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Accepted Manuscript

Title: Treatment of malodorous air in biotrickling filters: a


review

Authors: Piotr Rybarczyk, Bartosz Szulczyński, Jacek


G˛ebicki, Jan Hupka

PII: S1369-703X(18)30379-6
DOI: https://doi.org/10.1016/j.bej.2018.10.014
Reference: BEJ 7065

To appear in: Biochemical Engineering Journal

Received date: 21-6-2018


Revised date: 16-9-2018
Accepted date: 14-10-2018

Please cite this article as: Rybarczyk P, Szulczyński B, G˛ebicki J, Hupka J, Treatment
of malodorous air in biotrickling filters: a review, Biochemical Engineering Journal
(2018), https://doi.org/10.1016/j.bej.2018.10.014

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Treatment of malodorous air in biotrickling filters: a review

Piotr Rybarczyk1, Bartosz Szulczyński1, Jacek Gębicki1,* and Jan Hupka2

1 Gdańsk University of Technology, Faculty of Chemistry, Department of Chemical and Process


Engineering, 80-233 Gdańsk, Narutowicza 11/12 street, Poland
2 Gdańsk University of Technology, Faculty of Chemistry, Department of Chemical Technology, 80-

233 Gdańsk, Narutowicza 11/12 street, Poland


* Correspondence: jacek.gebicki@pg.edu.pl; Tel.: +48-58-347-27-52

Highlights

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 Biotrickling filtration gains importance as a sustainable air deodorization method

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 Selected microbial species and modified liquid phase improve biofiltration efficacy
 Enhanced removal of hydrophobic compounds in two-phase partitioning biofilters

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 On-line monitoring of biofiltration performance with e-nose is proposed

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Abstract: Odour nuisance, resulting mainly from the presence of the compounds containing

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osmophore group and characterized by low olfactory threshold, is associated with danger and may
be the cause of negative psychosomatic symptoms. Among different methods of malodorous air
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treatment, biological methods are of importance, mainly due to reduced operating costs, high
purification efficiency of voluminous gas streams characterized by low concentrations of odorants
and minute secondary pollution. Recently, biotrickling filtration has been one of the most attractive
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biological technique of air deodorization. This paper reviews the state-of-the-art on biotrickling
filtration and special attention is paid to the methods for evaluation of the process performance.
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The review presents the range of odorous chemical compounds that may be removed from air in
BTFs, highlighting the strategies for the removal of hydrophobic odorous air pollutants. The paper
is focused on the literature references regarding biotrickling filtration for the years 2010 – 2018.
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Keywords: biotrickling filter, biofiltration, odors, VOCs, air pollution, biofilter performance

1. Introduction
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Atmospheric air is an indispensable element of biological life. Ongoing progress in economic


and industrial development together with increasing number of people result in emissions of
pollutants of various kinds to ambient air [1–3]. The problem of air quality, especially when related
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to malodorous odors, is gaining importance both for the environmental and social reasons. Negative
impact of air pollutants can result from both intrinsic properties of individual chemical substances as
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well as synergistic amplification of hazardous properties of different chemicals. In some cases,


individual substances reveal small impact on particular element of biotic and abiotic environment,
nevertheless their influence can be significantly increased upon presence of other interacting
compounds [4–6]. Among plenty of chemical compounds, the odorous compounds (odors) play a
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significant role. The odors are volatile organic and inorganic compounds sensed by animals and
humans via olfactory receptors at very low concentrations and identified by brain as unpleasant
sensations [7,8]. Osmophore group contained in a molecule of chemical compound is responsible
for sensing of pleasant or unpleasant odour as well as odour character. Content of osmophore
groups in particular chemical compound also determines value of the parameter characterizing
olfactory threshold. Figure 1 presents exemplary osmophore groups of chemical compounds with
corresponding values of olfactory threshold. It is seen that the values of olfactory threshold may
differ by over a million times (from single ppb to thousands of ppm) depending on the osmophore
group present in chemical compound [9]. Reduction of odours emission to ambient air from different
fields of human activity becomes a priority for many countries all over the world.
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Figure 1. Exemplary osmophore groups of chemical compounds present in ambient air with

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corresponding ranges of olfactory threshold.
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Currently, only eleven out of twenty eight EU countries possess law regulations regarding the
odorous air quality standards [10–12]. The legislative works, however, have been preceding and
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more and more countries will soon implement the mentioned regulations. The sustainable air quality
management may be realized based on following requirements : i/ mitigation of air pollution via
application of BATs (Best Available Technologies), ii/ efficient and environment-friendly methods of
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air purification and deodorization, iii/ efficient and fast-responding air quality control and monitoring
systems.
Among above mentioned management tools, efficient methods of polluted air treatment are of
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special significance. Deodorization of gases polluted with odorous compounds may be realized via:
i/ removal of malodorous pollutants; ii/ transformation of malodorous pollutants into odorless
chemical compounds or the compounds characterized by high threshold of odor sensing; iii/
introduction of masking compounds that change the character or decrease the intensity of the smell.
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Four main groups of techniques used for the reduction of odorants concentration in air are
combustion, absorption, adsorption and biological methods [13]. Short summary of above
mentioned and other methods of deodorization is given in Table 1 [8,14]. Selection of the most
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effective method is difficult and depends on several factors i.e. emission intensity, types and
concentration of pollutants and odorous character of emitted gases [8]. Due to low operating costs,
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high possible effectiveness of deodorization, no secondary pollution and possibility to treat gases
with low odorant concentrations, biological methods, including various types of biofiltration
techniques, are superior compared to other above mentioned methods [15,16]. The growing
emphasis on sustainability will even more stimulate the application of biological processes for gas
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treatment [17] and biofiltration is regarded as a sustainable treatment technology [18].

Table 1. Basic characteristics of selected methods of air deodorization.


Deodorization method Application and advantages Disadvantages
Removal of water-soluble compounds
Wastewater generation and
(i.e. NH3, SO2, CO2, HCl); simple design
Absorption in water secondary odorous emissions,
and operation, low investment and
corrosion problems
operational costs
Treatment of gases from wastewater Wastewater generation, high cost
Absorption with chemical
treatment plants and food industry; high of chemically resistant materials,
reaction
deodorization efficiency, simple application of hazardous reagents
construction
Treatment of gases from food and
pharmaceutical industry; low operational A necessity of ozone removal from
Ozonation
costs, limited secondary pollution, treated gases
elimination of bacteria
Treatment of elevated-temperature
gases (i.e. from asphalt oxidation units); Requires uniform parameters of
Thermal oxidation
simple design and operation, limited treated gas, high operational costs
secondary pollution
Process requires limited
Treatment of gases from paint production
temperature and low gas humidity,
Adsorption and chemical industry; possible recovery
high operational costs, high risk of

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of solvents
sorbent pollution

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Treatment of non-toxic and low- Susceptible to changeable
Masking concentrated odorants; low investment conditions, requires efficient
costs, easy operation, short reaction time ventilation for indoor applications

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Treatment of gases from wastewater
Large surface area of the
treatment plants as well as industrial and
Biological methods installation, problems with

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agricultural facilities; low investment and
microbial overgrowth
operational costs, easy operation

The use of biological methods for the treatment of polluted and odorous air has been known for

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over 60 years. Devices called biofilters are used for this purpose i.e. in food processing plants,
sewage treatment plants and landfills [19]. Initially, bioreactors employing natural packing media
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(i.e.) conventional bioreactors were used. The research was initially concentrated on testing the
effects of packing elements material and applied microbial species. Scientific research as well as
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industrial applications were mainly devoted to the removal of various sulphur or nitrogen
compounds from waste air streams, such as those emitted from wastewater treatment plants [20].
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In general, great majority of studies are devoted to the removal of single compounds. Due to
operational problems of biofilter utilization (e.g. aging of packing materials), other configurations of
biofilters were developed, including biotrickling filters. The research switched to investigations of
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measures of improving the biofilters’ performance by means of various configurations (co-current


streams of gas and liquid phase, application of two or more bioreactors in series). Biotrickling filters
show better performance than traditional biofilters, offer greater process stability and control of
basic physicochemical parameters as well as do not require gas pre-humidification [21]. Current
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research includes investigations regarding an influence of starvation periods, analysis of mixture of


compounds, analysis of microbial species inhabiting the packing bed, process modeling including
unsteady-states, process scaling-upand the problem of the removal of compounds with different
affinities towards aqueous phase, especially hydrophobic compounds. The present paper reviews
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the applications of biotrickling filters, one of the bioreactor types for biofiltration, intended for air
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deodorization. Attention is paid to the methods of gas composition analysis necessary for the
evaluation of BTF performance. In the literature, few papers reviewing the application of BTFs for
odours abatement may be found [16,20,21]. To the best of our knowledge, there is no paper
presenting various approaches for evaluation of a BTF performance in a view of gas phase
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analysis. The paper presents the current state-of-the-art in the field of biotrickling filtration based on
recent literature references (for the years 2010 – 2018).The paper is organized as follows: in the
introductory part, means for the abatement of malodorous odours are described followed by the
general discussion on the biological methods of air deodorization. Then, description of biotrickling
filtration together with main process parameters and current research in the field of BTF are given.
For the clarity of presentation, summary of reviewed research on BTF is given in a form of a table,
presenting the removed substances and selected process. In the last section, the scope of
analytical tools used for the evaluation of a BTF performance is presented and discussed,
emphasizing the advantages of applying electronic nose for such a purpose. The paper ends with a
summary, depicting future development strategies in the field of biotrickling filtration.
2. Biofiltration for air deodorization
In general, the process of biofiltration consists in the decomposition of gas contaminants by
bacteria or other microorganisms inhabiting the porous packing bed of the biofilter. As a result of a
gas flow through the packing, the contaminants from the gas phase diffuse to the biofilm
surrounded by a liquid (usually aqueous) phase (Figure 2). The liquid phase is either supplied via
trickling the bed (mobile liquid phase) or it is supported by the gas humidification prior to its entering
to the biofilter. Pollutants adsorbed on and absorbed by the biofilm undergo biodegradation. Finally,
the cleaned gas leaves the biofilter [22,23].

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Figure 2. General mechanism of biofiltration.

The most popular types of devices used in biological air treatment include biofilters (BF),
bioscrubbers (BS) and biotrickling filters (BTF). Schemes of the mentioned bioreactors are given in
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Figure 3.
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Figure 3. Examples of the common apparatus for biofiltration: (a) biofilter, (b) bioscrubber, (c)
biotrickling filter.

The general mechanism of biofiltration is similar for all given bioreactor types, however they
differ in the construction as well as possible applications. In the case of a typical BF (Figure 3a), the
contaminated gas is humidified in a separate chamber prior to entering the biofilter. The biofilter is
packed with a bed made from natural materials. Microorganisms capable of degrading the
pollutants colonize the BF bed. The first step of biofiltration includes a mass transfer of given
compounds from the gas to the moist bed material or to the liquid phase. Then, the compounds
undergo biodegradation within the so called biofilm layer formed at the surface of packing elements
[16,24,25].
In the case of bioscrubbers (Figure 3b), the components from the gas phase penetrate to the

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liquid flowing counter-currently to the gas phase. The liquid is supplied with activated sludge and

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circulates in a closed system with periodical regeneration and aeration. Thus, the removal of
odorous compounds in BSs includes absorption of the compounds from the gas to liquid phase and
their further biodegradation or biotransformation by either heterotrophic or autotrophic microbes

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[16].
Biotrickling filters (Figure 3c) enable both the absorption and degradation of gaseous pollutants

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to take place in one apparatus. BTF is packed with a bed trickled with a liquid, usually enriched with
the nutrients for microorganisms. The role of the packing elements is to give a support to the
microbial growth and thus enable the biofilm formation. Contrary to BFs, packing of BTFs is made of
inert, usually ceramic or synthetic materials, while natural or biomass origin materials are rarely

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used. Table 2 presents a brief comparison of above given reactor types intended for biofiltration
[26–29].
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Table 2. Comparison of reactors for biofiltration.
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Bioreactor type Advantages Disadvantages
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Low investment and operational costs Decrease of efficiency for highly


Possibility to treat gas streams polluted with concentrated gas streams
a broad scope of chemicals Large surface area requirements
Biofilter
Ease of operation and maintenance Limited durability of a packing
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No secondary pollution Difficulty in controlling the process


Low pressure drop parameters (moisture, pH)
Treatment of high flow rates of gas streams Treatment of hydrophilic compounds
Operational stability Relatively complex operation and
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Bioscrubber Low pressure drop maintenance


Low space requirements Secondary pollution generation (sludge and
liquid waste streams)
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Low operating costs


Durability of a packing material Possibility of accumulation of excess
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Ease of process control biomass


Biotrickling filter
Relatively low surface area requirements Complex construction
Capability of treating acid degradation Secondary pollution generation
products of VOCs
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Another type of bioreactors applied for biofiltration are air-lift bioreactors [44,45]. In such kind of
bioreactors, the contaminant in the gaseous phase is forced to contact with a washing solution. The
biomass is dispersed in the liquid medium and is attached to a support materials suspended in the
liquid phase [46].Because of their high operational flexibility, short reaction time, great processing
capability, good mixing and possibility of achieving enhanced contact between microbial floc and
the substrate, airlift bioreactors have recently indicated their great potential for biopurification of
odours [30]. Airflit reactors have been successfully applied for the purification of air from
compounds such as toluene, trichloroethylene, hydrogen sulfide or phenol [31–34].
Other type of devices for biological gas cleaning are fluidized bioreactors. In a gas-solid
fluidized bioreactor, a bed of discrete particles is used to support microbial growth. The incoming
polluted air streams fluidizes the bed, and VOCs in the air undergo biodegradation by
microorganisms located at the particles [35]. Such an approach brings many advantages because
fluidization promotes homogenous conditions due to the rapid and uniform mixing of particles.
Furthermore, the fluidization state influences the mass transfer characteristics and the efficiency of
bioconversion in a fluidized reactor [36]. Fluidized-bed reactors have been successfully applied for
the removal of ethanol or toluene from the gas stream [35,37].
Biofiltration is an efficient technique applied especially for the removal of H 2S and NH3 from
gases originating from municipal and exhibiting particularly high odor nuisance [38,39]. Great
majority of the published studies on biofiltration concern the removal of single compounds belonging
to the group of volatile organic compounds (VOCs), e.g. toluene, ethanol, propanol, hexane [40–

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44]. Odor compounds are removed in biofilters packed with various types of beds: beds of natural

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origin (compost, peat, wood chips, composted leaves, waste biomass), ceramic elements, elements
from stainless steel and polyurethane foam. Unfortunately, relatively few papers concern the
biofiltration of a mixture of compounds [45–51]. The investigated mixtures are usually two- or three-

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component. Mixtures with such a lean composition serve as a poor model for real gas streams, i.e.
those arising from municipal landfills or various industrial plants.

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Biofilters are typically designed for the removal of water-soluble substances. This is
accomplished by moisturizing the filter packing elements with water, resulting in formation of
hydrophilic biofilm. The efficiency and the rate of removal of hydrophilic compounds is governed by

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the rate of their biodegradation by microorganisms inhabiting the biofilm. It is contrary when
compounds having greater affinity to the organic than aqueous phase are considered [44,52,53]. In
such a case, the efficiency treatment of such compounds may be low as a result of the low driving
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force (i.e. low concentration gradient) due to low transfer rates from the gas phase to aqueous
phase, including biofilm [54]. Therefore, a crucial step for the design of a biofiltration system is the
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definition of the main resistance to mass transfer (either mass transfer limitation or biological activity
limitation) [55]. Biofiltration of hydrophobic compounds, as given above, proceeds with a much
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lower yield than hydrophilic compounds and the treatment effectiveness depends on the rate of
mass transport of the component from the gas phase to the biofilm. The improvement of biofiltration
of hydrophobic compounds is a challenge in the biofilter design and it is currently the main research
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topic in this area [21,24,46]. In addition, attention is paid to the interaction between the groups of
compounds for synergistic or inhibitory effects of their simultaneous removal from gaseous streams
[56]. The key element responsible for the efficient performance of the biofilter is the presence of
microorganisms capable of decomposing specific chemical compounds. Biofilter beds are inhabited
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either by autochthonic or specially selected species of microorganisms using the pollutants of the
treated gas as an energy source. A promising solution for the effective removal of hydrophobic
compounds may be biotrickling filtration, especially when two-phase liquid systems are concerned
[57].
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3. Biotrickling filtration
Biofiltration by means of biotrickling filtration is currently considered to be the most promising
technology of biological air treatment [27,58,59]. This is mainly due to increased process stability,
ease of pH and temperature control and regulation, continuous nutrient supply, low flow resistance
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and reduced space requirements, comparing to traditional biofilters[16,21,60,61]. Additionally, the


application of a mobile liquid phase i.e. trickling liquid provides means for the washing out from the
bed the biodegradation intermediates which may inhibit the metabolic activity of the microorganisms
in traditional biofilters[62].
Biotrickling filters show especially high abatement performance for the treatment of H2S and
other water-soluble compounds [54]. However, for the biofiltration processes a challenge is the
treatment of pollutants hardly soluble in the aqueous phase i.e. hydrophobic compounds. However,
this drawback may be overcome to some extent in BTFs because of the possible modification of a
liquid phase e.g. by surfactant addition or two-liquid phase partitioning apparatus [16,24,46].
In a biotrickling filter, the gas is passed through a packed bed irrigated with a trickling liquid
which contains essential nutrients allowing the growth of microorganisms in the biofilm. The
mechanism of the process consists in simultaneously occurring processes of absorption of the
target compounds in the liquid surrounding the biofilm and their adsorption onto the biofilm-covered
particles followed by the subsequent biodegradation of the compounds in the biofilm (compare
Figure 2). The development of a biofilm is possible after inoculating the packed bed with
microorganisms because inert packing materials are used [16].
The key element of a BTF is a biofilm formed on the elements of a packed bed [28]. The biofilm
contains various kinds of microbes thanks to activity of which the transformation of pollutants to
inert final products take place. The microorganism types include bacteria, fungi, yeasts and molds.
The formation and growth of a biofilm is affected by several factors including pH, temperature,
oxygen concentration and the presence of nutrients and microelements [21]. The thickness of the

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biofilm, depending on a packing material and operating conditions, may vary from several

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micrometers up to several millimeters. The accumulation of biomass in BTF may finally result in
clogging when the biofilm thickness is too high. Such inconvenient conditions are depicted by an
increased pressure drop, bed channeling and a decrease in the removal efficiency [28].

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An important parameter for the functioning of a BTF is a pH of a trickling liquid. It is because
there are optimal values of pH ensuring the efficient activity of microorganisms. Usually, the optimal

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pH is close to neutral i.e. 7, but depending on the pollutants treated, acid products may be formed
(e.g. in the case of VOCs containing hetero-atoms) [28]. The pH control is usually performed by the
addition of caustic soda to the liquid [21].

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Biotrickling filters are superior to other types of bioreactors when both efficiency and economy
of the process is taken into account. The analysis and comparison of biotreatment with either
traditional biofilter or biotrickling filter was done e.g. by Morotti et al. [63]. According to Hernandez et
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al. [64], when considering two-liquid phase reactors, costs of air treatment are the lowest for BTFs
as compared to traditional stirred tank bioreactor or air-lift bioreactor (Table 3).
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Table 3. Comparison of reactors for biofiltration [64].


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Bioreactor Volumetric rate transfer for Power consumption per 1 m3


R/P, g h-1 kW -1
type VOC, g m-3 h-1 of treated gas (P), kW m-3
Biotrickling
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104 0.01 7618


filter
Stirred tank
88 21.91 4
bioreactor
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Air-lift
41 0.06 720
bioreactor

The research regarding BTFs is predominantly focused on the removal of single compounds,
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while the investigations on the mechanisms of mixed-pollutants removal are still in minority
[54,65,66]. In the perspective of industrial applications of BTFs, investigations on the removal of
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mixture of compounds is indispensable.

4. Operation of biotrickling filters


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4.1. Performance measures and important process parameters


The performance of BTF is usually described by three basic parameters, i.e. removal efficiency
(RE), elimination capacity (EC), and inlet loading rate (IL)[67], as given in following equations:
𝐶𝑖𝑛 − 𝐶𝑜𝑢𝑡
𝑅𝐸 = (1)
𝐶𝑖𝑛

𝑄 ∙ (𝐶𝑖𝑛 − 𝐶𝑜𝑢𝑡 )
𝐸𝐶 = (2)
𝑉
𝑄 ∙ 𝐶𝑖𝑛
𝐼𝐿 = (3)
𝑉

where: Cin, Cout – concentrations of target compound in the inlet and outlet streams, Q – gas
flow rate; V – volume of the filter bed.
Another important parameter describing the performance of BTF is the empty bed residence
time, EBRT, defined as follows [20]:
𝑉
𝐸𝐵𝑅𝑇 = (4)
𝑄
EBRT is usually of the order of several tenths to hundreds of seconds, and EBRT is higher at
the initial stages of BTF operation and may be decreased when stable conditions are reached [68].

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In general, an increase in EBRT results in an increase of RE. However, lower values of EBRT

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correspond to higher values of EC [69]. Additionally, Schiavon et al. [21] postulates a need for
compromise when expected RE and EC are regarded for large-scale processes so as to assure the
economic feasibility of the system operation. It is because maximal EC values are obtained at

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different conditions than in the case of RE due to increased inlet loading and decreased EBRT.
Among various operational parameters investigated for the operation of BTFs, following may

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be listed as critical for the bioreactor performance: the inlet pollutant load, pH, starvation periods
[70], biodiversity of microbial communities [71] and inoculation with different types of microbes [72],
working temperature and the packing material of the bed [73]. For example, operation of BTF at

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higher than ambient temperatures may improve both the elimination capacity and the ease of
operation of BTF [74]. Additionally, increased temperature during the BTF process may result in
reduction of operational stability problems such as organic acid production, pH decrease, foaming
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and clogging.
The effectiveness of biofiltration process is governed by the microbial activity in the biofilm.
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Thus, the assurance of the correct pH value is crucial for a given types of microbial communities.
Additionally, the efficiency of the process may be increased by applying pre-treatment operations,
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i.e. a hybrid process with UV radiation [15,68] (UV-BTF) for air deodorization.

4.2. Design of BTFs


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Biotrickling filtration is performed by using co- or counter-current flow of gas and liquid phases
[16]. Typically, a BTF consists of a packed column to which a gas phase and liquid phase (trickling
liquid) are supplied (Figure 3c). The mentioned phases may be supplied either co- or counter-
currently. The predominant option is to use the counter-current mode, which is typically convenient
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for absorption and related processes. However, due to the possible problems of clogging of lower
sections of a BTF filling (i.e. due to the biomass overgrowth), co-current mode is of interest.
Exemplary configurations of BTFs are given in Figure 4.
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An interesting approach towards the design of BTF is presented by Chen et al. [75]. The
proposed configuration consists of two packing layers in one column i.e. activated carbon-loaded
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polyurethane (an upper layer) and modified organism-suspended fillers (a lower layer). The location
of the packing resulted from the fact that the modified organism-suspended packing exhibited much
better mechanical strength and lower flow resistance than the polyurethane filler, which was
beneficial for mass transfer. Consequently, it was packed into the bottom layer, while the
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polyurethane with activated carbon was packed into the upper layer due to its porosity, thus
benefiting the gas distribution and prolonging the interfacial contact time. Both of above described
BTF layers were equipped with spray nozzles to deliver the trickling liquid over the packing.
Chaiprapat et al. compared the performance of a triple to single stage BTF [76]. The proposed
step feeding of the trickling liquid clearly resulted in an increase of a BTF performance.
BTFs are also combined with other processes to increase the overall treatment efficiency,
especially when persistent chemical compounds are treated. He et al. [77] investigated the removal
of mixture of VOCs from a paint production plant by means of BTF coupled with photocatalytic
oxidation, obtaining almost complete degradation of VOCs (RE~98%) compared to the removal
efficiency of about 70% when single BTF process was applied.
Various scale of BTFs apparatus are the subject of investigations from laboratory, through on-
site pilot [78,79] to full-scale industrial applications [80,81].

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Figure 4. Counter-current three-layer BTF (a), co-current BTF (b) and two-stage BTF (c).

4.3. Packing materials


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A packed bed is a crucial element of the BTF. It is so because it provides a necessary support
for the growth of microbes and is expected to ensure the possible high contact area between liquid
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and gas phases [16]. Various types of materials are used, including ceramic elements, polymeric
materials, open-pore synthetic foams, lava rock, glass beads, tire-derived rubber particles and
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organic materials like wood chips [70,82,83] .


A good packing material should have following properties [84]:
• High porosity for efficient distribution of a gas phase; the preferred porosity range is
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between 35 and 40%.


• High specific surface area enabling the development of the biofilm and increasing the
mass transfer from gas to biofilm.
• High water retention in order to prevent the bed drying.
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• Good bed drainage to wash out the reaction by-products.


• Good buffering capacity i.e. ensuring maintenance a pH of at least 3 which is vital when
inorganic contaminants are treated in biofilter.
• The material should be odorless.
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• The packing should offer low gas-phase pressure drop.


• The surface of the material should be hydrophilic to allow retaining of water which is very
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important to maintain water in the biofilms.


• Biofilter media should be possibly cheap and durable.
In general, BTFs employ synthetic or ceramic materials as bed packing (see Table 3) while the
application of natural materials is very limited. Synthetic bed materials favor the maintenance of a
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relatively constant pressure drop, lower than in the case of natural materials[16].
Due to the importance for biofiltration processes, packing materials have been thoroughly
investigated and evaluated in the literature[16]. Except for natural packing materials e.g. wooden
chips or pine bark, which are most used in traditional biofilters, plastic and ceramic fillings (Pall,
Rashig rings) have been applied in biotrickling filters. Such materials have been applied in
numerous studies and proved beneficial because of their stability, low cost and high porosity.
However, due to biofilm formation, especially plastic elements is difficult and thus the biofiltration
start-up process is relatively slow[85].
A relatively new packing materials applied in biotrickling filters are open-pore polyurethane
foams which were applied in the studies by Shareefdeen et al. in 1993[86]. Moe and Irvine
reportedmethods for manufacturing and characterizing polyurethane sponges tested to be suitable
for use in gas-phase biofilters[87]. An undoubted advantage of this type of filling is its open structure
and high porosity. This results in low pressure drop through the packing, corresponding to high gas
flow rates. Polyurethane foams are currently used as single elments or structural fillings. They were
successfully used for removal of toluene, hydrogen sulfide, ammonia or 2-
bytoxyethanol[62,83,88,89]. Additionally, it is possible to obtain polyurethane foams with specific
functional properties, which allows for the selection of the optimal packing characteristics for a
specific application of a biotrickling filter[90].

4.4. Microbial communities


Microorganisms are said to be the engine of the biotreatment process [16]. Taking into account

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the mechanism of air deodorization in BTFs, the microbial flora inhabiting the filter packing is a
crucial element enabling the biodegradation of the pollutants. The start-up procedure of biofilters

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may be realized with the use of different types of inoculums. Two main strategies include the
application of activated sludge from wastewater treatment plans or pure cultures of microbes. From
an economic view-point, the use of activated sludge from wastewater treatment plants is preferred

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due to ease of implementation and lower operational costs. On the other hand, the use of pure

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cultures as inoculum sources ensures shorter start-up periods and elimination of the possible
emissions of potentially pathogenic germs. It is worth noting that comparative studies of the
performance of similar bioreactors but for various inoculums sources are scarce in the literature
[89].

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According to Mudliar et al. [28], microorganisms are the catalysts for biodegradation and the
resulting deodorization of gas streams. The bed inoculation depends primarily on the type of
N
compounds to be treated, but also on the type of a packing material.
The formation of the biofilm in BTFs operating in acidic and neutral conditions was studied by
A
Tu et al. [91]. Biofilm formation is a dynamic process and its formation is said to be dependent upon
the microbial species, surface properties and various environmental factors. The development of
M

microbial communities with a broad tolerance range of pH, which is vital for a well-performance of a
BTF, may be accomplished by a combination of acclimated microbial consortia (prepared in
laboratory) with the activated sludge. The biofilm structure and stability depends on the pH and the
inlet loading rate. Additionally, the performance of BTF is said to be more dependent on the
ED

microorganism type than on the biomass quantity.


The biofilm formation may be preceded by inoculating the microflora onto the surface of
packing elements. The time of immobilization is rather long, reaching about 4-5 weeks while the
stable conditions are obtained within about 2 months [79]. The time required for the formation of a
PT

biofilm may be reduced e.g. by secondary acclimation of the microbial consortia for given set of
pollutants [92].
BTFs are generally inoculated with mixed microbial consortia. The choice of inoculum influence
E

the start-up of a BTF, the removal of pollutants and the reactor stability. BTFs may not achieve
satisfactory performance or some recalcitrant VOCs treatment due to slow microbial adaptation and
CC

growth. Bioaugmentation has been reported as a good alternative to enhance the degradation of
the recalcitrant compounds. It is a process in which selected strains are introduced into a biological
system to enhance the biological degradation activity and further improvement of the process
efficiency [17].
A

Elimination of dichloromethane from air streams by biotrickling filtration (alone or UV-assisted)


was investigated by Jianming et al. [15]. The results indicated that the for a UV-BTF system the
resulting biofilms consisted of diversified microbial communities. It is said that the increased
microbial diversity of UV–BTF improved VOC removal compared to BTF. Greater biodiversity is
known to increase ecological stability, and bacterial community evenness helps to maintain the high
performance of a bioreactor.
According to [93], the application of fungi may be of importance in comparison to bacteria.,
however the research regarding the application of fungal biofilters to treat VOCs is not broad. A
styrene degrading fungus, Sporothrixvariecibatuswas employed for styrene removal. That fungus
remained dominant in the biofilter reaching high elimination capacities. One of the main advantages
of stimulating fungal rather than bacterial growth for the biofiltration of hydrophobic VOCs is their
ability to completely mineralize these compounds under harsh conditions like acidic pH, low water
content and limited nutrient concentration.
Vergara-Fernandez [66] investigated the removal of three-component mixture (benzo[α]pyrene,
toluene and formaldehyde) using a mixed bacterial and fungal inoculation in a three-stage biofilter
with periodic trickling of mineral medium. Vermiculite was used as a packing material. It was found
that a proposed system effectively removed the mixture of above given odorous compounds from
air. The first stage of a biofilter (bottom) was predominantly inhabited by fungi, while the second and
third was colonized mainly by bacteria. A proposed system ensures high flexibility of gas treatment
in a broad range of investigated parameters (e.g. EBRT 30 – 154 s).
According to Estrada et al. [40], bacterial biofilters present a high microbial diversity and
robustness while fungal biofilters can withstand process instability and sudden pH changes.

T
However, fungal biofilters exhibit better performance for the treatment of hydrophobic VOCs.

IP
Additionally, it is found that presence of fungi is mainly responsible for the maintenance of functional
performance of a BTF during the fluctuating conditions [94].
The control of the biomass growth in the BTF is a very important operational aspect. The

R
applied measures of the limiting the biomass overgrowth include backwashing and bed stirring
(mechanical methods), chemical methods including nutrient or water deficiency, biological methods

SC
with starvation periods or application of biomass predators [21,28]. Increasing the rate of the liquid
spraying over the packing bed together with draining and refilling with a fresh trickling liquid may
also help to eliminate the problem of clogging [79,92].

U
Control of the bed clogging as a result of accumulation of the end-products of biodegradation
on the 3D-printed honeycomb-monolith packing was investigated by Qui and Deshusses [95]. It was
found that pigging may be an effective means for the removal of the accumulated products.
N
The current research regarding BTFs more and more often includes the determination and
quantification of microbial species occupying the packing elements [96–99]. Such an approach is
A
accomplished by the use of various techniques including e.g. qPCR. Selected examples of the
composition of biofilm, depending on the treated compounds, is given in Table 4.
M

Table 4. Selected research on the analysis of microbial species forming the biofilm.
ED

No Inoculation Identified species Target compound Reference


Fusarium solani B1 (CBS Mixture of
117476) and toluene,
1. Only microscopic observation [100]
Rhodococcus formaldehyde and
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erythropolis DSM 43066 benzo[a]pyrene


Bacteria:
Phyla Proteobacteria (alpha pinene or toluene
degradation), Actinobacteria (butanone or toluene
E

degradation), Nitrospira (toluene, hydrocarbons


Activated sludge from degradation), “Candidatus Saccharibacteria” TM7
CC

2. the municipal wastewater (toluene degradation) [94]


treatment plant Fungi:
Pezizomycotina subphylum (degradation of large
range of organic pollutants e.g. toluene,
ethylbenzene), Fusarium (aromatic hydrocarbons),
A

Chaetothyriales (toluene)
Purified colonies from
3. Bacillus sp.(Iso 7, B17) xylene [53]
the activated sludge
Sludge from full-scale Halothiobacillus neapolitanus
4. H2S [101]
activated sludge system NTV01
Microbial consortia
Achromobacter and Benzene, toluene,
5. enriched from petroleum [102]
Burkholderia xylene, styrene
polluted soil
Activated sludge from Bacillus sphaericus,
6. wastewater treatment Geobacillus H2S, NH3 [103]
plant thermoglucosidasius,
Micrococcus luteus (ATCC
9341)
Acclimated microbial
consortium from working [104]
7. Acidothiobacillus genus H2S
biofilter mixed with
activated sludge
Activated sludge or Acidobacterium, Rhodococcus
8. Toluene [105]
Burkholderia sp. T3 and Burkholderia

Biofiltration in its typical mode works by oxidation of treated compounds. However, anoxic
conditions may also be applied during the biological treatment. Comparison of aerobic and
anaerobic BTF for the degradation of volatile trihalomethanes on the example of chloroform was
investigated by Megebe et al. [106]. Treatment of H2S with BTF in anoxic conditions was studied by

T
Saucedo-Lucero et al. [107]. The authors conclude that the anoxic mode may be applied for gas

IP
streams where their dilution with oxygen may result in explosion, however the efficiency of
anaerobic treatment is lower than in the case of aerobic conditions.

R
4.5. Trickling liquid and its modifications

SC
A liquid mobile phase is a characteristic element of each BTF. The trickling liquid may be batch
or continuous [108]. An influence of the recirculation rate of a trickling liquid was investigated in
paper [59]. It was concluded that an increase in the recirculation rate was followed by an increase in
the removal efficiency when constant EBRT was taken into account. The operational ratio of gas to

U
liquid phase flow rate is typically of the order of several tenths [68].
Liquid trickled over the packing of a biofilter ensures humid conditions necessary for the
N
support of biofilm and microbial life. Additionally, nutrients present in trickling liquid enable the
efficient working of a biofilm [28]. Typically, BTFs employ aqueous solutions of nutrients (N, P, K, S)
A
and microelements, (vitamins, metals). Such systems are of importance when dealing with
hydrophilic compounds. Obviously, maintenance of a desirable pH value is accomplished by
M

regulating the pH of a trickling liquid.


An increase of the removal efficiencies of hydrophobic odorous compounds in biotrickling filters
may be accomplished i.e. by using 2-phase liquid by modification of the aqueous phase with an
organic phase, by addition of polymers or by addition of surface active substances. The concept of
ED

applying two liquid-phase systems arises from the enhanced biodegradability of hydrophobic
compounds when organic phase is present except water. The strategies include e.g. the addition of
silicon oil, paraffin oil and rubber tires from used tires among others [26,87]. Montes et al.
investigated the removal of α-pinene with aqueous phase supplied with silicone oil [110]. The
PT

removal of α-pinene increased tenfold as compared to the use of aqueous phase alone.
The problem of enhancing the solubility of CH4 in aqueous phase by the application of a two-
liquid phase partitioning BTF was studied by Lebrero et al. [57]. Additionally, microbial consortia
E

dedicated to the treatment of hydrophobic compounds were applied, resulting in an enhanced


methane removal in the investigated systems.
CC

Beside the composition of a trickling liquid, the liquid flow rate and its recycling are important
parameters regarding the performance of BTF. It is because the contact between the
microorganisms and the pollutants is possible only after the diffusion of pollutants in the liquid.
According to Mudliar et al. [28], early investigations of BTFs suggested that the greater gas-liquid
A

interface is generated for increased rates of the liquid flow, and thus the mass transfer is increase
and the BTF performance is greater. Moreover, it was found that the trickling liquid flow rate is a key
operational cariable in BTF system and has more impact on the rate of VOCs mass transfer from
gaseous to liquid phases than the inlet gas flow rate [64].
Application of BTFs with two-phase trickling liquid allows for an increased removal capabilities
in comparison with traditional BTF configuration (without the addition of an organic phase) when
hydrophobic compounds are to be treated [111].

4.6. Summary of research on BTF


The development of investigations on biotrickling filtration has been observed since the
beginning of 1990s. Initially, the investigations were concentrated on assessing the impact of basic
process parameters (e.g. EBRT, temperature, pH, flow pattern of phases) on the process
performance. Then, the researched switched to analysis of other various aspects of BTF, including
biofilm formation, application of various species of microbes, process scaling-up and analysis of
BTF performance for a mixture of VOCs. Table 5 presents a brief layout of research on BTF before
2010.

Table 5. Selected research on biotrickling filtration before 2010.

Removed
No. Topic of the study Year Reference
compound(s)

T
Influence of
1. BTEX 1999 [112]
temperature effects

IP
Application of
protozoan predation in
2. Toluene 1999 [113]
the biomass growth

R
control
Verification of
3. Dichloromethane simplified model for a 1991 [114]

SC
biotrickling filter
Application of two
liquid phases for
4. Alkanes 1999 [115]
improved removal of

5. H2S and toluene


lipophilic compounds
Simultaneous removal U 2002 [116]
N
of H2S and toluene
Highly effective
A
6. Nitrobenzene removal of 1997 [117]
nitrobenzene vapors
7. Toluene Application of fungi 1996 [118]
M

Investigations on
8. Toluene 1997 [119]
degradation kinetics
Successful industrial
9. Various 2001-2005 [28]
implementation of BTF
ED

Investigations on
10. Toluene effects of the liquid 2000 [120]
flow rate
Investigations on the
[21]
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11. Various oxygen availability 2005


within the biofilm
Investigations on the
12. BTEX startup period after 2007 [121]
E

BTF inoculation
CC

Table 6 presents the literature research on BTF with the focus on papers published in years
2010 – 2018. For the clearness of presentation of the range of odorous compounds treated in BTFs,
values of their Henry’s constant are given. Low values of H indicate that a compound is
A

hydrophobic, while high Henry’s constant values represent high hydrophilicity. In the final part of the
table there are also examples of the use of BTF for the removal of mixtures of odorous compounds.

Table 6. Summary of research on removal of odorous compounds by biotrickling filtration.


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``

SC
No. Removed Henry’s Packing Microbial flora Trickling BTF EBRT, Cin / IL RE Performance Aim of REF
substance constan material liquid dimensions, s evaluation investigations

U
t1 m
H D

N
1 Methane 0.00001 Polyurethane Type II MSM 1.00 0.080 240 IL: 0 – 500 ~40% GC-TCD Improvement of [57]
4 foam cubes methanotroph g m-3 h-1 methane abatement

A
M .sporium, in two-phase BTF
hydrophobic applying

M
microbial hydrophobic
consortium methanotrophs
2 Cyclohexane 0.00005 Polyurethane Acivodoraxsp. ASMM 1.00 0.318 18-37 0 – 720 ~99% Micro-FID Effects of EBRT, IL [122]
3 ED foam CHX 100 mg m-3 and starvation
periods on BTF
performance and
microbial diversity
3 Ethylene 0.00005 Perlite and Activated ASMM 0.81 0.010 30 8-100 70-95% FTIR Influences of liquid [51,
PT

9 glass beads sludge from mg m-3 spectrometer recirculation flow 52]


WWTP rates
4 Vinyl chloride 0.00038 Granular Activated ASMM 0.90 0.100 60 10-35 mg ~45% GC-FID Effect of process [123]
E

activated sludge form m-3 parameters


carbon mixed PVC WWTP (temperature, IL,
CC

with compost flow rates, pH) on


the removal
efficiency in pilot-
scale BTF
A

5 α-pinene 0.00058 Lava rock Mixed ASMM / 0.33 0.090 14-60 - - - Influence of addition [110]
microbial organic of an organic phase
culture phase to aqueous trickling
addition liquid
6 Hydrogen 0.001 Pall rings Aerobic sludge MSM 0.50 0.070 29-131 343-2003 99% Electrochemical Effects of packing [99]
sulfide from WWTP ppmv H2S sensor materials and pH on
the BTF
performance and
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SC
microbial diversity
Two-layer: Activated ASMM 1.8 0.25 53-79 15-50 mg <99% H2S sensor Effects of IL, EBRT, [70]

U
activated sludge from m-3 (analyzer) pH and starvation
carbon-loaded secondary time on BTF

N
polyurethane, sedimentation performance
modified tank

A
organism-
suspended
filler

M
Polypropylene - - 0.70 0.071 118 2000 – - Electrochemical Development of [108]
Pall rings 10000 H2S gas sensor dynamic model
ED ppmv describing
desulphurization of
biogas highly
loaded with H2S
HDPE random Halothiobacillu Thiosulp 0.56 0.475 40-120 0-1500 GFM41 biogas Effects of process [124]
PT

packing media sneapolitanus hate ppmv analytic parameters (EBRT,


NTV01 mineral handheld flow rates, IL) on
medium instrument BTF performance
E

Coconut husk Wastewater ASMM 0.30 0.044 100- 165-304 g 80-95% H2S analysis Effects of EBRT, [76]
mixed with from a digester 180 m-3 h-1 with cadmium liquid recirculation
CC

plastic pieces effluent from a sulfide method velocity and packing


storage pond bed configuration
in latex factory on the BTF
performance
A

Pall rings / Aerobic sludge ASMM 0.50 0.070 29-432 2000 ppmv <99% Electrochemical Effects of packing [99]
random from WWTP H2S sensor and pH on BTF
packing performance with
assessment of
microbial diversity
Open-pore Thiobacillusde ASMM 0.32 0.106 9-57 20-157 ~95% H2S sensor Effects of sulphate [83]
polyurethane nitrificans ppmv concentration, pH,
foam flow rates and IL on
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SC
the BTF
performance with

U
bacterial community
analysis

N
Bamboo Sulfide- ASMM 3.00 0.600 11.1-25 3.5-20 ~99% Online and Investigations of [73]
charcoal and oxidizing ppmv portable H2S operating

A
ceramsite bacteria detectors parameters
(activated (pressure drop, IL)
sludge from and metabolic

M
WWTP) pathways of
elemental S
Stainless steel
ED water 0.60 0.071 33-130 2000-1000 <90% Electrochemical Influence of H2S [125]
Pall rings ppmv sensor concentration and
gas contact time on
performance of
long-operated BTF
PT

3D-printed Activated ASMM 0.22 0.060 41 ~1000 ~95% Portable H2S Effects of H2S to O2 [95]
mesh sludge from ppmv analyzer ratio and analysis of
honeycomb WWTP mixed (Jerome 631-X) the fate of sulfur
E

monolith (PLA) with sulphur end products


oxidizing
CC

bacteria
Volcanic Mixed: ASMM 0.60 0.080 - 7.5-25 g 55-99% GC-FPD Effect of pH and IL [91]
stones acclimated m-3 h-1 on the BTF
microbial performance
A

consortia with
activated
sludge
Structured Mixed water 2.74 1.520 3-10 30-550 ~99% Electrochemical Effect of low EBRT [81]
synthetic microbial ppmv sensors, and high IL on the
EcoBase consortia olfactometry performance of a
media full-scale BTF
7 Ethylbenzene 0.0014 Open-pore Activated ASMM 0.78 0.010 15-60 720-2100 <99% GC-FID Comparison of the [126]
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SC
reticulated sludge from with the mg m-3 BTF performance
polyurethane WWTP addition (EBRT, IL) for

U
sponges of trickling liquid
Tween- enriched with

N
20 and Tween-20 and
Zn(II) Zn(II)

A
8 Toluene 0.0015 Polyurethane Acclimated Sulphate- 1.00 0.080 7-50 1-15 g m-3 ~70% GC-FID Development of a [55]
foam activated free model
sludge MSM characterizing a

M
mass transfer of
VOCs in BTF
Polyurethane
ED - MSM 1.00 0.080 7-50 5 g m-3 ~80% GC-FID Modeling and [127]
foam cubes verification of mass
transfer phenomena
in BTF
Kaldnes K1 Fresh activated MSM 0.60 0.070 180 2.5 g m-3 ~40-50% GC-FID, GC- Comparison of two [107]
PT

rings sludge TCD BTFs with different


liquid recycling and
renewal rates
E

Vertical bundle Nitrosomonas, water 1.00 1.950 - 14-20 mg <95% Olfactometry Analysis of the odor [128]
of plastic tubes Nitrobacter m-3 removal from a pig
CC

glued together production farm in a


BTF
9 Chloroform 0.0025 Pelletized Anaerobic ASMM 1.30 0.076 266.4 5 ppmv 60-80% GC-FID, GC- Removal of [106]
diatomaceous (Azospira sp.) with TCD gaseous chloroform
A

earth and aerobic additives in anaerobic BTF


(Fusarium sp.) and comparison
bacteria with aerobic BTF
10 Chloroben- 0.0027 Pelletized 1st BTF: MSM 0.95 0.080 20-90 200-800 >90% GC-FID Evaluation of the [72]
zene polyurethane Ralstoniapicket mg m-3 potential utility of
foam balls tii L2; 2nd BTF: bioaugmentation of
enriched BTF with
activated Ralstoniapickettii L2
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SC
sludge strain for increased
process efficiency

U
Activated Activated ASMM 1.20 0.100 28-90 649 – 2020 90-99% GC-FID Effects of EBRT [129]
carbon and sludge from mg m-3 and IL on steady-

N
multi-surface WWTP state operated BTF
hollow balls

A
11 Ethanethiol 0.0028 Ceramic Commercial MSM 1.20 0.140 66-332 0.42-2.03 45-70% GC-FID Comparison of the [69]
particles mixed culture mg dm-3 performance of BTF
B350 with RG- inoculated with RG-

M
1 strain 1 or B350
isolated from microorganisms
ED WWTP
12 Dichloro- 0.0036 Ether-based Acclimated ASMM 0.70 0.120 22-46 420-800 <85% GC-ECD Effects of combined [15]
methane polyurethane sewage sludge mg m-3 treatment
foam elements from WWTP (ultraviolet
pretreatment and
PT

BTF) on RE and
microbial diversity
13 Styrene 0.0038 Polypropylene Pseudomonas ASMM 3.51 1.080 41 - 62 0,2 – 1 g 78-94 GC-FID, OD, Elaboration of a [79]
E

Ralu rings sp. E-93486 m-3 HPLC for liquid mathematical model
for VOC removal in
CC

BTF
Polypropylene Activated MSM 1.63 0.114 15-30 55-312 ~90% Total Development and [78]
rings (lab sludge from mg m-3 hydrocarbon validation of a
scale) WWTP analyzer three-phase
A

dynamic model of
industrial-scale BTF
Polyurethane Pseudomonas ASMM 0.70 0.120 10-70 0.5-4 g m-3 ~65% GC-FID Analysis of BTF in [68]
foam putida mixed transient and
with activated steady-state with
sludge microbial analysis
Polypropylene Activated MSM + 1.63 0.144 15-30 55-323 mg 84-89% Hydrocarbon Investigations on [111]
rings sludge from silicone m-3 analyzer BTF performance in
R I
SC
WWTP oil NiraMercury 901 two-phase
partitioning BTF

U
Modified Activated - 0.80 0.010 28-113 195.2 – ~98% GC-FID Effect of secondary [92]
ceramic pellets sludge from 2112.3 acclimation on the

N
WWTP mg m-3 rapid development
of biofilm

A
Fern and Liquor of ASMM 0.48 0.4 21 161-2390 ~80% GC-FID Comparison of the [130]
plastic chips activated with milk mg m-3 performance of two
sludge pond kinds of packing

M
from WWTP
15 Methyl 0.052 Ceramic Activated Enriched 1.10 0.120 200- 0.12 – 7.5 <99% GC-FID Influence of EBRT [131]
acrylate ED particles sludge mineral 400 g m-3 and IL on BTF
medium performance with
assessment of
bacterial diversity
16 Ethyl acetate 0.059 Walnut shell Pseudomonas ASMM 1.00 0.062 60-75 10-5000 <99% GC-FID Testing of [132]
PT

putida PTCC ppm performance of


1694 inoculated walnut
shells for ethyl
E

acetate removal
17 Triethylamine 0.071 Lava rocks Activated Enriched 1.50 0.210 31-312 40-2600 99% UV-Vis Effects of EBRT [59]
CC

sludge from ASMM mg m-3 spectrophoto- and liquid


WWTP metry recirculation flow
rate on BTF
performance
A

Ceramic Commercial ASMM 0.60 0.140 42-166 0.1-0.6 mg ~99% no information Testing of B350 [133]
particles mixed culture dm-3 group of bacteria on
B350 the BTF
performance
Polyethylene Aminobactera ASMM 1.70 0.077 85-170 ~95- GC-FID Determination of the [97]
rings minovorans 100% elimination capacity
DSM 7048 of triethylamine in
BTF
R I
SC
18 Ammonia 0.59 Polyurethane Liquor from a ASMM 0.55 0.050 60 100-600 <99% Phocheck Studies of ammonia [62]
foam cubes bioreactor with ppm photoionization removal in BTF via

U
treating nutrients detector simultaneous
wastewater nitrification and

N
with phenol denitrification
and

A
formaldehyde
Mixture of RW - ASMM 1.80 0.500 31-156 200-600 ~95% Gas detection Influence of high [134]
materials and ppm tubes recycle liquid flow

M
chicken feces rate on the removal
of NH3
Polyurethane
ED Aerobic ASMM 0.50 0.090 2.1- 100-1400 ~95% Portable multi- Determination of [135]
foam cubes nitrifying 45.7 ppmv gas detector limits of possible EC
sludge MX6 iBird of NH3
19 1-butanol 1.1 Nutrient- Acclimated MSM 0.67 0.115 60-124 < 4.65 g m- <99% GC-FID Investigation on the [29]
3
enriched forest soil BTF performance at
PT

perlite aqueous high IL of H2S


suspension
20 Aniline 1.1 Ceramic Commercial ASMM 0.60 0.140 42-166 0.1-0.6 g <99% GC-FID Approach to [98]
E

particles mixed culture m-3 describe the


B350 mechanism of
CC

aniline removal in
BTF
21 Isopropanol 1.3 Mixed: random - Water 1.20 0.144 - - - Hydrocarbon Mass transfer [136]
Flexirings, analyzer Nira modeling in BTF
A

structured PAS Mercury 901


Winded Media
Plastic cross- Activated ASMM 0.80 0.114 14-160 1-500 mg <95% Total Effects of the [137]
flow structured sludge from m-3 hydrocarbon packing material on
material and WWTP analyzer Nira BTF performance
polypropylene Mercury 901-
rings random
packing
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SC
22 Ethanol 1.9 Clay balls Leachate of ASMM 1.00 0.150 66 0.47-2.36 ~80% Total Effect of EtOH [63]
dry compost g m-3 hydrocarbon concentration on

U
material analyzer the performance of
BF and BTF with

N
kinetics modeling
23 2-butoxy- 3.5 Polyurethane 1st BTF: ASMM 1.00 0.150 12.5 130 – 195 60-95% FID, total Effects of [71]

A
ethanol foam Pseudomonas / / g m-3 hydrocarbon inoculation
sp. BOE200, 0.70 0.105 analyzer procedure and
2nd BTF: different microbial

M
activated community on the
sludge form performance of BTF
ED WWTP
24 Benzene, - Blue mussel Activated Water 1.00 2.760 - 0.4 – 56 ~80-90% GC-MS Investigations of a [26]
toluene shells sludge for oil mg m-3 two-stage process
refinery WWTP performance (water
absorption and
PT

BTF) treating by-


products of oil
processing
E

25 Exhaust gases - - Activated - - - 20-100 - - - Analysis of bacterial [80]


from paint sludge from populations in an
CC

industry WWTP long-term operated


industrial BTF
26 Gas - Polypropylene Sulphur ASMM 0.53 0.071 - 2000-8000 70-99% Electrochemical Application of [138]
desulphurizati HD Q-PAC oxidizing ppmv sensors monitoring devices
A

on packing biomass for the assessment


of a bioreactor
performance
27 H2S + mixture - - Thiobacillus, - - - 17 25 ppmv 95% Olfactometry Description of the [139]
of VOCs activated upgrading of an
sludge industrial scale BTF
by increasing the
hydraulic capacity
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SC
28 Isobutyr- - HDPE KMB Activated MSM 1.00 0.044 60-200 14 – 355 g - GC-FID Assessment of the [74]
aldehyde, 2- rings nitrifying and m-3 h-1 efficiency of BTF

U
pentanone denitrifying working at higher
sludge temperatures

N
29 Methanol, - PVC spherical Mixed bacterial MSM 0.57 0.054 25-69 1-4 g m-3 <95% GC-FID Evaluation of [65]
ethanol, packing consortia simultaneous

A
acetone, elements (Pseudomonas removal of
toluene (mixed aeruginosa, hydrophobic and
or single) Bacillus sp. hydrophilic

M
and compounds
Chryseobacte-
ED riumjoo- stei)
30 Mixture: H2S, - Polyproplyene Candida ASMM 0.70 0.094 26-38 H2S: 0.01 – <99% Hand-held H2S Evaluation of one- [67]
methanol, α- pall rings boidinii, co- 1.4 g/m3 sensor, GC-FID stage BTF
pinene culture of Methanol: performance by
Rhodococcuse 0.05 – 3.3 investigating effects
PT

ry-thropolis g/m3 of different


and α-pinene: inoculating species,
Ophiostomas- 0.05 – 2.7 EBRT and process
E

tenoceras g/m3 mechanisms


31 Mixture: - Polyurethane Acclimated Sulphate- 1.00 0.080 7 – 50 ~1 mg m-3 <99% Electrochemical Analysis of BTF [140]
CC

methyl foam activated free sensor (MeSH), performance and


mercaptan, sludge MSM GC-FID RE of VOCs mixture
toluene, α- with microbial
pinene, community
A

hexane assessment
32 Organic waste - Ceramic Enriched ASMM 4.50 2.000 7.2-18 ~70-430 95-95% GC-MS Effects on technical [77]
gas in a paint particles and activated ppm (total parameters
plant Rashig rings sludge from VOCs) (temperature, IL,
WWTP flow rate) on the RE
of VOCs mixture in
BTF with
photocatalyticoxidati
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on
33 Trichloro- - Bituminous- Mixed ASMM 0.60 0.070 200 35-350 ~99% GC-FID / GC- Assessment of an [141]

U
ethylene, based GAC microbial ppm MS integrated process
perchloro- consortium performance

N
ethylene (ultraviolet oxidation
and BTF)
𝑚𝑜𝑙
Henry’s law [ ]

A
1 constants at 298.15 K,
𝑚3 ∙𝑃𝑎
ASMM – aqueous solution of mineral medium (mixture of minerals and nutrients, specific for each investigation); FID – flame ionization detector; GC – gas chromatography; HDPE

M
– high density polyethylene; MSM – mineral salt medium; PLA – polylactic acid; PVC – polyvinyl chloride; REF – reference; WWTP – wastewater treatment plant

ED
E PT
CC
A
``
The research review presented in Table 3 indicates that the majority of studies cover the
description of removal of single compounds. Usually, synthetic materials are used as packing for
BTFs and these are usually inoculated with activated sludge taken from selected steps of treatment
in wastewater treatment plants. The trickling liquid is usually an aqueous solution of mineral salts, in
many cases enriched with organic nutrients for microorganisms. The dimensions of bioreactors
differ from several centimeters to meters (from about 0.2 m to about 4 meters in height and from
0.01 m to about 2.5 in diameter), depending on the volume of treated gas as well as the scale of
investigations. As a result, EBRT values also differ, ranging from several seconds to several
minutes (from about 3 to more than 450 s). The research is currently focused on the effects of
interactions between removed compounds, especially including hydrophobic compounds and their
mixtures with hydrophilic compounds, evaluation of the composition of biofilm as a function of
treated compounds, effects of application of hybrid systems for gas deodorization (e.g. with UV

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radiation) as well as modeling of mass transfer phenomena. In terms of the analytical tools applied
for the process performance evaluation, gas chromatography coupled with flame ionization detector

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is the predominant method when lab-scale investigations are concerned. Industrially,
electrochemical sensors are mainly used.

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5. Evaluation of BTF performance

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As a result of a biofiltration process, the treated gas stream should present a lower
concentration of the target compound/s at the outlet comparing to the inlet. This change in
concentration is usually described with basic parameters given in section 4.1 i.e. removal efficiency,

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elimination capacity, inlet loading rate. It is therefore crucial to apply a proper methods for gas
analysis so that the required concentrations of gas pollutants may be determined. The information
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present in Table 3 shows that there are two dominant, fundamental approaches to evaluation of
purification effectiveness of air stream polluted with odorous compounds: analytical and sensory
approach. Sensory techniques (different types of olfactometry), in which human nose plays the role
A
of a measurement instrument, allow determination of summary concentration of odorous substance,
odour intensity and hedonic tone. However, these techniques are useless as far as on-line
M

measurements are concerned. Moreover, they exhibit the following limitations. There is a need for
polluted air sample collection and transportation to laboratory, which obviously influences on
extension of time necessary for a single analysis and can have a negative impact on obtained
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results due to a risk of analyte loss upon adsorption processes inside a bag [10,142,143]. Moreover,
it is difficult to evaluate odor concentrations, especially in case of variability of emission from a
biofilter.
There are also two dominant approaches in analytical methods. One of them consists in
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identification of particular component of odorous mixture, the other one relies on holistic analysis of
the entire odorous mixture. The first group includes chromatographic techniques, which are most
frequently employed for identification and quantitative determination of odorous pollutants in
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exhaust air from an installation. Information about chemical composition of the odorous mixture,
including sampling process and analysis execution (analytes derivatization, conditions of separation
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process), allows preliminary estimation of pollutants emission level from the biofilter and provides
valuable knowledge concerning effectiveness of the solutions aimed at deodorization of odorous
substances. Determination of a correlation between odour concentrations and chemical composition
of the air samples collected at the biofilter outlet makes it possible to identify the compounds, which
A

can have the biggest impact of strength of sensed odor. Application of the chromatographic
techniques allows for relatively high repeatability and reproducibility of results as compared to the
sensory techniques. Nevertheless, a fundamental drawback of the chromatographic techniques is
inability of holistic characterization of many odour features such as intensity and hedonic tone,
which are of primary importance as far as odour nuisance phenomenon is concerned [144–146].
The second analytical method for analysis of chemical compounds with respect to odour is
electronic nose technique. An electronic nose instrument is often defined as an analytical tool for
fast detection and discrimination of odorous substances mixtures due to imitation of operation of
human sense of smell. Identification of gas mixture composition is possible thanks to excitation of
all chemical sensors (each sensor is excited in different extent) comprising the electronic nose
instrument. The result is a characteristic set of responses from particular sensors, named a
response vector. Analysis of the response vector makes it possible to classify given air sample to a
particular set of response vectors identified earlier during a process of electronic nose training
[147,148]. The electronic nose instruments are most frequently utilized in qualitative analysis,
although it is also possible to employ them in quantitative analysis. Additional advantage of the
electronic noses is the suitability for on-line measurements as they do not exhibit olfactory
adaptation, unlike human nose [149–151]. Application range of these devices in outlet air quality
evaluation is strictly connected with numerous limitations of the chemical sensors (varying
sensitivity and selectivity) depending on actual measurement conditions (varying concentration of
odorous compounds, temperature, humidity). Selection of suitable chemical sensors for the
electronic nose instrument depends on the components of odorous mixture to be identified and their
expected concentration range.

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Table 7 provides a comparison of measurement utility properties of the methods for analysis of

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odorous compounds.

Table 7. Comparison of measurement utility properties of the methods for analysis of odorous

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compounds.
Properties Sensory methods Chromatographic Electronic nose

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methods

Legal regulation Yes, EN 13725:2003 Yes, for particular No


standard odorous compounds
Measuring element Human nose
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Different types of
detectors
Sensor matrix
N
Ability to determine low No/ yes depending on Yes Yes/ no depending on
concentrations the type of olfactometry the sensor matrix applied
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applied
Objectiveness of High for dynamic High Medium
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obtained results olfactometry, low for


remaining types of
olfactometry
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Identification of odour Yes No Poor


features
A need for sample Yes/ no depending on Yes No
preparation prior to the type of olfactometry
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analysis applied

Time of analysis Short Long Short


Suitability for on-line No No/ yes only for some Yes
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measurements types
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Cost of analysis High High Low

Abilities and limitations of particular methods of odour analysis suggest that the most
advantageous solution seems implementation of a few, supplementary techniques. In this way, it is
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possible to provide full evaluation of odorous compounds features including: concentration, odour
intensity, hedonic tone, odour character and olfactory threshold.

6. Concluding remarks and future development strategies


The mass transfer resistance between the gas-liquid phase of hydrophobic VOCs is large,
which limits its degradation, resulting in low removal efficiency in the bio-trickling filter. At present,
the pathways to improve the degradation of hydrophobic organic waste gas at domestic and foreign
mainly includes the following three aspects: surfactant addition, fungal biocatalysis, and design of
new biological filtration. The three enhancement pathways above have certain strengthening effects
on hydrophobic organic waste gas under laboratory conditions. However, each of the pathways has
certain drawbacks when it is promoted and applied. The synergistic removal of hydrophilic and
hydrophobic VOCs improves the removal efficiency of hydrophobic VOCs, which is superior to the
other three in terms of economy and production, and the gas in the actual plant is also emitted as a
mixed gas. This approach is clearly more realistic.
Biotrickling filtration has been proven to be an efficient method for the removal of odorous
compounds from air streams. Presented literature review reveals that the method is currently being
developed with a perspective of better understanding of the process mechanisms and modeling of
the process kinetics and efficiency, especially when mixture of compounds is treated. Nevertheless,
referring to earlier review papers in the field of BTFs, a significant progress in reporting research
data originating from pilot operations can be noticed.
The majority of reviewed papers deal with the removal of single pollutants in BTFs. Current

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topics in the field of air biofiltration include the simultaneous removal of various VOCs mixtures

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[152], with a special emphasis on the removal of hydrophobic compounds and strategies to improve
their removal from air streams [46].
Trends in the research on deodorization by means of BTFs should be focused on: (1)

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understanding the role of secondary microbial processes and biomass-growth control, (2)
investigating the relations between the kinetics and biodegradation, especially for mixtures of

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different compounds of various chemical properties, (3) process modeling and optimization, (4)
scaling-up of the process and (5) description of biochemical pathway of malodorous compounds.
The literature review indicates that there is an urgent need for investigating the mechanisms of

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biotrickling filtration on complex VOCs mixtures and the number of such papers is increasing.
Additionally, a growing interest is seen in the investigations regarding the changes of
composition of microbial species within the biofilm, especially when comparing the inoculums with
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the resulting biofilm composition after the bioreactor operation.
Several drawbacks of biotrickling filters, mainly related to the removal of hydrophobic VOCs,
A
may be overcome by the development of two-phase partitioning bioreactors and the studies of an
influence of hydrophilic compounds on the removal efficiency of hydrophobic compounds are
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currently important areas of investigations in this field [15,74,93,153]. Consequently, new chemical
and biological systems together with new design options of BTFs should be proposed for the
effective deodorization of air streams polluted with mixtures of compounds with different chemical
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properties. The development of BTFs should concentrate on industrial applications where


hydrophobic compounds are emitted to air e.g. petrochemical and pharmaceutical facilities.
Additionally, further investigations in the field of packing materials are also suggested. Optimization
of packing should result in minimizing death zones and short-circuiting and thus reduce the size of a
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biotrickling filter [100]..


Literature review reveals that little information is available on the measures for on-line
monitoring of the performance of BTF [138]. Therefore, for the further improvement of process
stability and efficiency, automated process control should be developed, even for the lab-scale
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investigations. Many methods of determination of malodorous substances are considered too


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expensive for elaboration of popular, widely-accessible measurement devices or systems for


monitoring of malodorous substances elimination from ambient air. Literature background as well as
theoretical fundamentals and operation principles of the electronic nose instruments suggest that in
the near future these devices, due to short time of analysis and possibility of on-line operation, can
A

be the main analytical tool for monitoring of gases purified from malodorous compounds.

Acknowledgments: The investigations were financially supported by the Grant No. UMO-
2015/19/B/ST4/02722 from the National Science Centre, Poland.
Conflicts of Interest: The authors declare no conflict of interest.
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