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

JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING(2023)

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摘要
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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关键词
Nanoreactor,Transition metals,Void-confinement effect,Selective hydrogenation,Nitrile,Hollow mesoporous nanospheres
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