<p>Converting aqueous ethanol into higher alcohols (HAs) serves as a promising and green pathway for synthesizing valuable chemicals and sustainable fuels from renewable resources. Despite its broad potential, direct carbon chain growth of ethanol toward value-add C<sub>6+</sub> HAs remains a great challenge. In this study, we developed a novel highly hydrophobic NiSn-SDB catalyst utilizing a straightforward physical ball-milling technique. This approach effectively modulates the catalyst's surface hydrophobicity, enhancing the adsorption of alcohol molecules. The optimized NiSn-SDB<sub>1/0.5</sub> catalyst achieved an outstanding catalytic performance with C<sub>6+</sub> HAs selectivity of 70.7% at 86.4% ethanol conversion rate. Notably, the catalyst demonstrated excellent kinetic efficiency, securing 67.1% ethanol conversion and 68.7% C<sub>6+</sub> HAs selectivity within only 1-h reaction. The crucial role of hydrophobic SDB modifier was demonstrated, which enhances the adsorption of HAs molecules, thus promoting the cross coupling process to yield C<sub>6+</sub> HAs. This research presents a highly effective and practical strategy for engineering robust, hydrophobic-modified catalyst for direct aqueous ethanol coupling.</p> Graphical Abstract <p></p> <p>Efficiently upgrading aqueous bio-ethanol into C<sub>6+</sub> higher alcohols (sustainable aviation fuel precursors) is highly desirable but severely hindered by mass-transfer resistances and premature intermediate desorption. Herein, we innovatively developed a NiSn-SDB composite catalyst featuring a physical hydrophobic microenvironment. Acting as a microscopic "molecular trap," the SDB polymer grants the catalyst exceptional interfacial tracking capability and robust spatial confinement, successfully overcoming the thermodynamic bottleneck of intermediate desorption. This strategy delivers outstanding performance for C<sub>6+</sub> alcohol synthesis, offering novel insights into breaking the kinetic limitations of continuous carbon chain propagation via surface microenvironment engineering.</p>

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Constructing Highly Hydrophobic NiSn-SDB Catalyst Via Facile Physical Mixing for Aqueous Ethanol Upgrading to C6 + Alcohols

  • Xiaoyu Li,
  • Jiajin Li,
  • Bo Chen,
  • Xiaoping Wu,
  • Songbai Qiu,
  • Qian Zhang,
  • Tiejun Wang

摘要

Converting aqueous ethanol into higher alcohols (HAs) serves as a promising and green pathway for synthesizing valuable chemicals and sustainable fuels from renewable resources. Despite its broad potential, direct carbon chain growth of ethanol toward value-add C6+ HAs remains a great challenge. In this study, we developed a novel highly hydrophobic NiSn-SDB catalyst utilizing a straightforward physical ball-milling technique. This approach effectively modulates the catalyst's surface hydrophobicity, enhancing the adsorption of alcohol molecules. The optimized NiSn-SDB1/0.5 catalyst achieved an outstanding catalytic performance with C6+ HAs selectivity of 70.7% at 86.4% ethanol conversion rate. Notably, the catalyst demonstrated excellent kinetic efficiency, securing 67.1% ethanol conversion and 68.7% C6+ HAs selectivity within only 1-h reaction. The crucial role of hydrophobic SDB modifier was demonstrated, which enhances the adsorption of HAs molecules, thus promoting the cross coupling process to yield C6+ HAs. This research presents a highly effective and practical strategy for engineering robust, hydrophobic-modified catalyst for direct aqueous ethanol coupling.

Graphical Abstract

Efficiently upgrading aqueous bio-ethanol into C6+ higher alcohols (sustainable aviation fuel precursors) is highly desirable but severely hindered by mass-transfer resistances and premature intermediate desorption. Herein, we innovatively developed a NiSn-SDB composite catalyst featuring a physical hydrophobic microenvironment. Acting as a microscopic "molecular trap," the SDB polymer grants the catalyst exceptional interfacial tracking capability and robust spatial confinement, successfully overcoming the thermodynamic bottleneck of intermediate desorption. This strategy delivers outstanding performance for C6+ alcohol synthesis, offering novel insights into breaking the kinetic limitations of continuous carbon chain propagation via surface microenvironment engineering.