Light olefins(C_(2)–C_(4))are fundamental building blocks for the manufacture of polymers,chemical intermediates,and solvents.In this work,we realized a composite catalyst,comprising MnxZry oxides and SAPO-34 zeolite...Light olefins(C_(2)–C_(4))are fundamental building blocks for the manufacture of polymers,chemical intermediates,and solvents.In this work,we realized a composite catalyst,comprising MnxZry oxides and SAPO-34 zeolite,which can convert syngas(CO+H_(2))into light olefins.MnxZry oxide catalysts with different Mn/Zr molar ratios were facilely prepared using the coprecipitation method prior to physical mixing with SAPO-34 zeolite.The redox properties,surface morphology,electronic state,crystal structure,and chemical elemental composition of the catalysts were examined using H_(2)-TPR,SEM,XPS,XRD,and EDS techniques,respectively.Tandem reactions involved activation of CO and subsequent hydrogenation over the metal oxide catalyst,producing methanol and dimethyl ether as the main reaction intermediates,which then migrated onto SAPO-34 zeolite for light olefins synthesis.Effects of temperature,pressure and reactant gas flow rate on CO conversion and light olefins selectivity were investigated in detail.The Mn_(1)Zr_(2)/SAPO-34 catalyst(Mn/Zr ratio of 1:2)attained a CO conversion of 10.8%and light olefins selectivity of 60.7%,at an optimized temperature,pressure and GHSV of 380℃,3 MPa and 3000h^(−1) respectively.These findings open avenues to exploit other metal oxides with CO activation capabilities for a more efficient syngas conversion and product selectivity.展开更多
基金financially supported by Youth Foundation of ZUST,China(2019QN_(2)3)and Foundation of State Key Laboratory of Highefficiency Utilization of Coal and Green Chemical Engineering(2019-KF-21).
文摘Light olefins(C_(2)–C_(4))are fundamental building blocks for the manufacture of polymers,chemical intermediates,and solvents.In this work,we realized a composite catalyst,comprising MnxZry oxides and SAPO-34 zeolite,which can convert syngas(CO+H_(2))into light olefins.MnxZry oxide catalysts with different Mn/Zr molar ratios were facilely prepared using the coprecipitation method prior to physical mixing with SAPO-34 zeolite.The redox properties,surface morphology,electronic state,crystal structure,and chemical elemental composition of the catalysts were examined using H_(2)-TPR,SEM,XPS,XRD,and EDS techniques,respectively.Tandem reactions involved activation of CO and subsequent hydrogenation over the metal oxide catalyst,producing methanol and dimethyl ether as the main reaction intermediates,which then migrated onto SAPO-34 zeolite for light olefins synthesis.Effects of temperature,pressure and reactant gas flow rate on CO conversion and light olefins selectivity were investigated in detail.The Mn_(1)Zr_(2)/SAPO-34 catalyst(Mn/Zr ratio of 1:2)attained a CO conversion of 10.8%and light olefins selectivity of 60.7%,at an optimized temperature,pressure and GHSV of 380℃,3 MPa and 3000h^(−1) respectively.These findings open avenues to exploit other metal oxides with CO activation capabilities for a more efficient syngas conversion and product selectivity.
