SCI和EI收录∣中国化工学会会刊

中国化学工程学报 ›› 2021, Vol. 36 ›› Issue (8): 101-110.DOI: 10.1016/j.cjche.2020.09.004

• Catalysis, Kinetics and Reaction Engineering • 上一篇    下一篇

One-step conversion of syngas to light olefins over bifunctional metal-zeolite catalyst

Ce Du1,2, Linet Gapu Chizema1, Emmerson Hondo1, Mingliang Tong1, Qingxiang Ma3, Xinhua Gao3, Ruiqin Yang1, Peng Lu1, Noritatsu Tsubaki2   

  1. 1 Zhejiang Provincial Key Lab for Chem. & Bio. Processing Technology of Farm Product, School of Biological and Chemical Engineering, Zhejiang University of Science and Technology, Hangzhou 310023, China;
    2 Department of Applied Chemistry, School of Engineering, University of Toyama, Gofuku 3190, Toyama 930-8555, Japan;
    3 State Key Laboratory Cultivation Base of Natural Gas Conversion, Ningxia University, Yinchuan 750021, China
  • 收稿日期:2020-04-28 修回日期:2020-08-11 出版日期:2021-08-28 发布日期:2021-09-30
  • 通讯作者: Peng Lu, Noritatsu Tsubaki
  • 基金资助:
    This research is financially supported by Youth Foundation of ZUST, China (2019QN23) and Foundation of State Key Laboratory of Highefficiency Utilization of Coal and Green Chemical Engineering (2019-KF-21).

One-step conversion of syngas to light olefins over bifunctional metal-zeolite catalyst

Ce Du1,2, Linet Gapu Chizema1, Emmerson Hondo1, Mingliang Tong1, Qingxiang Ma3, Xinhua Gao3, Ruiqin Yang1, Peng Lu1, Noritatsu Tsubaki2   

  1. 1 Zhejiang Provincial Key Lab for Chem. & Bio. Processing Technology of Farm Product, School of Biological and Chemical Engineering, Zhejiang University of Science and Technology, Hangzhou 310023, China;
    2 Department of Applied Chemistry, School of Engineering, University of Toyama, Gofuku 3190, Toyama 930-8555, Japan;
    3 State Key Laboratory Cultivation Base of Natural Gas Conversion, Ningxia University, Yinchuan 750021, China
  • Received:2020-04-28 Revised:2020-08-11 Online:2021-08-28 Published:2021-09-30
  • Contact: Peng Lu, Noritatsu Tsubaki
  • Supported by:
    This research is financially supported by Youth Foundation of ZUST, China (2019QN23) and Foundation of State Key Laboratory of Highefficiency Utilization of Coal and Green Chemical Engineering (2019-KF-21).

摘要: Light olefins (C2-C4) 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 + H2) 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 H2-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 Mn1Zr2/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 3000 h-1 respectively. These findings open avenues to exploit other metal oxides with CO activation capabilities for a more efficient syngas conversion and product selectivity.

关键词: Catalyst, C—C coupling, CO activation, Hydrogenation, Light olefins, Syngas

Abstract: Light olefins (C2-C4) 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 + H2) 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 H2-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 Mn1Zr2/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 3000 h-1 respectively. These findings open avenues to exploit other metal oxides with CO activation capabilities for a more efficient syngas conversion and product selectivity.

Key words: Catalyst, C—C coupling, CO activation, Hydrogenation, Light olefins, Syngas