JOURNAL OF WATER AND LAND DEVELOPMENT

e-ISSN 2083-4535

Polish Academy of Sciences (PAN) Institute of Technology and Life Sciences – National Research Institute (ITP – PIB)

JOURNAL OF WATER AND LAND DEVELOPMENT

DOI: 10.24425/jwld.2022.141558
2022, No. 54 (VII–IX): 84–93

Treatment of methanol-containing wastewater

at gas condensate production

Andrey Ivanov1) , Alexey Strizhenok1) , Gabriel Borowski2)

1)
Saint-Petersburg Mining University, Faculty of Mining Engineering, 21st Line of Vasilyevsky island, 2, 199106, Saint-Petersburg, Russia
2)
Lublin University of Technology, Faculty of Environmental Engineering, Poland

RECEIVED 22.07.2021 ACCEPTED 03.12.2021 AVAILABLE ONLINE 28.09.2022

Abstract: The purpose of the study was to assess the impact of industrial wastewater on the concentration of methanol
in the considered section of the Ob River basin, present proposals for the implementation of a new treatment system
and analyse the implementation results. On the basis of the results of the analysis of the known methods for reducing
the concentration of methanol in water, a new technological scheme for post-treatment of effluents using biological
treatment with methylotrophic Methylomonas methanica Dg bacteria was proposed. The calculation of the dilution of
treated wastewater using the “NDS Ecolog” program was carried out on the basis of the detailed calculation method
of Karaushev, the results of which showed a decrease in the concentration of methanol in the control section to
0.0954 mg∙dm–3 (permissible concentration is 0.1 mg∙dm–3). During the period of the flood of the Glukhaya channel, it
ceases to be a separate water body and, in fact, becomes part of the flood channel of the Ob River. Certain parts of the
flooded areas, due to elevation changes, communicate with the channel only during a short period of time when the
water level rises, i.e. 3–5 weeks during the flood period, and in fact remain isolated reservoirs for the rest of the time,
potentially acting as zones of accumulation and concentration of pollutants.

Keywords: biological treatment, gas condensate, hydrates, methanol, rectification, regeneration, wastewater

INTRODUCTION inhibitor. Gas hydrates are solid crystalline compounds that are
formed under certain temperature and pressure conditions from
The considered condensate stabilisation plant is one of the largest water and low molecular weight gases [BABENKO et al. 2020; ZOU
gas condensate processing plants in the Russian Federation. The et al. 2021]. Methanol, which belongs to the class of thermo-
plant processes oil and gas condensate mixture and produces dynamic inhibitors of hydrate formation, reduces the activity of
commercial products: motor gasolines, diesel fuel, jet fuel, water in water solution, which results in changing equilibrium
liquefied gases, gas condensate distillate, light and stable conditions for the formation of hydrates [KITAEV et al. 2021;
condensate [LITVINENKO 2020; LITVINENKO, MEYER 2017; QUIROZ MONDAL et al. 2016; QURESHI et al. 2020].
CABASCANGO, BAZHIN 2020]. The company’s environmental policy Thus, the injection of methanol into the bottomhole zone of
is based on ensuring the reduction of negative impact on the the well of gas hydrate fields not only causes the decomposition of
environment, resource conservation, taking the measures to gas hydrates at the bottom of the well, but also improves the
preserve the climate, biodiversity and compensation for the filtration characteristics of the bottomhole zone, i.e., the section
possible damage to the environment [BABENKO et al. 2020; of the formation adjacent to the wellbore. In addition, the high
FILATOVA et al. 2021]. In the gas industry, methanol is used as adsorption capacity of methanol is used to remove water after
a hydrate inhibitor [DVOYNIKOV et al. 2021a]. It enters the plant hydrostatic testing of gas pipelines, as well as in low-temperature
together with the oil and gas condensate mixture. processes for removal of carbon dioxide (CO2), hydrogen
Methanol is very important for the plants of the North sulphide (H2S) and other sulphur-containing organic compounds
[SHARIKOV et al. 2020]. This substance is used as a hydrate from natural gas [DIDMANIDZE et al. 2020].

© 2021. The Authors. Published by Polish Academy of Sciences (PAN) and Institute of Technology and Life Sciences – National Research Institute (ITP – PIB).
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 Andrey Ivanov, Alexey Strizhenok, Gabriel Borowski 85

The widespread use of methanol, especially at gas produc- The Ob River and its large tributaries are characterised by
tion plants of the Far North, is due to a number of reasons, spring-summer floods, low summer-autumn runoff, with rain
including its relatively low cost compared to other inhibitors of floods in the warm season (which are insignificant in size and
hydrate formation (glycols, surfactants, water-soluble polymer duration) and low runoff in winter. The duration of the flood
compositions), the highest antihydrate activity among the known varies from 100 to 130 days.
inhibitors, even at low temperatures, very low freezing point of The terrain is very swampy, and the marshes are unevenly
concentrated methanol solutions and their extremely low distributed throughout the territory. This is due to the flat
viscosity even at temperatures below –50°C [OHLSTRÖM et al. topography, shallow river slopes and extremely slow runoff, as
2001; SEMENOV et al. 2021; ZAGASHVILI et al. 2020]. Environmental well as shallow river incisions and poor drainage. There are
risks in the form of accidental emissions or spills of methanol can a large number of lakes in the region of the West Siberian
arise during its production, transportation, use and wastewater Lowland. This is caused by a combination of two factors,
accumulation of this substance [DEMIRBAS 2008; FERNANDEZ et al. i.e. excessive moisture and flatness of the surface. There are also
2007; MATVEEVA et al. 2017; TRICKEY et al. 2020]. The water of the drainless reservoirs with bitter salt water. There are also several
Ob River and water bodies of its basin, are characterised by high large reservoirs in this area. Most of the water bodies of Western
methanol concentrations due to the presence of developed natural Siberia are fisheries. Large rivers and floodplain lakes are the
gas fields and gas condensate industries in this area. main source for commercial fishing.
Methanol is supplied to the plant along with the oil and gas The taiga zone is usually characterised by alternating
condensate mixture [GRAAF, BEENACKERS 1996]. During the swamp and forest landscapes. In the region, there are mainly
production and transportation of hydrocarbons, a droplet liquid low-lying moss-grass and raised sphagnum bogs. Low-lying bogs
is formed in the flow. When it freezes, hydrate plugs (ice) are are usually located in the floodplains of rivers, and their
formed, which reduces the flow permeability or leads to vegetation is represented by sedges, willows and forbs (Scutella-
a complete stop of pumping [WANG et al. 2019]. The addition ria galericulata, Stellaria longifolia, Equisetum palustre, Galium
of a water-methanol mixture in the fields ensures the absence of uliginosum). The landscape of raised sphagnum bogs is mainly
hydrate deposits on the walls of main pipelines [LIU et al. 2016]. characterised by ridge-lake and ridge-hollow complexes with
The main purpose of the wastewater recovery unit with dwarf-sphagnum and dwarf-sphagnum-pine vegetation. Shrubs
methanol recovery and wastewater treatment is to recover are represented by Betula nana, Myrtus, Andromeda, Oxycóccus
and Vaccínium myrtíllus. The tree layer is represented by pines.
methanol from a water-methanol mixture by rectification
Their height is from 4 to 10 m, and the crown density does not
[DAVANI et al. 1986]. The methanol mixture is first separated
exceed 0.2–0.3 m. The moss cover is continuous, of sphagnum
from the condensate and then from the water by heating
mosses.
[BONDAREV et al. 2018]. The boiling point of methanol (65°C) is
The trees of the forest landscape are represented by Picea,
lower than that of water. The end product of the plant is 98%
Cedrus, Alnus, Pinus, Larix, Abies and Betula. Forests are
methanol, which is shipped by rail for reuse by mining
stretched out in narrow bands along river floodplains or arranged
companies. The aim of the study was to evaluate the degree
in a mosaic pattern. The forestry regulations provide for the
and nature of the impact of one of the condensate plants on the
following forest categories in the area where the plant is located:
methanol content in surface waters based on an analysis of the
valuable (protected forest belts located along water bodies; spawn-
available production data and a review of open sources, as well as
ing forest belts) and operational [Prikaz № 59-np … 2018].
to develop a new treatment system that will reduce the
The fauna of the region is represented by 60 species of mammals,
technogenic impact of the methanol-containing wastewater to
260 species of birds, 4 species of reptiles, 42 species of fish, as well
standard indicators.
as 6 species of amphibians (3 of which are in the Red Book by
BAYKALOVA et al. [2013]).
The following mammals have spread throughout the area:
MATERIALS AND METHODS Canis lupus, Ursus arctos, Mustela nivalis, Lepus timidus, Rattus
norvegicus, Mus musculus. Rangifer tarandus is a rare species.
The basin of the Ob River below the confluence of the Irtysh is Among birds, the most widespread are Falco (Falco peregrinus,
divided into two regions: Sredneobsky and Nizhneobsky. The F. columbarius, F. subbuteo), Bubo bubo, Larus (Hydrocoloeus
river flows along its entire length in a flat valley, the width of minutus, Chroicocephalus ridibundus, Leucophaeus modestus),
which is greater than 50 km. The Ob River is characterised by Grus (Grus communis, G. monacha, G. leucogeranus) and geese
a multi-arm channel. In the area of the city of Surgut, it is divided (Branta ruficollis, Plectropterus gambensis). The ichthyofauna of
into two main branches (Ob and Yuganskaya Ob). The the Middle Ob is represented by 22 species of fish. The most
Sredneobsk region is the place where other large rivers flow into important fishing objects in this part of the basin are
the river: Vakh, Bolshoi Yugan, Bolshoi Salym, as well as many representatives of the following species: Acipenser, Stenodus
small rivers. The main source of water for rivers in this place is leucichthys nelma, Coregonus muksun, Coregonus peled, Acipenser
large sediments, but also groundwater and liquid sediments. ruthenus, Lota lota, Esox lucius, Leuciscus idus, Rutilus, Carassius
The chemical composition of the river waters of the Ob- carassius, Leuciscus leuciscus, and Perca fluviatilis.
Irtysh basin enables to categorise them as waters of the calcium In winter, the rivers are fed by swamp waters, which are
group of the hydrocarbonate class. Relatively weak slope of the almost devoid of oxygen, but contain many organic substances,
terrain, as well as a large tortuosity coefficient (3–4) of the which in turn increase the productivity of water bodies. In
territories of the Khanty-Mansi Autonomous Okrug lead to addition, oxygen is consumed for the oxidation of ferrous iron
a rather slow flow of rivers. compounds that enter rivers from swamps. Mass death of fish is

© 2022. The Authors. Published by Polish Academy of Sciences (PAN) and Institute of Technology and Life Sciences – National Research Institute (ITP – PIB).
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86 Treatment of methanol-containing wastewater at gas condensate production

rarely observed in the Ob: under normal conditions, the fish have If there is data on the slope of the water surface, the
time to escape into non-clogged water bodies [STARIKOV 2012]. Equation (6) is applied:
In order to calculate the concentration in the control
Vr
section, a normative method was used, namely, a detailed method C ¼ pffiffiffiffiffiffiffiffi ð6Þ
Ha i
(numerical method) for solving the turbulent diffusion equation,
developed by A.V. Karaushev, makes it possible to obtain where: i = the slope of the water surface (%).
a concentration field of a substance within the entire calculated As a result of calculations performed from cross-section to
area from the point of release to the section under consideration. cross-section, a concentration field was obtained in the area below
The equation of turbulent diffusion for the conditions of the the place of discharge of pollutants. The detailed method of
spatial problem has the following form: Karaushev is a numerical method for solving the turbulent
diffusion equation and makes it possible to obtain a field of
!
@x S D @y2 S @z2 S concentration of a substance within the entire computational
¼ þ ð1Þ region from the place of wastewater discharge to the control
@X Vr @Y 2 @Z 2
section. There are no limitations to the applicability of this method.
where: D = the coefficient of turbulent diffusion, Vr = average
flow velocity in the considered section of the watercourse (m∙s–1),
∂X, ∂Y, ∂Z = coordinate change along the length, width and depth
RESULTS AND DISCUSSION
of the watercourse, respectively, relative to the origin of
The initial water-methanol mixture is supplied to the unit from
coordinates – the place of discharge, ∂XS, ∂YS, ∂ZS = change in
the tank farm. The plant includes the following structures and
the concentration of the considered polluting component along
systems: rectification unit, pretreatment unit, steam condensate
the length, width and depth of the watercourse relative to the
pumping station, control room, ventilation chambers, individual
concentration of the polluting component in waste water (mg∙m–3).
heating points, and household premises. The technological
The entire computational flow area was divided by the
process is controlled from the control room located in the
planes parallel to the coordinate planes into computational cells.
building of the auxiliary block.
The following relationships were established between the long-
The plant has three outlets used for the discharge of
itudinal and transverse dimensions of the design elements:
wastewater of the following categories.
1. Industrial stormwater, resulting from the use of water for the
0:25Vr @Z 2 0:5Qww
@X ¼ and @Z ¼ ð2Þ technological needs of the plant: washing of tanks and equip-
D Ha V r
ment; steaming containers and equipment; hydraulic testing of
where: Qww = the maximum wastewater discharge (m3∙s–1), tanks and equipment; testing of fire extinguishing systems; wet
Ha = the average depth in the considered section of the cleaning of technological premises. Moreover, this runoff con-
watercourse (m). tains the industrial stormwater from sites and landfills where
Determination of the coefficients of turbulent diffusion was technological equipment is located.
conducted by using the Karaushev method: 2. Domestic and domestic untreated sewage resulting from the
discharge from plumbing fixtures and showers; wet cleaning of
gHa Vr household premises.
D¼ ð3Þ 3. Methanol-containing wastewater generated as a result of the
MC
production activity of the low-pressure waste gas utilisation
where: g = gravitational acceleration (g = 9.8 m∙s–2), M = dimen- unit; prevention of hydrate formation; production activities
sionless parameter equal to M = 0.7C + 6, C = the Shezy of the wastewater utilisation unit with methanol recovery and
coefficient. wastewater treatment.
The Shezy coefficient is determined when there is data on The approved standards of permissible discharge by
the composition of bottom sediments or the roughness coefficient discharge are presented in Table 1.
of the bed of a water body. In the presence of the data on the The plant has a sewerage system. All types of wastewater are
granulometric composition of bottom sediments, the Strickler– collected in sewage pumping stations, and then they are transmitted
Manning formula is applied: to treatment facilities. The plant has three sewerage systems.
1. Household wastewater. Domestic wastewater is discharged to
� �16
Ha sewage pumping stations for domestic wastewater. Then it is
C ¼ 33 ð4Þ transmitted to the pumping station, and from it to the treat-
de
ment plant. From the pumping station of the household waste-
where: de = the effective diameter of bottom sediments, water of the plant, the wastewater first enters the mechanical
determined by the granulometric curve. grate, which retains large pollution of organic and mineral
If there is data on the roughness coefficient of the bed of origin. After passing through the mechanical grate, the waste-
a water body, the Pavlovsky formula is applied: water enters the primary clarifier. It is required for pre-
clarification of wastewater. Mechanical sedimentation of sus-
Ha1:6 pended solids takes place in it. From the primary sedi-
C¼ ð5Þ
nr mentation tank, wastewater enters the aeration tank for
removal of organic matter, as well as nitrogen and phosphorus
where: nr = the roughness coefficient of the bed of the water body. compounds. Further, the wastewater enters the secondary

© 2022. The Authors. Published by Polish Academy of Sciences (PAN) and Institute of Technology and Life Sciences – National Research Institute (ITP – PIB).
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 Andrey Ivanov, Alexey Strizhenok, Gabriel Borowski 87

Table 1. Data on wastewater discharges at the plant

Wastewater Actual Permissible Actual wastewater Approved standard

Wastewater
generation volume Name of substance concentration in concentration discharge in 2020 of permissible
outlet number
in 2020 (m3) 2020 (mg∙dm–3) (mg∙dm3) (Mg) discharge (Mg∙y–1)

petroleum products 19.25 0.45 7.191 0.2436

1 453227 sodium alkyl sulphate 0.50 0.13 0.187 0.0706
methanol 4.60 0.50 1.718 0.271
petroleum products 0.37 0.45 0.101 0.162
sodium alkyl sulphate 0.33 0.314 0.090 0.107
2 167271
methanol 0.22 0.50 0.060 0.179
phosphates by P 0.303 1.51 0.082 0.532
3 4205 methanol no data

Source: own elaboration.

clarifier. It is necessary to clarify the sludge mixture with the water recovery unit with methanol recovery and wastewater
subsequent return of sludge to the treatment systems and, if treatment.
necessary, remove it from the system. After passing through The main purpose of the unit is the recovery of methanol
the secondary sedimentation tank, the wastewater enters the from a water-methanol mixture by rectification. The methanol
clarified water tank. From there, it is fed to the adsorption mixture is first separated from the condensate and then from the
filter for final post-treatment. The filter contains a load repre- water by heating [LI 2003]. The boiling point of methanol (65°C)
sented by a sorbent. In order to improve the retention of is lower than that of water. The end product of the plant is 98%
pollutants on the filter media, a coagulant is supplied to the methanol, which is shipped by rail for reuse by mining
filters. Its supply is carried out from the coagulant tanks using companies. According to the company, the permissible concen-
metering pumps. After passing through the adsorption filter, tration of this alcohol in the discharged water is 2200 mg∙dm–3.
water enters the filtrate tank and it is supplied to wash the The actual concentration data are not provided. In this regard, an
approximate calculation was performed. The production capacity
filters. The water from the filtrate tank is also used for tech-
of the plant is 3∙109 kg of gas condensate per year. The mass of
nical needs. From the filtrate tank, water is supplied to the
methanol per 1000 m3 of gas condensate is 1 kg. The density of
ultraviolet disinfection unit, after which the purified water is
gas condensate is 700 kg∙m–3. The consumption of methanol-
fed to the discharge.
containing wastewater at the plant is 4204 m3∙y–1. On the basis of
2. Production wastewater. Industrial wastewater is discharged to
these data, the mass of methanol generated at the plant over the
sewage pumping stations; then, it enters the pumping station
year was found, i.e. 4285 kg∙y–1, and then the concentration of
of industrial effluents of the plant, and from it to treatment
methanol in industrial wastewater contaminated with methanol
facilities. The treatment facilities include, in series, mechanical was found, amounting to 1024.5 mg∙dm–3. The efficiency of
grids, an underground homogeniser-settling tank for water wastewater purification from methanol at the rectification plant is
purification from suspended solids and oil products, as well 98%; thus, the methanol content in the purified water was
as flow averaging, a block of adsorption filters of two-stage calculated, reaching 20.49 mg∙dm–3.
purification, and an ultraviolet disinfection unit. After treat- The media have repeatedly reported that the maximum
ment facilities, water is supplied for discharge. permissible concentration for methanol was exceeded down-
3. Industrial wastewater, contaminated with methanol. The in- stream the Ob River. The Ob River communicates with the
dustrial wastewater contaminated with methanol is discharged Glukhaya channel, into which methanol-containing wastewater is
to sewage pumping stations for the methanol-containing ef- discharged. In connection with the above, the calculation of the
fluents. Then, they are transmitted through the pressure sew- rate of dilution of wastewater in the “NDS Ecolog” program was
erage network to the treatment plant. The treatment facilities performed according to the detailed method of Karaushev. The
for methanol-containing effluents are represented by a bottom location of the discharge of methanol-containing wastewater into

Fig. 1. Field of flow directions in the Glukhaya channel; source: own elaboration

© 2022. The Authors. Published by Polish Academy of Sciences (PAN) and Institute of Technology and Life Sciences – National Research Institute (ITP – PIB).
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88 Treatment of methanol-containing wastewater at gas condensate production

the Glukhaya channel, the location of the control section and the assessed by conducting special comprehensive geological explora-
direction of the flow are shown in Figure 1. tion, the subject of which is the suitability for deep disposal of
The following discharge parameters were used in the waste, depending on the type, composition and properties of
calculation: discharge type – scattering, number of discharge waste, technology of preliminary preparation for liquidation.
heads – 2, estimated wastewater flow rate – 0.00013 m3∙s–1, The physicochemical method for purifying the water
wastewater flow rate – 0.8 m∙s–1, average outlet diameter – 0.5 m, containing methanol using ultraviolet radiation from excilamps
the distance from the point of release to the shore is 2 m, the (gas-discharge lamps) in the presence of nitric acid (HNO3). In
distance from the outlet to the surface of the water body is 0.5 m, this case, under the influence of ultraviolet radiation, the
the distance from the point of release to the control section is photolysis of water and nitric acid occurs with the formation of
500 m. The parameters of the water body at the point of release highly reactive radicals, i.e. OH, H, NO2 and NO, which
were also used in the calculation: the object is a river, the average subsequently enter into reactions with methanol with the
depth in the section under consideration is 5 m, the estimated formation of the final products, namely CO2, H2O and NH3.
flow rate is 1 m∙s–1, the estimated water flow rate of the water Under the experimental conditions, it was found that in the
body is 8.5 m3∙s–1, the average width of the water body in the methanol-containing water with the addition of nitric acid (at
section under consideration is 450 m, the tortuosity coefficient of a CH3OH:HNO3 ratio of 10: 1) under the action of ultraviolet
the river section is 1.2. radiation with a wavelength of λ = 172 nm (Xe2 is an excilamp),
The calculation showed that when the concentration of the methanol concentration in water in 16 min decreased from
methanol in wastewater is 20.49 mg∙dm–3 in the control section, 35.0 to 2.6 mg∙dm–3, i.e. 13.5-fold, and when using similar
the concentration is 2.12 mg∙dm–3. This water body belongs to the radiation with a wavelength λ = 222 nm (KrCl – excilamp)
highest fishery category, for this category of water bodies the decreased from 338.0 to 14.6 mg∙dm–3, that is, by a factor of 23
maximum permissible concentration for methanol is 0.1 mg∙dm–3, [MEDVEDEV et al. 2005].
which indicates the possibility of more than 20-fold excess of the There is a method for extracting methanol from industrial
standard concentration, in connection with the introduction of wastewater of gas condensate fields, which consists in the
measures for the additional treatment of methanol-containing regeneration of this substance by rectification, followed by deep
wastewater. catalytic oxidation of its residual amounts in the bottom residue
Typically, in gas processing plants, wastewater contains not (non-evaporated liquid) [KUZHAEVA et al. 2019a, b; SALIKHOV et al.
only methanol, but also other pollutants (hydrocarbons, phenols, 2020; YANG et al. 2019]. In this case, 100% oxidation of methanol
and others). A possible method for the disposal of such effluents in the bottom residue in a concentration of up to 1.5% is achieved
is combustion in gas flares [CHEIN et al. 2021; GHOSH et al. 2019; using a copper-chromium-magnesium and chromium-magne-
TEIXEIRA et al. 2018; 2019; TIMOSHENKO, SHPAK 1989]. Wastewater sium catalyst on an alumina carrier (Al2O3). The duration of
is injected via nozzles into a combustion chamber filled with flue contact of methanol-containing water with the catalyst is not less
gases heated to temperatures above 1000°C. Water instantly than 0.9 s at a temperature not lower than 450°C.
evaporates, and impurities dissolved or suspended in it burn out. The work aimed at developing a technology for separating
This method is convenient, but it also has many disadvantages. methanol from the wastewater from gas condensate fields and
Therefore, with relatively high fuel consumption reaching 100– returning the main part of methanol to the technological cycle,
200 kg∙m–3 of wastewater, the temperature in the combustion followed by bringing the residual concentration of methanol in
chamber is still insufficient for the complete decomposition of discharged process waters to the maximum permissible concen-
pollutants [MATANI, MALI 2019]. As a result, gases and dusty tration, which is very relevant [SCHABER, IVANOVA 2017; ZAPORO-
impurities are formed, requiring thorough additional cleaning in ZHETS, SHOSTAK 2019; ZHOU et al. 2014]. Regeneration of methanol
special devices, including electrostatic precipitators, scrubbers, can be carried out by rectification, as the most reliable and
adsorbers, multicyclones, etc. At the same time, the more efficient technology that allows extracting up to 99 wt. % methanol
powerful the plant, the higher the degree of environmental hazard with a residual concentration of about 1 wt. % and above
from emissions into the atmosphere and the more obvious the [BRENCHUGINA et al. 2007; NIASAR et al. 2019]. The wastewater
need to use new, more advanced cleaning methods and more containing methanol is neutralised with phosphoric acid,
reliable measures to protect the environment. In addition, this enriched with nitrogen sources, and subsequent treatment is
method is very expensive. carried out with the Methylomonas methanica Dj microorgan-
Another method of wastewater management, widely prac- isms. Using this method, the recommended pH should be 6.0–7.0,
ticed in the gas industry, is its underground disposal [DVOINIKOV and the temperature of the wastewater should be between 20 and
et al. 2021b]. It is carried out by pumping wastewater into deep, 37°C [MURZAKOV et al. 2005].
reliably isolated aquifers that do not contain fresh, balneological, Comparative characteristics of the considered methods of
mineral and thermal waters. Underground disposal of wastewater wastewater treatment from methanol are presented in Table 2.
in the area of the depression funnel in the water pumping system The rectification unit is used at the plant. Its efficiency is
of the developed natural gas field can be carried out if it is 98%, which is insufficient. On the basis of the results of the
impossible to purify wastewater from methanol and other assessment of the methods (Tab. 2), it is proposed to carry out
components to the required maximum permissible concentration additional treatment of the methanol-containing wastewater
[MA et al. 2020]. Geological formations that can limit the area of leaving the production water disposal unit with methanol
influence of waste and meet a number of requirements for the regeneration and wastewater treatment by using the biological
conditions of occurrence and properties of rocks can be used for treatment method.
such a deep placement of wastewater. Compliance of the Unlike chemical and physicochemical methods of purifica-
geological environment with the established requirements is tion, “reagents” (microorganisms) that carry out biological

© 2022. The Authors. Published by Polish Academy of Sciences (PAN) and Institute of Technology and Life Sciences – National Research Institute (ITP – PIB).
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 Andrey Ivanov, Alexey Strizhenok, Gabriel Borowski 89

Table 2. Comparative characteristics of methods of utilisation funnel and industrial methanol-containing wastewater, initially
and treatment of methanol-containing wastewater diluted with a nutrient medium to a methanol concentration in
the effluent of 1 g∙dm–3, is passed through it. Further, the
Method name Advantage Disadvantage concentration of methanol is increased to the values approxi-
convenient for many mately equal to 10 g∙dm–3, and the dilution with the nutrient
types of wastewater, high cost, not environ- medium is gradually reduced. At the stage of supplying waste-
Burning
including methanol- mentally friendly water containing 10 g∙dm–3 of methanol and its absence in the
containing ones effluent leaving the column, a pure culture of bacteria is isolated
the impossibility of by seeding the contents of the column onto an agar mineral
reducing the negative
proper control over the nutrient medium of the given composition and containing
impact on surface water,
Underground
eliminating the need for
spread of wastewater in 2.0 g∙dm–3 of methanol [GVOZDYAK et al. 1986]. As a result, the
disposal formations, irreversible desired strain of Methylomonas methanica Dg is obtained, capable
complete wastewater
pollution of under-
treatment of purifying the methanol-containing wastewater to maximum
ground formations
permissible concentrations [MURZAKOV et al. 2006].
the ability to purify For the possibility of reproduction of these microorganisms,
methanol-containing
The use of ultra- necessity of adding the following conditions must be met: pH value of 6–7,
wastewater to maximum
violet radiation nitric acid, high cost wastewater temperature from 20 to 37°C [KALYUZHNAYA et al.
permissible concentra-
tions 2015].
The average consumption of wastewater leaving the bottom
the ability to recover high cost, the need for
methanol for reuse, high additional treatment to water recovery plant with methanol regeneration is 0.48 m3∙h–1,
Rectification the methanol content is 20.49 mg∙dm–3, the wastewater
purification efficiency maximum permissible
(up to 98%) concentrations temperature is 24°C, the pH value is 7. While analysing the data
the ability to purify the need to maintain the above, it can be concluded that the conditions necessary for the
methanol-containing pH value within 6–7, the reproduction of microorganisms of the species Methylomonas
Biological wastewater to maximum need to maintain the methanica Dg are met. In order to carry out biological treatment,
treatment permissible concentra- wastewater temperature the following technological units are required: wastewater
tions, low cost com- in the range from 20 to homogeniser; aerotank; sump; and clarifying sorption filter [ALI
pared to other methods 37°C
SHAH et al. 2014; ZHANG et al. 2010]. An enlarged technological
Source: own study. scheme of these treatment facilities is shown in Figure 2.
After the installation of bottom water utilisation with
methanol recovery, the wastewater is pumped into the equaliser
purification are not added to water, but spontaneously develop in by means of a pump. Then, with the help of submersible pumps,
treatment facilities, forming microbial cenoses consisting of the averaged flow enters the aeration tank. The wastewater from
hundreds of different types of microorganisms [GUPTA, GOEL the aeration tank enters the settling tank. The sludge of the settler,
2019]. Therefore, for the stable and effective functioning of represented by the excess sludge, is pumped out to the sludge
biological treatment systems, it is important to maintain a certain treatment unit of the domestic wastewater treatment plant
technological regime, in which the necessary microbial cenosis is [CLAUSEN et al. 2010]. The required amount of return sludge is
formed, capable of purifying water, and cell aggregates are formed fed back to the aeration tank by means of a pump.
that are easily separated from the purified water. Further, for additional treatment from suspended solids,
The Methylomonas methanica Dg strain is obtained represented by activated sludge, wastewater is pumped to
selectively from the actual methanol-containing wastewater. In clarification-sorption filters. From them, the purified water is
order to implement the method, selection of methanol-assimilat- supplied to the filtrate tank. Then, with the help of a pump, the
ing culture is carried out [CHEN et al. 2017]. For this purpose, the required amount of water is supplied to flush the filter. After the
soil contaminated with methanol is placed in a vertical glass filter, the purified water is fed by gravity to discharge. From the

Fig. 2. Technological scheme of biological wastewater treatment from methanol; source: own elaboration

© 2022. The Authors. Published by Polish Academy of Sciences (PAN) and Institute of Technology and Life Sciences – National Research Institute (ITP – PIB).
This is an open access article under the CC BY-NC-ND license (https://creativecommons.org/licenses/by-nc-nd/3.0/)
90 Treatment of methanol-containing wastewater at gas condensate production

wastewater utilisation unit with methanol regeneration, waste- homogeniser, water enters the aeration tank. The volume of the
water flows by gravity into the equaliser. The homogeniser is aeration tank is determined by the Equation (8):
a tank with an aeration system for mixing and a pump for
pumping wastewater into the aeration tank, which allows �x � 0:35BOD5 � Qd
Va ¼ ð8Þ
reducing the volume of the remaining tanks up to 20%, 1000Xa
preventing the removal of activated sludge from the aeration
tanks, and ensuring a uniformly high cleaning efficiency. where: τх = the total age of activated sludge, τх = 12 (days),
From the homogeniser, the water is pumped into the Qd = daily wastewater consumption (m3·d–1), Ха = the dose of
aeration tank for biological treatment of wastewater from activated sludge taking into account biofilm on dry matter,
methanol. The aeration tank is a rectangular tank with an Ха = 4 g∙dm–3; BOD5A = the value of BOD5 removed in the
aeration system. The methylotrophic Methylomonas methanica aerotank (BOD 5A = 450 mg O 2 ∙dm –3 ); V a = 5.45 m 3
Dg bacteria are used in the aerotank for the biochemical (12∙0.35∙450∙11.52/4∙1000).
conversion of methanol. Wastewater is purified from methanol The volume of the aeration tank was taken as equal to 6 m3.
by microbiological transformation (oxidation) of this substance In order to saturate the water with oxygen, an aeration system is
through formaldehyde and formic acid to carbon dioxide and installed in the aeration tank. For this purpose, a fine-bubble
water: aeration system manufactured by one of the Russian companies
was selected.
CH3 OH ! HCOH ! HCOOH ! CO2 þ H2 O An air blower is required to supply air to the aeration
CH3 OH ! HCOH þ H2 system of the aeration tank. The air consumption required for
2CH2 O þ O2 ! 2HCOOH aeration is 20 m3∙h–1. A Zenova 2RB 410-013 single-stage vortex
HCOOH þ O2 ! CO2 þ H2 O blower was selected with the following characteristics: maximum
After passing the aeration tank, the wastewater flows by air flow 80 m3∙h–1, maximum air pressure 12 kPa, operating point
gravity into the sump. Mechanical sedimentation takes place in it, 20 m3∙h–1 at 120 kPa, power 0.37 kW at 2900 rpm.
as a result of which the activated sludge is separated from the In order to increase the efficiency of biological treatment,
wastewater [GAI, LIU 2017]. a flat loading was placed in the aerotank. Flat loading is designed
In this case, it is a vertical sump with a thin layer module. It to intensify the processes of biological wastewater treatment in
contains a pump for pumping return sludge, as well as a pump for aeration tanks. It is produced in the form of flat and corrugated
pumping out sludge, represented by excess sludge. The sludge is sheets of resistant polymeric materials with a mesh structure for
transferred for processing to the sludge treatment unit of the
domestic wastewater treatment plant. After passing through the
sump, the wastewater enters the clarified water tank, and from it,
with the help of a pump, it is supplied to the clarification-sorption
filter. This is necessary for the final post-treatment from
suspended solids represented by activated sludge. The filter
contains a load represented by a sorbent. After passing through
the filter, water enters the filtrate tank; then, water is supplied
from it to wash the filter. From the filtrate tank, wastewater flows
by gravity to the discharge. At the plant under consideration, the
consumption of methanol-containing wastewater is 0.48 m3∙h–1.
The daily flow rate is 11.52 m3 per day. The volume of the flow
average (m3) is calculated by the following formula:
Photo 1. Flat loading produced by one of the Russian companies
V ¼ Qah � �reg ð7Þ
(phot.: A. Ivanov)

where: Qah = average hourly consumption of wastewater (m3∙h–1); effective attachment of microorganisms and the formation of
the value of τreg is determined according to [SP 32.13330.2018]; stable biofilms. For this purpose, a flat loading made by one of the
Vу = 1.59 m3 (0.48∙3.3).
Russian companies was selected (Photo 1).
The volume of the average equal to 2 m3 was chosen. In
After passing the aeration tank, the wastewater flows by
order to mix water, an aeration system was installed in the
homogeniser. It includes a perforated aeration pipe and a blower. gravity into the sump. In it, the activated sludge is deposited along
A Zenova 2RB 210-M004 single-stage vortex blower was used to with the wastewater from the aeration tank. On the basis of the
supply air to the aeration system with the following character- average hourly flow rate of wastewater equal to 0.48 m3, a PVO-
istics: maximum air flow 80 m3∙h–1, maximum air pressure ON-2.5 thin-layer sedimentation tank by one of the Russian
12 kPa, operating point 20 m3∙h–1 at 12 kPa, power 0.37 kW at companies was selected. It has a productivity of 2.5 m3∙h–1, which
2900 rpm.
works as follows: wastewater, passed through the aeration tank,
A Pedrollo NGAm 1B centrifugal pump was selected to
flows into the settler flow distributor by gravity; then, the water is
supply waste water to the aeration tank, it is characterised by the
following parameters: maximum water flow 18 m3∙h–1, maximum directed to thin-layer modules operating on the principle of
water pressure 17 m of water column, operating point 12 m3∙h–1 counter-current water and sediment, suspended solids settle on
at 13 m of water column, power 0.55 kW at 2900 rpm. From the an inclined surface, and then descend into the conical part of the

© 2022. The Authors. Published by Polish Academy of Sciences (PAN) and Institute of Technology and Life Sciences – National Research Institute (ITP – PIB).
This is an open access article under the CC BY-NC-ND license (https://creativecommons.org/licenses/by-nc-nd/3.0/)
 Andrey Ivanov, Alexey Strizhenok, Gabriel Borowski 91

settler. An overflow partition is located in the upper part, through concentration of methanol in the water of the Glukhaya channel
which water falls into the clarified water tank by gravity. in the control station will decrease to 0.0954 mg∙dm–3, which is
Further, with the help of a submersible pump, the sludge is lower than the maximum permissible concentration for water
transferred to the unit for processing the sludge of domestic bodies of fishery appointment (0.1 mg∙dm–3).
wastewater. For this purpose, a centrifugal pump is installed. Part
of the sludge is fed back to the aeration tank via a return sludge
pump. After passing through the settling tank, wastewater enters CONCLUSIONS
the clarified water tank, and from it, with the help of a pump, goes
to the clarification-sorption filter for cleaning. A method for biological treatment of methanol-containing
On the basis of the average hourly flow rate of wastewater wastewater was proposed. The purification efficiency of the
equal to 0.48 m3∙h–1, a clarification-sorption filter was chosen proposed method was 96%. Thus, the concentration of methanol
with the following characteristics: loading volume 110 dm3, in the discharged water is equal to 0.82 mg∙dm–3. In turn, after the
productivity 1.1–2.6 m3∙h–1, pressure 20–40 kPa, filtration area discharge and dilution of wastewater, the concentration of
0.129 m2, backwash 4.5 m3∙h–1. Two filters were installed. This is methanol in the control section of the Glukhaya channel is
necessary so that while flushing one of them, the second 0.0954 mg∙dm–3, which does not exceed the established standard
continues to work, as well as in case of a malfunction of one of concentration for this water body. It was concluded that the
the filters. A centrifugal pump was used to supply wastewater to proposed method of biological wastewater treatment from
the filters. methanol can be implemented at the plant in question. What is
After passing through the filter, water enters the filtrate tank typical, the permissible concentration of methanol in wastewater
and water is supplied from it to wash the filter. The water from declared by the company is 2200 mg∙dm–3, nevertheless, the
the BF is also used for technical needs. The volume of the filtrate calculated concentration of methanol in wastewater that has
tank is determined by the Equation (9): undergone rectification, i.e. 20.49 mg∙dm–3 leads to the
concentration of 2.12 mg∙dm–3 in the control section (maximum
QFT � 20
VFT ¼ ð9Þ permissible concentration is 0.1 mg∙dm–3), which may indicate
60
incorrect accounting of data on the parameters of the water body
for dilution.
where: QFT = the flow rate of water required to flush the filter During the period of the flood of the Glukhaya channel, it
(m3∙h–1); VFT = 1.07 m3 (3.23∙20/60). ceases to be a separate water body and, in fact, becomes part of
One filter rinsing usually takes 10 min. A minimum of two the flood channel of the Ob River. If the Ob River is considered as
flushes is required, so the flush time is 20 min. The water a water body for dilution, then the permissible concentration of
consumption for washing the filter is determined by the Equation methanol in wastewater can be as high as those declared by the
(10): company. However, as is known, all calculation methods consider
QFT ¼ S � vw ð10Þ negative dilution conditions, and in the absence of a flood, the
Glukhaya channel is considered as an independent water body;
moreover, isolated by the natural relief from the main channel of
where: vw = the washing speed (vw = 25 m∙h–1), S = filtration area
the Ob River. In addition, certain parts of the flooded areas, due
(m2); QFT = 3.23 m3∙h–1 (0.129∙25).
to elevation changes, communicate with the channel only during
Thus, the required volume of the filtrate tank is 1.1 m3.
a short period of time when the water level rises, i.e. 3–5 weeks
In order to supply water for washing filters, a centrifugal
during the flood period, and in fact remain isolated reservoirs for
pump was used. Sorbent was selected as the filter loading. After
the rest of the time, potentially acting as zones of accumulation
passing through the filter, the purified water from the filtrate tank
and concentration of pollutants. This is aggravated by the fact
flows to the discharge by gravity. Container-type block-modular
that a network of technological roads on embankments has been
built in the flooded areas.

FUNDING

Fig. 4. Block-modular container-type treatment facilities: a) general view, The research was performed at the expense of the subsidy for the
b) arrangement of equipment in a container: 1 = control cabinet, 2, 3 = air state assignment in the field of scientific activity for 2021,
pumps, 4 = equaliser, 5 = aeration tank, 6 = settler, 7, 8 = filters, No. FSRW-2020-0014.
9, 10 = liquid pumps, 11 = filtrate tank; source: own elaboration

treatment facilities (standard sea container pallet wide

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