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<p>Here, a solvothermal method was utilized to prepare Co<sub>3</sub>O<sub>4</sub> with diverse values of adsorbed oxygen/lattice oxygen (O<sub>ads</sub>/O<sub>latt</sub>) and low-temperature reducibility by modulating H<sub>2</sub>O/CH<sub>3</sub>CH<sub>2</sub>OH solvent ratio. As the ethanol content increases, both O<sub>ads</sub>/O<sub>latt</sub> ratio and redox ability exhibit a marked progressive promotion owing to the rapid formation of Co(OH)<sub>2</sub> precipitation inhibited by ethanol. Compared to O<sub>ads</sub>/O<sub>latt</sub> ratio, low-temperature redox ability exhibits a stronger correlation with propane reaction rate at 210&#xa0;°C (R<sup>2</sup> = 0.97 vs 0.69), establishing it as the primary factor governing the reaction kinetics of low-temperature propane oxidation. Additionally, in-situ DRIFTS demonstrates that accelerated redox cycle of Co<sup>3+</sup>/Co<sup>2+</sup> drives the reaction pathway for propane oxidation: CH<sub>3</sub>CH<sub>2</sub>CH<sub>3</sub> → CH<sub>2</sub>CHCH<sub>3</sub> → CH<sub>2</sub>CHCOOH → CO<sub>3</sub><sup>2−</sup> → CO<sub>2</sub>. As a result, Co<sub>3</sub>O<sub>4</sub>-40 (H<sub>2</sub>O/CH<sub>3</sub>CH<sub>2</sub>OH solvent ratio = 0/40) displays a prominent excellent and competitive propane oxidation activity (R<sub>210°C</sub> = 3.42&#xa0;μmol g<sub>cat</sub><sup>−1</sup>&#xa0;s<sup>−1</sup>).</p>

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Accelerating the Co3+/Co2+ redox cycle of Co3O4 by solvent manipulation in solvothermal synthesis to drive propane oxidation at low temperature

  • 期刊论文

  • 发表日期：

    2026年1月20日

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  • Daifeng Lin,
  • Jiaqi Chen,
  • Chengkai Tang,
  • Fuhai Liu,
  • Manlin Zhou,
  • Zeyang Lu,
  • Wei Li,
  • Qian Zhuo,
  • Wenqing Yang,
  • Yongjin Luo

摘要

Here, a solvothermal method was utilized to prepare Co3O4 with diverse values of adsorbed oxygen/lattice oxygen (Oads/Olatt) and low-temperature reducibility by modulating H2O/CH3CH2OH solvent ratio. As the ethanol content increases, both Oads/Olatt ratio and redox ability exhibit a marked progressive promotion owing to the rapid formation of Co(OH)2 precipitation inhibited by ethanol. Compared to Oads/Olatt ratio, low-temperature redox ability exhibits a stronger correlation with propane reaction rate at 210 °C (R2 = 0.97 vs 0.69), establishing it as the primary factor governing the reaction kinetics of low-temperature propane oxidation. Additionally, in-situ DRIFTS demonstrates that accelerated redox cycle of Co3+/Co2+ drives the reaction pathway for propane oxidation: CH3CH2CH3 → CH2CHCH3 → CH2CHCOOH → CO32− → CO2. As a result, Co3O4-40 (H2O/CH3CH2OH solvent ratio = 0/40) displays a prominent excellent and competitive propane oxidation activity (R210°C = 3.42 μmol gcat−1 s−1).