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Effect of additive modification on the product distribution in CO hydrogenation catalyzed by Fe/g-C3N4

  • Bing Li,
  • Xinhua Gao,
  • Kangzhou Wang,
  • Yaqin Xing,
  • Caihu Li,
  • Qingxiang Ma,
  • Tian-sheng Zhao,
  • Jianli Zhang

摘要

The melamine thermal shrinkage method was used to prepare carbon nitride (g-C3N4). Fe/g-C3N4 was obtained by impregnation, and Na, K, and Zn additives were added as modifiers. The CO hydrogenation performances of the catalysts were studied before and after modification. The effect of additive modification on the textural properties of the Fe/g-C3N4 catalyst and product distribution of CO hydrogenation was investigated by combining several characterization techniques such as N2 physical adsorption and desorption, XRD, SEM, TEM, FT-IR, TG, CO2-TPD, Raman, XPS, and contact angle (CA) experiments. The textural characteristics and performance of the catalyst were markedly affected by the additive modifications. Na and K modifications weakened the strong interactions between Fe and g-C3N4 and improved the activity of the catalyst; additionally, hydrophilicity was enhanced. The Zn modified catalyst Fe/g-C3N4-Zn exhibited a weaker water gas shift reaction activity, and a lower CO2 selectivity was obtained for CO hydrogenation. In the CO hydrogenation reaction, the Na-modified and K-modified catalysts, which exhibit enhanced surface alkalinity, inhibited secondary olefin hydrogenation and displayed high olefin selectivity and lower CH4 selectivity. Fe/g-C3N4-Na exhibited the highest olefin selectivity, with C2=–C4= up to 47.5%, and an O/P value of 5.1.

Graphical abstract