Abstract <p>Methane, a potent greenhouse gas, poses a significant risk when released into the environment. In this work, a Pd/SiO<sub>2</sub>@CeO<sub>2</sub> catalyst was developed and evaluated for its methane oxidation performance under oxygen-rich environments. The 2.5 wt % Pd/SiO<sub>2</sub>@CeO<sub>2</sub> achieved 10, 50, and 90% CH<sub>4</sub> conversion at 225°C (<i>T</i><sub>10</sub>), 257°C (<i>T</i><sub>50</sub>), and 275°C (<i>T</i><sub>90</sub>). The 2.5 wt % Pd/CeO<sub>2</sub> was used as the reference catalyst that attained CH<sub>4</sub> conversion of 50 and 90% at comparatively higher temperatures of 300 and 350°C under identical reaction conditions. Decreasing the Pd loading in Pd/SiO<sub>2</sub>@CeO<sub>2</sub> to 1 wt % increased the <i>T</i><sub>10</sub>, <i>T</i><sub>50</sub>, and <i>T</i><sub>90</sub> to 257, 300, and 350°C, respectively. Furthermore, in a steady-state experiment of 10 h at 350°C, 2.5 wt % Pd/SiO<sub>2</sub>@CeO<sub>2</sub> exhibited excellent durability, sustaining a ≥95% CH<sub>4</sub> conversion without noticeable deactivation. In addition, variation in O<sub>2</sub> (0.5–8%) and CH<sub>4</sub> (0.11–0.5%) concentrations, and gas hourly space velocity (GHSV) between 48 000–58 000 mL g<sup>–1</sup> h<sup>–1</sup> did not affect the methane oxidation performance of 2.5&#xa0;wt % Pd/SiO<sub>2</sub>@CeO<sub>2</sub> at 350°C. Moreover, the 2.5 wt % Pd/SiO<sub>2</sub>@CeO<sub>2</sub> catalyst was thermally aged at 700°C for 3 h and still exhibited 90% methane conversion at 350°C. In contrast, the methane conversions of thermally aged 2.5 wt % Pd/CeO<sub>2</sub> catalyst decreased significantly to 46%. Field emission scanning electron microscopy (FESEM) results showed that the developed Pd/SiO<sub>2</sub>@CeO<sub>2</sub> catalyst possessed the core-shell structure with Pd and CeO<sub>2</sub> coated on uniform SiO<sub>2</sub> nanospheres (~500 nm). The methane oxidation performance of the developed Pd/SiO<sub>2</sub>@CeO<sub>2</sub>, when benchmarked against reported similar Pd-based catalysts, displays superior activity under comparable reaction conditions. Overall, the findings highlight the strong potential of Pd/SiO<sub>2</sub>@CeO<sub>2</sub> for mitigating methane emissions.</p>

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Pd/SiO2(Сore)@CeO2(Shell) Catalyst for Low-Temperature Methane Oxidation under Oxygen-Rich Environments

  • Khitish Mohapatra,
  • Prateek Khatri

摘要

Abstract

Methane, a potent greenhouse gas, poses a significant risk when released into the environment. In this work, a Pd/SiO2@CeO2 catalyst was developed and evaluated for its methane oxidation performance under oxygen-rich environments. The 2.5 wt % Pd/SiO2@CeO2 achieved 10, 50, and 90% CH4 conversion at 225°C (T10), 257°C (T50), and 275°C (T90). The 2.5 wt % Pd/CeO2 was used as the reference catalyst that attained CH4 conversion of 50 and 90% at comparatively higher temperatures of 300 and 350°C under identical reaction conditions. Decreasing the Pd loading in Pd/SiO2@CeO2 to 1 wt % increased the T10, T50, and T90 to 257, 300, and 350°C, respectively. Furthermore, in a steady-state experiment of 10 h at 350°C, 2.5 wt % Pd/SiO2@CeO2 exhibited excellent durability, sustaining a ≥95% CH4 conversion without noticeable deactivation. In addition, variation in O2 (0.5–8%) and CH4 (0.11–0.5%) concentrations, and gas hourly space velocity (GHSV) between 48 000–58 000 mL g–1 h–1 did not affect the methane oxidation performance of 2.5 wt % Pd/SiO2@CeO2 at 350°C. Moreover, the 2.5 wt % Pd/SiO2@CeO2 catalyst was thermally aged at 700°C for 3 h and still exhibited 90% methane conversion at 350°C. In contrast, the methane conversions of thermally aged 2.5 wt % Pd/CeO2 catalyst decreased significantly to 46%. Field emission scanning electron microscopy (FESEM) results showed that the developed Pd/SiO2@CeO2 catalyst possessed the core-shell structure with Pd and CeO2 coated on uniform SiO2 nanospheres (~500 nm). The methane oxidation performance of the developed Pd/SiO2@CeO2, when benchmarked against reported similar Pd-based catalysts, displays superior activity under comparable reaction conditions. Overall, the findings highlight the strong potential of Pd/SiO2@CeO2 for mitigating methane emissions.