Efficient Solar-Driven Hydrogen Transfer by Bismuth-Based Photocatalyst with Engineered Basic Sites
Photocatalytic organic conversions involving a hydrogen transfer (HT) step have attracted much attention, but the efficiency and selectivity under visible light irradiation still needs to be significantly enhanced. Here we have developed a noble metal-free, basic-site engineered bismuth oxybromide [...
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| Veröffentlicht in: | Journal of the American Chemical Society 2018-12, Vol.140 (48), p.16711-16719 |
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| container_title | Journal of the American Chemical Society |
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| creator | Dai, Yitao Li, Chao Shen, Yanbin Zhu, Shujie Hvid, Mathias S Wu, Lai-Chin Skibsted, Jørgen Li, Yongwang Niemantsverdriet, J. W. Hans Besenbacher, Flemming Lock, Nina Su, Ren |
| description | Photocatalytic organic conversions involving a hydrogen transfer (HT) step have attracted much attention, but the efficiency and selectivity under visible light irradiation still needs to be significantly enhanced. Here we have developed a noble metal-free, basic-site engineered bismuth oxybromide [Bi24O31Br10(OH)δ] that can accelerate the photocatalytic HT step in both reduction and oxidation reactions, i.e., nitrobenzene to azo/azoxybenzene, quinones to quinols, thiones to thiols, and alcohols to ketones under visible light irradiation and ambient conditions. Remarkably, quantum efficiencies of 42% and 32% for the nitrobenzene reduction can be reached under 410 and 450 nm irradiation, respectively. The Bi24O31Br10(OH)δ photocatalyst also exhibits excellent performance in up-scaling and stability under visible light and even solar irradiation, revealing economic potential for industrial applications. |
| doi_str_mv | 10.1021/jacs.8b09796 |
| format | Article |
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W. Hans ; Besenbacher, Flemming ; Lock, Nina ; Su, Ren</creator><creatorcontrib>Dai, Yitao ; Li, Chao ; Shen, Yanbin ; Zhu, Shujie ; Hvid, Mathias S ; Wu, Lai-Chin ; Skibsted, Jørgen ; Li, Yongwang ; Niemantsverdriet, J. W. Hans ; Besenbacher, Flemming ; Lock, Nina ; Su, Ren</creatorcontrib><description>Photocatalytic organic conversions involving a hydrogen transfer (HT) step have attracted much attention, but the efficiency and selectivity under visible light irradiation still needs to be significantly enhanced. Here we have developed a noble metal-free, basic-site engineered bismuth oxybromide [Bi24O31Br10(OH)δ] that can accelerate the photocatalytic HT step in both reduction and oxidation reactions, i.e., nitrobenzene to azo/azoxybenzene, quinones to quinols, thiones to thiols, and alcohols to ketones under visible light irradiation and ambient conditions. Remarkably, quantum efficiencies of 42% and 32% for the nitrobenzene reduction can be reached under 410 and 450 nm irradiation, respectively. The Bi24O31Br10(OH)δ photocatalyst also exhibits excellent performance in up-scaling and stability under visible light and even solar irradiation, revealing economic potential for industrial applications.</description><identifier>ISSN: 0002-7863</identifier><identifier>EISSN: 1520-5126</identifier><identifier>DOI: 10.1021/jacs.8b09796</identifier><identifier>PMID: 30394730</identifier><language>eng</language><publisher>United States: American Chemical Society</publisher><ispartof>Journal of the American Chemical Society, 2018-12, Vol.140 (48), p.16711-16719</ispartof><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-a324t-cbb9529abc27b1e8317e1a72274ad83b67c72856fac9450a1c3ac62c782d297f3</citedby><cites>FETCH-LOGICAL-a324t-cbb9529abc27b1e8317e1a72274ad83b67c72856fac9450a1c3ac62c782d297f3</cites><orcidid>0000-0003-0028-1335 ; 0000-0003-1534-4466 ; 0000-0002-1423-6431</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://pubs.acs.org/doi/pdf/10.1021/jacs.8b09796$$EPDF$$P50$$Gacs$$H</linktopdf><linktohtml>$$Uhttps://pubs.acs.org/doi/10.1021/jacs.8b09796$$EHTML$$P50$$Gacs$$H</linktohtml><link.rule.ids>314,776,780,2752,27053,27901,27902,56713,56763</link.rule.ids><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/30394730$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink></links><search><creatorcontrib>Dai, Yitao</creatorcontrib><creatorcontrib>Li, Chao</creatorcontrib><creatorcontrib>Shen, Yanbin</creatorcontrib><creatorcontrib>Zhu, Shujie</creatorcontrib><creatorcontrib>Hvid, Mathias S</creatorcontrib><creatorcontrib>Wu, Lai-Chin</creatorcontrib><creatorcontrib>Skibsted, Jørgen</creatorcontrib><creatorcontrib>Li, Yongwang</creatorcontrib><creatorcontrib>Niemantsverdriet, J. 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Remarkably, quantum efficiencies of 42% and 32% for the nitrobenzene reduction can be reached under 410 and 450 nm irradiation, respectively. The Bi24O31Br10(OH)δ photocatalyst also exhibits excellent performance in up-scaling and stability under visible light and even solar irradiation, revealing economic potential for industrial applications.</description><issn>0002-7863</issn><issn>1520-5126</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2018</creationdate><recordtype>article</recordtype><recordid>eNptkD1PwzAQhi0EoqWwMSOPDKT4I4mdkZZCkSqB1DJHtuO0rpK42A4o_55ULbAw-ax77j3dA8A1RmOMCL7fCuXHXKKMZekJGOKEoCjBJD0FQ4QQiRhP6QBceL_tvzHh-BwMKKJZzCgaAjUrS6OMbgJc2kq46NGZT93AeVc4u-6LlRONL7WDsoMT4-s2bKKJ8LqAbxsbrBJBVJ0P8MuEDZw1a9No7fpuzxgFlyZofwnOSlF5fXV8R-D9abaazqPF6_PL9GERCUriECkps4RkQirCJNacYqaxYISwWBScypQpRniSlkJlcYIEVlSolCjGSUEyVtIRuD3k7pz9aLUPeW280lUlGm1bnxNMEUp4jJMevTugylnvnS7znTO1cF2OUb7Xmu-15ketPX5zTG5lrYtf-Mfj3-r91Na2rukP_T_rG-UqgQs</recordid><startdate>20181205</startdate><enddate>20181205</enddate><creator>Dai, Yitao</creator><creator>Li, Chao</creator><creator>Shen, Yanbin</creator><creator>Zhu, Shujie</creator><creator>Hvid, Mathias S</creator><creator>Wu, Lai-Chin</creator><creator>Skibsted, Jørgen</creator><creator>Li, Yongwang</creator><creator>Niemantsverdriet, J. 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Soc</addtitle><date>2018-12-05</date><risdate>2018</risdate><volume>140</volume><issue>48</issue><spage>16711</spage><epage>16719</epage><pages>16711-16719</pages><issn>0002-7863</issn><eissn>1520-5126</eissn><abstract>Photocatalytic organic conversions involving a hydrogen transfer (HT) step have attracted much attention, but the efficiency and selectivity under visible light irradiation still needs to be significantly enhanced. Here we have developed a noble metal-free, basic-site engineered bismuth oxybromide [Bi24O31Br10(OH)δ] that can accelerate the photocatalytic HT step in both reduction and oxidation reactions, i.e., nitrobenzene to azo/azoxybenzene, quinones to quinols, thiones to thiols, and alcohols to ketones under visible light irradiation and ambient conditions. Remarkably, quantum efficiencies of 42% and 32% for the nitrobenzene reduction can be reached under 410 and 450 nm irradiation, respectively. 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| title | Efficient Solar-Driven Hydrogen Transfer by Bismuth-Based Photocatalyst with Engineered Basic Sites |
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