Biodegradation of pharmaceuticals in photobioreactors – a systematic literature review

Figures & data

Figure 1. PRISMA flow diagram for pharmaceuticals biodegradation in photobioreactors.

Figure 2. Types of micropollutants and their impact on the aquatic environment.

Table 1. Commonly used water treatment methods

Methods	Pharmaceutical Disposal Degree	Advantages	Disadvantages	Influencing factors	References
membrane bioreactor	Ibuprofen up to 99%, Carbamazepine up to 28%, Atenolol up to 96%	a small amount of sludge formed, possibility to modify, removal of high concentrations of pharmaceuticals, wide range of pharmaceuticals	membrane fouling, high cost, energy consumption	membrane type, physicochemical properties of micropollutants, operating condition,	[21]
conventional activated sludge	Ibuprofen up to 99%, Carbamazepine up to 25%, Atenolol up to 64%	cost, simple operation, simplicity in adjusting the parameters of the process	low efficiency in economic conditions, a small range of pharmaceuticals removed, requires a sludge recirculation system	hydrophobicity, properties of antibiotics, sludge properties, temperature, retention time,	[21]
sequencing batch reactor	Chiral pharmaceuticals (Alprenolol, Salbutamol, Norfluoxetine and so on), 48–63% on average	extensive modification possible, high loading rates, high tolerance to toxicity, simplicity in application and design	a low range of pharmaceuticals disposable	properties of antibiotics, HRT, SRT, sediment properties, temperature.	[22]
biological aerated filters system	Sulfamonomethoxine up to 99%, Sulfamethazine up to 23.7%, Amoxicillin up to 50.7%	low cost, energy consumption	susceptible to clogging, requires recirculation	HRT, pharmaceutical concentration	[23,24]
bioelectrochemical system	Ibuprofen up to 96.98%, Cefuroxime up to 100%	properties that stimulate the reaction, low cost, high yield, inhibit the production of toxic by-products, reduction of antibiotic resistance genes	high energy consumption,	electrochemical properties of pharmaceutical, electrodes, carbon source	[25,26]
constructed wetland	Carbamazepine up to 89.23–95.94%, Ibuprofen up to 89.50–94.73%, Sulfadiazine up to 67.20–93.68%	high efficiency, ecological, extensive range of removed compounds	possible use only at low concentrations of pharmaceuticals, depending on weather conditions	the water solubility of antibiotics, plant species, type of wetland, temperature, retention time,	[38]
biodegradation with UV irradiation	Clarithromycin up to 54–99%, Didofenac up to 40–99%, Lidocaine up to 94%	low cost, can be used as a pretreatment step, easy to apply	high cost, limited use only for removal photosensitive compounds, high energy consumption	UV dose, organic matter content, pharmaceutical chemical structure	[27]
biodegradation with ozone oxidation	Ibuprofen up to 95%, Metoprolol up to 60%, Sulfamethoxazole up to 95%	wide range of applications, there are no contraindications in the application	high cost, the difficulty of operations, process management	O3 concentration, pH,	[28]

Table 2. Biodegradation efficiency of pharmaceuticals in a photobioreactor

Component	Initial concentration	Microorganism	Mechanism	Metabolites	Final removal (%)	Observations	References
17α-ethinylestradiol	1 mg/L	Rhodopseudomonas palustris	Biodegradation	estrogen	70%	Efficient biodegradation of ethinylestradiol in a hybrid photoassisted microbial fuel cell with simultaneous production of hydrogen as biofuel	[31]
Alfuzosin Atenolol Atracurium Bisoprolol Bupropion Citalopram Clarithromycine Metoprolol	-	Green algae Dictyosphaerium	Biodegradation	-	64,0 99,0 97,0 97,0 93,0 98,0 90,0 99,0	The analysis showed no relationship between pharmaceutical removal and light intensity reaching the water surface of the algal culture. Light intensity inside the culture had a significant effect on the reduction.	[42]
Amoxicillin	10–150 mg/L	Chlorella sp.	Mainly photodegradation by algae, also self-decomposition and adsorption	-	>99.4%	-	[32]
Carbamazepin Sulfamethoxazole Tramadol	0.2 − 1 mg/L	Chaetoceros muelleri	Biodegradation and bioaccumulation	-	64.8–70.2%	The concentration of pharmaceuticals and personal care products (PPCP) affects the microalgae Chaetoceros muelleri (above 40 mg/L causes a decrease in cell viability, chlorophyll and protein content)	[40]
Carbamazepine Ibuprofen Hydrochlorothiazide Gemfibrozil Bisphenol A	10 mg/L	Periphyton <94% Phormidium	Biodegradation	-	6,0–87,0	Higher hydraulic retention time increased the removal rate. Long exposure time negatively affected the efficiency of the reactor.	[44]
Carbamazepine Diclofenac Ibuprofen Lorazepam Oxazepam Diazepam	665.1 ng/L carbamazepine, 555.9 ng/L diclofenac, 101.4 ng/L ibuprofen, 0.38 ng/L diazepam	microalgae	Biodegradation, adsorption and photodegradation	-	11% carbamazepine, 52% diclofenac, 70% ibuprofen, 83% lorazepam, 71% oxazepam, 94% diazepam	Humic acids and the carbon exudates from the microalgae may increase the photodegradation of diazepam, transparency of the PBR tube material may limit light penetration and the photodegradation rate of photosensitive compounds	[41]
Ciprofloxacin	2 mg/L	Laboratory algal/bacterial culture	Photodegradation	-	84,0		[37]
Diclofenac	25 mg/L	Chlorella sorokiniana, Chlorella vulgaris, Scenedesmus obliquus	-	-	S. obliquus (99%), C. vulgaris (71%), C. sorokiniana (67%)	-	[29]
Diclofenac	25 mg/L	Microalgal Chlorella sorokiniana, Chlorella vulgaris Scenedesmus obliquus,	Biodegradation and adsorption	-	>79,0	The addition of diclofenac resulted in increased biomass growth due to the organic carbon source.	[48]
Diclofenac Ibuprofen Paracetamol Metoprolol Carbamazepine Trimethoprim	147 µg/L 317 µg/L 337 µg/L 181 µg/L 117 µg/L 202 µg/L	Microalgae Chlorella sorokiniana	Biodegradation and photolysis	-	60,0–100,0	Ibuprofen and diclofenac were removed photolytically, metoprolol and paracetamol by a combination of photolysis and biodegradation. No significant effect of contaminant concentration on biomass decline was observed.	[39]
Diclofenac Ibuprofen Carbamazepine	carbamazepine 510 ng/L diclofenac < 200 ng/L ibuprofen < 100 ng/L	Microalgae Pediastrum sp., Chlorella sp., Scenedesmus sp., cyanobacteria Gloeothece sp	Diclofenac, ibuprofen – photodegradation	-	Carbamazepine approx. 15 diclofenac 61 ibuprofen approx. 33	Reduction of biofouling and transparency of the photobioreactor polymer are important	[45]
Ketoprofen Naproxen Ibuprofen Acetaminophen Lorazepam Hydrochlorothiazide Ofloxacin Ciprofloxacin Diltiazem	472 ng/L 2945 ng/L 52091 ng/L 54294 ng/L 3696 ng/L 228 ng/L 65ng/L 2629 ng/L 1678 ng/L	Microalgal of lake water from Pantà de Can Borrell	Biodegradation and/or chemical transformation	-	36,2 10,2 98,5 99,2 57,2 44,3 67,7 47,6 77,3	The efficiency of the process is highly influenced by temperature and solar radiation. A high percentage of removal was obtained for anti-inflammatory drugs (98%).	[36]
Ketoprofen	2 mM	Microalgal Chlorella Spirulina platensis and bacterial consortium	Biodegradation	-	100,0	Chlorella microalgae had significantly higher resistance to ketoprofen concentration. They were found to biodegrade faster under dark conditions.	[47]
Ketoprofen, Paracetamol Aspirin	0,5 mM 0,5 mM 0,5 mM	Microalga Chlorella and bacterial consortium	Biodegradation	-	95,0	The best removal of analgesics was achieved with constant lighting.	[43]
Sulfadiazine Sulfamethazine Sulfamethoxazole	0,12 mg/L sulfadiazine, 0,046 mg/L sulfamethazine, 0,14 mg/L sulfamethoxazole	Chlorella vulgaris	Adsorption, bioaccumulation, and biodegradation	-	more than 30% for the algae batch culture in the flask; between 50–80% for continuous culture in BF-MPBR	Algal biofilms in the reactor reduce the frequency of microalgae collection	[35]
Sulfamethazine Sulfathiazole Sulfamethoxazole	-	Green microalgae Botryococcus braunii	Biodegradation	soluble microbial products and extracellular polymeric substances	38% Sulfamethazine, 53% Sulfathiazole and Sulfamethoxazole	Botryococcus braunii can biodegrade sulfonamides using Submerged Membrane Photobioreactors SMPBR with high efficiency	[34]
Sulfathiazole Trimethoprim Sulfamethoxazole	-	Microalgae	Biodegradation, adsorption and photodegradation	-	60–100%, with the exception of the antibiotics sulfamethoxazole (46%)	Reactor size, specific mixed cultures, temperatures and pH influence the productivity of PBR	[46]
Tetracycline antibiotics	0,25–30 mg/L	Mixed algae	-	-	-	Increased antibiotic concentration negatively affects algal biomass growth and photobioreactor performance. Eukaryotic algae were more sensitive to tetracycline antibiotics than cyanobacterial species.	[33]
β-estradiol	2 mg/l	Consortium (mainly Chlorella and Pseudospongiococcum)	Sorption, biodegradation, photodegradation and volatilization	estrone	55–100	Season of the year and daylight affect the efficiency	[30]

Figure 3. The concept of pharmaceuticals removal in photobioreactors.

Table 3. Types of photobioreactors for the removal of pharmaceuticals

Component	Scale	Photobioreactor type	Photobioreactor volume [dm^3]	pH	T [°C]	Hydraulic retention time (HRT)	References
Tetracycline antibiotics	Laboratory	-	0.8	7.0	23	7 days	[33]
Carbamazepine Ibuprofen Hydrochlorothiazide Gemfibrozil Bisphenol A	Laboratory	Acrylic glass reactor	0.3	7.8	28	22 days	[44]
Carbamazepin Sulfamethoxazole Tramadol	Laboratory	Bubbling column	8	-	25	2.8 days	[40]
Diclofenac	Laboratory	Bubbling column	0.3	7.5	25	80 h	[48]
Diclofenac	Laboratory	Bubbling column	0.25	7.5	25	-	[29]
Ketoprofen	Laboratory	Flask	0.12	7.0	30	10 days	[47]
Diclofenac Ibuprofen Paracetamol Metoprolol Carbamazepine Trimethoprim	Laboratory	Flask	0.5	7.0	35,0	31 days	[40]
β-estradiol	Laboratory	Flask	0.25	-	23–27	-	[30]
Amoxicillin	Laboratory	Flask	0.25	-	25	-	[32]
Ketoprofen, Paracetamol Aspirin	Laboratory	Glass reactor	5	7.0	30	3–4 days	[43]
Ciprofloxacin	Laboratory	Glass reactor		7.0–10.0	20	3 days	[37]
Sulfadiazine Sulfamethazine Sulfamethoxazole	Laboratory	Microalgae biofilm membrane photobioreactor	1	-	26	1–2 days	[35]
β-estradiol	Pilot	Multitubular	1200	6.2–8.7	2.0–17.5	8–12 days	[30]
Antibiotics (9 types)	Pilot	Multitubular	1200	-	-	8–12 days	[4950]
Ketoprofen Naproxen Ibuprofen Acetaminophen Lorazepam Hydrochlorothiazide Ofloxacin Ciprofloxacin Diltiazem	Pilot	Multitubular	1200	7.0–9.0	-	8 days 12 days	[36]
Alfuzosin Atenolol Atracurium Bisoprolol Bupropion Citalopram Clarithromycine Metoprolol	Full-scale	Open photobioreactor	650	8.3	10–32	7 days	[42]
Hydrochlorothiazide, ibuprofen, carbamazepine and gemfibrozil	Laboratory	Periphyton photobioreactor	30	7.8–8.9	28	2–4 days	[44]
17α-ethinylestradiol	Laboratory	Photobioreactor with hybrid photoassisted microbial fuel cell (h-PMFC)	0.50	-	-	16 days	[31]
Diclofenac, carbamazepine	Full-scale	Semi-closed (hybrid) tubular horizontal	8500	7.6–8.9	17.5	16 days	[45]
Sulfathiazole Trimethoprim Sulfamethoxazole	Pilot plant at demonstrative scale	Semi-closed horizontal tubular	3 ∙ 11,700	-	25	5 days	[46]
Carbamazepine Diclofenac Ibuprofen Lorazepam Oxazepam Diazepam	Full-scale	Semi-closed tubular horizontal	2 ∙ 11,700	8–10.5	24–25	5 days	[41]
Sulfamethazine Sulfathiazole Sulfamethoxazole	Laboratory	Submerged membrane photobioreactors	0.8	8.9	30	3–5 days	[34]

Figure 4. Technological barriers associated with different process parameters of pharmaceuticals degradation in photobioreactors.

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