4.7 Article

Synergizing the Cu-only catalyst with the amino-modified mesoporous double-shelled nanoreactor for the selective transfer hydrogenation of nitriles

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ELSEVIER SCI LTD
DOI: 10.1016/j.jece.2022.109143

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Nanoreactor; Transition metals; Void-confinement effect; Selective hydrogenation; Nitrile; Hollow mesoporous nanospheres

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As a typical 3d transition metal, Cu exhibits competitive potential in the catalytic transfer hydrogenation of nitriles due to its low price and appropriate catalytic activity. Unfortunately, the Cu-based catalyst usually requires additional metals to realize good catalytic activity, this makes it difficult to understand the role of Cu. Herein, an amino-modified hollow mesoporous double-shell SiO2 @C (AmHMSiO2 @C) microsphere was applied as a nanoreactor, which achieves the high selective hydrogenation of nitriles over the Cu-only catalyst. The conversion and selectivity to primary amines were 100% and 96% respectively at 60 degrees C using amino borane as the hydrogen source, and the TOF reaches 199.75 h-1 for Cu. The unique structure of the Cu@AmHMSiO2 @C enhances the activity and stability of the Cu active sites. Comparative experiments demonstrate that the synergy between the nanoreactor and Cu nanoparticles enables the desirable catalytic performance toward the hydrogenation of nitriles to primary amines under mild reaction conditions. This work offers a distinct case for constructing an efficient Cu-based catalyst for heterogeneous hydrogenation reactions.
As a typical 3d transition metal, Cu exhibits competitive potential in the catalytic transfer hydrogenation of nitriles due to its low price and appropriate catalytic activity. Unfortunately, the Cu-based catalyst usually re-quires additional metals to realize good catalytic activity, this makes it difficult to understand the role of Cu. Herein, an amino-modified hollow mesoporous double-shell SiO2 @C (AmHMSiO2 @C) microsphere was applied as a nanoreactor, which achieves the high selective hydrogenation of nitriles over the Cu-only catalyst. The conversion and selectivity to primary amines were 100% and 96% respectively at 60 degrees C using amino borane as the hydrogen source, and the TOF reaches 199.75 h-1 for Cu. The unique structure of the Cu@AmHMSiO2 @C enhances the activity and stability of the Cu active sites. Comparative experiments demonstrate that the synergy between the nanoreactor and Cu nanoparticles enables the desirable catalytic performance toward the hydro-genation of nitriles to primary amines under mild reaction conditions. This work offers a distinct case for con-structing an efficient Cu-based catalyst for heterogeneous hydrogenation reactions.

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