TY - JOUR
T1 - Feasibility of Methane Oxidation on SSZ-13 Bridged Pd2OxSites
T2 - A Theoretical Study
AU - Canavan, Jesse
AU - Giewont, Kevin
AU - Kyriakidou, Eleni A.
AU - Walker, Eric A.
N1 - Publisher Copyright:
© 2022 American Chemical Society.
PY - 2022/10/13
Y1 - 2022/10/13
N2 - In this theoretical work, bridged Pd2Ox active sites on SSZ-13 are investigated for the feasibility of methane oxidation. An in-depth reaction mechanism was derived using density functional theory (DFT), and a portion of it was simulated with a microkinetic model. For |PdO2Pd| and |PdOPd|, which are bridge active sites within the zeolite framework, it was found that at 350 °C the rate-limiting step is water formation and not methane activation, which is usually assumed to be the rate-limiting step on similar active sites. Partial oxidation of methane to methanol was also investigated and was found to introduce large activation barriers that are likely too large to surpass.
AB - In this theoretical work, bridged Pd2Ox active sites on SSZ-13 are investigated for the feasibility of methane oxidation. An in-depth reaction mechanism was derived using density functional theory (DFT), and a portion of it was simulated with a microkinetic model. For |PdO2Pd| and |PdOPd|, which are bridge active sites within the zeolite framework, it was found that at 350 °C the rate-limiting step is water formation and not methane activation, which is usually assumed to be the rate-limiting step on similar active sites. Partial oxidation of methane to methanol was also investigated and was found to introduce large activation barriers that are likely too large to surpass.
UR - https://www.scopus.com/pages/publications/85139651240
UR - https://www.scopus.com/pages/publications/85139651240#tab=citedBy
U2 - 10.1021/acs.jpcc.2c06086
DO - 10.1021/acs.jpcc.2c06086
M3 - Article
AN - SCOPUS:85139651240
SN - 1932-7447
VL - 126
SP - 17123
EP - 17134
JO - Journal of Physical Chemistry C
JF - Journal of Physical Chemistry C
IS - 40
ER -