High-PerformanceNickel Phosphide Confined in SBA-15for Low-Temperature Hydrogenation of Biomass-Derived Compounds

Developing cost-effective and highly active catalysts for biomass conversion under mild conditions is crucial but challenging. In this work, we present an efficient strategy for confining ultrafine nickel phosphide nanoparticles within the mesoporous channels of SBA-15, using phytic acid (PA) as both a chelating agent and an environmentally friendly phosphorus source. The optimal catalyst, 0.3PNi/SBA-15, demonstrates great catalytic performance for the selective hydrogenation of methyl levulinate (ML) into γ-valerolactone (GVL) using molecular H<sub>2</sub> as a hydrogen source, achieving a high GVL mass productivity of 32.4 mol GVL·mol Ni<sup>–1</sup>·h<sup>–1</sup> at a low temperature of 90 °C, with water as the solvent. This performance is over 54 times higher than that of pristine Ni/SBA-15 and outperforms recently reported state-of-the-art nonprecious catalysts. Detailed characterizations and density functional theory calculations (DFT) reveal that precoating the inner surface of the SBA-15 channels with PA plays a key role in dispersing and forming ultrafine Ni<sub>3</sub>P active nanoparticles. The Ni<sup>δ+</sup> species generated in ultrafine Ni<sub>3</sub>P nanoparticles through electron transfer from Ni to P exhibit strong adsorption of ML and rapid desorption of GVL, enabling faster recovery of the active sites and consequently contributing to superior performance. Furthermore, 0.3PNi/SBA-15 also exhibits high catalytic performance for the hydrogenation of a variety of aldehydes, ketones, and nitroarenes. This work provides a convenient strategy for designing promising metal phosphide catalysts for upgrading biomass-derived compounds.

Publication Details

Journal
Figshare
Published
2025-03-07
DOI
https://doi.org/10.1021/acscatal.4c08049.s001
Primary Topic
Mycorrhizal Fungi and Plant Interactions
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article
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article

High-PerformanceNickel Phosphide Confined in SBA-15for Low-Temperature Hydrogenation of Biomass-Derived Compounds

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Mycorrhizal Fungi and Plant Interactions
article

High-PerformanceNickel Phosphide Confined in SBA-15for Low-Temperature Hydrogenation of Biomass-Derived Compounds

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Abstract

Developing cost-effective and highly active catalysts for biomass conversion under mild conditions is crucial but challenging. In this work, we present an efficient strategy for confining ultrafine nickel phosphide nanoparticles within the mesoporous channels of SBA-15, using phytic acid (PA) as both a chelating agent and an environmentally friendly phosphorus source. The optimal catalyst, 0.3PNi/SBA-15, demonstrates great catalytic performance for the selective hydrogenation of methyl levulinate (ML) into γ-valerolactone (GVL) using molecular H<sub>2</sub> as a hydrogen source, achieving a high GVL mass productivity of 32.4 mol GVL·mol Ni<sup>–1</sup>·h<sup>–1</sup> at a low temperature of 90 °C, with water as the solvent. This performance is over 54 times higher than that of pristine Ni/SBA-15 and outperforms recently reported state-of-the-art nonprecious catalysts. Detailed characterizations and density functional theory calculations (DFT) reveal that precoating the inner surface of the SBA-15 channels with PA plays a key role in dispersing and forming ultrafine Ni<sub>3</sub>P active nanoparticles. The Ni<sup>δ+</sup> species generated in ultrafine Ni<sub>3</sub>P nanoparticles through electron transfer from Ni to P exhibit strong adsorption of ML and rapid desorption of GVL, enabling faster recovery of the active sites and consequently contributing to superior performance. Furthermore, 0.3PNi/SBA-15 also exhibits high catalytic performance for the hydrogenation of a variety of aldehydes, ketones, and nitroarenes. This work provides a convenient strategy for designing promising metal phosphide catalysts for upgrading biomass-derived compounds.

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High-PerformanceNickel Phosphide Confined in SBA-15for Low-Temperature Hydrogenation of Biomass-Derived Compounds · Figshare (2025) | TGRS Research Map | TGRS