From Methane to Methanol: Pd-iC-CeO2 Catalysts Engineered for High Selectivity via Mechano-Chemical Synthesis

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<oai_dc:dc xmlns:dc="http://purl.org/dc/elements/1.1/" xmlns:oai_dc="http://www.openarchives.org/OAI/2.0/oai_dc/" xmlns:xsi="http://www.w3.org/2001/XMLSchema-instance" xsi:schemaLocation="http://www.openarchives.org/OAI/2.0/oai_dc/ http://www.openarchives.org/OAI/2.0/oai_dc.xsd">
  <dc:creator>Jiménez, Juan D.</dc:creator>
  <dc:creator>Lustemberg, Pablo G.</dc:creator>
  <dc:creator>Danielis, Maila</dc:creator>
  <dc:creator>Fernández-Villanueva, Estefanía</dc:creator>
  <dc:creator>Hwang, Sooyeon</dc:creator>
  <dc:creator>Waluyo, Iradwikanari</dc:creator>
  <dc:creator>Hunt, Adrian</dc:creator>
  <dc:creator>Wierzbicki, Dominik</dc:creator>
  <dc:creator>Zhang, Jie</dc:creator>
  <dc:creator>Qi, Long</dc:creator>
  <dc:creator>Trovarelli, Alessandro</dc:creator>
  <dc:creator>Rodriguez, Jose A.</dc:creator>
  <dc:creator>Colussi, Sara</dc:creator>
  <dc:creator>Ganduglia-Pirovano, M. Verónica</dc:creator>
  <dc:creator>Senanayake, Sanjaya D.</dc:creator>
  <dc:date>2024-08-06</dc:date>
  <dc:description>In the pursuit of selective conversion of methane directly to methanol in the liquid phase, a common challenge is the concurrent formation of undesirable liquid oxygenates or combustion byproducts. However, we demonstrate that monometallic Pd-CeO2 catalysts, modified by carbon, created by a simple mechanochemical synthesis method exhibit 100% selectivity towards methanol at 75°C, using hydrogen peroxide as oxidizing agent. The solvent-free synthesis yields a distinctive Pd-iC-CeO2 interface, where interfacial carbon (iC) modulates metal-oxide interactions and facilitates tandem methane activation and peroxide decomposition, thus resulting in an exclusive methanol selectivity of 100% with a rate of 117 µmol/gcat at 75°C. Notably, solvent interactions of H2O2 (aq) were found to be critical for methanol selectivity through a DFT-simulated Eley-Rideal-like mechanism. This mechanism uniquely enables the direct conversion of methane into methanol via a solid-liquid-gas process.</dc:description>
  <dc:identifier>https://materialscloud-archive-failover.cineca.it/record/2024.117</dc:identifier>
  <dc:identifier>doi:10.24435/materialscloud:dz-zz</dc:identifier>
  <dc:identifier>mcid:2024.117</dc:identifier>
  <dc:identifier>oai:materialscloud.org:2281</dc:identifier>
  <dc:language>en</dc:language>
  <dc:publisher>Materials Cloud</dc:publisher>
  <dc:rights>info:eu-repo/semantics/openAccess</dc:rights>
  <dc:rights>Creative Commons Attribution 4.0 International https://creativecommons.org/licenses/by/4.0/legalcode</dc:rights>
  <dc:subject>Pd.CeO2</dc:subject>
  <dc:subject>PdC.CeO2</dc:subject>
  <dc:subject>CH4</dc:subject>
  <dc:subject>CH3OH</dc:subject>
  <dc:subject>H2O2</dc:subject>
  <dc:subject>Eley-Rideal mechanism</dc:subject>
  <dc:title>From Methane to Methanol: Pd-iC-CeO2 Catalysts Engineered for High Selectivity via Mechano-Chemical Synthesis</dc:title>
  <dc:type>Dataset</dc:type>
</oai_dc:dc>