|
|
In situ DRIFTS study of photocatalytic CO 2 reduction under UV irradiation |
Jeffrey C. S. WU,Chao-Wei HUANG, |
Department of Chemical
Engineering, Taiwan University, Taipei 10617, China; |
|
|
Abstract Photocatalytic reduction of CO2 on TiO2 and Cu/TiO2 photocatalysts was studied by in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) under UV irradiation. The photocatalysts were prepared by sol-gel method via controlled hydrolysis of titanium (IV) butoxide. Copper precursor was loaded onto TiO2 during sol-gel procedure. A large amount of adsorbed H2O and surface OH groups was detected at 25°C on the TiO2 photocatalyst after being treated at 500°C under air stream. Carbonate and bicarbonate were formed rapidly due to the reaction of CO2 with oxygen-vacancy and OH groups, respectively, on TiO2 surface upon CO2 adsorption. The IR spectra indicated that, under UV irradiation, gas-phase CO2 further combined with oxygen-vacancy and OH groups to produce more carbonate or bicarbonate. The weak signals of reaction intermediates were found on the IR spectra, which were due to the slow photocatalytic CO2 reduction on photocatalysts. Photogenerated electrons merge with H+ ions to form H atoms, which progressively reduce CO2 to form formic acid, dioxymethylene, formaldehyde and methoxy as observed in the IR spectra. The well-dispersed Cu, acting as the active site significantly increases the amount of formaldehyde and dioxymethylene, thus promotes the photoactivity of CO2 reduction on Cu/TiO2. A possible mechanism of the photocatalytic CO2 reduction is proposed based on these intermediates and products on the photocatalysts.
|
Issue Date: 05 June 2010
|
|
|
Tseng I H, Chang W-C, Wu J C S. Photoreduction of CO2 using sol-gel derived titania and titania-supported copper catalysts. Appl Catal B: Environm, 2002, 37(1): 37―48
doi: 10.1016/S0926-3373(01)00322-8
|
|
Ulagappan N, Frei H. MechanisticStudy of CO2 Photoreduction in Ti silicalitemolecular sieve by FT-IR spectroscopy. J Phys Chem A, 2000, 104(33): 7834―7839
doi: 10.1021/jp001470i
|
|
Bando K K, Sayama K, Kusama H, Okabe K, Arakawa H. In-situFT-IR study on CO2 hydrogenation over Cu catalystssupported on SiO2, Al2O3, and TiO2. Appl Catal A: Gen, 1997, 165(1―2): 391―409
doi: 10.1016/S0926-860X(97)00221-4
|
|
Yang R, Fu Y, Zhang Y, Tsubaki N. Insitu DRIFT study of low-temperature methanol synthesis mechanism onCu/ZnO catalysts from CO2-containing syngasusing ethanol promoter. J Catal, 2004, 228(1): 23―35
doi: 10.1016/j.jcat.2004.08.017
|
|
Schilke T C, Fisher I A, Bell A T. In situInfrared study ofmethanol synthesis from CO2/H2 on titania and zirconia promoted Cu/SiO2. J Catal, 1999, 184(1): 144―156
doi: 10.1006/jcat.1999.2434
|
|
Nomura N, Tagawa T, Goto S. In situ FTIR study on hydrogenationof carbon dioxide over titania-supported copper catalysts. Appl Catal A: Gen, 1998, 166(2): 321―326
doi: 10.1016/S0926-860X(97)00271-8
|
|
Wu J C S, Cheng Y-T. In situ FTIRstudy of photocatalytic NO reaction on photocatalysts under UV irradiation. J Catal, 2006, 237(2): 393―404
doi: 10.1016/j.jcat.2005.11.023
|
|
Tseng I H, Wu J C S, Chou H-Y. Effects of sol-gel procedures on thephotocatalysis of Cu/TiO2 in CO2 photoreduction. J Catal, 2004, 221(2): 432―440
doi: 10.1016/j.jcat.2003.09.002
|
|
Liao L F, Lien C F, Shieh D L, Chen M T, Lin J L. FTIR study of adsorptionand photoassisted oxygen isotopic exchange of carbon monoxide, carbondioxide, carbonate, and formate on TiO2. J Phys Chem B, 2002, 106(43): 11240―11245
doi: 10.1021/jp0211988
|
|
Anpo M, Aikawa N, Kubokawa Y. Photocatalytic hydrogenationof alkynes and alkenes with water over titanium dioxide. Platinumloading effect on the primary processes. J Phys Chem, 1984, 88(18): 3998―4000
doi: 10.1021/j150662a027
|
|
Inoue T, Fujishima A, Konishi S, Honda K. Photoelectrocatalytic reduction of carbon dioxide inaqueous suspensions of semiconductor powders. Nature, 1979, 277(5698): 637―638
doi: 10.1038/277637a0
|
|
Howe R F, Gratzel M. EPRstudy of hydrated anatase under UV irradiation. J Phys Chem, 1987, 91(14): 3906―3909
doi: 10.1021/j100298a035
|
|
Serpone N, Lawless D, Disdier J, Herrmann J-M. Spectroscopic, photoconductivity, and photocatalyticstudies of TiO2 colloids: naked and with thelattice doped with Cr3+, Fe3+, and V5+ cations. Langmuir, 1994, 10(3): 643―652
doi: 10.1021/la00015a010
|
|
Fujishima A, Rao T N, Tryk D A. Titanium dioxide photocatalysis. J Photochem Photobiol C: Photochem Rev, 2000, 1(1): 1―21
doi: 10.1016/S1389-5567(00)00002-2
|
|
Tseng I H, Wu J C S. Chemicalstates of metal-loaded titania in the photoreduction of CO2. Catal Today, 2004, 97(2―3): 113―119
doi: 10.1016/j.cattod.2004.03.063
|
|
Szczepankiewicz S H, Colussi A J, Hoffmann M R. Infrared spectra of photoinducedspecies on hydroxylated titania surfaces. J Phys Chem B, 2000, 104(42): 9842―9850
doi: 10.1021/jp0007890
|
|
Hadjiivanov K, Bushev V, Kantcheva M, Klissurski D. Infrared spectroscopy study of the species arising duringnitrogen dioxide adsorption on titania (anatase). Langmuir, 1994, 10(2): 464―471
doi: 10.1021/la00014a021
|
|
George B, Mclntyre P: In: Infrared Spectroscopy: Analytical Chemistry by Open Learning. John Wiley and Sons, London, 1988
|
|
Boccuzzi F, Chiorino A. FTIRStudy of carbon monoxide oxidation and scrambling at room temperatureover copper supported on ZnO and TiO2. 1. J Phys Chem, 1996, 100(9): 3617―3624
doi: 10.1021/jp950542g
|
|
RaskÛ J, KecskÈs T, Kiss J. Adsorption and reaction offormaldehyde on TiO2-supported Rh catalystsstudied by FTIR and mass spectrometry. J Catal, 2004, 226(1): 183―191
doi: 10.1016/j.jcat.2004.05.024
|
|
AraÒa J, MartÌnez Nieto J L, Herrera Melin JA, DoÒa RodrÌguez J M, Gonzlez DÌaz O, PÈrez PeÒa J, Bergasa O, Alvarez C, MÈndez J. Photocatalytic degradationof formaldehyde containing wastewater from veterinarian laboratories. Chemosphere, 2004, 55(6): 893―904
|
|
Boccuzzi F, Chiorino A, Manzoli M. FTIR study of methanol decompositionon gold catalyst for fuel cells. J PowerSources, 2003, 118(1―2): 304―310
doi: 10.1016/S0378-7753(03)00075-2
|
|
Popova G Y, Yu T V A, Chesalov A, Stoyanov E S. In situ FTIR study of the adsorption of formaldehyde, formic acid,and methyl formate at the surface of TiO2 (Anatase). Kinet Catal, 2000, 41: 805―811
doi: 10.1023/A:1026681321584
|
|
Boccuzzi F, Chiorino A, Manzoli M, Andreeva D, Tabakova T. FTIRstudy of the low-temperature water-gas shift reaction on Au/Fe2O3 and Au/TiO2 catalysts. J Catal, 1999, 188(1): 176―185
doi: 10.1006/jcat.1999.2636
|
|
AraÒa J, DoÒa-RodrÌguez J M, Cabo C G i, Gonz·lez-DÌaz O, Herrera-Melin J A, PÈrez-PeÒa J. FTIRstudy of gas-phase alcohols photocatalytic degradation with TiO2 and AC-TiO2. Appl Catal B: Environm, 2004, 53(4): 221―232
|
|
Rhodes M D, Pokrovski K A, Bell A T. The effects of zirconia morphologyon methanol synthesis from CO and H2 over Cu/ZrO2 catalysts: Part II. Transient-responseinfrared studies. J Catal, 2005, 233(1): 210―220
doi: 10.1016/j.jcat.2005.04.027
|
|
Chen M T, Lien C F, Liao L F, Lin J L. In-situ FTIR study of adsorption and photoreactions of CH2Cl2 on powdered TiO2. J Phys Chem B, 2003, 107(16): 3837―3843
doi: 10.1021/jp0220884
|
|
Wong G S, Kragten D D, Vohs J M. The oxidation of methanolto formaldehyde on TiO2 (110)-supported vanadiafilms. J Phys Chem B, 2001, 105(7): 1366―1373
doi: 10.1021/jp003691u
|
|
Viewed |
|
|
|
Full text
|
|
|
|
|
Abstract
|
|
|
|
|
Cited |
|
|
|
|
|
Shared |
|
|
|
|
|
Discussed |
|
|
|
|