<p>The tandem conversion of C<sub>2</sub>H<sub>6</sub> and CO<sub>2</sub> provides an opportunity to utilize underused shale gas while reducing greenhouse gas emissions efficiently. Although desirable, this transformation poses considerable challenges, particularly in the realm of catalyst design either through CO<sub>2</sub>-assisted ethane dehydrogenation (CO<sub>2</sub>-EDH) to produce ethene or by dry reforming (DR) to produce syngas. Here, we found that the morphology of CeO<sub>2</sub> could determine which pathway was predominant. Transmission electron microscope (TEM) and X-ray photoelectron spectrometer (XPS) analyses of Pt and Sn showed that the spherical morphology of CeO<sub>2</sub> was more conducive to generating platinum-tin metal clusters than CeO<sub>2</sub> nanorod, illustrating the relatively high C<sub>2</sub>H<sub>4</sub> selectivity (93.50%) of the spherical structure. In contrast, the nanorod-shaped CeO<sub>2</sub> demonstrated enhanced activation of reactants and facilitated the reaction towards synthesis gas production, with a remarkable CO<sub>2</sub> conversion rate of 84%, which was much higher than previous works. Electron paramagnetic resonance (EPR) spectroscopy and XPS analysis of oxygen revealed that the nanorod-shaped CeO<sub>2</sub> had more oxygen vacancies, enhancing CO<sub>2</sub> adsorption capacity and promoting the dispersion of active species, which were crucial for efficient tandem catalytic reactions. These findings provide a promising approach to advancing catalyst design for efficient shale gas utilization in a carbon-negative manner.</p> Graphical Abstract <p></p>

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Morphology-dependent Selectivity Switching of CeO2 in Tandem Conversion of Ethane and CO2

  • Guozhi Lei,
  • Shengpeng Xia,
  • Kun Zhao,
  • Zengli Zhao,
  • Anqing Zheng

摘要

The tandem conversion of C2H6 and CO2 provides an opportunity to utilize underused shale gas while reducing greenhouse gas emissions efficiently. Although desirable, this transformation poses considerable challenges, particularly in the realm of catalyst design either through CO2-assisted ethane dehydrogenation (CO2-EDH) to produce ethene or by dry reforming (DR) to produce syngas. Here, we found that the morphology of CeO2 could determine which pathway was predominant. Transmission electron microscope (TEM) and X-ray photoelectron spectrometer (XPS) analyses of Pt and Sn showed that the spherical morphology of CeO2 was more conducive to generating platinum-tin metal clusters than CeO2 nanorod, illustrating the relatively high C2H4 selectivity (93.50%) of the spherical structure. In contrast, the nanorod-shaped CeO2 demonstrated enhanced activation of reactants and facilitated the reaction towards synthesis gas production, with a remarkable CO2 conversion rate of 84%, which was much higher than previous works. Electron paramagnetic resonance (EPR) spectroscopy and XPS analysis of oxygen revealed that the nanorod-shaped CeO2 had more oxygen vacancies, enhancing CO2 adsorption capacity and promoting the dispersion of active species, which were crucial for efficient tandem catalytic reactions. These findings provide a promising approach to advancing catalyst design for efficient shale gas utilization in a carbon-negative manner.

Graphical Abstract