Synthesis of Primary Amines via Reductive Amination of Aldehydes and Ketones Over a Ni‐Doped MFM‐300(Cr) Catalyst

The development of earth-abundant metal-based catalysts is an important goal for the synthesis of fine chemicals. Here, an active nickel catalyst supported on a robust metal-organic framework, MFM-300(Cr), is reported which shows an exceptional performance for reductive amination, a reaction that has long been dominated by noble metals. Ni/MFM-300(Cr) promotes the synthesis of 38 primary amines via reductive amination of their parent carbonyl compounds, including biomass-derived aldehydes and ketones, using NH<sub>3</sub> in the presence of H<sub>2</sub> operating under relatively mild conditions (5 bar and 160 °C). X-ray absorption spectroscopy confirms the formation of mixtures of metallic Ni<sup>0</sup> and Ni<sup>n+</sup> active sites, while in situ inelastic neutron scattering, coupled with modeling, reveals details of the mechanism of catalysis involving the formation of N-benzyl-1-phenylmethanediamine (BPDI) as an intermediate species in the generation of benzylamine. Cooperativity between Ni sites and MFM-300(Cr) creates an optimal microenvironment for the efficient activation of carbonyl compounds and the selective production of primary amines using a non-precious metal-based catalyst.

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Journal
Advanced Science
Published
2025-10-24
DOI
https://doi.org/10.1002/advs.202508892
Citations
3
Primary Topic
Asymmetric Hydrogenation and Catalysis
Type
article
Field-Weighted Citation Impact
1.61

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article

Synthesis of Primary Amines via Reductive Amination of Aldehydes and Ketones Over a Ni‐Doped MFM‐300(Cr) Catalyst

Svemir Rudić, Shaojun Xu, Luke L. Keenan, Yongqiang Q. Cheng et al.
3 citations
Advanced Science
Asymmetric Hydrogenation and Catalysis
1.61
article

Synthesis of Primary Amines via Reductive Amination of Aldehydes and Ketones Over a Ni‐Doped MFM‐300(Cr) Catalyst

Svemir Rudić, Shaojun Xu, Luke L. Keenan, Yongqiang Q. Cheng, Bing An, Sihai Yang⧫, Christopher M. A. Parlett, Zeyu Chen, Bing Han, Evan Tillotson, Martin Schröder, Ben F. Spencer, Danielle Crawshaw, Sarah J. Haigh, Wenyuan Huang, Jiangnan Li, Yinlin Chen, Yu Han, Xue Han
article en
3 citations

Abstract

The development of earth-abundant metal-based catalysts is an important goal for the synthesis of fine chemicals. Here, an active nickel catalyst supported on a robust metal-organic framework, MFM-300(Cr), is reported which shows an exceptional performance for reductive amination, a reaction that has long been dominated by noble metals. Ni/MFM-300(Cr) promotes the synthesis of 38 primary amines via reductive amination of their parent carbonyl compounds, including biomass-derived aldehydes and ketones, using NH<sub>3</sub> in the presence of H<sub>2</sub> operating under relatively mild conditions (5 bar and 160 °C). X-ray absorption spectroscopy confirms the formation of mixtures of metallic Ni<sup>0</sup> and Ni<sup>n+</sup> active sites, while in situ inelastic neutron scattering, coupled with modeling, reveals details of the mechanism of catalysis involving the formation of N-benzyl-1-phenylmethanediamine (BPDI) as an intermediate species in the generation of benzylamine. Cooperativity between Ni sites and MFM-300(Cr) creates an optimal microenvironment for the efficient activation of carbonyl compounds and the selective production of primary amines using a non-precious metal-based catalyst.

Advanced ScienceVol. 12(46)
Rutherford Appleton Laboratory (GB), Oak Ridge National Laboratory (US), Peking University (CN), Beijing Normal University (CN), Diamond Light Source (GB), University of Manchester (GB), Beijing National Laboratory for Molecular Sciences (CN)
National Science Foundation, Diamond Light Source, European Commission, National Natural Science Foundation of China, Engineering and Physical Sciences Research Council, Science and Technology Facilities Council, Beijing National Laboratory for Molecular Sciences, Oak Ridge National Laboratory
Openalex Percentile: Top 15%
Asymmetric Hydrogenation and Catalysis
1.61
DOIOpen Access PDFOpenAlex
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