Co–N2 Bond Precisely Connects the Conduction Band and Valence Band of g‐C3N4/CoCo‐LDH to Enhance Photocatalytic CO2 Activity by High‐Efficiency S‐Scheme
Precise regulation of photogenic electron transfer path plays an important role in improving photocatalytic carbon dioxide reduction efficiency and product selectivity. Herein, under the guidance of density functional theory calculation, the interface chemical bond (CoN2 bond) at the atomic level i...
| Main Authors: | , , , , , , , , , |
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| Format: | Article |
| Language: | English |
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Wiley-VCH
2023-11-01
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| Series: | Small Structures |
| Subjects: | |
| Online Access: | https://doi.org/10.1002/sstr.202300177 |
| _version_ | 1797504914001231872 |
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| author | Yi-lei Li Qing Zhao Xu-jia Liu Ying Liu Ying-juan Hao Xiao-jing Wang Xin-ying Liu Diane Hildebrandt Feng-yu Li Fa-tang Li |
| author_facet | Yi-lei Li Qing Zhao Xu-jia Liu Ying Liu Ying-juan Hao Xiao-jing Wang Xin-ying Liu Diane Hildebrandt Feng-yu Li Fa-tang Li |
| author_sort | Yi-lei Li |
| collection | DOAJ |
| description | Precise regulation of photogenic electron transfer path plays an important role in improving photocatalytic carbon dioxide reduction efficiency and product selectivity. Herein, under the guidance of density functional theory calculation, the interface chemical bond (CoN2 bond) at the atomic level is designed, and g‐C3N4/CoCo‐layered double hydroxide (LDH) heterostructure is manufactured. CoCo‐LDH with water oxidation ability and g‐C3N4 were combined to construct S‐scheme heterojunction with redox ability. The valence band and conduction band of g‐C3N4 and CoCo‐LDH are precisely connected by the interfacial CoN2 bond, which realizes the high‐speed transfer of electron transport. Despite the absence of cocatalyst, the heterojunction exhibits high water oxidation and carbon reduction capacity due to the precise regulation of CoN2 bonds. Theoretical calculations and experimental results show that the addition of CoCo‐LDH: reduces the oxidation overpotential of water to provide more H protons; regulates the delocalization charge of g‐C3N4; and reduces the energy barrier of the CO2 intermediate (*COOH) in the reduction half‐reaction. The results show that the selectivity of carbon‐based substances in the products was 100%, and the optimal CO yield was 71.39 μmol g−1 h−1, which is among the highest values of g‐C3N4‐based photocatalysts. |
| first_indexed | 2024-03-10T04:11:11Z |
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| id | doaj.art-72835d30d96a4c3a8f6d39f760a8afda |
| institution | Directory Open Access Journal |
| issn | 2688-4062 |
| language | English |
| last_indexed | 2024-03-10T04:11:11Z |
| publishDate | 2023-11-01 |
| publisher | Wiley-VCH |
| record_format | Article |
| series | Small Structures |
| spelling | doaj.art-72835d30d96a4c3a8f6d39f760a8afda2023-11-23T08:10:45ZengWiley-VCHSmall Structures2688-40622023-11-01411n/an/a10.1002/sstr.202300177Co–N2 Bond Precisely Connects the Conduction Band and Valence Band of g‐C3N4/CoCo‐LDH to Enhance Photocatalytic CO2 Activity by High‐Efficiency S‐SchemeYi-lei Li0Qing Zhao1Xu-jia Liu2Ying Liu3Ying-juan Hao4Xiao-jing Wang5Xin-ying Liu6Diane Hildebrandt7Feng-yu Li8Fa-tang Li9Hebei Key Laboratory of Photoelectric Control on Surface and Interface College of Science Hebei University of Science and Technology Shijiazhuang 050018 ChinaHebei Key Laboratory of Photoelectric Control on Surface and Interface College of Science Hebei University of Science and Technology Shijiazhuang 050018 ChinaHebei Key Laboratory of Photoelectric Control on Surface and Interface College of Science Hebei University of Science and Technology Shijiazhuang 050018 ChinaHebei Key Laboratory of Photoelectric Control on Surface and Interface College of Science Hebei University of Science and Technology Shijiazhuang 050018 ChinaHebei Key Laboratory of Photoelectric Control on Surface and Interface College of Science Hebei University of Science and Technology Shijiazhuang 050018 ChinaHebei Key Laboratory of Photoelectric Control on Surface and Interface College of Science Hebei University of Science and Technology Shijiazhuang 050018 ChinaInstitute for the Development of Energy for African Sustainability (IDEAS) University of South Africa (UNISA) Florida 1710 South AfricaKey International Joint Laboratory of New Energy Hebei University of Science and Technology Shijiazhuang 050018 ChinaSchool of Physical Science and Technology Inner Mongolia University Hohhot 010021 ChinaHebei Key Laboratory of Photoelectric Control on Surface and Interface College of Science Hebei University of Science and Technology Shijiazhuang 050018 ChinaPrecise regulation of photogenic electron transfer path plays an important role in improving photocatalytic carbon dioxide reduction efficiency and product selectivity. Herein, under the guidance of density functional theory calculation, the interface chemical bond (CoN2 bond) at the atomic level is designed, and g‐C3N4/CoCo‐layered double hydroxide (LDH) heterostructure is manufactured. CoCo‐LDH with water oxidation ability and g‐C3N4 were combined to construct S‐scheme heterojunction with redox ability. The valence band and conduction band of g‐C3N4 and CoCo‐LDH are precisely connected by the interfacial CoN2 bond, which realizes the high‐speed transfer of electron transport. Despite the absence of cocatalyst, the heterojunction exhibits high water oxidation and carbon reduction capacity due to the precise regulation of CoN2 bonds. Theoretical calculations and experimental results show that the addition of CoCo‐LDH: reduces the oxidation overpotential of water to provide more H protons; regulates the delocalization charge of g‐C3N4; and reduces the energy barrier of the CO2 intermediate (*COOH) in the reduction half‐reaction. The results show that the selectivity of carbon‐based substances in the products was 100%, and the optimal CO yield was 71.39 μmol g−1 h−1, which is among the highest values of g‐C3N4‐based photocatalysts.https://doi.org/10.1002/sstr.202300177carbon productsCoN2 bondphotocatalytic CO2 reductionS-scheme heterojunctionswater oxidation half-reaction |
| spellingShingle | Yi-lei Li Qing Zhao Xu-jia Liu Ying Liu Ying-juan Hao Xiao-jing Wang Xin-ying Liu Diane Hildebrandt Feng-yu Li Fa-tang Li Co–N2 Bond Precisely Connects the Conduction Band and Valence Band of g‐C3N4/CoCo‐LDH to Enhance Photocatalytic CO2 Activity by High‐Efficiency S‐Scheme Small Structures carbon products CoN2 bond photocatalytic CO2 reduction S-scheme heterojunctions water oxidation half-reaction |
| title | Co–N2 Bond Precisely Connects the Conduction Band and Valence Band of g‐C3N4/CoCo‐LDH to Enhance Photocatalytic CO2 Activity by High‐Efficiency S‐Scheme |
| title_full | Co–N2 Bond Precisely Connects the Conduction Band and Valence Band of g‐C3N4/CoCo‐LDH to Enhance Photocatalytic CO2 Activity by High‐Efficiency S‐Scheme |
| title_fullStr | Co–N2 Bond Precisely Connects the Conduction Band and Valence Band of g‐C3N4/CoCo‐LDH to Enhance Photocatalytic CO2 Activity by High‐Efficiency S‐Scheme |
| title_full_unstemmed | Co–N2 Bond Precisely Connects the Conduction Band and Valence Band of g‐C3N4/CoCo‐LDH to Enhance Photocatalytic CO2 Activity by High‐Efficiency S‐Scheme |
| title_short | Co–N2 Bond Precisely Connects the Conduction Band and Valence Band of g‐C3N4/CoCo‐LDH to Enhance Photocatalytic CO2 Activity by High‐Efficiency S‐Scheme |
| title_sort | co n2 bond precisely connects the conduction band and valence band of g c3n4 coco ldh to enhance photocatalytic co2 activity by high efficiency s scheme |
| topic | carbon products CoN2 bond photocatalytic CO2 reduction S-scheme heterojunctions water oxidation half-reaction |
| url | https://doi.org/10.1002/sstr.202300177 |
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