1. Supported PdZn nanoparticles for selective CO2 conversion, through the grafting of a heterobimetallic complex on CeZrOx.
- Author
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Ruzzi, Paolo, Salusso, Davide, Baravaglio, Matilde, Szeto, Kai C., De Mallmann, Aimery, Jiménez, Laia Gil, Godard, Cyril, Benayad, Anass, Morandi, Sara, Bordiga, Silvia, and Taoufik, Mostafa
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HETEROBIMETALLIC complexes , *FISCHER-Tropsch process , *CARBON dioxide , *CATALYST poisoning , *CERIUM oxides , *NANOPARTICLES - Abstract
Controlling the stoichiometry of supported bimetallic nanoparticles is essential in many catalytic reactions, notably selective CO 2 hydrogenation. Thus, a new strategy to ensure the preferred stoichiometry (1:1) of supported bimetallic PdZn nanoparticles is presented, involving the deposition of a heterobimetallic precursor, [PdZn(μ-OOCMe) 4 ] 2 on a CeZrO x support. After calcination and reduction, the material contained mainly a PdZn alloy, as revealed by powder XRD and XAFS, and further supported by XPS, TEM-EDX, elemental analysis and in-situ IR at low temperature using CO as probe molecule. Moreover, a minor phase of oxidized Zn was determined by XAFS. This PdZn/CeZrOx reduced catalyst was combined with SAPO-34 to form a tandem catalytic system for CO 2 conversion to hydrocarbons. This system could readily convert CO 2 and H 2 at high temperature (380 °C) into hydrocarbons with a conversion of 24% and high relative selectivity in light hydrocarbons (C2–C3: 82%) with virtually no deactivation of the catalyst after 16 h on stream. Controlled experiments were performed with Pd/CeZrOx and Zn/CeZrOx in order to gain supplementary insights on this system: Pd/CeZrOx gave only methane and Zn/CeZrOx gave mainly CO under the same conditions. The latter clearly shows that the control of the formation of PdZn phase has great impact for the selective production of hydrocarbons. [Display omitted] • Development of PdZn supported on CeO 2 , ZrO 2 and CeZrOx for the conversion of CO 2 to methanol. • Catalyst PdZn/CeZrOx presents highly dispersed bimetallic PdZn nanoparticles with 1:1 ratio. • CO 2 conversion to light hydrocarbons is studied over tandem catalysts comprising PdZn supported on oxide and SAPO-34. • PdZn/CeZrOx/SAPO-34 catalysts present high CO 2 conversion and selectivity in light hydrocabons. [ABSTRACT FROM AUTHOR]
- Published
- 2022
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