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1 Article

2 The Effect of Moisture Content on The Tar


3 Characteristic of Wood Pellet Feedstock in a
4 Downdraft Gasifier
5 Rizqi Fitri Naryanto 1,2*, Hiroshi Enomoto 1, Anh Vo Cong 1, Kazuki Fukadu 1, Zheng Zong 1,
6 Mera Kartika Delimayanti 3, Chuntima Chunti 4, and Reiji Noda 4
7 1 Division of Mechanical Science and Engineering, Graduate School of Natural Science and Technology,
8 Kanazawa University, Natural Science Research Building 3, Kakuma-machi, Kanazawa 920-1192, Ishikawa,
9 Japan; rizqi.fitri@stu.kanazawa-u.ac.jp; eno@se.kanazawa-u.ac.jp; voconganh@stu.kanazawa-u.ac.jp;
10 fukadu_k@stu.kanazawa-u.ac.jp; zongzheng1@stu.kanazawa-u.ac.jp
11 2 Department of Mechanical Engineering, Engineering Faculty, Universitas Negeri Semarang, Sekaran

12 Gunung Pati, Semarang 50229, Central Java, Indonesia; rizqi_fitri@mail.unnes.ac.id


13 3 Department of Computer and Informatics Engineering, Politeknik Negeri Jakarta, Depok 16425, Indonesia;

14 mera.kartika@tik.pnj.ac.id
15 4 Division of Environmental Engineering Science, Graduate School of Science and Technology, Gunma

16 University, Tenjin-cho, Kiryu-shi, Gunma 376-0011, Japan; t162c002@gunma-u.ac.jp; noda_r@gunma-


17 u.ac.jp
18 * Correspondence: rizqi.fitri@stu.kanazawa-u.ac.jp; rizqi_fitri@mail.unnes.ac.id

19 Received: date; Accepted: date; Published: date

20 Abstract: This study examined the tar characteristic of wood pellet using a downdraft gasifier
21 system. The wood pellet was used as a feedstock with a variation of moisture content between 2 to
22 6 wt%. Tar sample was taken using JP 2009-40885 method. Gas Chromatography-Mass
23 Spectrometry and Gravimetric analysis were used to identify and to analyze the tar sample,
24 respectively. The results show that the increase in moisture content slightly decreased the total
25 concentration of tar formation on the nine tar compounds of biomass. Additionally, the lowest
26 moisture content produced the highest light tar on tar classification due to the ease of ignition and
27 minimized the failure of the equipment. The lowest moisture content had the lowest tar density,
28 and this minimized the deposit of tar in the gasifier. Therefore, the lowest moisture content had low
29 tar production in the biomass gasification process using wood pellets.

30 Keywords: wood pellet, moisture content, tar formation, tar classification, tar density.
31

32 1. Introduction
33 The low availability and high demand of fossil fuel has led to an increase in its prices. Therefore,
34 biomass can be used to solve this issue. It might replace the demand for electricity, especially in the
35 village with limited access to power. It also can be used for other purposes, such as to drive internal
36 combustion engine or turbine engine. Gasification and combustion are the thermochemical
37 conversion that uses pressure, steam, and high temperature to change the biomass feedstock into gas
38 production called syngas/synthetic gas. The main component of syngas includes CO, N2, H2 and CO2,
39 and other hydrocarbons, such as CH4, C2H6 and C2H4, and tar compounds.
40 In thermochemical conversion such as biomass gasification has many advantages compared to
41 the combustion and pyrolysis process. This is because it has a lower tar production. In this research
42 the downdraft gasification system with 10 kW in a laboratory scale was used in this experiment. The
43 feedstock is divided into non-woody and woody feedstock. A non-woody feedstock has limitations,
44 such as producing higher ash, N2, and Sulphur content. However, the woody biomass is an organic

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45 material derived from a living organism that was used as fuel in energy generation Therefore wood
46 pellet is chosen since it is readily available and cheap. The particle size of feedstock affects the
47 gasification process. The proportional size particle of the wood pellet is below 6.3 mm and have a
48 mass fraction lower than 25 % [1,2]. According to Oveisi et.al, 12 % of steam can be generated easily
49 in case the moisture content is reduced from 35 % to 20 % on a wet basis (wb) [3]. For this reason, an
50 experiment was made in a 6 mm diameter of wood pellet feedstock with bulk density 790 kg/m3 and
51 moisture content variation in 2 wt%, 4 wt%, and 6 wt% respectively.
52 The composition of syngas yielded from the gasification process depends on the contents of
53 oxidizer such as oxygen in the air. Additionally, the amount of tar composition in syngas interferes
54 with the effectiveness of syngas [4,5]. Naryanto et al. stated that various chemical compounds existed
55 in tar formation and it had been affected by moisture content in the feedstock [6,7]. Tar can be defined
56 as oxygenated and hydrocarbon compounds in the combustible gas as good as Polycyclic Aromatic
57 Hydrocarbon (PAH) and higher than the molecular weight of benzene [8]. Three international
58 organizations agreed with this definition of tar, including the Energy Department of United States,
59 International Energy Agency (IEA), and The Directorate-General for Energy European Commission
60 (DG XVII) [9,10].
61 Tar is the unnecessary product in the biomass gasification since it makes the equipment
62 challenging to operate during combustion. The catalyst cannot overcome the tar problem for a long
63 operation in the biomass gasification[11]. For this reason, varying the moisture content of feedstock
64 must be done [12]. This variable affects tar characteristics such as tar formation, classification, and
65 density. Limited studies have examined the influence of moisture content on the tar characteristic.
66 Accordingly, this study aims to verify the effect of moisture content on the tar characteristic of the
67 wood pellet on the downdraft gasifier. The experiments were conducted with the variation of
68 moisture content of 2 wt%, 4 wt%, and 6 wt% with the fixed of air flow rate 80 L/min. The process
69 was used tar sampling method with patent number JP 2009-40885 from Japan Patent Office[13].

70 2. Materials and Methods

71 2.1. Wood Pellet Feedstock


72 In this experiment, the pellet from cedar wood was chosen because it contained higher lignin
73 than the other feedstock. It had around 25% lignin and served as a bonding agent for the production
74 of hydrocarbon [14]. The size of the wood pellet was approximately 12 mm length, 6 mm diameter,
75 and bulk density of 790 kg/m3, as shown in Figure 1 (a) (b). In this research, the initial moisture
76 content was around 7 wt% and was varied to 2 wt%, 4 wt%, and 6 wt%. In order to reduce it, drying
77 machine TTM-440N was used. Also, the Moisture Analyzer machine (AND MF-50) was used to
78 measure the wetness of wood pellet feedstock.
79

(a) (b)
80 Figure 1. (a) Length of wood pellet properties (b) Width of wood pellet properties
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81 Based on the Japan Industrial Standard (JIS), the Ultimate Analysis (UA) contain O, N, S, H, C
82 was shown in Table 1. Proximate Analysis (PA) as quantitative data of volatile matter, ash, fixed
83 carbon, and the low heating value was shown in Table 2.

84 Table 1. Ultimate Analysis (UA) of wood pellet

Ultimate analysis (wt%, dry ash-free) JIS M8813


O (balance) 43.37
N 0.09
S 0.09
H 6.43
C (dry, ash-free) 50.02

85 Table 2. Proximate Analysis (PA) of wood pellet

Proximate analysis (wt%, dry basis) JIS M8812


Volatile matter (dry base) 81.82
Ash 0.53
Fixed carbon 17.65
Low heating value (LHV) 15.37 MJ/kg-dry

86 2.2. Downdraft Gasifier System


87 This experiment utilized the downdraft gasifier in the gasification process to minimize tar
88 production. The Pellet Holder was used to fill the wood pellet on the feeder for the ignition in the
89 gasifier, which has a dimension of 120 mm inner diameter and 500 mm length. Moreover, the screw
90 for mixing the wood pellet was installed and made the temperature uniform. The air was used as an
91 oxidizer with a fixed air flow rate 80 L/min, and it was controlled by Gas Flow Rate Meter (Azbil
92 CMS200, made of Azbil Corporation, Japan). Additionally, the air supply was controlled by
93 Programmable Logic Control (PLC). The Soot remover was adopted to reduce the tar formation
94 because if the process only used the activated carbon as charcoal, it is not enough to minimize tar
95 production. The cooler with circulating water was used to reduce the temperature of syngas from the
96 gasifier. This syngas was processed by sucking in the suction pump before delivering it in the Buffer
97 tank. The process was continued by suction pump before delivering it in the Buffer tank. The
98 operating condition of these experiments included a uniform temperature between 400 – 600 oC.
99 Every data was saved in the data-logger product of National Instrument, USA. The yielded syngas
100 from the biomass gasification process was quantified for the tar compound using Gas
101 Chromatography (GCMS, Agilent, 490 Micro GC, TDC, Ar carrier). The block diagram of the biomass
102 gasification system is shown in Figure 2.

103
104 Figure 2. The biomass gasification system
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105 2.3. Tar Sampling


106 Some tar sampling methods improved in recent years are associated with the advantages and
107 disadvantages of the system [15]. The famous method for getting tar sampling was executed in the
108 liquid-cooled solvent method using isopropanol [16]. In this experiment, Tar sampling was carried
109 out between the gasifier and soot remover, and the sampling line was shielded from the gasifier at
110 250 oC to avoid many impurities, including ash, dust, and soot. The heating process was executed
111 before passing in the tar sampling bottle. Ethylene glycol was used as an antifreeze to keep cool the
112 tar in dewar vessel until -20 oC. The experiment equipment was shown in Figure 3. Three tar sampling
113 impinger bottles with 300 mm length and 24 mm inner diameter respectively were used to collect tar
114 in syngas through contact surface method with 30 ml of glass beads (AS ONE BZ-2, diameter 1.5-2.5
115 mm). The syngas flow rate was set to 8 L/min for 20 minutes and was intended to collect 160 L of
116 syngas from the tar sampling equipment. The collection process was based on the Standard of Tar
117 Sampling system conducted by tar protocol. The approach used was “Method and Apparatus for
118 Collecting Tar” with modification which had the patent number JP 2009-40885 in 2007 from Japan
119 Patent Office. It was developed by Hiroaki Ohara and Katsuaki Matsumura [13,17].
120 The tar in syngas was extracted using acetone with 99.5% purity in 50 ml through surface contact
121 with glass beads. Pure acetone was injected in the tar sampling bottle and was shucked at least fifteen
122 times to ensure the mixing of acetone and glass beads is homogenous. Filter (SIMPLEPURE, NY 0.45
123 µm) was used to remove the impurities such as soot, ash, and dust in the process extract tar sample.
124 All the tar sample was kept in the vial bottle 2 ml for the next analysis of the compounds using Gas
125 Chromatography-Mass Spectrometry (Shimadzu GC-MS QP2010 Plus). Finally, all of the apparatus
126 in tar sampling bottle was cleaned using fresh acetone and ultrasonic cleaning machine (AS ONE).
Gasifier Gas flow
Filter meter
Heated line Suction
(250oC) pump

Sampling bottle

Glass Glass Glass


Beads Beads Beads Dewar vessel

Ethylene glycol/water bath


(-20oC)
127
128 Figure 3. Tar Sampling Equipment

129 2.4. Test Procedure and Analysis of Tar Sampling


130 These experiments were conducted with the offline method by collecting the tar sample and
131 extracting it in an appropriate solvent for the next chemical analysis process. The process used
132 acetone with 99% purity as a solvent to liquefy the tar at the glass beads. Shimadzu GC-MS QP2010
133 Plus was used for analyzing the tar compound and for calibrating using standard reagent with 94%
134 to 99% purity. Nine chemical compounds of the tar were always found in every experiments as
135 follows: phenol, toluene, styrene, naphthalene, biphenyl, anthracene, indene, fluoranthene, and
136 pyrene, which were used as a tar standard on analyzing the sample. Tar sample in syngas was
137 quantified with the similarity index higher than 70 on Total Ion Chromatogram (TIC) peak level. The
138 result of tar compounds data yielded from GC-MS was analyzed deeply by GC Postrun software,
139 and the results are used to identify every compound separately. Another process was conducted to
140 measure the tar density by the Gravimetric method, which is a technique of using the number of ions
141 to analyze the density of compounds. In these experiments, the Dryer evaporated machine (IRIS
142 OHYAMA) and set the temperature at 65 oC were used to evaporate the acetone in the tar sample to
143 obtain the pure mass of tar compounds. Finally, the pure mass of tar compounds was quantified
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144 using a measurement machine of weight tar (Chyo JL-200) in high precision measurement balance in
145 sensitivity to 0.1 mg. Each Experiment equipment was shown in Figure 4 (a) (b) (c) below:

(a)

(b) (c)

146 Figure 4. (a) Shimadzu GC-MS QP2010 Plus (b) Dryer evaporated machine (IRIS OHYAMA) (c)
147 measurement machine of weight tar (Chyo JL-200)

148 3. Results and Discussion

149 3.1. Impact of Moisture Content on Tar Formation


150 The drying of biomass is required for thermal gasification to achieve higher efficiency. Drying
151 of the biomass is achieved by using solar energy or waste heat. Moreover, biomass is hygroscopic,
152 and therefore, even after it is dried, it can still absorb moisture from the atmosphere. Yang et al.
153 studied the effect of moisture content level in the fuel. The study established that a fixed air flow rate
154 and drier fuels have higher burning rates in comparison to wetter fuels [18]. When utilizing biomass
155 as fuel, its high moisture content affects tar formation on the syngas.
156 Even though tar problem is a primary concern lately, the terminology of tar is not well defined.
157 According to Maniatis et. al, different compounds with molecular weight more than 78 (benzene) can
158 be found and we defined as tar compounds [9,10]. The tar sample was quantified using gas
159 chromatography analysis and had focused on the nine tar compounds, including phenol (C6H5OH),
160 toluene (C7H8), indene (C9H8), naphthalene (C10H8), biphenyl (C12H10), fluorene (C13H10),
161 phenanthrene (C14H10), fluoranthene (C16H10) and pyrene (C16H10). This focused on the nine tar
162 compounds because all of them appeared in every experiment's results. Those nine tar compounds
163 was shown in Table 3.
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164 Table 3. The nine tar compounds in biomass

Compound Chemical Formula Molecular Weight Boiling Point


(g/mol) (oC)
Phenol C6H5OH 94.11 181.7
Toluene C7H8 92.14 110.6
Indene C9H8 116.16 181.6
Naphthalene C10H8 128.17 218
Biphenyl C12H10 154.21 255
Fluorene C13H10 166.22 295
Phenanthrene C14H10 178.23 336
Fluoranthene C16H10 202,26 375
Pyrene C16H10 202.25 404
165
166 All nine compounds were measured through tar concentration using the equation (1) shown
167 below:

168 = (1)

169 Where is a concentration of tar in syngas (g/Nm3), is the weight of tar in syngas (g), and
170 is the normal volume of syngas (Nm3). Additionally, the result of tar formation and concentration
171 with a variation of moisture content were calculated, and the results are shown in Figure 5.

172
173 Figure 5. Tar formation on airflow rate 80 L/min with variation moisture content 2 wt%, 4 wt%, and
174 6 wt%

175 Tar formation on airflow rate 80 L/min with 2 wt%, 4 wt%, and 6 wt% are shown in Figure 4.
176 The concentration in tar formation in descending order include phenol, naphthalene, phenanthrene,
177 fluorene, biphenyl, fluoranthene, pyrene, toluene, and indene. Phenol has the highest decreasing
178 value of tar concentration, as well as the increased moisture content. Phenol compound decreased in
179 tar concentration from 14.87 g/Nm3 in moisture content 2 wt% to 10.53 g/Nm3 in 6 wt%, including in
180 Heterocyclic Aromatic Compounds. Besides, the minority of the tar formation is toluene and indene,
181 which had declining concentration but rising moisture content. Toluene is a Light hydrocarbon
182 aromatic compounds (1 ring) which do not cause a problem in condensability and solubility. Indene
183 is Light polyaromatic hydrocarbon compounds (2–3 rings), which condense at low temperatures,
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184 even at very low concentrations. Toluene had a decreasing value of tar concentration from 1.60 g/Nm3
185 in moisture content 2 wt% to 0.20 g/Nm3 in 6 wt%. In Indene, the value decreased from 0.43 g/Nm3
186 in 2 wt% to 0.30 g/Nm3 in 6 wt%. The decreased value of the tar concentration for both toluene and
187 indene were attributed to wood pellet from lignin, cellulose, and hemicellulose, which contained
188 much oxygen.
189 The increasing moisture slightly decreased the tar concentration in the nine compounds.
190 Therefore, the result of this study is in line with Gautam et al., which stated that phenol, indene, and
191 toluene existed in the tar compounds from the biomass gasification process with the wood pellet as
192 the feedstock. Also, toluene and indene were found to be the majority due to the variation of the
193 biomass flow rate. However, this study showed that phenol was the majority with the variation of
194 the moisture content for the biomass gasification process [19].

195 3.2. Impact of Moisture Content on Tar Classification


196 A method for analysis of tar classification in syngas from biomass gasification has been actively
197 studied. The purpose of this analysis was to separate the tar classification into two categories,
198 including Light and Heavy tar. Light tar is mainly composed of "volatile and semi-volatile" aromatic
199 and phenolic compounds, while Heavy tar contains polar “non-volatile” compounds. Light tar may
200 pass through capillary gas chromatography (GC) column while the heavy tar might damage the
201 operation of the equipment. According to Zhang et al., the differentiation of tar classification based
202 on molecular weight can be determined by Gas Chromatography [20].
203 The biomass gasification generated syngas and tar, though the feedstock with higher moisture
204 content is difficult to ignite. Its gasification results is low gas yield and higher tar production. In the
205 downdraft gasifier, higher moisture content reduces the temperature of the reaction zone, leading to
206 the deposition of tar in the gasifier. In the experiment, tar was divided as Light and Heavy, which is
207 a phenol as the parameter of standard. In case the compounds have a molecular weight less than that
208 of phenol, they include light tar. Otherwise, in case the chemical compounds have molecular weight
209 more than phenol, they include heavy tar.
210 Figure 6 shows the formation of light and heavy tar in the biomass gasification process with
211 variation in moisture content. In Figure 6 (a), the tar formation on moisture content 2 wt% with air
212 flow rate 80 L/min shows different results. The tar concentration of light tar is 13.18 g/Nm3, which is
213 equal to 15.70% of total tar. The heavy tar has a concentration of 70.77 g/Nm3, which is equal to 84.30%
214 of the total in 83.95 g/Nm3. Figure 6 (b) shows the tar classification with a moisture content of 4 wt%
215 and light tar 2.81 g/Nm3, which is equal to 3.42%. The heavy tar is 79.41 g/Nm3, which is equal to
216 96.58% of the total concentration of 82.22 g/Nm3. Figure 6 (c) shows the same parameter with the
217 moisture content 6 wt%, where the concentration of light tar is 1.55 g/Nm3 or 2.16%, while heavy tar
218 is 70.32 g/Nm3 or 97.84% of the total 71.87 g/Nm3. This result shows that the production of light tar
219 decreased along with the increasing of moisture content while the heavy tar increased along with
220 increasing moisture content. This is the evidence that the lowest moisture content in 2 wt% is better
221 for the biomass gasification process due to yield less of heavy tar. More production of heavy tar leads
222 to extensive failure and plugging of the valve and reduces the performance of the biomass operating
223 system. The light tar was much easy to burnt compare to the heavy tar. This was due to the more
224 volatile chemical composition of light tar, such as hydrocarbon compounds.
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(a) (b)

(c)
225 Figure 6. (a) Tar formation on light and heavy tar in moisture content 2 wt% (b) Tar formation on
226 light and heavy tar in moisture content 4 wt% (c) Tar formation on light and heavy tar in moisture
227 content 6 wt%

228 3.3. Impact of Moisture Content on Tar Density


229 The study of tar protocol overcame the tar problem and included standardized methods for
230 sampling and analyzing it from the biomass gasification process. The tar protocol guideline
231 contributes to the alternatives of analyzing tar compounds and tar density. Gas chromatography use
232 to analyze tar compounds and this is widely implemented in studying the biomass gasification
233 process. Additionally, to analyze the tar density, the gravimetric method was used alongside the
234 distillation and evaporation processes [21,22]. The study utilized the distillation process to evaporate
235 the solvent with the specific boiling point. In this case, 3 grams mixture of tar sample and acetone
236 were heated for 5 hours at a temperature of 65 oC until all the acetone evaporated. The boiling point
237 of acetone is 56 oC allowed the separation of tar sample, and the entire acetone evaporated. The mass
238 pure tar residue remained and was defined as tar density.
239 The total amount of tar in the syngas was determined using equation (2) as follows:
240 = . (2)
241 Where the volume of tar in total amount syngas in is sampling (L), is the flow
242 rate of syngas in tar sampling (L/min) and is the sampling time of syngas (min),
243 The tar density in the syngas can be determined using equation (3):
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244 = 1000 (3)

245 Where is tar density in syngas (mg/m3), is a mass of tar in syngas in the sampling
246 (mg), and is the volume of tar in total amount syngas in the sampling (L).

247

248 Figure 7. Tar density on air flow rate 80 L/min with variation moisture content 2 wt%, 4 wt%, and 6
249 wt%

250 Figure 7 shows the result of gravimetric analysis for wood pellets in the biomass gasification
251 with a variation of moisture content. When the moisture content was 2 wt%, the tar density value
252 reached 1243.6 mg/m3. This value gradually increased when it was 4 wt%, and the tar density in
253 syngas was 1572.7 mg/m3. When the moisture content was 6 wt%, tar density reached 1600.8 mg/m3.
254 The moisture content increases proportionally, raising the tar density. This reduced the reaction zone
255 temperature in the gasifier, leading to the deposition of tar content. Additionally, the lowest moisture
256 content produces the lowest tar density. Contrary the higher value of tar density influenced and led
257 to the failure of the operation biomass gasification process.

258 4. Conclusions
259 The gasification process is significantly influenced tar characteristics. This study examined the
260 effect of moisture content on tar characteristics. In case the moisture content increased, the tar
261 concentration of the phenol compound decreased. The phenol is included in the heterocyclic aromatic
262 compound due to the wood pellet existed from lignin, cellulose, and hemicellulose, which contain
263 much oxygen. Moreover, the tar concentration of toluene and indene decreased. The increase in
264 moisture content resulted in heavy tar, which reduced the temperature of the reaction zone and led
265 to the deposition of tar in the gasifier. In consequence, the existence of heavy tar causes extensive
266 failure and plugging of the valve, reducing the performance of the biomass operating system.
267 Furthermore, the increase in moisture content initially increased the tar density, which led to the
268 failure of the gasification process. In contrast, the lowest moisture content produces lower tar density,
269 which is good for the gasification operating process.
270 Author Contributions: R.F.N. was responsible for the overall experiment, data analysis, arrangement, and
271 manuscript preparation. H.E. was primarily responsible for the data and manuscript confirmations. All authors
272 were equally responsible for finalizing the manuscript for submission

273 Funding: This research was funded by Indonesia Endowment Fund for Education (LPDP), grant number PRJ-
274 1621/LPDP.4/2019.

275 Acknowledgments: This work was supported by Indonesia Endowment Fund for Education (LPDP), Ministry
276 of Finance of Republic Indonesia (KEMENKEU) and Ministry of Research and Technology of Republic Indonesia
277 (KEMENRISTEK) and Ministry of Education and Culture of Republic Indonesia (KEMENDIKBUD) for the
Appl. Sci. 2020, 10, x FOR PEER REVIEW 10 of 11

278 scholarship and funding, and also Kanazawa University Japan and Gunma University Japan for the data
279 experiment and analyzing data.

280 Conflicts of Interest: The authors declare no conflict of interest.

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