TY - JOUR
T1 - Role of lattice oxygen in methane activation on Ni-phyllosilicate@Ce1-xZrxO2 core-shell catalyst for methane dry reforming
T2 - Zr doping effect, mechanism, and kinetic study
AU - Das, Sonali
AU - Jangam, Ashok
AU - Jayaprakash, Shanmukapriya
AU - Xi, Shibo
AU - Hidajat, Kus
AU - Tomishige, Keiichi
AU - Kawi, Sibudjing
N1 - Funding Information:
The research was supported by the National Environmental Agency of Singapore (NEA-ETRP Grant 1501 103),A*STAR (AME-IRG A1783c0016), and the Ministry of Education of Singapore (MOE2017-T2-2-130). The authors also gratefully thank the National University of Singapore for supporting the research.
Funding Information:
The research was supported by the N ational Environmental Agency of Singapore (NEA-ETRP Grant 1501 103), A*STAR ( AME-IRG A1783c0016) , and the Ministry of Education of Singapore ( MOE2017-T2-2-130) . The authors also gratefully thank the National University of Singapore for supporting the research.
Publisher Copyright:
© 2021
PY - 2021/8/5
Y1 - 2021/8/5
N2 - 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 C[sbnd]H 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.
AB - 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 C[sbnd]H 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.
KW - Ceria-zirconia
KW - Dry reforming of methane
KW - Mechanism and kinetics
KW - Methane activation
KW - Redox mechanism
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U2 - 10.1016/j.apcatb.2021.119998
DO - 10.1016/j.apcatb.2021.119998
M3 - Article
AN - SCOPUS:85101857151
SN - 0926-3373
VL - 290
JO - Applied Catalysis B: Environmental
JF - Applied Catalysis B: Environmental
M1 - 119998
ER -