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

来源：

APPLIED CATALYSIS B-ENVIRONMENTAL | 2021年 / 290卷

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.

引用

页数：15

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