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To cite this article: Jingxin Shi, Chunyan Xu, Yuxing Han & Hongjun Han (2020): Case study
on wastewater treatment technology of coal chemical industry in China, Critical Reviews in
Environmental Science and Technology, DOI: 10.1080/10643389.2020.1742530
Article views: 49
ABSTRACT
Coal chemical energy industry has
developed rapidly due to the pri-
mary position of coal in energy
reserves in China. At the same
time, coal chemical industry is
also a high-water consumption
industry. What’s more, coal chem-
ical wastewater contains high
concentration of phenols, NH3-N,
and toxic and harmful substances.
In the study, an all-round investi-
gation on wastewater treatment
technologies was conducted in
projects of the coal chemical
industry. These data were ana-
lyzed in detail from the aspects of
coal-to-gas project, coal-to-oil project, and coal-to-olefin project. In pretreatment, phenol
ammonia recovery device is the key section. At present, the process of first de-ammonia
with gas stripping method and then de-phenolization with extraction method is mostly
adopted in China. In microbiological treatment system, serious odor is diffused around
the sewage treatment facilities. Thus, negative pressure extraction measures should be
adopted in the microbiological treatment system. In addition, there is no suitable
method for the treatment of concentrated brine and crystal salt, so it needs further
study. Finally, this research can provide references for the problems of wastewater envir-
onment restriction existing in the long-term development of coal chemical industry.
1. Introduction
China’s energy structure is characterized by “rich coal, poor oil and gas”,
which determines that the development in China cannot be steady
conducted without coal (Zhao et al., 2013). In order to alleviate the contra-
diction between supply and demand of petroleum, natural gas, and other
CONTACT Jingxin Shi 15667087192@163.com State Key Laboratory of Urban Water Resource and
Environment, Harbin Institute of Technology, Harbin 150090, China; Yuxing Han yuxinghan@scau.edu.cn
School of Engineering, South China Agriculture University, Guangzhou, China.
ß 2020 Taylor & Francis Group, LLC
2 J. SHI ET AL.
EC anaerobic tower þ China coal longhua Relevant demonstration projects Patent technology is much, need COD 3000-4000 mg/L BOD All treated effluent The operation
BE biological Harbin; China in China can be referred. patent fee. 1500-2500 mg/L TN can be reused is stable.
enhanced process þ coal tuke; 200 mg/L Total phenol without outflow.
multi-stage A/O Datang fuxin. 500 mg/L Oil 150 mg/L COD 60 mg/L
NH3-N 15 mg/L
Activated coke Datang keqi Activated coke is self-sufficient Activation of activated coke is difficult; COD 4380 mg/L BOD After 2 years of Cannot meet the
adsorption þ and cheap; Activated coke The removal effect on inorganic 1400 mg/L NH3-N commissioning, the design requirements
microbiological can reduce the pollution of UF ions is poor; After the completion 200-250 mg/L Total effluent cannot reach of stable operation.
treatment film pollution and has the of the project, it has been in the phenol 920 mg/L Volatile phenol the standard and is
function of decolorizing debugging stage. Some problems 400 mg/L discharged into the
and deodoring. have been found in the evaporation pond.
debugging, and the design
requirements cannot be achieved.
Anaerobic Xinjiang qinghua Strong impact resistance; Large power consumption; Poor COD 4800 mg/L BOD The effluent cannot The effluent cannot
hydrolysis þ A/O Mature technology, easy microbiological treatment effect; 1400 mg/L NH3-N reach the design reach “zero
to operate. Large reaction tank volume; 310 mg/L requirement stably. discharge”.
Adsorbents have high investment
and consumption.
Anaerobic Inner Mongolia Effectively remove high ammonia Large floor area; Strong odor in - The effluent cannot There are some
hydrolysis þ SBR huineng; Shaanxi nitrogen; Simple device, low aerobic tank; Adsorbents have high reach the design problems in
jingbian. operating cost. investment and consumption. requirement stably. the design.
Anoxic-aerobic Shanxi linfen Simple process flow, strong Large power consumption; Packing COD 3000 mg/L NH3-N COD 140 mg/L Cannot meet the
process impact resistance; Low easy plugging; Poor effect on coal 650 mg/L Total NH3-N 230 mg/L design requirements
sludge yield. gasification wastewater treatment. phenol 250 mg/L Total phenol of stable operation.
0.9 mg/L
3T-BAF Shenhua ordos Strong impact resistance; Treatment of high concentration COD 5000 mg/L NH3-N Effluent is unstable. High concentration
Mature technology, wastewater adopts fenton and 300-500 mg/L Total of pollutants,
relatively easy to operate. ozone oxidation technology, which phenol 300-400 mg/L single nutrients,
has high treatment cost; 3T-BAF the lack of nitrogen
produce a large amount of H2S; and phosphorus;
High concentration of pollutants, Wastewater contains
single nutrients, and lack of a large number of oils,
necessary nitrogen and phosphorus phenol, long chain
nutrients in high concentration alkane substances,
organic wastewater are not resulting in poor
conducive to treatment effect and
microbiological treatment. unstable operation.
CRITICAL REVIEWS IN ENVIRONMENTAL SCIENCE AND TECHNOLOGY 9
Figure 1. Henan yima coal-to-gas project: (a) Hydrolysis acidification tank; (b) SBR; (c)
Floatation tank; (d) Advanced treatment.
tank (Figure 1c). The effluent of the air floating tank enters the filter,
whose main function is to intercept suspended substances (Tian, Ou, Liu,
Liang, & Pui, 2019). The effluent from the filter enters the chemical oxida-
tion process, which further reduces the concentration of refractory organic
matter in the wastewater (Figure 1d).
At present, the wastewater treatment plant operation has the issues of
serious foam problems, chemical dosage, and labor intensity. The TDS
of wastewater increases obviously due to the addition of a large number of
chemical agents. At the same time, air flotation pretreatment, SBR tank,
and other units in the operation of the wastewater treatment plant are not
covered for centralized treatment of odor.
invested 1.08 billion yuan to expand the project (250,000 t of methanol per
year), which was completed and put into production on December 30,
2008. The product quality reached the international AAA standard, and the
annual production capacity was 480,000 t of methanol.
Figure 2. China coal longhua Harbin coal chemical project: (a) EC anaerobic tower; (b) Rolling
contact oxidation process; (c) Coagulation precipitation process; (d) Biological aerated filter.
standards, GB8978-1996). COD removal ratio is more than 98%, and the
operation effect is stable for three years.
SDN tank. In the SDN tank, under the action of microbial metabolism,
most pollutants, such as COD, BOD, and NH3-N, are removed (Wang
et al., 2015). After the treatment by SDN, the sludge and wastewater are
separated in the secondary sedimentation tank, and the activated sludge
returns to the anoxic tank. The supernatant flows successively into the mix-
ing reaction tank and coagulation sedimentation tank. The supernatant of
coagulation sedimentation tank flows into the discharge tank for temporary
storage. At this time, the wastewater reaches the second-level discharge
standards (GB8978-1996, COD 120 mg/L, NH3-N 25 mg/L, and color
80 mg/L). The qualified wastewater will be lifted into the activated car-
bon filter adsorption tank to remove suspended substances and refractory
organic compounds. Then the wastewater from the activated carbon tank
will be temporarily stored in the collecting tank, and the water will be sent
to the production area for reuse by the recycling pump.
The sludge generated by the whole wastewater treatment system mainly
comes from the secondary sedimentation tank and the coagulation
CRITICAL REVIEWS IN ENVIRONMENTAL SCIENCE AND TECHNOLOGY 21
sedimentation tank. After concentration, the sludge is sent to the belt press
through the screw pump for dewatering treatment, and the generated cake
is transported abroad for disposal.
2. Waste problem
During the operation of each production unit of the project, a large
amount of solid waste and sludge will be generated, which are all hazard-
ous wastes (Di Fraia, Macaluso, Massarotti, & Vanoli, 2019). According to
the calculation, the amount of sludge from the wastewater is the largest,
accounting for more than 85% of the company’s total hazardous waste (Xu
et al., 2019). The existing process of sludge transportation and disposal
after dehydration has two disadvantages: the cost is high and the capacity
of local hazardous waste treatment centers is limited (Zeng et al., 2019). It
is suggested to adopt the process with long sludge age to reduce the
amount of residual sludge; Increase the return of residual sludge to the
anaerobic section; The residual sludge is put into the fluidized bed boiler
system and mixed into the coal burning system (accounting for 1% of the
coal) for high-temperature combustion.
treatment facilities adopt CAST process. The designed COD and NH3-N
values in the influent are 600-800 mg/L and 60-70 mg/L, respectively. The
actual COD and NH3-N values in the influent are 400-500 mg/L and 50-
60 mg/L, and B/C value is 0.5, which indicates that the wastewater has
good biodegradability.
The CAST microbiological treatment tank is operated by “influent-
aeration”, “influent-precipitation”, “influent-decanting”, and “influent-idle”
for 8 h and 3 cycles per day. The dissolved oxygen (DO) in the prereaction
area is controlled at 0.5 mg/L, the DO in the main reaction area is controlled
at 2-3 mg/L, and the reflux ratio in the main reaction area is 20%. The efflu-
ent from the CAST microbiological treatment tank is discharged from the
wastewater quality monitoring tank.
The wastewater treatment process is Wastewater ! Neutralization
tank ! Regulation tank ! CAST ! Effluent monitoring tank ! Standard
discharge. The CAST system is the main microbiological treatment process.
The treatment process of reclaimed water is as follows: Inlet !
Homogenizing tank ! Settling tank ! Non-valve filter ! Raw water
tank ! Self-cleaning filter ! Ultrafiltration device ! Ultrafiltration
tank ! Booster pump ! Filter ! High pressure pump ! Reverse osmo-
sis device ! Water tank ! Lifting pump ! Outlet.
The desalination water station of the project mainly supplies water for
boilers and some process water. The desalination water station is divided
into two sets of devices, namely raw water treatment system and conden-
sate recovery treatment system. The treated water volume of the
raw water treatment system is 1500 m3/h, the processing flow is
“Double membrane method (ultrafiltration þ reverse osmosis) þ Cation
exchange þ Anion exchange þ Mixed ion exchange”, and the total recov-
ery rate is about 65%. The recovered condensate includes turbine con-
densate (500 m3/h) and process condensate (500 m3/h). The process flow
is “Activated carbon filter þ Iron removal filter þ Mixed bed ion exchange
method”.
In the influent, COD is about 1300 mg/L, BOD is about 50 mg/L, and NH3-
N is about 250 mg/L; In the effluent, COD is about 60 mg/L, BOD is about
10 mg/L, and NH3-N is about 10 mg/L.
Figure 6. (a) Crystallized salt from the concentrated brine; (b) Effluents from each process.
Finally, the effluent is then lifted by the sewage pump to the multimedium
filter, activated carbon filter, ultrafiltration system, and reverse osmosis
device for advanced treatment.
gasifier is mainly due to the high content of sulfur, fluorine, and chlorine
in coal. Halogenated corrosion and sulfate corrosion can occur under cer-
tain conditions of temperature, pressure, and oxygen medium. This corro-
sion problem can be solved by using nickel - based wire to surfacing the
inner surface of gasifier. Now this problem has been basically solved, which
provides a reference for the application of moving bed gasification technol-
ogy in the same coal quality.
Because the high oil coal in Naomao lake is used in this project, the oil
content in the gasification wastewater is high (> 1000 mg/L in the influ-
ent), far exceeding the design value. As a result, the air flotation device is
severely foamized and cannot operate normally (Figure 7). And the overall
operation of the wastewater treatment in this project is bad. The concentra-
tions of COD and NH3-N in the influent are 4000 mg/L and 400 mg/L,
respectively. While COD and NH3-N in the effluent are 150-300 mg/L and
20-60 mg/L, respectively, which cannot meet the standards (First-level dis-
charge standards, GB8978-1996).
Figure 7. (a) Phenol ammonia recovery unit; (b) Air flotation device; (c) Main microbiological
treatment process; (d) Anaerobic reactor.
6. Summary
6.1. Pretreatment
Pretreatment includes precipitation, filtration, extraction, stripping, and
other units to remove part of the ash, oil, etc. Coal gasification wastewater
CRITICAL REVIEWS IN ENVIRONMENTAL SCIENCE AND TECHNOLOGY 33
(Zhuang, Hong, Han, & Shan, 2016). For enterprises adopting the fluidized
bed gasification technology, the composition of gasification wastewater is
relatively simple and the biodegradability is good. Therefore, conventional
microbiological treatment technology can meet the first-level discharge
standards of wastewater treatment. The concentration of organic pollutant
in coal direct liquefaction enterprise is high and it is difficult to treat. The
treatment of such wastewater is usually similar to the biological treatment
process of the fixed-bed gasification wastewater. In the treatment of high
concentration organic wastewater, it is found that EBA multistage micro-
biological combination process is a more suitable technique. After treat-
ment of EBA system, the wastewater can reach the first-level discharge
standards (GB8978-1996). COD removal ratio is more than 98%, and the
operation effect is stable.
fermentation of pollutants will cause the overflow of the regulating tank and
affect the environment. It is suggested to seal the regulating tank and
increase the treatment facilities of odor (Lee, Moon, & Cho, 2017). Negative
pressure extraction measures should be adopted in the regulating tank to
send the odor to the treatment system. Furthermore, some photocatalytic
advanced oxidation processes show a potential in degradation of volatile
organic compounds in industrial effluents (Fernandes, Ga˛gol, Makos, Ali
Khan, & Boczkaj, 2019a; Fernandes, Makos, Wang, & Boczkaj, 2019b), which
can be further studied in the treatment of coal industry wastewater.
3. Evaporation pond and salt
The wastewater treatment system mentioned above is mainly designed
based on the situation of wastewater generation under normal working
conditions, but the discharge of wastewater under abnormal working con-
ditions is huge. For example, the equipment needs to be cleaned before
driving, which will produce tens of thousands m3 of wastewater containing
suspended substances and iron. The recycling wastewater station will pro-
duce the premembrane wastewater in the process of chemical premem-
brane, and the salt content in the premembrane wastewater is high because
a large number of chemicals are added in the premembrane process.
Wastewater treatment station sludge needs to be cultivated and acclimated,
usually in 3 to 6 months, during which time wastewater treatment often
fails to achieve the expected effect and needs to be discharged. The fluctu-
ation of wastewater quantity and quality can occur in the case of startup
and production of each process unit, which will have an impact on the sub-
sequent wastewater treatment.
At present, in the Datang olefin project, Datang keqi coal-to-gas project,
and Shenhua coal-to-oil project, the evaporation pond maintains high
wastewater level, and basically all the wastewater generated by abnormal
working conditions is stored. The wastewater level of the evaporating pond
can be reduced by adding the spraying device and the backwater pump to
return the wastewater from the evaporating pond to the treatment plant
(Silva, Gonzalez, & Suarez, 2017). The infiltration of the concentrated brine
in the evaporation pond may cause the local groundwater pollution, and
improper disposal of soluble salt may cause secondary pollution. At pre-
sent, there is no proper way to dispose the crystallized salt produced by
evaporation crystallization.
7. Conclusion
To sum up, most of the projects that have been put into operation at present
have different degrees of environmental problems. So far, none of the projects
36 J. SHI ET AL.
Funding
This work was supported by National key research and development program-China
(2017YFB0602804).
ORCID
Jingxin Shi http://orcid.org/0000-0002-1504-5637
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