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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
被引:152
作者:
Das, Sonali
[1
]
Jangam, Ashok
[1
]
Jayaprakash, Shanmukapriya
[1
]
Xi, Shibo
[2
]
Hidajat, Kus
[1
]
Tomishige, Keiichi
[3
]
Kawi, Sibudjing
[1
]
机构:
[1] Natl Univ Singapore, Dept Chem & Biomol Engn, Singapore 119260, Singapore
[2] Inst Chem & Engn Sci, A STAR, 1 Pesek Rd, Singapore 627833, Singapore
[3] Tohoku Univ, Sch Engn, Dept Appl Chem, Aoba Ku, Aoba 6-6-07, Sendai, Miyagi, Japan
关键词:
Dry reforming of methane;
Redox mechanism;
Ceria-zirconia;
Mechanism and kinetics;
Methane activation;
METAL-SUPPORT INTERACTIONS;
CARBON-DIOXIDE;
SYNTHESIS GAS;
RARE-EARTH;
SOLID-SOLUTIONS;
NI;
CO2;
CEO2;
CH4;
SURFACE;
D O I:
10.1016/j.apcatb.2021.119998
中图分类号:
O64 [物理化学(理论化学)、化学物理学];
学科分类号:
070304 ;
081704 ;
摘要:
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, O-2-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-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.
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页数:15
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