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Bismuth atom tailoring of indium oxide surface frustrated Lewis pairs boosts heterogeneous CO2 photocatalytic hydrogenation
The surface frustrated Lewis pairs (SFLPs) on defect-laden metal oxides provide catalytic sites to activate H 2 and CO 2 molecules and enable efficient gas-phase CO 2 photocatalysis. Lattice engineering of metal oxides provides a useful strategy to tailor the reactivity of SFLPs. Herein, a one-step...
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| Published in: | Nature communications 2020-11, Vol.11 (1), p.6095-6095, Article 6095 |
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| creator | Yan, Tingjiang Li, Na Wang, Linlin Ran, Weiguang Duchesne, Paul N. Wan, Lili Nguyen, Nhat Truong Wang, Lu Xia, Meikun Ozin, Geoffrey A. |
| description | The surface frustrated Lewis pairs (SFLPs) on defect-laden metal oxides provide catalytic sites to activate H
2
and CO
2
molecules and enable efficient gas-phase CO
2
photocatalysis. Lattice engineering of metal oxides provides a useful strategy to tailor the reactivity of SFLPs. Herein, a one-step solvothermal synthesis is developed that enables isomorphic replacement of Lewis acidic site In
3+
ions in In
2
O
3
by single-site Bi
3+
ions, thereby enhancing the propensity to activate CO
2
molecules. The so-formed Bi
x
In
2-x
O
3
materials prove to be three orders of magnitude more photoactive for the reverse water gas shift reaction than In
2
O
3
itself, while also exhibiting notable photoactivity towards methanol production. The increased solar absorption efficiency and efficient charge-separation and transfer of Bi
x
In
2-x
O
3
also contribute to the improved photocatalytic performance. These traits exemplify the opportunities that exist for atom-scale engineering in heterogeneous CO
2
photocatalysis, another step towards the vision of the solar CO
2
refinery.
Surface frustrated Lewis pairs (SFLPs) provide a unique class of active sites that enable efficient gas-phase CO
2
photocatalysis. How to tailor the reactivity of the SFLPs represents a major challenge, which the authors address here by single-site Bi
3+
ion substitution of the SFLPs. |
| doi_str_mv | 10.1038/s41467-020-19997-y |
| format | article |
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2
and CO
2
molecules and enable efficient gas-phase CO
2
photocatalysis. Lattice engineering of metal oxides provides a useful strategy to tailor the reactivity of SFLPs. Herein, a one-step solvothermal synthesis is developed that enables isomorphic replacement of Lewis acidic site In
3+
ions in In
2
O
3
by single-site Bi
3+
ions, thereby enhancing the propensity to activate CO
2
molecules. The so-formed Bi
x
In
2-x
O
3
materials prove to be three orders of magnitude more photoactive for the reverse water gas shift reaction than In
2
O
3
itself, while also exhibiting notable photoactivity towards methanol production. The increased solar absorption efficiency and efficient charge-separation and transfer of Bi
x
In
2-x
O
3
also contribute to the improved photocatalytic performance. These traits exemplify the opportunities that exist for atom-scale engineering in heterogeneous CO
2
photocatalysis, another step towards the vision of the solar CO
2
refinery.
Surface frustrated Lewis pairs (SFLPs) provide a unique class of active sites that enable efficient gas-phase CO
2
photocatalysis. How to tailor the reactivity of the SFLPs represents a major challenge, which the authors address here by single-site Bi
3+
ion substitution of the SFLPs.</description><identifier>ISSN: 2041-1723</identifier><identifier>EISSN: 2041-1723</identifier><identifier>DOI: 10.1038/s41467-020-19997-y</identifier><identifier>PMID: 33257718</identifier><language>eng</language><publisher>London: Nature Publishing Group UK</publisher><subject>119/118 ; 140/146 ; 147/143 ; 639/4077/909/4101/4102 ; 639/638/77/890 ; 639/925/357/551 ; Active sites ; Bismuth ; Carbon dioxide ; Charge efficiency ; Charge transfer ; Humanities and Social Sciences ; Indium ; Indium oxides ; Ions ; Metal oxides ; multidisciplinary ; Oxides ; Photocatalysis ; Refineries ; Science ; Science (multidisciplinary) ; Shift reaction ; Substitution reactions ; Water gas</subject><ispartof>Nature communications, 2020-11, Vol.11 (1), p.6095-6095, Article 6095</ispartof><rights>The Author(s) 2020</rights><rights>The Author(s) 2020. This work is published under http://creativecommons.org/licenses/by/4.0/ (the “License”). Notwithstanding the ProQuest Terms and Conditions, you may use this content in accordance with the terms of the License.</rights><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c583t-2597510ba645c1ccdd3300be1f8e9fb14e8eaabee457d573c07fa6184fd7173c3</citedby><cites>FETCH-LOGICAL-c583t-2597510ba645c1ccdd3300be1f8e9fb14e8eaabee457d573c07fa6184fd7173c3</cites><orcidid>0000-0002-7651-3174 ; 0000-0002-6315-0925</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://www.proquest.com/docview/2473273139/fulltextPDF?pq-origsite=primo$$EPDF$$P50$$Gproquest$$Hfree_for_read</linktopdf><linktohtml>$$Uhttps://www.proquest.com/docview/2473273139?pq-origsite=primo$$EHTML$$P50$$Gproquest$$Hfree_for_read</linktohtml><link.rule.ids>230,314,727,780,784,885,25753,27924,27925,37012,37013,44590,53791,53793,74998</link.rule.ids></links><search><creatorcontrib>Yan, Tingjiang</creatorcontrib><creatorcontrib>Li, Na</creatorcontrib><creatorcontrib>Wang, Linlin</creatorcontrib><creatorcontrib>Ran, Weiguang</creatorcontrib><creatorcontrib>Duchesne, Paul N.</creatorcontrib><creatorcontrib>Wan, Lili</creatorcontrib><creatorcontrib>Nguyen, Nhat Truong</creatorcontrib><creatorcontrib>Wang, Lu</creatorcontrib><creatorcontrib>Xia, Meikun</creatorcontrib><creatorcontrib>Ozin, Geoffrey A.</creatorcontrib><title>Bismuth atom tailoring of indium oxide surface frustrated Lewis pairs boosts heterogeneous CO2 photocatalytic hydrogenation</title><title>Nature communications</title><addtitle>Nat Commun</addtitle><description>The surface frustrated Lewis pairs (SFLPs) on defect-laden metal oxides provide catalytic sites to activate H
2
and CO
2
molecules and enable efficient gas-phase CO
2
photocatalysis. Lattice engineering of metal oxides provides a useful strategy to tailor the reactivity of SFLPs. Herein, a one-step solvothermal synthesis is developed that enables isomorphic replacement of Lewis acidic site In
3+
ions in In
2
O
3
by single-site Bi
3+
ions, thereby enhancing the propensity to activate CO
2
molecules. The so-formed Bi
x
In
2-x
O
3
materials prove to be three orders of magnitude more photoactive for the reverse water gas shift reaction than In
2
O
3
itself, while also exhibiting notable photoactivity towards methanol production. The increased solar absorption efficiency and efficient charge-separation and transfer of Bi
x
In
2-x
O
3
also contribute to the improved photocatalytic performance. These traits exemplify the opportunities that exist for atom-scale engineering in heterogeneous CO
2
photocatalysis, another step towards the vision of the solar CO
2
refinery.
Surface frustrated Lewis pairs (SFLPs) provide a unique class of active sites that enable efficient gas-phase CO
2
photocatalysis. How to tailor the reactivity of the SFLPs represents a major challenge, which the authors address here by single-site Bi
3+
ion substitution of the SFLPs.</description><subject>119/118</subject><subject>140/146</subject><subject>147/143</subject><subject>639/4077/909/4101/4102</subject><subject>639/638/77/890</subject><subject>639/925/357/551</subject><subject>Active sites</subject><subject>Bismuth</subject><subject>Carbon dioxide</subject><subject>Charge efficiency</subject><subject>Charge transfer</subject><subject>Humanities and Social Sciences</subject><subject>Indium</subject><subject>Indium oxides</subject><subject>Ions</subject><subject>Metal oxides</subject><subject>multidisciplinary</subject><subject>Oxides</subject><subject>Photocatalysis</subject><subject>Refineries</subject><subject>Science</subject><subject>Science (multidisciplinary)</subject><subject>Shift reaction</subject><subject>Substitution reactions</subject><subject>Water 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atom tailoring of indium oxide surface frustrated Lewis pairs boosts heterogeneous CO2 photocatalytic hydrogenation</title><author>Yan, Tingjiang ; Li, Na ; Wang, Linlin ; Ran, Weiguang ; Duchesne, Paul N. ; Wan, Lili ; Nguyen, Nhat Truong ; Wang, Lu ; Xia, Meikun ; Ozin, Geoffrey A.</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c583t-2597510ba645c1ccdd3300be1f8e9fb14e8eaabee457d573c07fa6184fd7173c3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2020</creationdate><topic>119/118</topic><topic>140/146</topic><topic>147/143</topic><topic>639/4077/909/4101/4102</topic><topic>639/638/77/890</topic><topic>639/925/357/551</topic><topic>Active sites</topic><topic>Bismuth</topic><topic>Carbon dioxide</topic><topic>Charge efficiency</topic><topic>Charge transfer</topic><topic>Humanities and Social Sciences</topic><topic>Indium</topic><topic>Indium oxides</topic><topic>Ions</topic><topic>Metal 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China</collection><collection>Genetics Abstracts</collection><collection>Environment Abstracts</collection><collection>MEDLINE - Academic</collection><collection>PubMed Central (Full Participant titles)</collection><collection>Directory of Open Access Journals</collection><jtitle>Nature communications</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Yan, Tingjiang</au><au>Li, Na</au><au>Wang, Linlin</au><au>Ran, Weiguang</au><au>Duchesne, Paul N.</au><au>Wan, Lili</au><au>Nguyen, Nhat Truong</au><au>Wang, Lu</au><au>Xia, Meikun</au><au>Ozin, Geoffrey A.</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Bismuth atom tailoring of indium oxide surface frustrated Lewis pairs boosts heterogeneous CO2 photocatalytic hydrogenation</atitle><jtitle>Nature communications</jtitle><stitle>Nat Commun</stitle><date>2020-11-30</date><risdate>2020</risdate><volume>11</volume><issue>1</issue><spage>6095</spage><epage>6095</epage><pages>6095-6095</pages><artnum>6095</artnum><issn>2041-1723</issn><eissn>2041-1723</eissn><abstract>The surface frustrated Lewis pairs (SFLPs) on defect-laden metal oxides provide catalytic sites to activate H
2
and CO
2
molecules and enable efficient gas-phase CO
2
photocatalysis. Lattice engineering of metal oxides provides a useful strategy to tailor the reactivity of SFLPs. Herein, a one-step solvothermal synthesis is developed that enables isomorphic replacement of Lewis acidic site In
3+
ions in In
2
O
3
by single-site Bi
3+
ions, thereby enhancing the propensity to activate CO
2
molecules. The so-formed Bi
x
In
2-x
O
3
materials prove to be three orders of magnitude more photoactive for the reverse water gas shift reaction than In
2
O
3
itself, while also exhibiting notable photoactivity towards methanol production. The increased solar absorption efficiency and efficient charge-separation and transfer of Bi
x
In
2-x
O
3
also contribute to the improved photocatalytic performance. These traits exemplify the opportunities that exist for atom-scale engineering in heterogeneous CO
2
photocatalysis, another step towards the vision of the solar CO
2
refinery.
Surface frustrated Lewis pairs (SFLPs) provide a unique class of active sites that enable efficient gas-phase CO
2
photocatalysis. How to tailor the reactivity of the SFLPs represents a major challenge, which the authors address here by single-site Bi
3+
ion substitution of the SFLPs.</abstract><cop>London</cop><pub>Nature Publishing Group UK</pub><pmid>33257718</pmid><doi>10.1038/s41467-020-19997-y</doi><tpages>1</tpages><orcidid>https://orcid.org/0000-0002-7651-3174</orcidid><orcidid>https://orcid.org/0000-0002-6315-0925</orcidid><oa>free_for_read</oa></addata></record> |
| fulltext | fulltext |
| identifier | ISSN: 2041-1723 |
| ispartof | Nature communications, 2020-11, Vol.11 (1), p.6095-6095, Article 6095 |
| issn | 2041-1723 2041-1723 |
| language | eng |
| recordid | cdi_doaj_primary_oai_doaj_org_article_761bd719c6e94cb588e57065eef946ad |
| source | Open Access: PubMed Central; Publicly Available Content (ProQuest); Nature Journals Online; Springer Nature - nature.com Journals - Fully Open Access |
| subjects | 119/118 140/146 147/143 639/4077/909/4101/4102 639/638/77/890 639/925/357/551 Active sites Bismuth Carbon dioxide Charge efficiency Charge transfer Humanities and Social Sciences Indium Indium oxides Ions Metal oxides multidisciplinary Oxides Photocatalysis Refineries Science Science (multidisciplinary) Shift reaction Substitution reactions Water gas |
| title | Bismuth atom tailoring of indium oxide surface frustrated Lewis pairs boosts heterogeneous CO2 photocatalytic hydrogenation |
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