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Renewable and Sustainable Energy Reviews: Ranjit K. Nath, M.F.M. Zain, M. Jamil
Renewable and Sustainable Energy Reviews: Ranjit K. Nath, M.F.M. Zain, M. Jamil
art ic l e i nf o a b s t r a c t
Article history: Photocatalyst is needed for cleaner environment and a better quality of life. This fact leads an idea of
Received 17 February 2015 more eco-compatible use of light. This approach could become an integral component of strategies to
Received in revised form reduce indoor air pollutants through the use of photocatalysts as construction materials. In this study, we
6 January 2016
discuss the quality of indoor air, sources of pollutants in the indoor environment, and the photocatalysis
Accepted 3 May 2016
process. Moreover, the different parameters and uses of different photocatalysts in concrete for indoor air
purification, starting from the early research until the current research, are described, and the reaction
Keywords: mechanism of photocatalytic oxidation and sustainable construction by using photocatalysts are also
Environment reviewed.
Indoor air
& 2016 Elsevier Ltd. All rights reserved.
Photocatalyst
Pollutants
Volatile Organic Compounds
Contents
1. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1185
2. Quality of indoor environment . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1185
3. Sources of pollutants and its impact . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1186
4. Indoor air purification technology . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1186
5. Photocatalysis . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1186
5.1. Background . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1187
5.2. Activation of photocatalyst . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1187
5.3. Selection of photocatalyst . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1188
6. Significance of photocatalysts in sustainable construction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1189
7. Photocatalytic degradation of pollutants . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1189
7.1. Reaction mechanisms . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1189
7.2. Factors impacts on photocatalytic oxidation process . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1190
7.2.1. Pollutant types . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1190
7.2.2. Chemical interaction and competition . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1190
7.2.3. Concentration of pollutants and flow rates . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1190
7.2.4. Effects of retention/residence time . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1190
7.2.5. Relative humidity. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1191
7.2.6. Effect of temperature. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1191
7.2.7. UV intensity and wavelength . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1191
7.2.8. Photocatalytic degeneration or regeneration . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1191
8. Influence of tropical climate on photocatalyst performance . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1192
9. Conclusion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1192
n
Corresponding author. Tel.: þ 8801817750388; fax: þ88031714910.
E-mail addresses: rkn_chem@yahoo.com, ranjitkumarnath@gmail.com (R.K. Nath), fauzi@vlsi.eng.ukm.my, fauzizain@gmail.com (M.F.M. Zain), mjamil.ukm@gmail.com,
lynyeeha@gmail.com (M. Jamil).
1
Tel.: þ60389213184; fax: þ 60389118315.
2
Tel.: þ60123120002; fax: þ6038911 8304.
http://dx.doi.org/10.1016/j.rser.2016.05.018
1364-0321/& 2016 Elsevier Ltd. All rights reserved.
R.K. Nath et al. / Renewable and Sustainable Energy Reviews 62 (2016) 1184–1194 1185
regarding sustainable construction using a photocatalyst for Excellent class Good class
indoor air purification, sources of pollutants in the indoor envir-
onment, photocatalysis process and provides an overview of the Room Temperature °C 20 to o 25.5 o 25.5
current developments in this field. Relative Humidity % 40 to o 70 o 70
Air movement m/s o 0.2 o 0.3
Carbon Dioxide (CO2) ppmv o 800 o 1000
Carbon Monoxide (CO) μg/m3 o 2000 o 10,000
2. Quality of indoor environment Respirable Suspended Particulates μg/m3 o 20 o 180
(PM10)
Nitrogen Dioxide (NO2) μg/m3 o 40 o 150
People generally spend the largest portion of their time Ozone (O3) μg/m3 o 50 o 120
indoors. Indoor environmental quality is a key aspect in the Formaldehyde (HCHO) μg/m3 o 30 o 100
evaluation of green buildings aiming to achieve sustainable Volatile Organic Compounds (VOC) μg/m3 o 200 o 600
Radon (Rn) Bq/m3 o 150 o 200
development in nonresidential buildings, such as commercial,
Airborne Bacteria cfu/m3 o 500 o 1000
institutional, and industrial structures. Therefore, the quality of
1186 R.K. Nath et al. / Renewable and Sustainable Energy Reviews 62 (2016) 1184–1194
separated by forbidding bands. The presence of a forbidden band from the VB to the CB and subsequently show pairs of electron–
immediately above the occupied allowed states is the principal hole particles. Photocatalysts such as TiO2, ZnO, CdS, GaP, SiC, WO3,
difference in the electronic structures of a metal and a photo- ZnS, and CdSe have been found to exhibit certain photocatalytic
catalyst or an insulator. In the latter two substances, a gap exists activities [32]. VB and CB positions for various photocatalysts are
between the valence band (VB) and the conduction band (CB). The shown in Fig. 3. In the photodegradation process of VOCs to pro-
presence of a gap means that the electrons cannot easily be duce CO2 and H2O, photocatalysts with conduction band positions
accelerated into higher energy states. The energy diagram of a at positive values (versus the normal hydrogen electrode) are
semiconductor photocatalyst interface is shown in Fig. 2. Con- unsuitable for VOC degradation. Therefore, Fe2O3 and SnO2 cannot
jugated systems possess a low energy gap between the highest be used for VOC removal. Photocatalysts containing band gap
occupied molecular orbital (HOMO) and lowest unoccupied energies of 3 or below are unable to oxidize most of VOCs. Thus,
molecular orbital (LUMO) that corresponds to the frequency of GaAs, GaP, CdSe, CdS, Fe2O3, WO3, and SiC are not preferable for
visible light. In insulators, the energy gap is markedly greater than VOC degradation. Only TiO2can be used for VOC degradation.
the probability of excitation of an electron from the VB to the CB, The activation of photocatalysts and corresponding reactions
which is extremely low. In metals, no gap exists between occupied on the photocatalyst surface can be described by the following six
and unoccupied states [48,49]. steps [50]:
Photocatalytic reactions occur at the interface between catalyst
and reaction medium under the condition of irradiation with i. Adsorption of photons with an energy that matches or is
waves with electromagnetic field from UV and visible range of the greater than its band gap energy of the semiconductor.
spectrum. The photocatalyst is a semiconductor with a band gap ii. Promotion of an electron (e ) from the VB to the CB, with
between 1.4 and 4.6 eV [48]. Incident photons with energy concomitant generation of a hole (h þ ) in the VB;
exceeding the band gap energy are absorbed, and electrons jump iii. e and h þ diffusion and migration to the surface where they
can react.
iv. Recombination of electron–hole pairs.
v. Stabilization of e and h þ at the surface to form a trapped
electron and a trapped hole, respectively.
vi. Reduction of a suitable electron accepter and oxidation of a
suitable electron donor.
Fig. 3. Valence and conductive band positions for various photocatlysts, E (Electric potential) and NHE (Normal Hydrogen Electrode potential).
R.K. Nath et al. / Renewable and Sustainable Energy Reviews 62 (2016) 1184–1194 1189
Neutralization of OH group into OH by the hole kinetics are continuously being undertaken. The reaction rates of
þ þ VOCs depend on the pollutant. In general, higher soluble com-
ðH 2 O 3 H þ OH Þads þ hvb -OH þH þ ð2:3Þ
pounds tend to possess higher reaction rates. Thus, the order of
The hydroxyl radical (OH) and superoxide radical (O2 ) conversion rates is as follows: alcohols and glycol
anions have been suggested to be the primary oxidizing species in ethers 4aldehydes, ketones, and terpene hydrocarbons4aromatic
photocatalytic oxidation processes. These oxidative reactions and alkane hydrocarbons4 halogenated aliphatic hydrocarbons
would result in degradation of pollutants,as shown in the fol- [76]. However, VOCs are also known to fully oxidize, and several
lowing Eqs. (2.4) and (2.5). less desirable intermediates may be exposed [76].
Oxidation of the organic pollutants via successive attack by
(OH) radicals 7.2.2. Chemical interaction and competition
As described in Section 7.1, different reaction schemes exist
R þ OH-R' þ H 2 O ð2:4Þ
through dependence on the pollutant, resulting in different rates
Or by direct reaction with holes of photocatalytic degradation. Numerous pollutants are known to
þ be photo-oxidizable. However, the interaction and competition of
R þ h -R þ -degradation products ð2:5Þ
other pollutants has yet to be completely understood. In the pre-
The chain reactions continue until the VOC is completely sence of other chemicals, simultaneous photocatalytic oxidation
mineralized to CO2and H2O. Several side reactions may also be reactions may inhibit or promote removal rates. Pollutants such as
induced to generate volatile compounds, accelerating the oxida- SOx and BTEX are known to inhibit degradation of other pollutants,
tion process. For oxidation reactions to occur, the VB must possess whereas NO2 can enhance degradation. BTEX and SOx are known
a higher oxidation potential than the material under consideration to inhibit the degradation of formaldehyde. Both BTEX and SOx
[43]. The redox potential of the VB and the CB for different interfere with formaldehyde degradation, decreasing conversion
semiconductors vary between þ 4.0 and 0.5 V versus the stan- by 10%. SO2, which is first absorbed into the TiO2 surface, inhibits
dard hydrogen electrode (SHE), respectively [68]. The VB and CB absorption of formaldehyde. Similarly, BTEX competes for
energies of LiNbO3 are estimated to be þ0.48 and 3.30 V, absorption with formaldehyde [77] and interferes with NOx
respectively. These findings indicate that the band gap energy of reduction [75]. By contrast, NOx enhances the photodegradation of
the material is 3.78 eV and it therefore absorbs in near UV light various pollutants. For example, NOx increases formaldehyde
(λ o339 nm) [69,70]. Most VOCs possess potentials above that of photodegradation rates by 5% at low humidity and as much as 25%
the LiNbO3VB and therefore can be oxidized [14]. at high humidity [77]. When BTEX combines with NOx photo-
oxidation, the largest enhancement in degradation was observed
7.2. Factors impacts on photocatalytic oxidation process in pollutants with low reaction rates, including ethyl benzene and
toluene [75].
Many environmental factors affect photooxidation efficiency.
Understanding these relationships is progressive and often varies 7.2.3. Concentration of pollutants and flow rates
by photocatalytic material, thus making comparisons difficult. Removal efficiency is a function of the quantity of pollutants
However, known environmental factors consist of pollutant types, and exposure periods [78]. In a previous research, flow rates varied
pollutant competition, pollution concentrations, air velocity, rela- from 1 L/min to 6 L/min [1,56,79,80]. In TiO2 on roof tiles, when
tive humidity, UV light intensity, and photocatalytic degeneration longer periods of gas residence are adopted with lower amounts of
and regeneration. toluene gas, removal efficiencies increase; experiments employing
shorter periods and higher concentrations of toluene show
7.2.1. Pollutant types decreased efficiency [81]. Similar results were obtained in
Numerous pollutants threaten our society in both indoor and experiments with indoor use of TiO2 oxidation of ethylene, for-
outdoor environments. Emissions from vehicle combustion maldehyde, toluene, 1-butene, BTEX, and NOx [15,75]. For example,
include NOx, SO2, CO, and VOCs, all of which threaten both human an increase in flow rate decreased the removal efficiency of
health and the environment. For example, NO and VOC pollutants toluene from 95% to 65% [82]. The explanation provided was that
are precursors to smog. Furthermore, NOx, CO2, and SO2are the an increase in flow tends to decrease the residence time with the
leading causes of acid rain, which not only destroys the environ- photocatalytic reactor, whereas an increase in concentration of
ment by killing and reducing the biodiversity of forests and lakes pollutants tends to increase the mass transfer rate and accumu-
but also degrades our buildings [56,71]. Outdoor air also impacts lation of final products [75,81]. Accumulation of oxidation pro-
indoor environments. Indoor environments can be contaminated ducts on the catalyst surface inhibits the continuous absorption of
by chemical, organic, and particulate pollutants that migrate from pollutants, potentially leading to deactivation of photocatalysis
outdoors or result from gas stoves and other indoor emission [75]. Thus, research points to the main use of TIO2for mall pollu-
sources, such as building materials, radon, and environmental tant loads, similar to those found in indoor and outdoor air [81].
tobacco smoke [72]. Climate change can affect these factors. For However, locating photocatalytic surfaces near pollutants is crucial
example, changes in the outdoor concentrations of a pollutant to ensure exposure [10].
because of alterations in atmospheric chemistry or atmospheric
circulation can affect indoor concentrations. Measures to reduce 7.2.4. Effects of retention/residence time
energy use in buildings, such as lowering ventilation rates, may Retention period is used to refer the complete period of time
cause higher exposure to pollutants emitted from indoor sou- and residence time is used to refer the period of time that set in
rces. NOx and VOCs are both associated with sick building Customizing. The retention period can be longer than the resi-
syndrome [73]. dence time and cannot be set in customizing. The effect of resi-
The photodegradation rates of each pollutant vary because of dence time has been widely studied together with the initial
different absorption rates and reaction schemes. For example, pollutant concentration. Similar to the effects of initial pollutant
VOCs, such as benzene, toluene, ethylbenzene, and xylene (BTEX), concentration, two opposite effects have been observed. The
show various photo-steady states and reaction rates [74,75]. As a influence of mass transfer performs a significant function in the
result, attempts to describe the ability of a photocatalyst to effect of residence time. When the reaction is mass transfer-con-
degrade pollutants through better understanding of chemical trolled, the degradation rate of reactants increases with decreasing
R.K. Nath et al. / Renewable and Sustainable Energy Reviews 62 (2016) 1184–1194 1191
residence time [83]. With further decreases in contact time, the degradation. For TiO2, wavelengths smaller than 400 nm, which
photo-degradation rate changes from mass transfer control to corresponds to the UV radiation from the sun are, required for
reaction kinetic control and can be described by the L–H model. In irradiation. Higher intensities result in more photons and, conse-
this case, the degradation rate increases with increasing residence quently, higher photocatalytic oxidation rates [15,43,94]. The
time [84,85]. relationship between intensity versus photocatalytic oxidation
rate often shows a linear correlation. The rate of increase is
7.2.5. Relative humidity dependent on the chemical pollutant. For example, when the
Water vapor possesses negative and positive impact. This irradiance is changed from 0 mW/cm2 to 1500 mW/cm2, a linear
finding is unexpected, since water is a key source of hydroxyl impact may be observed, and the oxidation activity of o-xylene
radicals [15,81]. The absence of water in several chemicals is and ethylbenzene increases drastically while that of benzene and
known to hinder their reaction rates, as commonly observed in toluene increase only gradually [93,95]. In addition, the photo-
toluene, ethyl benzene, and formaldehyde photocatalytic oxida- catalytic oxidation of trichloroethylene is enhanced from
tion. Surprisingly, water can also inhibit photocatalytic oxidation 0.08 10 6 mol/s gas to 0.25 10 6 mol/s gases as light intensity
rates. Researchers suggest that water particles compete with increases from 0.08 mW/cm2 to 0.45 mW/cm2 [15]. The increase in
adsorbed pollutant molecules [30,81]. Another hypothesis is that intensity not only increases activity rates but affects the formed
water forms one or more layers of film, which prevents the pol- intermediates by increasing the availability of free radicals that
lutant from reaching the TiO2 layer [82]. Thus, excessive water enhance the products. For example, in a previous study, more
interferes with reaction rates, and an optimum humidity condition intermediates were formed using germicidal lamps with hig-
may exist [30]. her intensities in comparison with lower intensities of black
Optimal humidity conditions have been identified for the lamps [95].
removal of formaldehyde. At low humidity, insufficient radicals are
present; at high humidity, competition impacts the amount of 7.2.8. Photocatalytic degeneration or regeneration
pollutants absorbed. Studies suggest that 55% relative humidity is Another highly debated variable of photocatalysis is the pos-
optimal for the removal of formaldehyde [73]. However, whether sible degeneration of photocatalytic properties, which may
an optimal relative humidity level exists has been questioned by necessitate restoration of the photocatalytic properties of TiO2
several studies [73,82]. For example, Sleiman's research on the [92,96]. As a catalyst that undergoes no change, TiO2 can theore-
photocatalytic oxidation of toluene oxidation did not show an tically be used indefinitely [92]. Thus, degeneration is caused by
optimum relative humidity [82]. In addition, several pollutants, other factors, such as interference of absorbed intermediates and
such as trichloroethylene, exhibit only negative impacts when decreases in catalytic surface from the buildup of dirt, scum, gum,
water content is increased [15]. A second study on the reduction of oil, and grease, especially if used in outdoor environments [15,80].
formaldehyde did not find an optimal humidity level; instead, As such, removal of these absorbed products can induce regen-
conversion decreased from 80% to 54% when humidity was eration of photooxidation efficiency.
increased from 2100 pmv to 22,000 pmv [77]. When the same In an indoor experiment on the removal efficiencies of toluene
humidity increase is tested for toluene removal, the removal effi- and TiO2, degeneration was not detected after over 48 h of testing,
ciency decreased from 72% to 19%. These discrepancies indicate despite previous research findings on the deactivation of TiO2 and
that the impact of humidity is difficult to describe. Impact may even a slight, yellowish color change because of the accumulation
differ by pollutant type, concentration, and other possible of absorbed species from photocatalytic oxidation of toluene
experimental factors [75]. [81,97]. Therefore, research suggests that degeneration and accu-
mulation of products may be a function of time and concentration
7.2.6. Effect of temperature of pollutants present [82,98]. This concept may explain why Slei-
Temperature has been proven to be an important aspect in the man, who used considerably lower concentrations in 120 ppb
study of photocatalysis. Photocatalysis is activated by photons, and versus 290 ppb, did not observe degeneration effects [82]. Today,
photocatalytic reactions can operate at room temperature and are methods for regeneration are continuously being investigated.
relatively insensitive to temperature changes [23]. The literature Regeneration theories include washing surfaces with water to
shows that reaction rates are typically the highest for reactor simulate rain, blowing air, or surface burning [10,99]. Comparisons
temperature between 20 and 80 °C, whereas reaction rates gen- between regeneration methods have quickly eliminated air as a
erally decrease above 80 °C [86]. Water adsorbed on the surface of solution. For example, when flushed with clean air, TiO2 on roof
a semiconductor extensively performs a critical function in tiles does not show any change in its photocatalytic properties;
surface-mediated photocatalytic reactions, trapping VB holes and however, natural rain simulation showed 42% regeneration
forming hydroxyl radicals [87,88]. As the reactor temperature [81,100,101]. To test water theory, Beeldens et al. [10] removed
exceeds 80 °C and approaches the boiling point of water, loss of photocatalytic blocks from laboratory and field tests. The blocks
water on the material surface may limit photocatalytic reaction for laboratory tests were removed over several periods of time to
[89]. Furthermore, conventional hereterogenous catalytic reactions represent different exposure levels, and photocatalytic efficiencies
may occur at elevated temperatures, depending on the reacting were recorded before and after surface washing. The results
species and the catalyst [90]. Therefore, the effect of temperature demonstrated that additional washing could significantly improve
on a given photocatalytic reaction is highly dependent on the photocatalytic efficiency and maintain durability [10,102]. When
organic contaminant, intermediates, and build-up potential of the tested in outdoor environments, rainfall can help regenerate
catalyst surface. photocatalytic activities, offering results similar to those of
laboratory washing. Thus, several researchers recommend that
7.2.7. UV intensity and wavelength washing should be performed at least once every two months
Evidently, TiO2 requires light as an energy provider to function during the dry season [80,103]. However, water washing or rain is
and degrade pollutants. Several experiments show that photo- ineffective for eliminating adhesives and water-insoluble con-
degradation does not occur in the absence of light [56,73,91,92]. taminants. Thus, the use of a degreasing agent may be beneficial.
Changing the light source impacts the wavelength and photon Exposure to different contaminants depends on location, which
flux. The wavelength is primarily responsible for photocatalytic demonstrates that exposure to such contaminants can be con-
activity, whereas intensity or photon flux impacts the rate of trolled by locality [3]. Other proposed solutions from Zhao include
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