Elucidating the photocatalytic degradation pathway of acetaldehyde: An FTIR in situ study under atmospheric conditions

Hauchecorne, Birger; Terrens, Dieter; Verbruggen, Sammy W.; Martens, Johan A.; Langenhove, Herman Van; Demeestere, Kristof; Lenaerts, Silvia

doi:10.1016/j.apcatb.2011.06.026

Cited by 98 publications

(86 citation statements)

References 51 publications

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“…It is observed that the strong peak at 1693 cm -1 decreases in intensity during purging of the reaction cell with synthetic air, while the intensity of the broad peak at 1653 cm -1 increases and a new band appears at 1628 cm -1 . The latter two bands are assigned to the (C=O) and (C=C) vibrations of crotonaldehyde and show that aldehyde condensation occurs on anatase TiO 2 at room temperature, which is consistent with results of previous studies [31,32]. The band observed at 1168 cm -1 can be assigned to the C-C vibration mode in either of the aldehyde species.…”

Section: In Situ Ftir Spectroscopysupporting

confidence: 80%

“…Experiments conducted under ultrahigh vacuum conditions on rutile single crystals show that photo-fragmentation of acetaldehyde leads to cleavage of the C-C bond and release of a CH 3 • radical [11]. This is consistent with formate formation under atmospheric conditions, since it is expected that CH 3 • radicals will be re-adsorbed on the surface to form methoxy groups and subsequently converted to formate species [31]. Other reported intermediates are acetic acid and formaldehyde as well as different condensation products such as 3-hydroxybutanal and crotonaldehyde [13,38].…”

Section: Surface Reaction Kinetics On Tiosupporting

confidence: 52%

“…However, the crotonaldehyde coverage can also decrease via other reactions, for example through oxidation to formaldehyde or acetic acid [13,31,38]. Even though the latter represent minority surface reaction pathways, meaning that no major IR peaks associated with these species are observed in the experiments, they are nevertheless included in the model to account for mass balance and possible desorption.…”

mentioning

confidence: 99%

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Adsorption and photo-oxidation of acetaldehyde on TiO2 and sulfate-modified TiO2: Studies by in situ FTIR spectroscopy and micro-kinetic modeling

Topalian

Stefanov

Granqvist

et al. 2013

Journal of Catalysis

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Adsorption and photocatalytic oxidation of acetaldehyde have been investigated on TiO 2 and sulphate-modified TiO 2 films (denoted SO 4 -TiO 2 ). In situ Fourier transform infrared spectroscopy was used to study surface reactions as a function of time and number of experimental cycles. Spectral analysis and micro-kinetic modelling show that crotonaldehyde formation occurs spontaneously on TiO 2 but is impeded on SO 4 -TiO 2 , where instead acetaldehyde desorption is significant. Photo-oxidation yields significant amounts of formate on TiO 2 , and was identified as the rate-determining step and associated with site blocking.Significantly smaller amounts of formate were observed on SO 4 -TiO 2 , which is due to the acidity of this surface resulting in weaker bonding of aldehyde and carboxylate intermediate species. Our results are of considerable interest for applications to photocatalytic air purification and to surfaces with controlled wettability.

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Section: In Situ Ftir Spectroscopysupporting

confidence: 80%

Section: Surface Reaction Kinetics On Tiosupporting

confidence: 52%

mentioning

confidence: 99%

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Adsorption and photo-oxidation of acetaldehyde on TiO2 and sulfate-modified TiO2: Studies by in situ FTIR spectroscopy and micro-kinetic modeling

Topalian

Stefanov

Granqvist

et al. 2013

Journal of Catalysis

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“…The photocatalytic degradation of acetaldehyde was carried out in the gas phase over titania (Aerolyst 7710) by means of an in-house constructed FTIR in situ photoreactor by Hauchecorne et al [32]. Adsorption of acetaldehyde leads already to partial formation of 3-hydroxybutanal located at 1656 (υ(C=O)), 1445 (δ as (CH 3 )), 1426 (δ s (CH 3 )), 1343 (δ(CH)), and 1257 cm −1 (δ(COH)) and crotonaldehyde (1653 (υC=O)), 1625 (υ(C=C)), 1444 (δ as (CH 3 )), and 1377 cm −1 (δ s (CH 3 )) ( Figure 4.6).…”

Section: Oxidation Of Oxygen-containing Compoundsmentioning

confidence: 99%

“…FTIR spectra reveal different structured intermediate adsorbates. The reaction pathway is illustrated in Figure 4.7 [32]. Hernández-Alonso et al [33] used Operando FTIR spectroscopy to investigate the photocatalytic oxidation of acetone vapors over semiconductor films containing TiO 2 , mixed TiO 2 -ZrO 2 , and Zr-doped TiO 2 .…”

Section: Oxidation Of Oxygen-containing Compoundsmentioning

confidence: 99%

In Situ Studies on Photocatalytic Materials, Surface Intermediates, and Reaction Mechanisms

Kosslick

Tuấn

Bahnemann

2013

Heterogeneous Catalysts for Clean Technology

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IntroductionIncreasing industrialization, worldwide population growth, and urbanization lead to a rapidly growing demand for clean water. Shortage of water resources combined with increasing contamination of water from industry, agriculture, and households requires the development of efficient technology for clean water supplies [1][2][3][4]. Photocatalysis with heterogeneous catalysts is an attractive technology of great potential for remediation of polluted water. It requires no additional chemicals and may operate with sunlight with the catalysts easily recovered and reused. However, this technology still suffers from some severe shortcomings such as low efficiency, quantum yield, use of energy by limited use of the spectral range of light, and rapid deactivation. The development of advanced photocatalysts by rational design requires an improved understanding of underlying processes regarding charge separation and transfer in the photosemiconductors, the formation of intermediates, reaction mechanisms, and proceeding deactivation processes. Despite the huge number of photocatalytic investigations, these problems remained unsolved. Common investigation methods are performed under ''ideal'' conditions in order to avoid interferences in analysis and focus on main products. In situ investigations are a key to improve the understanding of the basics of heterogeneous photocatalytic processes markedly. This contribution focuses, therefore, on in situ investigations of heterogeneous photocatalytic systems for oxidative depollution of water or related selective oxidation of organics. So far, Fourier transform infrared (FTIR) and electron paramagnetic resonance (EPR) techniques play an important role both because of the achieved experimental level and added value of information about the nature of formed surface intermediates and reaction products as well as on charge separation and electron and hole formation/transfer and nature of active sites and reactive radicals present or formed during the photocatalytic reaction. Electrochemical methods for photocatalyst characterization are not included. The application of surface science methods for photocatalyst characterization [5] and new materials for heterogeneous water splitting have been reviewed in detail recently [6]. Background information achieved with common methods regarding Heterogeneous Catalysts for Clean Technology: Spectroscopy, Design, and Monitoring, First Edition. Edited

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3D Hierarchical ZnIn₂S₄ Nanosheets with Rich Zn Vacancies Boosting Photocatalytic CO₂ Reduction

Rao

Song

et al. 2019

Adv Funct Materials

325

142

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Zinc vacancy (VZn) is successfully introduced into 3D hierarchical ZnIn2S4 (3D‐ZIS). The photo‐electrochemical experiments demonstrate that the charge separation and carrier transfer are more efficient in the 3D‐ZIS with rich VZn. Of note, for the first time, it is found that VZn can decrease the carrier transport activation energy (CTAE), from 1.14 eV for Bulk‐ZIS (Bulk ZnIn2S4) to 0.93 eV for 3D‐ZIS, which may provide a feasible platform for further understanding the mechanism of photocatalytic CO2 reduction. In situ Fourier transform infrared (FT‐IR) results reveal that the presence of rich VZn ensures CO2 chemical activation, promoting single‐electron reduction of CO2 to CO2−. In addition, in situ FT‐IR and CO2 temperature programmed desorption results show that VZn can promote the formation of surface hydroxyl. To the best of current knowledge, there are no reports on the photoreduction of CO2 simply by virtue of 3D‐ZIS with VZn and few literature reports on the photocatalytic reduction of CO2 concerned with CTAE. Additionally, this work finds that surface hydroxyl may play a crucial role in the process of CO2 photoreduction. The work may provide some novel ways to ameliorate solar energy conversion performance and a better understanding of photoreaction mechanisms.

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Elucidating the photocatalytic degradation pathway of acetaldehyde: An FTIR in situ study under atmospheric conditions

Cited by 98 publications

References 51 publications

Adsorption and photo-oxidation of acetaldehyde on TiO2 and sulfate-modified TiO2: Studies by in situ FTIR spectroscopy and micro-kinetic modeling

Adsorption and photo-oxidation of acetaldehyde on TiO2 and sulfate-modified TiO2: Studies by in situ FTIR spectroscopy and micro-kinetic modeling

In Situ Studies on Photocatalytic Materials, Surface Intermediates, and Reaction Mechanisms

3D Hierarchical ZnIn₂S₄ Nanosheets with Rich Zn Vacancies Boosting Photocatalytic CO₂ Reduction

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Elucidating the photocatalytic degradation pathway of acetaldehyde: An FTIR in situ study under atmospheric conditions

Cited by 98 publications

References 51 publications

Adsorption and photo-oxidation of acetaldehyde on TiO2 and sulfate-modified TiO2: Studies by in situ FTIR spectroscopy and micro-kinetic modeling

Adsorption and photo-oxidation of acetaldehyde on TiO2 and sulfate-modified TiO2: Studies by in situ FTIR spectroscopy and micro-kinetic modeling

In Situ Studies on Photocatalytic Materials, Surface Intermediates, and Reaction Mechanisms

3D Hierarchical ZnIn2S4 Nanosheets with Rich Zn Vacancies Boosting Photocatalytic CO2 Reduction

Contact Info

Product

Resources

About

3D Hierarchical ZnIn₂S₄ Nanosheets with Rich Zn Vacancies Boosting Photocatalytic CO₂ Reduction