Tuning selectivity in the direct conversion of methane to methanol: bimetallic synergistic effects on the cleavage of C-H and O-H bonds over NiCu/CeO₂ catalysts


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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>Lustemberg, Pablo G.</dc:creator>
  <dc:creator>Senanayake, Sanjaya D.</dc:creator>
  <dc:creator>Rodriguez, Jose A.</dc:creator>
  <dc:creator>Ganduglia-Pirovano, M. Verónica</dc:creator>
  <dc:date>2022-06-10</dc:date>
  <dc:description>The efficient activation of methane and simultaneous water dissociation are crucial in many catalytic reactions on oxide-supported transition metal catalysts. On very low-loaded Ni/CeO₂ surfaces, methane easily fully decomposes, CH₄ -&gt; C + 4H,  and water dissociates, H₂O -&gt; OH + H. However, in important reactions such as the direct oxidation of methane to methanol (MTM), where complex interplay exists between reactants (CH₄, O₂), it is desirable to avoid the complete dehydrogenation of methane to carbon.  Remarkably, the barrier for the activation of C-H bonds in CHx (x= 1-3) species on Ni/CeO₂ surfaces can be manipulated by adding Cu, forming bimetallic NiCu clusters, whereas the ease for cleavage of O-H bonds in water, is not affected by ensemble effects, as obtained from density functional theory-based calculations. CH4 activation occurs only on Ni sites and H₂O activation on both Ni and Cu sites. The MTM reaction pathway for the example of the Ni₃Cu₁/CeO₂ model catalyst predict higher selectivity and a lower activation barrier for methanol production, compared with that for Ni₄-CeO₂. These findings point toward a possible strategy to design active and stable catalysts which can be employed for methane activation and conversions.</dc:description>
  <dc:identifier>https://archive.materialscloud.org/record/2022.75</dc:identifier>
  <dc:identifier>doi:10.24435/materialscloud:8y-7m</dc:identifier>
  <dc:identifier>mcid:2022.75</dc:identifier>
  <dc:identifier>oai:materialscloud.org:1376</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>bimetallic</dc:subject>
  <dc:subject>ceria</dc:subject>
  <dc:subject>methane activation</dc:subject>
  <dc:subject>water activation</dc:subject>
  <dc:title>Tuning selectivity in the direct conversion of methane to methanol: bimetallic synergistic effects on the cleavage of C-H and O-H bonds over NiCu/CeO₂ catalysts</dc:title>
  <dc:type>Dataset</dc:type>
</oai_dc:dc>