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<p>The hydrogenation of esters to corresponding alcohols is a crucial yet challenging process in sustainable chemistry, demanding efficient and stable non-noble metal catalysts. In this study, a CuZnO<sub>x</sub>/CeO<sub>2</sub> metal-oxide catalyst was synthesized via a metal-organic framework (MOF)-derived route for the hydrogenation of cyclohexyl acetate. The catalyst, featuring highly dispersed Cu species and low Cu loading (11.4wt%), was obtained by calcining a Ce-MOF precursor incorporated with Cu and Zn. By modulating the reduction temperature, the mixed valence state Cu<sup>0</sup> and Cu<sup>+</sup> active species were observed to coexist on the catalyst surface. After systematic investigation of structure-activity relationship in catalytic hydrogenation, and the optimized CuZnO<sub>x</sub>/CeO<sub>2</sub>-400-350 catalyst reached 99.9% conversion of cyclohexyl acetate, with selectivity of 98.2% to cyclohexanol under mild conditions (240&#xa0;°C, 3 MPa H<sub>2</sub>, 11.4 wt% Cu loading in actual, 4&#xa0;h). Moreover, it exhibited outstanding recyclability, maintaining over 99.0% conversion and above 97.0% cyclohexanol selectivity after five cycles. XRD and XPS analyses revealed no significant changes in the crystal structure or Cu<sup>0</sup>/Cu<sup>+</sup> species after reaction, confirming excellent resistance to sintering and remarkable structural stability. This work affords a feasible way for designing high-performance catalysts for ester hydrogenation, demonstrating significant potential for industrial application.</p> Graphical Abstract <p></p>

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Enhanced Hydrogenation of Cyclohexyl Acetate by Cu0–Cu+ Dual Sites on the Bundled CuZnOx/CeO2 Catalysts

  • 期刊论文

  • 发表日期：

    2026年7月21日

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  • Zeyun Sun,
  • Jiapan Wang,
  • Weijia Pu,
  • Yang Liu,
  • Yahui Xiao,
  • Yanfeng Pu,
  • Junwei Zhao,
  • Yong Liu

摘要

The hydrogenation of esters to corresponding alcohols is a crucial yet challenging process in sustainable chemistry, demanding efficient and stable non-noble metal catalysts. In this study, a CuZnOx/CeO2 metal-oxide catalyst was synthesized via a metal-organic framework (MOF)-derived route for the hydrogenation of cyclohexyl acetate. The catalyst, featuring highly dispersed Cu species and low Cu loading (11.4wt%), was obtained by calcining a Ce-MOF precursor incorporated with Cu and Zn. By modulating the reduction temperature, the mixed valence state Cu0 and Cu+ active species were observed to coexist on the catalyst surface. After systematic investigation of structure-activity relationship in catalytic hydrogenation, and the optimized CuZnOx/CeO2-400-350 catalyst reached 99.9% conversion of cyclohexyl acetate, with selectivity of 98.2% to cyclohexanol under mild conditions (240 °C, 3 MPa H2, 11.4 wt% Cu loading in actual, 4 h). Moreover, it exhibited outstanding recyclability, maintaining over 99.0% conversion and above 97.0% cyclohexanol selectivity after five cycles. XRD and XPS analyses revealed no significant changes in the crystal structure or Cu0/Cu+ species after reaction, confirming excellent resistance to sintering and remarkable structural stability. This work affords a feasible way for designing high-performance catalysts for ester hydrogenation, demonstrating significant potential for industrial application.

Graphical Abstract