September 19, 2024
Journal Article

Hydrogen Spillover is Regulating Minority Rh1 Active Sites on TiO2 in Room-Temperature Ethylene Hydrogenation

Abstract

The complicated dynamics of active sites in single-atom catalysts (SACs) under reducing conditions limits their applications in hydrogenation reactions, and the fundamental understanding of their operation. Herein, we report that on Rh1/TiO2, *H spillover during room-temperature ethylene hydrogenation hydroxylates and reduces TiO2, which regulates Rh1, enhancing their intrinsic activity by 9-fold. Spectroscopic and kinetic evidence suggests that the spillover of *H is suppressed by their facile reaction with C2H4, most of the spilled *H are non-reactive spectators, and the majority (> 99%) of turnovers occur on a small subset (

Published: September 19, 2024

Citation

Chen L., D. Meira, L. Kovarik, and J. Szanyi. 2024. Hydrogen Spillover is Regulating Minority Rh1 Active Sites on TiO2 in Room-Temperature Ethylene Hydrogenation. ACS Catalysis 14, no. 10:7369-7380. PNNL-SA-191971. doi:10.1021/acscatal.4c00482

Research topics