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Photodegradation Efficiencies in a Photo-CREC Water-II Reactor Using Several TiO2 Based Catalysts

  • Benito Serrano Rosales , Jesus Moreira del Rio , Jesus Fabricio Guayaquil und Hugo de Lasa EMAIL logo
Veröffentlicht/Copyright: 14. Mai 2016
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International Journal of Chemical Reactor Engineering
Aus der Zeitschrift International Journal of Chemical Reactor Engineering Band 14 Heft 3

Abstract

This study reports phenol degradation using several TiO2 photocatalysts (DP25, Anatase 1, Hombikat UV-100, Anatase 2) in a Photo-CREC Water-II Reactor. The physicochemical properties of the photocatalysts used, such as crystallinity, superficial area, and pore size distribution are reported. Reactor efficiencies are calculated using both Quantum Yields (QYs) and Photochemical and Thermodynamic Efficiency Factors (PTEFs). This is accomplished using phenol and phenol intermediate photoconversion rates. This allows the determination of hydroxyl radical consumption rates, at every step of the photodegradation process. With these data, and with the absorbed photon rates, energy efficiencies are calculated. It is shown that for the best performing photo catalysts the maximum QYs reach 50 % levels. These favourable photoconversion efficiencies confirm the critical importance of having available highly performing photocatalysts and photoreactors, such is the case of Photo-CREC Water-II Reactor unit.

Keywords: heterogeneous photocatalysis; reactor efficiency; phenol; OH radicals; photons; water

Notation

CiConcentration of i Species,μmole m–3 or ppmC
Ci,e.Concentration of i Species at Equilibrium,μmole m–3 or ppmC
ki→kkinetic constant associated with the species “i” being converted in species “k”s–1
KiAdsorption Constant for i Species,m3 μmole–1
Ki*Dimensionless Adsorption Constant or “i” Species-
Ni,adsAdsorbed “i” speciesμmole
Ni,L“i” species in the liquid phaseμmole
Ni,TTotal “i” species distributed in liquid and sorbed phasesμmole
qiConcentration of “i” species in solid phaseμmole g–1
qi,eConcentration of “i” species in solid phase at equilibriumμmole g–1
qi,mMaximum concentration of “i” species in solid phaseμmole g–1
QabsRate of Irradiated Energy Absorbed in a Photocatalytic Reactor,W
QusedRate of Irradiated Energy Used to Form OH• Radicals,W
riReaction rate of Component iμmole gcatirr–1 s–1
ri,jRate of Component i in reaction Step j,μmole gcatirr–1 s–1
rOH∙,TTotal Rate of OH• radicals consumed per unit weight of irradiated catalyst,μmole gcatirr–1 s–1
rOH∙,jRate of OH• radicals consumption in reaction Step j,μmole gcatirr–1 s–1
RkRate of Photoconversion in Step kμmole gcatirr–1 s–1
tIrradiation Timemin
VTotal Reactor Volumem3
W
WirrWeight of Irradiated Photocatalystg
Greek symbols
ΔHOH∙Enthalpy of Formation of an OH• GroupJ mol–1
γFraction of Irradiated Energy with a Wavelength Smaller than 388 nm-
ηOH∙Fraction of Photon Energy Used in Forming an OH• Radical-,
ν0H,jStoichiometric coefficient for the consumption of OH• Radical in step “j”-
νi,jStoichiometric coefficient for the consumption of i species in step “j”-
Acronyms
LVRPALocal Volumetric Rate of Photon Absorption
OH•Hydroxyl Radicals
ppmCgCarbon/g of solution × 106
QYQuantum Yield
QYavAverage Quantum Yield
PTEFPhotochemical Thermodynamic Efficiency Factor
PTEFavAverage Photochemical Thermodynamic Efficiency Factor

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Appendix I. Adsorption constants for the various photocatalysts

Table 4:

Adsorption constants and maximal quantities of several chemical species absorbed on different TiO2 catalysts (Moreira et al., 2012).

CatalystPhenolHydroquinoneCatecholAcetic acid
KiACIKACIKACIKACI
DP250.1070.0310.0950.0450.1390.0670.0210.018
Anatase 10.1710.0590.2400.1300.1560.1340.1680.143
Hombikat UV-1000.1570.0670.1380.0750.2030.1410.0580.019
Anatase 20.2480.1180.3390.1430.2330.0560.0770.027
qi,max,iCIqmaxCIqmaxCIqmaxCI
DP251.9910.2001.6970.3091.1320.1590.4320.280
Anatase 11.8880.1621.8140.1870.4580.1060.0700.015
Hombikat UV-1000.7840.0890.0720.1080.1530.0230.0930.016
Anatase 21.3240.1961.1740.0700.5280.0250.1730.027
[1]

From the results reported in Table 4, it can be concluded that KA chemical species adsorption constants for the different TiO2 catalysts studied, followed the sequence: phenol adsorption > hydroquinone adsorption > catechol adsorption > acetic acid adsorption. This same trend applies to the qi,max, the maximum “i” chemical species adsorbed amount per unit catalyst weight.

Appendix II. Accounting total changes of chemical species

For phenol, a Langmuir isotherm can be considered as follows:

(40)qph=KphqmphCph1+KphCph+Ko−DHBCo−DHB+Kp−DHBCp−DHB+KacCac

In addition, for catechol (o-DHB), hydroquinone (p-DHB) and carboxylic acids, the following equation can be postulated:

(41)qo−DHB=Ko−DHBqmo−DHBCo−DHB1+KphCph+Ko−DHBCo−DHB+Kp−DHBCp−DHB+KacCac
(42)qp−DHB=Kp−DHBqmp−DHBCp−DHB1+KphCph+Ko−DHBCo−DHB+Kp−DHBCp−DHB+KacCac
(43)qac=KacqmacCac1+KphCph+Ko−DHBCo−DHB+Kp−DHBCp−DHB+KacCac

The total derivative for phenol is then:

(44)dqphdt=∂qph∂CphdCphdt+∂qph∂Co−DHBdCo−DHBdt+∂qph∂Cp−DHBdCp−DHBdt+∂qph∂CacdCacdt

Using the eq. (6) for phenol, and substituting this into eq. (47):

(45)dCph,Tdt=dCphdt+WV{∂qph∂CphdCphdt+∂qph∂Co−DHBdCo−DHBdt+∂qph∂Cp−DHBdCp−DHBdt+∂qph∂CacdCacdt}

Furthermore, when evaluating the partial derivatives involved in eq. (45), the results can be expressed as:

(46)∂qph∂Cph=Kphqmph+Ko−DHBKphqmphCo−DHB+Kp−DHBKphqmphCp−DHB+KacKphqmphCac(1+KphCph+Ko−DHBCo−DHB+Kp−DHBCp−DHB+KacCac)2
(47)∂qph∂Co−DHB=−Ko−DHBKphqmphCph1+KphCph+Ko−DHBCo−DHB+Kp−DHBCp−DHB+KacCac2
(48)∂qph∂Cp−DHB=−Kp−DHBKphqmphCph1+KphCph+Ko−DHBCo−DHB+Kp−DHBCp−DHB+KacCac2
(49)∂qph∂Cac=−KacKphqmphCph(1+KphCph+Ko−DHBCo−DHB+Kp−DHBCp−DHB+KacCac)2

Replacing eq. (46) into (49) in eq. (45), the following is obtained,

(50)dCph,Tdt=dCphdt1+Kph∗

With

(51)Kph∗=WVKphqmph+Ko−DHBKphqmphCo−DHB+Kp−DHBKphqmphCp−DHB+KacKphqmphCac1+KphCph+Ko−DHBCo−DHB+Kp−DHBCp−DHB+KacCac2+−Ko−DHBKphqmphCph1+KphCph+Ko−DHBCo−DHB+Kp−DHBCp−DHB+KacCac2dCo−DHBdCph+−Kp−DHBKphqmphCph1+KphCph+Ko−DHBCo−DHB+Kp−DHBCp−DHB+KacCac2dCp−DHBdCph+−KacKphqmphCph1+KphCph+Ko−DHBCo−DHB+Kp−DHBCp−DHB+KacCac2dCacdCph

This expression accounts for the adsorption of phenol and its intermediates, during the reaction process. A similar process calculation can be used for the other species (o-di-hydroxyphenol, p-di-hydroxyphenol, carboxylic acids) as reported by Serrano et al. (2009)

Appendix III. PTEF definition accounting for adsorbed species

(52)rOH•,T=[4rph,1+2rph,2+2rph,3+28rph,4+0+2rp−DHB,6+26rp−DHB,7+8rac,8]
(53)rOH,T=−VWirr+4dCph,1dt1+Kph∗+2dCph,2dt1+Kph∗+2dCph,3dt1+Kph∗+28dCph,4dt1+Kph∗+2dCp−DHB,6dt1+Kp−DHB∗+26dCp−DHB,7dt1+Kp−DHB∗+8dCac,8dt1+Kac∗

Note that the change of concentrations can be considered to display a Langmuir-Hinselwood form as follows:

(54)dCi,jdt=νi,jkiCi1+KphCph+Ko−DHBCo−DHB+Kp−DHBCp−DHB+KphCph

Replacing eq. (54) in eq. (14), results in the following:

(55)rOH∙,T=−VWirr4kph−AcCph1+Kph∗+2kph−oDHBCph1+Kph∗+2kph−pDHBCph1+Kph∗+28kph−CO2Cph1+Kph∗+2kpDHB−AcCp−DHB1+KpDHB∗+26kpDHB−CO2Cp−DHB1+KpDHB∗+8kAc−CO2CAc1+KAc∗1+KphCph+Ko−DHBCo−DHB+Kp−DHBCp−DHB+KacCac

Furthermore, substituting eq. (55) into the PTEF equation yields the following:

(56)PTEF=−rOH∙ΔHOH∙WirrQabs=((4kph−ac+2kph−o−DHB+2kph−p−DHB+28kph−CO2)Cph(1+Kph∗)+(2kp−DHB−ac+26kp−DHB−CO2)Cp−DHB(1+Kp−DHB∗)+8kac−CO2CAc(1+KAc∗))/(1+KphCph+Kpho−DHBCo−DHB+Kp−DHBCp−DHB+KAcCAc)ΔHOH∙VQabs

Appendix IV. Estimated ki kinetic parameters

Table 5:

Estimated kinetic parameter ki for DP25 in 1/s.

ParameterSymbolValue95 % CI
kph−Ack11.007 × 10–33.848 × 10–4
kph−oDHBk21.483 × 10–36.931 × 10–4
kph−pDHBk33.610 × 10–38.697 × 10–4
kph−CO2k44.189 × 10–34.641 × 10–4
koDHB−pDHBk51.595 × 10–29.040 × 10–3
koDHB−Ack69.417 × 10–4N/A
kpDHB−CO2k71.273 × 10–21.954 × 10–3
kAc−CO2k87.840 × 10–33.190 × 10–3
Table 6:

Estimated kinetic parameter ki for Anatase 1 in 1/s.

ParameterSymbolValue95 % CI
kph−oDHBk11.004 × 10–21.722 × 10–3
kph−pDHBk28.503 × 10–31.642 × 10–3
kph−CO2k34.907 × 10–35.274 × 10–4
koDHB−Ack44.508 × 10–29.268 × 10–3
kpDHB−Ack52.135 × 10–25.098 × 10–3
kAc−CO2k64.546 × 10–34.318 × 10–4
Table 7:

Estimated kinetic parameter ki for Hombikat UV-100 in 1/s.

ParameterSymbolValue95 % CI
kph−BQk11.134 × 10–34.774 × 10–4
kph−pDHBk21.622 × 10–35.616 × 10–4
kph−CO2k35.844 × 10–32.411 × 10–4
kBQ−pDHBk41.870 × 10–29.584 × 10–3
kpDHB−Ack51.487 × 10–22.060 × 10–3
kAc−CO2k64.381 × 10–21.325 × 10–2
Table 8:

Estimated kinetic parameter ki for Anatase 2.

ParameterSymbolValue95 % CI
kph−oDHBk12.656 × 10–31.023 × 10–3
kph−pDHBk28.319 × 10–31.205 × 10–3
kph−CO2k39.202 × 10–36.635 × 10–4
koDHB−pDHBk42.734 × 10–21.316 × 10–2
kpDHB−Ack58.918 × 10–32.070 × 10–3
kpDHB−CO2k61.231 × 10–23.284 × 10–3
kAc−CO2k71.395 × 10–24.455 × 10–3
Published Online: 2016-5-14
Published in Print: 2016-6-1

©2016 by De Gruyter

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  12. Staggered Grid Finite Volume Approach for Modeling Single Particle Char Gasification
  13. High Efficiency CeCu Composite Oxide Catalysts Improved via Preparation Methods for Propyl Acetate Catalytic Combustion in Air
  14. Hydrodesulfurization of Dibenzothiophene in a Micro Trickle Bed Catalytic Reactor under Operating Conditions from Reactive Distillation
  15. Surface Modification of the ZnO Nanoparticles with γ-Aminopropyltriethoxysilane and Study of Their Photocatalytic Activity, Optical Properties and Antibacterial Activities
  16. One-Pot Isomerization of n-Alkanes by Super Acidic Solids: Sulfated Aluminum-Zirconium Binary Oxides
  17. Photocatalytic Decomposition of Metoprolol and Its Intermediate Organic Reaction Products: Kinetics and Degradation Pathway
https://doi.org/10.1515/ijcre-2016-0024
Schlagwörter für diesen Artikel
heterogeneous photocatalysis; reactor efficiency; phenol; OH radicals; photons; water

Artikel in diesem Heft

  1. Frontmatter
  2. Editorial
  3. In Honour of Professor Serge Kaliaguine
  4. Research Articles
  5. Core/Shell Nanostructured Materials for Sustainable Processes
  6. Photodegradation Efficiencies in a Photo-CREC Water-II Reactor Using Several TiO2 Based Catalysts
  7. Hydrotreatment of Light Cycle Oil Over a Dispersed MoS2 Catalyst
  8. Hybrid Ionic Liquid-Chitosan Membranes for CO2 Separation: Mechanical and Thermal Behavior
  9. Photo-oxidation of Tributyltin, Dibutyltin and Monobutyltin in Water and Marine Sediments
  10. Contribution of Pd Membrane to Dehydrogenation of Isobutane Over a New Mesoporous Cr/MCM-41 Catalyst
  11. Self Diffusivity of n-Dodecane and Benzothiophene in ZSM-5 Zeolites. Its Significance for a New Catalytic Light Diesel Desulfurization Process
  12. Staggered Grid Finite Volume Approach for Modeling Single Particle Char Gasification
  13. High Efficiency CeCu Composite Oxide Catalysts Improved via Preparation Methods for Propyl Acetate Catalytic Combustion in Air
  14. Hydrodesulfurization of Dibenzothiophene in a Micro Trickle Bed Catalytic Reactor under Operating Conditions from Reactive Distillation
  15. Surface Modification of the ZnO Nanoparticles with γ-Aminopropyltriethoxysilane and Study of Their Photocatalytic Activity, Optical Properties and Antibacterial Activities
  16. One-Pot Isomerization of n-Alkanes by Super Acidic Solids: Sulfated Aluminum-Zirconium Binary Oxides
  17. Photocatalytic Decomposition of Metoprolol and Its Intermediate Organic Reaction Products: Kinetics and Degradation Pathway
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