Unraveling the role of GaZrOx structure and oxygen vacancy in bifunctional catalyst for highly active and selective conversion of syngas into light olefins

Abstract

The direct conversion of syngas to light olefins (STO) over metal oxide-zeolite (OX-ZEO) bifunctional catalyst has aroused wide interest. However, due to unmatched reaction temperature for CO conversion to oxygenated hydrocarbons over metal oxide (200–300 °C) and C−C coupling reaction over zeolite (350–450 °C), it is still a great challenge to achieve both high light olefins selectivity and high CO conversion; moreover, the reaction mechanism needs to be further studied. Herein, the Ga-Zr oxide is taken as a probe oxide to mix with SAPO-34 zeolite for STO. A high light olefins selectivity of 88.6% is achieved at an extremely high CO conversion of 51.6% with a stable activity for 200 h. The incorporation of Ga into ZrO2 generates the GaZrOx solid solution structure with abundant concentration of oxygen vacancy and hydroxy group, the strong synergetic effect between Ga and Zr in GaZrOx benefits the CO activation and CH3O* formation at high temperatures (280–430 °C), providing a compatible temperature match for C−C coupling over SAPO-34. The GaZrOx is a promising and potential catalyst for industrial application in direct conversion of syngas to olefins, aromatics, and liquid fuels.