Efficient photocatalytic decomposition of perfluorooctanoic acid by indium oxide and its mechanism.
Identifieur interne : 000E51 ( Main/Exploration ); précédent : 000E50; suivant : 000E52Efficient photocatalytic decomposition of perfluorooctanoic acid by indium oxide and its mechanism.
Auteurs : RBID : pubmed:22489882English descriptors
- KwdEn :
- Adsorption (radiation effects), Caprylates (chemistry), Caprylates (radiation effects), Carbon (analysis), Catalysis (radiation effects), Electron Spin Resonance Spectroscopy, Fluorine (analysis), Fluorocarbons (chemistry), Fluorocarbons (radiation effects), Indium (chemistry), Magnetic Resonance Spectroscopy, Models, Chemical, Molecular Conformation, Spectroscopy, Fourier Transform Infrared, Spin Labels, Time Factors, Titanium (chemistry), Ultraviolet Rays, Water Pollutants, Chemical (chemistry), Water Pollutants, Chemical (radiation effects).
- MESH :
- chemical , analysis : Carbon, Fluorine.
- chemical , chemistry : Caprylates, Fluorocarbons, Indium, Titanium, Water Pollutants, Chemical.
- radiation effects : Adsorption, Caprylates, Catalysis, Fluorocarbons, Water Pollutants, Chemical.
- Electron Spin Resonance Spectroscopy, Magnetic Resonance Spectroscopy, Models, Chemical, Molecular Conformation, Spectroscopy, Fourier Transform Infrared, Spin Labels, Time Factors, Ultraviolet Rays.
Abstract
Perfluorooctanoic acid (C(7)F(15)COOH, PFOA) has increasingly attracted worldwide concerns due to its global occurrence and resistance to most conventional treatment processes. Though TiO(2)-based photocatalysis is strong enough to decompose most organics, it is not effective for PFOA decomposition. We first find that indium oxide (In(2)O(3)) possesses significant activity for PFOA decomposition under UV irradiation, with the rate constant about 8.4 times higher than that by TiO(2). The major intermediates of PFOA were C(2)-C(7) shorter-chain perfluorocarboxylic acids, implying that the reaction proceeded in a stepwise manner. By using diffuse reflectance infrared Fourier transform spectroscopy, (19)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(2)O(3) surface in a bidentate or bridging configuration, which is beneficial for PFOA to be directly decomposed by photogenerated holes of In(2)O(3) under UV irradiation, while PFOA coordinates to TiO(2) in a monodentate mode, and photogenerated holes of TiO(2) 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.
DOI: 10.1021/es204279u
PubMed: 22489882
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<record><TEI><teiHeader><fileDesc><titleStmt><title xml:lang="en">Efficient photocatalytic decomposition of perfluorooctanoic acid by indium oxide and its mechanism.</title><author><name sortKey="Li, Xiaoyun" uniqKey="Li X">Xiaoyun Li</name><affiliation wicri:level="1"><nlm:affiliation>State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, Beijing 100084, China.</nlm:affiliation><country xml:lang="fr">République populaire de Chine</country><wicri:regionArea>State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, Beijing 100084</wicri:regionArea></affiliation></author><author><name sortKey="Zhang, Pengyi" uniqKey="Zhang P">Pengyi Zhang</name></author><author><name sortKey="Jin, Ling" uniqKey="Jin L">Ling Jin</name></author><author><name sortKey="Shao, Tian" uniqKey="Shao T">Tian Shao</name></author><author><name sortKey="Li, Zhenmin" uniqKey="Li Z">Zhenmin Li</name></author><author><name sortKey="Cao, Junjie" uniqKey="Cao J">Junjie Cao</name></author></titleStmt><publicationStmt><date when="2012">2012</date><idno type="doi">10.1021/es204279u</idno><idno type="RBID">pubmed:22489882</idno><idno type="pmid">22489882</idno><idno type="wicri:Area/Main/Corpus">000D80</idno><idno type="wicri:Area/Main/Curation">000D80</idno><idno type="wicri:Area/Main/Exploration">000E51</idno></publicationStmt></fileDesc><profileDesc><textClass><keywords scheme="KwdEn" xml:lang="en"><term>Adsorption (radiation effects)</term><term>Caprylates (chemistry)</term><term>Caprylates (radiation effects)</term><term>Carbon (analysis)</term><term>Catalysis (radiation effects)</term><term>Electron Spin Resonance Spectroscopy</term><term>Fluorine (analysis)</term><term>Fluorocarbons (chemistry)</term><term>Fluorocarbons (radiation effects)</term><term>Indium (chemistry)</term><term>Magnetic Resonance Spectroscopy</term><term>Models, Chemical</term><term>Molecular Conformation</term><term>Spectroscopy, Fourier Transform Infrared</term><term>Spin Labels</term><term>Time Factors</term><term>Titanium (chemistry)</term><term>Ultraviolet Rays</term><term>Water Pollutants, Chemical (chemistry)</term><term>Water Pollutants, Chemical (radiation effects)</term></keywords><keywords scheme="MESH" type="chemical" qualifier="analysis" xml:lang="en"><term>Carbon</term><term>Fluorine</term></keywords><keywords scheme="MESH" type="chemical" qualifier="chemistry" xml:lang="en"><term>Caprylates</term><term>Fluorocarbons</term><term>Indium</term><term>Titanium</term><term>Water Pollutants, Chemical</term></keywords><keywords scheme="MESH" qualifier="radiation effects" xml:lang="en"><term>Adsorption</term><term>Caprylates</term><term>Catalysis</term><term>Fluorocarbons</term><term>Water Pollutants, Chemical</term></keywords><keywords scheme="MESH" xml:lang="en"><term>Electron Spin Resonance Spectroscopy</term><term>Magnetic Resonance Spectroscopy</term><term>Models, Chemical</term><term>Molecular Conformation</term><term>Spectroscopy, Fourier Transform Infrared</term><term>Spin Labels</term><term>Time Factors</term><term>Ultraviolet Rays</term></keywords></textClass></profileDesc></teiHeader><front><div type="abstract" xml:lang="en">Perfluorooctanoic acid (C(7)F(15)COOH, PFOA) has increasingly attracted worldwide concerns due to its global occurrence and resistance to most conventional treatment processes. Though TiO(2)-based photocatalysis is strong enough to decompose most organics, it is not effective for PFOA decomposition. We first find that indium oxide (In(2)O(3)) possesses significant activity for PFOA decomposition under UV irradiation, with the rate constant about 8.4 times higher than that by TiO(2). The major intermediates of PFOA were C(2)-C(7) shorter-chain perfluorocarboxylic acids, implying that the reaction proceeded in a stepwise manner. By using diffuse reflectance infrared Fourier transform spectroscopy, (19)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(2)O(3) surface in a bidentate or bridging configuration, which is beneficial for PFOA to be directly decomposed by photogenerated holes of In(2)O(3) under UV irradiation, while PFOA coordinates to TiO(2) in a monodentate mode, and photogenerated holes of TiO(2) 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><pubmed><MedlineCitation Owner="NLM" Status="MEDLINE"><PMID Version="1">22489882</PMID><DateCreated><Year>2012</Year><Month>05</Month><Day>15</Day></DateCreated><DateCompleted><Year>2012</Year><Month>09</Month><Day>07</Day></DateCompleted><DateRevised><Year>2013</Year><Month>11</Month><Day>21</Day></DateRevised><Article PubModel="Print-Electronic"><Journal><ISSN IssnType="Electronic">1520-5851</ISSN><JournalIssue CitedMedium="Internet"><Volume>46</Volume><Issue>10</Issue><PubDate><Year>2012</Year><Month>May</Month><Day>15</Day></PubDate></JournalIssue><Title>Environmental science & technology</Title><ISOAbbreviation>Environ. Sci. Technol.</ISOAbbreviation></Journal><ArticleTitle>Efficient photocatalytic decomposition of perfluorooctanoic acid by indium oxide and its mechanism.</ArticleTitle><Pagination><MedlinePgn>5528-34</MedlinePgn></Pagination><ELocationID EIdType="doi" ValidYN="Y">10.1021/es204279u</ELocationID><Abstract><AbstractText>Perfluorooctanoic acid (C(7)F(15)COOH, PFOA) has increasingly attracted worldwide concerns due to its global occurrence and resistance to most conventional treatment processes. Though TiO(2)-based photocatalysis is strong enough to decompose most organics, it is not effective for PFOA decomposition. We first find that indium oxide (In(2)O(3)) possesses significant activity for PFOA decomposition under UV irradiation, with the rate constant about 8.4 times higher than that by TiO(2). The major intermediates of PFOA were C(2)-C(7) shorter-chain perfluorocarboxylic acids, implying that the reaction proceeded in a stepwise manner. By using diffuse reflectance infrared Fourier transform spectroscopy, (19)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(2)O(3) surface in a bidentate or bridging configuration, which is beneficial for PFOA to be directly decomposed by photogenerated holes of In(2)O(3) under UV irradiation, while PFOA coordinates to TiO(2) in a monodentate mode, and photogenerated holes of TiO(2) 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.</AbstractText></Abstract><AuthorList CompleteYN="Y"><Author ValidYN="Y"><LastName>Li</LastName><ForeName>Xiaoyun</ForeName><Initials>X</Initials><Affiliation>State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, Beijing 100084, China.</Affiliation></Author><Author ValidYN="Y"><LastName>Zhang</LastName><ForeName>Pengyi</ForeName><Initials>P</Initials></Author><Author ValidYN="Y"><LastName>Jin</LastName><ForeName>Ling</ForeName><Initials>L</Initials></Author><Author ValidYN="Y"><LastName>Shao</LastName><ForeName>Tian</ForeName><Initials>T</Initials></Author><Author ValidYN="Y"><LastName>Li</LastName><ForeName>Zhenmin</ForeName><Initials>Z</Initials></Author><Author ValidYN="Y"><LastName>Cao</LastName><ForeName>Junjie</ForeName><Initials>J</Initials></Author></AuthorList><Language>eng</Language><PublicationTypeList><PublicationType>Journal Article</PublicationType><PublicationType>Research Support, Non-U.S. Gov't</PublicationType></PublicationTypeList><ArticleDate DateType="Electronic"><Year>2012</Year><Month>05</Month><Day>01</Day></ArticleDate></Article><MedlineJournalInfo><Country>United States</Country><MedlineTA>Environ Sci Technol</MedlineTA><NlmUniqueID>0213155</NlmUniqueID><ISSNLinking>0013-936X</ISSNLinking></MedlineJournalInfo><ChemicalList><Chemical><RegistryNumber>0</RegistryNumber><NameOfSubstance>Caprylates</NameOfSubstance></Chemical><Chemical><RegistryNumber>0</RegistryNumber><NameOfSubstance>Fluorocarbons</NameOfSubstance></Chemical><Chemical><RegistryNumber>0</RegistryNumber><NameOfSubstance>Spin Labels</NameOfSubstance></Chemical><Chemical><RegistryNumber>0</RegistryNumber><NameOfSubstance>Water Pollutants, Chemical</NameOfSubstance></Chemical><Chemical><RegistryNumber>045A6V3VFX</RegistryNumber><NameOfSubstance>Indium</NameOfSubstance></Chemical><Chemical><RegistryNumber>15FIX9V2JP</RegistryNumber><NameOfSubstance>titanium dioxide</NameOfSubstance></Chemical><Chemical><RegistryNumber>284SYP0193</RegistryNumber><NameOfSubstance>Fluorine</NameOfSubstance></Chemical><Chemical><RegistryNumber>335-67-1</RegistryNumber><NameOfSubstance>perfluorooctanoic acid</NameOfSubstance></Chemical><Chemical><RegistryNumber>4OO9KME22D</RegistryNumber><NameOfSubstance>indium oxide</NameOfSubstance></Chemical><Chemical><RegistryNumber>7440-44-0</RegistryNumber><NameOfSubstance>Carbon</NameOfSubstance></Chemical><Chemical><RegistryNumber>D1JT611TNE</RegistryNumber><NameOfSubstance>Titanium</NameOfSubstance></Chemical></ChemicalList><CitationSubset>IM</CitationSubset><MeshHeadingList><MeshHeading><DescriptorName MajorTopicYN="N">Adsorption</DescriptorName><QualifierName MajorTopicYN="N">radiation effects</QualifierName></MeshHeading><MeshHeading><DescriptorName MajorTopicYN="N">Caprylates</DescriptorName><QualifierName MajorTopicYN="Y">chemistry</QualifierName><QualifierName MajorTopicYN="Y">radiation effects</QualifierName></MeshHeading><MeshHeading><DescriptorName MajorTopicYN="N">Carbon</DescriptorName><QualifierName MajorTopicYN="N">analysis</QualifierName></MeshHeading><MeshHeading><DescriptorName MajorTopicYN="N">Catalysis</DescriptorName><QualifierName MajorTopicYN="N">radiation effects</QualifierName></MeshHeading><MeshHeading><DescriptorName MajorTopicYN="N">Electron Spin Resonance Spectroscopy</DescriptorName></MeshHeading><MeshHeading><DescriptorName MajorTopicYN="N">Fluorine</DescriptorName><QualifierName MajorTopicYN="N">analysis</QualifierName></MeshHeading><MeshHeading><DescriptorName MajorTopicYN="N">Fluorocarbons</DescriptorName><QualifierName MajorTopicYN="Y">chemistry</QualifierName><QualifierName MajorTopicYN="Y">radiation effects</QualifierName></MeshHeading><MeshHeading><DescriptorName MajorTopicYN="N">Indium</DescriptorName><QualifierName MajorTopicYN="Y">chemistry</QualifierName></MeshHeading><MeshHeading><DescriptorName MajorTopicYN="N">Magnetic Resonance Spectroscopy</DescriptorName></MeshHeading><MeshHeading><DescriptorName MajorTopicYN="N">Models, Chemical</DescriptorName></MeshHeading><MeshHeading><DescriptorName MajorTopicYN="N">Molecular Conformation</DescriptorName></MeshHeading><MeshHeading><DescriptorName MajorTopicYN="N">Spectroscopy, Fourier Transform Infrared</DescriptorName></MeshHeading><MeshHeading><DescriptorName MajorTopicYN="N">Spin Labels</DescriptorName></MeshHeading><MeshHeading><DescriptorName MajorTopicYN="N">Time Factors</DescriptorName></MeshHeading><MeshHeading><DescriptorName MajorTopicYN="N">Titanium</DescriptorName><QualifierName MajorTopicYN="N">chemistry</QualifierName></MeshHeading><MeshHeading><DescriptorName MajorTopicYN="Y">Ultraviolet Rays</DescriptorName></MeshHeading><MeshHeading><DescriptorName MajorTopicYN="N">Water Pollutants, Chemical</DescriptorName><QualifierName MajorTopicYN="N">chemistry</QualifierName><QualifierName MajorTopicYN="N">radiation effects</QualifierName></MeshHeading></MeshHeadingList></MedlineCitation><PubmedData><History><PubMedPubDate PubStatus="aheadofprint"><Year>2012</Year><Month>5</Month><Day>1</Day></PubMedPubDate><PubMedPubDate PubStatus="entrez"><Year>2012</Year><Month>4</Month><Day>12</Day><Hour>6</Hour><Minute>0</Minute></PubMedPubDate><PubMedPubDate PubStatus="pubmed"><Year>2012</Year><Month>4</Month><Day>12</Day><Hour>6</Hour><Minute>0</Minute></PubMedPubDate><PubMedPubDate PubStatus="medline"><Year>2012</Year><Month>9</Month><Day>8</Day><Hour>6</Hour><Minute>0</Minute></PubMedPubDate></History><PublicationStatus>ppublish</PublicationStatus><ArticleIdList><ArticleId IdType="doi">10.1021/es204279u</ArticleId><ArticleId 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