Layered double hydroxide derived NiAl-oxide hollow nanospheres for selective transfer hydrogenation with improved stability

Abstract

Selective transfer hydrogenation (STH) is an efficient strategy in biomass upgradation, especially for the production of unsaturated alcohols from biomass-derived α,β-unsaturated aldehydes. Design of effective catalysts with excellent stability for the STH is highly desired. Here, we report the synthesis of Ni₃Al₁-oxide hollow nanospheres (h-Ni₃Al₁-800) derived from Ni₃Al₁ layered double hydroxide grafted on hollow polymer spheres (HPS@Ni₃Al₁-LDH) by calcination at 800 °C in air. h-Ni₃Al₁-800 is an efficient catalyst for the STH of α,β-unsaturated aldehydes with selectivities towards α,β-unsaturated alcohols >99% at almost full conversions. More importantly, h-Ni₃Al₁-800 can be recycled at least 12 times without loss of activity. Experimental results and DFT calculations prove that the Al dopant in h-Ni₃Al₁-800 provides much stable Ni^δ+-type (2 < δ < 3) acid–base pairs which can efficiently catalyze the STH with improved stability. This work provides a promising direction for the design of STH catalysts that have potential for industrial applications.