<p>Unburned methanol emissions from methanol-fueled engines have attracted significant attention owing to their inherent toxicity and the associated threats to environmental and human health. Catalytic oxidation has been established as a promising and efficient strategy for methanol removal. In this study, a series of Co-modified Cu/ZSM-5 catalysts with varying Co doping amounts (<i>x</i> = 0, 0.1, 0.3, 0.5, 0.7 wt%) were synthesized via the impregnation method, and their catalytic performance for methanol oxidation was evaluated. The results demonstrate that the introduction of a moderate amount of Co significantly enhances catalytic activity. Notably, Co<sub>0.5</sub>Cu/ZSM-5 catalyst attained 90% methanol conversion at 160&#xa0;°C (T<sub>90</sub>), considerably outperforming Cu/ZSM-5 catalyst. This enhancement is primarily attributed to the strong interaction between the Co and Cu bimetals. On one hand, this interaction induces the formation of surface oxygen vacancies, which promote the production and migration of reactive oxygen species. On the other hand, the enrichment of Co<sup>3+</sup> species improves the overall redox capability of Co<sub>0.5</sub>Cu/ZSM-5 catalyst and optimizes the surface basic site distribution. In-situ DRIFTS indicates that Co incorporation facilitates the rapid transformation of the key formate intermediate. Additionally, the methanol oxidation reaction over Co<sub>0.5</sub>Cu/ZSM-5 catalyst exhibits a pronounced temperature dependence.</p> Graphical Abstract <p></p>

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Effect of Co Modification on Methanol Oxidation Performance of Cu/ZSM-5 Catalysts: Redox Capability and Basic Site Distribution

  • Sihan Yin,
  • Zhitao Han,
  • Jiyue Wang,
  • Junhao Jing,
  • Liangzheng Lin,
  • Yang Che,
  • Yangbo Deng

摘要

Unburned methanol emissions from methanol-fueled engines have attracted significant attention owing to their inherent toxicity and the associated threats to environmental and human health. Catalytic oxidation has been established as a promising and efficient strategy for methanol removal. In this study, a series of Co-modified Cu/ZSM-5 catalysts with varying Co doping amounts (x = 0, 0.1, 0.3, 0.5, 0.7 wt%) were synthesized via the impregnation method, and their catalytic performance for methanol oxidation was evaluated. The results demonstrate that the introduction of a moderate amount of Co significantly enhances catalytic activity. Notably, Co0.5Cu/ZSM-5 catalyst attained 90% methanol conversion at 160 °C (T90), considerably outperforming Cu/ZSM-5 catalyst. This enhancement is primarily attributed to the strong interaction between the Co and Cu bimetals. On one hand, this interaction induces the formation of surface oxygen vacancies, which promote the production and migration of reactive oxygen species. On the other hand, the enrichment of Co3+ species improves the overall redox capability of Co0.5Cu/ZSM-5 catalyst and optimizes the surface basic site distribution. In-situ DRIFTS indicates that Co incorporation facilitates the rapid transformation of the key formate intermediate. Additionally, the methanol oxidation reaction over Co0.5Cu/ZSM-5 catalyst exhibits a pronounced temperature dependence.

Graphical Abstract