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<p>Given the escalating industrial demand for γ-butyrolactone (GBL) as a critical chemical intermediate, dehydrogenation of 1,4-butanediol (BDO) to GBL has been a sustainable and environmentally friendly approach. Key challenges persist in simultaneously enhancing catalytic activity/stability and elucidating structure-activity relationships. In this work, a series of copper based catalysts (FBDH) with different ZnO contents (0, 5, 10, 20 wt%) were prepared by coprecipitation method. Physicochemical properties characterization indicated the doping of ZnO could increase the specific surface area, dispersion of Cu nanoparticles and promote the formation of moderate to strong acid sites as well as Brønsted acid sites. Dehydrogenation of BDO to GBL over the Cu-based catalysts was carried out in a fixed bed reactor. The yield of GBL reached 97.6% with a 99.6% conversion of BDO over FBDH-Zn20% at 220 ℃ (LHSV = 1.0&#xa0;h<sup>− 1</sup>), higher than that of FBDH (Conversion: 99. 6% Selectivity: 94.9% Yield: 94.5%) at the same condition. Density functional theory (DFT) calculations revealed that ZnO incorporation in FBDH lowers the activation barrier for BDO dehydrogenation by 1.2&#xa0;eV, thereby enhancing both selectivity and conversion rates. This work proposes a facile strategy for Cu-based catalyst structure design, target products regulation and catalysis mechanism investigation.</p> Graphical Abstract <p></p>

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Selectively Regulated Dehydrogenation of 1,4-Butanediol to γ-Butyrolactone via Tailoring the Structure of Copper Based Catalysts

  • 期刊论文

  • 发表日期：

    2025年6月11日

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  • Siqi Zhang,
  • Shenghua Yuan,
  • Lingchen Meng,
  • Huiling Wu,
  • Haodong Li,
  • Bofan Liu,
  • Ri Duan,
  • Haijiao Xie

摘要

Given the escalating industrial demand for γ-butyrolactone (GBL) as a critical chemical intermediate, dehydrogenation of 1,4-butanediol (BDO) to GBL has been a sustainable and environmentally friendly approach. Key challenges persist in simultaneously enhancing catalytic activity/stability and elucidating structure-activity relationships. In this work, a series of copper based catalysts (FBDH) with different ZnO contents (0, 5, 10, 20 wt%) were prepared by coprecipitation method. Physicochemical properties characterization indicated the doping of ZnO could increase the specific surface area, dispersion of Cu nanoparticles and promote the formation of moderate to strong acid sites as well as Brønsted acid sites. Dehydrogenation of BDO to GBL over the Cu-based catalysts was carried out in a fixed bed reactor. The yield of GBL reached 97.6% with a 99.6% conversion of BDO over FBDH-Zn20% at 220 ℃ (LHSV = 1.0 h− 1), higher than that of FBDH (Conversion: 99. 6% Selectivity: 94.9% Yield: 94.5%) at the same condition. Density functional theory (DFT) calculations revealed that ZnO incorporation in FBDH lowers the activation barrier for BDO dehydrogenation by 1.2 eV, thereby enhancing both selectivity and conversion rates. This work proposes a facile strategy for Cu-based catalyst structure design, target products regulation and catalysis mechanism investigation.

Graphical Abstract