A Recent Advancement on Treatment Technologies for Handling of Pharma Waste water

Narendra Kumar S¹, Muralidhara P L², Lingayya Hiremath¹, Swathi P R²

¹Department of Biotechnology, RVCE, Bengaluru

²Department of Chemical Engineering, RVCE, Bengaluru

*Corresponding Author E-mail: narendraks@rvce.edu.in

ABSTRACT:

The Pharmaceutical Industry produces a wide variety of products in batch or semi-batch processes where the usage of water in many processing equipment plays an important role. The wastewater that is generated from these industries may contain pharmaceutical compounds that are let out in the aquatic environment. The characteristics of pharmaceutical wastewater are clearly mentioned. The wastewater generated in between the processes may contain many chemicals and pharmaceutical compounds that have to be treated. It is very much necessary to analyze the treatment technologies and implement properly, such that the pharmaceutical compounds are disposed of in safe limits. All the various treatments used are presented clearly in this review. Generally, one method employed will not lead to complete removal of contaminants; there must be a combination of the process for efficient removal.

KEYWORDS: Pharmaceutical wastewater, treatment, Characterization, Physico-chemical, BOD, COD, Advanced Oxidation.

INTRODUCTION:

In the past few decades, Industrialisation has played a prominent role in the development of economic growth. This led to a large amount of discharge of waste materials into the water bodies which in turn increased the various kinds of diseases and further led to the production of a wide array of pharmaceuticals in many developing countries. Pharmaceutical industries have contributed a lot to high economic growth and rank third in the world in terms of volume and employment. Along with the processing of pharmaceuticals, there is also a huge amount of disposal of waste into the river, sea and sewage water which has given rise to severe water pollution.

The microbial resistance, chemical persistence, and synergistic effects of the pharmaceuticals which are present at the trace concentrations are still unknown (Madukasi 2010). The awareness of pharmaceutical products in environmental water bodies is reflected in the literature since the 1990s with exponentially increasing studies concerning the presence of water pollutants. There are many treatment methods employed to produce clean water but some chemicals do persist and they are called as “emerging pollutants” (Kummerer 2009). The ultrapure water is only used once in the processing of pharmaceutical products. Due to the strict regulations by Indian pharmacopeia commission, the water cannot be reused in the production of pharmaceuticals. Therefore the residues of these products pose difficulties to the aquatic environment due to their presence and toxic nature.

The analysis, occurrence, and fate of pharmaceuticals in wastewater and treatment are already studied with prominence on their removal efficiency. Not only the industries let out the pharmaceuticals into water bodies, but there are also many sources from which the pharmaceuticals enter into the aquatic environment which is clearly shown in Figure 1.

More than 30 different pharmaceutical substances have been found in several Asian countries in the aquatic environment which include surface waters, groundwater and drinking water in concentrations greater than the detection limit as shown in Figure 2 (Beek 2016). These findings have investigated the presence of pharmaceutical products in the environment and the possible risks they may pose to humans and the environment.

The current review highlights the various treatment technologies that have been used to treat the pharmaceutical wastewater from past few years till now. The majority concern nowadays is regarding the sludge disposal problem, after the treatment of wastewater using various techniques. The extent to widen few outstanding strategies for some of the old problems using green chemistry and waste minimization principles is necessary.

Characteristics of Pharmaceutical Industrial wastewater

The most important step in the selection of treatment method of pharmaceutical industrial wastewater is to characterize the properties of the wastewater. Many researchers have already reported the characteristics of wastewater for physicochemical properties and few of them are clearly mentioned in Table 1. The characteristics of Pharmaceutical Industrial wastewater mainly depend on the raw materials, equipment, and manufacturing process involved in the industry.

Treatment of Pharmaceutical Industrial wastewater

Wastewater generated from pharmaceutical industries varies in many different ways like composition, quantity, season and even time which mainly depend on the raw material and the process that is used in the industry. The quality of available water depends on the location of the industry. The methods employed to treat raw water are involved in the removal of contaminants to a safe level prescribed by the pollution control boards. Hence it is very difficult to specify the type of method applied for the treatment of wastewater. The analysis of the information shows that there are few general approaches to treat pharmaceutical wastewater (Gadipelly 2014). They are as follows: recovery of drugs from wastewater or solvents, Biological treatment, physicochemical treatment, an advanced oxidation process, and hybrid technologies.

Table 1: Physicochemical Characteristics of Pharmaceutical wastewater

Parameters	(Vuppala 2005)	(Saleem 2007)	(Badawy 2009)	(Madukasi 2010)	(Kavitha 2012)	(Gome 2013)	(Imran 2014)	(Arshad 2015)
pH	6.8	6.2-7	8.4±4.5	6.6±0.2	7.81	6.9	6-6.9	7
TSS (mg/l)	686.7	690-930	133.3±171	425±2.3	4300	680	761-1202	-
TDS (mg/l)	1237	600-1300	17251	1600±1.1	2846	1760	1433-3788	-
BOD (mg/l)	620	1300-1800	2650	146±0.3	4132	140	263-330	131
COD (mg/l)	1290	2500-3200	9703	8480±932	7280	540	2565-28640	329
Alkalinity (mg/l)	460	90-180	-	-	-	-	-	-
Oil and grease (mg/l)	16	-	214.9	-	-	-	1925-3964	26
Chlorides (mg/l)	108	-	-	-	1000	-	-	-
Sulphates (mg/l)	-	-	788	-	500	-	-	-

Biological treatment:

Aerobic treatment:

It is the most widely used treatment in many effluent treatment plants. It mainly includes the activated sludge process and membrane bioreactors.

Activated Sludge Process:

The temperature and the microbial species selected always have a prominent role to play in the Activated sludge process. The COD removal in this process was studied between 30-70⁰C at the interval of 5⁰C showed that high temperature were the limiting factors to achieve this removal (Lapara 2001). Some studies also suggested that the normal operating conditions used in the activated sludge process could not successfully remove the pharmaceuticals from the wastewater. The removal efficiencies mainly depend on the removal of the Active Pharmaceutical Ingredients (API) from wastewater. The efficiency of the process also depends on the removal of the compound of interest (Joss 2005). Studies also suggest that removal is very crucial when APIs develop resistance to the process.

Membrane Bioreactors:

These reactors are successful in removal of organics and can replace other methods; they even work under the combination with activated sludge process or hybrid systems. To increase the efficiency of pilot scale studies, the sequential batch reactors and membrane bioreactors have been studied after the activated sludge process (Radjenovic 2007). The main advantage is that they can treat variable compositions of wastewater. For example, a 10m³ per day capacity MBR operated at a pharmaceutical facility in Taiwan, removed 95% of COD and 99% of BOD (Chang 2008). Some APIs are smaller than membrane pores and hence they easily escape into the water bodies. So in order to arrest these compounds, very minute membrane is required, so reverse osmosis or nanofiltration is the only option for their removal.

Anaerobic treatment:

In the present situations, anaerobic fermentation is the most used approach. It has many advantages like low sludge production, few nutrients are needed low energy consumption, no air is required. Up flow anaerobic sludge blanket (UASB) reactor is the most widely used high-rate anaerobic system for domestic and industrial wastewater treatment. For the treatment of diluted pharmaceutical fermentation wastewater, it was found that increasing the Organic Loading Rate (OLR) from 2.7 to 7.2 kg COD/m³/day led to an increase in COD removal from 83% to 91% for continuous operation of 140 days (Chen 2014). UASB is not only used in lab scale, but it is also used as a pre-treatment step in industries. The Up-flow anaerobic batch reactor has been very efficient in the removal of high concentrations of pharmaceutical products from pharmaceutical wastewater. It was found that good COD removal efficiencies 70–75% were obtained at low OLRs (Chelliapan 2014). The combination of Anaerobic Multi-Chambered Bioreactor and Aerobic Stirred Tank Reactor treatment system was effective in removing Oxytetracycline (OTC) from synthetic wastewater with high yields (>95%) at OTC loadings < 177.78 g of OTC/ (m³/day), respectively.

Physico-Chemical Treatments:

These are also known to be the advance treatment methods which are usually required to speed up the removal efficiency of secondary treatment. These include Membrane separation, UV irradiation, and Activated carbon.

Membrane Separation:

Poor fouling and the resistance to chlorine significantly decrease the service life of membrane hindering the application to wastewater treatment. The study revealed that when the feed concentration increases up to 800 ppm, a novel synthesized membranes can still exhibit a high rejection of over 92% (Quan 2015). Few studies suggested that NF was the standard membrane for the removal of pharmaceutical compounds. The work done using the RO membrane was more beneficial for the fermentation process (Zhou 2013). Some studies demonstrate that RO can effectively remove nearly all of the pharmaceuticals (83-99%), in particular, the RO removal mechanisms are emphasized because of their utmost important role in eliminating micro-pollutants (Ng 2011).

UV Irradiation:

Longer irradiation time is needed, if only UV process is used (Claus and Gerhard 1997). The degradation of wastewater by TiO₂ and UV alone is negligible (Jallouli 2015) and that degradation rates can greatly enhance by coupling of TiO₂ with UV (Rubinowska 2013). In some cases, membrane bioreactors are used as a pre-treatment to the process. MBR treatment showed only low degradation capacity for persistent pharmaceuticals (e.g. diurnal removal rate of 25% for diclofenac) promising results were obtained by applying UV irradiation and H₂O₂ (Klepiszewski 2011).

Activated Carbon:

Activated carbon can be used for both natural and synthesized organic contaminants. The adsorption using activated carbon is always an efficient process in separation because it has a high surface area. It was found that both Powdered Activated Carbon (PAC) (5mg/L) and Granular Activated Carbon (GAC) removed greater than 90% of estrogens (Snyder 2007). The performance of PAC can be improved by increasing the retention time. The separation of carbon from the water is the difficulty of using PAC. So the removal or separation of carbon requires sedimentation or membrane filtration. The series of GAC column removed 99% of the total mercury and 90% copper removal pharmaceutical wastewater. The column was also effective in turbidity as well as 96% phenol removal (Goel 2015). Many research studies have taken place as activated carbon to be the pre-treatment step along with the other technologies due to its removal efficiency.

Advanced Oxidation Process:

Ozonation:

Ozonation is mainly employed for the removal of antibiotics. It is a strong oxidizing agent that decomposes to give hydroxyl ions which are strong oxidizers than ozone itself. There are many substances that can resist ozone and hence this method cannot be applied to all the wastewater treatments. Compounds with an activated aromatic ring are susceptible to ozonation, whereas compounds with amide structures are resistant to this process (Shinohara 2007). There will be increased pharmaceutical compound oxidation by increased ozonation levels. Several research results demonstrated that suspended solids have merely a small effect on the oxidation of pharmaceuticals (Huber 2005). It was shown that the COD removal efficiency was increased from 41% to 53% using ozonation along with activated sludge processes (Alaton 2002). This ozone system increases the energy demand over conventional wastewater treatment by 40-50% (Larsen 2004).

Photocatalysis:

Photocatalysis is the acceleration of a photochemical transformation by the action of a catalyst such as TiO₂ or Fenton’s reagent (Deegan 2011). The literature has shown that improvement of removal efficiency by photodecomposition can be done by combining this process with physical and chemical operations. Titania is the most widely investigated of the heterogeneous photocatalyst due to its cost effectiveness, inert nature and photostability (Gaya 2008). This is best process for removal of higher COD and other contaminants to reach biological treatment level. The removal rates of antibiotic are about 98% when it is used along with UV process (Addamo 2005). The research is also done using solar irradiation from economic point of view regarding the treatment of pharmaceuticals from wastewater (Reyes 2006; Żmudzki 2015). The difficulty lies in managing the intermediate and end products obtained by the photocatalytic process.

Electrochemical oxidation:

The anodes made of graphite, Pt, TiO₂, IrO₂, PbO₂, several Ti-based alloys and more recently, boron-doped diamond (BDD) electrodes are generally used for electrochemical oxidation. Electrocoagulation has superior performances in treating effluents containing suspended solids, oil and grease, and even organic or inorganic pollutants that can be flocculated (Chen 2004). With the adequate combination of current density and flow rate, almost 100% total organic carbon removal was observed (Domínguez 2012). The BDD anodes have received growing attention for pollutants oxidation since they exhibit significant chemical and electrochemical stability, good conductivity as well as they achieve increased rates of mineralization with very high current efficiencies (Comninellis 2008). The work has been carried out only in small scale. Implementation of this work to a larger scale will always be in the progress.

Wet air oxidation:

The phenomenon involved in this process is that the improvement in the contact between molecular oxygen and organic matter that has to be oxidized. This process can treat organic toxic waste that can be coupled with any other biological sludge processes. Typical conditions are 200-325⁰C, 50-175 bar and 1 hour for the temperature, pressure and residence time respectively, the COD removal was 90-95% (Debellefontaine 2000). This process was estimated as one of the possible pre-treatment methods for the biological oxidation process because the biodegradability of the sample was increased (Gotvajn 2007). Due to the formation of refractory intermediates like short chain carboxylic acids, the complete oxidation of organic pollutants to CO₂ and water is very tough to achieve.

Ultrasound irradiation:

It is a recent technique that has been followed and has less interest for the wastewater treatment. Very few literatures have been obtained regarding the study of ultrasonic irradiation in the removal of pharmaceuticals from the wastewater. The study has been carried out by the removal of estrogenic compounds from wastewater (Belgiorno 2007; Suri 2007). Pyrolytic reactions inside or near the bubble as well as solution radical chemistry are the two major pathways of sonochemical degradation (Emery 2005). So in the study of literature it is clearly understood that instead of using any one process for adequate removal of contaminants the combination of process are to be used for the proper treatment.

CONCLUSION:

Various treatment systems have been contributed greatly to treat the pharmaceutical compounds present in wastewater. Many more chemicals are added to the existing pharmaceutical compounds for the advanced processes which are introduced recently. Majority of the studies only concentrate on the removal and the disappearance of few parent compounds will not lead to the complete removal of products. The new advancements with high engineered aspects have led to the development of the better wastewater treatment plants in the industries.

The research of pharmaceutical industrial wastewater is more problematic due to the difficulties in accessing the data from industries. So some researchers have either prepared a stock solution or used hospital wastewater for their treatment. There are also a few cases where the original pharmaceutical wastewater has been used for the treatment. The comparison of the treatments is not at all possible due to a difference in the quality of wastewater used. Research should be improvised in order to increase the efficiency of treatment processes.

Based on the molecular size of the particles, membrane separation plays a major role in separation. The combinations and use of hybrid systems are carried out widely and the removal efficiencies are quite higher in these cases. Each treatment process has its own role to play, but the selection of treatment mainly depends on the removal of pharmaceutical compounds present in the water.

The recycling and reuse of the water should be carried out in industry. But unfortunately, only the removal of pharmaceutical compounds is seen everywhere. More research should be done regarding recycling; its efficiency should be very high that water should be used for processing and other purposes. As already mentioned more emphasis is on “removal” rather than recovery. So the research should be based on recovering the valuable products and reuse of those solvents which can be used in the industries. Rather than stating the problem, more interest should be given on the recovery and reuse of pharmaceutical wastewaters.

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Received on 31.05.2019 Modified on 10.06.2019

Research J. Pharm. and Tech. 2020; 13(4):1979-1984.

DOI: 10.5958/0974-360X.2020.00356.X