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 5 ( 2 0 2 0 ) 1 1 5 1 e1 1 5 7

Available online at www.sciencedirect.com

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Analysis of nitrogen oxide emissions from modern

vehicles using hydrogen or other natural and
synthetic fuels in combustion chamber*

S.E. Shcheklein*, A.M. Dubinin

Ural Federal University Named After the First President of Russia B.N. Yeltsin, 19 Mira Str., Yekaterinburg, 620002,
Russia

article info abstract

Article history: The paper presents a calculated analysis of the equilibrium emission of nitrogen oxides on
Received 28 October 2019 the exhaust of carburetor and diesel internal combustion engines. The temperature of fuel
Accepted 29 October 2019 oxidation is assumed to be 1,400
C while the pressure for carburetor and diesel engines is
Available online 26 November 2019 assumed to be 60 atm and 80 atm respectively. The studies have been carried out for
natural and synthetic fuels such as hydrogen, ethanol, methanol, petroleum, diesel fuel
Keywords: and methane at the excess air coefficient corresponding to the fuel oxidation temperature
Nitrogen oxides of 1,400
C. In the paper, the method for calculating the equilibrium composition based on
Hydrogen the equilibrium constant and mass conservation equations has been applied. It is shown
Ethanol that with an increase in pressure from 1 atm to 60 atm for carburetor engines and up to
Methanol 80 atm for diesel engines, the reaction of nitrogen dioxide formation may shift towards an
Petroleum increase in NO2. The formation of NO may be not affected by the increase in pressure by
Methane virtue of the fact that the reaction proceeds without changes in the amount. It has been
determined that NO is the major atmospheric pollutant. However, it would be advisable to
use more extensively the fuels characterized by the lowest output of nitrogen dioxide
(methane and methanol), since nitrogen dioxide (NO2) related to the 2nd hazard class is
appeared to be the most dangerous to humans. It has been revealed that the reduction in
oxidation temperature using hydrogen as a fuel for electrochemical current generators
may allow reducing nitrogen oxide emissions by more than an order of magnitude as
compared to the best results for ICE.
© 2019 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.

*
This paper is the English version of the paper reviewed and published in Russian in International Scientific Journal for Alternative
Energy and Ecology “ISJAEE”, issue 291e293, number 07e09, date March 31, 2019.
* Corresponding author.
E-mail address: s.e.shcheklein@urfu.ru (S.E. Shcheklein).
https://doi.org/10.1016/j.ijhydene.2019.10.206
0360-3199/© 2019 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.
1152 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 5 ( 2 0 2 0 ) 1 1 5 1 e1 1 5 7
Nomenclature
Acronyms
ICE internal combustion engine
Greek words
m volume concentration of components in a gas
mixture
Sni sum of mixture components after reaction, m3/
m3
Svi algebraic sum of kilomoles of reaction (1e7)
components before and after reaction
Latin words
Kр equilibrium constant of reaction (1)
P pressure, atm
R universal gas constant, kkal/mol К
r concentration in a base mixture, g$mol/l
T temperature, К
to admitted temperature, K (
C)
Z varying equilibrium concentration, m3/m3
Superscripts and subscripts
in inert gases
p equilibrium
* after reaction (7)
о standard parameters
Introduction
In recent years, the possibility of using natural gas and
different types of synthetic fuels for application in power
engineering and transport has been explored [1e5].
An interest in these studies has arisen in connection with
the necessity to reduce the dependence on imported fuel re-
sources, primarily oil, which show a steady growth trend in
cost as well as to use available resources of biomass, coal,
domestic and industrial organic waste.
On the other hand, the developed (USA, EU, Japan etc.)
countries and emerging (China, India, Brazil etc.) countries are
facing the issue of negative environmental impact of trans-
port and power engineering. First and foremost, there is a
problem of reducing greenhouse effect caused by fuel com-
bustion products, the main one being carbon dioxide.
In addition to fuel, combustion reaction may require an
oxidizer, and the only oxidizer for power engineering and
transport is atmospheric air consisting of more than 70% ni-
trogen. At high temperatures typical for the fuel combustion,
and when the excess oxidizer volume (in relation to stoi-
chiometric) is required, various nitrogen compounds may be
formed in fuel combustion products. Most of these com-
pounds are anthropogenic as well as strictly limited [6e8].
Nitrogen dioxide and nitrogen oxide may pose the greatest
danger. The results of a study on the content of nitrogen ox-
ides (NOx) in big cities in a number of countries show a sub-
stantial increase of such compounds exceeding the
established norms by several times in some instances [9e12].
Reduction of NOx emissions from modern vehicles and power
plants may be achieved by improving the design of engines
and furnaces, applying neutralization systems, and increasing
quality requirements for conventional fuels [13e16].
The formation of nitrogen oxides while using modern
synthetic fuels has not been sufficiently studied so far. On the
other hand, new fuels may be an efficient instrument for
improving environmental condition [17,18].
The paper presents the results of theoretical study on NOx
formation while using conventional and new vehicle fuels.
Formation of nitrogen oxides
There are three known mechanisms for nitrogen oxide for-
mation, according to which they are divided into thermal, fuel
and prompt nitrogen oxides. Fuel oxides may be formed from
nitrogen compounds chemically bound to the fuel used, being
typical for solid fuels (coal, wood etc.). Prompt oxides may
arise from air nitrogen at high temperatures (more than
2,000
С). Thermal mechanism is the main one for modern
internal combustion engines (ICE) running on liquid and
gaseous fuels at moderate temperatures. Thermal oxides may
be produced by the oxidation of air nitrogen, and their con-
centration cannot exceed the equilibrium [19]. It has been
shown in pioneering works of Y.B. Zel’dovich [20] that the
formation of nitrogen oxides during fuel combustion in the air
is based on the nonbranched chain reaction wherein atoms of
oxygen and nitrogen may play an active role. It has been
determined that the energy barrier of NO formation reaction is
sufficiently high, being composed of the energy of the oxygen
atom formation (499$103kJ) and the energy of the oxygen atom
interaction with nitrogen molecule (314$103kJ), and could be
overcome at sufficiently high temperatures only.
According to [20], the dependence of NO equilibrium con-
centration on temperature may be determined as follows:

. pffiffiffi pffiffiffiffiffiffiffiffiffiffiffiffiffi
p
rNO ¼ 8 3 , ro2 rN2 ,expð21400 = RTÞ
Here, rO2 ; rN2 are concentrations of oxygen and nitrogen in a
base mixture, g$mol/l; R ¼ 1.98kkal/mol$K.
The analysis of NOx formation for the admitted combus-
tion temperature range in modern ICE and in fuels of different
chemical compositions is provided below.
Nitrogen oxide formation
The oxidation reaction of molecular nitrogen by air oxygen
may run in the following way:
N2þО2 ¼ 2NO. (1)
Logarithm of the equilibrium constant for reaction (1)
[21,22] may be written as follows:
 
lgKp ¼  9; 581 T  0:022lgT þ 0:068,105 T2 þ 1:38: (2)
The equilibrium constant for reaction (1) at the admitted
temperature to ¼ 1,673 K (1,400
С) can be written as:
Kp ¼ 40$106.
 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 5 ( 2 0 2 0 ) 1 1 5 1 e1 1 5 7 1153

On the other hand, the following condition is met for the A part of the formed NO may be spent on the formation of
equilibrium mixture [23,24]: NO2 according to reaction (7).
 P 2  Logarithm of the equilibrium constant for reaction (7) [21]
X
r P may be written as follows:
Kp ¼
NO  P vi : (3)
rPN2  rPO2 ni
 
lgK*р ¼ 6; 017:2 T  0:998lgT þ 0:302,103 T

Here, equilibrium concentrations of N2 and O2 in combustion 0:237,105 T2  5:175:
products of the first stage may be written as follows [23,24]:
For the admitted temperature to ¼ 1,673 K (1,400
С) it may
p
rN2 ¼ rN2  0; 5Z; (4) be written as follows:

p
rO2 ¼ rO2  0; 5Z; (5) K*p ¼ 50 106.

Here, rN2 and rO2 are volume ratios of N2 and O2 in combustion Also, the following relation holds for equilibrium condi-
products of various fuels at the excess air coefficient (a) at tions [28,29]:
which the temperature of combustion products is equal to
P
2
1,673 K (to ¼ 1,400
С); P is the pressure of mixture, atm; ni is a r*NO2  P vi
P
sum of mixture components, m /m . 3 3 K*P
¼  2 P : (8)
r*NO r*O2 ni
In this instance, fuel oxidation may assume the form
P
shown in Table 1 [25e27]. Here, vi ¼ vNO2  vNO  vO2 ¼ 2e2e1 ¼ e1. The reaction is
accompanied by a decrease in volume. An increase in pressure
Concentration of N2 and O2 in oxidation products shifts the equilibrium towards an increase in NO2
concentration.
For example, concentrations for Н2 may take the following We shall introduce the following notations of the mixture
forms: rN2 ¼ 1þ3:196þ0:35
3:196
¼ 0:703m3/m3; rO2 ¼ 1þ3:196þ0:35
0:35
¼ components [23,24]:
3 3
0:0769m /m .
p
We shall denoterNO ¼ Z. r*NO2 ¼ Z* ; (9)
Reaction (1) proceeds without changes in volume as fol-
P P
lows: vi ¼ vNO  vN2  vO2 ¼ 2e1 e 1 ¼ 0. Then, ðP= ni Þ0 ¼ 1. r*O2 ¼ rO2  0:5Z* ;
p
(10)
Here, the pressure does not affect the reaction.
Taking into account equations (4) and (5), equation (3) r*NO ¼ rNO  Z* ;
p
(11)
could be written as follows:
 

p p
Kр ¼ z2 =ðrN2  0:5z rO2  0:5z (6) rин ¼ 1  rO2 þ rNO :
p
Solving this equation, we find thatrNO ¼ Z, while the values Here, rin is the volume fraction of inert ingredients (H2O, CO2).
p p
forrN2 and rO2 (m3/m3) may be found from equations (4) and (5) Then,
respectively. X  p 
p 
The results for each fuel are given in Table 2 and Fig. 1. ni ¼ Z* þ rNO  Z* þ rO2  0:5Z* þ rin ¼
These results will be used further to determine equilibrium
¼ rNO þ rO2  0:5Z* þ 1  rO2  rNO ¼ 1  0:5Z* :
p p p p
p
concentrationrNO2 .
p p
The values for rNO and rO2 are given in Table 2.
Formation of nitrogen dioxide We shall use the previously obtained equilibrium values
for NO formation (see Table 2) to write equation (8) in the
The main reaction of NO2 formation in combustion products following way:
may correspond to oxidation of the formed nitrogen oxide by
 1
the residual oxygen as follows: ðZ* Þ2 P ðZ* Þ2 ð1  0:5Z* Þ
K*р ¼  2 ¼  * 2 * :
rNO r*O2
* 1  0:5Z* rNO rO2 P
2NO þ О2 ¼ 2NO2. (7)

Table 1 e Excess air coefficients and fuel combustion reactions at 1,400
C.

Fuel Excess air coefficient a Equation
Hydrogen 1.7 H2 þ 0.85(О2 þ 3.76 N2) ¼ H2O þ 3.196N2 þ 0.35О2
Ethanol 1.55 C2 H5 OH þ 4.66(О2 þ3.76 N2) ¼ 2СO2 þ 3H2O þ 17.52N2 þ 1,66О2
Methanol 1.5 C H3 OHþ2.25(О2 þ3.76 N2) ¼ СO2 þ 2H2O þ 8.46N2 þ 0,75О2
Petroleum 1.6 C7 H16 þ 17.6(О2 þ 3.76 N2) ¼ 7СO2 þ 8H2O þ 66.176N2 þ 6,6О2
Diesel 1.4 C8 H18 þ 17.5(О2 þ 3.76 N2) ¼ 8СO2 þ 9H2O þ 65.8N2 þ 5О2
Methane 1.43 СH4 þ 2.86(O2 þ 3.76N2) ¼ CO2 þ 2H2O þ 10.7536N2 þ 0,86О2
1154 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 5 ( 2 0 2 0 ) 1 1 5 1 e1 1 5 7

Table 2 e Equilibrium concentrations of NO, N2 and О2 (m3/m3) in combustion products of the first stage.
Characteristic Notation Hydrogen Ethanol Methanol Petroleum Diesel Methane
p
rNO m3/m3 0.0015347 0.0014707 0.0013602 0.0015702 0.0013615 0.0013717
p
rN2 m3/m3 0.7022683 0.72383 0.692195 0.753134 0.74875 0.735177
p
rO 2 m3/m3 0.0762234 0.067916 0.060745 0.074406 0.056267 0.058163

Fig. 1 e Equilibrium NO concentrations in combustion Fig. 2 e Equilibrium concentrations of NO2 in combustion

products. products (P ¼ 1 atm).

The solution for determining NO2 concentration may be

found from the following equation:
 2

K*P , r*NO , r*O2 , P ¼ ðZ* Þ2 ,ð1  0; 5Z* Þ: (12)

Valuesr*NO2 ¼ Z* andr*NO may be determined from equations

(12) and (11) respectively. Then, their sumr*NO þ r*NO2 may be
found. Calculation results at pressure of 1 atm are shown in
Table 3 and Fig. 2, while those at pressure 60 atm and 80 atm
for carburetor and diesel ICE respectively are shown in Fig. 3.
As expected, an increase in pressure may result in the
increased equilibrium concentration of NO2 by more than 10
times. Hence, the increase in thermodynamic parameters of
the combustion in ICE as a means to increase their energy
efficiency may simultaneously result in negative environ-
mental consequences (Fig. 4). Fig. 3 e Equilibrium NO2 concentrations in combustion
This phenomenon requires developing more efficient products (P ¼ 60 atm for carburetor ICE and P ¼ 80 atm for
methods for neutralizing combustion products in regard to all diesel ICE).
fuels under consideration.
According to International norms (CAS 10102-44-02) and
Russian National norms (GN 2.1.6.695e8), NO2 maximum
Results and discussion single concentration should not exceed the value of 0.085 mg/
m3 while its mean daily concentration should not be more
Nitrogen dioxide (NO2) related to the 2nd hazard class chem- than 0.04 mg/m3 [6,7,12,13]. However, numerous experiments
ical substances may be most dangerous for humans. carried out in recent years around the world demonstrate a

Table 3 e Equilibrium concentrations of NO2, NO, and NOx in combustion products, m3/m.3.
Characteristic Pressure, atm Hydrogen Ethanol Methanol Petroleum Diesel Methane
r*NO2 1 2.99E-06 2.71E-06 2.37E-06 3,023E-06 2.28E-06 2.33E-06
60 2.32E-05 2.1E-05 1.836E-05 2.346E-05 e 1.812E-05
80 e e e e 2.01E-05 e
r*NO 1 0.00156 0.00147 0.00136 0.00157 0.00136 0.00137
r*NOx 60 0.001563 0.00149 0.00138 0.00159 e 0.00139
80 e e e e 0.00138 e
 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 5 ( 2 0 2 0 ) 1 1 5 1 e1 1 5 7
Fig. 4 e Equilibrium concentrations of NOx in combustion
products (P ¼ 60 atm for carburetor ICE and P ¼ 80 atm for
diesel ICE).
significant excess of these levels [30e34] owing mainly to the
expansive growth of the vehicle fleet. The situation is espe-
cially alarming in megacities and countries having rapid
economic growth [35]. To reduce NOx concentration, the cat-
alytic and non-catalytic neutralization methods are being
developed. Thus, the Exon Research Engineering Company
has developed and patented the method for deoxidizing NO to
molecular nitrogen by adding ammonia or urea to exhaust
gases [36e41]. The way out of this situation may also lie
through increasing the development of electric transport, low-
temperature technologies for using fuel as well as measures
and administrative regulations to improve the use of vehicles
and industrial enterprises in centers of population [42,43]. The
experience of Canada wherein NO2 concentration in cities has
been reduced by more than twice due to a number of
administrative measures taken over the period from 1998 to
2013 [44] may be required of great interest in this regard.
It may be advisable to compare nitrogen oxide emissions
from different natural and synthetic fuels with allowance for
their different energy values and hence different amount of
the required oxidizer (air) in order to obtain an equal energy
efficiency (fuel consumption per 100 km).
Specific values for NO2 and NOx emissions calculated with
allowance for actual combustion values are given in Figs. 5
and 6.
Fig. 5 e Specific NO2 concentration in combustion products
(P ¼ 60 atm for carburetor ICE and P ¼ 80 atm for diesel
ICE).
1155
Fig. 6 e Specific NOx concentration in combustion products
(P ¼ 60 atm for carburetor ICE and P ¼ 80 atm for diesel
ICE).
It can be seen from the data provided in Figs. 5 and 6 that
methanol and methane may have the lowest emission level of
the most dangerous gas (NO2).
These results could be used in complex optimization of the
energy and ecological efficiency of modern and advanced ICE
in combination with other factors characterizing the effect of
thermodynamic parameters on the specific fuel consumption
and the formation of other anthropogenic combustion prod-
ucts [46].
However, lowering the fuel oxidation temperature may
become an efficient method for reducing nitrogen oxide
emissions. For example, using hydrogen as a fuel for electro-
chemical current generators may allow abandoning ICE in
vehicles as well as reducing nitrogen oxide emissions by more
than an order of magnitude. Thus, calculations carried out on
the basis of this method for a power plant with a high-
temperature electrochemical generator (to ¼ 1,058 K) using
hydrogen as a fuel and atmospheric air as an oxidizer [45]
have shown that total NOx concentration in combustion
products may be reduced by 32 times, as compared to ICE.
Conclusion
Modern high-temperature methods for using natural and
synthetic fuels as an oxidizer of atmospheric air inevitably
result in formation of substantial amount of various nitrogen
oxides.
The higher the concentration of N2 and O2 in fuel oxidation
products, the higher is that of NO and NO2 in exhaust gases.
For example, the concentration of nitrogen is 8.8% higher and
oxygen is 22% higher during petroleum oxidation as compared
to methanol oxidation, so the output of nitrogen oxide is 14%
higher and nitrogen dioxide is 21% higher than during meth-
anol oxidation.
An increase in pressure from 1 atm to 80 atm during diesel
fuel oxidation may increase NO2 concentration by 8.8 times
while the concentration of other fuels under consideration
has demonstrated 7.8 times increase with an increase in
pressure from 1 atm to 60 atm.
1156 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 5 ( 2 0 2 0 ) 1 1 5 1 e1 1 5 7

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