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<p>The hydrogenation of CO<sub>2</sub> to methanol represents a promising route for carbon capture and utilization, yet designing catalysts that simultaneously achieve high activity, selectivity, and stability remains a major challenge. Here, we engineer a Fe-Zn co-doped ZrO<sub>2</sub> catalyst featuring highly active interfacial sites using a CO<sub>2</sub> supercritical treatment strategy. <i>In situ</i> spectroscopic and microscopic characterizations confirm that the Fe-Zn dual-doping formed asymmetric M-O-Zr (M = Fe, Zn) sites and increased the oxygen vacancy concentration, which significantly enhances CO<sub>2</sub> adsorption and promotes the hydrogenation of key intermediates (HCOO* and COOH*) toward methanol. The optimized Fe<sub>2</sub>Zn-ZrO<sub>2</sub> catalyst exhibits a methanol formation rate more than 10 times that of undoped ZrO<sub>2</sub>, achieving 81.9% methanol selectivity at 300 °C. Moreover, it demonstrates remarkable stability over 100 h and a high space-time yield of 655.5 g kg<sup>−1</sup> h<sup>−1</sup> under industrially relevant conditions. This work highlights the crucial role of bimetallic doping in constructing highly active interfacial sites and provides a feasible strategy for developing efficient CO<sub>2</sub> hydrogenation catalysts.</p>

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Fe-Zn co-doping creates highly active interfaces on ZrO2 for efficient CO2 hydrogenation to methanol

  • 期刊论文

  • 发表日期：

    2026年4月14日

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  • Lijun Zhang,
  • Luyao Wu,
  • Teng Li,
  • Shuangqian Wang,
  • Zhiwei Ye,
  • Bo Wang,
  • Peng Qin,
  • Mengying Du,
  • Qingchen Feng,
  • Chenchen Cai,
  • Wei Xia,
  • Guangbo Liu,
  • Zhirong Zhang,
  • Jie Zeng,
  • Noritatsu Tsubaki

摘要

The hydrogenation of CO2 to methanol represents a promising route for carbon capture and utilization, yet designing catalysts that simultaneously achieve high activity, selectivity, and stability remains a major challenge. Here, we engineer a Fe-Zn co-doped ZrO2 catalyst featuring highly active interfacial sites using a CO2 supercritical treatment strategy. In situ spectroscopic and microscopic characterizations confirm that the Fe-Zn dual-doping formed asymmetric M-O-Zr (M = Fe, Zn) sites and increased the oxygen vacancy concentration, which significantly enhances CO2 adsorption and promotes the hydrogenation of key intermediates (HCOO* and COOH*) toward methanol. The optimized Fe2Zn-ZrO2 catalyst exhibits a methanol formation rate more than 10 times that of undoped ZrO2, achieving 81.9% methanol selectivity at 300 °C. Moreover, it demonstrates remarkable stability over 100 h and a high space-time yield of 655.5 g kg−1 h−1 under industrially relevant conditions. This work highlights the crucial role of bimetallic doping in constructing highly active interfacial sites and provides a feasible strategy for developing efficient CO2 hydrogenation catalysts.