIN numerical
simulations. The chemical reaction rate of species production
was integrated into the reaction distance to obtain the
decomposition consumption ratio of species by the Okafor-
Mech. The consumption proportion of digital representation
36054 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 7 ( 2 0 2 2 ) 3 6 0 4 6 e3 6 0 5 7

Fig. 11 e Sensitivity analysis of the laminar burning velocities for NH3/H2/air flame at XH2 ¼ 0.3, P ¼ 0.1 MPa, 0.5 MPa, and
T ¼ 298 K, 443 K.

Fig. 12 e The main reaction pathway of N-containing species for NH3/H2/air flame by the Okafor-Mech at XH2 ¼ 0.3 (a)
P ¼ 0.1 MPa and T ¼ 298 K, (b) P ¼ 0.5 MPa and T ¼ 298 K, (c) P ¼ 0.1 MPa and T ¼ 443 K, and (d) P ¼ 0.5 MPa and T ¼ 443 K.
Black represents the lean flame (4 ¼ 0.8) and red represents the rich flame (4 ¼ 1.2). (For interpretation of the references to
colour in this figure legend, the reader is referred to the Web version of this article.)
 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 7 ( 2 0 2 2 ) 3 6 0 4 6 e3 6 0 5 7
participating in reaction species, black represents the lean
flame (4 ¼ 0.8) and red represents the rich flame (4 ¼ 1.2). The
initial reactant NH3 was transformed by H radicals into NH2
radicals and NH radicals and finally formed N2.
It can be seen that from the oxygen-sufficient lean com-
bustion environment to the fuel-sufficient rich combustion
environment, the O content in the reaction environment
gradually decreased. The H free radicals generated by NH3
decomposition gradually increased, which gradually decreased
the reaction with OH radicals, and the reactant þ H reaction
significantly increased in Fig. 12. Combined with the distribu-
tion of the maximum mole fractions of OH and H shown in
Fig. 10 for the initial conditions, it can be concluded that the
laminar burning velocity of NH3/H2/air flame under lean flame
conditions was mainly affected by OH radicals. It was mainly
affected by H radicals under rich combustion conditions, which
should be established on all initial conditions.
NH3 decomposition products (NH2 radicals and NH radicals)
consumed each other via the elementary reaction NH2 þ NH
/ N2H2 þ H. The stable trend of NH radical consumption
fraction was slightly affected by P and T. NHx showed a more
obvious pressure dependence than NOx throughout the whole
chemical reaction pathway. The N2 generated by the elemen-
tary reaction NNH þ O2 increased significantly upon increasing
the P. The mole fraction of the elementary reaction NH2 þ NO
/ NNH þ OH was small, but the sensitivity analysis in Fig. 11
showed that this reaction has a high sensitivity coefficient to
promote the overall reaction. Interestingly, the elementary
reaction N þ O2 / NO þ O showed an increasing trend upon
increasing P. It can be seen from Fig. 12 that HNO, NO, and N2O
radicals were the main nitrogen oxides produced during the
reaction process of NH3/H2/air flame, which were mainly ob-
tained by the oxidation of NH radicals. The elementary reac-
tion HNO þ H / H2 þ NO decreased significantly upon
increasing P in both lean flame and rich flame. The NO radical
consumption fraction remained stable under different condi-
tions. The elementary reaction N2O þ H / N2 þ OH decreased
upon increasing P, especially under lean flame (4 ¼ 0.8).
However, the influence of the initial T on the chemical reaction
path of N-containing species for NH3/H2/air flame was weaker
than that of the initial P. Combined with the conclusion in
section 3.4 in this paper, it can be concluded that temperature
improved the chemical reaction rate, but it did not affect the
reaction proportion of each species.
Conclusion
This work provides accurate experimental data of the laminar
burning velocities of new carbon-free fuels NH3/H2/air flame
under different initial conditions. The dynamic simulations of
NH3/H2/air flame were studied combined with experimental
data. Analyzing the influence of different initial conditions on
premixed flame results revealed several conclusions.
1 The overall activity of reactants was improved upon
increasing the proportion of hydrogen in the NH3/H2/air
mixture fuel. Pressure and temperature had more signifi-
cant effects on the laminar burning velocity of premixed
flame at a high hydrogen ratio. At 4 ¼ 1.0, upon increasing
36055
the temperature, the flame that would have been extin-
guished even at a low hydrogen ratio (XH2 ¼ 0.1) could be
well propagated. However, under a high pressure, the
flame was extinguished even a high hydrogen ratio
(XH2 ¼ 0.5).
2 In the NH3/H2/air premixed flame, the equivalent ratio of
the maximum laminar burning velocity was only related to
the proportion of fuel and had no connection to the initial
conditions of the premixed fuel. The laminar burning ve-
locity of the NH3/H2/air flame decreased upon increasing
the pressure and increased upon increasing the hydrogen
ratio and temperature, which was confirmed for all initial
conditions.
3 Through comparative analysis, it can be concluded that the
trends of the maximum mole fraction of H radicals and the
law of laminar burning velocities of NH3/H2/air flame were
the same for all initial working conditions. In the case of
rich combustion, the same laminar burning velocity is
guaranteed and less NO is produced. It was found that
there were great differences in the normalized sensitivity
of the elementary reactions during lean combustion and
rich combustion, and the pressure had a more significant
effect on the normalized sensitivity of the elementary re-
actions. The analysis of the NH3/H2/air chemical reaction
path showed that the consumption of each species under
different conditions. Increasing the temperature did not
affect the proportion of each species in the reaction.
Declaration of competing interest
The authors declare that they have no known competing
financial interests or personal relationships that could have
appeared to influence the work reported in this paper.
Acknowledgements
This work is supported by the Fundamental Research Funds
for the Central Universities (No. 2022JBZY033), the National
Natural Science Foundation of China (No. 51706014) and the
Fundamental Research Funds for the Central Universities (No.
2022YJS084).
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