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

摘要

The hydrogenation of levulinic acid (LA) to gamma-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@ZrO2@C single-atom catalyst was prepared via an in-situ synthesis approach during the assembly of UiO-66, followed by confined pyrolysis. The Ir@ZrO2@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 delta+ atoms onto nano-tetragonal ZrO2 confined in the amorphous carbon was identified for the Ir@ZrO2@C. The strong metal-support interaction and the confinement of the amorphous carbon account for the ultra-stability of the Ir@ZrO2@C. (C) 2019 Elsevier Inc. All rights reserved.