Tuning Nano-Nickel Catalyst Hydrogenation Aptitude by On-the-Fly Zirconium Doping

Abstract

The effect of nano-Ni catalyst post-synthetic Zr-modification on hydrogenation reaction of 6-methyl-5-hepten-2-one was investigated in a fixed bed continuous-flow micro-reactor to produce fine chemicals. The catalytic performance revealed that Zr-doping achieved by surface organometallic chemistry approach modifies the natural aptitude of nickel to hydrogenate C=C bond, since the addition of small quantities of zirconium significantly increased the amount of unsaturated and saturated alcohols formed in 6-methyl-5-hepten-2-one hydrogenation. Quantum chemical calculations revealed a stronger interaction between Zr←O=C that promotes the formation of C=C semihydrogenation product and enhances the probability of complete hydrogenation. The on-the-fly strategy presented herein enables for rapid optimization and understanding of catalytic processes.