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Journal Pre-proof Thermochemical conversion of coal and biomass blends in a top-lit updraft fixed bed reactor: experimental assessment of the ignition front propagation velocity D.A. Quintero-Coronel, Y.A. Lenis-Rodas, L.A. Corredor, P. Perreault, A. Gonzalez- Quiroga PII: S0360-5442(20)32809-7 DOI: https://doi.org/10.1016/j.energy.2020.119702 Reference: EGY 119702 To appear in: Energy Received Date: 22 June 2020 Revised Date: 21 November 2020 Accepted Date: 22 December 2020 Please cite this article as: Quintero-Coronel DA, Lenis-Rodas YA, Corredor LA, Perreault P, Gonzalez- Quiroga A, Thermochemical conversion of coal and biomass blends in a top-lit updraft fixed bed reactor: experimental assessment of the ignition front propagation velocity, Energy, https://doi.org/10.1016/ j.energy.2020.119702. This is a PDF file of an article that has undergone enhancements after acceptance, such as the addition of a cover page and metadata, and formatting for readability, but it is not yet the definitive version of record. This version will undergo additional copyediting, typesetting and review before it is published in its final form, but we are providing this version to give early visibility of the article. Please note that, during the production process, errors may be discovered which could affect the content, and all legal disclaimers that apply to the journal pertain. © 2020 Elsevier Ltd. All rights reserved.

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Page 1: Thermochemical conversion of coal and biomass blends in a

Journal Pre-proof

Thermochemical conversion of coal and biomass blends in a top-lit updraft fixed bedreactor: experimental assessment of the ignition front propagation velocity

D.A. Quintero-Coronel, Y.A. Lenis-Rodas, L.A. Corredor, P. Perreault, A. Gonzalez-Quiroga

PII: S0360-5442(20)32809-7

DOI: https://doi.org/10.1016/j.energy.2020.119702

Reference: EGY 119702

To appear in: Energy

Received Date: 22 June 2020

Revised Date: 21 November 2020

Accepted Date: 22 December 2020

Please cite this article as: Quintero-Coronel DA, Lenis-Rodas YA, Corredor LA, Perreault P, Gonzalez-Quiroga A, Thermochemical conversion of coal and biomass blends in a top-lit updraft fixed bed reactor:experimental assessment of the ignition front propagation velocity, Energy, https://doi.org/10.1016/j.energy.2020.119702.

This is a PDF file of an article that has undergone enhancements after acceptance, such as the additionof a cover page and metadata, and formatting for readability, but it is not yet the definitive version ofrecord. This version will undergo additional copyediting, typesetting and review before it is publishedin its final form, but we are providing this version to give early visibility of the article. Please note that,during the production process, errors may be discovered which could affect the content, and all legaldisclaimers that apply to the journal pertain.

© 2020 Elsevier Ltd. All rights reserved.

Page 2: Thermochemical conversion of coal and biomass blends in a

Credit Author Statement

Quintero-Coronel D A: Methodology, Validation, Investigation, Writing - Original Draft. Lenis-Rodas Y A: Methodology, Validation, Investigation, Writing - Original Draft. Corredor L A: Conceptualization, Supervision, Funding acquisition. Perreault, P: Conceptualization, Writing - Review & Editing. Gonzalez-Quiroga A1: Conceptualization, Writing - Review & Editing, Supervision.

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Thermochemical conversion of coal and biomass blends in a top-lit updraft fixed bed

reactor: experimental assessment of the ignition front propagation velocity

Quintero-Coronel D A1,2, Lenis-Rodas Y A1,3, Corredor L A1, Perreault, P4, Gonzalez-Quiroga A1*

1UREMA Research Unit, Department of Mechanical Engineering, Universidad del Norte,

Barranquilla, Colombia

2GITYD Research Unit, Department of Mechanical Engineering, Universidad Francisco de Paula

Santander, Ocaña, Colombia

3Department of Mechanical Engineering, Institución Universitaria Pascual Bravo, Medellin,

Colombia

4Sustainable Energy, Air and Water Technology (DuEL) Group, University of Antwerp, Antwerp,

Belgium

Corresponding author*: [email protected]

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Thermochemical conversion of coal and biomass blends in a top-lit updraft fixed bed

reactor: experimental assessment of the ignition front propagation velocity

Abstract

Co-thermochemical conversion of coal and biomass can potentially decrease the use of fossil

carbon and pollutant emissions. This work presents experimental results for the so-called top-lit

updraft fixed bed reactor, in which the ignition front starts at the top and propagates downward

while the gas product flows upwards. The study focuses on the ignition front propagation velocity

for the co-thermochemical conversion of palm kernel shell and high-volatile bituminous coal.

Within the range of assessed air superficial velocities, the process occurred under gasification and

near stoichiometric conditions. Under gasification conditions increasing coal particle size from 7.1

to 22 mm decreased ignition front velocity by around 26% regardless of the coal volume

percentage. Furthermore, increasing coal volume percentage and decreasing coal particle size result

in product gas with higher energy content. For the operation near stoichiometric conditions,

increasing coal volume percentage from 10 to 30% negatively affected the ignition front velocity

directly proportional to its particle size. Additional experiments confirmed a linear dependence of

ignition front velocity on air superficial velocity. Further steps in the development of the top-lit

updraft technology are implementing continuous solids feeding and variable cross-sectional area

and optimizing coal particle size distribution.

Keywords: TLUD, combustion, gasification, front propagation, syngas, burning rate

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1. Introduction

Fixed bed reactors for solid fuel gasification and combustion are widespread at the laboratory and

industrial scales [1], [2]. Typically, the ignition front establishes near the bottom, and the product

gas flows either upward or downward. This work focuses on the top-lit updraft (TLUD) fixed bed

reactor in which the ignition front starts at the top and then propagates downward. The product gas

flows upwards through the bed of char and ashes left behind by the ignition front. Improved

cookstoves take advantage of the TLUD operation mode to separate gasification from the

combustion of the product gas with secondary air [3], [4]. TLUD cookstoves feature lower specific

fuel consumption and use a wide variety of millimeter-to-centimeter-size biomass particles. Grate

furnaces for (co-)combustion of biomass, coal, and solid waste also take advantage of the TLUD

configuration. In a grate furnace, a moving or vibrating grate transports the solids, primary air

enters from below, and combustion with secondary air occurs on top of the bed [5]–[7]. Here we

assess the ignition front propagation velocity for the co-thermochemical conversion of palm kernel

shell (PKS) and high-volatile bituminous coal (HVBC) in a TLUD fixed bed reactor.

The TLUD operation mode is also referred to in the literature as an inverted downdraft [8]–[10],

reverse downdraft [11]–[13], and reverse combustion [14]. However, in an actual downdraft, the

solids move downward towards the ignition zone. On the other hand, in the TLUD configuration,

the ignition front propagates downward through a static solids bed. The TLUD concept dates as

early as the 1980s when its capabilities as an improved biomass cookstove started to be explored

[15]. Most of the published research on TLUD concentrates on the development of improved

biomass cookstoves [3], [16]–[19]. Other TLUD-related applications are biochar [20], syngas [21]–

[24], and combined biochar-syngas production [9], [25], [26]. Likewise, bench-scale experiments in

TLUD fixed bed reactors provide fundamental data for the design and operation of grate furnace

combustors for solid waste [7], [27], [28] and biomass [5], [29].

The thermochemical conversion of PKS-HVBC blends in a TLUD fixed bed reactor remains

unreported according to the best of the authors’ knowledge. Coal is a conventional raw material for

thermochemical conversion because of its abundant reserves. However, coal is of fossil origin,

emits significant amounts of pollutants such as H2S, SOx, and NOx, and its reactivity is relatively

low. Biomass, on the other hand, is a renewable feed of relatively high reactivity. Nevertheless,

biomass is less available than coal and shows seasonal variation. Processing coal-biomass blends

allows overcoming, at least partially, the abovementioned disadvantages [30], [31].

Thermogravimetric analysis (TGA) of PKS-coal blends revealed enhancement of the thermal

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degradation kinetics [32]–[34]. PKS-coal co-gasification in a bubbling fluidized bed showed

positive results in improved bed uniformity, syngas yield, and syngas energy content [35], [36].

Two main operation regimes for TLUD fixed bed reactors are distinguishable from a plot of the

ignition front velocity vs. air superficial velocity [13], [14]. First, the gasification regime with

oxidization reactions in the gas and char reduction reactions in the solid phase. In the gasification

regime, the solid phase temperature is lower than the gas phase temperature, and a diffusion-

controlled flaming combustion model reproduces experimental observations [13]. Increasing air

superficial velocity leads to the char oxidation regime in which char and gas-phase oxidation

reactions simultaneously occur. In the char oxidation regime, the temperature difference between

the solid and gas phases decreases due to the simultaneous oxidation of volatiles and char.

Additionally, the ignition front propagation velocity appears to follow a universal trend irrespective

of biomass type, consistent with a diffusion-limited process [13].

The assessment of the ignition front propagation velocity reveals the performance and operational

stability of TLUD gasifiers and combustors. The TLUD device incorporates several thermocouples

at different axial locations to record the sudden temperature increase due to the downward

propagation of the ignition front. Measuring ignition front propagation velocity is a practical way of

assessing the influence of several factors on the performance of TLUD gasifiers and combustors.

Such factors include superficial velocity, feedstock type, particle size, moisture content, particle

size, reactor geometry, among others [13], [37], [38]. The ignition front propagation velocity, the

elemental composition of the feedstock, bulk density, and cross-sectional area allow calculating the

equivalence ratio, which gives a first indication of the operating regime. The equivalence ratio, peak

temperatures, and elemental compositions are the input for gasification models, which give a

preliminary indication of syngas composition.[10], [14], [39], [40].

The TLUD fixed bed reactor could generate syngas with potential for thermal and electric power

generation [21]–[23]. The char oxidation regime is also attractive because the fuel converts entirely,

and heat losses are minor. Thus, the ignition front propagation velocity emerges as a critical

parameter for the operation and control of TLUD gasifiers and combustors. Additionally, bench-

scale TLUD experiments provide fundamental data to validate more elaborated numerical models

and the design, operation, and optimization of grate furnaces. Nevertheless, the lack of experimental

information on the ignition front propagation velocity hinders TLUD-based biomass-coal co-

conversion technologies. This experimental work contributes to closing that gap by assessing the

effects of the air superficial velocity, coal particle size, and coal volume percentage on the ignition

front propagation velocity.

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2. Experimental procedures

This section describes the type of feedstock, the experimental setup, and the operational procedures

and conditions.

2.1 Feedstock

This study uses PKS, one of the main byproducts of the palm oil industry. The particle size of PKS,

according to sieve analysis, amounted to 4.9 ± 2.3 mm (mean and standard deviation) [41]. The

relatively high energy content and particle density make PKS very attractive for gasification. PKS

was co-processed with HVBC in the sieve fractions 4.7-9.5 mm, 9.5-12.7 mm, and 19.1-25.4 mm

[42]. The moisture contents of the air-dried PKS and HVBC amounted to 6.0 and 10 wt. %,

respectively.

2.2 Experimental setup

Figure 1 shows a schematic illustration of the experimental setup. The TLUD fixed bed reactor

consists of a cylindrical tube with an internal diameter of 152.4 mm and a height of 900 mm. A

fiberglass thermal insulation layer 25 mm thick surrounds the metallic tube. A 600 W blower

(model STPT600-B3, Stanley) feeds ambient air into the gasifier via a 63.5 mm internal diameter

pipe. Before entering the gasifier, air passes through a manual control valve and an air velocity flow

sensor (model 8455, TSI). Four K-type thermocouples with a sensitivity of 41 µV/°C and a

measuring range of -200-1350 °C measured the solids bed temperature. The tip reached the center

of the bed, as illustrated in Figure 1. The setup includes a data acquisition system (model USB 6341

BNC Pinout, National Instruments) acting as an interface between measurements and a computer.

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Figure 1 Schematic representation of the top-lit updraft (TLUD) fixed bed reactor setup.

2.3 Experimental conditions

This study uses PKS, a byproduct of the palm oil industry, taken from the same lot used by

Verdeza-Villalobos et al. [41]. The HVBC comes from Norte de Santander state (Colombia), where

the ceramic industry uses this type of coal for heating purposes.

The ignition front propagation velocity, ��, is given by Equation 1. Here ∆� represents the distance

between consecutive thermocouples and �� the time required by thermocouple � (corresponding to

��) to reach 500 °C.

��

∆�

��� � ��

Eq. 1

The experimental variables were air superficial velocity �, coal particle size ��� (taken as the

average from the upper and lower sieve sizes) and coal volume percentage ���. Table 1 summarizes

the operating conditions for the initial set of duplicated experiments. The total mass for the lower

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and higher ��� levels amounted to 3.65 kg and 4.03 kg, respectively. Likewise, the respective mass

percentages of coal for the lower and higher ��� levels were 15% and 40%. Previous experiments

with PKS in a similar TLUD setup served as a reference to define the � levels [43].

Table 1 Experimental conditions for the initial set of duplicated experiments, where � represents

air superficial velocity, ��� carbon mean particle size, and ��� carbon volume percentage.

Experiment ��, m s-1 ���, mm ���, % v/v 1-1 0.18 7.1 10 1-2 0.18 7.1 30 1-3 0.18 22.2 10 1-4 0.18 22.2 30 1-5 0.46 7.1 10 1-6 0.46 7.1 30 1-7 0.46 22.2 10 1-8 0.46 22.2 30

Table 2 summarizes the conditions for the second set of experiments, which further evaluated the

influence of � and ��� on ��.

Table 2. Experimental conditions of the second set of experiments. Experiments 2-1 and 2-3 were

single runs.

Experiment ��, m s-1 ���, mm ���, % v/v 2-1 0.18 11.1 20 2-2 0.32 11.1 20 2-3 0.46 11.1 20

Note that HVBC in the particle size range 4.7-9.5 mm contains particles slightly coarser than PKS

particles. The HVBC particle size approximately resembles biomass particles transported directly

from the palm oil mill. This selection bases on the hypothesis that relatively uniform particle size

can potentially enhance thermal conversion and decrease pressure drop [44].

On the other hand, the recommended particle size for fixed bed gasifiers amounts to 1/10 of the

inner diameter [45]. The recommended maximum particle size for our TLUD gasifier amounts to

around 15 mm, i.e., this work reports experiments with coal particles that fall within that limit and

coal exceeding such a limit. Using coarser material entails lower energy consumption in coal size

reduction. The purpose here is to gain insight into the TLUD fixed bed reactor performance under

those conditions.

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2.4 Setup operation

A typical experiment started by filling the chamber with a PKS-HVBC blend reaching a fuel

column of around 440 mm height. Graduated cylindrical tubes served to measure the corresponding

PKS and HVBC volumes. The PKS-HVBC blend was shaken for two minutes in a third container

and then mixed and transferred manually to the reactor. Introducing the thermocouples sequentially

as the solids level rose helped to avoid the formation of empty pockets. Subsequently, � increased

gradually until reaching the set point. The data acquisition process started once � stabilizes.

Finally, a layer of particulate solids soaked in mineral diesel was added at the top and then ignited

with a torch lit.

3. Results and discussion

This section starts with the composition of the feedstock in terms of their proximate and ultimate

analyses. Next, we present the temperature profiles and the reference temperature for calculating ��.

Then we discuss the results for each set of experiments separately, focusing on the ignition front

velocity and the equivalence ratio. The section finalizes with an outlook with further steps in the

development of the TLUD technology.

3.1 Feedstocks composition

This study used PKS from the same lot evaluated by Verdeza-Villalobos et al. [41], so proximate

and ultimate analysis in Table 3 coincide with those in that study. Our proximate analysis indicates

that the coal used here classifies as high volatile bituminous coal, according to ASTM D388-12.

This result agrees with the origin of the sample, Norte de Santander state (Colombia), which

produces this type of coal. Table 3 shows the ultimate analysis for high volatile bituminous coal

from that state. Akkaya [46] used nonlinear parametric regression and artificial neural network

models to predict elemental composition from proximate analysis with a correlation coefficient of

0.9896 for carbon (C). Akkaya's model predicts a C content 11.7% lower than that reported in Table

3.

Table 3 shows that the most salient differences between PKS and HVBC stem from their carbon (C)

and oxygen (O) contents. HVBC has around 1.4 times more C than PKS, but its O content is less

than half than that of PKS. HVBC contains more sulfur (S) and almost no nitrogen (N) when

compared to PKS. However, S and N together represent less than two percent on a dry-ash-free

basis (dafb) for PKS and HVBC.

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On a dry basis, HVBC contains around three times more fixed carbon (FC) than PKS, but its

volatile matter (VM) content is less than half than that of PKS. FC relates to the yield of char

produced during the devolatilization process. FC is mostly carbon but contains minor quantities of

H, O, N, and S, which do not drive off with the gases. FC is the combustible residue left after VM

distills off. A feedstock with high VM content ignites easily and is highly reactive in combustion

applications. The VM content is naturally high for many biomasses; however, its contribution to the

higher heating value (HHV) is relatively low due to its high O content. Finally, HVBC contains

more than five times ash compared with PKS. Ash could melt and agglomerate, which exacerbates

air channeling and can ultimately block the passage of gases.

Table 3 Elemental composition on a dry-ash-free basis (dafb), proximate analysis on a dry basis

(db), and higher heating value (HHV) of the feedstock. VM represents volatile matter, and FC fixed

carbon.

Analysis/parameter Palm kernel shell, PKS

High volatile bituminous coal, HVBC

C, % wt dafb 53.8 74.6c H, % wt dafb 6.13 6.07c N, % wt dafb 0.88 0.05c S, % wt dafb 0.11 1.91c O, % wt dafb 39.0 17.4c Molar H/C ratio 1.36 0.97 Molar O/C ratio 0.54 0.18 VM, % wt db 81.6 29.3 FC, % wt db 14.6 51.7 Ash, % wt db 3.78 19.0 HHV, kJ/kg db 21073a 25781b

aGaur and Reed correlation [47], bMason and Ghandi correlation [48], cUltimate analyses from [42]

3.2 Temperature profiles

Figure 2 shows how temperature varies with time at each thermocouple location during a typical

experiment. The ignition front propagation results in a sudden temperature increase reaching

maximum values of around 1000 °C. The calculation of �� via Equation 1 is sensitive to differences

in both the slope of the � vs. � curve and the time interval ���-�� (corresponding to ��� and ��).

Figure 2 indicates that temperature in the range of 300-600 °C could serve as a reference to

calculate ��. Previous studies used 300 °C [49], 400 °C [21], 500 °C [50], and 700 °C [51] as the

reference temperature.

Linear regression of the observed � vs. �� profile in the temperature range 300-600 °C data showed

correlation coefficients higher than 0.96 for all experimental runs. Figure 3 shows �� for 500 °C

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and � values from the linear regression models. Similar calculations for 300 °C and 600 °C showed

a maximum relative difference of 5.71% to 300 °C and 4.21% to 600 °C with that for 500 °C.

Hence, from now on, we use 500 °C as the reference for calculating ��.

Figure 2 A) Typical temperature profiles for the top-lit updraft thermal co-processing of palm

kernel shell (PKS) and high-volatile bituminous coal (HVBC). B) Close view of the temperature

profile T1. � represents temperature, � time, and � superficial velocity.

3.3 Results for the initial set of experiments

Table S1 in the Supplementary Material shows the analysis of variance (ANOVA) for the average

�� from the first set of experiments. The ANOVA indicates that �, ��� and their interaction are the

most significant factors. The Durbin-Watson statistic is 2.56 and the corresponding ����� and

�!��� for a significant level of 0.05 were 0.86 and 1.76. The Durbin-Watson statistic falls outside

the ����� � �!��� range, i.e., there is no indication of positive autocorrelation in the residues.

3.3.1 Ignition front propagation velocity

Figures 3 and 4 show the results for the first set of experiments listed in Table 1. Figures 3A and 3B

correspond to a ��� of 10% and ��� values of 7.1 mm and 22.2 mm, respectively. Figures 3C and

3D show equivalent results for a ��� of 30%. The vertical bars at each � value correspond to �� for

the thermocouple locations 1-2, 2-3, and 3-4. A visual inspection of Figure 3 reveals differences in

�� with the axial position. These differences in �� are more evident for the higher ��� and the lower

��� levels (i.e., Figure 3C). A direct proportion characterizes the dependence of the maximum

temperature on �. Additionally, the maximum temperature features higher values for the lower ���

level (i.e., Figure 3A and Figure 3B). Figure 3A shows that the increment in � from 0.18 ms-1 to

vs

vs m

s -1

T, °

C

t, s t, s

T, °

C

A B

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0.46 ms-1 raised the maximum temperatures ��", �"#, and �#$ by around 18%, 20%, and 13%,

respectively. Overall, Figures 3B, 3C, and 3D show the same dependence for the maximum

temperature (with increments in the range 10-25%).

Figure 3 shows that for the lower level of � the increment in ��� lowered �� by around 26% for

both ��� levels (Figure 3A vs. Figure 3B, and Figure 3C vs. Figure 3D), but the increment in ���

did not influence �� in either case (Figure 3A vs. Figure 3C, and Figure 3B vs. Figure 3D). Results

are not conclusive when considering the influence of ��� on �� for the higher level of � due to the

scattering of the data. Results for the higher level of � indicate that increasing ��� leads to ��

around 10% higher for the lower ��� level and 17% lower for the higher ��� level. Finally, for the

higher level of �, the increment in ��� lowered �� by around 14% and 35% for the lower and the

higher ��� levels, respectively.

The Biot dimensionless group (%&), given by Equation 2, represents the ratio of intraparticle

conduction and interfacial convection time scales [52]. In Equation 2 '� represents the characteristic

length scale, ℎ� the convective heat transfer coefficient between the coal particle and the carrier gas

and )� the thermal conductivity. Provided that %& > 1 intraparticle conduction limits the observed

reaction rate. To evaluate %&, ℎ� was calculated via the Ranz-Marshall correlation [53] with '�

equal to ���. For the operating conditions in Table 1 %& varies in the range 2.4-6.3, and even if '� is

reduced to a half, %& is still higher than one. The analysis of %& shows that for our experiments the

thermal conversion of coal was always limited by intraparticle conduction. Additionally, the ratio of

intraparticle conduction and interfacial convection time scales for the higher ��� level was more

than twice than that for the lower.

%&

ℎ�'�

)�

Eq. 2

The ignition source for flame propagation is radiation from the hot layer just above the unconverted

material [13]. A plausible explanation for the differences in �� with the axial position is the effect

of the ashes on the emissivity. When char and ashes start to accumulate and char oxidation become

important, the formed ashes could stay on the surface of the solids which brings down the

emissivity [54]. Understanding the variation of emissivity with the axial position is critical for

unraveling the abovementioned variability in ��, as well as for the validation of numerical models.

Our results for the effect of ��� on �� are in agreement with previous experimental studies for

biomass in TLUD fixed bed reactors [10], [37], [51], [55]–[57]. Section 3.1 already discussed the

most salient differences in composition between HVBC and PKS. Those compositional differences,

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and the fact that HVBC is around 1.6 times denser than PKS, might be responsible for the observed

effect of ��� on ��. The negative impact of ��� on ��, particularly at the higher ��� value is

consistent with the marked difference in VM between HVBC and PKS. Experiments with biomass

showed that an increment in bulk density of the bed results in lower �� [25], [51], [58], [59], which

is also consistent with our results regarding the effect of ���. Finally, experiments with biomass

fixed beds also showed that increasing particle size could cause canalization and stagnant zones

[56], [60]. Those effects could explain the relatively high scattering of the date, especially in Figure

3C and Figure 3D.

Figure 3 Ignition front propagation velocity (��) and maximum temperature (�,-.) as a function of

air superficial velocity ( �). A) Coal volume 10% and coal particle size 7.1 mm; B) Coal volume

10% and coal particle size 22.2 mm; C) Coal volume 30% and coal particle size 7.1 mm; D) Coal

volume 30% and coal particle size 22.2 mm. Error bars represent the difference between the

average and individual values of duplicated experiments.

u f ,

mm

s-1

Tm

ax,

°C

vs , m s-1 0.18 0.46 0.460.18

A B

DC

uf 12

uf 23uf 34

T 12

T 23

T 34

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3.3.2 Calculated equivalence ratio

The equivalence ratio, Φ, given by Equation 3, represents the actual air-fuel ratio (01) divided by

the stoichiometric air-fuel ratio (01�). The calculation of 01� requires the elemental compositions in

Table 3, together with the mass percentages of PKS and HVBC given in section 2.3. The

calculation of 01, on the other hand, necessitates the mass of converted fuel per unit time (23 �)

together with the air mass flow rate (23 -& ). The mass flow rate 23 � indicates, given by Equation 4,

results from the product of ��, the cross-sectional area 04 and the density of the bed 56�7.

Φ 01

01�

Eq. 3

23 � ��0456�7 Eq. 4

The parameter Φ provides a first indication of the operating regime for the TLUD fixed bed reactor.

For gasification, Φ typically lies in the range 0.2-0.4 while Φ values higher than one correlate with

combustion. Note that Φ greater than 0.4 may result in excessive formation of CO2 and H2O at the

expense of CO and H2. Figure 4 reveals a direct proportion between � and Φ, which is consistent

with a higher fuel consumption rate as � increases. Additionally, these results confirm the potential

of the TLUD setup to operate within a wide range of Φ with PKS-HVBC blends.

For the lower � level, Figure 4 shows that Φ varies in the range of 0.48-0.80. For these conditions,

the TLUD fixed bed reactor operates in the gasification regime [13]. Volatile oxidization reactions

in the gas phase and char reduction reactions in the solid phase occur in the gasification regime.

Note that excessive formation of CO2 and H2O results in a synthesis gas of relatively low heating

value. For the higher � level, Figure 4 shows that Φ varies in the range 0.89-1.1. For these

experiments, the Φ value indicates that the TLUD fixed bed reactor operates near stoichiometric

conditions. Under those conditions, oxidation reactions may occur in both the solid and gas phases.

Further increasing � could finally cause cooling by convection and shift the process to fuel-lean

conditions. The C content estimated from our proximate analysis via Akkaya's model [46] amounts

to 65.8, while table 3 reports a C content of 74.6. We calculated the equivalence ratio with both C

contents and found that the equivalence increases by less than 1% when the predicted C percentage

is used. Due to the relatively high C content in HVBC, C mainly determines the equivalence ratio.

Increasing ��� negatively affected �� while the opposite happened to Φ irrespective of the ��� level

in both cases. For the lower level of �, Figure 4 shows that the increment in ��� increased Φ by

around 35% for both ��� levels (Figure 4A vs. Figure 4B and Figure 4C vs. Figure 4D). On the

other hand, for the same � level, the increment in ��� yielded a 19% decrease in Φ for both ���

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levels. For the higher level of � the increment in ��� decreased Φ by around 9% for the lower ���

level but featured an increment of 20% in Φ for the higher ��� level. Results are also contrasting

when considering the influence of ��� for the higher level of � as it was the case with ��. In this

case, increasing ��� leads to �� 5% lower for the lower ��� and 25% higher for the higher ���.

Note that increasing ��� leads to higher 56�7 and eventually to higher 23 �, even if �� decreases.

Figure 4 Equivalence ratio (Φ) as a function of air superficial velocity ( �). A) Coal volume 10%

and coal particle size 7.1 mm; B) Coal volume 10% and coal particle size 22.2 mm; C) Coal volume

30% and coal particle size 7.1 mm; D) Coal volume 30% and coal particle size 22.2 mm. Error bars

represent the difference between the average and individual values of duplicate experiments.

3.4 Results for the second set of experiments

Figures 5 and 6 show the results for the second set of experiments listed in Table 2. Linear

regression of the observed �� vs. � data shows a correlation coefficient of 0.97. The �� value for

the lower � level differs by less than 8% with the corresponding values in Figure 3. This result is

consistent with the observation that the influence of ��� and ��� on �� is minor for the lower �

vs , m s-1 0.18 0.46 0.18 0.46

Φ,

-

C

A B

C D

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level. On the other hand, for the higher � level, the result is similar to the one for the higher ���

and lower ��� levels, but differs significantly with that for the higher ���.and ��� levels.

Figure 5 Ignition front propagation velocity and maximum temperature as a function of air

superficial velocity, coal volume 20%, and coal particle size 11.1 mm. Error bars represent the

difference between the average and individual values of duplicate experiments.

Figure 6 shows that Φ increases by 36% when � increases from 0.18 ms-1 to 0.32 ms-1 but remains

nearly constant with a further increase in � to 0.46 ms-1. The Φ for the lower � level lies in

between the corresponding result for the higher ��� level in Figure 4. The latter observation is also

valid for the higher � level, which is an indication of consistency for results in Figures 4 and 6.

u f ,

mm

s-1

vs , m s-1 0.18 0.32 0.46

vs , m s-1 0.18 0.32 0.46

Φ, -

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Figure 6 Equivalence ratio as a function of air superficial velocity, coal volume 20%, and coal

particle size 11.1 mm. Error bars represent the difference between the average and individual values

of duplicate experiments.

3.5 Product gas composition

A validated gasification model for a downdraft gasifier was used to gain insight into the product gas

composition [61]. The model was validated for biomass; here we validated the model for coal and

coal-biomass blends [62] with satisfactory results as shown in the Supplementary Material. The

model assumes chemical equilibrium and requires the elemental composition of the feed,

equivalence ratio, and maximum temperature. Figure 7 shows the composition and lower heating

value of the product gas (LHV;) for the lower level of �. Results for dry gas composition and LHV;

correspond to Figures 3A-4A, Figures 3C-4C, and Figures 3D-4D. Note that Φ higher than 0.65

results in negligible fractions of combustible gases. The volume fraction of CH4 is absent from

Figure 7 because it amounts to less than 0.1%.

The Φ range reported in the previous section produced syngas without the potential for power

generation in combustion engines of displacing natural gas in burners. The gas stream

corresponding to the upper end of Φ is suitable for direct use in cooking purposes without

secondary air, steam generation, thermal inputs in brick furnaces, power generation in the Organic

Rankine cycle, among other applications. The gas stream corresponding to the lower end of Φ has

around half of the LHV expected for air-blown gasifiers. Increasing coal volume percentage or

decreasing coal particle size can potentially enhance syngas quality under these conditions.

Decreasing v> leads to lower Φ and consequently to syngas with higher LHV.

Two primary uncertainty sources affect the predictions in Figure 7, the inherent gasification model

uncertainty, and the HVBC C content uncertainty. The average relative difference between model

predictions and measurements amount to 1.04% for CO, 2.63% for CO2, and 13.5% for H2. On the

other hand, the C content predictions reported in Table 3 and that calculated from our proximate

analysis show relative differences for CO, CO2, and H2 of 6.5%, 2.3%, and 12.9%, respectively.

Figure7 incorporates these uncertainties as to the square root of the sum of squares of individual

uncertainty values.

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Page 19: Thermochemical conversion of coal and biomass blends in a

Figure 7 Simulated composition and lower heating value of the product gas for the lower level of

air superficial velocity [63]. Results correspond to gas composition on a dry basis. Figures 3A-4A,

3C-4C, and 3D-4D show the corresponding ignition front propagation velocities and equivalence

ratios for columns A, C, and D.

For the lower level of � the increment in ��� leads to a Φ greater than 0.65 and a negligible

fraction of combustible gases in the product gas. For the lower levels of �, ��� and ���, Figure 7

shows that the product gas contains limited amounts of H2 and CO and features LHV; of around 1

MJ m-3. For the sake of comparison, note that syngas from air-blown fluidized bed biomass gasifiers

shows LHV; values in the range 3.5-6.0 MJ m-3 [1]. Starting from the lower levels of � and ���,

increasing ��� reduced Φ and yielded a product gas with a LHV; of around 1.7 MJ m3. A

subsequent increment in ��� increased Φ, which resulted in a product gas with almost no

combustible gases. Summing up, those results indicate that for the lower � level further increments

in ��� or decrements in ��� should result in product gas with higher LHV;. Another feasible path

towards product gas with higher energy content is decreasing �, although the latter results in lower

product gas throughput.

3.5 Outlook

The preceding subsections confirmed the potential for a stable operation within a wide range of

equivalence ratios with biomass-coal blends. So far, however, the TLUD technology seems

A C DΦ

LHV

, kJ

m-3

Con

cent

ratio

n,

%V

ol.

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restricted to batch operation, particularly at a low scale in remote rural areas. Further steps in

developing this technology relate to exploiting the biomass-coal synergy and implementing

continuous solids feeding together with variable gas throughput.

Blends of small and large particles improved the stability of the ignition front and broadened the �

operation range [59]. The main reason is that for relatively small particles (%& ≤ 1) intraparticle

conduction does not limit their conversion rate, i.e., they release volatiles at a relatively high rate.

Coal-biomass blends naturally benefit from the abovementioned effect due to their vast differences

in VM. Besides, ��� offers an additional degree of freedom to operate within a wide range of � and

optimize Φ. An aspect requiring further attention is the effect of the ashes on the emissivity and

consequently on �� when char and ashes start to accumulate on top of the unconverted material.

The batch operation mode of the TLUD fixed bed reactor limits their application range and

deployment scale. A further step in the development of this technology is the continuous feeding of

particulate solid fuel. An option to realize this idea is combining a solids feeding screw and a

second screw inside the reactor. The former delivers the feedstock near the bottom while the latter

keeps the ignition front within certain axial positions. Ideally, ashes spill over the top of an inner

tube and drop in an annular zone. To the best of the author's knowledge, a TLUD fixed bed reactor

with continuous solids feeding remains unreported.

The incorporation of sections with different cross-sectional area provides further flexibility to the

aforementioned continuous TLUD operation. In a typical straight TLUD, increasing air superficial

velocity shifts the operation regime from the gasification regime to the char oxidation regime. This

result implies that syngas throughput cannot increase without changing its composition. A device

with different cross-sections allows increasing syngas throughput while keeping its composition.

The screw inside the device is essential for keeping the ignition front at the desired location.

Finally, the gas phase composition is necessary to elucidate further the potential applications of

biomass-coal co-conversion in TLUD fixed bed reactors.

4. Conclusions

Co-thermochemical conversion of coal and biomass could decrease fossil carbon usage, mitigate

pollutant emissions while enhancing coal reactivity. This work presents an experimental

investigation of this process in a to-lit updraft fixed bed reactor or TLUD. The work focused on the

ignition front propagation velocity for thermal co-processing of palm kernel shell and high-volatile

bituminous coal. Experiments within a wide range of experimental conditions shed light on the

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effects of the air superficial velocity, coal particle size, and volume percentage. The investigation

used an in-house, designed, and built TLUD setup.

Results revealed differences in ignition front propagation velocity, ��, with the axial position. A

direct proportion characterizes the dependence of the maximum temperature on air superficial

velocity. Additionally, increasing the coal volume percentage negatively affected the maximum

temperature reached in the TLUD reactor. Results confirmed the TLUD setup potential to operate

within a wide range of equivalence ratios with PKS-HVBC blends. For the lower air superficial

velocity level, the calculated equivalence ratio varied in the range 0.48-0.80, i.e., the TLUD fixed

bed reactor operated under gasification conditions. For the higher air superficial velocity, the

equivalence ratio varied in the range 0.89-1.1, i.e., near stoichiometric conditions. This result

indicates that, for the latter conditions, oxidation reactions may occur in both the solid and gas

phases. Further increasing the air superficial velocity could cause cooling by convection.

For the lower level of air superficial velocity, the increment in coal particle size lowered �� for both

��� levels, but the increment in coal volume percentage did not influence ��. Results were

contrasting when considering the influence of coal particle size on �� for the higher level of air

superficial velocity due to data scattering. For the higher level of air superficial velocity, the

increment in coal volume percentage lowered �� indirect proportion to the coal particle size.

Additional experiments confirmed the linear dependence of �� on the air superficial velocity within

the assessed experimental range. Under gasification conditions, further increments in ��� or

decrements in ��� should result in product gas with higher LHV;.

The TLUD operation mode still represents a relatively uncharted fixed bed reactor. Its capabilities

indicate that further and more frequent uses will come over the next decade. The TLUD fixed bed

reactor shows excellent potential for the thermal conversion of solids fuel in the rapidly developing

energy and environmental engineering fields.

Nomenclature

ANOVA Analyses of variance 04 Cross-sectional area m2 %& Biot number, ℎ�'� )�⁄ dafb Dry-ash-free basis db Dry basis ����� Critical point Durbin-Watson statistic ��� Coal particle size mm

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�!��� Critical point Durbin-Watson statistic 10 Actual fuel-air ratio 10� Stoichiometric fuel-air ratio FC Fixed carbon % wt HHV High heating value kJ kg-1 ℎ� Convective heat transfer coefficient W m-2 K-1 HVBC High-volatile bituminous coal LHVg Lower Heating Value of gas kJ m-3 '� Characteristic length scale of a solid particle mm 23 -& Air mass flow rate kg s-1 23 � Fuel mass flow rate kg s-1 PKS Palm kernel shell � Temperature °C � time s TGA Thermogravimetric analysis TLUD Top-lit updraft �,-. Maximum temperature °C �� Ignition front propagation velocity mm s-1 VM Volatile matter % wt ��� Coal volume percentage % v v-1 � Air superficial velocity m s-1 ∆� Distance between consecutive thermocouples mm )� Solid thermal conductivity W m-1 °C-1 Φ Equivalence ratio 56�7 Bed density kg m-3

Acknowledgments

MINCIENCIAS supported this work through the Ph.D. National Scholarship Becas Bicentenario

2019 Contract UN-OJ-2020-47414. This work was also supported by "Convocatoria 753 para la

formación de capital humano de alto nivel para el Departamento Norte de Santander". The research

leading to these results has received funding from the research project UN-OJ 2019-45458 by

Universidad del Norte.

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Highlights

• Gasification and near stochiometric operation conditions with biomass-coal blends

• Notable variability of the ignition front propagation velocity with axial position

• Minor influence of coal percentage on ignition front velocity for gasification

• Coal percentage decreases ignition front velocity near stochiometric conditions

• Continuous feeding and adjustable throughput critical for technology development

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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.

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