Direct Conversion of Syngas into Light Olefins over Zirconium‐Doped Indium(III) Oxide and SAPO‐34 Bifunctional Catalysts: Design of Oxide Component and Construction of Reaction Network
- 27 February 2018
- journal article
- research article
- Published by Wiley in ChemCatChem
- Vol. 10 (7) , 1536-1541
Abstract
The direct synthesis of light olefins from syngas over a bifunctional catalyst containing an oxide and zeolite has been proven to be a promising strategy. Nevertheless, an unclear reaction network hinders any further enhancement in catalytic performance, such as increasing the conversion of CO. We herein report a novel bifunctional catalyst composed of a InZr binary oxide and SAPO‐34 zeolite displaying superior CO conversion (27.7 %) with selectivity to light olefins (73.6 %) at 400 °C, 2.0 MPa. We demonstrate that the Zr‐doped body‐centered cubic In2O3 phase, exhibiting higher stability than pure In2O3 under a reducing atmosphere, is the active oxide component for the initial activation of CO. A complete reaction network is proposed by DFT calculations and model reactions, revealing that CO activation over Zr‐In2O3 follows a quasi‐CO2 hydrogenation pathway and methanol is the key intermediate to be transformed into light olefins in zeolites. Moreover, inhibiting excessive hydrogenation is an effective strategy to achieve higher performance.Keywords
Funding Information
- China Postdoctoral Science Foundation (2017M611644, 2016M600348)
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