Interfacial Spontaneous Reduction Strategy to Synthesize Low-Valent Pt Single-Atom Catalyst for Boosting Hydrosilylation

A heterogeneous N-coordinated Pt single-atom catalyst with low valence was synthesized via an “interfacial spontaneous reduction (ISR)” strategy under mild conditions, using cheap and widely available industrial raw materials. The reducing groups were modified onto commercial carbon black XC-72R, which was able to reduce the Pt species at the solid–liquid interface without the need of an extra reducing agent, followed by in situ coordination of the reduced Pt atoms, preventing their aggregation. The prepared Pt single-atom catalyst (Pt₁–N–C) acted as an actual reactive center for hydrosilylation and catalyzed the reaction directly, resulting in the absence of an induction period and an ultrahigh turnover frequency of 9.3 × 10⁶ h^–1. Moreover, the catalysts can be used on a wide range of olefin and silane substrates, achieving a turnover number of over 4.5 × 10⁶ in the subkilogram-scale reaction. The ISR strategy provides a low-cost method to prepare noble metal single atoms on industrial-grade materials with the potential for large-scale preparation and application.