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<p>To address the shortcomings of 3D-printed catalysts and develop a highly efficient, recyclable monolithic catalyst for Knoevenagel condensation, a dual approach combining chemical functionalization and 3D-printing optimization was employed. Specifically, halloysite clay was first functionalized with a cyclodextrin-containing, melamine-based polymer to form HPCD, which served as a support for immobilizing silicotungstic acid (SiW) to yield HPCD-SiW. The electrostatic interactions between SiW and the melamine moieties of the polymer, alongside the formation of an inclusion complex with the cyclodextrin groups, successfully suppressed SiW leaching. HPCD-SiW was then 3D-printed to form a monolithic catalyst. To prevent the full coverage of HPCD-SiW with the polymeric network and enhance its accessibility, ethylene glycol (EG) was introduced as a porogen during 3D printing. This cost-effective porogen was easily removed via leaching post-printing, successfully imparting porosity to the final structure, designated as 3D-HPCD-SiW-EG. A comparison of the properties and catalytic activity of 3D-HPCD-SiW-EG against an EG-free monolith confirmed the effectiveness of this porogen-leaching approach in generating pores, resulting in superior catalytic activity due to more highly exposed active sites. Furthermore, its robust mechanical stability and minimal SiW leaching simplified catalyst recovery and significantly improved recyclability.</p>

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Combination of porogen leaching approach and DLP 3D-printing method for fabrication of catalytic monolith with improved accessibility to catalyst

  • 期刊论文

  • 发表日期：

    2026年8月3日

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  • Mahdi Rahebi,
  • Samahe Sadjadi,
  • Amir Masood Rezadoust,
  • Eric Monflier

摘要

To address the shortcomings of 3D-printed catalysts and develop a highly efficient, recyclable monolithic catalyst for Knoevenagel condensation, a dual approach combining chemical functionalization and 3D-printing optimization was employed. Specifically, halloysite clay was first functionalized with a cyclodextrin-containing, melamine-based polymer to form HPCD, which served as a support for immobilizing silicotungstic acid (SiW) to yield HPCD-SiW. The electrostatic interactions between SiW and the melamine moieties of the polymer, alongside the formation of an inclusion complex with the cyclodextrin groups, successfully suppressed SiW leaching. HPCD-SiW was then 3D-printed to form a monolithic catalyst. To prevent the full coverage of HPCD-SiW with the polymeric network and enhance its accessibility, ethylene glycol (EG) was introduced as a porogen during 3D printing. This cost-effective porogen was easily removed via leaching post-printing, successfully imparting porosity to the final structure, designated as 3D-HPCD-SiW-EG. A comparison of the properties and catalytic activity of 3D-HPCD-SiW-EG against an EG-free monolith confirmed the effectiveness of this porogen-leaching approach in generating pores, resulting in superior catalytic activity due to more highly exposed active sites. Furthermore, its robust mechanical stability and minimal SiW leaching simplified catalyst recovery and significantly improved recyclability.