Das, S.; Jangam, A.; Jayaprakash, S.; Xi, S. B.; Hidajat, K.; Tomishige, K.; Kawi, S., Role of lattice oxygen in methane activation on Ni-phyllosilicate@Ce1-xZrxO2 core-shell catalyst for methane dry reforming: Zr doping effect, mechanism, and kinetic study. Applied Catalysis B: Environmental 2021, 290, Article no.: 119998, DOI: 10.1016/j.apcatb.2021.119998.
Sandwich structured core-shell Ni-Phyllosilicate@Ce1-xZrxO2 catalysts with high coke resistance and activity are reported for DRM. Optimal Zr loading (x = 0.05 – 0.1) in the Ce1-xZrxO2 shell is observed to significantly increase the intrinsic activity for DRM. Extensive catalyst characterization using HRTEM, XRD, TPR, O2-TPD, XPS, EXAFS and CO pulse chemisorption indicates that the enhancement in DRM activity upon Zr doping can be attributed to the increase in lattice oxygen mobility of the ceria-zirconia shell and stronger metal-support interaction with Ni. It is inferred from a rigorous kinetic and mechanism study that the lattice oxygen of Ce1-xZrxO2 not only participates in the oxidation of carbonaceous reaction intermediates but also facilitates the rate determining step of Csingle bondH bond dissociation of CH4 on Ni by an oxygen-mediated dissociation pathway. The involvement of lattice oxygen in methane activation and dissociation manifests in the higher DRM activity of the Zr-doped catalyst with maximum oxygen storage capacity.
This research / project is supported by the National Environment Agency (NEA), Singapore - Environment Technology Research Programme (ETRP)
Grant Reference no. : NEA-ETRP Grant 1501 103
This research / project is supported by the Agency for Science, Technology and Research (A*STAR) - Advanced Manufacturing and Engineering Individual Research Grant (AME IRG)
Grant Reference no. : A1783c0016
This research / project is supported by the Ministry of Education, Singapore - -
Grant Reference no. : MOE2017-T2-2-130