Catalysts and Biocatalysts Combinations for Hydrocarbon Pollutants Elimination: Comparison
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Due to the presence of environmental problems, it is urgent to improve the processes aimed at the processing and purification of hydrocarbon-containing wastes and wastewaters. The research presents the latest achievements in the development of nanostructured catalysts made from different materials that can be used to purify oil-polluted wastewaters (petroleum refinery wastewater, oilfield-produced water, sulfur-containing extracts from pre-oxidized crude oil and oil fractions, etc.) and eliminate components of hydrocarbon pollutants (polyaromatic hydrocarbons, phenols, etc.). The results of the analysis of possible combinations of chemical and biological catalysts for deeper and more effective solutions to the problems are discussed. The possibilities of highly efficient elimination of hydrocarbon pollutants as a result of the hybrid application of nanoparticles (graphene oxide, mesoporous silica, magnetic nanocatalysts, etc.) or catalytic nanocomposites for advanced oxidation processes and biocatalysts (enzymes, cells of bacteria, mycelial fungi, phototrophic microorganisms and natural or artificial microbial consortia) are analyzed. 

  • nanocatalysts
  • nanocomposites
  • hydrocarbon pollutants

1. Introduction

In the 21st century, industries related to the extraction, transportation, storage, processing and use of hydrocarbon raw materials continue to actively develop. Various wastewaters of oil-producing, oil-refining, chemical, transporting and other fields of industry form multi-tonnage effluents containing residual concentrations of hydrocarbons [1][2][3][4]. The volume of oilfield-produced water (OPW) alone is on average at least 250 million barrels per day worldwide [2][5][6]. Crude oil emulsions and hydrocarbon-contaminated wastewaters and soils are considered sources of potential threat to the environment and living objects [7].
Polyaromatic hydrocarbons (PAHs) and benzene, toluene, ethylbenzene, and xylenes (BTEX) usually predominate among dissolved organic compounds in hydrocarbon-containing wastes [8].
Hydrocarbon-containing wastewaters may contain various toxic organic compounds: aromatic substances, MTBE (methyl tert-butyl ethers), naphthenic acids, methanol, ketones, ethers, brominated organic compounds, estrogens, PCBs (polychlorinated biphenyls), phthalates, linear alkyl benzene sulfonates, furans and others [1][4][9][10]. However, BTEX are rarely considered due to their high volatility and rapid decomposition in water as a source of serious ecotoxicological effects. It is believed that phenols and PAHs (naphthalene, acenaphthylene, acenaphthene, fluorene, phenanthrene, anthracene, fluoranthene, pyrene, chrysene and others) pose the greatest danger to the environment and human health. Alkylphenols, especially with long (C7–C9–carbon) chain, and naphthenic acids can have a significant negative effect on the endocrine system, causing estrogenic effects in vertebrates [6][11].

2. Combined Applications of NCs and BCs for Elimination of Hydrocarbon Pollutants

It is known today that chemical-only or biocatalytic-only approaches are rarely used for deep wastewater treatment containing hydrocarbon pollutants. The mechanisms of action of NCs and BCs for individual application are described in detail in many articles and mainly depend on the chemical composition of hydrocarbon pollutants and catalysts, as well as the conditions for the treatment of contaminants [4][9][12][13][14][15][16]. The possibility of their combination at the secondary and tertiary stages of wastewater treatment is most often considered [10][17]. The development and implementation of NCs and NComs (Table 1) in combination with highly efficient BCs (Table 2) is the basis for successfully solving urgent problems related to the processes of water and soil purification from hydrocarbon pollutants. Two approaches to the integration of chemical and biocatalytic stages of wastewater treatment are known: (a) sequential physical–chemical and biocatalytic treatment conducted in different combinations and (b) the simultaneous carrying out of physical–chemical treatments and biodegradation in one reactor.
Table 1. Advanced oxidation processes with NCs and NComs for degradation of hydrocarbon pollutants *.
NCs/NComs; Size (nm)

[Reference]		 Pollutants Reaction Conditions Removal

Efficiency (%)
Heterogeneous photocatalysis
TiO2

O
2
, 100 ℃, 0.5 h
89.58% of COD, 87.38% of TOC
* COD—chemical oxygen demand; MIL—Materials of Institute Lavoisier; MIL-101(Cr)—metal–organic frameworks (MOFs) based on chromium (III) and polymeric terephthalate; M.MIL-100(Fe)—mesoporous metal–organic framework based on iron (III) carboxylate; OPW—oilfield-produced water; PAHs—Polycyclic aromatic hydrocarbons; PRW—petroleum refinery wastewater; SOG—soap oil and grease; TiO2@ZnHCF—Titanium dioxide based zinc hexacyanoferrate framework; TOC—Total organic carbon.
Table 2. Biocatalytic treatments of various hydrocarbon pollutants.
Biocatalyst [Reference] Pollutants Conditions and Degradation Efficiency
Homogenous BCs
(30 nm) [18] Phenol (300 ± 7 mg/L), soap oil and grease (SOG) (4000 ± 23 mg/L) in oil refinery wastewater 8 g/L of catalyst, aeration flow rate of 1.225 L/min, 90 min 76% of phenol and 88% of SOG
Achromobacter xylosoxidans [33] Pyrene 100 mg/L pH 7–9, 37–40 °C, 0–2.5% NaCl,

15 days, 50% of of pyrene
TiO2

(44.3–48.0 nm) 		[19] Anthraquinone

(0.5 mg/L)		 200 mg/L of catalyst, solar irradiation 100 mW/cm2, 240 min 57%
Haematite (α-Fe2O3) [20] Petroleum refinery wastewater

COD 1257 mg/L		 pH 7.5, 1.494 g/L of catalyst, H2O2/COD ratio of 1 mg/mg, UV-A lamp solar irradiation,

90 min		 90.85% of COD
Petroleum refinery wastewater


(52.2 mg/L COD)
Membrane bioreactor (MBR)-H
2
O
2
/UV Hybrid pretreatment before nanofiltration


80% of COD degradation for 1 h
To choose a hybrid approach to the removal of pollutants, one of the key parameters is the initial chemical content of the cleaning object and the initial concentration of toxic components. At high concentrations of phenol in effluents, it is recommended to carry out preliminary chemical treatment in combination with further biocatalytic stages [63].
Petroleum refinery wastewater is a complex mixture of hydrocarbons, sulfides, ammonia, oils, suspended and dissolved solids and heavy metals. Depending on the type of wastewater (desalinated, acidic, spent alkaline and oily wastewaters), various sequential combined physical–chemical-biocatalytic purification methods are proposed at the secondary treatment stage (ozonation with treatment in a biofilm reactor with a movable layer or photocatalysis with treatment in a biofilm reactor with a compacted layer, etc.) [17][64].
For the purification of oilfield-produced water containing a mixture of suspended substances (including PAHs: pyrene, phenanthrene, anthracene and naphthalene) and dissolved organic (a mixture of phenol, benzene, xylenes, toluene and ethylbenzene) and non-organic (cations of barium, calcium, magnesium, sodium, potassium and heavy metals and anions such as chloride) compounds, biocatalytic treatment is usually carried out at the secondary stage of purification. Aerobic biocatalytic treatment is followed by a tertiary deep purification stage, which includes one or more stages: electrodialysis, macroporous polymer extraction (MPPE), microporous membrane treatment, electrolysis, ion exchange and AOPs [10]. In general, with the subsequent combination of several approaches to purification, the biocatalytic stages are now successfully combined with membrane technology, advanced oxidation processes (AOPs), electrochemical methods and other modern purification technologies. Among the advantages of hybrid sequential or one-time implemented processes, their environmental friendliness and the possibility of saving resources are indicated. Thus, for the complete mineralization of organic compounds, photocatalysis usually requires too much energetic costs and is often accompanied by the formation of dangerous by-products. The combination of photocatalysis and biodegradation joins the advantages of both technologies; is characterized by simple functioning, low energy consumption and high cleaning efficiency; and represents an actual direction of the current trend of research [65][66].
Membrane bioreactors are increasingly being offered as the technological design of hybrid processes associated with the deep purification of real wastewater [62][67]. Among the main competitive advantages of membrane technologies, it is possible to note the production of highly purified wastewater and the possible separation of growing biomass in a membrane bioreactor. In membrane bioreactors, biological purification is successfully combined with the microfiltration/ultrafiltration/nanofiltration/direct osmosis of effluents. At the tertiary stage of purification, membrane bioreactors are combined with membrane distillation and electrodialysis [68]. To improve the operation of membrane bioreactors, the use of various nanomaterials is being actively mastered [69]. Membrane systems based on nanomaterials provide an increase in the available flow rate per square unit of the membrane and contribute to the even more efficient removal of target contaminants with a longer period of membrane operation [68]. It is obvious that the development of membrane technologies in combination with nanomaterials with NCs and BCs is a fundamental trend in the current development of technologies for the elimination of hydrocarbon pollutants.
The successful application of a membrane bioreactor was demonstrated during the purification of petroleum refinery wastewater using a hybrid approach combining the intimate coupling of photocatalysis and biodegradation (ICPB) [67]. ICPB assumes the simultaneous carrying out of physical–chemical treatment and biodegradation in one reactor and ensures the achievement of good results in the decomposition of PAHs [65].
When combining different processes in one reactor, biodegradable intermediate products obtained as a result of the physical–chemical treatment of waste are immediately biodegradable. Thus, during the photocatalytic destruction of toluene, its partial transformation to biodegradable intermediates was ensured. Then, the appeared product was immediately mineralized by microorganisms [70].
Today, hybrid processes such as ICPB are known for the degradation of hydrocarbon pollutants (Table 3) [67][70][71][72][73][74][75][76][77][78] and some persistent and toxic organic pollutants [65]. At the same time, it can be argued that research in this direction is currently almost at the initial stage of development but will actively advance in the near future.
Table 3. Variants of the intimate coupling of photocatalysis and biodegradation (ICPB) for hydrocarbon pollutants treatment *.
Pollutants

[Reference]		 NCs/NCs; Size (nm)

Physical or/and Chemical Treatment		 BC/Co-Substrate Removal Efficiency (%)
Naphthalene,

Phenanthrene,

Anthracene,

Fluoranthene,

Pyrene (PAHs) in soil (200 mg/kg) 		[71] Ag3PO4@Fe3O4

UV-visible light

photocatalyst

(100–300 nm)		 Adapted consortium (sewage sludge) in microcapsules of Ca-alginate gel and carboxymethyl cellulose 94% of PAHs mixture,

~100% of naphthalene, phenanthrene, anthracene,

~93% of fluoranthene, pyrene

for 30 days
Phenanthrene in water (PAH) [72] Composite Mn3O4/MnO2-Ag3PO4

photocatalyst under visible light illumination		 Biofilms with Shewanella, Sedimentibacter, Comamonas, Acinetobacter and Pseudomonascells 96.2% degradation for 20 min,

100% non-toxic intermediates

for 10 h
Phenanthrene

in water 		[73] Cu/N-codoped TiO2 photocatalyst under UV or visible light illumination PAH-degrading bacterial consortium with Pseudomonadaceae cells UV (88.63% ± 0.71%) or visible light (62.87% ± 2.19%) from 10 mg/L for 6 h at room temperature;

9.31% ± 0.82% when only cells as BCs

are used
ZnO or NiO [13] [36Anthracene

(101.8 mg/L)		 pH 7.2, 55.6 mg/L of catalyst, emulsion solution—230 min, anthracene aqueous ethanol solution—280 min 90% with ZnO and 87% with NiO for anthracene emulsion solution; 81% with ZnO and 86% with NiO for anthracene aqueous ethanol solution
] Oilfield-produced water (7 mg total hydrocarbons/L) and crude oil (32 mg total hydrocarbons/L) 5 days, 20 °C; 36.8 ± 4.2 μmol photons/m2
Pyrene (PAH) [74]/s Cu/N-codoped TiO2 photocatalyst under visible or UV light illumination

28.5% degradation from

oilfield-produced water;

34.3% degradation from crude oil		 PAH-degrading bacterial consortium 63.89% ± 1.03%

(Visual light biol. treatment)

>61.27% ± 1.08% (UV biol. treatment)

>59.58% ± 1.15% (UV)

>57.41% ± 1.13% (Visual light)

>6.65% ± 0.72% (biol. treatment)

>1.70% ± 0.34% (control)		 ZnO nanorods

2.11 ± 0.32 μm length and 96.26 ± 11.13 nm diameter 		[21]
Rhodocccus erythropolis or Pseudomonas stuzeri [37]Phenol

(10 mg/L)		 PAHs

(332.2 mg/kg soil)pH 5,

visible light 1000 W/m		2, 5 h 84.3%
Slurry Bioreactor, 28 °C, pH 8.2; 8 mg/L dissolved oxygen, 15 days, 70–80% degradation
Phenol, 4-chlorophenol (4-CP), and 4-fluorophenol (4-FP) [75] N-doped TiO2 (30 nm) coated POHFs/combined UV and visible light Microbial consortium: Scenedesmus obliquus

(		S. obliquus) biofilm with Rhodococcus and

Pseudomonas cells The removals of DOC and COD of the phenolic compounds in mixture

(1.06 mM phenol, 0.39 mM of 4-CP and 0.45 mM of 4-FP) for 11 h are

~98% and ~91%, respectively		 ZnO/SiO2 with Palash leaves extract

(3–35 nm)
Brevibacillus brevis[22] Acenaphthylene (176 mg/L), COD (497 mg/L) in petrochemical wastewater [38]1 g/L of catalyst, 30 °C,

visible light, 4 h		 79% of Acenaphthylene, 70% of COD
Naphthalene and pyrene

(100 mg/L)		 pH 5.0, 25 °C, 18 days, 80% of naphthalene
Toluene [70] N-doped TiO2/PP Microbial

consortium		 99%, with the elimination capacity of 550 g/m3/h HS-CuS-HNCs

Hierarchically structured CuS hollow nanocatalyst 		[12]
Proteus mirabilis [38
1,2,4 trichlorobenzene [76]Petroleum refinery wastewater

(COD 380 mg/L)		 pH 7.6, 1 g/L

of catalyst, 180 min, 10 cycles		 about 66% of COD
pH 5.0, 25 °C, 18 days, 94% of naphthalene ] Sugarcane cellulose-TiO2 Microbial

consortium		 68.01%, which is 14.81% higher than that of biodegradation or photocatalysis alone, and the mineralization rate is 50.30%, which is 11.50% higher than that of photocatalysis alone TiO2@ZnHCF

Titanium dioxide based zinc hexacyanoferrate framework nanocomposite (100 nm) 		[23]
Rhodococcus quinshengi [38]Tricyclic PAHs:

acenaphthene, phenanthrene and fluorine

(2 mg/L)		 Neutral pH, 15 mg/L of catalyst, sunlight, 6 h 93–96% from water, 82–86% from soil, 81.63–85.43% from river sediment
pH 5.0, 37 °C, 18 days, biodegradation:

94% of naphthalene, 56% of pyrene
Phenol (100 mg/L) [77] CdS@SiO2@TRP nanocomposite photocatalyst under intermittent visible light irradiation Adapted

Pseudomonas putida cells		 Simultaneous removal

97.24% of phenol for 10 h		 Fe3O4/Cu2O-Ag nanocomposite (5 nm) [24] PAHs: naphthalene (5 mg/L), benzo(a)pyrene (5 mg/L), anthracene (5 mg/L)
R. ruber Ac-1513 D and

R. erythropolis Ac-1514 D [39]0.5 g/L of catalyst, visible light, 60–180 min 80–90%
Petroleum hydrocarbons 446.7–526.8 g/kg dry soil
Petroleum refinery wastewater [67] Anatase nanocrystalline particles TiO2 (14 nm), catalyst concentrationAerobic-anaerobic bioremediation method with 108 cells/mL; nitrate salt is used as electron acceptor on area 25 × 30 m2 3 times with a 3-week interval; 20–30 °C; 63 days; Degradation of saturated, aromatic and resin-asphaltene was 72.6%, 66.5% and 57.2%, respectively. Microbial consortium in Membrane Bioreactor, pH 10 100 mg/L of TiO2;

32% and 67% of TOC and

TN for 90 min		 MIL-101(Cr)/Fe3O4-SiO2

(35% of Fe		3O4-SiO2)

Superhydrophobic composite

(400/80–120 nm) 		[14] Synthetic and real oilfield-produced water (TPH 170 mg/L, COD 550 mg/L) pH 4, 0.5 g/L of catalyst, visible and UV light, 150 min
R. ruber Ac-1513 D and

R. erythropolis Ac-1514 D [40] Oil products

482 g/kg dry soil (48%)		 Hydrolysis of the bituminous crust by calcium hydroxide (2%) 3 times with a 3–4-day interval; bioremediation with Rhodococcus strains (10697.7% and 99.2% of TPH, 95.17% and 96.6% of COD from real and synthetic OPW, respectively
cells/mL) was conducted 3 times with a 7-day interval;
Benzene (100 mg/L), toluene(100 mg/L), and xylene (100 mg/L) [78]

20–30 °C, pH 7.8; 33 days for 26.4–48.2% degradation of oil pollution		 Fenton-like oxidation process
Zinc sulfide (ZnS) nanoparticles (20–90 nm), UV-A light, 28 °C, pH 4 Aspergillus niger 100% for 1 h R. ruber Ac-1513 D and R. erythropolis Ac-1514 D [41] Oil products

98 g/kg dry soil (9.8%)		 Anaerobic bioremediation, 109 cells/mL

electron acceptor Ca(NO		3)2; 1.25%, 28 °C,

pH 7.8; 10 days; potential degradation of the oil pollution 90% for 90 days		 Nanoscale zero-valent iron (nZVI), commercial

(50 nm) 		[25]
Extremophilic consortium: Ochrobactrum, Bacillus, Marinobacter, Pseudomonas, Water from oil and gas exploration site (15 different PAHs present in real water samples; Naphthalene (201.46 μg/L) and benzo(g,h,i) perylene

(23.15 μg/L)		 Martelella, Stenotrophomonas and Rhodococcus [42]pH 2.94, 4.35 g/L of nZVI,

1.60 g/L of H		 Low-molecular-weight (LMW) petroleum hydrocarbons (200 ppm) such as anthracene, phenanthrene,

2O2, 199.90 min 89.5% and 75.3% of PAHs and COD, respectively
fluorene and naphthalene Soil, 8% salinity, pH 10, 60 °C,

8 days, 100% degradation efficiency		 MgAl-LDH@Fe3O4 [26] Concentrated liquor of gas field wastewater (refractory organic pollutants) pH 5, heterogeneous electro-Fenton system, 4 h 88.18% for COD
High-molecular-weight (HMW) hydrocarbons such as pyrene (100 ppm), benzo(e)pyrene (20 ppm), benzo(k)fluoranthene

(20 ppm) and

benzo(a)pyrene (20 ppm)		 Soil, 8% salinity, pH 10, 60 °C,

8 days, 93%, 60%, 55% and 51% degradation		 Cl/S-codoped carbon nitride nanotube clusters (Cl/S-TCN) [27] Oilfield-produced water
Consortium: Campylobacter hominis, Bacillus cereus, Dyadobacter koreensis, Pseudomonas aeruginosa, Micrococcus luteus [pH range 3–9, metal-free photo-Fenton, 10 mM H2O2 82.6% for COD
43] Bonny light crude oil 2% (v/v) crude oil, 30 °C,

21 days 73% degradation		 Ozonation
Consortium of genus Pseudomonas, Methylobacillus, Nocardioides, Achromobacter, Methylophilaceae, Pseudoxanthomonas, Caulobacter [15] The final concentration of total PAHs from coal and petroleum was 97.63 mg/ kg dry weight soil 35 days, 25 °C, in soil;

75% PAHs		 CuO/Activated carbon

(250~350 nm) 		[28] Heavy oil refinery wastewater (oil 78 mg/L, COD 2950 mg/L) pH 7.3, 5.0 g of catalyst,

90 mg/L of O		3, 75 min 94.2% of COD

89.7% of oil
Halophilic bacterial consortium [44] PAHs Sulfate radical-based oxidation
12 days, pH 7.4, 40 g/L NaCl concentration OMS-2

Manganese oxide octahedral molecular sieve nanorods 		[29] PAH: phenanthrene (1.0 mg/L) in water and sewage pH range 4–11, 0.1 g/L of catalyst,

peroxomonosulfates

6 mmol/L, room temperature, 360 min, 3 cycles		 >99%, 68%, 82% and 79% from model wasterwater, tap water, Yellow river and Qinghai lake, respectively
Hybrid chemical processes with nanocatalysts


low-molecular-weight (above 90% for phenanthrene and fluorene) and high-molecular-weight (69  ±  1.4 and 56  ±  1.8% at 50 and 100 mg/L of pyrene) polycyclic aromatic hydrocarbons (PAHs)
Benthic diatom-associated bacteria [45] 3 μg/L Benzo(a)pyrene and 265 μg/L fluoranthene 7 days, 88% of fluoranthene,

79% of Benzo(a)pyrene
Consortium: Aspergillus niger,

Aspergillus sydowii,

Fusarium lichenicola [46] 101.7 mg/L PAHs

in oilfield wastewater		 21 days, 85.2% degradation

(with 100% naphthalene and chrysene)
Consortium of Chlorella sp. and Rhodococcus wratislaviensis with

preliminary adaptation 		[47] Mixture of 50 mg/L phenanthrene, 10 mg/L pyrene,

10 mg/L benzo[a]pyrene		 24 °C, 200 μmol photons/m2/s,

150 rpm, 21 days

100% degradation		 HS-CuS-HNCs

Hierarchically

structured CuS hollow nanocatalyst 		[12
Nannochloropsis oculata]

or 		Isochrysis galbanaPetroleum refinery wastewater

(COD 380 mg/L)		 Heterogeneous

photocatalysis/H		2O2

pH 2, 0.2 g/L of catalyst, 10 mM H		2O2, room temperature, 2 h 95% of Phenol,

95% of Biphenol A, 85% of

Atrazine
CuO/ZrO2

nanocomposite

40.32 nm 		[31]
Halomonas shengliensis [34] Pyrene 50 ppm 25 °C, 10 g/L NaCl; 50% degradation
Penicillium sp. [35] Crude oil 1% (v/v) 14 days, 30 °C; 57% degradation with

preliminary adaptation 		[48]Heterogeneous Oilfield-produced water

(270 mg oil/L)

photocatalysis/H		2O2

pH 7.6, 1000 mg/L of catalyst, 3000 mg/L of H		2O2, room temperature, solar-light, 2 h pH 7.2, 25 ± 1 °C,

light photoperiod—18:6 (2000 lux);		 Marine diesel

(100 mg/L)
Chlorella vulgaris 98% of COD


66.5–68% degradation M.MIL-100(Fe)@ZnO [30] Phenol (5 mg/L),

Biphenol A (5 mg/L),

Atrazine (5 mg/L)
Immobilized BCs including self-immobilized systems (biofilms) Heterogeneous
Bacterial consortium immobilized in magnetic floating biochar gel beads [49] Pyrene (20 mg/L), benzo(a)pyrene (10 mg/L),

indeno(1,2,3-		cd)pyrene

(10 mg/L)

photocatalysis/H		2O2

0.5 g/L of catalyst, 400 °C, 0.3 g/L of H		2O2, visible light, 6 h Seawater, pH 8.1, 30 °C, 30‰ salinity, 16 days.96.96%


Biodegradation:

89.8%, 66.9% and 78.2% of

PYR, BAP and INP, respectively		 Cu-based perovskite oxides (La2CuO4) [32]
Biofilm and pellets of consortium (key functional genera: Rhodobacter, Citreibacter, and Roseovarius) [50]Petroleum refining wastewater

(COD 3800 mg/L

TOC 1259 mg/L)		 Oilfield-produced water

(6.38 ± 2.31 mg oil/L)Wet air oxidation

processes/H		2O2 pH 7.5–8.0,

0.75 g/L of catalyst, 7 mL/L of

30% H		2 multistage bio-contact oxidation reactor, pH 7.5–8.1, 45–50 °C,

44.07% oil degradation
Microbial mats (cyanobacteria and bacteria) [51] Oilfield-produced water

(4.3 ± 1.0 mg of the C		10 to C30 alkanes/g mats) 28 days, 30 °C, 50 rpm, pH 8.5, 18 ppt salinity, with partially hydrolyzed polyacrylamide;

41–49% degradation
Active sludge [52] Synthetic produced water

(255 mg oil/L)		 Aeration tank, 3.5 L/min air, pH 6.0,

7 days; 51 g/L sodium chloride,

99.01 ± 0.28% degradation
This system contained dissolved air flotation (DAF), yeast bioreactor (yeast immobilized on policyurepan), upflow anaerobic sludge blanket reactor (UASB), and biological aerated filter [53] Oilfield wastewater

(145 mg oil/L)		 60 days,

99.6% oil degradation
Native halophilic bacterial consortium immobilized on walnut shell [54] Synthetic oilfield-produced water (191 mg/L oil) 48 days, moving bed biofilm reactor,

97.8% oil degradation
Methanogenic culture derived from a high-temperature oil reservoir production water [55] Paraffinic n-alkanes

(C22–C30)		 97% degradation and biogas accumulation, 736 days
Consortium immobilized in cryogel of poly (vinyl alcohol): AC1 (80% anaerobic sludge plus 10% Desulfovibrio vulgaris plus 10% Clostridium acetobutilycum) for the straight-run gasoline fraction (Nafta) and AC3 (70% anaerobic sludge plus

10% 		D. vulgaris plus

10% 		C. acetobutilycum plus

5% 		Rhodococcus ruber plus

5% 		Rhodococcus erythropolis) for the straight-run diesel oil raction, non-hydrotreated vacuum gas oil, gas condensate, and crude oil [56] Sulfur-containing extracts from pre-oxidized crude oil, non-purified vacuum gas oil, straight-run gasoline fraction (Naphtha), gas condensate and straight-run diesel fraction

(7–10 g/L COD)		 Biotransformation in methanogenic anaerobic reactor,

100% conversion of S-organic compounds to inorganic sulfide or biomass, biogas accumulation with 68–76% of CH		4 for 20 days
Consortium immobilized in cryogel of poly (vinyl alcohol): AC6 (80% anaerobic sludge plus

10% 		Rhodococcus opacus plus

10% 		Desulfovibrio desulfuricans) [57] Sulfur-containing extracts from pre-oxidized crude oil and oil fractions with hydrolysates of chicken manure and Chlorella vulgaris biomass (6.4–16 g/L COD) Biotransformation in methanogenic anaerobic reactor, 100% conversion of S-organic compounds to inorganic sulfide or biomass, biogas accumulation with greater than

70% of CH		4 for 6–42 days
Consortium immobilized in cryogel of poly(vinyl alcohol): AC6 (80% anaerobic sludge plus

10% 		R. opacus plus

10% 		D. desulfuricans) and

AC7 (90% adapted DEAMOX sludge plus 10% anaerobic sludge) 		[57] Sulfur-containing extracts from non-purified vacuum gas oil with hydrolysates of chicken manure and Chlorella vulgaris biomass

(6.4 g/L COD)		 The two-stage biotransformation in methanogenic anaerobic reactor (MAR) and denitrifying ammonium oxidation (DEAMOX) reactor;

100% conversion of S-organic compounds to inorganic sulfide or biomass, biogas accumulation with 70% of CH		4 for 20 days
Combination of BCs with nanomaterials
S. aestuarii 357 [58] Naphthalene

(0.128 mg/L)		 Two stages: (1) the formation of the naphthalene@FeNP-NDI-DA complex with FeNP-NDI-DA nanoparticals; (2) addition of S. aestuarii 357; 100% biodegradation
Brevibacillus parabrev

1.13 × 10		8 cells/mL [59] Oily wastewater: Tetradecane 3% Magnetic NPs of Fe3O4 (10 nm) 76% tetradecane was degraded by cells for 15 days
Halamonas sp., Vibrio gazogenes or Marinobacter hydrocarbonoclasticus [60] Crude oil (375 mg/L) Polyvinylpyrrolidone (PVP)-coated iron oxide NPs (11.2 nm)

100% oil degradation for 24–48 h
M. hydrocarbonoclasticus [61] Crude oil (0.5% w/v) Facile chemical modification of mesoporous

silica NPs (mSNPs) (10 nm)

100% oil degradation for 45 days
Bacillus cereus

1.55 × 10		5 cells/mL [16] PAHs: Anthracene, phenanthrene Graphene oxide quantum dots (GOQDs)

52.7% degradation of PAHs for 3.5 days

(1.7% degradation in control sample)
Consortium in

membrane bioreactor 		[62]
* TOC—total organic carbon; TN—total nitrogen; TRP—thermal-responsive polymer, which was composed of N-isopropyl acrylamide, acrylamide and the cross-linker N,N′-methylenebisacrylamide; PP—polypropylene; POHFs—photocatalytic optical hollow fibers; DOC—dissolved organic carbon.
Among the known ICPB processes involving NCs, processes with TiO2 and its derivatives predominate, which provide the destruction of toluene [70], phenanthrene [73], pyrene [74], phenol, 4-chlorophenol (4-CP) and 4-fluorophenol (4-FP) [75], 1,2,4-trichlorobenzene [76] and petroleum refinery wastewater [67].
For those processes, where a comparative assessment of the effectiveness of joint and separate applications of biocatalysis and photocatalysis was carried out, the ICPB priority was shown [74][76]. The processes of hybrid biological and photocatalytic degradation of PAHs in soil with Ag3PO4@Fe3O4 and in water with Mn3O4/MnO2- Ag3PO4 have been studied with the combined use of microbial BCs and NCs with photocatalytic activity in visible light [71][72]. The test of biocompatibility showed that Ag3PO4@Fe3O4 had practically no negative effect on the activity of soil microorganisms. These results open up new prospects for the joint use of photochemistry and biocatalytic technologies to solve urgent problems of environmental biotechnology, particularly for the removal of hydrocarbon pollutants.
For hybrid systems involving the combined use of chemical and biological catalysis, it is important to not only ensure the biocompatibility of components but also protect the activity of BCs. A hybrid photo-controlled reversible photocatalytic ICPB system has been developed with a mechanism of protecting microorganisms from the attack of reactive oxidative species formed during photocatalysis [77]. The surface of the CdS-photocatalyst was coated with SiO2, and then a thermosensitive polymer (TRP) was applied to cover the surface of CDs@SiO2. This polymer was composed of N-isopropyl acrylamide, acrylamide, and the cross-linker (N,N′-methylenebisacrylamide). The resulting CdS@SiO2@TRP was attached to the surface of graphene (photothermal converter) to form a photo-controlled reversible photocatalytic system. Without light irradiation, soluble pollutants were biodegraded or absorbed by the CdS@SiO2@TRP. Under light irradiation, reactive oxidative species, photogenerated due to the activation of the protective polymer cover, were formed inside CDs@SiO2@TRP and photocatalytically decomposed the pollutants without contact between reactive oxidative species and microorganisms.
It should be noted that in hybrid systems, in addition to chemical and biocatalytic components, there is most often an important component such as a carrier, whose role is not limited to protecting BCs from the influence of negative environmental factors, particularly free radicals [79]. Among carriers, priority is given to biocompatible materials (cellulose, ceramics and loofah) [66][80]. Microcapsules based on Ca-alginate gel and carboxymethyl cellulose successfully protected BCs from direct contact with the photocatalyst and free radicals, increasing the life of BCs during the photocatalytic decomposition of PAHs [71]. Cellulose used as a carrier provided conditions for the growth of cells of the genus Ruminiclostridium used as BCs and played an additional role of co-substrate [76]. In this case, the cellulose carrier was not only biocompatible but also biodegradable. The presence of a co-substrate or its formation in the workflow can contribute to improving the efficiency of the implementation of hybrid processes. Not only the carrier but also low-molecular-weight substances (acetic or propionic acids formed in the bioreactor or introduced from outside) can also act as co-substrates and electron donors and contribute to the course of photocatalytic reactions [76]. Today, the development of hybrid processes depends on the development of three-dimensional carriers characterized as affordable, high strength, biocompatible, porous and reproducible in characteristics.
It should be noted that the effective use of hybrid processes is influenced by temperature and pH. Currently, a significant part of chemical reactions occurring in the presence of NCs do not require the use of extreme temperatures (Table 1), and this allows them to be considered in combination with BCs (Table 2 and Table 3).
The use of sewage with natural microbial consortia, possessing activity at pH 5.5–7.4 (Table 2), can be considered optimal for simultaneous physical–chemical treatment and biodegradation, which generally corresponds to most modern approaches to the degradation of hydrocarbon pollutants using NCs (Table 1). If necessary, the range of operating pH values can be expanded when using microscopic fungi as BCs [78] and synthetic or adapted consortia [42]. Thus, the use of Aspergillus niger cells in combination with NPs of ZS provides 100% destruction of 100 mg/L venzene, 100 mg/L toluene and 100 mg/L xylene w for 1 h at pH 4 [78]. BCs themselves play an important role in achieving the effective destruction of toxicants in the organization and implementation of hybrid processes [81]. It is possible to increase the activity of BCs by combining different cells and enzymes instead of their individual use [66]. This can also help to increase the stability of their action in the extended pH range. The selection of the BCs most suitable for combination, based on a deep knowledge of their properties, certainly underlies the further development of hybrid systems for purification from hydrocarbon pollutants.

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