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  Pd supported on Carbon Nitride Boosts the Direct Hydrogen Peroxide Synthesis

Arrigo, R., Schuster, M. E., Abate, S., Giorgianni, G., Centi, G., Perathoner, S., et al. (2016). Pd supported on Carbon Nitride Boosts the Direct Hydrogen Peroxide Synthesis. ACS Catalysis, 6(10), 6959-6966. doi:10.1021/acscatal.6b01889.

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Arrigo, Rosa1, 2, Autor           
Schuster, Manfred Erwin1, Autor           
Abate, Salvatore3, Autor
Giorgianni, Gianfranco3, Autor
Centi, Gabriele3, Autor
Perathoner, Siglinda3, Autor
Wrabetz, Sabine1, Autor           
Pfeifer, Verena1, Autor           
Antonietti, Markus4, Autor
Schlögl, Robert1, 2, Autor           
Affiliations:
1Inorganic Chemistry, Fritz Haber Institute, Max Planck Society, ou_24023              
2Max-Planck-Institut für Chemische Energiekonversion, Stiftstrasse 34-36, 45470 Mülheim an der Ruhr, Germany, ou_persistent22              
3Università degli Studi di Messina, V.le F. Stagno D'Alcontres 31, 98166 Messina, Italy, ou_persistent22              
4Markus Antonietti, Kolloidchemie, Max Planck Institute of Colloids and Interfaces, Max Planck Society, ou_1863321              

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 Zusammenfassung: Herein, the development of an improved Pd on carbon nitride catalyst for the direct H2O2 synthesis from the elements is reported. Microcalorimetric CO chemisorption is used for characterizing the chemical speciation of the Pd selective and unselective sites. Selectivity trends among the samples suggest that a bare metal surface with a differential heat of CO chemisorption ranging between 140 and 120 kJ*mol-1 is responsible for the total O2 hydrogenation, while a maximum threshold value of differential heat of CO chemisorption of approximately 70 kJ*mol-1 is necessary for the partial hydrogenation of O2 to H2O2. Such low differential heat of CO chemisorption indicates a low exposed metallic Pd surface subjected to electron-withdrawing from the surrounding ligands, i.e. the N functional group on the carbon support. With respect to N-containing carbon nanotubes, carbon nitrides provide: higher concentration of N sites; a flexible network of π-conjugated polymeric subunits with sp3 linking subunits; a flakes-like morphology with high exposure of reactive C edge terminations. This results in a more effective kinetic stabilization of the electronically modified Pd species.

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 Datum: 2016-07-062016-09-012016-10-07
 Publikationsstatus: Erschienen
 Seiten: 18
 Ort, Verlag, Ausgabe: -
 Inhaltsverzeichnis: -
 Art der Begutachtung: Expertenbegutachtung
 Identifikatoren: DOI: 10.1021/acscatal.6b01889
 Art des Abschluß: -

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Titel: ACS Catalysis
  Kurztitel : ACS Catal.
Genre der Quelle: Zeitschrift
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Affiliations:
Ort, Verlag, Ausgabe: Washington, DC : ACS
Seiten: 8 Band / Heft: 6 (10) Artikelnummer: - Start- / Endseite: 6959 - 6966 Identifikator: Anderer: 2155-5435
CoNE: https://pure.mpg.de/cone/journals/resource/2155-5435