Review On The Photocatalytic Degradation of Dyes and Antibacterial Activities of Pure and Doped-Zno

International Journal of Science and Research (IJSR)
ISSN (Online): 2319-7064

Index Copernicus Value (2013): 6.14 | Impact Factor (2013): 4.438
Review on the Photocatalytic Degradation of Dyes

and Antibacterial Activities of Pure and Doped-ZnO
Tesfay W. Gebreslassie1, Manjunatha Pattabi2, Rani M. Pattabi3
1, 2, 3
Department of Materials Science, Mangalore University, Mangalagangothri 574 199, India
Abstract: This paper reviews the recent advances on the photocatalytic and antibacterial activities of ZnO, metal-doped ZnO, non
metal-doped ZnO and nano-composite of ZnO synthesized using different methods. Materials with different morphologies and
structures have been investigated, by different groups, under UV, visible light and sunlight irradiations. The majority of data reveal
superior performance of modified ZnO nanomaterials compared to unmodified ZnO nanomaterials. The nanocomposite of ZnO
exhibits highest photocatalytic and antibacterial activity among all nanomaterial. The degradation of the dyes depends on both its
concentration as well as the amount of photocatalyst.
Keywords: Photocatalyst, Degradation, antibacterial activity
1. Introduction defect sites of the photocatalysts are thought to be a main

factor affecting the electron–hole recombination process
Textile industries are vast sectors especially in developing during photocatalysis [12-13].
countries. Among these various textile industries dyeing
process use large volume of water for dyeing, fixing and Many researches have focused on addressing issues through
washing. The textile industries use more than 10,000 different approaches including growing nanostructures with a
different dyes and the worldwide annual production of large fraction of polar surfaces, alloying with low band gap
dyestuffs is over 7 × 105 tons [1-2]. Among several classes of materials, doping with metals and inserting carbon allotropes
textile dyestuffs, reactive dyes contribute about 50% of the including graphene, carbon nanotubes (CNTs) and fullerenes
total market share and the most common group used as to achieve effective electron transport [13-14]. The creation
chromophore is the azo followed by anthraquinone. Dyes lost of polar surfaces and doping with metals are particularly
in wastewater could vary up to 50% during promising routes to improve the photocatalytic properties
manufacturing/processing operations. The release of those [13]. Unsaturated coordination bonds are highly reactive and
colored wastewaters in the ecosystem constitutes a dramatic are favorable for the adsorption of oxygen molecules
source of pollution which causes these effluents to be toxic resulting in a large number of H2O2 radicals which can
and mostly non-biodegradable. The coloration is visible even improve the photocatalytic properties [14]. Wang and co-
in very low dye concentrations [3-4]. As a result, workers [15] have shown that faceted ZnO prism quantum
technological systems for the removal of organic pollutants dots with polar surfaces adsorb OH- ions resulting in
such as adsorption on active carbon, reverse osmosis, ion improved photocatalytic activity. They have also investigated
exchange on synthetic adsorbent resins, ozonation and hierarchical mixed metal oxide structures grafted onto ZnO
biological methods are evaluated. All of these methods have and demonstrated improved visible light photocatalytic
advantages and drawbacks but these processes have very activity which is attributed to the large fractions of (0001)
high operating costs. However, these conventional treatment facets [16].
methods cannot effectively remove the dyes from effluents so
finding an effective technique is necessary [5]. The advantages of photocatalyst modifications are also to
delay electron–hole recombination to broaden the absorption
Heterogeneous photocatalysis is a promising technology for spectrum to facilitate some specific reactions on the surface
the removal of dyes from wastewater. It has great potential as of photocatalysts and to improve photo-stability. To
an environmental friendly, low cost and sustainable overcome the problems of anodic photo-corrosion and
technology. According to the different scholars there are instability of zinc oxide in acidic or alkaline media, doping of
various semiconductors including TiO2 [6], Fe2O3 [7], ZnO transition metals like Ag, Pd, Pt, Au and Fe with ZnO has
[8] and CuO [9] used as photocatalysts because of their proved beneficial [17-19].
ability to decolorize dye containing wastewater.
ZnO has wide band gap energy (= 3.37 eV) which limits light
Of the various semiconductor materials ZnO stands out due absorption to the UV region. A possible strategy to extend
to its properties and wide applications. ZnO has band gap ZnO photo-absorption to visible light may be the
energy of 3.37 eV for efficient absorption in larger fraction modification of its VB position by nonmetal doping such as
of solar energy and has a low cost. Therefore, it is considered N, F, S, P etc. Among the nonmetals N is widely acceptable
as a favorable material with potential use in photocatalysis owing to its compatible size to O and the smallest ionization
[10]. The photocatalytic activities of semiconductors are energy [20]. The doping of nonmetal in ZnO may cause band
correlated to the morphology, crystalline phase, porosity and gap narrowing, thus, shifting the photo-absorption edge of
surface area of the materials [11]. Additionally, the surface ZnO to visible region. Many methods such as chemical-
precipitation [21], thermal oxidation process [22],
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Paper ID: SUB157019 2252
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hydrothermal synthesis [23], sol-gel method [24], and obtained after slow and thorough vaporization of water at
microwave radiation [25] have been used to successfully 800C in air and were denoted as 300-ZnO, 400-ZnO, 500-
synthesize the ZnO, metal-doped ZnO nanocrystals. Methods ZnO and 600-ZnO respectively. The effect of cooling rate on
such as molecular beam epitaxy[26], pulsed laser ablation ZnO photocatalytic activity was analyzed and same amount
[27] and chemical vapor deposition [28] have been utilized to of intermediate products at 6000C were soaked in air and
dope nonmetal into ZnO. cooled naturally to room temperature and denoted as
600(air)-ZnO [32].
2. Synthesis Methods
(ii) Doped ZnO nanocrystals
(i) ZnO
Li et al [29] prepared ZnO crystalline powder solvo- Singh et al [33] prepared N-doped p-type ZnO nanocrystals
thermally. Aqueous solutions of zinc nitrate hexahydrate and by chemical route. Aqueous solutions of zinc acetate were
sodium hydroxide were prepared using de-ionized water. mixed with appropriate amount of aqueous solutions of
NaOH solution was added drop wise into Zn(NO3)2 solution ammonia. Then, stoichiometric amount of tetra methyl
at room temperature under vigorous stirring which results in ammonium hydroxide (TMAH) were mixed in the solutions
the formation of a white suspension. The suspensions were and stirred constantly. The mixtures were poured into a
separated with a centrifuge, thrice washed with distilled reaction vessel and kept on the stirrer at 1000C. The color of
water and finally washed with absolute alcohol. The the solutions changed from colorless to light milky white due
separated powders were dried at 600C in an oven and to the formation of colloidal Zn(OH)2 nanocrystals. The
obtained as the precursor. Subsequently, some amount of the reaction mixtures were kept inside a microwave oven at
precursor materials and NaCl were added into absolute 2500C. The white precipitates of N-doped ZnO NPs formed
alcohol, the mixture is sealed in a Teflon-lined autoclave were extracted by repeated washings. These precipitates were
with an interior volume filled in 35%. The autoclave is dried at 600C [33].
treated solvo-thermally at 1800C. Then, the resulting white
precipitates were washed with distilled water and alcohol Ag-doped ellipsoid ZnO nanostructures were synthesized by
several times and ZnO crystallites were obtained [29]. simple low temperature (~600C) solution process using
Zn(NO3)2.6H2O, AgNO3 and NaOH as precursors.
ZnO nanorods were synthesized by Onwudiwe et al. [30]. Zn(NO3)2.6H2O and AgNO3 were dissolved in de-ionized
Zinc acetate and polyvinylpyrolidone (PVP) were dissolved water under continuous stirring at room-temperature followed
into water. The solution was stirred at room temperature and by drop wise addition of NaOH solution [34]. Few drops of
sonicated. Then, water was removed by slow evaporation and NaOH were added to the resultant solutions under continuous
the resulting white solid product was grounded in a mortar stirring until pH reaches 11. The stirring of the solutions was
and pyrrolyzed at 3300C in a tube furnace under nitrogen continued. The final solutions were heated and refluxed.
flow. The resultant white solid powder was washed with de- After completing the reaction, the solution was cooled to
ionized water and ethanol to remove any remaining ions from room-temperature and finally grayish white precipitates were
the final products and finally dried at 600C in air. The PVP obtained after decanting the supernatant liquid. The
polymeric network was slowly burned off from the outer precipitates were washed with de-ionized water followed by
surface of the complex below 2000C and decomposition of ethanol and dried in an oven at 500C [34].
the zinc acetate at 3300C results in ZnO nanorods [30].
Viswanatha et al [35] synthesized tin-doped zinc oxide (Sn-
Synthesis of ZnO nanoparticless (NPs) by thermal doped ZnO) using zinc sulfate and different concentrations of
decomposition of zinc peroxide was demonstrated by SnCl2. NaOH solutions were added drop wise into a solution
Uekawa et al. [31]. Aqueous solutions of Zn(NO3)2.6H2O mixture containing zinc sulphate and different concentrations
and NaOH were reacted and the resultant zinc hydroxide of SnCl2 with constant stirring. Cetyl trimethyl ammonium
(Zn(OH)2) precipitates were centrifuged. The precipitates bromide (CTAB) was added as capping agent which inhibits
were separated and re-dispersed in distilled water. The anomalous growth of crystals. The resulting solutions were
solutions were again centrifuged and the precipitates were stirred constantly at room temperature. The white precipitates
dispersed in H2O2 aqueous solution. The dispersed solutions obtained were centrifuged, washed with distilled water and
were heated at 750C to yield a translucent sol of zinc alcohol. It was dried at 800C in an oven. The samples were
peroxide and dried at 750C. ZnO NPs could be obtained by calcined in a furnace at 6000C to obtain Sn-doped ZnO NPs
firing the dried sol at temperatures above 473K [27]. The as- [35].
synthesized NPs were calcined at 3000C in a furnace to
obtain spherical shaped ZnO NPs [31]. Zinc oxide (ZnO) and gadolinium-doped zinc oxide (Gd-
doped ZnO) nanostructures were synthesized using a simple
Fang et al [32] synthesized ZnO NPs by using hydrothermal sonochemical method. The as-synthesized nanostructures
method. The initial precursor of zinc acetate dihydrate was prepared by sonochemical method possessed higher
directly heated to different temperatures (300, 400, 500 and photocatalytic activity than the as-synthesized nanostructures
6000C) in ambient atmosphere with a heating rate of 250C/hr. prepared by conventional method [36]. Different amount of
Then, the hot intermediate products were taken out and Gd(NO3)3.6H2O was added to the solutions of zinc acetate.
immediately soaked in distilled water in a 5 cm × 10 cm NaOH solution was added to the mixtures until the pH
quartz boats. Finally, the resulting white powders were reaches 10. Then, the mixtures were sonicated in a bath type
sonicator at a frequency of 36 kHz. The resulting white
Volume 4 Issue 7, July 2015
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precipitates were washed thrice with absolute ethanol, washed by absolute ethanol and de-ionized water several
distilled water and dried at 800C [37]. times and dried at 800C [44].
ZnO NPs were synthesized by a modified non-basic solution Dou et al. [45] reported the microwave synthesis of Ag-ZnO-
route [38]. Zinc acetate dihydrate (Zn(Ac)2.2H2O was grapheme nanocomposites. Graphite and NaNO3 were added
dissolved into methanol under continuous stirring till a in a flask containing H2SO4 under stirring in an ice bath.
transparent solution was formed. The solutions were heated Potassium permanganate (KMnO4) was added slowly to the
at 800C under reflux to obtain a white colloidal product. It mixture. The ice bath was removed and the suspensions were
was collected and dried at 800C in air. The resultant product heated to 350C while stirring. The color of the solution
was semi-crystalline ZnO. The crystalline ZnO NPs were changed to dark. H2SO4 was added slowly to the suspension
prepared by heating the semi-crystalline ZnO at 4000C in air which was kept at 600C. The solution was cooled to room
in a tube furnace. Nitriding process was carried out by temperature. The color of the solution changed to luminous
heating the semi-crystalline or crystalline ZnO at 4000C in a yellow after H2O2 was added into the mixture. The
tube furnace with a flux flow of gaseous NH3. Then, N-doped precipitates were centrifuged and washed with the mixture of
ZnO were formed [39]. H2SO4 and H2O2 ten times, with HCl five times and with
distilled water three times and then, finally dried at 450C in
Pure ZnO powder and NH4NO3 were mixed by grinding with vacuum [45].
a pestle at room temperature using an agate mortar. Then, the
mixture was transferred into a ceramic crucible and calcined Ag-ZnO-graphene nanocomposites were prepared from
at 6000C in a furnace. For comparison, N-doped P25 TiO2 graphine oxide (GO). Different amount of graphine oxide
was also synthesized. For preparing N-doped Degussa (P25) (GO) was dispersed in water and kept in a bath type
TiO2, P25 TiO2 powder and NH4NO3 were mixed by grinding ultrasonicator and then, Zn(NO3)2.6H2O solution, AgNO3,
at room temperature. Then, the mixture was transferred into a C6H12N4 were added into the mixture and the mixtures were
ceramic crucible and calcined at 6000C in a furnace and N- sonicated at 900C. All the samples synthesized were
doped ZnO, N-doped P25 TiO2 was obtained [40]. centrifuged and washed with distilled water several times and
dried at 450C in vacuum [45].
(iii) ZnO nanocomposites
Zinc acetate [Zn(CH3COO)2.2H2O] was first dissolved in a 2-
Kim et al [41] synthesized Ag-doped ZnO/fly ash composite methoxyethanol(C3H8O2) and monoethanolamine (MEA,
by a hydro-thermal process. Some amount of fly ash (FA) in C2H7NO) solution at room temperature. The solution was
distilled water was pulverized ultra-sonically in a bath stirred at 600C until it become clear and homogeneous.
sonicator. Solutions of the following were prepared: Bis-hexa Aluminum nitrate [Al (NO3)3.9H2O] and/or cadmium nitrate
methylene triamine, zinc nitrate hexahydrate and AgNO3, all [Cd(NO3)2.6H2O] were added into some of the previous
in distilled water. Zinc nitrate and bis-hexamethylene solutions in an appropriate ratio. Then, it was stirred
triamine solutions were blended and vigorously stirred. The vigorously at 600C. The resulting mixtures were dried at
as-synthesized FA and AgNO3 solutions were added to the 1800C. The gel was first heated at 3000C and calcined in an
above solutions. The solutions were put into a Teflon oven at 8000C to obtain (Cd, Al)-co-doped ZnO NPs [46].
crucible and maintained inside the autoclave for Pure and doped ZnO nanostructures have been synthesized
hydrothermal treatment at 1400C [42]. Pristine-ZnO flowers and reported by many groups. Reddy et al. [47] have carried
and Ag-doped ZnO nanocomposites were synthesized out antibacterial studies on (Ag, Co) co-doped ZnO NPs.
without FA. The hydro-thermal plants were cooled to room ZnO nanorods doped with Mn2+, Co2+ and Ni2+ were
temperature. Then, the nanocomposites were filtered and synthesized and characterized by Murugadoss [48].
washed many times with distilled water and ethyl alcohol Rajkumar et al. [49] have presented a simple method for
with cellulose acetate membrane filter. The as-synthesized synthesis of dumbbell shaped ZnO nanorods. Mechano-
nanocomposites were dried at 1200C and used for further chemical method was adopted by Wang et al. [50] to
analysis [41]. synthesize S and N-doped ZnO NPs. Yang and co-workers
[51] succeeded in synthesizing corn-like znO nanostructures
ZnO NPs, zinc oxide carbon nanotubes (ZnO-CNTs) and investigated their photoluminescence. N-doped ZnO
nanocomposites were synthesized using a sol method [43]. bundle-like nanostructures were synthesized and studied by
Copper-doped zinc oxide (Cu-doped ZnO) NPs embedded in Zong et al. [52]. A solvo-thermal treatment approach yielding
carbon nanotubes (CNTs) exhibiting enhanced visible light mesoporous ZnO nanospheres with enhanced photocatalytic
photocatalytic activity was synthesized by Ahmad et al. [44]. activity was reported by Zhang et al. [53]. Er-N co-doped
Zinc acetate and appropriate amount of copper acetate was ZnO nanowires were synthesized by ion implantation [54].
dissolved in diethyl glycol. Subsequently, de-ionized water Al-doped conductive powders of ZnO [55], Sb-doped NPs
was added into the as-synthesized solution. The mixtures [56] prepared by different methods have also been reported.
were magnetically stirred at 160–1800C in air, forming aged
homogeneous sol. Then, purified CNTs were dispersed into 3. Characterization Techniques
the sol with ultrasonication. The solutions were slowly heated
to 160–1800C with vigorous magnetic stirring. It was cooled Reddy et al [47] characterized pure ZnO, Zn0.95Co0.05O,
to room temperature and Cu-doped ZnO-CNTs Zn0.95Ag0.05O and Zn0.90Co0.05Ag0.05O NPs using x-ray
nanocomposites were obtained after centrifuging. It was diffraction (XRD). The diffraction peaks of all samples were

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matched with the hexagonal wurtzite ZnO data. There were concentrations of Sn the optical absorption edge slightly
no characteristic peaks of impurity phases regardless of the shifted towards the longer wavelength region which is
dopant concentrations, confirming high purity of the as- attributed to the change in the grain size [35].
synthesized NPs. Thus, the wurtzite structures were not
modified by addition of Ag and Co into ZnO host material. ZnO and nitrogen-doped ZnO (ZnO:N) were characterized
After the samples were annealed at 5000C, the crystallite from XRD data [33]. The sharp intense peaks of ZnO
sizes of the as-synthesized NPs were estimated from confirmed good crystalline nature of ZnO:N. The peaks
Scherer’s equation originating from (100), (002), (101), (102), (110), (103) and
(112) reflections are of hexagonal ZnO doped with N. All the
diffraction peaks are in good agreement with that of the
λ is X-ray wavelength, θ is the Bragg angle, β is the full hexagonal wurtzite structure of ZnO. The relative intensity of
width at half maximum (FWHM) of the prominent diffraction peaks (100)/(002) in all three samples are nearly 1.2 which
peak. clearly supports the formation of non spherical ZnO:N NPs
Quantitative analyses were made for Co and Ag contents in and indicating the formation of rod shaped ZnO
ZnO samples at different doping levels [47]. nanostructures[33].
The crystallinity of ZnO nanorods synthesized by Increasing nitrogen concentration increases the 2Θ value and
Murugadoss [48] was investigated by XRD pattern. The crystallite size. The slightly larger 2Θ values for ZnO:N is
peaks at scattering angles (2ϴ) of 31.4, 33.2, 35.1, 46.3, due to the bond length of Zn–N (1.88 A0) being smaller than
55.4, 61.6 and 66.6 corresponding to the reflection from that of Zn–O (1.93 A0). These results clearly support the
(100), (002), (101), (102), (110), (103) and (112) crystal incorporation of nitrogen into the ZnO lattice forming Zn:N
planes were observed respectively. The peaks were assigned i.e. substituting oxygen with nitrogen in ZnO [33].
to diffractions from various planes corresponding to
hexagonal structure of ZnO. The crystallite sizes of Mn2+, The dependence of absorption coefficients on the photon
Co2+ and Ni2+ doped ZnO were determined by means of X- energy for the ZnO:N NPs have also been carried out [33]. A
ray line-broadening method [48]. change in the energy gap with N concentration is observed,
caused by the variation in size of the particles with nitrogen
The size of the crystallites estimated from XRD patterns are concentration. As the nitrogen concentration increases from 3
of the order of 8-12 nm. The full width at half maximum at% to 6 at%, there is an increase in band gap energy by 0.38
(FWHM) of the diffraction peaks of pure ZnO NPs are eV but as concentration is further increased to 9 at% there is
broader than that of the doped nanocomposites. No a decrease in band gap energy by an amount of 0.1eV with
diffraction peaks of other compounds are observed. The ZnO respect to 3 at% concentration . An increase in nitrogen
nanorods prepared by chemical method have high concentration from 3 at% to 6 at% also increases the carrier
crystallinity and high purity. The observed interplaner concentration which cause a blue shift in absorption spectra
spacing of pure ZnO are indexed to hexagonal wurtzite with while a further increase in nitrogen concentration i.e. up to 9
lattice constant of about 0.2476 nm (d101). When dopant ions at%, causes decreasing carrier concentration. This result
were introduced in ZnO lattice, the interplanar spacing of agrees well with the result of Hall measurements. The as-
ZnO changed. The interplanar spacings were 0.2504, 0.2397 synthesized ZnO:N NPs have very large direct band gap
and 0.2392 nm for Mn2+, Co2+ and Ni2+ doped ZnO energy [33].
nanostructures respectively. The doped ions were
successfully incorporated into ZnO lattice sites [48]. Wang et al [50] investigated the UV-visible absorbance of S-
doped ZnO. Compared with ZnO in which absorbance occurs
However, the crystal quality of Co and Ni-doped ZnO is only in the UV range under 400 nm, extension of the
significantly better than that of Mn-doped ZnO. The absorbance is clearly observed in these samples into the
substitution of the Zn ions by Co and Ni into ZnO lattice is visible range for wavelength as long as 500 nm. The
due to smaller ionic radius of Co and Ni than Zn though the extension of absorbance reflects doping effects of sulfur and
crystal quality of doped ZnO is decreased by impurity ions of is confirmed by XRD [50].
Mn, Co and Ni, [48].
The UV–Vis absorption spectra of pure ZnO, calcined zinc
The ultraviolet visible (UV-Vis) spectra of Sn-doped ZnO oxide at 6000C (ZnO-600), N-doped P25 TiO2 and N-doped
NPs were obtained by precipitation method and showed a ZnO were evaluated [40]. Pure ZnO and ZnO-600 exhibited
small red shift in the absorption peaks with increasing Sn band edge absorption at around 390 nm but with little
concentration [35]. The small shift in the absorption band is absorption of visible-light [40]. However, for N-doped ZnO,
attributed to the doping of Sn into ZnO. The band gaps of Sn- it displayed a distinct tailing absorption covering the whole
doped ZnO are calculated by using the formula visible region. Photo-absorption feature reported for N-doped
ZnO suggests that the as-synthesized N-doped ZnO have the
Where E is band gap energy, h is Planck’s constant, C the potential to be a visible light driven photocatalyst.
speed of light and λ is the wave length. Furthermore, the visible-light absorption ability of the as-
synthesized N-doped ZnO is better than those of pure ZnO,
The band gaps of Sn-doped ZnO at different concentrations ZnO-600 and N-doped P25 [40].
are found to be in the range 3.40 to 3.33 eV. With increasing

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The transmission electron microscopy (TEM) image of ZnO morphology. Almost the same homogeneous structures are
revealed a tetrapod structure with a size distribution of 200- obtained for ZnO doped with 3% Sb. But when doping is
500 nm in diameter and of ~3 μm in length [54]. The branch increased from 3% Sb to 5% Sb, finer particles are observed
of tetrapods displayed a conjunctional shape whose radial with heterogeneous morphology. [56]
size at the middle is less than that at the two ends. The
growth mechanism is interpreted as vapor-liquid-solid (VLS) From SEM observations the Segmented Flow Tubular
process which generally involves nucleation which induces Reactor (SFTR) process is found to produce particles
the epitaxial growth. The estimated interatomic spacing is homogeneous in size with narrow particle size distribution
about 0.52 nm which is consistent with the lattice constant c (PSD) and equiaxed morphologies [57]. The average size of
of ZnO. After ion implantation of Er3+, the crystalline quality SFTR produced particles with polyacrylic acid (Al0-PAA) at
is found to degrade gently [54]. Similarly, the solubility of the initial point of Al addition is dv50 = 64 nm. The addition
Er3+ in ZnO host is low because the radius of Zn2+ is smaller of very small amount of Al (Al/Zn = 0.01) decreases the size
than that of Er3+ ion and their formal valences are different. to dv50 = 46 nm. The power of the SFTR allowed a
The studies showed that ion implantation offered the continuous production of very homogeneous ZnO
possibility of controlling the number of atoms and their depth nanocrystals in a very reproducible way [57]. The
profile by changing the implantation parameters [54]. investigation showed that this behavior is extended to Al-
doped ZnO with different Al amounts.
Viswanatha et al [35] evaluated the morphology of the Sn-
doped ZnO NPs using TEM. The sizes of the Sn-ZnO NPs NPs are also formed via the microwave-assisted
are found to be in the range ~60 nm. Although the NPs are hydrothermal method. By adding some amount of Al an
slightly agglomerated, their grain boundaries are clearly elongation is observed in many particles obtained by
distinguishable and the crystal images of the product are microwave-assisted hydrothermal method (MW-Al0) [57].
clearly observed. Nanosize crystallites are seen as closely The addition of polyacrylic acid (PAA) is found to inhibit the
grouped together and formed a small flake like morphology. elongated growth and lead to smaller and more homogeneous
Doping of Sn does not change the shape of the NPs. The particles (150–200 nm) with equiaxed morphologies.
selected area electron diffraction (SAED) pattern showed the Without any additive/dopant the microwave-assisted
crystalline nature of Sn-doped ZnO NPs [35]. hydrothermal method led to a chaotic nucleation and growth
which led to less control on the final particle size and PSD
Scanning electron microscopy (SEM) is one of the promising than when using the SFTR. This is mainly explained by the
techniques for the morphology studies of the samples and use of a micro-mixer in the SFTR which controls the initial
gives important information regarding the shape and size of supersaturation and the smaller reaction volume which
the particles. The morphologies of samples are approximately ensures a more homogeneous heating and concentration
hexagonal in accordance with the XRD analysis [55]. The profile [57].
average grain size and surface roughness of aluminum-doped
zinc oxide (AZO) particles decrease as reducing the amount SEM images of Eu-doped ZnO NPs revealed smaller
of oxygen present in AZO which surrounds the atmosphere in crystalline size as compared to pure ZnO NPs [58].
post-calcined. Al-doped ZnO showed that the as-synthesized Introduction of Eu3+ ions into the ZnO lattice decreases the
particle sizes are uniformly distributed on the surface. This aggregation of NPs and consequently decreases the size of
result is attributed to the AZO post calcined under reduced the particles. Using manual microstructure distance
atmosphere (CO). This kind of atmosphere causes more measurement software, the size distribution of the Eu-doped
defects such as oxygen vacancies, Zn interstitial and Al3+ ZnO NPs is found to be in the range of 30–40 nm which is
substituted Zn2+. The existence of more defects greatly much smaller than that of pure ZnO NPs which have sizes in
decreases the grain size and the surface roughness due to Al3+ the range 200–250 nm [58].
substituting Zn2+ completely and uniformly [55].
4. Photocatalytic Degradation of Dyes
SEM images of ZnO:N nanostructures synthesized at
different nitrogen concentrations showed the formation of The degradation of methylene blue (MB) was evaluated in
uniform size dumbbell shaped ZnO:N nanorods. In the the presence and absence of ZnO nanoflowers under UV
sample in which the concentration of nitrogen relative to ZnO irradiations [59]. In the absence of ZnO, there is no
is 3 Atm% the length is about 1.7μm and central width about degradation of MB. The characteristic peak of MB (λ = 664
250 nm. It was found that as the relative concentration of nm) is taken as a standard for evaluation of photocatalytic
nitrogen is increased it gives rise to the formation of activity. As irradiation time is increased, the intensity of
nanorods of ZnO i.e. there is a decrease in the aspect ratio of absorbance peak declined. 83% degradation of MB is
the nanorods with increasing nitrogen concentration [33]. achieved in the presence of ZnO nanoflowers [59].
Principally, the generation of electron–hole pairs by ZnO
The morphology of nanocrystalline pure ZnO and Sb-doped nanoflowers and its destination is the basic mechanism
ZnO nanopowders were studied by SEM [56]. The SEM behind photo-degradation in the presence of ZnO
images revealed that the surface morphologies of ZnO NPs nanoflowers. The degradation reaction kinetics followed a
are affected by concentration of doped-Sb. The SEM images first order at a low concentration of the dye [59].
of pure ZnO NPs are well defined and distinguishable from
each other. At 1% composition of Sb-doping in ZnO NPs, the
particles are smaller, darker and have a homogeneous
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The photo-degradation of MB under UV irradiation and observed under UV irradiation. The photocatalytic activity is
without UV irradiation was studied both in the presence and dependent on the morphology of ZnO films. The activity
absence of ZnO. The photocatalytic degradation of MB is showed the following order: ZnO films deposition at 2 days
found to be 37.15% by using CdS NPs whereas ZnO time (3#) > ZnO films deposition at 1 day time (2#) > ZnO
nanoflowers showed 83% degradation. This showed that ZnO films deposition at 3 days time (4#) > ZnO films deposition
nanoflowers are better photocatalysts than CdS NPs. The at 5 hours time (1#). After irradiations, the aqueous solution
degradation of MB using ZnO NPs by Barnes et al. [60] of RhB is almost eliminated by film 3#. After the degradation
showed only 18% degradation of MB thus suggesting a experiments, the regenerated photocatalyst were washed and
greater efficacy of ZnO nanoflowers for photo-degradation of dried before further run. After 5 runs, 87% degradation is
MB [59]. completed [63].
The authors also examined the photo-stability of ZnO Solar energy absorption is more effective in film 3# with
nanoflowers. The photo-degradation efficiency after 3 ZnO cages on the surface which plays the role of RhB
consecutive recycles is found to be 74% indicating good molecules traps. Under UV irradiation, as long as photons
photo-stability of the nanoflowers. The rate of recovery is entered into ZnO cages, they are reflected by the cage bars
found to be about 90%; this shows great applicability of ZnO many times before escaping. The increase in reflecting times
nanoflowers in industrial photocatalysis processes. in cages led to absorption of photons by ZnO cages [63].
Once an RhB molecule enters into ZnO cages, they have
The mechanism responsible for the photocatalytic activity more opportunity to contact the surface of ZnO materials
suggested was the one proposed by Sun and co-workers [61]. than on other films. RhB molecules react with hydroxyl
The electron-hole pairs are produced under UV light, when radicals on the surface of ZnO more smoothly. Therefore,
ZnO are illuminated with UV light irradiations having larger most of RhB molecules are completely degraded before they
photon energy than the band gap of the ZnO nanoflowers. diffuse out of cages [63].
These act as powerful oxidizing and reducing agents. The
photo-generated electrons and holes are transferred to the 4.1. Degradation of Dyes Using Metal-Doped ZnO
surface of the crystal where the water adsorbed on the ZnO
nanoflowers trapped the holes leading to the formation of The degradation of MO was investigated using ZnO and
hydroxyl radicals (∙OH). The presence of oxygen (O2) silver-doped zinc oxide NPs in aqueous solutions under UV
prevents the recombination process of electron and hole pair, irradiations [64]. The studies were carried out with Ag-doped
and initiates the formation of an anion radical (∙O∙2) by ZnO NPs prepared with various molar ratios of Zn(NO3)2 to
accepting electrons from the conduction band (CB) AgNO3 ratios, viz. 0, 0.01, 0.03, 0.05 and 0.07 labeled as
associated with the proton, to give ∙OH. The ∙OH and ∙O2 AZ0, AZ1, AZ3, AZ5 and AZ7. Ag-doped ZnO NPs possessed
degrade the aromatic ring of MB by opening it at the azo higher photocatalytic activities than pure ZnO. The
bond and the hydroxylated ring. The oxygen vacancy on the photocatalytic activities of Ag-doped ZnO first increased
surface acts as an active center which captures the photo- with increasing Ag content up to 3% (AZ3), and slightly
induced electrons. These inhibited the photon–electron decreased with further increase in content of Ag. AZ3 is
recombination thereby increasing the photocatalytic activity. found to be the most active which shows a photocatalytic
activity about 2 times higher than pure ZnO (AZ0). Further, it
The photocatalytic degradation of methyl orange (MO) was is also found that the degradation rate of MO under the real
assessed by using ZnO nanosheets and nanotubes after sunlight irradiation is complete after irradiation for 100 min
prolonged exposure to UV light in aqueous solution [62]. by adding sample AZ3.
The optical absorption spectra of MO solution at different
time intervals of the photo-degradation reactions over ZnO The enhanced photocatalytic activity of Ag-doped ZnO, as
nanosheets and ZnO nantubes were taken. For both samples, suggested by Zheng et al. [65], is attributed to the better
the degradation behaviors are found to be similar but the time charge separation formed as a result of Ag hindering the
consumed for degradation is different. These results showed recombination of photo-induced electrons. When the content
that the degradation efficiency depends on the morphology of of Ag is below the optimal value, the higher the content of
ZnO. The effect of morphology on the photo-degradation Ag in composite is, the higher the photocatalytic activity of
efficiency is ascribed to the following reason: when the size Ag-doped ZnO heterostructure photocatalyst. When the
of ZnO crystals decreases, the amount of the dispersion of content of Ag is above the optimal value, metallic Ag act as
particles per volume in the solution increases resulting in the recombination centers which is caused by the electrostatic
enhancement of photon absorbance. ZnO nanosheets are attraction of negatively charged Ag and positively charged
found to be more effective on the degradation of MO than the holes. Furthermore excessive Ag reduced the number of
nanotubes, possibly due to their higher surface area and photons absorbed by the photocatalyst because of light-
consequent larger contact area between photocatalyst and filtered effect.
target material [62].
Aluminum-doped zinc oxide (AZO) was prepared with
The degradation of organic azo-dye N, N, N’, N’-tetra different electrical conductivities under different post-
ethylated rhodamine (RhB) was examined under UV calcined atmospheres [55]. AZO possessed more
irradiation [63]. The degradation of RhB was done with photocatalytic activity than pure ZnO which is ascribed to the
different amounts of ZnO photocatalysts. In the absence of a Al3+ entering into the ZnO lattice substituting the Zn2+ site
catalyst, only a slow decrease in the concentration of RhB is which made the particle size small and caused an increase in
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the carrier concentration. The photocatalytic activities of The enhanced photocatalytic activity of Nb-loaded ZnO NPs
AZO in different post-calcined atmospheres are different, found in the study is thus, ascribed to Nb acting as electron
with the sample post-calcined under reduced atmosphere trap centre which decreases electron-hole pair recombination
(CO) showing highest photocatalytic activity. This is because rate. If the amount of Nb-loading is higher than the optimal
under reduced atmosphere the generated oxygen is value, the activity of ZnO NPs decreases probably because an
consumed, prompting the larger generation of oxygen excess amount of Nb become the center for recombination of
vacancy which makes the Al3+ effectively substitute the Zn2+ photo-induced electron and hole pairs [67].
sites. So the carrier concentration increases, causing a
reduction in resistivity. As the carrier concentration Reactive oxygen species (ROS) generations by pure and Se-
increases, the intermediate energy gap between VB and CB doped ZnO NPs were investigated for degradation of trypan
become more active. Therefore, during light irradiation the blue (TB) under UV light (340–360 nm). This wavelength
free electrons are easily decomposed from the AZO, resulting region corresponds to the order of band gaps of the doped
in the formation of positively charged hole allowing better and pure ZnO NPs. The degradation of TB was examined by
electrical conductivity. The hole generates H+ and •OH from oxidative processes. Compared to the control batch which is
H2O whereas the electrons activate O2 to become superoxide not treated with ZnO NPs, the degradation of TB dye is more
anion radicals •O2 in air. This reacted with H2O, forming for the batches treated respectively with 5 wt% Se-doped
H2O2 which further yielded reactive •OH [55]. The generated ZnO NPs and pure ZnO NPs in the presence of UV light
radicals caused MO dye decomposition. illumination [68]. The dye degradation efficiency is several
folds higher for Se-doped ZnO NPs than that of pure ZnO
Photocatalytic degradation of cresols was studied under NPs. Such high efficiency of dye degradation by Se-doped
visible light irradiation using commercial zinc oxide (C- ZnO NPs is attributed to higher ROS generation. The results
ZnO), manganese-doped zinc oxide (Mn-doped ZnO) and on ROS induced dye degradation are consistent with the
uncalcined zinc oxide (U-ZnO) [66]. The photocatalytic literature [69]. The doping of Se in ZnO NPs enhanced ROS
activities of the nanomaterials depend on the adsorption of generation and this led to higher dye degradation than pure
the amount of removable pollutants over nanomaterials. The ZnO NPs [68].
amount of adsorbed cresols on the C-ZnO, U-ZnO and Mn-
doped ZnO were evaluated. The results are given in 4.2. Degradation of Dyes Using Non-Metal Doped ZnO
increasing order C-ZnO ≤ U-ZnO ≤ 0.5% Mn ≤ 1% Mn-
doped ZnO. However, the adsorption decreases above 1% The as-synthesized N-doped ZnO microcrystals possessed
Mn. The adsorption of cresols on 1% Mn-doped ZnO is the much higher photocatalytic activity than commercial pure
highest attributing to it has the highest Brunauer-Emmett- ZnO in the decomposition of formaldehyde under visible-
Teller (BET) surface area. light (λ > 420 nm) [40]. Zinc oxide doped with nitrogen (N-
doped ZnO) at the interstitial sites creates intra-band gap N
The reaction rates and degradation efficiency are given in related defects about 1.2–1.3 eV above the VB edge which
the order 1% Mn-doped > U-ZnO > C-ZnO. This is are responsible for the absorption of visible light. The intra-
attributed to characteristics of the photocatalyst such as band gap N related defects (NO) is stable in either the neutral
decreasing particle size, agglomeration size and increasing (NO0) or −1 charge states (NO−). The existence of NO− and
surface area. Another reason is related to overlap of the t2g of NO0 intra-band gap states allow N-doped ZnO to absorb the
Mn with the VB of ZnO. Average particle size of as- needed photon energy for moving electrons from VB to CB
synthesized ZnO is 30–40 nm while C-ZnO particle size is via two different steps of electron excitation i.e. the electron
400-500 nm and surface area of pure ZnO is greater than the excitation from NO− to CB and from VB to NO0 in which the
surface area of C-ZnO. Therefore, the improvement of intra-band gap N related defects plays the role of electron
degradation efficiency and rate of reaction is due to the transfer intermediate.
surface area difference [66].
The degradation of formaldehyde is carried out in the
The percentage degradation of phenol was evaluated as a presence pure ZnO and N-doped ZnO and described in terms
function of time using pure and Nb-doped ZnO NPs by of Langmuir Hinshel wood model [40]. The degradation of
loading different amounts of Nb [67]. A 0.50 mol% Nb- formaldehyde followed a first order kinetics. The
loaded ZnO NPs possessed the highest photocatalytic activity photocatalytic activities of N-doped ZnO NPs deteriorated
among all samples and took shortest time to complete phenol with recycling. The photocatalysts are separated from the
degradation process. The results clearly suggested that the suspension by filtration and washed with de-ionized water to
photocatalytic activities of ZnO NPs are greatly improved by remove the suspensions. The photocatalysts were dried and
loading an appropriate amount of Nb. The optimal amount of weighed after each cycle. Moreover, the mass lost during
Nb is found to be 0.50 mol% for degradation of the organic each cycle is lower than 3 wt. % which meant the recovery
compound tested. It was also reported that increasing Nb efficiency of N-doped ZnO is above 97 wt. % for each cycle
loading results in an enlarged surface area of the Nb-loaded [40]. The as-synthesized N-doped ZnO NPs is easily
ZnO nanomaterials. However, an increase in surface area is recovered from the suspension by filtration after the
likely not the main factor affecting the photocatalytic activity photocatalysis reaction, and further used for another
of Nb-loaded ZnO. This is supported by the facts that photocatalysis reaction. 94% degradation ratio of
although the surface area of 1 mol% Nb-loaded ZnO NPs are formaldehyde is achieved in the first three cycles and 91% in
higher than 0.5 mol% Nb-loaded ZnO NPs, its photocatalytic the fifth cycle. This is because of the high photocatalytic
activity is lower [67]. activity of N-doped ZnO and excellent photochemical
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stability. The as-synthesized N-doped ZnO micropolyhedrons increasing of graphene amount. However, when the loading
are therefore, promising photocatalysts in removing amount exceeded 1.0 wt%, the photocatalytic activities of
formaldehyde pollutants from wastewater due to its high Ag-ZnO-graphene samples decreases as the amount of
visible light photocatalytic activities and excellent graphene is increased. For MO solution in the presence of
photochemical stability [40]. Ag-ZnO-graphene, almost all of MO is degraded under UV
irradiation. The maximum absorbance at 464 nm almost
4.3. Photocatalytic Degradation of Dyes Using disappeared after irradiation [45].
Nanocomposite
Kinetic analysis of MO degradation is conducted to
The photocatalytic activities of ZnO–CdS core–shell understand the photocatalytic efficiency of the Ag-ZnO-
nanostructure coated on glass were investigated by graphene composites. The reaction kinetics is described in
degradation of Congo red (CR) dye in aqueous solutions terms of Langmuir Hinshel Wood model:
[70]. The photocatalytic degradation of organic pollutants
takes place on the surface and the solution pH play an
important role in the process. The absorption spectra of CR is where (-dC/dt) is the degradation rate of MO, k is the
taken at different irradiation times using ZnO/CdS which is photocatalysis rate constant, C is the concentration and K is
coated on glass, at a solution of pH = 3, 7.4 and 9. The the equilibrium adsorption coefficient of MO. KC is
maximum degradation of CR at solution pH = 3, 7.4 and 9 negligible when value of C is very small. The above equation
occurred at 75 min, 107 min and 90 min respectively. can be described as first-order kinetics model:
The pH of the solutions thus, seems to affect the rate of

reaction on photocatalyst surfaces which is related to the Where C0 is the initial concentration and kapp is the apparent
surface charge properties of the semiconductors. The point of rate constant. kapp determines a photocatalytic activity
zero charge (pzc) for ZnO is at pH 9 [70]. The photocatalyst independent of the adsorption period in the dark and the
is positively charged at pH < pzc which favored adsorption concentration of MO remaining in the solution. kapp of Ag-
of the negatively charged CR due to the interaction of holes ZnO-graphene with 1.0 wt% GO addition is about 3.1 times
or hydroxyl radicals with Congo red. At pH > pzc, the that of Ag-ZnO and nearly 4.8 times of pure ZnO.
photocatalyst surface become negatively charged and
adsorption of CR is not favorable [70]. Photoluminescence (PL) studies on these samples showed
that there are a great number of surface deep traps or intrinsic
The studies showed that under dark conditions, the defects such as oxygen vacancies and interstitial zinc. The PL
degradation of CR is negligible. The presence of both light intensities of these samples increase in the following order:
irradiation and photocatalysts are necessary for the efficient Ag-ZnO-graphene, Ag-ZnO, ZnO. The orders of PL
photocatalytic degradation of CR [70]. Pure ZnO possessed a intensities of the samples are in accordance with the
lower photocatalytic activity under the same conditions. photocatalytic activities [45].
When ZnO and CdS are coupled together then, they form
core–shell nanostructures and photons are absorbed in both The authors explain the enhancement of the photocatalytic
ZnO and CdS surface, and electron-hole pairs are formed. activity based on the lifetime of photo-excited electron-hole
The electrons are transferred from CdS to ZnO with pairs. The work functions of Ag and ZnO are about ˗4.26 eV
formation of a hole on CdS. The electron and hole pairs are and ˗5.2 eV [45]. The Fermi energy of Ag being higher than
efficiently separated which is regarded as the key factor for that of ZnO favored the transfer of electrons from Ag to ZnO,
the improvement of photocatalytic activities of the ZnO–CdS reached equilibrium, and formed the new Fermi energy [71].
core–shell nanostructures [70]. When the Ag-ZnO nanocomposites were illuminated under
Another factor affecting the photocatalytic activities of the UV light with photon energy higher or equal to the band gap
core–shell is the loading content of the active components. of ZnO, electrons in the VB were excited to the CB and left
The photocatalytic degradation rate of CR is enhanced with the corresponding holes in the VB. Since the bottom of the
increasing content of ZnO up to ZnO(0.2 M)/CdS(0.075 M) CB of ZnO is higher than the new equilibrium Fermi energy
which is reached at 88.0% irradiation [70]. level of Ag-ZnO, the photo-induced electrons are transferred
from the CB of ZnO to the Ag and holes remained in VB of
The photocatalytic activity of the Ag-ZnO-graphene with ZnO [71]. Therefore, the recombination of electrons and
different amounts of graphene loading is investigated for the holes are effectively delayed. Graphene is a zero band gap
degradation of MO [45]. In the absence of photocatalysts, no semiconductor having a work function of ˗4.42 eV. The
significant decrease is observed in the concentration of MO photo-induced electrons are also transferred from ZnO to
under UV irradiations. The photocatalytic activity of ZnO is graphene which left holes in VB of ZnO. Therefore, the most
improved by incorporation of Ag [71]. The addition of effective electron–hole separation of Ag-ZnO-graphene
graphene enhanced the photocatalytic performance nanocomposites achieves the highest photocatalytic activity
significantly. In addition, Ag-ZnO-graphene photocatalyst [45].
with different amount of graphene loading shows different
photocatalytic activities. Ag-ZnO-graphene nanocomposites
exhibited the highest photocatalytic activity when the content
of graphene is 1.0 wt%. When the loading amount is below
1.0 wt%, the photocatalytic activities improved with
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4.4. Effect of Concentration of Dyes on Photocatalytic The effect of initial concentration of the dye on degradation
Activity of Photocatalysts under sunlight and UV light irradiation was performed by
varying the dye concentration from 1 mgL−1 to 25 mgL−1 with
The reaction rate was performed by varying the constant catalytic loading of 100 mg [76]. The degradation of
concentrations of indigo carmine at a fixed amount of Se- MB increases with concentration up to 5 mgL−1 and 3 mgL−1
doped ZnO NPs [72]. The reaction rate was found to under sunlight and UV light irradiation respectively, and
decrease with increasing concentrations of indigo carmine. shows a steady decrease in the degradation[74]. In low
This is because with increase in the dye concentration, the concentrations reverse effect is observed. The optimal
solution become more intense in color and the path length of concentration of degradation is 5 mgL−1 under sunlight and 3
the photons entering the solution is decreased resulting in mgL−1 under UV light. As the reaction under sunlight and
only a few photons reaching the catalyst surface. Hence, the UV light proceeded to completion at 120 min, the
productions of hydroxyl radicals are reduced. Therefore, the comparison of efficiency is done based on the percentage
degradation efficiency is reduced [72]. degradation at 15 min. 93% of MB degradation is observed
for 15 min in sunlight whereas only 69% was observed under
The mineralization of chemical oxygen demand (COD) was UV light. Degradation of MB occurs faster in sunlight than
determined at different stages. The dye is mineralized into UV light. The results are in good agreement with earlier
H2O, CO2 and simpler inorganic salts after it was irradiated reports [75] that ZnO–TS (tapioca starch) NPs could harvest
in presence of Se-doped ZnO photocatalysts [72]. The maximum solar energy by making use of sunlight for
degradation efficiency of the photocatalyst is calculated by degradation of water bound organic compounds [76].
the following formula.
4.5. Effect of Photocatalyst Loading
Sowbhagya and Ananda, [72] investigated the effect of

The effect of initial acid orange 7 (AO7) concentrations on
photocatalyst loading by varying the amount of
its sonocatalytic decolorization efficiency was investigated
photocatalysts. An increase in photocatalyst loading increases
by varying initial dye concentrations [37]. The decolorization
dyes removal efficiency. Further increase in the amount of
efficiency of AO7 is inversely proportional to its initial
the photocatalyst decreases the photocatalytic activity of the
concentrations. As the initial concentrations of the dye were
catalyst. The reason for the decrease in degradation rate is
increased, the sonocatalytic decolorization of AO7 decreases
due to the aggregation of Se-doped ZnO NPs at high
[37]. This negative effect is because of the following reasons:
concentrations causing a decrease in the number of surface
active sites which increases the opacity and light scattering.
The number of dye molecules that are adsorbed on the
This decreases the passage of light through the sample.
surface of photocatalyst increases because of the increment in
Therefore, there is an optimized photocatalyst loading [72].
dye concentration. In addition, at a high dye concentration a
significant amount of UV light is absorbed by the dye
The catalyst dosages of Gd-doped ZnO increased by
molecules [37]. The generation of OH∙ radicals on the surface
increasing the catalytic decolorization of acid orange 7
of catalyst is likely be reduced since active sites on the
(AO7) within a reaction time for some range [37]. A high
surface of the catalyst are occupied by the dye ions [37].
amount of catalyst dosages favored the decolorization of
AO7. An increase in catalytic decolorization of AO7
With increasing dye concentration the numbers of hydroxyl
increased with photocatalyst dosage and these results from
radicals required for decolorization of dye molecules
increasing the available surface area containing active
increases. However, the formation of hydroxyl radicals
reaction sites. Consequently, it generates more OH∙ radicals
remain constant for a given catalyst dosage, irradiation time
for the degradation of AO7 [37]. Ultrasonic irradiation is
and intensity. The catalytic degradation process is therefore
diminished due to the blockage of active reaction sites of the
promising at low concentration of pollutants [37].
photocatalyst and aggregation of the as-synthesized
The effect of initial concentration of direct blue 71 (DB71)
photocatalyst in the solution [37].
on the catalytic degradation of DB71 was investigated using
ZnO NPs [73]. DB71 oxidation process was tested by
Excessive amount of catalyst in the solution results in the
treating at different initial concentrations of DB71 at pH 2.5
scattering of ultrasound and blocked the transmission of
with photocatalysts [73]. The color removal efficiency is
ultrasound waves and energy near the surface of the catalyst
found to decrease as initial dye concentration increased. As
thus decreasing the rates of catalytic degradation reactions
the initial concentration of dye is increased, more and more
[37]. In addition, excessive catalyst dosage causes: (i)
dye molecules are adsorbed on the surface of ZnO powder
increasing OH- consumption at the interface of bubble and
[73]. The large amount of adsorbed dye is thought to have an
solution (ii) accumulation of byproducts in the cavity bubbles
inhibitive effect on the reaction of dye molecules with
for lower collapsed temperatures and lead less powerful
sonocatalytic holes or •OH radicals because of the lack of any
collapse.
direct contact between them. The removal rate decreases
because the concentration of dye increases with no increase
Ramasami et al. [76] studied the optimal catalyst loading
in the •OH radical concentration responsible for their
under both sunlight and UV irradiations by varying the
reduction [73].
amount of ZnO NPs. The degradation of MB is completed at
around half-time (30min) for all ZnO NPs concentrations.
Initially the degradation of MB increases with increase in the
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catalytic load under sunlight and UV light illuminations. Culture media containing this bacterial strain was treated
Increasing load of catalyst increases the surface area of the with Se-doped ZnO NPs in a wide range of concentrations.
catalyst exposed to the radiation, thereby increasing the They observed a delay in the onset of bacterial growth as also
degradation [74]. Further increase in catalytic loading led to an enhancement in the inhibition of bacterial growth with
aggregation according to Ramasami et al. [76] shielding of increasing concentration of NPs. Surprisingly, although
the photocatalyst and deactivation of the excited state bactericidal condition could be achieved with pure ZnO NPs,
molecules due to collision with ground state molecules as only 51% growth inhibition was observed for the same
observed by Neppolian et al. [74] and increasing turbidity of concentration of Se-doped ZnO NPs.
the suspension (Kansal et al. [77]) which finally results in
decreasing degradation [76] . Therefore, the possibility of Se acting as additional
micronutrients for bacterial growth and ROS scavenging
5. Antibacterial Activities of Photocatalysts capability was explored. Inductively Coupled Plasma Mass
Spectrometry (ICP-MS) measurements on culture media
The antibacterial activities of ZnO and Ag-doped ZnO treated with Se-doped ZnO NPs revealed that 30% of the
suspensions of particles of different sizes around 17 nm and total Se content in the Se-doped ZnO NPs is released into the
12 nm towards Gram positive (M. leutus) and Gram negative media. The effect of Se content on the antibacterial activity
(K. pneumonia) bacteria were investigated in aqueous Luria was studied by spiking the equivalent Se concentration in the
broth (LB) by the well diffusion method [78]. The culture media pre-treated with pristine ZnO NPs. These
antibacterial activity increases with decreasing particle size; studies revealed that the Se release from the Se doped ZnO
this is due to greater penetrating ability and reactivity of NPs were used as micronutrients and they may also take part
smaller particles arising as a result of an increase in the in scavenging ROS from the culture media.
surface area to volume ratio of small sized particles. The
observed mean inhibition zones for ZnO are around 14 and Ag-doped ZnO [81] showed a much stronger antibacterial
18 mm against M. leutus. When Ag-doped ZnO nanorods activity on Gram-positive bacteria than on Gram-negative
were studied against the same bacteria and these values are bacteria. The difference in activity against these two types of
increased to 19 and 23 mm [78]. The observed antibacterial bacteria is explained as due to the presence of an outer
activity of NPs could either be a consequence of direct membrane covering the peptidoglycan layer in Gram
interaction with the microbial cells (e.g. interrupted trans negative bacteria. The antibacterial activities for S. aureus of
membrane electron transfer, disrupted/penetrated the cell Ag-doped ZnO powders were higher than for commercial
envelope and oxidized cell components)/due to secondary ZnO NPs [81].
products (e.g. reactive oxygen species (ROS)). The creation
of active species by photo-induced reaction is the main The antibacterial activity is suggested to be through the
source towards the bacterial toxicity in the case of metal - release of Zn2+ from the ZnO powders by mechanical
transition metal oxide compounds (MTMC). A possible destruction of the cell membrane by penetration of NPs
mechanism for the creation of active species has been put through the production of active oxygen species generated
forwarded by Padmavathy and Vijayaraghavan [79] who from the surface of ZnO. These reactive species may be
reported that holes produced when ZnO activated by white generated by photocatalytic reactions of ZnO under UV light.
lights split the H2O molecule from the suspension of ZnO
into hydroxyl radicals (OH-) and hydrogen ion (H+). The The antibacterial activity of sulphated cyclodextrin (sb-cd)
dissolved oxygen molecules are converted to superoxide cross linked cotton fabric treated with Ag, ZnO and TiO2
radical anions (∙O2-) which reacts with hydrogen ion (H+) and against Gram positive bacteria (S. aureus) and Gram negative
produce HO2∙ radicals. These hydroxyl radicals produce bacteria (E. coli) was carried out by Selvam et al. [82]. The
hydrogen peroxide anions HO2- which react with hydrogen to untreated cotton fabrics have no antibacterial effect. But sb-
produce H2O2 molecules. The generated H2O2 molecules cd cross linked fabric exhibited maximum of 85% reduction
penetrate the cell membrane and kill the bacteria [79]. for S. aureus and 78% reduction for E. coli. The sulfur and
nitrogen units in the sb-cd endow it with the antibacterial
NPs rendered an effective antibacterial agent when compared activity. 100% activity against both S. aureus and E. coli at
to pure ZnO [78]. Both the samples have strong antibacterial 30 min is exhibited by the sb-cd cross linked ZnO NPs
activity against both Gram negative and gram positive. coated fabric.
Similar results are observed on the antibacterial activity of
Ag doped ZnO NPs against E.coli by Venkatasubramanian The ZnO band gap is believed to play a role in the generation
and Sundaraj [80]. The inhibitory effect increases, as the of ROS. The generated ROS brings about oxidant injury to
concentration of ZnO NPs increases with Ag-doped ZnO NPs the surface of the membrane of the microorganism [83].
exhibiting much enhanced antibacterial activity compared to Because of its positive zeta potential, ZnO NPs rupture the
ZnO NPs. The studies were conducted on Ag doped ZnO cell membrane of E. coli (Gram negative) on contact and
NPs in different Ag concentrations. The results showed releases Zn2+ ions. This causes lysosomal and mitochondrial
increasing inhibition rate at both higher Ag concentrations damage which leads to the death of bacterial cells [25].
and catalyst concentrations.
Ramasami et al. also carried out antibacterial studies of ZnO–
Dutta et al [68] reported an anomalous behaviour in the TS (Tapioca starch) NPs against Gram negative bacteria K.
antibacterial activity of Se-doped ZnO NPs against E. coli. aerogenes, E. coli, P. aeruginosa and Gram positive bacteria
S. aureus using agar well diffusion method. The ZnO NPs
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showed activity against P. aeruginosa and S. aureus but not 6. Conclusion
against K. aerogenes and E. coli. [76].
Nanomaterials of metal and non metal doped, and
Ag/ZnO composites are synthesized by a solution method. nanocomposite of ZnO have been synthesized and studied by
Their antimicrobial activities under UV irradiation were many researchers. The as-synthesized nanomaterials were
tested as powders and after deposition on cotton and used for photo-degradation of organic pollutants in aqueous
cotton/polyester blended textile fabrics [84]. Whereas the media under UV, Visible and sun light irradiation. Doping of
untreated fabrics have no antibacterial activities, the non metals into ZnO modified the electronic absorption
antibacterial activity of Ag/ZnO NPs is found to increase properties ZnO. The band gap narrows thus, extending the
with increasing concentration of silver. Increasing optical absorption of ZnO into the visible light region. Non-
antimicrobial activity of NPs with Ag is attributed to an metal doping enabled ZnO to harvest more photons thereby
increase in active surface area with decreasing crystallite improving their photocatalytic activity. Metal-doped ZnO
size. shows an enhanced photocatalytic activity for degradation of
Sawai et al. [85] proposed the generation of hydrogen the organic pollutants possibly by facilitating the electron-
peroxide from the surface of ZnO as an effective means for hole separation. The photocatalytic activity of
the inhibition of bacterial growth. With decreasing particle nanocomposites of ZnO is also found to increase due to
size, the number of ZnO NPs per unit volume of the powder increased active sites.
increases and results in an increase the surface area and
increasing the generation of hydrogen peroxide. The The concentration of the dye and the amount of the
differences in the reactivity of cell walls of the two bacteria photocatalyst had an effect on the photocatalytic degradation
are submitted to the antimicrobial effect of Ag-ZnO NPs. The of the dyes. As the concentration of the dyes increased the
better antimicrobial activity against Gram positive M. luteus photocatalytic activity of the photocatalyst decreased. The
as compared to Gram negative E. coli is accounted by vast amount of data surveyed suggest that the antibacterial
considering the difference in the composition and structure of potential of modified ZnO and nanocomposite is higher than
the cell walls of Gram-positive and Gram-negative bacteria. the unmodified ZnO.
The cell wall of the Gram-negative bacteria consists of lipids,
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Review On The Photocatalytic Degradation of Dyes and Antibacterial Activities of Pure and Doped-Zno

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International Journal of Science and Research (IJSR)

ISSN (Online): 2319-7064

Review on the Photocatalytic Degradation of Dyes

Keywords: Photocatalyst, Degradation, antibacterial activity

1. Introduction defect sites of the photocatalysts are thought to be a main

Volume 4 Issue 7, July 2015

Volume 4 Issue 7, July 2015

The pH of the solutions thus, seems to affect the rate of

Sowbhagya and Ananda, [72] investigated the effect of

Volume 4 Issue 7, July 2015

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