4.6 Article

Exploring the Zn-regulated function in Co-Zn catalysts for efficient hydrogenation of ethyl levulinate to γ-valerolactone

Journal

CATALYSIS SCIENCE & TECHNOLOGY
Volume 12, Issue 13, Pages 4325-4338

Publisher

ROYAL SOC CHEMISTRY
DOI: 10.1039/d2cy00244b

Keywords

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Funding

  1. National Natural Science Foundation of China [31760190, 11764026, 21531003, 21501024, 21971035]
  2. Yunnan Provincial Department of Science and Technology [202101BD070001-007]
  3. Young and Middle-aged Academic and Technical Leaders Project in Yunnan Province [202105AC160129]
  4. Science and Technology Planning Project of Yunnan Province [202001AT070080]
  5. Yunnan Provincial Department of Education Fund [2020J0399]
  6. Jilin Scientific and Technological Development Program [20170101198JC, 20190103017JH]
  7. Jilin Education Office [JJKH20180015KJ]
  8. Opening Project of Key Laboratory of Polyoxometalate and Reticular Material Chemistry of Ministry of Education
  9. Key Laboratory of State Forestry Administration for Highly-Efficient Utilization of Forestry Biomass Resources in Southwest China [2020-KF12, 2020-KF13]

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In this study, a series of CoZn catalysts with controlled Zn content were prepared and investigated for the catalytic hydrogenation of biomass-based ethyl levulinate. The results show that the optimum Zn content significantly enhances the activity and stability of the catalyst, and influences the structural characteristics, dispersion of active sites, and mass transfer of the substrate.
A series of CoZn catalysts supported on N-doped porous carbon (CoxZny@NPC-T) with controlled Zn content prepared at different calcination temperatures are studied for catalytic hydrogenation of biomass-based ethyl levulinate to gamma-valerolactone, in which Zn is introduced as a regulator. The catalytic activity of optimum Co3Zn1@NPC-600 is 13 times higher than that of Co@NPC-600. The high activity of the catalyst is attributed to the Zn content: the amount of Zn not only regulates the content of active Co(0) and promotes the activation of hydrogen, but also affects the content of acidic sites and optimizes the adsorption of intermediates. Meanwhile, the content of Zn will also optimize the structural characteristics of the catalyst, thereby increasing the dispersion of active sites and mass transfer of the substrate. The regulated function of the Zn content, including electronic effects, acid site effects and size effects, is discussed in detail. In addition, the doping of Zn also helps to improve the stability of cycling performance. The strategy of adjusting the catalytic performance by the doping content provides support and examples for the rational design of highly active and stable catalysts.

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