Life Cycle of Polymer NanocompositesMatrices in Hazardous Waste Treatment

R. O. Abdel Rahman, O. A. Abdel Moamen, and E. H. El-Masry

ContentsIntroduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2Hazardous Waste Management . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3PNC Design . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 6PNC Application in Hazardous Waste Management . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 9

PNC Membranes in Hazardous Waste Treatment . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 9PNC Application in Photocatalytic Degradation of Hazardous Contaminants . . . . . . . . . . . . . . 12PNC Application in Sorption of Hazardous Contaminants . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 13PNC Application to Improve Hazardous Waste Immobilization . . . . . . . . . . . . . . . . . . . . . . . . . . . . 17

PNC End of Life Cycle . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 17PNC Thermal Degradation . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 18PNC Ashes Immobilization . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 19

References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 20

AbstractThe strengthened international and national regulatory requirements on hazard-ous contaminants discharge drives the research and development efforts to findand optimize novel materials that could be used effectively in removing thesecontaminants from different waste streams and isolating them from the accessibleenvironment. The evolution of nanosciences and nanotechnologies led to con-siderable improvement in hazardous contaminants separation and degradationtechnologies, where nano-materials (NM) and nanocomposites were proposedfor sorptive removal, catalytic degradation, and disinfections. On the otherside, polymers and polymer composites have been extensively applied inthe management of hazardous wastes in membrane separation, sorption, andimmobilization of radioactive wastes. To improve the performance and stabilityof these materials, hybrid polymer nanocomposites (PNC) were evaluated.

R. O. Abdel Rahman (*) · O. A. Abdel Moamen · E. H. El-MasryHot Laboratory Center, Atomic Energy Authority of Egypt, Cairo, Egypte-mail: alaarehab@yahoo.com; karimrehab1@yahoo.com; roabdelrahman@gmail.com

© Springer Nature Switzerland AG 2019C. M. Hussain, S. Thomas (eds.), Handbook of Polymer and Ceramic Nanotechnology,https://doi.org/10.1007/978-3-030-10614-0_50-1

1

In this chapter, the life cycle of PNC applied in the management of hazardouswastes will be traced. The considered life cycle stages are design and preparation,applications, and management of contaminated PNC (end of life cycle). The mainaim of this work is to summarize the current knowledge in the field by presentingPNC application in membrane separation, photocatalytic degradation, and sorp-tive removal of hazardous contaminants. The gaps in the application of thesematerials in radioactive waste immobilization will be highlighted. Finally the endof life cycle will be addressed by presenting thermal degradation and immobili-zation of PNC and identifying the challenges that associate them.

KeywordsHazardous waste · Radioactive waste · Polymer nano-composite · Sorption ·Membrane · Photo-catalytic degradation · End of life cycle manamgnet · Thermaldegradation · Radioactive waste immobilization · Disposal

Introduction

Environmental pollution problems, which were identified within the last fewdecades, were linked to the increased human activities. These problems arise as aresult of uncontrolled and planned releases of different substances into the environ-ment in a way that prevents natural restorations (Abdel Rahman et al. 2014a, b;Abdel Rahman 2019). Controlling and preventing environmental pollutions isreceiving great attention globally, where growing research efforts were dedicatedto investigate the possibility of developing new materials that could be used tomanage hazardous wastes and remediate contaminated sites (Abdel Rahman 2019).Among these materials, nano-materials (NMs) have been extensively reported topossess distinguished properties due to their large surface area and quantum tunneleffects that promote their efficient applications in contaminants removal eitherwithin the waste management or remediation activities (Abdel Rahman and Michael2017; Abdel Rahman et al. 2019; Hussain and Mishra 2018a, b; Hussain andKharisov 2017).

Polymer nanocomposites (PNCs) integrate the characteristics of both polymersand nano-materials (NMs) (Smith and Yeomans 2009). They were developed toaddress some technical and safety concerns of NMs applications, which includereduced efficiency as a result of particles agglomeration, separation difficulty, lack ofcompatibility assessments with subsequent hazardous wastes immobilization anddisposal activities, potential health risks due to nano-toxicity that associate thehandling of these materials throughout their life cycle, increased health risks duringthe management of exhausted NM, and lack of adequate discharge legislations(Abdel Rahman and Michael 2017; Abdel Rahman et al. 2019). PNCs could beoptimized for certain application by engineering the polymer, NMs, and preparationconditions (Chaurasia et al. 2015). Subsequently, PNCs are available in wide rangeof structures of variable thermomechanical, physicochemical, and radiation resis-tance properties. These features led to considerable progress in their environmentalapplications in gas separation, nano- and ultrafiltration, sorptive removal of

2 R. O. Abdel Rahman et al.

hazardous compounds, UV shielding, and radiation dosimeter and protection.Despite PNCs have successfully addressed the reduction of occupational nano-toxicity health risk, separation, and agglomeration problems, there is a need tohighlight their end of life cycle especially for those applied in the management ofhazardous wastes. In this work, the life cycle of PNCs in hazardous aqueous wastemanagement will be traced starting from preparation, application, and disposal. Inthis context, hazardous waste management will be overviewed including hazardouswaste classification criteria, their sources, and management schemes. PNC engineer-ing will be presented by displaying PNC classification, preparation, and character-ization techniques. PNC application in several hazardous waste treatments includingmembrane separation, photocatalytic degradation, sorptive removal, and wasteimmobilization will be summarized. Finally, the routes for the end of PNC lifecycle will be presented including the thermal degradation and ashes immobilization.

Hazardous Waste Management

Human activities led to inescapable generation of wastes of different physical,chemical, and biological characteristics. These wastes might be classified as hazard-ous or nonhazardous wastes based on their characteristics and the existing regulatoryguidelines. Hazardous characteristics that are frequently considered duringwaste classification include explicability, oxidizing ability, flammability, toxicity,and eco-toxicity, corrosivity, carcinogenicity, infectious, and radioactivity (AbdelRahman and Saleh 2018; Gmbh 2008). Recently, some organizational efforts wereinitiated to update old guidelines and/or issue new guidelines on waste classificationand hazardous waste inventory development (Commission of The EuropeanCommunities Eurostat 2010; Commission notice on technical guidance on theclassification of waste 2018; EPA 2015; Hazardous wastes 2007).

Hazardous wastes generation are noted for several human activities including butnot limited to petroleum and natural gas, mining and ore processing, textile, papersand pulp, electric and electronic devices, metal processing and finishing, leather, andchemical productions, i.e., paints and dyes, pesticides, fertilizers, and pharmaceutics.On the other hand, radioactive wastes are generated as a result of radioisotopeproductions and applications, research and development, and nuclear power gener-ation (Abdel Rahman et al. 2014a; Commission of The European CommunitiesEurostat 2010; Abdel Rahman 2012; Abdel Rahman et al. 2016). Separate class ofradioactive wastes is generated as a result of the mining and ore process activities,which includes naturally occurring radioactive materials (NORM) and technologi-cally enhanced naturally occurring radioactive materials (TENORM) (AbdelRahman et al. 2014a, b). It should be noted that radioactive wastes management isreceiving special attention as it is usually regulated under conventional and nuclearregulatory bodies.

Generally, hazardous wastes management should ensure occupational andenvironmental safety according to international, regional, and national legislativecommitments (Abdel Rahman et al. 2014a, b; Commission of The EuropeanCommunities Eurostat 2010; Abdel Rahman 2012). Historical management schemes

Life Cycle of Polymer Nanocomposites Matrices in Hazardous Waste Treatment 3

rely on direct disposal of these wastes in landfills, deep wells, oceans, and seas orincineration according to available regulation at that time (Hazardous wastes 2007;Spence and Shi 2004; Abdel Rahman et al. 2014c). Figure 1 shows the contributionof each disposal method to the management of organic chemicals within the late1970s–1980s of the last century (Hazardous wastes 2007). Later legislative andregulatory frameworks were updated and modified, and strengthened requirementswere set on the discharge and disposal practices to ensure the protection of theenvironment. Accordingly, the 3R strategy (reduction, reuse, and recycle) wasadopted to ensure better quality for discharge effluents and minimize the disposedwastes volume. Currently, 3R strategy is applied, and conventional waste treatmenttechnologies are used, with strengthened safety requirements, to reduce the volumeof the generated hazardous wastes; then the treatment residues, in the form of sludge,exhausted resins, ashes, etc., are immobilized and disposed in engineered facility.For aqueous wastes, solvent extraction, chemical precipitation and coagulation,evaporation, ion exchange and sorption, advanced oxidation and reduction, andmembrane separation are usually used, whereas incineration, emulsification,and absorption are used to treat organic wastes (Commission of The EuropeanCommunities Eurostat 2010; Abdel Rahman et al. 2014c). The residues that resultfrom these treatment processes should be immobilized in a suitable form that ensurestheir stabilization and solidification (Spence and Shi 2004; Abdel Rahman et al.2014c). Immobilization is a main activity in the management of radioactive wastesas it is recommended internationally and regulated nationally (Abdel Rahman et al.2014a, c; Abdel Rahman 2012). For hazardous wastes, US EPA suggested the use ofimmobilization (solidification and stabilization) technology for hazardous sludgesthat contain inorganic contaminants. For hazardous waste sludges or distillationbottoms that contain organic and inorganic contaminants, thermal treatmentwas recommended followed by ashes immobilization, a list of EPA-recommended

Landfill Controlled Incineration

Un-Controlled

Incineration

Deep well Disposal

Biological treatment

Recovery

USA

Landfill

Incineration

Others

Ocean dumping

UK

Fig. 1 Contribution of the historical management option to the treatment of organic chemicalsduring 1970–1980s in (a) USA and (b) UK. (Adapted from (Hazardous wastes 2007))

4 R. O. Abdel Rahman et al.

Table 1 Summary of the best demonstrated technology to manage different types of hazardouswastes

Technology Waste

Thermal treatment or immobilization Thallium compounds including (acetate,carbonate, chloride, thallic oxide, sulfate, andnitrates)

Immobilization Ignitable, corrosives, reactive sulfides, Ba, Cd,Cr, Pb (including Pb(C2H3O2)2, Pb3(PO4)2,Pb3(C2H5O4)2, Hg(<260 mg/kg), Ag, Se(including H2SeO3, SeS2)Sludges from wastewater treatment of:(a) Al coating except for some zirconium

phosphating processes(b) Anhydrous or hydrated chromium oxide

green pigments productionEmission control dust/sludge from:(a) Primary steel production in electric

furnaces (<15% Zn)(b) Secondary lead smelting

Heavy ends from the production oftoluenediamine via hydrogenation ofdinitrotoluene

Incineration and immobilization Wastes generated from petroleum industryincluding(a) Leaded tank bottoms(b) Dissolved air flotation (DAF) float from(c) Slop oil emulsion solids(d) Heat exchanger bundle cleaning sludges(e) API separator sludges(f) Still bottom from distillation of benzyl

chloride(g) Distillation bottom from phenol/acetone

production from cumene and Aniline production(h) Spent catalyst from the hydrochlorinator

reactor in the production of 1,1,1-trichloroethane(i) Process wastes from certain chlorinated

aliphatic hydrocarbons(j) Decanter tank tar sludge from coking

operation(k) Creosote

Precipitation and immobilization Waste generated from the treatment of emissioncontrol dust/sludge from secondary leadproduction using acid leaching

Alkaline chlorination, precipitation, andimmobilization

Spent cyanide plating bath solutions, platingsludges from cyanide process, spent stripping,and cleaning solutions from cyanide processes

Combined electrolytic oxidation + alkalinechlorination + precipitation + immobilization

Cyanide processing including spent cyanidesolutions from salt bath cleaning, quenchingwastewater treatment sludges, and nickelcyanideArgenate (1-), bis(cyano-C)-potassium

Life Cycle of Polymer Nanocomposites Matrices in Hazardous Waste Treatment 5

technology to manage different hazardous wastes is provided in Table 1 (Spence andShi 2004; EPA).

Research efforts in hazardous waste management could be divided into twoclasses: the first aims at enhancing the performance and costs of conventionaltechnologies and reducing their negative environmental impact, and the second isdirected to getting innovative technologies into industrial-scale applications (AbdelRahman 2016). Among these researches, a great attention was paid to NM and PNCapplication in hazardous waste management, where these materials were tested fortheir potential use in treatment and remediation activities (Abdel Rahman et al.2014b; Abdel Rahman and Michael 2017; Hussain and Mishra 2018a, b; Hussainand Kharisov 2017; Smith and Yeomans 2009; Abdel Rahman 2016; Abdel Rahmanet al. 2011). Within this context, NMs of different structural configurations weretested to remove hazardous metal ions by photocatalytic effect or sorption withspecial attention to the separation difficulties and reducing particles agglomeration;these materials include zeolites, silica, carbonaceous materials, metal oxides, andzero-valent elements. The studies of these materials extended from the treatment ofwastewater to its application in in-situ and ex-situ remediation activities.

PNC Design

PNC is classified based on the structure and dispersion of NM (polymers, clay, andmetallic nanoparticles) in the polymeric matrix, where NM structures of three, two,and one dimension in the form of particles, sheets and flakes, and fibers, respectively,could be used (Fig. 2). On the other hand, NMs dispersion (morphology) is catego-rized into three types as follows:

(i) Exfoliated dispersion: uniform NMs dispersion is achieved as a result ofextensive polymer penetration into the layer structure of the nanoparticles.

(ii) Intercalated dispersion: several polymer chains are incorporated into NMlayers or tubes so that a well-ordered multilayer with alternating polymerchain and NM layers are repeated within few nanometers.

(iii) Immiscible dispersion: no polymer penetration into the layer structure couldbe achieved, so phase separation occurs (micro-composite).

NMs dispersion in PNC could be determined by balancing the factors that affectthe total energy and entropy of the PNC system, where the high surface area of NMsfavors their agglomeration with strong attractive forces and imposes entropic pen-alties on the penetrated polymer molecules (Manias et al. 2006; Ginzburg et al. 2009;Vaia and Giannelis 1997). These entropic penalties arose from the interfacial tensionand polarity of the system components and could be compensated by the presence ofsurfactant (Manias et al. 2006; Vaia and Giannelis 1997). Subsequently, duringmixing, the energy of PNC system could be described as an additive function ofthe polar and apolar interaction energies between NM layers and the penetratedpolymer (Manias et al. 2006). Figure 3 illustrates the relation between the polymer

6 R. O. Abdel Rahman et al.

free energy per unit area of NM layers (F) and separation distance between the layers(d). A monotonically decreasing relation will favor exfoliated dispersion, whereasmonotonically increasing relation will favor immiscible. Intercalation dispersionwas reported for curves that have a minimum at finite separation (Manias et al.2006; Ginzburg et al. 2009; Vaia and Giannelis 1997).

There are different available procedures that could be used to prepare PNCs;achieving efficient PNC necessitates the selection of the most suitable preparationtechnique to achieve the required performance. Generally, PNC could be prepared byin-situ synthesis or by dispersing NM in the polymeric matrix. In this respect, thepreparation processes could be classified as in-situ, intercalation, direct mixing, andex-situ based methods. Table 2 summarizes the features of the methods that could beapplied to prepare intercalated and exfoliated PNCs. The use of melt techniques,

Fig. 2 PNC classification based on nano-materials dimension

Fig. 3 Nano-materialsdispersion in PNC as afunction of the polymer-freeenergy and the distancebetween NM layers. (Adaptedfrom (Ginzburg et al. 2009))

Life Cycle of Polymer Nanocomposites Matrices in Hazardous Waste Treatment 7

Table

2Preparatio

nprocedures

features

forthesynthesisof

intercalated

andexfoliatedPNC

Procedu

res

Metho

dAdv

antages

Disadvantages

Large

scale

application

In-situ

Precursorsof

NM

andpo

lymer

aremixed

Gas-phase

(phy

sicalin

situ)or

liquid-ph

ase

(chemicalin

situ)metho

dscouldbe

used

Usedforthermo-setand–p

lastic-

basedPNC

Con

trolledparticlesize

Highshearmixingisrequ

ired

toprevent

NM

agglom

eration.

Solvent

elim

inationisaconcern

Lim

ited

application

Intercalation

Solution

intercalation

NM

aresw

ollenanddiffused

insolvent,then

thepo

lymer

orpo

lymer

precursorsisadded

anddissolvedin

thesolvent,andfinally

the

solventiselim

inated

Fastandun

iform

dispersion

ofNMs

App

liedforpo

lymerswith

lowor

even

nopo

larity

Requireslargesolventquantitythat

affecttheenvironm

entalim

pactand

econ

omyof

theprocess

Optim

izationrequ

ired

foreverysystem

,i.e.,po

lymer/NM/solvent

Lim

ited

application

Melt

intercalation

Mixture

ofmoltenpo

lymer

andNM

isannealed

Env

iron

mentally

friend

lyandsimpler

Com

patib

lewith

thepo

lymer

indu

strialprocess,i.e.,extrusionand

injectionmolding

Defecttowardpo

lyolefins

Maintaining

delaminated

PNC

morph

olog

yisun

certainatlow

temperature

App

licable

Melt

blending

Polym

erismeltand

then

NMsareaddedand

mixed

athigh

temperature

athigh

shearing

rate

Econo

micalandenvironm

entally

friend

lyUse

ofspecialmixers

The

high

shearcandamageNM

andthe

polymer

App

licable

Mixing

Solvent

mixing

MixingNMsandpo

lymer

inthepresence

ofsolvent

Goo

ddispersion

requ

ires

loweringthe

polymer

viscosity

coup

ledwith

applying

mechanicalagitatio

nor

sanitatio

n

Requireslargesolventquantitythat

affecttheenvironm

entalim

pactand

econ

omyof

theprocess

Not

applicable

Meltm

ixing

NMsandthepo

lymer

mixture

isheated

and

mixed

tillachieving

aho

mog

eneous

material

Econo

micalandenvironm

entally

friend

lyNM

mod

ificatio

ncouldbe

affected

App

licable

Ex-situ

NM

isdispersedin

polymer

solutio

nor

melt

Widevariability

indesign

and

optim

izationof

PNC

Hom

ogenou

sdispersion

isdifficultto

achieve

App

licable

8 R. O. Abdel Rahman et al.

Table 3 Features of characterization techniques for PNC applications

Uses Technique Limitations

Detection of impurity in organic phases;identification of the structure byidentifying the function groups;identification of interactionmechanisms

UV Poor resolution and provides limitedinformation for some compounds, i.e.,Ag/PNC

FTIR Small signal-to-noise ratio which canaffect oxidation identification of PNC-nano tubes oxidized by Hummer’stechnique

XPS Considerable errors associateheterogeneous surfaces analysisCan lead to degradation of PNC-basedmembraneApplied for dry samples

EDX Some samples are exposed to beamdamage, which requires the utility of alow current

Identification of crystalline structure,crystallinity degree, crystal size, andphase orientation

WAXD Peak broadening at small crystal sizeslimits its applicability to characterizelayered NM and exfoliated PNCs

SAXS Applied for materials in the range of30–50 nm

UAXS Applied for materials in the range of15 nm–2 μm

Study of the particle size; morphologyexamination; identification of NMdispersion state; visual examination ofphase distribution and surface topology(SPM, STM, AFM only);Determination of surface elasticity,magnetic characteristics, specificmolecular interactions of the surface,and frictional characteristics (AFMonly)

SEM, Applicable in the range 100 μm–10 nmand limited to conductive dry samples

TEM Applicable in the range of 10 μm–1 nm,and the thickness is limited to 200 nmRequires special preparationIf not will optimized, can cause damageto the sample by the incident electronbeam, i.e., in case of poly crystallinePNC

SPM &STM

Applicable in the range of100 μm–10 nm and limited toconductive materialsIt requires minimization of allmechanical and electrical noises

AFM Scanning speed is limited and can leadto thermal driftAFM images may be influenced by thepiezoelectric material, where the roughspecimens with steep walls can inducehysteresis

(continued)

Life Cycle of Polymer Nanocomposites Matrices in Hazardous Waste Treatment 9

Table 3 (continued)

Uses Technique Limitations

Evaluation of thermodynamicparameters, i.e., specific heat capacity,glass transition temperature, changes inenthalpy, and cure relaxationEvaluation of degradation and thermalstabilityMeasurement of storage and lossmodulus (DMA only)

DSC, Data interpretation is quite complexthan other thermal technique

DTA, Reaction or transition estimations isonly 20–50% DTA

TGA, Overlapping weight losses may occursuch as several peaks or shoulders

DMA The obtained data are affected stronglyby the sample dimensions, scale, andthe degree of NMs dispersion

Specific surface area, Porosity porevolume

BET It necessitates low experimentaltemperatures to avoid structure changeof the specimen, and the sample must bedry powderThis technique needs a lot of time foradsorption of gas molecules to occur

Fig. 4 PNC characterization techniques

10 R. O. Abdel Rahman et al.

either intercalated mixing, melt blend, or direct mixing, can affect the surfacemodification of the NM and in some cases PNC morphology, whereas the use ofthe solvent methods, intercalated or direct mixing, requires large amount ofsolvents which is environmentally unfavorable. Currently, research areas in thisfield investigate the use of natural sources, nonhazardous solvents, and energy-efficient processes in the preparation of PNC such as polylactic acid (PLA)-and biopolyester-based green composites, etc. to address this point. A variety oftechniques are available to characterize PNC to enable the researchers to understandthe basic chemical and physical characteristics of the prepared materials. Figure 3and Table 3 illustrate these techniques and list their limitations for PNC character-izations (Fig. 4) (Abdel Rahman and Michael 2017).

PNC Application in Hazardous Waste Management

PNC Membranes in Hazardous Waste Treatment

Membrane separation is a physicochemical process that depends on the presenceof a barrier that permits selective transport of some molecules, ions, or particlesunder certain driving force, i.e., pressure, concentration, and potential differences.Fig. 5 summarizes the features of pressure-driven membrane separation processes,i.e., microfiltration (MF), ultrafiltration (UF), nanofiltration (NF), forward osmo-sis (FO), and reverse osmosis (RO). Polymeric membranes are widely applied inthese processes of different modules including tubular, spiral wound, and plateand frame. Despite their lower hydrophilicity, surface charge, and mechanical,thermal, and chemical stability compared by ceramic membrane, they are widelyapplied in water and wastewater treatment (Wagner 2000; Ursino et al. 2018;Kausar 2018). The main drawback of polymeric membranes is there irreversiblefouling that leads to loss of permeability, increased energy consumption, and shortoperating life (Kausar 2018). PNC was tested to address this drawback, wherephotocatalytic materials are used as NMs (Ag, carbon nanotubes (CNT),graphene, TiO2, ZnO) to improve biofouling resistance (Gehrke et al. 2015; Nget al. 2013). Different polymeric matrices were tested including polyvinylidenefluoride (PVDF), polysulfone (PSF), polyethersulfone (PES), polyamide (PI),polyvinyl alcohol (PVA), and poly(methyl methacrylate) (PMMA) (Liang et al.2012; Zhang et al. 2012, 2014, 2016; Hong and He 2012; Pintilie et al. 2017; Shahand Murthy 2013; Bahadar et al. 2015; Shen et al. 2013; Isawi et al. 2016; Aminiet al. 2016; Zhao et al. 2017). Some reported studies indicated that the use ofAl2O3, TiO2, and graphene can enhance the hydraulic, mechanical, and thermalproperties of the membrane (Abdel Rahman et al. 2011, 2014c; EPA; AbdelRahman 2016; Manias et al. 2006; Ginzburg et al. 2009; Vaia and Giannelis1997; Wagner 2000; Ursino et al. 2018; Kausar 2018; Gehrke et al. 2015; Ng etal. 2013; Amini et al. 2016). Table 4 summarizes some recent studies on PNCapplication as MF, UF, NF, FO, and RO (Liang et al. 2012; Zhang et al. 2014;Hong and He 2012; Pintilie et al. 2017; Zhang et al. 2012, 2016; Shah and Murthy

Life Cycle of Polymer Nanocomposites Matrices in Hazardous Waste Treatment 11

2013; Bahadar et al. 2015; Shen et al. 2013; Isawi et al. 2016; Amini et al. 2016;Zhao et al. 2017). The phase inversion method produces heterogeneous membranemorphology of porous support and the active layer, whereas the sol-gel methodproduces homogenous membrane morphology by control pore size distributionand volume fraction (Nishihora et al. 2019; Fard et al. 2018). PNC membranedesign should consider the effect of the amount of NM incorporated in thepolymer, where reported study indicated that the use of Ag can reduce the voidvolume and subsequently the permeability. Nano-Zr, Mg, and Al were proposed toincrease the permeate flux, but careful consideration should be given to theretention performance.

Natural PNC membranes are environmentally friendly during their productionand at the end of their life cycle. The development of natural PNC membrane is stillslow, where limited studies are available on the use of protein-based membrane(Hoek et al. 2017). Alginate CNT is receiving a considerable attention; alginate-aligned CNT have exceptional transport characteristics and gating potential. Thepreparation of this material with <0.01% pore having 10 Å diameter could granteegood performance of the thin film RO membranes. This material is challenged by thedifficulty of scaling up the preparation process, low chemical stability in acidic

Fig. 5 Features of different membrane processes

12 R. O. Abdel Rahman et al.

Table 4 Application of PNC to improve membrane performance in separating differentcontaminants

Process PNCPreparationmethod Application Features Ref.

MF PVDF/ZnO

Nonsolvent-induced phaseseparation(NIPS)

Sodiumalginate, humicacid, BSA,NaN3, CaCl2,MgCl2.NaHCO3,NaCl

Enhancedhydrophilicity,mechanical strength,and anti-irreversiblefouling

(Liang etal. 2012)

Phaseinversionprocess

Cu removalBSA

Enhancedhydrophilicity,permeability, andantifouling ability

(Zhang etal. 2014)

Phaseinversionmethod

COD removal Enhancedhydrophilicity andlowest roughness

(Hongand He2012)

UF PSF/ZnO Phaseinversionmethod

N/A Enhancedhydrophilicity, flux,permeability,retention, andporosity.

(Pintilieet al.2017)

PES/AgNO3

Phaseinversionmethod

Biofoulingresistance, E.coli and P.aeruginosa

Increase inhydrophilicity andpermeate flux;exhibited excellentantibacterial activity

(Zhang etal. 2012)

NF PSF/CNT Phaseinversionmethod

Cr(VI), Cd(II)removal

Enhanced thermalstability,hydrophilicity, andadsorptive nature

(ShahandMurthy2013)

Celluloseacetate/ZnO

Sol–gel Zn2+, Cd2+,Pb2+, Mn2+,Ni2+, Fe2+, Al3+, Sb3+, Sr3+

Removal

Increases inantibacterial activity,high permeability,high selectivitytoward Fe ions

(Bahadaret al.2015)

(PI/PVA)/AgNPs

In situpreparation

Biofoulingresistance andNa2SO4

removal

Enhanced saltrejection,hydrophilicity, andbiofouling resistance

(Zhang etal. 2016)

PMMA/CNT

Graftingpolymerization

NaCl, Na2SO4

removalIncrease inhydrophobicity,improve selectivity,and permeability

(Shen etal. 2013)

RO PI/ZnO Free radicalgraftpolymerization

Mono- andbivalent ionsremoval andbiofouling

Enhances the tensilestrength, elongationbreak, and Young’smodulus values.Better antibacterial

(Isawi etal. 2016)

(continued)

Life Cycle of Polymer Nanocomposites Matrices in Hazardous Waste Treatment 13

media, short-term chemical stability in water, and short-term fouling resistance(Hoek et al. 2017).

PNC Application in Photocatalytic Degradation of HazardousContaminants

NMs have great potential as catalysts and redox active media due to their largespecific surface area, high reactivity and shape-dependent optical, and electronic andcatalytic property, which have attracted many researchers to design highly efficientphoto-/chem-catalytic materials for purification of contaminated waters and gases.Common catalytic NM includes semiconductors, i.e., TiO2, ZnO, CdS, and WO3;zero-valence metal, i.e., Fe0, Cu0, and Zn0; and bimetallic nanoparticles, i.e., Fe/Pd,Fe/Ni, Fe/Al, and Zn/Pd. They usually serve as catalysts or redox reagents fordegradation of a large variety of hazardous contaminants such as polychlorinatedbiphenyls, azo dyes, halogenated aliphatics, and organochlorine pesticides.PNCs are studied for their potential to reduce separation problems associated ofthe application of these NMs. Table 5 comprises several polymer-based nano-composites (PNCs) for degradation of pollutants (Iketania et al. 2003; Ameen etal. 2011; Zhu et al. 2009; Xu et al. 2010; Wang et al. 2010; Ponder et al. 2000; Donget al. 2010; Wu and Ritchie 2006; Lin et al. 2009).

PNC Application in Sorption of Hazardous Contaminants

Adsorption techniques are widely used in wastewater treatment and gas purificationas one of the most effective and simplest approaches to remove hazardous contam-inants. PNC design is based on the use of conventional polymers, i.e., porous resinsand ion exchangers, and biopolymer, i.e., alginate and cellulose, is under investiga-tion (Guo and Chen 2005; Zouboulis and Katsoyiannis 2002; Blaney et al. 2007; Panet al. 2007a, b, 2008; Zhang et al. 2008). Conventional polymeric sorbents or ionexchangers proved their efficiency to produce PNC with excellent mechanicalstrength and adjustable surface chemistry. Currently, the use of magnetic NM in

Table 4 (continued)

Process PNCPreparationmethod Application Features Ref.

resistance andhydrophobicity

FO PSF/TiO2

Phaseinversionmethod

NaCl Improved separationproperties andhydrophobicity

(Amini etal. 2016)

FO PVDF/ZnO

Nips. Desalinationand watertreatment

Increases theseparation water flux

(Zhao etal. 2017)

14 R. O. Abdel Rahman et al.

the preparation of PNC sorbent is promising, where their use allows easy separationof the PNC beads under the effect of magnetic field. These materials allow the designof efficient removal processes with easily separation and regeneration. Magnetite(Fe3O4), maghemite (Fe2O3), and jacobsite (MnFe2O4) NM were proposed in thisaspect to be loaded in/on the polymeric matrix, i.e., alginate beads. A series ofmagnetic alginate polymers were prepared, and batch experiments were conductedto investigate their ability to remove heavy metal ions (Ngomsik et al. 2005; Liu etal. 2009; Rocher et al. 2008) (Co(II), Cr(VI), Ni(II), Pb(II), Cu(II), Mn(II), La(III))and organic dyes (Rocher et al. 2008) (methylene blue and methyl orange) fromaqueous solutions.

Nano-Prussian blue (PB) polymer and cyano-bridge coordination polymer, eithercoated on or intercalated in magnetite, were studied for the removal of cesium as oneof the major contaminants in radioactive wastewaters (Abdel Rahman and Michael2017; Jang and Lee 2016). These materials show distinguished performance inremoving cesium due to small hydrated radius of cerium that allows its entrapmentin transition metal hexacyanoferrate (THM) channels and the presence of hydro-philic defect sites on the PB nanoparticles (Jang and Lee 2016; Gasser et al. 2016).

Table 5 PNCs applications in photocatalytic degradation of hazardous pollutants

NM type PNC type used Preparation Contaminants Ref.

Semiconductor Poly(dimethylsiloxane)(PDMS)–TiO2

Sol–gel Methylene blue andacetaldehyde in120 min

(Iketaniaet al.2003)

Poly(1-naphthylamine)(PNA)–TiO2

In-situ Methylene blue dye,in 160 min

(Ameenet al.2011)

Chitosan–CdS Simulatingbiomineralization

Congo Red at pH 6in 180 min

(Zhu etal. 2009)

Zero valence Poly(vinylpyrrolidone)(PVP)–Fe

Electrospinning Degradation ofbromate, in 20 min

(Xu et al.2010)

Carboxymethylcellulose–Fe

In-situ synthesis Cr (VI), pH 5.5 in60 min

(Wang etal. 2010)

Resin–Fe In-situ synthesis Cr(VI) and Pb(II),pH 2.67 and 2.92 in60 days

(Ponderet al.2000)

Bimetallic Sodiumcarboxymethylcellulose-Fe/Pd

In-situ synthesis Para-nitrochlorobenzene,pH 5.5 in 120 min

(Dong etal. 2010)

Celluloseacetate–Ni/Fe

Solvent cast Degradation oftrichloroethylene,pH 6.5–7 in120–150 min

(Wu andRitchie2006)

Resin–Pd/Sn In-situ Degradation oftrichloroethylene,pH 7.1–7.3 in 2 days

(Lin et al.2009)

Life Cycle of Polymer Nanocomposites Matrices in Hazardous Waste Treatment 15

Table 6 summarizes some typical application of PNCs as sorbent for the removalhazardous contaminants (Guo and Chen 2005; Zouboulis and Katsoyiannis 2002;Blaney et al. 2007; Pan et al. 2007a, b, 2008; Zhang et al. 2008; Jang and Lee 2016;Rule et al. 2014).

PNC Application to Improve Hazardous Waste Immobilization

Hazardous wastes immobilization aims to improve the mechanical performance(solidification) and the containment performance (stabilization) of the waste byentrapping/retaining them in a suitable matrix (Abdel Rahman and Michael 2017;Spence and Shi 2004; Abdel Rahman et al. 2014c; Abdel Rahman and Ojovan 2016;

Table 6 Polymer-based nanocomposites (PNCs) for sorption of hazardous pollutants

PNC type usedSynthesisprotocol Materials removed Ref.

Cellulose–ironoxyhydroxide

In-situ synthesis Sorption capacities are 99.6 and33.2 mg/g for As(III) and As(V),pH 7 in 24 h

(Guo andChen 2005)

Alginate–iron oxides Combinedalginate dopingand coating withoxide

Arsenic removed from 50 to<10 ppb within 230 BV for As(V), 45 BV for As(III), pH 5 in24 h

(ZouboulisandKatsoyiannis2002)

IRA–hydrated ferricoxide

Oxidizing anion– ferrous sulfatesolution on resin

P(V) removed from 100 to<5 ppb within 10,000 BV, pH 5–7in 4–5 days

(Blaney et al.2007)

Polymeric cationexchanger–hydratedferric oxide

Precipitation ofiron(III)hydroxides fromFeCl3

Removal of Pb(II), Cu(II), Cd(II);metal ions removal from 1 ppm to<5 ppb within 7000 BV, pH 5 in100 min

(Pan et al.2007a)

Polymeric cationexchanger–hydrousmanganese oxide

Oxidation of thepreloaded Mn(II)

Removal of Pb(II), Cd(II), Zn(II);Kd increased by 20–800 times ascompared to host exchangers,sorption capacities increased by50–300%, pH 6–8

(Pan et al.2008)

Polymeric cationexchanger–Zr(HPO3S)2

In-situ Removal of Pb(II), Cd(II), Zn(II);Pb(II) removed from 50–130 to<10 ppb within 50,000 BV, Cd(II)removed from 80–140 to <3 ppbwithin 9000 BV BV, pH 4–6 in24 h

(Zhang et al.2008)

Polymeric cationexchanger–Zr(HPO4)2

In-situ Pb(II) removed from 40 to<0.05 mg/L within 2000 BV BV,pH 3–6 and 24 h

(Pan et al.2007b)

Nano-Prussian blue(PB)–Fe3O4

Ex-situ Cs removed at pH 10 sorptioncapacity280.82 mg/g

(Jang andLee 2016)

Cellulosebeads–Fe3O4

Ex-situ U removal at pH 7 sorptioncapacity 7.6 mg/g in 150 min

(Rule et al.2014)

16 R. O. Abdel Rahman et al.

Abdel Rahman and Zaki 2009). Different matrices are being applied to immobilizethe hazardous wastes, i.e., cement, polymers, bitumen, ceramic, and glasses.Research efforts in this field aim at improving the mechanical and containmentperformances of these matrices (Abdel Rahman et al. 2014a, c, 2019; Abdel Rahmanand Michael 2017; Spence and Shi 2004; EPA; Abdel Rahman 2016; Abdel Rahmanand Ojovan 2016; Abdel Rahman and Zaki 2009). Generally, NMs were tested toimprove the mechanical performance of cement-based materials and chemicallybonded phosphate ceramic, but there is no research on the effect of these materialsor PNC on the immobilization of hazardous materials (Abdel Rahman and Michael2017; Colorado et al. 2011).

Radioactive waste immobilization in polymeric matrix has been practicedwidely for several decades; this immobilization route was challenged by thereduced radiation stability and relatively high cost (Abdel Rahman et al. 2014c).Conventionally, epoxy, polyesters, polyethylene, polystyrene and copolymers, ureaformaldehyde, polyurethane, phenol-formaldehyde, and polystyrene are applied toimmobilize low- and intermediate-level radioactive wastes. PNC was reported tohave improved radiation stability properties due to the large volume fraction grainboundaries of the NM that act as effective sinks for radiation-induced defects(Nambiar et al. 2013). This effect led to the investigation of the effect of heavymetal nanoparticle on the shielding performance of PNC (Nambiar et al. 2013;Hashim and Hadi 2017). Studies on the feasibility of using NM to improve thetraditional radioactive waste polymerization were not investigated.

PNC End of Life Cycle

In general, the end of PNC life cycle is a challenge, where their recycling is verylimited to specific channels and they have to be disposed of. Recent studies referredto thermal decomposition as the main end of life cycle for these materials followedby ashes disposal in engineered landfill (Sotiriou et al. 2015, 2016; Adam andNowack 2017; Pourchez et al. 2018; Abdel Rahman 2010). An alternative end oflife cycle route was proposed for bio-polymeric PNC and includes biodegradationfollowed by disposal of the sludge in engineered landfill. An estimate of the globallife emission of engineered NM during their life cycle indicated that 63–91% ofthese materials are routed to engineered landfills; emissions to soil and water wereconcluded to represent about 25 and 7% of the material flow where air emission waslimited to 1.5% (Keller et al. 2013). Figure 6 illustrated the contribution of fivemetallic NM to the estimated global life emissions (Keller et al. 2013). NM releasemechanisms from PNC, applied in different industrial applications, during theirproduction and storage stages were identified to include passive diffusion, desorp-tion, and dissolution into external liquid media, but the release and post-releaseanalysis of the integrated life cycle was not addressed (Duncan and Pillai 2015).Specific studies on the life cycle of PNC applied in hazardous waste managementwere not conducted.

Life Cycle of Polymer Nanocomposites Matrices in Hazardous Waste Treatment 17

PNC Thermal Degradation

In general, thermal degradation involves waste oxidation in controlled or excess airand produces ashes and aerosols (Abdel Rahman and Zaki 2009; Abdel Rahman2010; Majka et al. 2016). Polymer thermal degradation process consists of threesteps (Pourchez et al. 2018; Duncan and Pillai 2015; Majka et al. 2016; Fina andCamino 2011; Lopez-Cuesta and Longuet 2014):

1. At sufficiently high temperature, thermo-oxidative combustion occurs at the toplayer of the polymer, and pure thermal degradation occurs in the underlyinglayers.

2. Ignition occurs when the gas concentration, produced by the thermo-oxidativedegradation, reaches the lower flammability limit.

3. After ignition, limited oxygen at the surface will require additional temperature tosustain the same gas concentration.

During this process the polymer decomposes via random or side-group scissionor monomer reversion, where the temperature plays a key role in this aspect. Thedecomposition of acrylic polymers, polymerized using a free radical method, pro-ceeds via scissions of head-to-head linkages, followed by scissions at the chain-endinitiation from vinylidene ends, and ends by random scission (Kashiwagi). It shouldbe noted that the decomposition products from random and side-group scission aredifferent, where the first produce alkanes, alkenes, and alkadienes, whereas the

Fig. 6 Estimate of nano-materials release based on maximum global production and high releaseestimates. (Adapted from (Keller et al. 2013))

18 R. O. Abdel Rahman et al.

second produce aromatic gases (Lopez-Cuesta and Longuet 2014). The presence ofNM in PNC affects the degradation process, where nano-clay reduced the ignitiontime and the thermo-oxidative layer thickness as a result of the oxidation ofgenerated gases by NM (Fina and Camino 2011). Subsequently, the design of thethermal degradation process should consider the effect of NM on the degradationprocess and the polymer decomposition mechanisms.

To ensure the occupational safety during the operation of the thermal degradationprocess and minimize NM release, the design of the thermal treatment of PNCshould consider the partitioning of NM between the ashes and aerosols, the physi-cochemical and morphological characteristics of the produced aerosols and ashes,and the occupational exposure (Sotiriou et al. 2015; Pourchez et al. 2018). Thermo-plastic polymeric matrix modified with inorganic NM was found to lead to minimumNM release, and the chemical composition of the aerosols and ashes is influenced bythe presence of the NM (Sotiriou et al. 2016). Inorganic NMs have higher potentialreleases than carbonaceous NM, where they were detected in the aerosols and ashes(Sotiriou et al. 2016; Singh et al. 2016). Increasing the combustion temperature from500 �C to 800 �C led to increased concentration of nano-materials in the aerosols andashes (Sotiriou et al. 2016). Thermal degradation of PNC used in the management ofhazardous wastes was not studied, where the synergetic effect of the NM andinorganic contaminants on the thermal degradation process and the release of bothcontaminants and NMs should be identified.

PNC Ashes Immobilization

The specific toxicity of the hazardous ashes is higher than the original wastes due totheir dispersive nature, so these ashes should be immobilized in a suitable matrix(Abdel Rahman and Zaki 2009; Abdel Rahman 2010). Hazardous ash immobilizationin cement-basedmaterials was applied (Spence and Shi 2004; Abdel Rahman and Zaki2009). These materials are composed of hydraulic binder, water, and additive/supple-mentary materials. Blended cement, a class of cement-based material with additivegreater than 15%, was tested to immobilize inorganic hazardous wastes (AbdelRahman and Ojovan 2016). In some classes of the blend cement (S, IS, SM), slag isused to replace cement to reduce the cost, increase the precipitation of heavy metalsand sulfide, lower lanthanides and actinides solubility, and reduce the permeability ofthe immobilized waste (Spence and Shi 2004; Abdel Rahman 2016). Fly ashes, limefly ashes, and cement ashes were used to immobilize inorganic hazardous wastes, i.e.,heavy metal sludge. The partial replacement of fly ashes in the later class is used toreduce the cost and improve immobilized waste properties as a result of the changes ofthe calcium silicate hydrate composition and pore structure refinement (Spence andShi 2004). Nano modification of cement-based materials was studied using differentmetal oxides, hydroxides, and carbonates (Abdel Rahman and Michael 2017). NanoTiO2, carbon nanotubes, and phosphate were found to accelerate the hydration,increase the strength, and decrease the compressive strength, respectively (AbdelRahman and Michael 2017). Incineration of PNC that was applied in the treatment

Life Cycle of Polymer Nanocomposites Matrices in Hazardous Waste Treatment 19

of hazardous wastes, i.e., membranes, photocatalytic materials, or sorbent, will lead tothe generation of hazardous ashes and aerosol as a result of the presence of NM and theinorganic hazardous contaminants. The feasibility of immobilizing the produced ashesin a suitable waste form was not studied.

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