Regulation of functional groups on graphene quantum dots directs selective CO2 to CH4 conversion

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dc.citation.firstpage5265en_US
dc.citation.journalTitleNature Communicationsen_US
dc.citation.volumeNumber12en_US
dc.contributor.authorZhang, Tianyuen_US
dc.contributor.authorLi, Weitaoen_US
dc.contributor.authorHuang, Kaien_US
dc.contributor.authorGuo, Huazhangen_US
dc.contributor.authorLi, Zhengyuanen_US
dc.contributor.authorFang, Yanboen_US
dc.contributor.authorYadav, Ram Manoharen_US
dc.contributor.authorShanov, Vesselinen_US
dc.contributor.authorAjayan, Pulickel M.en_US
dc.contributor.authorWang, Liangen_US
dc.contributor.authorLian, Chengen_US
dc.contributor.authorWu, Jingjieen_US
dc.date.accessioned2021-09-23T17:11:37Zen_US
dc.date.available2021-09-23T17:11:37Zen_US
dc.date.issued2021en_US
dc.description.abstractA catalyst system with dedicated selectivity toward a single hydrocarbon or oxygenate product is essential to enable the industrial application of electrochemical conversion of CO2 to high-value chemicals. Cu is the only known metal catalyst that can convert CO2 to high-order hydrocarbons and oxygenates. However, the Cu-based catalysts suffer from diverse selectivity. Here, we report that the functionalized graphene quantum dots can direct CO2 to CH4 conversion with simultaneous high selectivity and production rate. The electron-donating groups facilitate the yield of CH4 from CO2 electro-reduction while electron-withdrawing groups suppress CO2 electro-reduction. The yield of CH4 on electron-donating group functionalized graphene quantum dots is positively correlated to the electron-donating ability and content of electron-donating group. The graphene quantum dots functionalized by either –OH or –NH2 functional group could achieve Faradaic efficiency of 70.0% for CH4 at −200 mA cm−2 partial current density of CH4. The superior yield of CH4 on electron-donating group- over the electron-withdrawing group-functionalized graphene quantum dots possibly originates from the maintenance of higher charge density of potential active sites (neighboring C or N) and the interaction between the electron-donating group and key intermediates. This work provides insight into the design of active carbon catalysts at the molecular scale for the CO2 electro-reduction.en_US
dc.identifier.citationZhang, Tianyu, Li, Weitao, Huang, Kai, et al.. "Regulation of functional groups on graphene quantum dots directs selective CO2 to CH4 conversion." <i>Nature Communications,</i> 12, (2021) Springer Nature: 5265. https://doi.org/10.1038/s41467-021-25640-1.en_US
dc.identifier.digitals41467-021-25640-1en_US
dc.identifier.doihttps://doi.org/10.1038/s41467-021-25640-1en_US
dc.identifier.urihttps://hdl.handle.net/1911/111406en_US
dc.language.isoengen_US
dc.publisherSpringer Natureen_US
dc.rightsThis article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/.en_US
dc.rights.urihttp://creativecommons.org/licenses/by/4.0/.en_US
dc.titleRegulation of functional groups on graphene quantum dots directs selective CO2 to CH4 conversionen_US
dc.typeJournal articleen_US
dc.type.dcmiTexten_US
dc.type.publicationpublisher versionen_US
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