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<p>The production of valuable chemicals from glycerol can alleviate its large market surplus and reduce emissions that arise from petrochemical-based feedstocks. Here we show that a thermo-electroreduction strategy can expand the scope of glycerol valorization to a product of higher effective H/C ratio, such as propylene glycol. The thermal dehydration of glycerol unlocks the hydroxyacetone intermediate, which can undergo subsequent electrocatalytic hydrogenation to propylene glycol using Co-cluster-decorated Cu foam electrocatalyst. Theoretical simulations suggest that Co/Cu modulates the adsorption configuration of hydroxyacetone, such that all functional groups are in similar distance from the surrounding water layer and the surface. This can facilitate low-energy-barrier hydrogenation of the O atom on hydroxyacetone by solvated H species through an Eley-Rideal-type mechanism, followed by spontaneous hydrogenation of the adjacent C atom. We thus achieve high Faradaic efficiencies towards propylene glycol of ~81% even at current densities up to 1000 mA/cm<sup>2</sup>.</p>

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A thermo-electroreduction strategy unlocks propylene glycol synthesis from glycerol at ampere level current density

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年11月29日

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  • Huaiyu Chang,
  • Longhai Zhang,
  • Ziyu Mi,
  • Panyawut Tonanon,
  • Chengyi Liu,
  • Xun Cao,
  • Mingsheng Zhang,
  • Jiajian Gao,
  • Shibo Xi,
  • Richard D. Webster,
  • Haobo Li,
  • Wan Ru Leow

摘要

The production of valuable chemicals from glycerol can alleviate its large market surplus and reduce emissions that arise from petrochemical-based feedstocks. Here we show that a thermo-electroreduction strategy can expand the scope of glycerol valorization to a product of higher effective H/C ratio, such as propylene glycol. The thermal dehydration of glycerol unlocks the hydroxyacetone intermediate, which can undergo subsequent electrocatalytic hydrogenation to propylene glycol using Co-cluster-decorated Cu foam electrocatalyst. Theoretical simulations suggest that Co/Cu modulates the adsorption configuration of hydroxyacetone, such that all functional groups are in similar distance from the surrounding water layer and the surface. This can facilitate low-energy-barrier hydrogenation of the O atom on hydroxyacetone by solvated H species through an Eley-Rideal-type mechanism, followed by spontaneous hydrogenation of the adjacent C atom. We thus achieve high Faradaic efficiencies towards propylene glycol of ~81% even at current densities up to 1000 mA/cm2.