Fe(III)-functionalized carbon dots—Highly efficient photoluminescence redox catalyst for hydrogenations of olefins and decomposition of hydrogen peroxide

Handle URI:
http://hdl.handle.net/10754/623544
Title:
Fe(III)-functionalized carbon dots—Highly efficient photoluminescence redox catalyst for hydrogenations of olefins and decomposition of hydrogen peroxide
Authors:
Bourlinos, Athanasios B.; Rathi, Anuj K.; Gawande, Manoj B.; Hola, Katerina; Goswami, Anandarup; Kalytchuk, Sergii; Karakassides, Michael A.; Kouloumpis, Antonios; Gournis, Dimitrios; Deligiannakis, Yannis; Giannelis, Emmanuel P.; Zboril, Radek
Abstract:
We present the first bottom-up approach to synthesize Fe(III)-functionalized carbon dots (CDs) from molecular precursors without the need of conventional thermal or microwave treatment and additional reagents. Specifically, sonication of xylene in the presence of anhydrous FeCl3 results in oxidative coupling of the aromatic substrate towards Fe(III)-functionalized CDs. The as-prepared CDs are spherical in shape with a size of 3–8 nm, highly dispersible in organic solvents and display wavelength-dependent photoluminescence (PL). The iron ions attached to the surface endow the CDs with superior catalytic activity for olefin hydrogenation with excellent conversion and selectivity (up to 100%). The Fe(III)-CDs are more effective in the hydrogenation of a series of electron donating or withdrawing olefin substrates compared to conventional homogeneous or heterogeneous Fe(III)-based catalysts. The as-prepared heterogeneous nanocatalyst can be used repeatedly without any loss of catalytic activity. Importantly, the stability of the new catalysts can be easily monitored by PL intensity or quantum yield measurements, which certainly opens the doors for real time monitoring in a range of applications. Additionally, to the best of our knowledge, for the first time, the oxidative property of Fe-CDs was also explored in decomposition of hydrogen peroxide in water with the first order rate constant of 0.7 × 10−2 min−1, proving the versatile catalytic properties of such hybrid systems.
Citation:
Bourlinos AB, Rathi AK, Gawande MB, Hola K, Goswami A, et al. (2017) Fe(III)-functionalized carbon dots—Highly efficient photoluminescence redox catalyst for hydrogenations of olefins and decomposition of hydrogen peroxide. Applied Materials Today 7: 179–184. Available: http://dx.doi.org/10.1016/j.apmt.2017.03.002.
Publisher:
Elsevier BV
Journal:
Applied Materials Today
KAUST Grant Number:
KUS-C1-018-02
Issue Date:
21-Mar-2017
DOI:
10.1016/j.apmt.2017.03.002
Type:
Article
ISSN:
2352-9407
Sponsors:
The authors acknowledge the support from the Ministry of Education, Youth and Sports of the Czech Republic (LO1305 and CZ.1.05/2.1.00/19.0377), the assistance provided by the Research Infrastructure NanoEnviCz supported by the Ministry of Education, Youth and Sports of the Czech Republic under project no. LM2015073 as well as Award No. KUS-C1-018-02 made by King Abdullah University of Science and Technology (KAUST). This work was further supported by Student Project IGA_PrF_2017_025 of Palacký University. The authors also acknowledge the help of Dr. Ondrej Malina, Dr. Martin Petr, Dr. Radka Krikavova and Dr. Daikopoulos with material characterization of the samples.
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DC FieldValue Language
dc.contributor.authorBourlinos, Athanasios B.en
dc.contributor.authorRathi, Anuj K.en
dc.contributor.authorGawande, Manoj B.en
dc.contributor.authorHola, Katerinaen
dc.contributor.authorGoswami, Anandarupen
dc.contributor.authorKalytchuk, Sergiien
dc.contributor.authorKarakassides, Michael A.en
dc.contributor.authorKouloumpis, Antoniosen
dc.contributor.authorGournis, Dimitriosen
dc.contributor.authorDeligiannakis, Yannisen
dc.contributor.authorGiannelis, Emmanuel P.en
dc.contributor.authorZboril, Radeken
dc.date.accessioned2017-05-15T10:35:07Z-
dc.date.available2017-05-15T10:35:07Z-
dc.date.issued2017-03-21en
dc.identifier.citationBourlinos AB, Rathi AK, Gawande MB, Hola K, Goswami A, et al. (2017) Fe(III)-functionalized carbon dots—Highly efficient photoluminescence redox catalyst for hydrogenations of olefins and decomposition of hydrogen peroxide. Applied Materials Today 7: 179–184. Available: http://dx.doi.org/10.1016/j.apmt.2017.03.002.en
dc.identifier.issn2352-9407en
dc.identifier.doi10.1016/j.apmt.2017.03.002en
dc.identifier.urihttp://hdl.handle.net/10754/623544-
dc.description.abstractWe present the first bottom-up approach to synthesize Fe(III)-functionalized carbon dots (CDs) from molecular precursors without the need of conventional thermal or microwave treatment and additional reagents. Specifically, sonication of xylene in the presence of anhydrous FeCl3 results in oxidative coupling of the aromatic substrate towards Fe(III)-functionalized CDs. The as-prepared CDs are spherical in shape with a size of 3–8 nm, highly dispersible in organic solvents and display wavelength-dependent photoluminescence (PL). The iron ions attached to the surface endow the CDs with superior catalytic activity for olefin hydrogenation with excellent conversion and selectivity (up to 100%). The Fe(III)-CDs are more effective in the hydrogenation of a series of electron donating or withdrawing olefin substrates compared to conventional homogeneous or heterogeneous Fe(III)-based catalysts. The as-prepared heterogeneous nanocatalyst can be used repeatedly without any loss of catalytic activity. Importantly, the stability of the new catalysts can be easily monitored by PL intensity or quantum yield measurements, which certainly opens the doors for real time monitoring in a range of applications. Additionally, to the best of our knowledge, for the first time, the oxidative property of Fe-CDs was also explored in decomposition of hydrogen peroxide in water with the first order rate constant of 0.7 × 10−2 min−1, proving the versatile catalytic properties of such hybrid systems.en
dc.description.sponsorshipThe authors acknowledge the support from the Ministry of Education, Youth and Sports of the Czech Republic (LO1305 and CZ.1.05/2.1.00/19.0377), the assistance provided by the Research Infrastructure NanoEnviCz supported by the Ministry of Education, Youth and Sports of the Czech Republic under project no. LM2015073 as well as Award No. KUS-C1-018-02 made by King Abdullah University of Science and Technology (KAUST). This work was further supported by Student Project IGA_PrF_2017_025 of Palacký University. The authors also acknowledge the help of Dr. Ondrej Malina, Dr. Martin Petr, Dr. Radka Krikavova and Dr. Daikopoulos with material characterization of the samples.en
dc.publisherElsevier BVen
dc.subjectEnvironmental remediationen
dc.subjectFluorescenceen
dc.subjectGraphene quantum dotsen
dc.subjectOlefins reductionen
dc.subjectOxidative couplingen
dc.subjectRedox nanocatalysisen
dc.titleFe(III)-functionalized carbon dots—Highly efficient photoluminescence redox catalyst for hydrogenations of olefins and decomposition of hydrogen peroxideen
dc.typeArticleen
dc.identifier.journalApplied Materials Todayen
dc.contributor.institutionRegional Centre of Advanced Technologies and Materials, Department of Physical Chemistry, Faculty of Science, Palacky University, Slechtitelu 27, 783 71 Olomouc, Czech Republicen
dc.contributor.institutionPhysics Department, University of Ioannina, 45110 Ioannina, Greeceen
dc.contributor.institutionCentre of Excellence in Advanced Materials, Manufacturing, Processing and Characterization (CoExAMMPC) and Division of Chemistry, Department of Sciences and Humanities, Vignan's Foundation for Science, Technology and Research University (VFSTRU; Vignan's University), Vadlamudi, Guntur 522 213, Andhra Pradesh, Indiaen
dc.contributor.institutionMaterials Science and Engineering, University of Ioannina, 45110 Ioannina, Greeceen
dc.contributor.institutionMaterials Science and Engineering, Cornell University, 326 Bard Hall, Ithaca, NY 14853, United Statesen
kaust.grant.numberKUS-C1-018-02en
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