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Modulating Local Charge Distribution of Carbon Nitride for Promoting Exciton Dissociation and Charge‐Induced Reactions
The sustainable light can generate reduction and oxidation centers in situ through the generation of photoexcited electrons and holes in the presence of photocatalyst. However, the photoexcited electrons and holes have huge Coulombic attraction and high exciton binding energy due to the weak screeni...
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| Published in: | Small (Weinheim an der Bergstrasse, Germany) Germany), 2021-08, Vol.17 (32), p.e2100698-n/a |
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| cites | cdi_FETCH-LOGICAL-c3508-1ccf683ef76702a05e01025aa2ba5d28002e6e72d90b4e3d186dfeb031e584a03 |
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| container_issue | 32 |
| container_start_page | e2100698 |
| container_title | Small (Weinheim an der Bergstrasse, Germany) |
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| creator | Chen, Guang Zhang, Zi‐Dan Liao, Ya‐Xian Zhang, Ze You, Ye‐Zi |
| description | The sustainable light can generate reduction and oxidation centers in situ through the generation of photoexcited electrons and holes in the presence of photocatalyst. However, the photoexcited electrons and holes have huge Coulombic attraction and high exciton binding energy due to the weak screening effect and dielectric properties in many low‐dimensional conjugated polymers, such as carbon nitride. Reducing the exciton binding energy of carbon nitride and promoting the conversion of excitons into free charge carriers are necessary for improving the activity of photocatalytic reactions but still very challenging. Here, by introducing amino‐cyano functional groups into carbon nitride, it is demonstrated that excitons can be effectively dissociated into electrons and holes by finely controlling the charge distribution of heptazine ring. It is found that carbon nitride with heptazine rings of positive charge distribution can greatly reduce the exciton binding energy to 24 from 71 meV. Compared with heptazine ring having negative charge distribution, heptazine ring with positive charge distribution can increase photocatalytic hydrogen production of carbon nitride by up to ten times. This work provides an easy way to promote the dissociation of excitons in carbon nitride by regulating the charge distribution.
By introducing amino‐cyano group into carbon nitride, the charge distribution of heptazine ring in carbon nitride can be controlled by adjusting the degree of protonation. Carbon nitride with positive charge distribution has a very low exciton binding energy, showing more efficient exciton dissociation and improved photocatalytic performance. |
| doi_str_mv | 10.1002/smll.202100698 |
| format | article |
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By introducing amino‐cyano group into carbon nitride, the charge distribution of heptazine ring in carbon nitride can be controlled by adjusting the degree of protonation. Carbon nitride with positive charge distribution has a very low exciton binding energy, showing more efficient exciton dissociation and improved photocatalytic performance.</description><identifier>ISSN: 1613-6810</identifier><identifier>EISSN: 1613-6829</identifier><identifier>DOI: 10.1002/smll.202100698</identifier><language>eng</language><publisher>Weinheim: Wiley Subscription Services, Inc</publisher><subject>Binding energy ; Carbon ; Carbon nitride ; Charge distribution ; Current carriers ; Dielectric properties ; Dielectric strength ; Electrons ; exciton binding energy ; exciton dissociation ; Excitons ; Functional groups ; Hydrogen production ; Nanotechnology ; Oxidation ; Photocatalysis</subject><ispartof>Small (Weinheim an der Bergstrasse, Germany), 2021-08, Vol.17 (32), p.e2100698-n/a</ispartof><rights>2021 Wiley‐VCH GmbH</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c3508-1ccf683ef76702a05e01025aa2ba5d28002e6e72d90b4e3d186dfeb031e584a03</citedby><cites>FETCH-LOGICAL-c3508-1ccf683ef76702a05e01025aa2ba5d28002e6e72d90b4e3d186dfeb031e584a03</cites><orcidid>0000-0002-2965-2614 ; 0000-0001-6555-0183</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://onlinelibrary.wiley.com/doi/pdf/10.1002%2Fsmll.202100698$$EPDF$$P50$$Gwiley$$H</linktopdf><linktohtml>$$Uhttps://onlinelibrary.wiley.com/doi/full/10.1002%2Fsmll.202100698$$EHTML$$P50$$Gwiley$$H</linktohtml><link.rule.ids>315,786,790,27957,27958,50923,51032</link.rule.ids></links><search><creatorcontrib>Chen, Guang</creatorcontrib><creatorcontrib>Zhang, Zi‐Dan</creatorcontrib><creatorcontrib>Liao, Ya‐Xian</creatorcontrib><creatorcontrib>Zhang, Ze</creatorcontrib><creatorcontrib>You, Ye‐Zi</creatorcontrib><title>Modulating Local Charge Distribution of Carbon Nitride for Promoting Exciton Dissociation and Charge‐Induced Reactions</title><title>Small (Weinheim an der Bergstrasse, Germany)</title><description>The sustainable light can generate reduction and oxidation centers in situ through the generation of photoexcited electrons and holes in the presence of photocatalyst. However, the photoexcited electrons and holes have huge Coulombic attraction and high exciton binding energy due to the weak screening effect and dielectric properties in many low‐dimensional conjugated polymers, such as carbon nitride. Reducing the exciton binding energy of carbon nitride and promoting the conversion of excitons into free charge carriers are necessary for improving the activity of photocatalytic reactions but still very challenging. Here, by introducing amino‐cyano functional groups into carbon nitride, it is demonstrated that excitons can be effectively dissociated into electrons and holes by finely controlling the charge distribution of heptazine ring. It is found that carbon nitride with heptazine rings of positive charge distribution can greatly reduce the exciton binding energy to 24 from 71 meV. Compared with heptazine ring having negative charge distribution, heptazine ring with positive charge distribution can increase photocatalytic hydrogen production of carbon nitride by up to ten times. This work provides an easy way to promote the dissociation of excitons in carbon nitride by regulating the charge distribution.
By introducing amino‐cyano group into carbon nitride, the charge distribution of heptazine ring in carbon nitride can be controlled by adjusting the degree of protonation. Carbon nitride with positive charge distribution has a very low exciton binding energy, showing more efficient exciton dissociation and improved photocatalytic performance.</description><subject>Binding energy</subject><subject>Carbon</subject><subject>Carbon nitride</subject><subject>Charge distribution</subject><subject>Current carriers</subject><subject>Dielectric properties</subject><subject>Dielectric strength</subject><subject>Electrons</subject><subject>exciton binding energy</subject><subject>exciton dissociation</subject><subject>Excitons</subject><subject>Functional groups</subject><subject>Hydrogen production</subject><subject>Nanotechnology</subject><subject>Oxidation</subject><subject>Photocatalysis</subject><issn>1613-6810</issn><issn>1613-6829</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2021</creationdate><recordtype>article</recordtype><recordid>eNqFkb9OwzAQhyMEEqWwMkdiYWmxncRxRhQKVEoB8WeOHPtSXCVxsRPRbjwCz8iT4LSoSCxMPvu-7-TTz_NOMRpjhMiFratqTBBxF5qwPW-AKQ5GlJFkf1djdOgdWbtAKMAkjAfeaqZlV_FWNXM_04JXfvrKzRz8K2Vbo4quVbrxdemn3BSuulPuVYJfauM_GF3rjTlZCdW6rpOsFopvJN7In2FfH5_TRnYCpP8IXPRde-wdlLyycPJzDr2X68lzejvK7m-m6WU2EkGE2AgLUVIWQBnTGBGOIkAYkYhzUvBIEuYWBwoxkQkqQggkZlSWULj1IGIhR8HQO9_OXRr91oFt81pZAVXFG9CdzUkUxhFJSNSjZ3_Qhe5M437nKIoIIYwmjhpvKWG0tQbKfGlUzc06xyjvg8j7IPJdEE5ItsK7qmD9D50_zbLs1_0GEG6Ohw</recordid><startdate>20210801</startdate><enddate>20210801</enddate><creator>Chen, Guang</creator><creator>Zhang, Zi‐Dan</creator><creator>Liao, Ya‐Xian</creator><creator>Zhang, Ze</creator><creator>You, Ye‐Zi</creator><general>Wiley Subscription Services, Inc</general><scope>AAYXX</scope><scope>CITATION</scope><scope>7SR</scope><scope>7U5</scope><scope>8BQ</scope><scope>8FD</scope><scope>JG9</scope><scope>L7M</scope><scope>7X8</scope><orcidid>https://orcid.org/0000-0002-2965-2614</orcidid><orcidid>https://orcid.org/0000-0001-6555-0183</orcidid></search><sort><creationdate>20210801</creationdate><title>Modulating Local Charge Distribution of Carbon Nitride for Promoting Exciton Dissociation and Charge‐Induced Reactions</title><author>Chen, Guang ; Zhang, Zi‐Dan ; Liao, Ya‐Xian ; Zhang, Ze ; You, Ye‐Zi</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c3508-1ccf683ef76702a05e01025aa2ba5d28002e6e72d90b4e3d186dfeb031e584a03</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2021</creationdate><topic>Binding energy</topic><topic>Carbon</topic><topic>Carbon nitride</topic><topic>Charge distribution</topic><topic>Current carriers</topic><topic>Dielectric properties</topic><topic>Dielectric strength</topic><topic>Electrons</topic><topic>exciton binding energy</topic><topic>exciton dissociation</topic><topic>Excitons</topic><topic>Functional groups</topic><topic>Hydrogen production</topic><topic>Nanotechnology</topic><topic>Oxidation</topic><topic>Photocatalysis</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Chen, Guang</creatorcontrib><creatorcontrib>Zhang, Zi‐Dan</creatorcontrib><creatorcontrib>Liao, Ya‐Xian</creatorcontrib><creatorcontrib>Zhang, Ze</creatorcontrib><creatorcontrib>You, Ye‐Zi</creatorcontrib><collection>CrossRef</collection><collection>Engineered Materials Abstracts</collection><collection>Solid State and Superconductivity Abstracts</collection><collection>METADEX</collection><collection>Technology Research Database</collection><collection>Materials Research Database</collection><collection>Advanced Technologies Database with Aerospace</collection><collection>MEDLINE - Academic</collection><jtitle>Small (Weinheim an der Bergstrasse, Germany)</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Chen, Guang</au><au>Zhang, Zi‐Dan</au><au>Liao, Ya‐Xian</au><au>Zhang, Ze</au><au>You, Ye‐Zi</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Modulating Local Charge Distribution of Carbon Nitride for Promoting Exciton Dissociation and Charge‐Induced Reactions</atitle><jtitle>Small (Weinheim an der Bergstrasse, Germany)</jtitle><date>2021-08-01</date><risdate>2021</risdate><volume>17</volume><issue>32</issue><spage>e2100698</spage><epage>n/a</epage><pages>e2100698-n/a</pages><issn>1613-6810</issn><eissn>1613-6829</eissn><notes>ObjectType-Article-1</notes><notes>SourceType-Scholarly Journals-1</notes><notes>ObjectType-Feature-2</notes><notes>content type line 23</notes><abstract>The sustainable light can generate reduction and oxidation centers in situ through the generation of photoexcited electrons and holes in the presence of photocatalyst. However, the photoexcited electrons and holes have huge Coulombic attraction and high exciton binding energy due to the weak screening effect and dielectric properties in many low‐dimensional conjugated polymers, such as carbon nitride. Reducing the exciton binding energy of carbon nitride and promoting the conversion of excitons into free charge carriers are necessary for improving the activity of photocatalytic reactions but still very challenging. Here, by introducing amino‐cyano functional groups into carbon nitride, it is demonstrated that excitons can be effectively dissociated into electrons and holes by finely controlling the charge distribution of heptazine ring. It is found that carbon nitride with heptazine rings of positive charge distribution can greatly reduce the exciton binding energy to 24 from 71 meV. Compared with heptazine ring having negative charge distribution, heptazine ring with positive charge distribution can increase photocatalytic hydrogen production of carbon nitride by up to ten times. This work provides an easy way to promote the dissociation of excitons in carbon nitride by regulating the charge distribution.
By introducing amino‐cyano group into carbon nitride, the charge distribution of heptazine ring in carbon nitride can be controlled by adjusting the degree of protonation. Carbon nitride with positive charge distribution has a very low exciton binding energy, showing more efficient exciton dissociation and improved photocatalytic performance.</abstract><cop>Weinheim</cop><pub>Wiley Subscription Services, Inc</pub><doi>10.1002/smll.202100698</doi><tpages>7</tpages><orcidid>https://orcid.org/0000-0002-2965-2614</orcidid><orcidid>https://orcid.org/0000-0001-6555-0183</orcidid></addata></record> |
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| subjects | Binding energy Carbon Carbon nitride Charge distribution Current carriers Dielectric properties Dielectric strength Electrons exciton binding energy exciton dissociation Excitons Functional groups Hydrogen production Nanotechnology Oxidation Photocatalysis |
| title | Modulating Local Charge Distribution of Carbon Nitride for Promoting Exciton Dissociation and Charge‐Induced Reactions |
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