Highly Active and Air-Stable Iron Phosphide Catalyst for Reductive Amination of Carbonyl Compounds Enabled by Metal–Support Synergy DOI

Tomohiro Tsuda,

Hiroya Ishikawa, Min Sheng

et al.

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: unknown

Published: April 16, 2025

Iron has long been recognized as an ideal catalytic material for sustainable chemistry. However, conventional iron catalysts employed in liquid-phase hydrogenation reactions suffer from poor activity and air instability, severely restricting their wide applicability practical use. Herein, we present the development of highly active air-stable phosphide nanocrystal immobilized on zirconia (Fe2P NC/ZrO2) reductive amination aldehydes ketones. The Fe2P NC/ZrO2 catalyst demonstrated broad substrate applicability, high recyclability, scalability both gram-scale continuous-flow processes. This leverages synergistic metal-support effect NCs ZrO2 support, leading to 313 times higher than that nanoparticle catalysts. In-depth mechanistic studies elucidated distinctive interplay between significantly accelerates ammonolysis Schiff bases, a key step boosting reaction efficiency. study sets new benchmark iron-based catalysis, offering robust alternative precious metals, thereby contributing chemical manufacturing green organic synthesis.

Language: Английский

One‐Step Low‐Temperature Synthesis of Metastable ε‐Iron Carbide Nanoparticles with Unique Catalytic Properties Beyond Conventional Iron Catalysts DOI Creative Commons
Yusuke Hirayama, Akira Miura, Motoaki Hirayama

et al.

Small, Journal Year: 2025, Volume and Issue: unknown

Published: April 24, 2025

Abstract ε ‐Iron carbide has garnered increasing interest for its superior magnetic characteristics and catalytic performance compared to other iron carbides. However, metastable nature posed significant challenges synthesis, often requiring ultrahigh pressure, multistep processes, complex reaction condition control, highly toxic reagents. Consequently, the properties of ‐iron remain largely unexplored. A simplified synthesis method can accelerate exploration new functionalities. In this study, a novel one‐step selective nanoparticles under mild conditions via wet‐chemical approach is presented. method, Fe 3 (CO) 12 , cetyltrimethylammonium bromide (CTAB), bis(pinacolato)diboron (B 2 pin ) are added hexadecylamine reacted at 220 °C—a simple process that eliminates need extreme pressures substances. Detailed investigations elucidate crucial roles CTAB B in facilitating formation carbide. This accessible efficient further enable discovery unprecedented reductive amination benzaldehyde, distinct from those conventional nanoparticle catalysts. Density functional theory calculations reveal insights into electronic states responsible activity nanoparticles.

Language: Английский

Citations

0

Highly Active and Air-Stable Iron Phosphide Catalyst for Reductive Amination of Carbonyl Compounds Enabled by Metal–Support Synergy DOI

Tomohiro Tsuda,

Hiroya Ishikawa, Min Sheng

et al.

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: unknown

Published: April 16, 2025

Iron has long been recognized as an ideal catalytic material for sustainable chemistry. However, conventional iron catalysts employed in liquid-phase hydrogenation reactions suffer from poor activity and air instability, severely restricting their wide applicability practical use. Herein, we present the development of highly active air-stable phosphide nanocrystal immobilized on zirconia (Fe2P NC/ZrO2) reductive amination aldehydes ketones. The Fe2P NC/ZrO2 catalyst demonstrated broad substrate applicability, high recyclability, scalability both gram-scale continuous-flow processes. This leverages synergistic metal-support effect NCs ZrO2 support, leading to 313 times higher than that nanoparticle catalysts. In-depth mechanistic studies elucidated distinctive interplay between significantly accelerates ammonolysis Schiff bases, a key step boosting reaction efficiency. study sets new benchmark iron-based catalysis, offering robust alternative precious metals, thereby contributing chemical manufacturing green organic synthesis.

Language: Английский

Citations

0