Journal of Hazardous Materials 415 (2021) 125608

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Journal of Hazardous Materials

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Effective practical removal of acetaldehyde by a sandwich-type

plasma-in-honeycomb reactor under surrounding ambient conditions
Nosir Matyakubov a, Duc Ba Nguyen a, b, *, Shirjana Saud a, Iljeong Heo c, Sang-Joon Kim c,
Young Jin Kim c, Jin Hee Lee c, Young Sun Mok a, **
a
Department of Chemical and Biological Engineering, Jeju National University, Jeju 63243, Republic of Korea
b
Institute of Research and Development, Duy Tan University, Danang 550000, Viet Nam
c
Environment & Sustainable Resources Research Center, Korea Research Institute of Chemical Technology, Daejeon 34114, Republic of Korea

A R T I C L E I N F O A B S T R A C T

Editor: Dr. Rinklebe Jörg The effective removal of acetaldehyde by humidified air plasma was investigated with a high throughput of
contaminated gas in a sandwiched honeycomb catalyst reactor at surrounding ambient temperature. Here,
Keywords: acetaldehyde at the level of a few ppm was successfully oxidized by the honeycomb plasma discharge despite the
Honeycomb discharge harsh condition of large water content in the feed gas. The conversion rate of acetaldehyde increased signifi­
Humidified air plasma
cantly with the presence of catalysts coating on the surface channels. The increased conversion rate was also
Acetaldehyde removal
obtained with a high specific energy input (SEI) and total flow rate. Interestingly, the conversion changed
Low-temperature removal of acetaldehyde
negligibly under the acetaldehyde concentration range from 5 to 20 ppm. However, the conversion rate
decreased toward increased water amount in the feed gas. Notably, about 60% of acetaldehyde in the feed was
oxidized under SEI of 40 J/L at water amounts ≤ 2.5%, approximately 0.5 g/kWh for acetaldehyde removal.
Also, the plasma-catalyst reaction was superior to the thermal reactive catalyst for acetaldehyde removal in
airborne pollutants. In comparison with other plasma-catalyst sources for acetaldehyde removal, the energy
efficiency under the condition is comparable. Moreover, the honeycomb plasma discharge features high
throughput, avoiding pressure drop, and straightforward reactor configuration, suggesting potential practical
applications.

1. Introduction 2011; Klett et al., 2014; Hadei et al., 2019).

Several techniques have been proposed to remove acetaldehyde and
Removal of volatile organic compounds (VOC) such as acetaldehyde other VOCs, namely thermal oxidation, thermal catalytic oxidation
is interesting and worthy of research due to the requirement of purified (Lejeune et al., 2020), and plasma (Klett et al., 2012) or plasma-catalytic
contaminated gases (Chang et al., 2019; Bogaerts et al., 2020; Lejeune reaction (Nóbrega et al., 2019; Veerapandian et al., 2019). Among these,
et al., 2020). Indeed, VOCs are identified as primary contributors to plasma-assisted VOC removal is a powerful approach with fast conver­
environmental pollution due to their toxic nature, categorization as sion, easy control, and compatible diversification with VOC sources.
hazardous materials, severe effects on human health, and they are active Thermal plasma features both thermal and plasma activations, resulting
players in atmospheric photochemical reactions (Jacobson, 2012). It has in high-performance VOC removals (Zhu et al., 2017), especially when
also been widely used as a solution in industrial processes, emitted from VOCs require harsh decomposition conditions, such as chemical com­
agricultural products, and exists in diesel exhaust gas emissions. pounds consisting of aromatic rings. However, with indoor VOC emis­
Consequently, removal of VOCs in contaminated gases is required before sions, like acetaldehyde, where contaminated gas is at surrounding
emitting the gas into the atmosphere. Among these VOCs, the emission ambient temperature (~25 ◦ C), thermal processes (thermal processes
of acetaldehyde from various outdoor (combustion engines of trans­ with/out catalyst oxidation or thermal plasma) has a disadvantage due
portation and power plants; agricultural products) and indoor sources to high-energy consumptions. Specifically, with a relative thermal pro­
are in a significant amount (Gustafson et al., 2007; Sarigiannis et al., cess, an operating temperature of several hundred ◦ C may be required

* Corresponding author at: Department of Chemical and Biological Engineering, Jeju National University, Jeju 63243, Republic of Korea.
** Corresponding author.
E-mail addresses: band@plasma.ac.vn (D.B. Nguyen), smokie@jejunu.ac.kr (Y.S. Mok).

https://doi.org/10.1016/j.jhazmat.2021.125608
Received 4 December 2020; Received in revised form 26 February 2021; Accepted 4 March 2021
Available online 8 March 2021
0304-3894/© 2021 Elsevier B.V. All rights reserved.
N. Matyakubov et al. Journal of Hazardous Materials 415 (2021) 125608

for an active oxidation reaction; that is, the contaminated gas needs to Hensel et al., 2005, 2007; Hensel, 2009; Kang et al., 2013). Recently, a
be heated from the surrounding ambient temperature (~25 ◦ C) to ach­ humidified air plasma inside a commercial honeycomb monolith with a
ieve temperature activation. Since the specific heat capacity of air is diameter of 93 mm and a length of 50 mm was successfully produced by
approximately 1.2 J/L (29 J/mol) for increasing 1 ◦ C (Prudich et al., a sandwich reactor (Nguyen et al., 2020b); in addition, the plasma
2008), the energy consumption requirement is at least 90 J/L for heating discharge is highly dependent on the amount of water in the feed gas.
gas from 25◦ to 100◦ C. However, according to previous literature reports Fortunately, this condition is similar to actual indoor emissions of VOCs;
(Chiper et al., 2006; Klett et al., 2012; Jia et al., 2018; Lee et al., 2020), the water amount can be dependent on the surrounding ambient
the energy level (~90 J/L) delivered by nonthermal plasma(NTP) was conditions.
proposed for the effective removal of acetaldehyde. This comes from This study focused on the removal of acetaldehyde in a honeycomb
using the primary input energy to produce energetic electrons, ions, plasma reactor. Here, the plasma reactor was created by a commercial
radicals, and excited species instead of heating gas molecules in the NTP. honeycomb catalyst located between two electrodes like a sandwich.
As a result, NTP features a reactive chemical cocktail at near room The feed gas is a simulated indoor acetaldehyde emission, i.e., a low
temperature. acetaldehyde concentration in a humidified air. The removal of acetal­
A dielectric barrier discharge (DBD) reactor is a common NTP that dehyde by the humidified air plasma was examined with several factors:
has been used widely in VOC as well as acetaldehyde removal (Cools concentration of acetaldehyde, humidity of feed gas, total flow rate,
et al., 2019; Li et al., 2020). The DBD has a simple plasma system design metal absence/presence on the monolith, input energy, and process
and stable plasma discharge with current extinguishing on the surface of time. As a result, the honeycomb plasma discharge is capable of acet­
dielectric layer between two electrodes. Moreover, there is a synergetic aldehyde removal with extensive gas volume treatment at room tem­
effect of plasma coupled with a catalyst for VOC removal (Feng et al., perature. Furthermore, the plasma chemistry of honeycomb discharge
2018). As a result, a packed-bed DBD is frequently used to investigate was also discussed in this study.
VOC removal (Li et al., 2020). Although a packed-bed DBD successfully
removes VOC, the system is limited to high flow rates due to 2. Experimental
high-pressure drop. An alternative approach to addressing this issue is
the production of plasma in a honeycomb-structured catalyst (Mizuno The decomposition of acetaldehyde was investigated by a giant
and Craven, 2019). Several configurations have been useful for the plasma volume of humidified air under surrounding ambient conditions.
generation of honeycomb discharge, including DBD, corona discharge, The humidified air plasma produced in a honeycomb-type monolith
and ignition plasma discharge along with back corona discharge (Saud plasma reactor with an experimental setup is shown in Fig. 1. The
et al., 2021); unfortunately, there is still a constraint on the size of the plasma is based on AC discharge and generated in the zone created by
honeycomb (≤30 mm) (Nguyen et al., 2020b). Among these plasma two parallel stainless-steel perforated disks (168 holes; diameter hole of
configurations, the generation of plasma in a honeycomb with a 3 mm; a discharge gap of 52 mm). The commercial honeycomb (93-mm
sandwich-type honeycomb plasma reactor is simple, capable of oper­ diameter, 50-mm length, 300 cpsi) located inside the gap with the
ating with a large honeycomb size, and facilitates practical applications. honeycomb touched the ground electrode. The catalyst was produced by
Indeed, the configuration consists of a honeycomb catalyst that is Ceracomb Co., Ltd., Korea. The metal catalyst composition of the
sandwiched in two parallel electrodes (Okubo et al., 2003, 2004, 2007; monolith was examined by an inductively coupled plasma atomic

Fig. 1. Schematic diagram of the experimental setup.

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N. Matyakubov et al. Journal of Hazardous Materials 415 (2021) 125608

emission spectrophotometer (5100 ICP-OES, Agilent, USA). The result ( ) ( ( ) ( ))⃒T2

presented that the surface of honeycomb channels consisted of La, Pt, J 1 C3 C5 ⃒⃒
Equivalent SEI = C1T +C2C3coth − C4C5tanh ⃒
Pd, and Co with 0.03, 0.03, 0.07, and 0.10 wt%, respectively, based on a L 24,450 T T T1

total monolith weight of ~260 g. (5)

The feed gas was a mixture of acetaldehyde with a large volume of
moisture air. The flow rate of acetaldehyde was controlled via a N2 flow Where: T1 is 298 K (initial gas temperature, 25 ◦ C); T2 is operating
through the Erlenmeyer flask containing acetaldehyde, kept in a water temperatures; 24,450 is a constant for calculating equivalent SEI based
bath at 5 ◦ C. Individually, 7.1 ml/min N2 flow through the Erlenmeyer on gas volume at 25 ◦ C, C1 = 28,958, C2 = 9390, C3 = 3012,
flask was introduced by a mass flow controller (AFC500, Atovac Co., C4 = 7580, and C5 = 1484.
Korea); subsequently, the mixture of N2 and acetaldehyde was diluted The acetaldehyde, CO2, and O3 components in the gas outlet were
with another 86 ml/min N2, first-time dilution. To obtain 5 ppm acet­ analyzed with several types of equipment. Briefly, the concentration of
aldehyde, the 4 ml/min of first-time diluted acetaldehyde mixture was acetaldehyde was determined by a gas chromatography (GC, Bruker
incorporated with 60 L/min humid air, the second-time dilution. The 450-GC, USA). The O3 concentration in the gas outlet was indicated with
humidified air flow rates were controlled by ball flowmeters (Dwyer, gas detector tubes (No 0.18 M Ozone, 4–400 ppm, GASTEC Corp.,
RMA-25-SSV, USA). Furthermore, the absolute humidity of water vapor Japan). Furthermore, light emission from plasma discharge was recor­
was regulated by the dry-air part mixed with the remained humidified ded with an optical emission spectrometer (OES, AvaSpec-2048 XL,
air. The absolute water vapor was calculated via temperature and rela­ Netherlands). The temperature of the gas outlet was monitored with a
tive humidity (RH); these parameters were measured by a humidity copper thermal sensor. The thermal sensor was located inside the reactor
meter (TES Electrical Electronic Corp., TES-1370 NDIR CO2 Meter, at 30-mm and 10-mm distance from the center axis and ground elec­
Taiwan). In this study, the water amount was examined up to 3.3%, trode, respectively. Since the monolith is 93-mm in diameter, it should
corresponding to RH 100% at 26 ◦ C; the range is similar to the water be mentioned that the temperature measurement is a representation of a
level in the indoor emission. positioned temperature, not the average temperature for the gas outlet.
The contaminated air plasma was ignited and sustained by 400-Hz
AC high voltage from a high-voltage transformer (Tae Hwa Electric 3. Results and discussion
Co., Korea); the primary voltage up to 300 V was provided by a fre­
quency converter (Sampoong Power Co., Ltd., Korea). During plasma 3.1. Dependence of honeycomb discharge on acetaldehyde concentration
discharge, electrical parameters were recorded by a digital oscilloscope and process time
(Tektronix, DPO 3034, USA). The oscilloscope was installed with a high
voltage probe (P6015A, Tektronix, USA) and a current monitor (2100, The honeycomb discharge strongly depends on the physicochemical
Pearson Electronics, USA) used for the measurement of applied high honeycomb surface, i.e., humidity, relative permittivity (dielectric
voltage and total current, respectively. Here, it should be noted that the constant), and conductivity (Nguyen et al., 2020a, 2020b; Saud et al.,
waveforms were acquired with the average mode of 8 samples by the 2021). In this study, the effect of acetaldehyde on the plasma discharge
oscilloscope setting. Plasma discharge dissipated to the honeycomb was investigated under the presence or absence of 100 ppm acetalde­
catalyst was calculated by integrating instantaneous voltage and cur­ hyde in the 70 L/min of humidified air (water content of 3.3%). Herein,
rent, as shown in Eq. (1). Furthermore, other parameters used for the high acetaldehyde inlet concentration was used to rapidly obtain a
analysis, i.e., specific energy input (SEI), removal efficiency (conversion, steady-state of acetaldehyde adsorption on the surface. The monolith
η) of acetaldehyde, and an equivalent SEI, are also defined. catalyst was dried at 300 ◦ C for 3 h to remove the contaminated
∫ ∫ chemicals and water; the monolith catalyst was cooled to 110 ◦ C in the
Discharge Power, P(W) =
1 T
Pinstantaneous dt =
1 T
V(t)I(t) dt (1) oven and then cooled back to room temperature inside a desiccator. The
T 0 T 0 dried monolith catalyst was assembled into the reactor, and the hu­
( ) midified gas was fed through the reactor. The high voltage of 20 kV
Specific Energy Input, SEI
J
=
P(W)
× 60 (2) started power delivery to the electrodes; the discharge power and gas
L Q(L/min) temperature were recorded during plasma discharge. The evolution of
the discharge power and temperature with the absence/presence of
Weight of C2 H4 O conversion
Removal Efficiency, η(%) = acetaldehyde is shown in Fig. 2.
Weight of C2 H4 O inlet This figure demonstrated a negligible effect of acetaldehyde on the
[ ] (3)
Coutlet
= 1− × 100
Cinlet C2 H4 O

Weight of C2 H4 O conversion (g)

Energy Efficiency, EE(g/kWh) =
Energy consumption (kWh)
3.6 × 44.05 × Cinlet × η
=
24.45 × SEI
(4)

Where: Cinlet/outlet (ppm) is the concentration of acetaldehyde (CH3CHO)

in the gas inlet/outlet; 1 mol of acetaldehyde has a weight 44.05 g;
1 mol of gas under atmosphere and at 25 ◦ C (298 K) has a volume of
24.45 L; 3.6 is a factor to obtain g/kWh with concentration unit as ppm
in the Eq. (4).
The equivalent SEI of the thermal catalyst process was estimated
through input energy for heating air from room temperature (25 ◦ C) to
the operating temperature, adopted from elsewhere (Saud et al., 2020).
Fig. 2. Effects of presence/absence of acetaldehyde on the discharge power and
gas outlet temperature (Applied voltage = 20 kV; C2H4O inlet = 100 ppm;
water content = 3.3%; total flow rate = 70 L/min).

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N. Matyakubov et al. Journal of Hazardous Materials 415 (2021) 125608

gas temperature and early discharge power (< 20 min). However, for same SEI is higher for the bare monolith than the monolith catalyst. The
process time above 20 min, the discharge power decreased slightly in difference between the bare and catalytic monoliths on the discharge
the acetaldehyde presence. Whereas, in the absence of acetaldehyde, the power can be explained by implementing the physicochemical surface of
discharge power was maintained and reached the steady-state. Conse­ honeycomb channels due to the coated layer. Indeed, a total metal
quently, after 60 min, the discharge power with acetaldehyde equaled component of 0.23%, M/Al2O3 (M = Co, La, Pd, Pt), was present on the
89% of the discharge power without acetaldehyde, meaning that the coated layer of monolith catalyst, whereas the bare monolith was made
discharge power decreased by 11%. The phenomenon can be explained from 2MgO.2Al2O3.5SiO2 (typical ceramic materials). Furthermore, the
by the change of physicochemical property of honeycomb channel sur­ reactor’s capacitance with the monolith catalyst was observed to be
faces after absorbing acetaldehyde from the feed gas. The acetaldehyde higher than that of the bare monolith; the capacitance also strongly
adsorption of the monoliths was given in Fig. S1 (Supplementary Data). depends on the humidified feed gas (Nguyen et al., 2020b; Saud et al.,
To sum up, although the concentration of acetaldehyde was at a level of 2021). The plasma discharge behavior in the sandwich-type honeycomb
100 ppm, the discharge power of the honeycomb discharge still discharge consisted of two stages in each phase of voltage (positive and
decreased with the presence of acetaldehyde in the feed gas. negative), i.e., the capacitive stage and followed the discharge stage.
Effects of process time on the acetaldehyde removal were investi­ Consequently, a larger capacitance leads to an increase in discharge
gated in terms of SEI (discharge power) and acetaldehyde concentration current as well as discharge power (Nguyen et al., 2020b; Saud et al.,
in the gas outlet, as shown in Fig. 3. The results revealed a low con­ 2021). Furthermore, metals distributed on the surface of honeycomb
centration of acetaldehyde in early time (20-min process time) in the gas channels would improve the electrical conductivity of the monolith; it is
outlet. After that, the concentration gradually increased and reached a also a reason for increased discharge power with the monolith catalyst.
steady-state at a processing time above 50 min. However, the outlet gas The effect of the coated layer on the conversion of acetaldehyde was
humidity rose rapidly within 5 min and reached the steady-state (Sup­ also examined and presented in Fig. 4(c). This indicated that the con­
plementary Data, Fig. S2). The adsorption of water and acetaldehyde by version via the catalyst is superior to bare at the same SEIs; moreover,
the monolith catalyst can explain both the low acetaldehyde concen­ the conversion rate increased towards SEI for both monolith cases. The
tration and humidity at the early time. As a result, the plasma process different conversion of acetaldehyde under bare monolith/monolith
reached a steady-state after 50 min for all parameters; the conversion of catalyst is described by the coated layer presence on the monolith. This
acetaldehyde was about 39% at these conditions. Consequently, in suggested that there is an incorporated effect of the coated layer with
further experiments, all data were recorded when the process obtained a plasma for the acetaldehyde conversion in the honeycomb plasma
steady-state under these conditions. discharge. To sum up, the commercial honeycomb catalyst with the
presence of a metal coated layer improved discharge power and
3.2. A role of metal catalyst on the acetaldehyde removal process increased the acetaldehyde conversion by the plasma-catalytic reaction.
Due to an extensive range of SEI that can be carried out with the
Fig. 4(a) showed the discharge power of the monolith catalyst was monolith catalyst, high removal efficiency of acetaldehyde can be ob­
larger than that of the bare monolith under the same conditions. Pre­ tained by a plasma-catalyst discharge. For instance, about 67% of
cisely, at the same applied voltage, dissipated input energy on the acetaldehyde in the gas inlet was converted at SEI of 54 J/L in the case of
monolith catalyst is superior to the bare monolith under the same other plasma-catalyst.
conditions. A high discharge power in the monolith catalyst resulted More activated sites in the honeycomb catalyst can explain the
from the high intensity of the discharge current. Indeed, the discharge increased conversion rate of acetaldehyde with the honeycomb catalyst.
power is estimated by integrating instantaneous power (multiplication Indeed, the conversion of acetaldehyde can occur in both gas phase and
of voltage with the current), as given in Eq. (1). Therefore, under the channel surfaces. Several possible reactions for acetaldehyde removal
same voltage, high intensities of current lead to high discharge power. during plasma-catalyst discharge are given in R1–20; for referencing,
For instance, the curves of voltage and discharge current under bare/ their rate constants under the absence of plasma discharge at room
catalytic monoliths are presented in Fig. 4(b). This showed that the temperature (300 K) were acquired from (Manion et al., 2020). Herein,
current intensities of catalyst are superior to bare, especially during the reactions are interactions between O•, •OH, •CH3, •CHO, and
plasma discharges (around high voltage peaks). As a result, the CH3CHO molecules, due to low dissociation energy of O2, H2O, and
discharge power of the bare monolith is 27.4 W, while it is 54.2 W for CH3CHO (~5 eV); the phenomenon was supported by a negligible NOx
the monolith catalyst case. The applied voltage required to obtain the concentration in the gas outlet with/out acetaldehyde in the feed gas,
due to considerable dissociation energy of N2 (~9.79 eV). Since the
coated catalyst layer improved the adsorption of reactive species and
created more catalyst active sites, reactive species can be absorbed,
followed by the reaction on those sites (Tu et al., 2019). As a result,
besides acetaldehyde converted by plasma reaction in the gas phase, the
plasma-catalyst active sites have added the conversion.
Dissociation of gas molecules by e/M (excited species).

CH3CHO + e/M ↔ •CH3 + •CHO + e/M (3.78 eV) (R1)

H2O + e/M ↔ •OH + H• + e/M (4.46 eV) (R2)

3 3 1
O2 + e/M → O( P) + O( P, D) + e/M (5.15 eV) (R3)
4 4 2
N2 + e/M → N( S) + N( S, D) + e/M (9.79 eV) (R4)

Possible main reactions between species for O3 generation or acet­

aldehyde removal.

O2 + O• + T → O3 + T k(298 K) = 6.01E-34 [cm6/molecule2 s] (R5)

Fig. 3. Evolution of the concentration of acetaldehyde and discharge power 3
O3 → O• + O2 k(300 K) = 4.38E-26 [cm /molecule s] (R6)
under applied voltage = 15 kV and water amount of 2.5% (C2H4O
inlet = 23 ppm; total flow rate = 40 L/min). CH3CHO + O3 → HO3 + CH3CO k(300 K) = 6.72E-29 [cm3/molecule s](R7)

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N. Matyakubov et al. Journal of Hazardous Materials 415 (2021) 125608

Fig. 4. Comparison between the bare monolith and monolith catalyst on the (a) discharge power, (b) curve of voltage and current discharge at 25 kV, and (c)
conversion of acetaldehyde (total flow rate = 60 L/min; water content = 2.5%; C2H4O inlet = 5 ppm).

CH3CO + O3 → Products k(300 K) = 4.08E-11 [cm3/molecule s] (R8)

3.3. Dependence of the acetaldehyde removal on the input parameters
CH3CO + O• → CO2 + •CH3 k(300 K) = 1.60E-11 [cm3/molecule s] (R9)

CH3CHO + O• → CH3CO + •OH k(300 K) = 4.58E-13 [cm3/molecule s] 3.3.1. Effects of flow rate on acetaldehyde removal process
(R10) Fig. 5(a) presented that the conversion rate of acetaldehyde
increased with the total gas flow from 20 to 60 L/min, corresponding to
CH3CHO + •OH → CH3CO + H2O k(300 K) = 1.49E-11 [cm3/molecule s] gas hourly space velocity (GHSV) from 3500 to 10,600 h− 1, at the same
(R11) SEI of 25 J/L. Since the concentration of acetaldehyde was fixed at
5 ppm in the feed during varying total flow rates, the absolute amount of
•CH3 + O• → H2 + HCO k(298 K) =4.0E-1 [cm3/molecule s] (R12)
acetaldehyde conversion significantly increased toward the flow rate.
3
•CH3 + O• → CH2O + H• k(298 K) =9.4E-11 [cm /molecule s] (R13) Generally, when a decrease in the retention time by adjusting the flow
rate, the conversion rate would be decreased (Chang et al., 2019).
3
•CH3 + O• → CH3O• k(300 K) =2.60E-14 [cm /molecule s] (R14) However, in this study, the phenomena did not occur with the retention
3
•CH3 + O• → Products k(298 K) =1.26E-10 [cm /molecule s] (R15) time decreased from 0.48 to 0.16 s for a total flow rate of 20 and
60 L/min, respectively. A reason for explaining the result is a linear
•CH3 + •OH → Products k(300 K) =1.20E-10 [cm3/molecule s] (R16) amount of O•/O3 generation with a total flow rate by the plasma system.
To validate, the concentration and total amount of O3 under the same
•CH3 + O3 → Products k(298 K) =2.20E-12 [cm3/molecule s] (R17)
conditions without acetaldehyde in the feed were plotted in Fig. 5(b).
3
HCO + O• → CO2 + H• k(300 K) =4.6E-1 [cm /molecule s] (R18) The figure demonstrated that the experimental data are in agreement
with the supposition. Specifically, the total O3 generation increased
HCO + •OH → CO + H2O k(296 K) =1.83E-10 [cm /molecule s] 3
(R19) from 0.07 to 0.16 g-O3/h toward the flow rate, although the concen­
tration of O3 decreased slightly from 28 to 22 ppm under this condition.
HCO + O3 → CO2 + O2 + H• k(298 K) =8.30E-13 [cm3/molecule s] (R20)
Furthermore, the O3 concentration in the gas outlet with 5-ppm

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N. Matyakubov et al. Journal of Hazardous Materials 415 (2021) 125608

(b). As seen from this figure, the massive resistance (45.5 MΩ) at 1.0%
water was suddenly dropped to a level of 9 MΩ when the water amount
reached 1.5%. Consequently, the current intensity increased signifi­
cantly, although the applied voltage was the same. As discharge power is
an integration of voltage and current, as shown in Eq. 1, a high discharge
power was obtained under a high-water amount. In another viewpoint,
the plasma discharge in a sandwich-type honeycomb plasma discharge is
like DBD discharge, which consisted of charge and discharge phase
(Nguyen et al., 2020b; Saud et al., 2021); therefore, an increase in the
reactor capacitance is a result for high plasma discharge. Both trends of
the resistance and capacitance under the water variation in the feed gas
agreed to increased plasma discharge.
In contrast, acetaldehyde conversion decreased towards increased
water amount in the feed gas, as presented in Fig. 6(c). This means that
energy efficiency for acetaldehyde removal decreased at a high-water
amount. A decrease in O3 generation at a high humidified air plasma
can explain the decrease in acetaldehyde conversion at a higher water
amount in the feed (Nguyen et al., 2020b). Another reason could be the
increased input power used to dissociate water and oxygen species (O•,
O3) reacted with water or hydroxyl radicals (•OH) under a larger water
amount that resulted in a low acetaldehyde conversion. To sum up,
humidity is an inhibitor of the acetaldehyde conversion in the honey­
comb discharge, around 60% acetaldehyde (inlet 5 ppm) in the hu­
midified air (≤3.3%) can be converted under SEI of 60 J/L.

3.3.3. Effects of the initial acetaldehyde concentration on acetaldehyde

removal process
The conversion rate of acetaldehyde decreased negligibly with the
variation of inlet acetaldehyde concentration in the range of 5–20 ppm,
as presented in Fig. 7. In detail, under the variation of inlet concentra­
tion, the conversion rate slightly decreased from 67.4% to 65.7% at SEI
of 55 J/L and water content of 2.5%. Suggesting the removal efficiency
of acetaldehyde is maintained by the system despite the changes in the
Fig. 5. (a) Effects of flow rate on the removal of acetaldehyde with inlet inlet concentration. In other words, more acetaldehyde molecules can be
acetaldehyde fixed at 5 ppm and (b) formation of O3 at SEI of 25 J/L under the destroyed by the plasma-catalyst discharge under these conditions. The
absence of acetaldehyde (water content = 2.5%). emission of O3 during this experiment was also plotted; this indicated
the O3 was emitted at the level of 25–30 ppm.
acetaldehyde in the feed gas is 13 and 14 ppm with a total flow rate of 20
and 30 L/min, respectively. The significant O3 emission, while incom­ 3.4. Plasma chemistry of honeycomb discharge
plete acetaldehyde decomposition in the gas outlet, can be explained by
massive O2 (~205,000 ppm) in comparison to acetaldehyde (5–20 ppm) OES of the honeycomb plasma discharge from the 2-mm gap, the
in the gas phase conjugated with the reaction rate of R5, which is power electrode and honeycomb monolith catalyst, is shown in Fig. 8.
comparable to other reactions with acetaldehyde as reactants (R7–20). The typical spectrum is similar to other humidified air plasma spectra
To sum up, the conversion rate of acetaldehyde increased with the total (Nguyen et al., 2020a), which consisted of high intensities of N2 line in
flow rate. C3Πu − B3Πg system (the second positive system of N2) and N+ 2 lines with
∑ 2∑+
B2 + u − X g system (the first negative system of N2 ) (Pearse and
+

3.3.2. Effects of the humidity on acetaldehyde removal process Gaydon, 1976). Moreover, the NO lines from 200 to 300 nm in the A2
∑+
Humidity has an adverse effect on the plasma for VOCs as well as → X2Π system (nitrogen third positive, γ system) were also not
acetaldehyde removal (Zhu et al., 2014), owing to decreasing efficiency detected (inset figure). Due to water presence in the discharge zone,
removal of VOC. Unfortunately, an indoor emission of VOC is a typical there is a potential presence of OH lines in the spectra. However, with
atmosphere that consisted of 1.5–3.5% water vapor, which depends on the high-intensity emission of N2 background gas, the OH lines have
the surrounding ambient conditions. However, the humidified feed gas been observed unclearly in the spectrum. Specifically, the OH lines at
is a critical factor for the plasma performance in the honeycomb 295 and 308 nm can be merged with the N2 emission at 296 and 315 nm,
discharge, i.e., poor honeycomb plasma discharge is solved with suffi­ respectively. In the case of the 390 nm OH line, the line can be identified
cient water vapor in the feed gas. In this study, the effect of water due to incomplete merger with 394 nm N2 line, as presented in the inset
amount in the feed gas on the plasma performance for acetaldehyde figure; as seen from this figure, the C2 band at 516 nm was also not
removal was examined under varying SEI from 10 to 70 J/L. observed, although 5 ppm acetaldehyde was in the feed. The O3 con­
Fig. 6(a) demonstrated that the discharge power, as well as SEI, centration was detected at 30 ppm in the gas outlet; however, the O lines
increased when the water amount in the feed increased at the same at 777 nm and 884 nm were also not identified in the spectrum (Nguyen
applied voltage. In other words, to obtain similar discharge power or et al., 2020c). Consequently, under the humid condition and atmo­
SEI, the applied voltage requirement decreased at high humidity. The spheric, the OES of the honeycomb discharge is primary emissions of N2
tendency is in agreement with that obtained by a bare monolith (Nguyen and N+ 2 in the range of [290–460 nm].
et al., 2020b). The increased discharge power can be explained by the
significant decrease in resistance or increase of capacitance of the
reactor under the high-water amount in the feed gas, as shown in Fig. 6

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N. Matyakubov et al. Journal of Hazardous Materials 415 (2021) 125608

Fig. 6. Effects of water amount in the feed gas on the (a) discharge power, (b) capacitor and resistance under without plasma discharge (the reactor was unconnected
with plasma power supply), and (c) removal of acetaldehyde (C2H4O inlet = 5 ppm; total flow rate = 60 L/min).

a NTP, which features electrons, ions, radicals, excited species (a

chemical cocktail of reactive species, as presented in the OES), despite
low temperatures of gas molecules. Fortunately, the interaction between
the humidified air plasma and the surface of the monolith catalyst
improved acetaldehyde removal at low temperatures instead of high
temperatures in the thermal process. The required high temperature of
the thermal reactivated catalyst is a disadvantage because the contam­
inated gas is close to room temperature; therefore, equivalent SEI is
above 200 J/L to reactivate catalyst by heating the gas inlet and catalyst.
In contrast with the plasma reactivated catalyst, it only consumed
several tens of J/L to produce the chemical cocktails and converted
acetaldehyde. In summary, the plasma-activated catalyst for acetalde­
hyde removal is superior to the thermal catalytic process. However, the
limited input power dissipated on the honeycomb monolith need to be
overcome for completing the removal of acetaldehyde by the plasma-
catalyst.
Fig. 7. Effects of initial concentration of acetaldehyde on the conversion rate A comparison between several plasma-catalyst systems for acetal­
(total flow rate = 60 L/min; water amount = 2.5%; SEI = 55 J/L). dehyde removal is presented in Table 1. This indicated that almost all
processes by either one stage or two stages of plasma with catalyst
require energy consumption at a level of 100 J/L for acetaldehyde
3.5. Comparison of acetaldehyde removal by the honeycomb plasma with removal, which also validated again for the low-energy consumption by
other processes NTPs, as mentioned above. In comparison between the sandwich-type
honeycomb plasma discharge and other plasma-catalyst processes, the
A comparison between thermal reactivated catalyst and plasma- energy efficiency by the honeycomb discharge is the lowest. The lowest
catalyst for acetaldehyde removal in humid air was shown in Fig. 9. energy efficiency can be explained by the lowest inlet concentration of
The figure demonstrated that the energy consumption of plasma-catalyst acetaldehyde (5 ppm). It should be mentioned that high-energy con­
was supper less than that of thermal reactivated catalyst. Specifically, sumptions would be required to treat a few ppm contaminated chem­
the gap between the two methods is approximately 200 J/L for icals in background gases (Mok et al., 2019; Vega-González et al., 2020).
obtaining the same acetaldehyde conversion in the range of 25–70%. Another reason is that high humidities in the feed gas led to a decrease in
The significant difference between the two methods can be explained by energy efficiency (Section 3.3). However, in the feed gas case, the

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N. Matyakubov et al. Journal of Hazardous Materials 415 (2021) 125608

Fig. 8. Optical emission spectrum at 2-mm discharge gap of high-voltage electrode and monolith catalyst at SEI of 40 J/L (total flow rate = 60 L/min; water
amount = 2.5%; SEI = 40 J/L; C2H4O inlet = 5 ppm).

honeycomb discharge operated under high throughput and humid

conditions. In summary, the acetaldehyde removal by the honeycomb
plasma discharge showed a comparable removal efficiency with other
processes. The system operated with the simulated indoor emission of
acetaldehyde as the feed gas, suggesting its practical applicability for
acetaldehyde removal.

4. Conclusion

A honeycomb plasma discharge in a sandwich-type honeycomb

plasma reactor presented high performance of acetaldehyde removal in
the simulated indoor emission of acetaldehyde. The result displayed that
the presence of metal catalysts on the monolith surface is very important
to obtain higher discharge power, resulting in elevated acetaldehyde
conversion. Additionally, the increased flow rate positively affected
acetaldehyde conversion due to the increased O•/O3 generation toward
raised flow rate at constant SEI and acetaldehyde concentration.
Fig. 9. A Comparison between thermal catalytic activity and plasma for acet­ Moreover, the removal efficiency also strongly depended on the hu­
aldehyde conversion based SEI consumption (GHSV = 10,600 h− 1; water midified air, i.e., the conversion rate of acetaldehyde decreased at
amount = 2.5%; C2H4O inlet = 5 ppm). higher humidification of air. However, the plasma-catalyst system
featured at least 60% conversion of acetaldehyde in the contaminated

Table 1
A comparison between several plasma-catalyst systems for acetaldehyde removal process under atmospheric pressure condition.
Type of reactor Catalyst Flow H2O GHSV* C2H4O SEI η EE Ref.
rate (inlet)

Plasma Configuration Materials Shape L/min % h-1 ppm J/L % (g/kWh)

Corona Plasma alone – – N/A 0 N/A 500 210 95 14.7 (Klett et al., 2012)
Plasma alone – – 1 0 1340 200 380 77 2.63 (Chang et al., 2019)
DBD Two stages Mn− Co/HZSM-5 Powder 1 0 1340 200 380 ~96 3.3
DBD Plasma alone – – 0.1 0 1270 500 300 70 7.6 (Jia et al., 2018)
One stage Au/TiO2/SiO2 Bead 0.1 0 1270 500 150 97 42.60
DBD Plasma alone – – 0.1 0 1270 500 150 25 5.4 (Jia et al., 2013)
One stage Ag/TiO2/SiO2 Pellet 0.1 0 1270 500 150 97 21
DBD Plasma alone – – 0.1 0 1270 500 150 55 11.9 (Vega-González et al.,
One stage Ag/TiO2/SiO2 Pellet 0.1 0 1270 500 70/350/ 33/ 15.3/8.1/ 2020)
1150 87/98 2.8
SHD One stage M/Al2O3 (M = Co, Honeycomb 60 1.8/ 10192 5 40/54/ 67/ 0.54/ This work
La, Pd, Pt) 2.5/3.3 66 67/60 0.40/0.30

SHD: Sandwich-type honeycomb plasma discharge; SEI: specific energy input; η: removal efficiency; EE: energy efficiency; GHSV* was calculated based volume of
plasma/-catalyst discharge zone.

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Declaration of Competing Interest humidity using a catalytic non-thermal plasma system over Mn-loaded Y zeolites.
Mater. Lett. 262, 127051 https://doi.org/10.1016/j.matlet.2019.127051.
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Biard, P.-F., 2020. Novel and sustainable catalytic Ruthenium-doped glass foam for
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