4.7 Article

Insight into deactivation of the carbon-/sintering-resistant Ni@Silicalite-1 for catalytic partial oxidation of methane to syngas

期刊

FUEL
卷 320, 期 -, 页码 -

出版社

ELSEVIER SCI LTD
DOI: 10.1016/j.fuel.2022.123892

关键词

Partial oxidation of methane; Syngas; Nickel catalyst; Silicalite-1; Nickel phyllosilicate

资金

  1. National Natural Science Foundation of China [22072043, 21773069, 21703069]
  2. Key Basic Research Project from the Shanghai Municipal Science and Technology Commission, China [18JC1412100]

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Ni-based catalysts with Ni nanoparticles embedded in S-1 zeolite show high activity/selectivity and resistance to carbon deposition and Ni-sintering. However, they still suffer from deactivation due to the formation of a dense Ni-3(Si2O5)(2)(OH)(2) layer that blocks the contact between Ni and reactants.
Ni-based catalysts show good activity and selectivity for the catalytic partial oxidation of methane (CPOM) to syngas, but still suffer from carbon deposition and Ni-sintering. Herein, Ni nanoparticles of 3-7 nm are successfully embedded inside the crystal of silicalite-1 (S-1) zeolite via one-pot hydrothermal synthesis. The Ni@S-1 catalysts, with high activity/selectivity, show high carbon-/sintering-resistance but still deactivates fast. The surface of Ni nanoparticles involved in the reaction is oxidized to form intermediate NiO species, which may react with the circumambient SiO2 (from S-1) in the presence of water vapor (by-product and/or intermediate-product of CPOM reaction) to form a dense Ni-3(Si2O5)(2)(OH)(2) layer around Ni nanoparticles. The formed Ni-3(Si2O5)(2)(OH)(2) compounds are hard to be reduced (even in H-2 at 800 degrees C; thus losing capacity to involve catalytic reaction cycle) while completely blocking the Ni-0 sites from contacting with reactants, which is the main cause for the Ni@S-1 deactivation. Not surprisingly, such deactivation problem can be solved easily by replacing Ni with highly anti-oxidative metals such as Rh.

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