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<p>Cycloalkanes and cyclohexanols find diverse applications, including sustainable aviation fuel, fuel additives, and value-added chemicals. These compounds can be produced via complete or selective hydrodeoxygenation (HDO) of lignin-derived phenolic monomers. In this study, a urea-assisted method was employed to control the size of Ru nanoparticles (NPs) and tune the surface-active sites on Ru metal supported on CN<sub><i>x</i></sub>. By adjusting the Ru-to-urea molar ratio, both the size of Ru NPs and the metallic-to-oxide ratio of Ru were controlled, along with the incorporation of N atoms into the RuO<sub>2</sub> surface coordination. In the absence of urea, the Ru/CN<sub><i>x</i></sub>(1:0) catalyst, containing 4.8 nm Ru NPs, achieved complete HDO of 4-propyl guaiacol to <i>n</i>-propyl cyclohexane through ring saturation, followed by hydro-demethoxylation of the C–OCH<sub>3</sub> group, and hydrogenolysis of the–OH group, with a 97.0% yield at an initial H<sub>2</sub> pressure of 1.5 MPa, 200 °C, and 20 h in water. The final hydrogenolysis step was inhibited over the urea-assisted catalysts. The Ru/CN<sub><i>x</i></sub>(1:8) catalyst, containing 3.1 nm Ru NPs, achieved a maximum selectivity of 67.6% for <i>n</i>-propyl cyclohexanol, along with complete conversion of 4-propyl guaiacol. Similar trends were observed in the product distribution when upgrading reductive catalytic fractionation bio-oil over Ru/CN<sub><i>x</i></sub>(1:0) and Ru/CN<sub><i>x</i></sub>(1:8).</p>

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Tuning surface-active sites of Ru catalysts for the selective deoxygenation of lignin monomers to fuels and chemicals

  • 期刊论文

  • 发表日期：

    2025年2月8日

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  • Rizky Gilang Kurniawan,
  • Jongho Choi,
  • Neha Karanwal,
  • Seung Min Kim,
  • Seok Ki Kim,
  • Deepak Verma,
  • Jaehoon Kim

摘要

Cycloalkanes and cyclohexanols find diverse applications, including sustainable aviation fuel, fuel additives, and value-added chemicals. These compounds can be produced via complete or selective hydrodeoxygenation (HDO) of lignin-derived phenolic monomers. In this study, a urea-assisted method was employed to control the size of Ru nanoparticles (NPs) and tune the surface-active sites on Ru metal supported on CNx. By adjusting the Ru-to-urea molar ratio, both the size of Ru NPs and the metallic-to-oxide ratio of Ru were controlled, along with the incorporation of N atoms into the RuO2 surface coordination. In the absence of urea, the Ru/CNx(1:0) catalyst, containing 4.8 nm Ru NPs, achieved complete HDO of 4-propyl guaiacol to n-propyl cyclohexane through ring saturation, followed by hydro-demethoxylation of the C–OCH3 group, and hydrogenolysis of the–OH group, with a 97.0% yield at an initial H2 pressure of 1.5 MPa, 200 °C, and 20 h in water. The final hydrogenolysis step was inhibited over the urea-assisted catalysts. The Ru/CNx(1:8) catalyst, containing 3.1 nm Ru NPs, achieved a maximum selectivity of 67.6% for n-propyl cyclohexanol, along with complete conversion of 4-propyl guaiacol. Similar trends were observed in the product distribution when upgrading reductive catalytic fractionation bio-oil over Ru/CNx(1:0) and Ru/CNx(1:8).