Operando and Postreaction Diffraction Imaging of the
La–Sr/CaO Catalyst in the Oxidative Coupling of Methane Reaction
Version 2 2019-01-24, 05:18
Version 1 2019-01-15, 14:18
Posted on 2019-01-24 - 05:18
A La–Sr/CaO
catalyst was studied operando during the oxidative
coupling of methane (OCM) reaction using the X-ray diffraction computed
tomography technique. Full-pattern Rietveld analysis was performed
in order to track the evolving solid-state chemistry during the temperature
ramp, OCM reaction, as well as after cooling to room temperature.
We observed a uniform distribution
of the catalyst main components: La2O3, CaO–SrO
mixed oxide, and the high-temperature rhombohedral polymorph of SrCO3. These were stable initially in the reaction; however, doubling
the gas hourly space velocity resulted in the decomposition of SrCO3 to SrO, which subsequently led to the formation of a second
CaO–SrO mixed oxide. These two mixed CaO–SrO oxides
differed in terms of the extent of Sr incorporation into their unit
cell. By applying Vegard’s law during the Rietveld refinement,
it was possible to create maps showing the spatial variation of Sr
occupancy in the mixed CaO–SrO oxides. The formation of the
Sr-doped CaO species is expected to have an important role in this
system through the enhancement of the lattice oxygen diffusion as
well as increased catalyst basicity.
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Matras, Dorota; D. M. Jacques, Simon; Poulston, Stephen; Grosjean, Nicolas; Estruch Bosch, Cristina; Rollins, Benjamin; et al. (2019). Operando and Postreaction Diffraction Imaging of the
La–Sr/CaO Catalyst in the Oxidative Coupling of Methane Reaction. ACS Publications. Collection. https://doi.org/10.1021/acs.jpcc.8b09018
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AUTHORS (11)
DM
Dorota Matras
SD
Simon D. M. Jacques
SP
Stephen Poulston
NG
Nicolas Grosjean
CE
Cristina Estruch Bosch
BR
Benjamin Rollins
JW
Jonathan Wright
MM
Marco Di Michiel
AV
Antonios Vamvakeros
RC
Robert J. Cernik
AB
Andrew M. Beale