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<p>Hydroformylation is an important industrial process for aldehyde production, but the separation of homogeneous Rh catalysts and the leaching of active Rh species remain major challenges. Here we show a heterogeneous Rh catalyst for formaldehyde hydroformylation to glycolaldehyde (GA) based on immobilized rhodium carbonyl species anchored on functionalized SiO<sub>2</sub>. Spectroscopic characterization confirms that Rh species are stabilized through Rh-P interactions, while the coordination environment of Rh can be tuned by catalyst preparation atmosphere. The catalyst prepared under syngas atmosphere generates HRh(CO)<sub>2</sub>L species, exhibiting higher catalytic activity and significantly lower Rh leaching than that prepared under N<sub>2</sub> atmosphere, without requiring additional soluble phosphine ligands. Density functional theory (DFT) calculations reveal the origin of the enhanced activity and stability by clarifying the reaction pathway and coordination stability of the active species. These findings provide insights into the structure-performance relationship of heterogeneous Rh catalysts for formaldehyde hydroformylation.</p><p></p>

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Formaldehyde hydroformylation over a heterogeneous catalyst based on a functionalized rhodium-biphosphine unit

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年8月1日

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  • Yuntao He,
  • Wanting Xia,
  • Luyang Qiao,
  • Zongkai Wu,
  • Xinyi Cao,
  • Yong Gao,
  • Jiankai Cheng,
  • Zhangfeng Zhou,
  • Yuangen Yao

摘要

Hydroformylation is an important industrial process for aldehyde production, but the separation of homogeneous Rh catalysts and the leaching of active Rh species remain major challenges. Here we show a heterogeneous Rh catalyst for formaldehyde hydroformylation to glycolaldehyde (GA) based on immobilized rhodium carbonyl species anchored on functionalized SiO2. Spectroscopic characterization confirms that Rh species are stabilized through Rh-P interactions, while the coordination environment of Rh can be tuned by catalyst preparation atmosphere. The catalyst prepared under syngas atmosphere generates HRh(CO)2L species, exhibiting higher catalytic activity and significantly lower Rh leaching than that prepared under N2 atmosphere, without requiring additional soluble phosphine ligands. Density functional theory (DFT) calculations reveal the origin of the enhanced activity and stability by clarifying the reaction pathway and coordination stability of the active species. These findings provide insights into the structure-performance relationship of heterogeneous Rh catalysts for formaldehyde hydroformylation.