<p>The upgrading of underutilized methane in shale gas with anthropogenic CO<sub>2</sub> can produce the value-added syngas via dry reforming. Nickel-based catalysts, due to their efficiency and cost-effectiveness, have received widespread attention. However, Ni-catalyzed dry reforming of methane is usually subjected to sintering or coking-induced instability. To address these issues, a series of Al<sub>2</sub>O<sub>3</sub>-supported nickel nanoparticle catalysts with uniform sizes are synthesized by varying the calcination temperatures and applied in methane dry reforming (DRM). Ni/Al<sub>2</sub>O<sub>3</sub>-700 °C catalyst behaves better catalytic performance compared to the other catalysts, which can be attributed to its higher metal dispersion and stronger metal-support interaction. In addition, the abundant moderate-strength basic sites and optimal Al<sub>IV</sub>/Al<sub>VI</sub> ratio can promote the adsorption and activation of CO<sub>2</sub> and suppress the deep cracking of CH<sub>4</sub> for Ni/Al<sub>2</sub>O<sub>3</sub>-700 °C catalyst, respectively, causing the enhancement of anti-coking performance. Furthermore, combining CH<sub>4</sub>-temperature programmed surface reaction and <i>in situ</i> Fourier transform infrared spectroscopy demonstrates that the presence of CO<sub>2</sub> can promote the activation of CH<sub>4</sub> for Ni/Al<sub>2</sub>O<sub>3</sub>-700 °C catalyst, which is rate-determining step for DRM system. These findings provide valuable theoretical guidance for the rational design of Ni-based catalysts with enhanced catalytic performance.</p>

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Ni nanoparticles with high thermal stability for methane dry reforming

  • Meng Han,
  • Dan Guo,
  • Xuening Zhang,
  • Yitong Yao,
  • Haozhe Zhang,
  • Yifei Lu,
  • Zelong Fu,
  • Jing Lv,
  • Yong Wang,
  • Joe Yeang Cheah,
  • Shengping Wang,
  • Xinbin Ma

摘要

The upgrading of underutilized methane in shale gas with anthropogenic CO2 can produce the value-added syngas via dry reforming. Nickel-based catalysts, due to their efficiency and cost-effectiveness, have received widespread attention. However, Ni-catalyzed dry reforming of methane is usually subjected to sintering or coking-induced instability. To address these issues, a series of Al2O3-supported nickel nanoparticle catalysts with uniform sizes are synthesized by varying the calcination temperatures and applied in methane dry reforming (DRM). Ni/Al2O3-700 °C catalyst behaves better catalytic performance compared to the other catalysts, which can be attributed to its higher metal dispersion and stronger metal-support interaction. In addition, the abundant moderate-strength basic sites and optimal AlIV/AlVI ratio can promote the adsorption and activation of CO2 and suppress the deep cracking of CH4 for Ni/Al2O3-700 °C catalyst, respectively, causing the enhancement of anti-coking performance. Furthermore, combining CH4-temperature programmed surface reaction and in situ Fourier transform infrared spectroscopy demonstrates that the presence of CO2 can promote the activation of CH4 for Ni/Al2O3-700 °C catalyst, which is rate-determining step for DRM system. These findings provide valuable theoretical guidance for the rational design of Ni-based catalysts with enhanced catalytic performance.