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Applied Water Science, Volume 2: Remediation Technologies Inamuddin
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ISBN 978-1-119-72476-6
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1
Miguel A ´ ngel González-Curbelo, Javier González-Sálamo, Diana A. Varela-Martínez and Javier Hernández-Borges
Ashish Kapoor, Elangovan Poonguzhali, Nanditha Dayanandan and Sivaraman Prabhakar
13.4
13.5
13.6
Srivastava
Sharma
18.4
18.6
18.7
18.7.5
18.7.9
18.7.10
18.8 Methods for Qualitative Determination of Water
18.8.1
18.8.2
18.8.3
Charles Oluwaseun Adetunji, Wilson Nwankwo, Olusola Olaleye, Olanrewaju Akinseye, Temitope Popoola and Mohd Imran Ahamed
19.1 Introduction
19.2
19.2.1
19.2.2.1
(TiO2) Nanoparticles
19.2.2.2 Zinc Oxide Nanoparticles (ZnO NPs) 508
19.2.2.3
19.2.3
19.2.4
19.2.5 Modes of Action of These Nanofluids 509
19.2.5.1 Carbon-Based Nano-Adsorbents (CNTs) for Organic Expulsion
19.2.5.2
19.2.5.3
19.2.5.4
19.2.5.5
19.2.5.6 Some Applications of Nanofluids in the Treatment of Water
Preface
Applied Water Science
I-Fundamentals and Applications
Inamuddin1, Mohd Imran Ahamed2, Rajender Boddula3 and Tauseef Ahmad Rangreez4
1Department of Applied Chemistry, Zakir Husain College of Engineering and Technology, Faculty of Engineering and Technology, Aligarh Muslim University, Aligarh, India
2Department of Chemistry, Faculty of Science, Aligarh Muslim University, Aligarh, India
3CAS Key Laboratory of Nanosystem and Hierarchical Fabrication, National Center for Nanoscience and Technology, Beijing, China
4Department of Chemistry, National Institute of Technology, Srinagar, Jammu and Kashmir, India
Water is one of the precious and basic needs of life for all living beings and is a precious national asset. Without it, the existence of life cannot be imagined. Availability of pure water is decreasing day by day, and water scarcity has become a major problem that is faced by our society for the past few years. Hence, it is essential to find and disseminate the key solutions for water quality and scarcity issues. The inaccessibility and poor water quality continue to pose a major threat to human health worldwide. Around billions of people lacking to access drinkable water. The water contains the pathogenic impurities, which are responsible for water-borne diseases. The concept of water quality mainly depends on the chemical, physical, biological, and radiological measurement standards to evaluate the water quality and determine the concentration of all components and then to compare the results of this concentration with the purpose for which this water is
used. Therefore, awareness and a firm grounding in water science are the primary needs of readers, professionals, and researchers working in this research area.
This book explores the basic concepts and applications of water science. It provides an in-depth look at water pollutants’ classification, water recycling, qualitative and quantitative analysis, and efficient wastewater treatment methodologies. It also provides occurrence, human health risk assessment, strategies for removal of radionuclides, and pharmaceuticals in aquatic systems. The book chapters are written by leading researchers throughout the world. This book is an invaluable guide to students, professors, scientists, and R&D industrial specialists working in the field of environmental science, geoscience, water science, physics, and chemistry.
Chapter 1 provides a general overview of different analytical methodologies that have been proposed for the analysis of phthalic acid esters in water samples. Special attention has been given to methods based on the application of sorbent-based microextraction techniques (i.e., solid-phase microextraction and micro solid-phase extraction magnetized or not, among others).
Chapter 2 discusses the occurrence, dissemination, and behavior of pharmaceuticals in aquatic environments. Human exposure pathways and health risks, including the emergence of antimicrobial resistance are summarized. Risk factors promoting human exposure in developing countries are discussed. Methods for removal of pharmaceuticals and future research directions are also highlighted.
Chapter 3 focuses on the latest developments in the methods for the oil/ water separation through filtration of the membrane using distinct materials with surface properties that are super wetting.
Chapter 4 presents the fundamental studies on the interdisciplinary issue of microplastic-based pollution of water environments; the scientific approach and roadmap to this complex problem are discussed.
Chapter 5 summarizes the routes of formation of organic and inorganic chloramines upon chlorination disinfection. Chloramine’s possible health risks to humans including mutagenicity and hemolytic anemia are discussed. Further, the analytical methods for their control in aqueous environments are summarized. Selective methods including chromatographic and pH-controlled colorimetric techniques are highlighted.
Chapter 6 highlights the removal of industrial dyes using different approaches such as clay-based adsorbents, membrane filtration, and chemical treatment with special focus on clay-based low-cost adsorbents. The
results of dyes’ adsorption study are discussed and compared with other reported wastewater treatment technologies.
Chapter 7 provides a general description of biochar material from the preparation (synthetic methods) to its application as a powerful adsorbent in the wastewater treatment field. Recent advancements of biocharsupported materials with a focus on their applications for different contaminants’ removal and the underlying mechanisms are also discussed.
Chapter 8 focuses on biological processes for swine wastewater treatment. Therefore, it details the swine wastewater characteristics, microorganisms, metabolic pathways involved, and biological processes in swine wastewater treatment. Besides, challenges and prospects in this research field are also presented.
Chapter 9 discusses various imperative techniques to detect hazardous metal ions in various water reservoirs. The toxicological effects of various metal ions on living beings and atmosphere along with their detection limits, in addition to future perspectives of these procedures, are highlighted.
Chapter 10 discusses the production of hydrogen-rich water and its role in medical applications. Firstly, a concise discussion of two of the production methods of hydrogen-rich water is provided. Lastly, the medical benefits, medical applications, and the safety of hydrogen-rich water are discussed in detail.
Chapter 11 focuses on the application of hydrosulfide treatment in medicine, agriculture, and industry fields. Hydrosulfide anion is considered as an innovative gaseous signaling molecule and plays significant biological roles in the organisms. Its performance is discussed in detail for the improvement of biotic/abiotic stress tolerance of cells.
Chapter 12 discusses the properties of available radionuclides including uranium, lead, polonium, cesium, strontium, thorium, radon, and radium. Moreover, the health problem caused due to these radionuclides contaminated water is also highlighted. Techniques involved in the removal of radionuclides including ion exchange, aeration, filtration, nanofiltration, and flocculation are summarized.
Chapter 13 reviews the developing applications of membrane contactors in water treatment and desalination demonstrating their ability to substitute or supplement the conventional separation processes. The advantages and limitations of membrane contactors are discussed and their potential for value recovery from spent streams of small and medium industries are highlighted.
Chapter 14 comprehensively reviews all the sulfate remediation technologies and also lists various methods involved in tackling the sulfate
problem from wastewater. Both conventional methods and modern-day technologies are covered in this chapter for sulfate removal.
Chapter 15 discusses the various sources and pathways of heavy metals’ movement and accumulation in the environment. The toxicity effects of these heavy metals on human health are also presented. Various bioindicators and biomarkers generally used for the assessment of heavy metal-based pollution about intake, hazard, toxicity, and transfer factor are discussed. Also, details of various indices associated with health risk, carcinogenic risk, and exposure assessment are focused and recommended.
Chapter 16 emphasizes that the analysis of water is an important multistep process and vital for surveillance and management. The monitoring should be a dynamic procedure with the adoption of techno-economic and state-of-art techniques. We need to improve water quality, minimize pollutants, conserve for the generations, and upgrade awareness levels. Every drop of water counts and has the hidden story of life.
Chapter 17 deals with chemical standards for water quality and explains the philosophy of establishing these standards. In addition to the effect of inorganic substances on water quality, it takes into account the future development of water analysis to make water clean and suitable for human use.
Chapter 18 describes the different approaches used to measure water both quantitatively and qualitatively. The dischargeable and acceptable limits are also tabulated in this chapter as per WHO and BIS guidelines. The simulation equations for estimating the water quality index are presented. Additionally, wastewater treatment techniques are also explained in three stages.
Chapter 19 discusses the application of nanofluids as one of the sustainable bioremediation techniques for the treatment and purification of heavily contaminated water. Different types of nanofluids used in the treatment of water such as zero-valent metal nanoparticles, metal oxides nanoparticles, carbon nanotubes, and nanocomposites are also highlighted.
1
Sorbent-Based Microextraction Techniques for the Analysis of Phthalic Acid Esters in Water Samples
Miguel Ángel González-Curbelo1, Javier González-Sálamo2,3, Diana A. Varela-Martínez1,2 and Javier Hernández-Borges2,3*
1Departamento de Ciencias Básicas, Facultad de Ingeniería, Universidad EAN, Bogotá D.C., Colombia
2Departamento de Química, Unidad Departamental de Química Analítica, Facultad de Ciencias, Universidad de La Laguna (ULL). Avda. Astrofísico Fco. Sánchez, San Cristóbal de La Laguna, España
3Instituto Universitario de Enfermedades Tropicales y Salud Pública de Canarias, Universidad de La Laguna (ULL). Avda. Astrofísico Fco. Sánchez, San Cristóbal de La Laguna, España
Abstract
Current society is living in a world in which it is exposed to a broad spectrum of contaminants that can pose different risks for health. In this sense, we are daily bombarded with news related to pollution by plastic residues (especially in the oceans), being one of the main issues that humans must face today, not only because of the direct effects of plastics but also because of the variety of contaminants they can release to the environment. Probably, the most important ones are phthalic acid esters (PAEs), since they easily migrate from the polymeric matrix to the surrounding media, acting as endocrine disruptors in human organisms and resulting in multiple diseases. Their occurrence in water matrices is of especial importance, since it is essential for life, and the presence of PAEs, even at very low levels, can cause serious health problems. This book chapter aims at providing a general and critical overview of the different analytical methodologies that have been developed for the analysis of PAEs in water samples and which are based on the application of sorbent-based microextraction techniques, which is one of the current trends in the Analytical Chemistry field.
Phthalic acid esters (PAEs) are a group of dialkyl or alkylaryl esters of phthalic acid (see Figure 1.1), commonly known as phthalates, which are widely used as additives in the polymer industry but also added to paints, adhesives, lubricants, and cosmetics, among others [2]. As an example, low-molecular PAEs such as butyl benzyl phthalate (BBP), dibutyl phthalate (DBP), and diethyl phthalate (DEP) are widely used as solvents and emulsifiers to maintain color and fragrance mainly in beauty products and pharmaceuticals, while high-molecular PAEs such as di(2-ethylhexyl) phthalate (DEHP) are highly used as plasticizers to make polymeric materials more workable and flexible. As a result of the extremely high production of such products, especially plastics, PAEs are exorbitantly present in the daily life. Among them, DEHP is the most currently used. In fact, its production as plasticizer is estimated to be a quarter of the total [3, 4]. Due to these widespread applications and intensive production, together with the fact that they are only retained in the polymer structure through weak secondary molecular interactions and not covalently, PAEs can easily migrate to the environment. As a result, PAEs have become ubiquitous contaminants in the environment, in particular, they can be found in natural waters such as lake, river, sea, and ground waters [5, 6], especially those adjacent or downstream from industrial locations [5]. In addition, their possible migration to drinking waters that are in contact with plastic materials like mineral and tap waters must also be taken into account, as well as their final presence in waste waters [5, 7].
It has already been demonstrated that many PAEs act as endocrine disruptors and that they can be toxic for reproduction, even at extremely low concentrations [8–11]. Even more worrying is the fact that certain PAEs can be easily degraded in the environment by bacteria and fungi and their degradation products can also have an important toxicity. Such is the case of DEHP that can be degraded to DBP, DEP, and especially to mono-2-ethylhexyl phthalate (MEHP), which has shown to be more toxic than DEHP [12, 13] (see Figure 1.2). As a result of the high human exposure to PAEs and their metabolites, their potential risks for health and their persistence, several organizations have established an increasingly broad and restrictive legislation. As examples, the European Union has
Name
Dimethyl phthalate
Diethyl phthalate
Di(2-methoxyethyl) phthalate
Dipropyl phthalate
Di(2-ethoxyethyl) phthalate
Benz ylbutyl phthalate
Dibutyl phthalate
Diisobutyl phthalate
Abbreviations
listed several PAEs as compounds suspected to produce endocrine abnormalities [15] and the International Agency for Research on Cancer has classified DEHP in the group 2B (possibly carcinogenic to humans) [16]. Moreover, the US Environmental Protection Agency (EPA) has included several PAEs (BBP, DBP, DEHP, DEP, dimethyl phthalate (DMP), and di-n-octyl phthalate (DNOP)) in its priority list of pollutants and has DMP DEP
DMEP
DPP
DEEP
BBP
DBP
DIBP
Di(2-butoxyethyl) phthalate
Di-n-pentyl phthalate
Diisopentyl phthalate
Dicyclohexyl phthalate
Dihexyl phthalate
DBEP
DNPP
DIPP
DCHP
DHXP
Di(2-ethylhexyl) phthalate
Di-n-octyl phthalate
Diisononyl phthalate
Diisodecyl phthalate
DEHP
DNOP
DINP
DIDP
Figure 1.1 The chemical structures of PAEs. Adapted from [1]. PAEs, phthalic acid esters.
De -esteri cation De -esteri cation
Trans-esteri cation De-esteri cation
Trans-esteri cation
Trans-esteri cation
Trans-esteri cation
Figure 1.2 DEHP biodegradation pathways to obtain MEHP, DBP, and DEP. Reprinted from [14] with permission from Elsevier. DBP, dibutyl phthalate; DEHP, di-2-ethylhexyl phthalate; DEP, diethyl phthalate; MEHP, mono-2-ethylhexyl phthalate; PA, polyacrylate.
established limits of 6 µg/L and 400 µg/L for DEHP and di(2-ethylhexyl) adipate (DEHA) in drinking water, respectively [17], while this maximum allowed concentration has been established in 8 µg/L for DEHP by the World Health Organization [18] and in 1.3 µg/L in surface waters by the European Union [19]. Considering all the above mentioned, it is clear that there is an increasing need to develop highly sensitive and reliable analytical methods for monitoring trace amounts of PAEs in different samples and, especially, in water.
PAEs have been analyzed in water samples using gas chromatography (GC) coupled to flame ionization detectors (FIDs) [20], mass
spectrometry (MS) [21] and tandem MS (MS/MS) [22], or highperformance liquid chromatography (HPLC) coupled to diode array detectors (DADs) [23], ultraviolet (UV) [24], and MS [25]. Among them, GC is normally the preferred technique since most PAEs are nonpolar and thermostable. It is important to notice that, in all these analytical methods, it has been necessary to include previous sample preparation steps before instrumental analysis to achieve accurate and sensitive results. These steps consist on the isolation and pre-concentration of PAEs since they can be found in water samples at extremely low concentrations. However, since PAEs are not ionizable in water, these samples are normally analyzed directly or after a simple filtration without pH adjustment regardless of the sample preparation technique used in each case [26].
In this context, special attention should be paid to the risk of sample contamination during their analysis, which would result in false positives and/or over-estimated concentrations. As it has already been said, PAEs are ubiquitous contaminants and this includes their possible presence in any laboratory since they can be found in solvents, reagents, filters, etc. Consequently, previous washing steps using PAE-free solvents, if possible (since most organic solvents also contain some PAEs), subsequent heating of non-volumetric glassware at high temperatures (450–550°C) for several hours (4–5 h), washing volumetric or any glassware material with strong oxidizing agents, and, in some cases, even wrapping in heat-treated aluminum foil to avoid adsorption of PAEs from the air are carried out, among others [27–29]. Despite all these precautions, residues of PAEs may finally appear, and the analysis of blanks should be developed on a daily basis in every batch of samples so that background levels can be suitably subtracted [21, 25, 30].
Until very recently, the most widely used sample preparation methods, also for the analysis of PAEs in water samples, have been based on the use of liquid-liquid extraction (LLE) and solid-phase extraction (SPE) [31, 32]. The need for developing quicker, simpler, and miniaturized extraction procedures able to maintain or even to improve the required sensitivity of the analysis has resulted in the development of new sample preparation techniques. In this sense, microextraction techniques have gained notoriety since the extraction is carried out using amounts of extracting phase much smaller than the sample amount (extraction of analytes is not always exhaustive). Microextraction techniques have inherent advantages such as exceptionally high enrichment factors, simplicity, time saving, and the generation of small amounts of organic solvent or reagents wastes, without affecting reproducibility, and compatibility with most analytical
instrumentation [33–36]. Among these new alternatives, sorbent-based microextraction techniques have been widely used due to the great diversity of commercially available sorbents, as well as new extraction sorbents (in particular nanomaterials) that are constantly being proposed for their direct use or after a previous functionalization to enhance their selectivity [35–37].
As a result of the above-mentioned issues, the aim of this book chapter is to provide a general overview of the sorbent-based microextraction techniques applied to the analysis of PAEs in water samples, which mainly include solid-phase microextraction (SPME), dispersive SPE (dSPE), and magnetic dSPE (m-dSPE), among others. The extraction ability to quantitatively and selectively extract these target analytes will be commented and discussed.
1.2 Solid-Phase Microextraction
SPME has been the sorbent-based microextraction technique most used for the analysis of PAEs in water samples (see Table 1.1) probably, among other reasons, because it allows to reduce the risk of PAEs contamination during sample extraction with respect to other conventional extraction techniques. On the one hand, the absence of organic solvents and additional steps reduces PAEs background levels. On the other, water is in many occasions a simple and clean matrix that contains few interferences, so the direct immersion (DI) mode can be used without hardly any impairment of its lifetime (except for waste waters or marine water). Moreover, in SPME, extraction, pre-concentration and direct desorption into analytical instruments can be easily integrated in most cases.
The first studies in which SPME was applied for PAEs extraction from water samples dealt with the direct application of commercial fiber coatings, including polydimethylsiloxane (PDMS), polyacrylate (PA), PDMS-divinylbenzene (DVB), carboxen (CAR)-PDMS, and carbowax (CW)-DVB. As examples, Cao [21] demonstrated the better performance of PDMS-DVB fibers compared to PDMS and DVB-CAR-PDMS fibers for the headspace (HS) SPME extraction of nine PAEs (DMP, DEP, DIBP, DBP, BBP, DHXP, DEHA, DEHP, and DNOP) from bottled water samples, while Polo et al. [28] found that PDMS-DVB fibers also give higher extraction efficiency than PDMS, PA, CAR-PDMS, and CW-DVB fibers for DBP, BBP, and DNOP, but CAR-PDMS and PA fibers show a better extraction performance for DMP and DEP, and for DEHP, although the first one provided better results for simultaneous analysis of the target PAEs from bottled,
Reference
Table 1.1 Some examples of the application of SPME and SBSE for the analysis of PAEs in water samples. PAEs
A multifactor categorical design was used for optimization purposes. PDMS-DVB fiber showed higher extraction efficiency than PDMS, PA, CARPDMS and CW-DVB fibers for DBP, BBP, and DNOP, but CARPDMS for DMP and DEP, and PA for DEHP. DI-SPME provided better sensitivity than HS mode [28]
87–110% at 0.5 and 2.5 µg/L One sample of each water were analyzed and contained all PAEs at levels from 0.011 to 6.17 µg/L
0.0067– 0.34 µg/L
Matrix (sample amount)
SPME DMP, DEP, DBP, BBP, DEHP, and DNOP Mineral, river, industrial port, sewage, and waste waters (10 mL) SPME using a PDMS-DVB fiber, stirring at 100°C in DI mode for 20 min, and desorption at 270°C for 5 min GC-MS
