Journal Pre-proofs

Improvement of coal boiler’s efficiency after application of liquid fuel addi-

tive

Robert Junga, Janusz Pospolita, Patrycja Niemiec, Maciej Dudek, Rafał

Szleper

PII: S1359-4311(20)33145-8
DOI: https://doi.org/10.1016/j.applthermaleng.2020.115663
Reference: ATE 115663

To appear in: Applied Thermal Engineering

Received Date: 4 March 2020

Revised Date: 2 June 2020
Accepted Date: 23 June 2020

Please cite this article as: R. Junga, J. Pospolita, P. Niemiec, M. Dudek, R. Szleper, Improvement of coal boiler’s
efficiency after application of liquid fuel additive, Applied Thermal Engineering (2020), doi: https://doi.org/
10.1016/j.applthermaleng.2020.115663

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Improvement of coal boiler’s efficiency after application
of liquid fuel additive

Robert Jungaa,∗, Janusz Pospolitaa , Patrycja Niemieca , Maciej Dudekb , Rafal

Szleperc
a Department of Thermal Engineering and Industrial Facilities, Opole University of
Technology. 5 Mikolajczyka St, 45-271 Opole, Poland
b RENERGI Sp. z.o.o. 17B/3 Koziorożca St, 80-299 Gdańsk, Poland
c Energetyka Cieplna Opolszczyzny ECO S.A. 15 Harcerska St, 45-118 Opole, Poland

Abstract

The aim of research is to provide a comprehensive view of the combustion

process of coal with a liquid fuel additive. The studies were carried out in lab-
oratory conditions and on low and high power boilers which are usually used
in households and local district heating plants. TGA/DSC analysis shows that
the additive decreases the ignition temperature of coal as well as increases the
maximal heat flow and its temperature. Application of the additive significantly
decreases oxygen O2 concentration, while maintaining the same flue gas tem-
perature. This affects the increase of efficiency of low power boiler by 2.49 p.p.
(percentage point). Emission of hydrocarbons, formaldehyde, benzene and hy-
drogen cyanide was lowered, whereas there was no significant impact on SO2
and NOx emission. The studies carried on the industrial boiler with thermal
output of 12 MW demonstrate that the flue gas heat loss and unburnt fuel heat
loss decreased by ca. 2 p.p. As a result, the efficiency increased from ca. 86 to
88% which, in turn, influences the decrease of CO2 emission per unit of energy
by 5%. The originality of the work is comprehensive research on the impact of
additive on the coal combustion process, mainly concerning the efficiency.
Keywords: fuel additives, coal combustion, thermogravimetry, boiler,
efficiency.

∗ Corresponding author. Tel.: +48 774498457; fax: +48 774499906

Email address: r.junga@po.opole.pl (Robert Junga)

Preprint submitted to Journal of LATEX Templates June 2, 2020

1 1. Introduction

2 Power industry and district heating in Poland are mostly based on bitumi-
3 nous coal [1]. At present, several power units with the power of 1000 MWe are
4 brought in exploitation. They fulfill all current emission standards and their
5 efficiency reaches the level of 92-94% [2]. This operation allows for the elimina-
6 tion of older units while maintaining safety in the power system. At the same
7 time, other high power boilers are being modernized in order to improve their
8 efficiency and reduce pollutants emissions. The activities in this field include:
9 the replacement of burners, modernization within the secondary air distribu-
10 tion system, OFA and SOFA nozzles [3], ROTAMIX [4], as well as the selective
11 catalytic reduction SCR system [5]. In addition to high power boilers exist-
12 ing in the power industry and district heating, there is a whole group of heat
13 sources with different powers occurring in the industry and numerous municipal
14 facilities. These are mainly fixed grate boilers and, with the power of 5 ÷ 10
15 MWt , moving grate boilers, which have a significant share in the consumption
16 of coal. In this group, a new generation of boilers is also introduced. They are
17 equipped with precise air distribution and automation systems, optimizing the
18 combustion process, therefore their efficiency is relatively high (85-89%). The
19 only limitation is the characteristic of the combustion process on the grate which
20 requires a greater excess of air, and it causes relatively high unburnt carbon heat
21 loss [6]. Despite changes in regulations in Poland and many incentives to use
22 other, alternative sources of energy, e.g. gas boilers and district heating, coal-
23 fired boilers will still dominate in the power industry and heating technology in
24 Poland for a long time.
25 Currently, low-rank coals with poor calorific values are also burnt. Their ash
26 causes fouling of heat surfaces and leads to slagging. Some alkali compounds
27 in ash have a very low melting point. Due to this fact, the ash can deposit on
28 clean superheater surfaces, initiating a gradual increase in the thickness and size
29 of deposit layers. Ash deposits, apart from other exploitation issues, decrease

2
30 boiler efficiency and increase fuel consumption [7]. Attempts to use coal addi-
31 tives to improve the quality of fuel have been undertaken with various success
32 for many years. The main purpose of such operations is to reduce the suscep-
33 tibility of ash particles to form conglomerates, as well as to decrease adhesive
34 properties of ash. In this way, the contamination of boilers heating surfaces
35 can be reduced [8]. There is also an indication that fuel additives can simplify
36 cleaning of boilers surfaces and reduce deposits that already exist. One of the
37 most known substances applied for this purpose in the polish power industry is
38 an oily suspension of copper oxychloride [9]. The aim of the application of other
39 additives is to reduce the emissions of sulfur and nitrogen compounds [10]. A
40 popular sorbent used in the flue gas desulfurization is calcium carbonate. Iron,
41 aluminium, calcium and silicon oxides additives were, in turn, found to decrease
42 NOx emissions and limit slagging within the boiler [11, 12], whereas glycerol was
43 found to increase combustion efficiency and reduce NOx emissions [13, 14].
44 An extended review of research into the influence of the additives on the
45 combustion of coal is presented in [15]. It puts forward a classification of ad-
46 ditives dividing them into organic and inorganic, as well as presenting further
47 systematics, subordinating chemical compounds to each group. The review of
48 methods, mainly in laboratory scale, were also provided. It can be concluded
49 that the studies concerned mainly high concentrations of additives, within a
50 few or a dozen or so percent. Therefore, the authors indicate lack of research of
51 additives at lower concentrations. Moreover, there are not many publications
52 regarding the influence of fuel additives on the effectiveness of the combustion
53 process and boilers efficiency. Daood et al. [11] showed the results of tests car-
54 ried out on both experimental set-up and commercial high-power boiler. The
55 additive used was a mixture of oxides (mainly of iron) whose amount was rela-
56 tively high (1.3 ÷ 13%) in relation to the fuel. After additive application, the
57 unburnt carbon heat loss was reduced by 19 ÷ 63%. In addition, short-term
58 studies conducted on the industrial boiler indicated that when the additve to
59 fuel ratio was fixed at 10%, the unburnt carbon heat loss decreased from 12
60 to 7%. It was also observed that boiler’s efficiency increased (by 2%) and the

3
61 emissions of NOx were reduced. Persson et al. [16] found that the addition of
62 magnesium oxide and magnesium hydroxide reduces the amount of unburnt car-
63 bon in ash by over 50%. However, no significant increase in the boiler’s efficiency
64 was noticed. As pointed out by the authors, the research time was too short
65 to observe reliable dependencies, therefore change in efficiency was negligible.
66 The positive role of magnesium compounds as the fuel additives components
67 was also discussed in the report of the European Commission [17].
68 To emphasize the impact of one of the commercial fuel additives on the
69 efficiency of the boiler, the authors carried out extensive research on a steam
70 boiler with a thermal output of 41 MWt [18]. The studies conducted in in-
71 dustrial conditions lasted about 2 months and they showed that the additive
72 increased boiler’s efficiency by 0.5 ÷ 1 p.p. (percentage point). These studies
73 were preceded by the tests in a laboratory scale which are the main subject of
74 this publication. The research was carried out in the field of thermogravimetric
75 analysis, as well as the combustion tests performed on boilers with significantly
76 lower thermal outputs, which are usually used in households and local district
77 heating plants.
78 Both the previously mentioned EC report [17] as well as the IEA Clean
79 Center report [19] indicate that there is a lack of commercially available additives
80 of confirmed effectiveness. It is still a challenge to search for new, effective fuel
81 additives, the use of which would bring tangible benefits in terms of improving
82 the energy and emission parameters of solid fuel boilers. The research on the
83 effectiveness of additives is mainly carried out in a micro-scale or on industrial
84 units. The studies on industrial boilers are time-consuming and expensive,
85 and the results are often burdened with disturbances related to the operation of
86 boilers. Therefore, it is important to develop a methodology that, in accordance
87 with sustainable development, will allow a reliable assessment of the additive
88 impact. Such methodology is put forward in the article including the results
89 obtained for the tested additive. The methodology consists of a gradual increase
90 of the research scale, from the tests on analytical devices, through low-power
91 boilers, and ending up on industrial units. This procedure avoids unnecessary

4
92 investments, and the effects are verified in a most possibly comprehensive way.
93 It was assumed that the low power boilers are the units with the power of ≤
94 200 kW which are mainly used in housing and public buildings. Regarding the
95 high power boilers, the authors assume boilers with the power of over 0.5 MW,
96 which can be mainly found in the industry.

97 2. Materials and methods

98 The aim of the research was to assess the influence of the fuel additive on
99 the combustion process of bituminous coal. The studies were divided into three
100 stages. During the first period of tests, research on combustion with and without
101 the fuel additive in the laboratory scale was carried out. For this purpose, the
102 STA (Simultaneous Thermal Analysis) technique was used, which allows the
103 measurement of mass changes TG (Thermogravimetric) and thermal effects DSC
104 (Differential Scanning Calorimetry) at the same time. The thermogravimetric
105 apparatus was the NETZSCH STA 449 F3 Jupiter.
106 The second stage consisted of combustion tests conducted on a water boiler
107 EKR (SIMAR) with thermal output of 10 kW. During this part of measure-
108 ments, the operation parameters were recorded, as well as the efficiency and
109 pollutants emissions.
110 In the third stage, the influence of the fuel additive on the coal combus-
111 tion in industrial conditions was checked. The studies were carried out on a
112 water boiler WR-10 with nominal thermal output of 11.6 MW. This stage also
113 comprised the assessment of operation parameters, efficiency, as well as the
114 concentration of pollutants in the flue gases. The fundamental conditions of
115 particular measurements are listed in Table 1.

5
 Table 1: The primary conditions and scope of particular measurements.

Subsection Experiment Fuel + additive A Aim

2.2 Labolatory conditions Coal - ignition and burn-out temperature

TGA/DSC Coal + A (0.1 l/kg) - thermal effects

- maximal mass loss rate and its temperature

2.3 Labolatory condtions Coal A0 (75% of nto*) - efficiency

Low power boiler Coal A0 + 5% A (74% of nto*) - pollutants emission

EKR 10 kW Coal A1 (86% of nto*)

6

Coal A1 + 5% A (87% of nto*)

Coal A2 (72% of nto*)

Coal A2 + 5% A (78% of nto*)

2.4 Industrial conditions Coal B0 (55% of nto*) - efficiency

Industrial boiler Coal B0 + A (1 l/t) (51% of nto*) - pollutants emission

WR-10 Coal B0 + A (1 l/t) (52% of nto*)

Coal B0 + A (1 l/t) (48% of nto*)

Coal B0 + A (1 l/t) (60% of nto*)

* nominal thermal output.

116 2.1. Characterization of the fuel additive

117 The applied additive was a 20% aqueous solution of four different com-
118 pounds. It contained manganese (II) acetate tetrahydrate, isopropanol, acetic
119 acid glacial ...% and N,N-Dimethylethanolamine. The first component was used
120 to increase the oxidizing abilities of fuel, therefore it should act as a catalyst
121 and reduce unburnt fuel heat loss. Isopropanol was used to prevent from ice
122 caps in dosing lines, whereas N,N-Dimethylethanolamine was found to prevent
123 from corrosion. Acetic acid glacial ...% was, in turn, added for experimental
124 purposes as the component which should remove deposits from boilers surfaces.
125 The detailed description about the content of each component, as well as the
126 possible mechanism of reactions, can be found elsewhere [18].

127 2.2. TGA/DSC experiments

128 Laboratory combustion tests TGA/DSC (Thermogravimetry and Differen-

129 tial Scanning Calorimetry) were performed in the NETZSCH STA 449 F3
130 Jupiter analyzer. The samples with the weight of 10 ± 0.1 mg were heated
131 in Al2 O3 crucibles with lids with holes from ambient temperature to 1000o C.
132 The heating rate β was 10o C/min and the air flow was fixed at 70 ml/min.
133 Before the analyzes, the apparatus was calibrated using indium, tin, bismuth,
134 zinc, aluminium and gold. Then a correction curve was prepared in order to
135 eliminate the influence of buoyancy effect. In addition, TGA/DSC analyses of
136 combustion of coal and coal mixed with the additive were repeated at least twice
137 to ensure the reproducibility of results.
138 Samples of coal with and without the additive were prepared similarly. 3 g
139 of coal were put into two dishes. Coal sample without the additive was poured
140 with 3 ml of water and precisely mixed, whereas the sample of coal with the
141 additive was mixed with 3 ml of a solution of the additive and water at the
142 ratio of 1:9. Then both samples were dried in a laboratory dryer for 24 h at the
143 temperature of 40o C and, after drying, closed in hermetic containers.

7
144 2.3. Low power boiler experiments
145 In the laboratory tests performed on low power boiler, three assortments of
146 coal were used and marked as A0, A1 and A2. A0 and A2 coals were preliminar-
147 ily sieved in order to obtain 5-6 mm grain size and after that, dried to air-dried
148 state. A1 coal was only dried in laboratory conditions.
149 Physico-chemical parameters of coals used in both low power and indus-
150 trial tests were established according to the standards listed in Table 2. This
151 table also shows the scope, measuring methods, as well as the uncertainty of
152 the parameters studied. The physico-chemical properties of A0 coal were es-
153 tablished in the accredited labolatory Zaklad Pomiarowo-Badawczy Energetyki
154 ENERGOPOMIAR Sp. z o.o., whereas the properties of A1 and A2 coals were
155 determined in Laboratorium Analiz Instrumentalnych w Energetyce i Ochronie
156 Środowiska at Opole University of Technology. The results obtained are pre-
157 sented in Table 3.

Table 2: The uncertainty of the parameters characterizing coal and combustion residues prop-

erties.

Parameter Test procedure/Standard Unit Uncertainty U (k = 2)

Moisture content PN80/G04511 % ± 0.6

Volatile matter content PN-G-04516:1998 % ± 0.8

Ash content PB01 from 8.04.2009 % ± 0.2

Carbon content PNG-04571:1998 % ±0.5

Hydrogen content PNG-04571:1998 % ± 0.3

Nitrogen content PNG-04571:1998 % ± 0.1

Sulfur content PNG-04584:2001 % ± 0.03

Lower heating value PNG-04513:1981 kJ/kg ± 226

Carbon content in the ash* PB02 outside the scope of accreditation % assumed: ± 0.1

* only in industrial boiler experiments.

158 The laboratory tests on EKR (SIMAR) boiler were carried out with the use

8
 Table 3: Physico-chemical properties of A0, A1 and A2 coals.

Parameter Unit A0 A1 A2

Moisture content %, a.d. 4.92 4.90 4.92

Volatile matter content %, d.b. 34.87 - 35.56

Ash content %, d.b. 7.70 7.36 6.51

Carbon content %, d.b. 74.40 78.99 83.54

Hydrogen content %, d.b. 4.64 4.79 4.92

Nitrogen content %, d.b. 1.59 1.85 1.87

Sulfur content %, d.b. 0.66 0.60 0.50

Lower heating value MJ/kg, a.d. 26.5 24-25* 25-26*

a.d. - air-dried, d.b. - dry basis, * - value declared by the manufacturer

159 of experimental set-up which scheme is presented in Fig. 1. The basic elements
160 are: boiler (1), central heating pipe system, hot water tank (2) with the capacity
161 of 1 m3 , circulation pump (3) with electronically controlled rotational speed,
162 three-way valve (4) with a regulator for controlling the valve actuator and air
163 cooled heat exchangers (5) up to 100 kW. The set-up also consists of heat
164 meter including a microprocessor heat converter (6), rotor flow transducer (F)
165 and resistance temperature sensors (To on the supply and Tr on the return).
166 Concentrations of gaseous pollutants were measured by means of measuring
167 tracks consisting of an exhaust gas conditioner (7) and analyzer (8). In the
168 experimental studies, two flue gas analyzers were used: PHOTON MADUR
169 and GASMET DX-4000.
170 The technical data of EKR (SIMAR) boiler are presented in Table 4. The
171 boiler tests were conducted in accordance with the requirements included in
172 EN:303-2/2012 standard [20]. The series of tests with and without the fuel
173 additive were carried out alternately, determining the influence of the additive
174 on the combustion of each assortment of coal. The additive dose was given in
175 the form of a solution sprayed on a fuel layer before pouring to the coal hopper.

9
 Figure 1: Experimental set-up for solid fuel combustion tests.

176 Apart from fundamental operation parameters of the EKR boiler, the NOx , SO2
177 and CO emissions were recorded.

Table 4: Data of the EKR (SIMAR) boiler.

Parameter Unit Value

Nominal thermal output kW 9.8

Supply water temperature oC 70

Return water temperature oC 60

Coal feed rate kg/h 1.71

Efficiency in nominal conditions % 88

Flue gas temperature oC 190

O2 vol.% d.g. 9.68

CO vol.% d.g. 689

NOx vol.% d.g. 387

SO2 vol.% d.g. 784

10
 Figure 2: Scheme of the WR-10 boiler.

178 2.4. Industrial boiler experiments

179 The studies of WR-10 moving grate boiler were conducted in the months of
180 January and February 2016 in the heating plant of Nowa Sól (Poland). The
181 aim of the research was to determine particular heat losses, efficiency, as well
182 as gaseous and dust emissions during combustion of coal with and without the
183 additive. The scheme of the WR-10 boiler is presented in Fig. 2, whereas Table
184 5 shows its nominal parameters.

11
 Table 5: Nominal parameters of the WR-10 boiler.

Parameter Unit Value

General data

Nominal thermal output MW 11.6

Inlet water pressure MPa 1.2

Inlet water temperature oC 70

Outlet water temperature oC 130

Boiler efficiency % 85
12

Flue gases data

Flue gas temperature oC 180

Flue gas volume flow m3 /h 31,010

O2 in the flue gas % 8.2

CO2 in the flue gas % 11.3

CO in the flue gas % 0.01519

Fuel characteristics

Fuel - Coal of 31.2 type

Lower heating value MJ/kg 20.0-24.0

Volatile matter content % ≥ 28

Ash content % < 20

Moisture content % < 12

Sulfur content % 0.6÷0.7

185 After inspection of the boiler and preliminary tests, 5 measuring series with
186 similar thermal loads and coal properties were carried out. Care was taken so
187 that the operating parameters of the boiler remained constant. The airflow was
188 kept stable and it was adjusted to the thermal load. The air distribution was
189 not changed as well.
190 At the end of January, it was decided to carry out the first three-hour mea-
191 suring series without the fuel additive. Subsequently, in the month of February,
192 four independent three-hour series of tests with the additive were performed.
193 Due to the failure, the first measuring series with the additive was shortened
194 to 2 hr and 20 min. The date of each test, thermal loads and their standard
195 deviations are provided in Table 6. It was also necessary to check the proper-
196 ties of coal and combustion residues. Therefore, the samples were collected and
197 analyzed in each series of tests. Coal samples were collected from the conveyor
198 belt, whereas combustion residues were colleted from the slag conveyor belt.

Table 6: The course of tests on the WR-10 boiler.

No. Series marking Additive Thermal load Standard deviation

1 1 No 6.41 MW 0.08 MW

2 2a Yes 5.98 MW 0.72 MW

3 3a Yes 6.03 MW 0.15 MW

4 4a Yes 5.53 MW 0.42 MW

5 5a Yes 7.03 MW 0.26 MW

199 In the experimental studies carried out on the WR-10 boiler, HORIBA PG
200 250A was used to determine the chemical composition and concentration of
201 gaseous pollutants in the flue gases. The automatic gravimetric dust meter
202 P-10 ZA with the Central Unit of Dust Meter CJP 10 were used to assess
203 the thermodynamic parameters, gas flow rate, as well as the concentrations of
204 particulate pollutants.

13
205 3. Results and discussion

206 3.1. TGA/DSC experiments

207 Figs. 3-4 show the TG/DTG and DSC curves, respectively. As can be
208 observed from DTG curves (first derivative of TG curve), the combustion process
209 of coal with and without the additive consists of two stages occuring in the
210 same temperature range. After evaporation of water, there is one prominent
211 peak accounting for sample burning. In spite of the fact that the combustion
212 of both samples is similar, some differences can be noticed. First of all, in the
213 combustion process of coal there is a gain in weight after evaporation of water
214 caused by chemisorption of oxygen [21]. When the additive is applied, sample
215 mass constantly decreases and no gain in weight can be observed. Moreover,
216 the sample mass that remains in the crucible after combustion is slightly lower
217 with the additive.
218 On the basis on the thermogravimetric results, some basic combustion pa-
219 rameters were determined and listed in Table 7. Due to faster weight loss in TG
220 curve, the sample with the additive has a slightly lower value of ignition temper-
221 ature Ti , determined according to the intersection method based on [22]. The
222 combustion process ends in the same temperature Tb for both samples, there-
223 fore the combustion time tb of coal with the additive is also slightly longer. The
224 DTG curve demonstrates that the maximal mass loss rate DT Gmax is greater
225 for the raw coal sample, and it occurs in lower temperature. However, the DSC
226 curve shows that the maximal heat flow increased by nearly 12% after additive
227 application. The area under the exothermic peak also increased which means
228 that the additive affects the amount of evolved heat from the fuel unit. The
229 combustion of the raw coal sample gives 18.3 kJ/g of heat, whereas with the
230 additive it increases to 20.0 kJ/g. Similar results with manganese compounds
231 in a small scale were observed by different researchers. He et al. [23] and Ma et
232 al. [24] stated that the addition of MnO2 clearly reduces the ignition tempera-
233 ture of coal. Moreover, the additive affected the amount of heat evolved during
234 combustion and it increased from 13561 to 13697 J/g [23].

14
Figure 3: TG/DTG curves.

Figure 4: DSC curves.

15
 Table 7: Basic combustion parameters obtained from TG/DSC analysis.

Parameter Name Unit Coal Coal + A

Ti Ignition temperature oC 398.0 390.0

Tb Burn-out temperature oC 605.0 605.0

tb Combustion time min 20.6 21.4

DT Gmax Maximal mass loss rate %/min -5.86 -5.70

TDT G Temperature of maximal mass loss rate oC 475.8 476.1

DSCmax Maximal heat flow mW/mg 17.07 19.08

TDSC Temperature of maximal heat flow oC 479.6 487.9

235 3.2. Low power boiler experiments

236 Table 8 shows the results of combustion studies of three coals, whose proper-
237 ties are given in Table 3. As can be observed, the main effect of the application of
238 the additive is the reduction of oxygen O2 concentration in the flue gases by 0.17,
239 0.86 and 2.49 p.p. in comparison to the A0, A1 and A2 coal tests, respectively.
240 In all experiments boiler control settings remained unchanged. The change in
241 combustion conditions after additive application caused that the amount of air
242 changed slightly, in consequence leading to change in flue gas volume flow QF G .
243 The consequence of changing combustion conditions was also the change in flue
244 gas composition, as well as flue gas temperature TF G . The decrease in oxygen
245 O2 concentration is proportional to the increase of CO2 concentration. The
246 increase of CO2 concentration influences, in turn, on the decrease of flue gas
247 heat loss Sf , and thus affects the efficiency ηk . The boiler efficiency, calculated
248 by the indirect method, was slightly improved after application of the additive.
249 However, it must be emphasized that the positive effect of the increase in ef-
250 ficiency ηk by 0.7, 0.5 and 2.2 p.p. in A0, A1 and A2 coals, respectively, was
251 observed in each series of tests. Greater effects of improving coal combustion
252 efficiency, i.e. 3.10-6.15%, were observed with the addition of 0.5% of waste
253 iron residue. However, these studies were conducted under strictly controlled

16
254 conditions in a laboratory scale drop tube furnace [25].
255 The efficiency was influenced by the flue gas heat loss Sf which is the func-
256 tion of the flue gas volume flow QF G , flue gas temperature TF G and flue gas
257 components as well. To achieve high boiler efficiency, it is desirable to reduce the
258 flue gas heat loss by lowering the flue gas temperature. Such effect was observed
259 only in A0 + A test. Regarding the A1 and A2 coal tests, the increase of the
260 flue gas temperature was observed after application of the additive. However,
261 this slight increase of TF G was compensated by the significant increase in CO2
262 concentration, which ultimately resulted in the increase of the boiler efficiency
263 ηk in each test.
264 The aim of the additive application is not only to increase the boiler’s ef-
265 ficiency but also to reduce the pollutants in the flue gases. During the tests,
266 no reduction of the SO2 concentration was found. The nitrogen oxides NOx
267 concentration was, in turn, slightly reduced but it can be stated that this de-
268 crease is within the measurement uncertainty limits. Particular attention should
269 be paid on the CO concentration which was increased after application of the
270 additive. This phenomenon resulted from oxygen O2 deficiency, which led to
271 the increased incomplete combustion heat loss. It needs to be highlighted that
272 regarding the boilers with the power of up to 100 kW, such devices are sensitive
273 to small changes in oxygen O2 concentration. The application of the additive
274 which interferes the optimal value of the excess air coefficient λ, requires a cor-
275 rection of the air supply to the combustion process. This is due to the fact that
276 the small working space of the combustion chamber is very sensitive to small
277 changes in the amount of air. Since the purpose of the research was to identify
278 the additive influence, therefore no attempts were made to correct the amount
279 of air. Nevertheless, the experiments performed clearly indicate the need to
280 optimize the amount of air when burning fuels with additives.

17
 Table 8: Results of combustion tests of A0, A1 and A2 coals with and without the additive.

Parameter Name A0 A0 + A A1 A1 + A A2 A2 + A

P Thermal output, kW 7.5 7.4 8.6 8.7 7.2 7.8

ηk Efficiency calculated by heat loss method (indirect method), % 86.7 87.4 85.1 85.6 84.3 86.5

TF G Flue gas temperature, o C 215 196 248 254 203 210

dp Flue gas pressure, Pa 7 5 8 8 8 8

QF G Flue gas volume flow, Nm3 /h 15.59 15.16 20.14 19.09 21.41 18.43

O2 Oxygen concentration, % 9.07 8.90 8.53 7.67 10.91 8.42

18

SO2 Sulfur dioxide concentration, mg/m3 599 539 718 743 - -

NOx Nitrogen oxides concentration, mg/m3 365 336 315 310 362 349

CO Carbon monoxide concentration, mg/m3 1443 2271 1732 1826 2826 3125

CO2 Carbon dioxide concentration, % 10.61 10.67 11.01 11.81 8.91 11.03

Sf Flue gas heat loss, % 12.5 11.3 13.9 13.4 14.0 11.7

Snc Unburnt fuel heat loss, % 0.80 1.27 0.97 1.02 1.71 1.74

λ Excess air coefficient 1.78 1.78 1.72 1.59 2.12 1.71

To Supply water temperature, o C 68 67 73 73 62 63

Tr Return water temperature, o C 61 59 59 59 50 50

mw Water flow rate, m3 /h 1.05 0.95 0.54 0.54 0.54 0.54

* it is heat loss due to: dry flue gas, evaporation of water formed due to hydrogen and hydrocarbons in the fuel, moisture content in the

fuel and moisture content in the air.

281 Regarding the emission of selected hydrocarbons, the emission of methane,
282 ethylene, propane, formaldehyde, benzene and hydrogen cyanide was reduced
283 on average by 17, 29, 25, 15, 16 and 5%, respectively. The effect of thermal
284 decomposition of flammable gases such as hydrocarbons can be explained by
285 their affinity to the oxidation to secondary products such as CO, CO2 and H2 O
286 in the gas phase. The degree of conversion of these compounds is dependent on
287 the temperature range.

Table 9: Concentration of volatile organic compounds during combustion of A0, A1 and A2

coals with and without the additive, mg/m3 at 10% O2 .

Parameter Name A0 A0 + A A1 A1 + A A2 A2 + A

CH4 Methane 27 23 42 32 17 15

C2 H4 Ethylene 10 7 22 16 10 7

C3 H8 Propane 0.47 0.36 0.87 0.71 0.76 0.48

CH2 O Formaldehyde 7 7 11 8 6 5

C6 H6 Benzene 28 23 57 42 23 22

HCN Hydrogen cyanide 300 300 411 387 285 258

288 3.3. Industrial boiler experiments

289 The results of tests carried out on WR-10 moving grate boiler are presented
290 in Table 10 and subsequent figures. Thermal load of the boiler was maintained
291 at the similar level, resulting from heat demand. However, little deviations
292 (Table 6) are unavoidable due to e.g. the operation of automatics of the boiler.
293 The lower heating value LHV of coal was variable during the measurements. It
294 fluctuated in the range of 22 545 kJ/kg (5a) and 25 027 kJ/kg (4a).
295 The efficiency ηk in the first series of tests (1 - without the additive) was at
296 the level of 86.05%. This value resulted from relatively high flue gas heat loss Sf
297 (7.23%) and unburnt fuel heat loss Snc (4.33%), which was a consequence of the
298 presence of combustible particles in the slag. The average value of the flue gas

19
299 heat loss Sf in January, when the additive was not applied, reached the value of
300 8.42%. Moreover, the average efficiency of the boiler in January, determined on
301 the basis of operating parameters and average properties of combustion residues,
302 was 84.98%.
303 In February, four series of measurements (2a, 3a, 4a, 5a) with the fuel ad-
304 ditive were carried out. The results are presented in Table 10 and in Figs.
305 5-7. These figures also contain the average values from January (without the
306 additive) and February (with the additive) for comparative purposes.

20
 Table 10: Average values of operating parameters of WR-10 boiler in five series of measurements performed in January and February.

Parameter Measurement series

1 2a 3a 4a 5a

Fuel feed rate Bp , kg/h 1 128.1 1 027.2 1 039.3 913.7 1 305.7

Lower heating value of fuel LHV , kJ/kg 23 495 23 298 24 003 25 027 22 545

Thermal output P , MW 6.405 5.983 6.029 5.526 7.032

Efficiency calculated by heat loss method (indirect method) ηk , % 86.05 89.35 89.27 88.29 85.68

Standard uncertainty u(ηk ) 3.07 2.37 2.30 2.46 2.96

21

Flue gas temperature TF G ,o C 122.5 116.9 123.9 124.6 131.7

O2 in the flue gas, % 10.18 7.41 7.03 7.67 9.94

PM in the flue gas at 6.0% O2 , mg/Nm3 92 40 48 133 60

SO2 in the flue gas at 6.0% O2 , mg/Nm3 1719 1934 1732 1462 1451

NOx in the flue gas at 6.0% O2 , mg/Nm3 334 338 357 276 382

CO in the flue gas at 6.0% O2 , mg/Nm3 252 43 17 358 82

CO2 in the flue gas, % 9.61 11.92 12.49 11.99 9.82

Flue gas volume flow QF G , m3 /h 18 387 13 144 12 999 11 089 17 833

Flue gas heat loss* Sf , % 7.23 5.58 5.46 5.25 6.74

Unburnt fuel heat loss (bottom and fly ash losses) Snc , % 4.33 2.59 2.93 3.82 5.31

Heat generated from the fuel unit Hf , kJ/kg 21 121 21 667 21 580 22 498 20 034

* it is heat loss due to: dry flue gas, evaporation of water formed due to hydrogen and hydrocarbons in the fuel,

moisture content in the fuel and moisture content in the air.

307 Fig. 5 shows the values of the flue gas heat loss Sf and unburnt fuel heat loss
308 Snc in particular series of tests, as well as the average values of Sf and Snc in
309 January and February. The average values of heat losses were determined based
310 on the indications of measuring instruments and periodic results of properties of
311 combustion residues. The average values from January provide additional infor-
312 mation on the heat loss reference level, because only one series of tests without
313 the additive was carried out. Regarding the series of tests performed with the
314 additive, the flue gas heat loss Sf was lower by ca. 2 p.p. in comparison to the
315 series of tests carried out in January (without the additive). This regularity is
316 also visible in the case of the average values of Sf determined for the months
317 of January and February. However, the results of series 5a aberrate from the
318 regularity and that could be caused by the operational problems occurring at
319 that time.
320 Similar results are obtained for the unburnt fuel heat loss Snc , which is
321 significantly lower during combustion with the additive. As before, series 5a
322 abberates from the results. The average values of Snc in February are lower
323 than in January by ca. 2 p.p. Higher degree of fuel burn-up brings about the
324 decrease of oxygen O2 concentration in the flue gases as well. This occurs when
325 comparing series 2a, 3a and 4a with the reference series 1, and the average values
326 for January and February. The average O2 concentration in the flue gases in
327 January was 8.89%, while in series 1 it was 10.18%. Regarding the tests with
328 the additive performed in February, the O2 concentration was 6.28% and in
329 particular series of tests (2a-5a), it reached the values of 7.41, 7.03, 7.67 and
330 9.94%, respectively.
331 The consequence of decrease in the heat losses is also higher boiler’s efficiency
332 ηk . The values of ηk are presented in Fig. 6. The efficiency ηk in the reference
333 series was 86.05% and the average efficiency in the series of tests carried out with
334 the additive was 88.15%, which gives an increase by ca. 2 p.p. Similar result
335 was shown in [11], i.e. net 2% improvement of combustion thermal efficiency
336 which was observed during combustion of coal with the additive on a pulverized
337 coal-fired boiler with maximum continuous rating steam generation of about

22
Figure 5: Flue gas heat loss Sf , unburnt fuel heat loss Snc and O2 concentration in the flue

gases.

Figure 6: Average efficiency ηk in January and February and in particular measurement series.

23
 Figure 7: W e1 and W e2 factors.

338 280 tons/h. The additives to oil, prepared based on organic solid were, in turn,
339 found to increase efficiency of a steam boiler with the power of 320 MW by
340 0.3-0.5% [26]. The difference of monthly averages is even greater as it reached
341 the value of 4 p.p. It is a very good result, especially considering still low CO
342 emissions. Higher degree of fuel burn-up and therefore generation of greater
343 amount of energy is also consistent with the DSC results (Fig. 4). This mainly
344 applies to area under the curves, as well as the the values of DSCmax and TDSC
345 parameters.
346 Combustion of coal with the fuel additive had also an influence on the CO2
347 emission factors. Their values, determined by measurements, are presented in
348 Fig. 7. Regarding the CO2 emission in relation to the fuel unit (W e1 [kg
349 CO2 /kg fuel]), the factor’s value is the higher, the greater is the carbon content
350 in the fuel and the better is the degree of fuel burn-up (lower unburnt fuel heat

24
351 loss Snc ). The W e1 factor can be determined as follows:

kg
W e1 = 1.96 · 10−2 · [CO2 ] · qF G , (1)
kg
352 where:
353 [CO2 ] is the carbon dioxide concentration, %,
354 qF G is the amount of flue gases in Nm3 /kg of fuel.
355 The values of W e1 factor differ insignificantly (except 5a series) and these
356 differences stem mainly from slight changes in coal properties and measurement
357 uncertainty. After rejecting 5a series, the relative difference between the average
358 value of W e1 factor in 2a, 3a, 4a series and reference series (1) is 3.05%.
359 More reliable is the CO2 emission factor in relation to the unit of energy
360 produced in the boiler (W e2 [kg CO2 /MJ]). Regarding the reference series,
361 it reached the value of 0.1065 kg CO2 /MJ, and in other series of tests it is
362 significantly lower. The average value of W e2 factor for the series of tests carried
363 out with the fuel additive is 0.0963 kg CO2 /MJ, which gives a decrease by
364 9.5% with regard to the reference series. After rejecting 5a series during which
365 disruptions occured, the relative decrease of W e2 factor is still high (8.5%).
366 Remembering that

W e1
W e2 = , (2)
LHV · ηk
367 and subtracting previously indicated value (3.05%) related to the changes
368 of fuel properties and measurement uncertainty, the relative decrease of W e2
369 factor is still lower by over 5% when burning with the fuel additive. It means
370 that the CO2 emission per unit of heat is also by 5% lower. Moreover, no
371 evident influence on the flue gas temperature TF G , SO2 and NOx concentration
372 was found during combustion with the additive.

373 4. Conclusions

374 The studies carried out with the use of TGA/DSC technique showed that the
375 combustion with and without the additive is similar but there are few prominent

25
376 differences. First of all, the additive affects the ignition temperature Ti which
377 is lower by ca. 10 o C. There is also no gain in weight after evaporation of water
378 which is identified with chemisorption of oxygen. The DSC curves demonstrate
379 that the additive has a positive influence on the amount of heat evolved from
380 the fuel unit. It is evident that the additive increases the maximal heat flow and
381 the temperature of its occurrence. Moreover, sample mass after combustion is
382 slightly lower when the additive is applied.
383 The research carried out on a low power boiler showed that the additive
384 influences the oxygen O2 concentration in the flue gases which decreased in the
385 range of 0.17 ÷ 2.49 p.p. (percentage point). On the other hand, the CO2
386 concentration increased. This was associated with the reduction of the flue gas
387 heat loss and a slight increase in boilers efficiency. In the analyzed series of
388 tests, this increase was in the range of 0.7 ÷ 2.2 p.p. Moreover, no changes in
389 the emission levels of SO2 and NOx were found. Nevertheless, the increase in
390 CO concentration was observed and it may result from comprehensive changes
391 in the combustion process and better use of the oxidant. What is more, there
392 was a prominent decrease in the concentration of hydrocarbons, formaldehyde,
393 benzene and hydrogen cyanide as a result of the additive application.
394 Regarding the studies carried out on the industrial boiler WR-10, the addi-
395 tive decreased the flue gas heat loss Sf and unburnt fuel heat loss Snc by ca. 2
396 p.p. As a consequence, the efficiency ηk increased from 86.05% to 88.15%. The
397 difference is even higher when one compares the monthly averages from January
398 (without the additive) and February (with the additive). Then the difference
399 increases to approximately 4 p.p. The increase of efficiency ηk contributes not
400 only to fuel savings. It also decreases CO2 emission per unit of energy by 5%.

401 Acknowledgements

402 The authors are grateful to Innovation Norway for the financial support of
403 the research.

26
 Nomenclature
Bp Fuel feed rate, kg/h
DT G Derivative Thermogravimetric
LHV Lower heating value, MJ/kg
OF A Over Fire Air
P Thermal output, kW or MW
QF G Flue gas volume flow, m3 /h or Nm3 /h
SCR Selective Catalytic Reduction
Sf Flue gas heat loss, %
Snc Unburnt fuel heat loss, %
SOF A Super Over Fire Air
ST A Simultaneous Thermal Analysis
Tb Burn-out temperature, o C
TF G Flue gas temperature, o C
T GA/DSC Thermogravimetric and Differential Scanning Calorimetry
Ti Ignition temperature, o C
To Supply water temperature, o C
Tr Return water temperature, o C
W e1 CO2 emission in relation to fuel unit, kg/kg
W e2 CO2 emission in relation to unit of energy, kg/MJ

β heating rate, o C/min

ηk efficiency calculated by indirect method, %
λ excess air coefficient
mw Water flow rate, m3 /h
p.p. percentage point
qF G Amount of flue gases, Nm3 /kg of fuel
tb Combustion time, min

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 complex research of the fuel additive with the use of TGA/DSC and two coal boilers
 additive changes the characteristic parameters of coal
 application of the additive decreases oxygen concentration
 efficiency of low power boiler increased by 2.49 percentage point
 efficiency of industrial power boiler increased by 2 percentage point
Declaration of interests

☒ 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.

☐The authors declare the following financial interests/personal relationships which may be considered
as potential competing interests: