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<p>This study investigates the in-situ hydrogenation upgrading of coal pyrolysis gas-phase tar using a nickel-based catalyst, examining the effects of Ni loading and the Si/Al ratio of HZSM-5 on catalytic performance, and employing deuterium isotope tracing to elucidate the reaction mechanism. The results showed that in the Ni/γ-Al<sub>2</sub>O<sub>3</sub> catalyst, a Ni loading of 5 wt% achieved the optimal upgrading effect, with light aromatic hydrocarbon content reaching 61.68% and cycloalkane content at 9.58%; In the Ni/HZSM-5 catalyst, a Si/Al ratio of 50 exhibited the highest monocyclic aromatic hydrocarbon selectivity (41.62%, an increase of 38.2% compared to the None group) and the lowest polycyclic aromatic hydrocarbon content (21.74% for bicyclic and 8.72% for tricyclic). NH<sub>3</sub>-TPD and elemental analysis indicated that increased acid content enhanced sulfur and nitrogen removal efficiency (35.8% and 29.5%), but excessive acidity reduced tar yield to 5.332 wt%. EA-IRMS results under deuterium atmosphere showed that the catalyst with a Si/Al ratio of 50 had the highest deuterium content of 1.745&#xa0;mg/g, confirming that the synergistic effect between acidic sites and Ni active centers promotes the activation and incorporation of external hydrogen.</p>

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In situ hydrogenation upgrading of coal pyrolysis gas phase tar using nickel-based catalysts: catalytic principles and isotope tracing insights

  • 期刊论文

  • 发表日期：

    2025年10月8日

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  • Menglong Niu,
  • Yongge Xue,
  • Ben Niu,
  • Yinlong Chen,
  • Lei Zhang,
  • Xindong Li

摘要

This study investigates the in-situ hydrogenation upgrading of coal pyrolysis gas-phase tar using a nickel-based catalyst, examining the effects of Ni loading and the Si/Al ratio of HZSM-5 on catalytic performance, and employing deuterium isotope tracing to elucidate the reaction mechanism. The results showed that in the Ni/γ-Al2O3 catalyst, a Ni loading of 5 wt% achieved the optimal upgrading effect, with light aromatic hydrocarbon content reaching 61.68% and cycloalkane content at 9.58%; In the Ni/HZSM-5 catalyst, a Si/Al ratio of 50 exhibited the highest monocyclic aromatic hydrocarbon selectivity (41.62%, an increase of 38.2% compared to the None group) and the lowest polycyclic aromatic hydrocarbon content (21.74% for bicyclic and 8.72% for tricyclic). NH3-TPD and elemental analysis indicated that increased acid content enhanced sulfur and nitrogen removal efficiency (35.8% and 29.5%), but excessive acidity reduced tar yield to 5.332 wt%. EA-IRMS results under deuterium atmosphere showed that the catalyst with a Si/Al ratio of 50 had the highest deuterium content of 1.745 mg/g, confirming that the synergistic effect between acidic sites and Ni active centers promotes the activation and incorporation of external hydrogen.