Novel layered double hydroxide/oxide-coated nickel-based core–shell nanocomposites for benzonitrile selective hydrogenation: An interesting water switch

•Two novel Ni@mSiO2@LDO and Ni@mSiO2@LDH nanocomposites were first prepared.•They can be interconverted through calcination/reduction and hydration.•Water acted as a switch to tune their structures and acid–base properties.•These nanocomposites showed different selectivity in benzonitrile hydrogenation.

Two novel layered double hydroxide (LDH)/layered double oxide (LDO)-coated nickel-based core–shell nanocomposites were first prepared from a hydrotalcite-like precursor. Water was found to act as a switch to tune the structures and acid–base properties between Ni@mSiO2@LDO and Ni@mSiO2@LDH, as demonstrated by transmission electron microscopy and temperature-programmed desorption of ammonia, resulting in chemoselective hydrogenation of benzonitrile to afford N-benzylidenebenzylamine (selectivity 92.3%) and benzylamine (selectivity 76.1%), respectively.

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