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Low-Temperature Methane Activation Reaction Pathways over Mechanochemically-Generated Ce<sup>4+</sup>/Cu<sup>+</sup> Interfacial Sites.

Author information

Affiliations

  • 1. TASC Laboratory, CNR- Istituto Officina dei Materiali, Trieste, 34149, Italy.
      Authors
    • Mauri S 1
    • Camellone MF 1
    • Braglia L 1
    • Fabris S 1
    • Piccinin S 1
    • Torelli P 1
    (6 authors)
  • 2. Dipartimento Politecnico and INSTM, Università degli Studi di Udine, Via del Cotonificio 108, Udine, 33100, Italy.
      Authors
    • Calligaro R 2
    • Boaro M 2
    • Trovarelli A 2
    (3 authors)
  • 3. Physics Department, Università degli Studi di Trieste, Via Alfonso Valerio 2, Trieste, 34127, Italy.
      Authors
    • Pauletti CF 3
    (1 author)

ORCIDs linked to this article

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Small (Weinheim an der Bergstrasse, Germany), 11 Jun 2024, 20(42):e2403028
https://doi.org/10.1002/smll.202403028 PMID: 38860552 

Abstract 

Methane is a valuable resource and its valorization is an important challenge in heterogeneous catalysis. Here it is shown that CeO2/CuO composite prepared by ball milling activates methane at a temperature as low as 250 °C. In contrast to conventionally prepared catalysts, the formation of partial oxidation products such as methanol and formaldehyde is also observed. Through an in situ Diffuse Reflectance Infrared Fourier Transform Spectroscopy (DRIFTS) and operando Near Edge X-Ray Absorption Fine Structure Spectroscopy (NEXAFS) approach, it can be established that this unusual reactivity can be attributed to the presence of Ce4+/Cu+ interfaces generated through a redox exchange between Ce3+ and Cu2+ atoms facilitated by the mechanical energy supplied during milling. DFT modeling of the electronic properties confirms the existence of a charge transfer mechanism. These results demonstrate the effectiveness and distinctiveness of the mechanical approach in creating unique and resilient interfaces thereby enabling the optimization and refining of CeO2/CuO catalysts in methane activation reactions.

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Read article at publisher's site: https://doi.org/10.1002/smll.202403028

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Nanoscience Foundry and Fine Analysis (1)