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Efficient Photocatalytic Decomposition of Perfluorooctanoic Acid by Indium Oxide and Its Mechanism

Identifieur interne : 001D28 ( Main/Repository ); précédent : 001D27; suivant : 001D29

Efficient Photocatalytic Decomposition of Perfluorooctanoic Acid by Indium Oxide and Its Mechanism

Auteurs : RBID : Pascal:13-0090637

Descripteurs français

Pascal (Inist)
- Photocatalyse, Oxyde d'indium, Oxyde de titane, Rayonnement UV, Spectrométrie FTIR, Spectrométrie réflexion, Epuration eau usée, Epuration physicochimique, Traitement eau, Mécanisme réaction, Cinétique chimique, Spectrométrie RPE, Spectrométrie RMN, Dégradation photochimique, Acide carboxylique, Fluor composé organique, Acide perfluorooctanoïque, Polluant émergent.

English descriptors

KwdEn :
- Carboxylic acid, Chemical reaction kinetics, EPR spectrometry, Emerging contaminant, Fourier-transformed infrared spectrometry, Indium oxide, NMR spectrometry, Organic fluorine compounds, Perfluorooctanoic acid, Photocatalysis, Photochemical degradation, Physicochemical purification, Reaction mechanism, Reflection spectrometry, Titanium oxide, Ultraviolet radiation, Waste water purification, Water treatment.

Abstract

Perfluorooctanoic acid (C₇F₁₅COOH, PFOA) has increasingly attracted worldwide concerns due to its global occurrence and resistance to most conventional treatment processes. Though TiO₂-based photocatalysis is strong enough to decompose most organics, it is not effective for PFOA decomposition. We first find that indium oxide (In₂O₃) possesses significant activity for PFOA decomposition under UV irradiation, with the rate constant about 8.4 times higher than that by TiO₂. The major intermediates of PFOA were C₂-C₇ shorter-chain perfluorocarboxylic acids, implying that the reaction proceeded in a stepwise manner. By using diffuse reflectance infrared Fourier transform spectroscopy, ¹⁹F magic angle spinning nuclear magnetic resonance, and electron spin resonance, we demonstrate that the terminal carboxylate group of PFOA molecule tightly coordinates to the In₂O₃ surface in a bidentate or bridging configuration, which is beneficial for PFOA to be directly decomposed by photogenerated holes of In₂O₃ under UV irradiation, while PFOA coordinates to TiO₂ in a monodentate mode, and photogenerated holes of TiO₂ preferentially transform to hydroxyl radicals, which are inert to react with PFOA. PFOA decomposition in wastewater was inhibited by bicarbonate and other organic matters; however, their adverse impacts can be mostly avoided via pH adjustment and ozone addition.

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Pascal:13-0090637

Le document en format XML

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<author><name>XIAOYUN LI</name>
<affiliation wicri:level="1"><inist:fA14 i1="01"><s1>State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University</s1>
<s2>Beijing 100084</s2>
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<country>République populaire de Chine</country>
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<author><name>PENGYI ZHANG</name>
<affiliation wicri:level="1"><inist:fA14 i1="01"><s1>State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University</s1>
<s2>Beijing 100084</s2>
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<author><name>LING JIN</name>
<affiliation wicri:level="1"><inist:fA14 i1="01"><s1>State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University</s1>
<s2>Beijing 100084</s2>
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<author><name>TIAN SHAO</name>
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<author><name>ZHENMIN LI</name>
<affiliation wicri:level="1"><inist:fA14 i1="01"><s1>State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University</s1>
<s2>Beijing 100084</s2>
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<author><name>JUNJIE CAO</name>
<affiliation wicri:level="1"><inist:fA14 i1="01"><s1>State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University</s1>
<s2>Beijing 100084</s2>
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<seriesStmt><idno type="ISSN">0013-936X</idno>
<title level="j" type="abbreviated">Environ. sci. technol.</title>
<title level="j" type="main">Environmental science & technology</title>
</seriesStmt>
</fileDesc>
<profileDesc><textClass><keywords scheme="KwdEn" xml:lang="en"><term>Carboxylic acid</term>
<term>Chemical reaction kinetics</term>
<term>EPR spectrometry</term>
<term>Emerging contaminant</term>
<term>Fourier-transformed infrared spectrometry</term>
<term>Indium oxide</term>
<term>NMR spectrometry</term>
<term>Organic fluorine compounds</term>
<term>Perfluorooctanoic acid</term>
<term>Photocatalysis</term>
<term>Photochemical degradation</term>
<term>Physicochemical purification</term>
<term>Reaction mechanism</term>
<term>Reflection spectrometry</term>
<term>Titanium oxide</term>
<term>Ultraviolet radiation</term>
<term>Waste water purification</term>
<term>Water treatment</term>
</keywords>
<keywords scheme="Pascal" xml:lang="fr"><term>Photocatalyse</term>
<term>Oxyde d'indium</term>
<term>Oxyde de titane</term>
<term>Rayonnement UV</term>
<term>Spectrométrie FTIR</term>
<term>Spectrométrie réflexion</term>
<term>Epuration eau usée</term>
<term>Epuration physicochimique</term>
<term>Traitement eau</term>
<term>Mécanisme réaction</term>
<term>Cinétique chimique</term>
<term>Spectrométrie RPE</term>
<term>Spectrométrie RMN</term>
<term>Dégradation photochimique</term>
<term>Acide carboxylique</term>
<term>Fluor composé organique</term>
<term>Acide perfluorooctanoïque</term>
<term>Polluant émergent</term>
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<front><div type="abstract" xml:lang="en">Perfluorooctanoic acid (C<sub>7</sub>
F<sub>15</sub>
COOH, PFOA) has increasingly attracted worldwide concerns due to its global occurrence and resistance to most conventional treatment processes. Though TiO<sub>2</sub>
-based photocatalysis is strong enough to decompose most organics, it is not effective for PFOA decomposition. We first find that indium oxide (In<sub>2</sub>
O<sub>3</sub>
) possesses significant activity for PFOA decomposition under UV irradiation, with the rate constant about 8.4 times higher than that by TiO<sub>2</sub>
. The major intermediates of PFOA were C<sub>2</sub>
-C<sub>7</sub>
 shorter-chain perfluorocarboxylic acids, implying that the reaction proceeded in a stepwise manner. By using diffuse reflectance infrared Fourier transform spectroscopy, <sup>19</sup>
F magic angle spinning nuclear magnetic resonance, and electron spin resonance, we demonstrate that the terminal carboxylate group of PFOA molecule tightly coordinates to the In<sub>2</sub>
O<sub>3</sub>
 surface in a bidentate or bridging configuration, which is beneficial for PFOA to be directly decomposed by photogenerated holes of In<sub>2</sub>
O<sub>3</sub>
 under UV irradiation, while PFOA coordinates to TiO<sub>2</sub>
 in a monodentate mode, and photogenerated holes of TiO<sub>2</sub>
 preferentially transform to hydroxyl radicals, which are inert to react with PFOA. PFOA decomposition in wastewater was inhibited by bicarbonate and other organic matters; however, their adverse impacts can be mostly avoided via pH adjustment and ozone addition.</div>
</front>
</TEI>
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<fA11 i1="01" i2="1"><s1>XIAOYUN LI</s1>
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<fA11 i1="02" i2="1"><s1>PENGYI ZHANG</s1>
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<fA11 i1="03" i2="1"><s1>LING JIN</s1>
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<fA11 i1="04" i2="1"><s1>TIAN SHAO</s1>
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<fA11 i1="05" i2="1"><s1>ZHENMIN LI</s1>
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<fC01 i1="01" l="ENG"><s0>Perfluorooctanoic acid (C<sub>7</sub>
F<sub>15</sub>
COOH, PFOA) has increasingly attracted worldwide concerns due to its global occurrence and resistance to most conventional treatment processes. Though TiO<sub>2</sub>
-based photocatalysis is strong enough to decompose most organics, it is not effective for PFOA decomposition. We first find that indium oxide (In<sub>2</sub>
O<sub>3</sub>
) possesses significant activity for PFOA decomposition under UV irradiation, with the rate constant about 8.4 times higher than that by TiO<sub>2</sub>
. The major intermediates of PFOA were C<sub>2</sub>
-C<sub>7</sub>
 shorter-chain perfluorocarboxylic acids, implying that the reaction proceeded in a stepwise manner. By using diffuse reflectance infrared Fourier transform spectroscopy, <sup>19</sup>
F magic angle spinning nuclear magnetic resonance, and electron spin resonance, we demonstrate that the terminal carboxylate group of PFOA molecule tightly coordinates to the In<sub>2</sub>
O<sub>3</sub>
 surface in a bidentate or bridging configuration, which is beneficial for PFOA to be directly decomposed by photogenerated holes of In<sub>2</sub>
O<sub>3</sub>
 under UV irradiation, while PFOA coordinates to TiO<sub>2</sub>
 in a monodentate mode, and photogenerated holes of TiO<sub>2</sub>
 preferentially transform to hydroxyl radicals, which are inert to react with PFOA. PFOA decomposition in wastewater was inhibited by bicarbonate and other organic matters; however, their adverse impacts can be mostly avoided via pH adjustment and ozone addition.</s0>
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<s1>ACT</s1>
<s5>02</s5>
</fC03>
<fC03 i1="02" i2="X" l="ENG"><s0>Indium oxide</s0>
<s1>ACT</s1>
<s5>02</s5>
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<fC03 i1="02" i2="X" l="SPA"><s0>Indio óxido</s0>
<s1>ACT</s1>
<s5>02</s5>
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<fC03 i1="03" i2="X" l="FRE"><s0>Oxyde de titane</s0>
<s1>ACT</s1>
<s5>03</s5>
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<fC03 i1="03" i2="X" l="ENG"><s0>Titanium oxide</s0>
<s1>ACT</s1>
<s5>03</s5>
</fC03>
<fC03 i1="03" i2="X" l="SPA"><s0>Titanio óxido</s0>
<s1>ACT</s1>
<s5>03</s5>
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<s5>06</s5>
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<fC03 i1="06" i2="X" l="SPA"><s0>Espectrometría reflexión</s0>
<s5>06</s5>
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<fC03 i1="07" i2="X" l="FRE"><s0>Epuration eau usée</s0>
<s5>07</s5>
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<s5>07</s5>
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<s5>08</s5>
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<s5>10</s5>
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<s5>10</s5>
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<s5>10</s5>
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<s5>11</s5>
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<s5>11</s5>
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<s5>11</s5>
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<s5>12</s5>
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<s5>12</s5>
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<s5>13</s5>
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<s5>13</s5>
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<fC03 i1="13" i2="X" l="SPA"><s0>Espectrometría RMN</s0>
<s5>13</s5>
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<fC03 i1="14" i2="X" l="FRE"><s0>Dégradation photochimique</s0>
<s5>35</s5>
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<s5>35</s5>
</fC03>
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<s5>35</s5>
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<s5>36</s5>
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<s5>36</s5>
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<s5>36</s5>
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<s5>37</s5>
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<s5>37</s5>
</fC03>
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<s4>CD</s4>
<s5>96</s5>
</fC03>
<fC03 i1="17" i2="X" l="ENG"><s0>Perfluorooctanoic acid</s0>
<s4>CD</s4>
<s5>96</s5>
</fC03>
<fC03 i1="17" i2="X" l="SPA"><s0>Ácido perfluorooctanoico</s0>
<s4>CD</s4>
<s5>96</s5>
</fC03>
<fC03 i1="18" i2="X" l="FRE"><s0>Polluant émergent</s0>
<s4>CD</s4>
<s5>97</s5>
</fC03>
<fC03 i1="18" i2="X" l="ENG"><s0>Emerging contaminant</s0>
<s4>CD</s4>
<s5>97</s5>
</fC03>
<fC03 i1="18" i2="X" l="SPA"><s0>Contaminante emergente</s0>
<s4>CD</s4>
<s5>97</s5>
</fC03>
<fC07 i1="01" i2="X" l="FRE"><s0>Polluant organique persistant</s0>
<s5>43</s5>
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<s5>43</s5>
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<s5>43</s5>
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<s2>NA</s2>
<s5>44</s5>
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<s5>44</s5>
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<fC07 i1="02" i2="X" l="SPA"><s0>Compuesto orgánico</s0>
<s2>NA</s2>
<s5>44</s5>
</fC07>
<fN21><s1>063</s1>
</fN21>
</pA>
</standard>
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   |clé=     Pascal:13-0090637
   |texte=   Efficient Photocatalytic Decomposition of Perfluorooctanoic Acid by Indium Oxide and Its Mechanism
}}

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Efficient Photocatalytic Decomposition of Perfluorooctanoic Acid by Indium Oxide and Its Mechanism

Efficient Photocatalytic Decomposition of Perfluorooctanoic Acid by Indium Oxide and Its Mechanism

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