Discovering Partially Charged Single-Atom Pt for Enhanced Anti- Ma rkovnikov Alkene Hydrosilylation

摘要

The hydrosilylation reaction is one of the largest-scale application of homogeneous catalysis and is widely used to enable the commercial manufacture of silicon products. However, considerable issues including disposable platinum consumption, undesired side reactions and unacceptable catalyst residues still remain. Here, we synthesize a heterogeneous partially charged single-atom platinum supported on anatase TiO_(2) (Pt_(1)~(δ+)/TiO_(2)) catalyst via an electrostatic-induction ion exchange and two-dimensional confinement strategy, which can catalyze hydrosilylation reaction with almost complete conversion and produce exclusive adduct. Density functional theory calculations reveal that unexpected property of Pt_(1)~(δ+)/TiO_(2) originates from atomic dispersion of active species and unique partially positive charge Pt~(δ+) electronic structure that conventional nanocatalysts do not possess. The fabrication of single-atom Pt_(1)~(δ+)/TiO_(2) catalyst accomplishes a reasonable use of Pt through recycling and maximum atom-utilized efficiency, indicating the potential to achieve a green hydrosilylation industry.