4.6 Article

Catalytic Performance of Various Zinc-Based Binary Metal Oxides/H-RUB-13 for Hydrogenation of CO2

Journal

INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
Volume 61, Issue 29, Pages 10409-10418

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acs.iecr.2c00160

Keywords

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Funding

  1. National Key R&D Program of China [2018 YFB 0 6 0 4 8 0 2, 2020YFA0210900]
  2. National Natural Science Foundation of China [U1910203, U1862101, 21991092, 21802157]
  3. Natural Science Foundation of Shanxi Province of China [201901D211581]
  4. Youth Innovation Promotion Association CAS [2021172]
  5. Autonomous research project of State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, CAS [2020BWZ004]
  6. Young Talent Training Program of State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, CAS [2021BWZ003, BK2018001]

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This research focuses on the direct formation of light olefins from CO2 hydrogenation. Bifunctional catalysts composed of zinc-based metal oxides and H-RUB-13 zeolite were prepared, and the selectivity of C2-4 olefins reached 64.7-83.2%. ZnZrOx/H-RUB-13 showed the highest CO2 conversion due to the presence of oxygen vacancies. Interestingly, propene and butene were the dominant hydrocarbons, indicating the potential of H-RUB-13 zeolite to suppress ethene formation. However, the distribution of light olefins also depended on the overall acidity of the bifunctional catalyst, with ZnCrOx/H-RUB-13 showing higher ethene selectivity.
Direct formation of light olefins (C-2(=)-C-4(=)) from CO2 hydrogenation is attractive because it decreases the greenhouse effect and gives value-added chemicals concurrently. Although it has been extensively studied and significant progress has been made, controllable regulation of light olefin distribution remains a challenge. Herein, the bifunctional catalysts composed of various zinc-based binary metal oxides and H-RUB-13 zeolite were prepared, including ZnZrOx/H-RUB-13, ZnAlOx/H-RUB-13, ZnGaOx/H-RUB-13, and ZnCrOx/H-RUB-13, and the C2-4 olefin selectivity in hydrocarbons reaches 64.7-83.2% at a CO2 conversion of 10.2-15.5%. ZnZrOx/H-RUB-13 shows the highest CO2 conversion as a result of the presence of larger amounts of oxygen vacancies that promote CO2 adsorption and activation. More interestingly, propene and butene are the dominant hydrocarbons, and C-3(=) + C-4(=) accounts for > 90% of light olefins. This confirms the potential of H-RUB-13 zeolite to suppress ethene formation. However, the distribution of light olefins also depends on the global acidic property of the bifunctional catalyst. ZnCrOx/H-RUB-13 with strong acidity shows higher ethene selectivity because of the promotion of the aromatic-based cycle.

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