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

DOI: 10.1016/j.jcat.2019.03.035 DOI Help

Authors: Wenxiu Cao (Dalian Institute of Chemical Physics, Chinese Academy of Sciences; Jishou University) , Lu Lin (Dalian Institute of Chemical Physics, Chinese Academy of Sciences) , Haifeng Qi (Dalian Institute of Chemical Physics, Chinese Academy of Sciences; University of Chinese Academy of Sciences) , Qian He (Cardiff Catalysis Institute, Cardiff University) , Zhijie Wu (China University of Petroleum) , Aiqin Wang (Dalian Institute of Chemical Physics, Chinese Academy of Sciences) , Wenhao Luo (Dalian Institute of Chemical Physics, Chinese Academy of Sciences) , Tao Zhang (Dalian Institute of Chemical Physics, Chinese Academy of Sciences)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Journal Of Catalysis , VOL 373 , PAGES 161 - 172

State: Published (Approved)
Published: May 2019
Diamond Proposal Number(s): 18909

Abstract: 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@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, PH2 = 40 bar in pH = 3 or pH = 1 aqueous solution). By thorough spectroscopy characterizations, a well-defined structure of atomically dispersed Irδ+ 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.

Journal Keywords: Biomass; Catalyst stability; Levulinic acid; In-situ synthesis; Single-atom catalysis

Subject Areas: Chemistry

Diamond Offline Facilities: Electron Physical Sciences Imaging Centre (ePSIC)
Instruments: E01-JEM ARM 200CF