In-situ synthesis of single-atom Ir by utilizing metal-organic frameworks: An acid-resistant catalyst for hydrogenation of levulinic acid to γ-valerolactone

The hydrogenation of levulinic acid (LA) to γ-valerolactone (GVL) is a key reaction for the production of renewable chemicals and fuels, wherein acid-resistant and robust catalysts are highly desired for practical usage. Herein, an ultra-stable 0.6 wt% Ir@ZrO 2 @C single-atom catalyst was prepared via an in-situ synthesis approach during the assembly of UiO-66, followed by confined pyrolysis . The Ir@ZrO 2 @C offered not only a quantitative LA conversion and an excellent GVL selectivity (>99%), but also an unprecedented stability during recycling runs under harsh conditions (at T = 453 K, P H2  = 40 bar in pH = 3 or pH = 1 aqueous solution). By thorough spectroscopy characterizations, a well-defined structure of atomically dispersed Ir δ+ atoms onto nano-tetragonal ZrO 2 confined in the amorphous carbon was identified for the Ir@ZrO 2 @C. The strong metal-support interaction and the confinement of the amorphous carbon account for the ultra-stability of the Ir@ZrO 2 @C.