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<p>Efficiently converting CO<sub>2</sub> into methanol through catalytic process is an important approach to alleviate energy crisis and realize the “net-zero emissions” and resource utilization of CO<sub>2</sub>, especially at high temperature above 320&#xa0;°C. Herein, this study reports a ZnZrOx composite metal oxide catalyst that can efficiently convert CO<sub>2</sub> and H<sub>2</sub> to methanol. A series of ZnZrOx catalysts with varying Zr/Zn ratios (Zr/Zn = 5, 10, 20, 30 and 50, molar ratio) were synthesized via coprecipitation method, and they were comprehensively characterized by XRD, TEM-mapping, ICP, H<sub>2</sub>-TPR, CO<sub>2</sub>-TPD and XPS techniques. The influence of Zr/Zn ratio on the physical and chemical properties of prepared ZnZrOx catalysts and the promoting effect of Zn on oxygen vacancies were also thoroughly discussed. In addition, the catalytic performance of ZnZrOx catalysts for CO<sub>2</sub> hydrogenation to methanol at high temperature was evaluated systematically. The tetragonal phase of <i>t</i>-ZrO<sub>2</sub> was observed in ZnZrOx, and Zn and Zr species were uniformly dispersed throughout the catalysts. The excellent synergistic effect between ZrO<sub>2</sub> and Zn of ZnZrOx catalyst with appropriate Zr/Zn ratio promotes the H<sub>2</sub> activation and CO<sub>2</sub> adsorption, and also the concentration of oxygen vacancies directly regulates the activation of CO<sub>2</sub>. Under the reaction condition of 350&#xa0;°C, 3&#xa0;MPa and GHSV = 3000&#xa0;h<sup>−1</sup>, ZnZrOx catalyst with Zr/Zn ratio of 30 exhibits the outstanding catalytic performance for CO<sub>2</sub> hydrogenation to methanol. The CO<sub>2</sub> conversion reaches as high as 33.8%, and the selectivity and STY of methanol are 98.3% and 7.7&#xa0;mmol&#xa0;h<sup>−1</sup>&#xa0;g<sup>−1</sup>, respectively, demonstrating the catalyst’s superior CO<sub>2</sub> conversion capabilities at high temperature.</p>

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Study on ZnZrOx catalysts with varying Zr/Zn ratio for CO2 hydrogenation to methanol at high temperature

  • 期刊论文

  • 发表日期：

    2026年5月25日

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  • Lu Zhang,
  • Pingping Zhao,
  • Jianqing Li,
  • Guangbo Liu,
  • Jingli Wu,
  • Pengjie Miao,
  • Zhenkun Liu,
  • Teng Li,
  • Yingluo He,
  • Noritatsu Tsubaki,
  • Jinhu Wu

摘要

Efficiently converting CO2 into methanol through catalytic process is an important approach to alleviate energy crisis and realize the “net-zero emissions” and resource utilization of CO2, especially at high temperature above 320 °C. Herein, this study reports a ZnZrOx composite metal oxide catalyst that can efficiently convert CO2 and H2 to methanol. A series of ZnZrOx catalysts with varying Zr/Zn ratios (Zr/Zn = 5, 10, 20, 30 and 50, molar ratio) were synthesized via coprecipitation method, and they were comprehensively characterized by XRD, TEM-mapping, ICP, H2-TPR, CO2-TPD and XPS techniques. The influence of Zr/Zn ratio on the physical and chemical properties of prepared ZnZrOx catalysts and the promoting effect of Zn on oxygen vacancies were also thoroughly discussed. In addition, the catalytic performance of ZnZrOx catalysts for CO2 hydrogenation to methanol at high temperature was evaluated systematically. The tetragonal phase of t-ZrO2 was observed in ZnZrOx, and Zn and Zr species were uniformly dispersed throughout the catalysts. The excellent synergistic effect between ZrO2 and Zn of ZnZrOx catalyst with appropriate Zr/Zn ratio promotes the H2 activation and CO2 adsorption, and also the concentration of oxygen vacancies directly regulates the activation of CO2. Under the reaction condition of 350 °C, 3 MPa and GHSV = 3000 h−1, ZnZrOx catalyst with Zr/Zn ratio of 30 exhibits the outstanding catalytic performance for CO2 hydrogenation to methanol. The CO2 conversion reaches as high as 33.8%, and the selectivity and STY of methanol are 98.3% and 7.7 mmol h−1 g−1, respectively, demonstrating the catalyst’s superior CO2 conversion capabilities at high temperature.